☆ 4.6 Review

Recent Advances in Non-Precious Metal Single-Atom Electrocatalysts for Oxygen Reduction Reaction in Low-Temperature Polymer-Electrolyte Fuel Cells

CHEMCATCHEM (2023)

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Article Chemistry, Multidisciplinary

ZIF-8-Derived Dual Metal (Fe, Ni)-Nitrogen-Doped Porous Carbon for Superior ORR Performance in Universal Acid-Base Properties Solutions

Zijian Zhou et al.

Summary: Fe-N/C catalysts show comparable oxygen reduction reaction (ORR) activity to Pt/C catalysts, making them the most promising non-precious metal material for research. However, their development and application are limited by the Fenton effect and inadequate stability. In this study, FeNi-nitrogen-doped porous carbon (FeNi-NPC) catalysts were fabricated using a solvent thermal method, with glucose as a soft template to control the pore structure and active specific surface area. Due to the electronic effect of the bimetal, FeNi-NPC catalysts exhibit superior ORR activity and stability to Pt/C catalysts in both acidic and alkaline conditions. They also demonstrated higher peak power densities in proton exchange membrane fuel cells (PEMFC) compared to currently reported M-N/C catalysts. This work will contribute to the design of efficient ORR electrocatalysts in PEMFC devices.

ISRAEL JOURNAL OF CHEMISTRY (2023)

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Article Chemistry, Physical

Novel acid-free process intensification for the synthesis of non-precious metal-nitrogen-carbon electrocatalysts for oxygen reduction reaction

Alessio Cosenza et al.

Summary: In this study, a set of PGM-free mono-metallic electrocatalysts were synthesized using multiple silica templates and a modified acid-free sacrificial support method. The iron-based electrocatalysts showed higher activity for oxygen reduction reaction (ORR) compared to other catalysts.

JOURNAL OF POWER SOURCES (2023)

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Article Chemistry, Physical

Lignin-derived bimetallic platinum group metal-free oxygen reduction reaction electrocatalysts for acid and alkaline fuel cells

Mohsin Muhyuddin et al.

Summary: Metal-nitrogen-carbons (M-N-Cs) are reliable substitutes for platinum-group-metals (PGMs) for oxygen reduction reaction (ORR), and can be economically produced by utilizing waste biomass as a low-cost carbon source. In this study, electrocatalysts derived from lignin-derived activated char were fabricated and characterized. The results showed that the metal phthalocyanine-functionalized activated char exhibited defect-rich architecture and various nitrogen-containing active moieties, leading to appreciable ORR activity in both acidic and alkaline conditions. Moreover, the integrated L_FeMn cathode electrocatalyst demonstrated promising performance in both PEMFC and AEMFC, with a peak power density of 261 mW cm-2 at -577 mA cm-2.

JOURNAL OF POWER SOURCES (2023)

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Article Chemistry, Physical

State-of-the-art and developmental trends in platinum group metal-free cathode catalyst for anion exchange membrane fuel cell (AEMFC)

Mosaddek Hossen et al.

Summary: Non-platinum catalysts are essential for the economical application of AEMFC, and this review summarizes the advancements in the synthesis of different components and structures of catalysts. Thirteen catalysts have surpassed the peak power density threshold of 1000 mW.cm-2, including Metal-Nitrogen-Carbon (M-N-C), Bimetals-Nitrogen-Carbon (MM-N-C), Transition metal oxides (TMO), and non-metallic catalysts (NMC). The improvement in catalyst's porosity, surface area, conjugation of active sites, and synthesis procedures greatly affect the ORR activity and fuel cell performance.

APPLIED CATALYSIS B-ENVIRONMENTAL (2023)

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Article Chemistry, Physical

Altering the spin state of Fe-N-C through ligand field modulation of single-atom sites boosts the oxygen reduction reaction

Dongping Xue et al.

Summary: This study demonstrates the electron spin-state modulation of Fe active centers in SA Fe-N-C catalysts, resulting in improved ORR activity. By converting defect-rich pyrrolic N-coordinated FeNx sites, the low-spin state of Fe active centers can be transformed into a high-spin state, enhancing the ORR reaction kinetics significantly. The designed Fe-N4-HS catalyst shows comparable ORR activity to commercial Pt/C catalyst and exhibits higher performances in proton exchange membrane fuel cells and zinc-air batteries.

NANO ENERGY (2023)

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Review Chemistry, Multidisciplinary

Rational Design of Atomically Dispersed Metal Site Electrocatalysts for Oxygen Reduction Reaction

Kechuang Wan et al.

Summary: This review provides a systematic summary of the design principles for high-efficiency atomically dispersed metal site electrocatalysts (ADMSEs), including the fundamental mechanisms, theoretical calculations, characterization techniques, synthesis methods, and effective strategies. The challenges in practical applications and future research directions are also proposed. This review aims to enhance the understanding of catalytic mechanisms and provide valuable guidance for the development of advanced ADMSEs for sustainable energy conversion and storage techniques.

ADVANCED SCIENCE (2023)

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Article Chemistry, Physical

Cu-N-bridged Fe-3d electron state regulations for boosted oxygen reduction in flexible battery and PEMFC

Fantao Kong et al.

Summary: A novel multi-step collaborative synthesis strategy was proposed to fabricate N-bridged Fe and Cu diatomic electrocatalysts with tunable electronic structures. The optimized catalyst exhibited significantly enhanced oxygen reduction reaction performances in both alkaline and acidic media.

ENERGY STORAGE MATERIALS (2023)

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Article Nanoscience & Nanotechnology

Atomically Dispersed Isolated Fe-Ce Dual-Metal-Site Catalysts for Proton-Exchange Membrane Fuel Cells

Bolong Yang et al.

Summary: By constructing Fe-Ce atomic pairs, the adsorption structure is changed and the linear relationship between catalytic activity and adsorption energy of reaction intermediates based on single-metal sites is broken, leading to excellent oxygen reduction reaction (ORR) performances of the FeCe-SAD/HPNC catalyst.

ACS APPLIED MATERIALS & INTERFACES (2023)

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Article Chemistry, Multidisciplinary

Hierarchically Porous Carbons with Highly Curved Surfaces for Hosting Single Metal FeN4 Sites as Outstanding Oxygen Reduction Catalysts

Guangbo Chen et al.

Summary: A Fe-N-C electrocatalyst with dense FeN4 sites on hierarchically porous carbons with highly curved surfaces (FeN4-hcC) is reported, which displays exceptional ORR activity in acidic media. When integrated into a membrane electrode assembly, the corresponding cathode shows a high maximum peak power density and operating durability over 30,000 cycles, outperforming previously reported Fe-N-C electrocatalysts. This work provides new insight into the carbon nanostructure-activity correlation for ORR catalysis and offers a new approach to designing advanced single-metal-site catalysts for energy-conversion applications.

ADVANCED MATERIALS (2023)

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Article Chemistry, Physical

Atomization driven crystalline nanocarbon based single-atom catalysts for superior oxygen electroreduction

Jae Young Jung et al.

Summary: This study demonstrates the occurrence of atom-migration-trapping (AMT) phenomena in crystalline porous nanocarbon and develops highly efficient single-atom catalysts (SACs) through systematic investigation of atomization process and chemical state of active sites. The pre-formed N-functionalities in the catalyst play a crucial role in capturing single metal species, and additional ammonia treatment successfully modulates the coordination geometry of active sites. The atomic cobalt catalyst exhibits superior oxygen reduction activity and remarkable power performance in single-cell experiments, surpassing reported Co-N atomic catalysts.

APPLIED CATALYSIS B-ENVIRONMENTAL (2023)

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Article Engineering, Environmental

In-situ growth of carbon nanotubes for improving the performance of Co-N/ C in membrane fuel cell

Xi-Ming Qua et al.

Summary: In this study, massive carbon nanotubes (CNTs) were grown in-situ during the synthesis of Co-N/C catalysts by precisely controlling the reactant ratio. The dense deformed Co-N4 sites were anchored on the in-situ grown CNTs, improving the triple-phase boundary and proton electronic conductivity of membrane electrode assemblies (MEA). The target catalyst Co-N/C-1/4.4 exhibited high activity in both oxygen reduction reaction and fuel cell tests, with improved stability.

CHEMICAL ENGINEERING JOURNAL (2023)

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Article Chemistry, Multidisciplinary

Decoupling the Contributions of Different Instability Mechanisms to the PEMFC Performance Decay of Non-noble Metal O2-Reduction Catalysts

Secil Unsal et al.

Summary: Non-noble metal catalysts (NNMCs) have the potential to replace expensive Pt-based materials in proton exchange membrane fuel cells (PEMFCs), but their poor durability hinders their commercial implementation. The degradation mechanisms include operative demetallation, electro-oxidation of the carbonaceous matrix, and chemical degradation caused by H2O2 radicals. However, the relative contributions of these mechanisms to overall performance loss are not well understood. In this study, degradation protocols were used to determine that H2O2-related instability is dependent on the ORR charge, while electro-oxidation of the carbon matrix at high potentials is more detrimental to NNMCs' activity than demetallation at low potentials.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2023)

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Article Chemistry, Multidisciplinary

High Density Single Fe Atoms on Mesoporous N-Doped Carbons: Noble Metal-Free Electrocatalysts for Oxygen Reduction Reaction in Acidic and Alkaline Media

Haifang Xie et al.

Summary: Efficient oxygen reduction reaction (ORR) electrocatalysts are in high demand for various renewable energy systems. This study reports the synthesis of a highly efficient ORR electrocatalyst composed of N-doped mesoporous carbon and single Fe atoms. The material exhibits excellent electrocatalytic activity for ORR in acidic and alkaline media, comparable to Pt/C. It also demonstrates high durability and tolerance to methanol crossover reaction, making it suitable for proton exchange membrane fuel cells and zinc-air batteries.

SMALL (2023)

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Article Multidisciplinary Sciences

Interfacial assembly of binary atomic metal-Nx sites for high-performance energy devices

Zhe Jiang et al.

Summary: An interfacial assembly strategy has been developed to construct single-atom binary Fe/Co-Nx sites with a high accessible site density, which leads to increased power densities in fuel cells and Zn/air batteries.

NATURE COMMUNICATIONS (2023)

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Article Chemistry, Physical

Promoting ZIF-8-Derived Fe-N-C Oxygen Reduction Catalysts via Zr Doping in Proton Exchange Membrane Fuel Cells: Durability and Activity Enhancements

Bin Chi et al.

Summary: This study reports the co-doping of Zr and Fe dual metal sites into a ZIF-8-derived mesoporous carbon for improved durability and activity in the oxygen reduction reaction. The Zr-doped Fe-N-C catalyst showed only 25% voltage loss after 20 hours of continuous operation and retained 40% of its initial performance after 100 hours, outperforming the catalyst without Zr doping. The cathode also exhibited significantly enhanced ORR activity, achieving a maximum power density of 0.72 W cm-2.

ACS CATALYSIS (2023)

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Review Chemistry, Applied

Metal-organic frameworks based single-atom catalysts for advanced fuel cells and rechargeable batteries

Yifei Wu et al.

Summary: Next-generation energy storage systems such as fuel cells, metal-air batteries, and alkali metal (Li, Na)-chalcogen (S, Se) batteries have gained attention for their high energy density and low cost. Incorporating efficient catalysts into these systems is crucial due to poor reaction kinetics. Single-atom catalysts (SACs) using metal-organic frameworks (MOFs) as templates have emerged as promising solutions, offering high metal loadings, adjustable structures, porosity, and tailored catalytic sites. This review summarizes strategies for fabricating MOFs-based SACs, their role in these batteries, and discusses their applications and prospects in energy storage systems.

JOURNAL OF ENERGY CHEMISTRY (2023)

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Article Chemistry, Physical

Surface Curvature Effect on Dual-Atom Site Oxygen Electrocatalysis

Ritums Cepitis et al.

Summary: Improved oxygen electrocatalysis is crucial for meeting the increasing energy demand. Metal-nitrogen-carbon (M-N-C) materials show promise as catalysts due to their tunable activity through variations in electronic and geometric properties, including surface curvature. However, the influence of surface curvature on M-N-Cs has not been extensively explored. In this study, a realistic in-pore dual-atom site M-N-C model was developed, and density functional theory was used to investigate the effect of surface curvature on oxygen reduction and evolution reactions. The findings suggest that adjusting the surface curvature can enhance the catalytic activity for mono- and bifunctional oxygen electrocatalysis.

ACS ENERGY LETTERS (2023)

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Article Multidisciplinary Sciences

Fe/Co dual metal catalysts modulated by S-ligands for efficient acidic oxygen reduction in PEMFC

Feng Liu et al.

Summary: Here, a conceptual strategy for introducing spatial sulfur (S)-bridge ligands to regulate the coordination environment of Fe-Co-N dual-metal centers (Spa-S-Fe,Co/NC) is reported. The Spa-S-Fe,Co/NC catalyst showed significantly enhanced oxygen reduction reaction (ORR) performance and satisfactory long-term durability in acidic electrolyte. Experimental and theoretical studies revealed that the excellent acidic ORR activity with remarkable stability observed for Spa-S-Fe,Co/NC is attributable to the charge-modulation of Fe-Co-N bimetallic centers by the spatial S-bridge ligands, achieving optimal adsorption-desorption of ORR oxygenated intermediates. These findings provide a unique perspective to optimize the electrocatalytic performance of catalysts with dual-metal centers by regulating their local coordination environment.

SCIENCE ADVANCES (2023)

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Article Chemistry, Multidisciplinary

Ultrastable Fe-N-C Fuel Cell Electrocatalysts by Eliminating Non-Coordinating Nitrogen and Regulating Coordination Structures at High Temperatures

Dongsheng Xia et al.

Summary: By conducting high-temperature synthetic chemistry between 1100 and 1200 degrees C, the catalytic and storage stability of Fe-N-C materials have been greatly improved. The optimized catalyst shows excellent stability in proton exchange membrane fuel cells, with over 80% performance retention after 30 hours under H-2/O-2 condition and no activity loss after 35 days of storage, while maintaining competitive oxygen reduction reaction activity and fuel cell performance.

ADVANCED MATERIALS (2023)

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Article Chemistry, Physical

Transition-Metal and Nitrogen-Doped Carbon Nanotube/Graphene Composites as Cathode Catalysts for Anion-Exchange Membrane Fuel Cells

Jaana Lilloja et al.

Summary: Transition-metal and nitrogen-doped graphene-like material and carbon nanotube composites are synthesized and utilized as cathode catalysts in anion exchange membrane fuel cells. The materials exhibit similar physicochemical properties and electrocatalytic performances with different yields of HO2- formation. The M-N-Gra/CNT catalysts, especially CoFe-N-Gra/CNT, combined with Aemion+ reinforced anion-exchange membrane, show excellent AEMFC performance comparable to that of Pt/C with a peak power density of 638 mW cm(-2), attributed to the presence of M-Nx sites, carbon-encapsulated transition-metal nanoparticles, and nitrogen-containing moieties.

ACS APPLIED ENERGY MATERIALS (2023)

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Article Engineering, Environmental

Transition metal (Fe, Co, Mn, Cu) containing nitrogen-doped porous carbon as efficient oxygen reduction electrocatalysts for anion exchange membrane fuel cells

Srinu Akula et al.

Summary: Delving into highly active and cost-efficient electrocatalysts for oxygen reduction reaction (ORR) is crucial for large-scale application of polymer electrolyte fuel cells. Anion exchange membrane fuel cells (AEMFCs) are promising clean energy devices with mild reaction conditions and the possibility of employing Pt-free catalysts for ORR. This study focuses on the development of non-Pt catalysts for AEMFC by preparing metal-nitrogen-carbon (M-N-C) electrocatalysts through a robust synthesis method using transition metal impregnated melamine-phloroglucinol-formaldehyde (MPF) polymeric networks. The catalysts with optimized metal content and pyrolysis temperature showed enhanced ORR performance due to their prominent textural properties and efficient active centers. Iron-doped (MPF/Fe) and cobalt-doped (MPF/Co) catalysts performed the best with half-wave potential (E1/2) values of 0.81 and 0.80 V vs RHE, attributed to the highly active M-Nx sites and hierarchical porous structure. The outstanding electrochemical stability and high-power density in AEMFC (up to 347 mW cm-2) demonstrate the potential of these M-N-C catalysts for fuel cell applications.

CHEMICAL ENGINEERING JOURNAL (2023)

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Review Chemistry, Multidisciplinary

The Active Sites and Corresponding Stability Challenges of the M-N-C Catalysts for Proton Exchange Membrane Fuel Cell

Ruolin Peng et al.

Summary: Proton exchange membrane fuel cells (PEMFCs) have gained significant attention as alternatives to internal combustion engines, but their commercialization is hindered by the high cost of platinum group metal (PGM) catalysts. Therefore, the development of PGM-free catalysts based on earth-abundant elements is considered a favorable solution. This review summarizes recent research on the active sites, stability improvement, and degradation mechanisms of PGM-free catalysts.

CHINESE JOURNAL OF CHEMISTRY (2023)

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Article Electrochemistry

Cobalt-, iron- and nitrogen-containing ordered mesoporous carbon-based catalysts for anion-exchange membrane fuel cell cathode

Jaana Lilloja et al.

Summary: Cobalt-, iron- and nitrogen-doped ordered mesoporous carbon (OMC)-based electrocatalysts are prepared and characterized as cathode catalysts for anion-exchange membrane fuel cell (AEMFC). The doped catalysts show high electrocatalytic activity and stability, with CoFe-N-OMC/CNT achieving the highest peak power density of 336 mW cm-2 in AEMFC testing.

ELECTROCHIMICA ACTA (2023)

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Article Chemistry, Physical

A plasma-assisted approach to enhance density of accessible FeN4 sites for proton exchange membrane fuel cells

Yanrong Li et al.

Summary: A plasma-assisted method was used to enhance the porosity of nitrogen-doped carbon, leading to an increase in the density and utilization of FeN4 sites in Fe-N-C catalysts. This approach achieved outstanding catalytic performance in oxygen reduction reaction.

JOURNAL OF COLLOID AND INTERFACE SCIENCE (2023)

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Article Chemistry, Physical

Noble-Metal-Free FeMn-N-C catalyst for efficient oxygen reduction reaction in both alkaline and acidic media

Shuaili Zhao et al.

Summary: A bimetallic FeMn(mIm)-N-C composite with encapsulation-ligand exchange technique is prepared as an efficient ORR catalyst, showing outstanding performance and durability. It exhibits E1/2 values of 0.861 V and 0.778 V in alkaline and acid solutions, and demonstrates exceptional power densities and long-term stability in assembled Zn-Air batteries and proton exchange membrane fuel cells compared to 20% Pt/C.

JOURNAL OF COLLOID AND INTERFACE SCIENCE (2023)

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Review Chemistry, Physical

Progress and perspective of single-atom catalysts for membrane electrode assembly of fuel cells

Zhongxin Song et al.

Summary: A fuel cell is an energy conversion device that continuously releases electrical energy through electrochemical reactions. Single-atom catalysts (SACs) with 100% atom utilization efficiency have shown remarkable performance in fuel cells, saving costs. This review introduces the synthesis and application of SACs, providing experiences for the development of potential industrialized fuel cell catalysts in the future.

CARBON ENERGY (2023)

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Article Chemistry, Physical

Transformation of the Active Moiety in Phosphorus-Doped Fe-N-C for Highly Efficient Oxygen Reduction Reaction

Jeonghan Roh et al.

Summary: Iron- and nitrogen-doped carbon (Fe-N-C) materials have been modified through phosphine-gas treatment to form FeN3PO active moiety, which enhances the catalytic performance of Fe-N-C in the oxygen reduction reaction (ORR) in both alkaline and acidic electrolytes. The proposed ORR mechanism based on FeN3PO moiety facilitates *OH desorption and is validated in anion exchange membrane fuel cells (AEMFCs) and proton exchange membrane fuel cells (PEMFCs).

ACS CATALYSIS (2023)

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Review Chemistry, Multidisciplinary

Review on the Degradation Mechanisms of Metal-N-C Catalysts for the Oxygen Reduction Reaction in Acid Electrolyte: Current Understanding and Mitigation Approaches

Kavita Kumar et al.

Summary: One bottleneck in the widespread use of fuel cell vehicles, especially PEMFCs, is the high cost of the cathode due to the need for precious metals as catalysts. Short-term solutions involve improving platinum utilization, while long-term solutions involve developing catalysts based on Earth-abundant elements. The degradation mechanisms of Metal-N-C electrocatalysts in the acidic environment of PEMFCs are an important research topic, with recent advances in understanding its mechanisms and mitigation approaches.

CHEMICAL REVIEWS (2023)

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Article Chemistry, Physical

Design of Co-NC as efficient electrocatalyst: The unique structure and active site for remarkable durability of proton exchange membrane fuel cells

Kyungmin Im et al.

Summary: In this study, a unique Co-N-C catalyst with a developed pore structure was successfully synthesized using a melamine-encapsulated Co-ZnO-C composite. The catalyst showed superior stability and 4-electron oxygen reduction reaction (ORR) activity, due to the closed interaction between the Co-N4 moiety and organic adducts. Experimental results demonstrated that the Co-N-C catalyst exhibited remarkable durability with only 6.7% performance degradation after 100 hours, and high stability in real device operation.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Chemistry, Physical

Mesoporous textured Fe-N-C electrocatalysts as highly efficient cathodes for proton exchange membrane fuel cells

Srinu Akula et al.

Summary: The new PGM-free PEMFC cathode catalyst materials synthesized using the VariPore (TM) method by Pajarito Powder, LLC show high activity and stability, with mesoporous structure facilitating an effective reaction path.

JOURNAL OF POWER SOURCES (2022)

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Article Chemistry, Physical

Pyrrolic N wrapping strategy to maximize the number of single-atomic Fe-Nx sites for oxygen reduction reaction

Gil-Seong Kang et al.

Summary: This study developed a strategy to increase the number of Fe-N-x active sites in Fe-N-C catalysts by enhancing the electrostatic interactions. By dispersing pyrrolic N-rich carbon (pNC) on the surface of a metal-organic framework (MOF), the number of active sites on the derived hollow carbon framework dramatically increased. The synthesized catalysts were applied in an anion exchange membrane fuel cell (AEMFC) and exhibited satisfactory performance in terms of current density and power density.

JOURNAL OF POWER SOURCES (2022)

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Article Chemistry, Physical

Catalysis stability enhancement of Fe/Co dual-atom site via phosphorus coordination for proton exchange membrane fuel cell

Yinuo Wang et al.

Summary: By regulating the coordination anions, the stability of NPMCs can be improved, providing a new approach to enhance the stability of dual-atom catalysts.

NANO RESEARCH (2022)

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Article Chemistry, Physical

Atomically Dispersed Fe-Co Dual Metal Sites as Bifunctional Oxygen Electrocatalysts for Rechargeable and Flexible Zn-Air Batteries

Yuting He et al.

Summary: This study presents atomically dispersed Fe-Co dual metal sites derived from Fe and Co codoped zeolitic imidazolate frameworks, showing excellent bifunctional catalytic activity for ORR and OER in alkaline media. The FeCo-NC catalyst exhibits outstanding stability and is integrated into an air electrode for fabricating rechargeable and flexible Zn-air batteries, achieving a high power density and long-cycle stability. This work offers a method to design and synthesize atomically dispersed multi-metal site catalysts for advanced electrocatalysis.

ACS CATALYSIS (2022)

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Article Chemistry, Physical

Time-Resolved Potential-Induced Changes in Fe/N/C-Catalysts Studied by In Situ Modulation Excitation X-Ray Absorption Spectroscopy

Kathrin Ebner et al.

Summary: The development of inexpensive Fe/N/C-materials shows promise for catalyzing the oxygen reduction reaction and reducing CO2, but their application in commercial devices requires improvements in performance and stability; a lack of understanding of the nature of their active sites and catalytic mechanisms currently hinders progress.

ADVANCED ENERGY MATERIALS (2022)

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Article Chemistry, Physical

Fe Single-Atom Catalysts on MOF-5 Derived Carbon for Efficient Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells

Xiaoying Xie et al.

Summary: The development of Fe single-atom catalysts using MOF-5 as a precursor has led to the creation of highly-porous carbon with an ultrahigh specific surface area, resulting in improved performance in proton exchange membrane fuel cells for the oxygen reduction reaction. The Fe SAC-MOF-5 catalyst demonstrated excellent half-wave potential and peak power density due to the high density of single Fe atoms and increased exposure of active sites on the external surface area of the carbon support.

ADVANCED ENERGY MATERIALS (2022)

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Review Chemistry, Physical

Dual-Metal Atom Electrocatalysts: Theory, Synthesis, Characterization, and Applications

Angus Pedersen et al.

Summary: This review examines the research progress of dual-metal atom catalysts in electrochemistry, including their advantages, current challenges, and future research directions.

ADVANCED ENERGY MATERIALS (2022)

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Article Chemistry, Physical

Boosting activity toward oxygen reduction reaction of a mesoporous FeCuNC catalyst via heteroatom doping-induced electronic state modulation

Jong Gyeong Kim et al.

Summary: FeCuxNC catalysts with ordered mesoporous grain-shaped particles were prepared and characterized, showing controlled electronic state of active sites and enhanced oxygen reduction reaction performance compared to Pt/C in alkaline conditions.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

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Article Chemistry, Physical

Transition metal and nitrogen-doped mesoporous carbons as cathode catalysts for anion-exchange membrane fuel cells

Jaana Lilloja et al.

Summary: Transition metal-and nitrogen-doped mesoporous carbons were prepared, characterised, and utilized as ORR electrocatalysts in an AEMFC. Fe-N-MPC, CoFe-N-MPC and FeMn-N-MPC showed the best performance and excellent stability in alkaline solution, with Fe-N-MPC and FeMn-N-MPC exhibiting the lowest HO2- yield. FeMn-N-MPC and Fe-N-MPC reached power densities of 474 and 473 mW cm-2 in the AEMFC.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Chemistry, Physical

Site-density engineering of single-atomic iron catalysts for high-performance proton exchange membrane fuel cells

Feng Liu et al.

Summary: A novel polydopamine-metal complex-assisted pyrolysis strategy was used to produce catalysts with hierarchically porous carbon support and highly exposed dense-FeN4 sites, leading to significantly enhanced performance for oxygen reduction reaction (ORR) and superior power densities in proton exchange membrane fuel cells (PEMFCs). The quantitative relationship between the active site activity and ORR performance was established, highlighting the dominating role of FeN4 site density in the observed excellent PEMFC performance. This work provides a useful guidance for the design and development of novel highly-efficient single-atomic catalysts for renewable energy applications.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Review Electrochemistry

Review-Single-Atom Catalysts as Promising Candidates for Single-Atom Catalysts as Promising Candidates for Electrochemical Applications

Somayeh Tajik et al.

Summary: This review article focuses on the recent applications of single-atom catalysts (SACs) in electrocatalysis, including CO2 reduction, oxygen evolution, hydrogen evolution, oxygen reduction, and electrochemical detection. By precise scientific design and controllable construction of SACs, cost-effective and environmentally friendly catalysts can be obtained.

JOURNAL OF THE ELECTROCHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Geometrically Deformed Iron-Based Single-Atom Catalysts for High-Performance Acidic Proton Exchange Membrane Fuel Cells

Lei Shi et al.

Summary: This article proposes a simple but efficient method to synthesize a geometrically deformed single Fe site catalyst by trace NaCl-coating-assisted pyrolysis of Fe-containing zeolitic imidazolate frameworks. The newly developed catalysts exhibit improved oxygen reduction reaction (ORR) performance due to the significantly exposed active sites and enhanced mass transport. The enhanced intrinsic activity is attributed to the synergy of deformed Fe-N-4 moieties and the surrounding graphitic N dopant. Additionally, the locally increased graphitization can efficiently reduce carbon corrosion, thereby promoting catalyst stability.

ACS CATALYSIS (2022)

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Article Chemistry, Physical

Anion Exchange Membranes for Fuel Cells: State-of-the-Art and Perspectives

Huanhuan Chen et al.

Summary: Fuel cell technology is a clean energy generation method that enables carbon neutrality. This Perspective highlights recent trends in the fabrication of high-performance anion exchange membranes (AEMs) and identifies future directions. The success in polymer design is expected to lead to the development of long-lasting fuel cells, reducing carbon emissions and facilitating sustainable development.

ADVANCED ENERGY MATERIALS (2022)

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Article Chemistry, Physical

Hierarchical porous single-wall carbon nanohorns with atomic-level designed single-atom Co sites toward oxygen reduction reaction

Jae Young Jung et al.

Summary: Hierarchical pore structure is crucial for effective mass transfer and utilization of active sites in single-metal atom catalysts. A strategy involving thermal and ammonia annealing was developed to generate hierarchical porous structure and enhance the catalytic activity of Co-N-x sites on carbon nanohorns. Experimental results showed that this strategy achieved remarkably high power density in commercialized membrane electrode assemblies.

NANO ENERGY (2022)

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Article Chemistry, Physical

Rationalization on high-loading iron and cobalt dual metal single atoms and mechanistic insight into the oxygen reduction reaction

Min Jiang et al.

Summary: This study presents an effective plasma engineering strategy for constructing Fe/Co dual single atoms with high loading on nitrogen-doped carbon nanofibers, which exhibit superior performance in oxygen reduction reactions. The N-3-Fe-Co-N-3 moieties are identified as the main active sites, with in situ XAS and Raman spectroscopy revealing structural changes during the reaction. The high loading of single atoms and enhanced activity make the catalyst promising for practical applications in Al-air batteries and PEMFCs.

NANO ENERGY (2022)

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Review Chemistry, Physical

Exploring Durable Single-Atom Catalysts for Proton Exchange Membrane Fuel Cells

Xin Wan et al.

Summary: This review explores the structure-stability relationship of Fe-N-C catalysts, providing valuable guidance for improved stability. Recent achievements include the discovery of several site-specific degradation mechanisms and identification of intrinsically stable active sites, and the discussion of Fe-free single-atom catalysts as an alternative solution.

ACS ENERGY LETTERS (2022)

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Article Chemistry, Physical

High loading of single atomic iron sites in Fe-NC oxygen reduction catalysts for proton exchange membrane fuel cells

Asad Mehmood et al.

Summary: This study demonstrates the achievement of high active site density in non-precious iron-based catalysts by exchanging iron into a preformed carbon-nitrogen matrix, coordinated solely as single-atom Fe-N-4 sites. The catalyst shows excellent performance in proton exchange membrane fuel cells, delivering high current densities and turnover frequency.

NATURE CATALYSIS (2022)

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Review Chemistry, Physical

A review on anion exchange membranes for fuel cells: Anion-exchange polyelectrolytes and synthesis strategies

Jiaqiang Huang et al.

Summary: This paper reviews the performance, synthesis and modification methods, and alkaline stability protection of anion-exchange polyelectrolytes (AEPs) in alkaline fuel cells, and summarizes the current research and development status. The evaluation and comparison of different types of AEPs and AEMs deepen the understanding of AEPs in AEMFC.

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY (2022)

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Review Chemistry, Physical

Dual-atom catalysts for oxygen electrocatalysis

Juan Wang et al.

Summary: This review systematically summarizes the current advances of dual-atom catalysts for ORR and OER electrocatalysis. The intrinsic advantages of dual-atom catalysts and the mechanisms focusing on the electronic structure of active sites are discussed. The structure-activity relationship is comprehensively discussed based on theoretical simulations and experimental results, providing a methodology for rational structural design. The current synthesis methods and performance comparison are presented, and future perspectives for the development of advanced dual-atom catalysts for ORR and OER electrocatalysis are highlighted.

NANO ENERGY (2022)

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Article Energy & Fuels

Atomically dispersed iron sites with a nitrogen-carbon coating as highly active and durable oxygen reduction catalysts for fuel cells

Shengwen Liu et al.

Summary: In this study, a highly durable and active Fe-N-C catalyst was synthesized by depositing a thin layer of nitrogen-doped carbon on the catalyst surface. The stability improvement of the catalyst can overcome the cost barriers of hydrogen fuel cells.

NATURE ENERGY (2022)

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Article Chemistry, Multidisciplinary

Reconstruction of Highly Dense Cu-N4 Active Sites in Electrocatalytic Oxygen Reduction Characterized by Operando Synchrotron Radiation

Gengyu Xing et al.

Summary: This study presents a dual nitrogen source coordinated strategy to achieve high density Cu-N-4 SAS, which exhibits superior ORR activity and stability in alkaline media. The Cu-N-4 SAS supported on 3D N-doped carbon nanotubes/graphene structure shows promising performance in H-2/O-2 AEMFC.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Physical

The strain induced synergistic catalysis of FeN4 and MnN3 dual-site catalysts for oxygen reduction in proton-/anion- exchange membrane fuel cells

Shiqing Huang et al.

Summary: A new Fe-Mn-N-C dual-atom catalyst has been synthesized in this study, which improves the activity of oxygen reduction reaction by tailoring its electronic structure, and exhibits excellent performance in proton/anion-exchange membrane fuel cells.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Engineering, Environmental

Atomically dispersed Fe-Cu dual-site catalysts synergistically boosting oxygen reduction for hydrogen fuel cells

Zeyu Xiao et al.

Summary: Compared to most single-atom catalysts, dual-atom catalysts demonstrate better catalytic performance. In this study, atomically dispersed FeCu-NC catalyst was synthesized and showed superior half-wave potential and peak power density in alkaline medium, highlighting the synergistic mechanism of dual-atom sites in improving catalytic activity.

CHEMICAL ENGINEERING JOURNAL (2022)

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Article Chemistry, Multidisciplinary

Identification of the Catalytically Dominant Iron Environment in Iron- and Nitrogen-Doped Carbon Catalysts for the Oxygen Reduction Reaction

Lingmei Ni et al.

Summary: By using Mossbauer spectroscopy and quantum chemistry, researchers have established an active site model for metal-and nitrogen-doped carbon catalysts obtained through pyrolysis. They found that pyrrolic nitrogen coordination is the active site, and identified a previously unknown intermediate.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

A highly efficient axial coordinated CoN5 electrocatalyst via pyrolysis-free strategy for alkaline polymer electrolyte fuel cells

Bolong Yang et al.

Summary: In this study, a new synthetic method for preparing an oxygen reduction reaction (ORR) catalyst with Co-N5 active sites was successfully developed. Compared with the traditional Co-N-4 active sites, the obtained catalyst showed higher half-wave potential and maximum power density in alkaline polymer electrolyte fuel cells (APEFCs). The rate of ORR was significantly increased by modulating the electronic and geometric structure. Additionally, in-situ Raman spectroscopy demonstrated that Co-N-5 is the active site and axial Co-N coordination can enhance O-2 adsorption and activation, thereby boosting ORR performance. This research provides atomic-level insight into the relationship between the electronic structure of the active center and the ORR performance, as well as guidance for the rational design of high-efficiency electrocatalysts.

NANO ENERGY (2022)

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Article Chemistry, Physical

AgNPs@Fe-N-C oxygen reduction catalysts for anion exchange membrane fuel cells

Yongping Yang et al.

Summary: This study constructs a composite catalyst of AgNPs@Fe-N-C, which demonstrates outstanding ORR performance and durability in alkaline condition. AEMFC based on this composite catalyst shows high peak power density and long-term device durability, surpassing Fe-N-C-based AEMFC.

NANO ENERGY (2022)

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Article Electrochemistry

Iron and Nickel Phthalocyanine-Modified Nanocarbon Materials as Cathode Catalysts for Anion-Exchange Membrane Fuel Cells and Zinc-Air Batteries

Yogesh Kumar et al.

Summary: In this study, six bimetallic N-doped carbon-based catalysts were prepared by using different carbon supports. The electrocatalytic activity of these catalysts was investigated in various configurations, including AEMFC and RZAB. FeNiN-MC and FeNiN-MWCNT catalysts exhibited excellent electrocatalytic activity, performing well in the ORR and OER.

CHEMELECTROCHEM (2022)

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Review Chemistry, Multidisciplinary

Atomically dispersed dual-metal-site PGM-free electrocatalysts for oxygen reduction reaction: Opportunities and challenges

Xiaoxuan Yang et al.

Summary: This review provides a comprehensive analysis of the advances in developing atomically dispersed dual-metal site catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. It explores the structure-property correlation and inherent effects of dual metal sites, and discusses the challenges in rational design, precise synthesis, and high-fidelity structural characterization of dual-metal site catalysts.

SUSMAT (2022)

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Review Chemistry, Multidisciplinary

Non-precious transition metal single-atom catalysts for the oxygen reduction reaction: progress and prospects

Penggang Jiao et al.

Summary: This review summarizes the recent research progress of non-precious transition metal single-atom catalysts (NPT-SACs) for the oxygen reduction reaction (ORR) in Zn-air batteries and fuel cells, discusses the preparation methods and factors affecting performance, and presents the existing challenges and future directions.

NANOSCALE (2022)

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Article Chemistry, Multidisciplinary

Seizing gaseous Fe2+ to densify O2-accessible Fe-N4 sites for high-performance proton exchange membrane fuel cells

Shu-Hu Yin et al.

Summary: Increasing the density of Fe-N-4 sites in Fe-N-C materials can enhance the kinetics of the oxygen reduction reaction in proton exchange membrane fuel cells. A surface-rich pyridinic-N carbon substrate has been shown to be more favorable for forming surface Fe-N2+2 sites with superior intrinsic activity. These structural advantages contribute to the high performance of Fe-g-NC/Phen in fuel cells.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises

Yanghua He et al.

Summary: In this Account, recent advances in synthesizing efficient PGM-free catalysts for proton-exchange membrane fuel cells (PEMFCs) were highlighted, with an emphasis on effective strategies to improve activity and stability. The formation mechanism of MN4 active sites and their correlation to catalytic properties were discussed, providing guidance for rational catalyst design. The trade-off between activity and stability was identified as a key challenge in developing efficient catalysts for PEMFCs.

ACCOUNTS OF MATERIALS RESEARCH (2022)

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Review Chemistry, Multidisciplinary

Understanding the Catalytic Sites of Metal-Nitrogen-Carbon Oxygen Reduction Electrocatalysts

Ming-Xi Chen et al.

Summary: Research has shown that M-N-C catalysts for PEMFCs are the most promising candidates to replace Pt-based catalysts, but the high-temperature pyrolysis process often leads to high structural heterogeneity, which hinders the identification of the catalytic active structure and further impacts the catalyst performance.

CHEMISTRY-A EUROPEAN JOURNAL (2021)

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Review Chemistry, Multidisciplinary

In Situ/Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy

Janis Timoshenko et al.

Summary: X-ray absorption spectroscopy (XAS) is a crucial method for investigating the structure and composition of heterogeneous catalysts, revealing the nature of active sites and establishing links between structural motifs, local electronic structure, and catalytic properties. Recent advancements in instrumentation and data analysis approaches for deciphering X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra have been discussed, with emphasis on applications in the field of heterogeneous catalysis, particularly in electrocatalysis.

CHEMICAL REVIEWS (2021)

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Review Chemistry, Physical

Methods for assessment and measurement of the active site density in platinum group metal-free oxygen reduction reaction catalysts

Alisa Kozhushner et al.

Summary: Recent research has found that platinum group metal-free oxygen reduction reaction catalysts show potential as alternatives to Pt-based catalysts in polymer electrolyte fuel cells, but their durability and stability issues remain. Only electrochemical techniques, such as square wave voltammetry and Fourier transform alternating current voltammetry, are suitable for accurate measurement of active site density in these catalysts.

CURRENT OPINION IN ELECTROCHEMISTRY (2021)

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Review Chemistry, Multidisciplinary

Single Atom Catalysts for Fuel Cells and Rechargeable Batteries: Principles, Advances, and Opportunities

Yuchao Wang et al.

Summary: This paper discusses the importance of developing efficient and robust electrochemical energy storage systems, as well as the role of single atom catalysts in improving device performance. Additionally, it summarizes the working principles and challenges of next-generation electrochemical energy storage and conversion devices.

ACS NANO (2021)

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Article Chemistry, Multidisciplinary

Dynamically Unveiling Metal-Nitrogen Coordination during Thermal Activation to Design High-Efficient Atomically Dispersed CoN4 Active Sites

Yanghua He et al.

Summary: The structural evolution of CoN4 sites during thermal activation was studied using a ZIF-8-derived carbon host. It was found that the critical transition occurs at 700 degrees C with optimal conversion at 900 degrees C, resulting in the highest intrinsic activity and four-electron selectivity for the ORR.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Waste pig blood-derived 2D Fe single-atom porous carbon as an efficient electrocatalyst for zinc-air batteries and AEMFCs

Hee Soo Kim et al.

Summary: Biomass, specifically waste pig blood, was successfully used as a precursor for manufacturing highly efficient Fe-N-C oxygen reduction reaction catalyst. The study demonstrated the potential for low-cost, high-performance electrocatalysts derived from abundant and renewable biomass sources.

APPLIED SURFACE SCIENCE (2021)

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Article Chemistry, Physical

Atomic Fe Dispersed Hierarchical Mesoporous Fe-N-C Nanostructures for an Efficient Oxygen Reduction Reaction

Yu Zhou et al.

Summary: Due to the scarcity and high cost of precious metals, the hydrogen economy may rely on non-platinum-group-metal catalysts. A study found that a stabilized single-atom Fe and N co-doped ordered mesoporous carbon nanosphere catalyst exhibits excellent activity and durability, surpassing the current state-of-the-art Pt/C electrocatalysts.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Fe-N-C Electrocatalysts' Durability: Effects of Single Atoms' Mobility and Clustering

Kavita Kumar et al.

Summary: Second pyrolysis of Fe-N-C catalysts leads to larger mesopore size, higher iron content, and N-pyridinic moieties, resulting in improved ORR activity and selectivity. Aging morphology of catalysts varies significantly depending on whether they underwent a second pyrolysis, with Fe-clusters formation and partial corrosion observed in Fe-HT2 after load cycling aging at 80 degrees C. No clustering was observed at 60 degrees C, suggesting potential guidelines for enhancing stability of Fe-N-C materials.

ACS CATALYSIS (2021)

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Review Chemistry, Physical

Coordination Engineering of Single-Atom Catalysts for the Oxygen Reduction Reaction: A Review

Jincheng Zhang et al.

Summary: The article discusses the importance of single-atom catalysts in promoting future renewable energy supplies and sustainable environments, with a particular emphasis on the excellent catalytic performance of transition-metal SACs in the field of oxygen reduction reactions. Regulating the coordination environments of SACs poses a challenging problem.

ADVANCED ENERGY MATERIALS (2021)

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Review Chemistry, Physical

Mapping transition metal-nitrogen-carbon catalyst performance on the critical descriptor diagram

Stefania Specchia et al.

Summary: The study highlights the increasing interest in platinum group metal-free electrocatalysts, particularly transition metal-nitrogen-carbon catalysts, as cheap alternatives to Pt-based catalysts for oxygen reduction. Unified activity-stability correlations are crucial for practical guidelines in rational catalyst design. Characterization techniques for studying activity descriptors, such as active site density and turnover frequency, are discussed in relation to the morphology of these electrocatalysts.

CURRENT OPINION IN ELECTROCHEMISTRY (2021)

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Review Chemistry, Physical

Mapping transition metal-MN4 macrocyclic complex catalysts performance for the critical reactivity descriptors

Jose H. Zagal et al.

Summary: This paper provides an overview of the progress in developing platinum group metal-free (PGM-free) electrocatalysts for the oxygen reduction reaction in polymer electrolyte fuel cells, focusing on the most advanced class of transition metal-nitrogen-carbon ORR catalysts with high activity and long-term durability.

CURRENT OPINION IN ELECTROCHEMISTRY (2021)

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Review Chemistry, Multidisciplinary

Directly Probing the Local Coordination, Charge State, and Stability of Single Atom Catalysts by Advanced Electron Microscopy: A Review

Peter Tieu et al.

Summary: The development of single atom catalysts (SACs) with carefully controlled properties has been driven by the need for atom efficient catalysts. Advances in transmission electron microscopy (TEM) techniques, including aberration correction, spectroscopy, and in situ/operando observation, have enabled researchers to study SACs at an atomic scale, providing crucial information about their location, characteristics, and stability.

SMALL (2021)

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Article Chemistry, Physical

Transition-Metal- and Nitrogen-Doped Carbide-Derived Carbon/Carbon Nanotube Composites as Cathode Catalysts for Anion-Exchange Membrane Fuel Cells

Jaana Lilloja et al.

Summary: The transition-metal- and nitrogen-codoped carbide-derived carbon/carbon nanotube composites have been prepared and characterized as cathode catalysts in anion-exchange membrane fuel cells. These catalysts exhibit excellent electrocatalytic performance, stability, and have a good combination of micro- and mesoporous structures. The CoFe-N-CDC/CNT material shows a current density close to 500 mA cm(-2) at 0.75 V and a peak power density exceeding 1 W cm(-2) in H-2/O-2 AEMFCs.

ACS CATALYSIS (2021)

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Article Chemistry, Multidisciplinary

Highly Accessible Atomically Dispersed Fe-Nx Sites Electrocatalyst for Proton-Exchange Membrane Fuel Cell

Jianing Guo et al.

Summary: The study introduces a facile method for synthesizing atomically dispersed Fe-N-x species on hierarchically porous carbon nanostructures as an efficient and stable catalyst for oxygen reduction in acidic media for proton exchange membrane fuel cells. The designed hierarchical pore structure facilitates mass transport and utilization of active sites, leading to higher power density in devices.

ADVANCED SCIENCE (2021)

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Article Chemistry, Physical

Maximizing the Active Site Densities of Single-Atomic Fe-N-C Electrocatalysts for High-Performance Anion Membrane Fuel Cells

Subin Park et al.

Summary: The study introduces a simple and effective strategy to maximize active site density using a ZnCl2 activation method, applied to metal organic framework-derived Fe-N-C catalyst, showing superior ORR activity and AEMFC performance. Through electrochemical analysis and AEMFC testing, the practical application potential of this strategy is demonstrated.

ACS APPLIED ENERGY MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells

Lin Guo et al.

Summary: A sulfur-doped Mn-N-C catalyst was synthesized through an effective adsorption-pyrolysis process, exhibiting favorable oxygen reduction reaction (ORR) activity in acidic media. The catalyst showed enhanced performance and stability in comparison to the S-free catalyst, with insights provided into catalyst degradation associated with Mn oxidation and agglomeration. The promoted ORR activity was mainly attributed to the spatial effect from the repulsive interaction between the ORR intermediates and adjacent S dopants.

ACS NANO (2021)

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Article Chemistry, Multidisciplinary

Porphyrin Aerogel Catalysts for Oxygen Reduction Reaction in Anion-Exchange Membrane Fuel Cells

Noam Zion et al.

Summary: The study reports the synthesis, characterization, and utilization of heat-treated iron porphyrin aerogels as cathode catalysts in AEMFCs. The best performing aerogel reached a peak power density of 580 mW cm(-2) and a limiting current density of 2.0 A cm(-2), considered state-of-the-art for PGM-free based AEMFCs.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Understanding of Neighboring Fe-N4-C and Co-N4-C Dual Active Centers for Oxygen Reduction Reaction

Huanxin Li et al.

Summary: The study reports FeCo-N-doped hollow carbon nanocages as efficient catalysts with neighboring Fe-N-4-C and Co-N-4-C dual active centers, showing better catalytic activity than Fe single-metal catalyst for oxygen reduction reaction. This highlights the important role of synergy between dual active centers in reducing the reaction energy barriers for ORR.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Materials Science, Multidisciplinary

Understanding how single-atom site density drives the performance and durability of PGM-free Fe-N-C cathodes in anion exchange membrane fuel cells

Horie Adabi et al.

Summary: The study demonstrates that the handling of Fe-N-C catalyst precursors can significantly impact the formation of single metal atoms or large particles, leading to drastic differences in catalyst structure, activity, and performance in AEMFCs.

MATERIALS TODAY ADVANCES (2021)

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Article Green & Sustainable Science & Technology

Non-precious metal cathodes for anion exchange membrane fuel cells from ball-milled iron and nitrogen doped carbide-derived carbons

Sander Ratso et al.

Summary: This study demonstrates a synthesis method for producing highly active non-precious metal catalysts on carbon materials, achieving improved oxygen reduction reaction activity by optimizing synthesis parameters in fuel cell environments.

RENEWABLE ENERGY (2021)

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Article Chemistry, Physical

Molten NaCl-Assisted Synthesis of Porous Fe-N-C Electrocatalysts with a High Density of Catalytically Accessible FeN4 Active Sites and Outstanding Oxygen Reduction Reaction Performance

Qing Wang et al.

Summary: This study presents a simple NaCl-assisted method to fabricate high-performance nitrogen-doped carbon electrocatalyst Fe/NC-NaCl with abundant FeN4 sites. The catalyst exhibits outstanding ORR performance with high half-wave potential and peak power density, ranking it among the most active M-N-C materials reported to date.

ADVANCED ENERGY MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Atomic-Scale Engineered Fe Single-Atom Electrocatalyst Based on Waste Pig Blood for High-Performance AEMFCs

Jiho Lee et al.

Summary: Waste pig blood is a sustainable precursor for functional electrocatalysts, but impurities hinder its performance. Hierarchical 2D porous Fe single-atom catalysts were successfully synthesized on a graphene oxide support, showing excellent ORR performance.

ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2021)

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Article Nanoscience & Nanotechnology

Bifunctional Oxygen Electrocatalysis on Mixed Metal Phthalocyanine-Modified Carbon Nanotubes Prepared via Pyrolysis

Yogesh Kumar et al.

Summary: This study demonstrates that mixed metal phthalocyanine-modified multiwalled carbon nanotubes can serve as an alternative to Pt in low-temperature fuel cells; FeCoN-MWCNT and FeMnN-MWCNT catalysts exhibit excellent oxygen reduction and oxygen evolution activity; scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy are effective tools for studying the surface morphology and structure of catalysts.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Chemistry, Multidisciplinary

Fe-N-C Electrocatalysts with Densely Accessible Fe-N4 Sites for Efficient Oxygen Reduction Reaction

Yazhou Zhou et al.

Summary: This study demonstrates an in situ trapping strategy using nitrogen-rich molecules to enhance the amount of accessible Fe-N-4 sites in Fe-N-C electrocatalysts, leading to improved ORR activity.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Iron, Nitrogen Co-Doped Carbon Spheres as Low Cost, Scalable Electrocatalysts for the Oxygen Reduction Reaction

Jingyu Feng et al.

Summary: Atomically dispersed transition metal-nitrogen-carbon catalysts are emerging as low-cost electrocatalysts for the oxygen reduction reaction in fuel cells. A synthesis strategy for these catalysts is still required, as well as a greater understanding of their mechanisms. Iron, nitrogen co-doped carbon spheres (Fe@NCS) have been prepared and FeN4 is identified as the main form of iron existing in the obtained Fe@NCS. Starting from Fe2+ and Fe3+ precursors, catalysts show chemical and structural differences. Fe2+@NCS-A displays better catalytic activity for the oxygen reduction reaction and shows potential for developing high-performance, low-cost fuel cell catalysts.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Hydrogen Passivation of M-N-C (M = Fe, Co) Catalysts for Storage Stability and ORR Activity Improvements

Jieyuan Liu et al.

Summary: Long-term exposure of M-N-C catalysts in air causes surface oxidation and hydroxylation, leading to decreased ORR activity and fuel-cell performances. Hydrogen passivation protects active sites and improves storage stability of the catalysts.

ADVANCED MATERIALS (2021)

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Review Chemistry, Physical

Synthesis strategies of templated porous carbons beyond the silica nanocasting technique

Noel Diez et al.

Summary: The review discusses the importance of porous carbons in environmental remediation and emerging energy applications. It highlights sustainable templating strategies using easily removable inorganic particles or polymeric materials. The fundamental aspects, advances, applications, and challenges of producing porous carbons with various morphologies and pore structures are analyzed in detail.

CARBON (2021)

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Article Electrochemistry

Enhancing the electrocatalytic activity of Fe phthalocyanines for the oxygen reduction reaction by the presence of axial ligands: Pyridine-functionalized single-walled carbon nanotubes

Maria Paz Oyarzun et al.

Summary: In this study, the electrocatalytic activity of FePc and 16(Cl)FePc for the oxygen reduction reaction was examined when adsorbed on SWCNT or py-SWCNT. The results showed that ORR activity is higher on py-SWCNT compared to SWCNT, and 16(Cl)FePc exhibited higher activity than FePc due to the electron-withdrawing effect of chlorine atoms.

ELECTROCHIMICA ACTA (2021)

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Article Chemistry, Multidisciplinary

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N-3 as an Active Site for the Oxygen Reduction Reaction

Ji Yang et al.

Summary: Atomically dispersed Cu-N-C single-atom catalysts with Cu2+-N-4 structure exhibit comparable activity and superior durability to Pt/C in the electrochemical reduction of oxygen. The dynamic evolution of Cu-N-4 to Cu-N-3 and further to HO-Cu-N-2 under ORR conditions is identified, with the low-coordinated Cu+-N-3 being determined as the real active site. The findings may guide the design of more efficient low-cost catalysts.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Physical

Chemical vapour deposition of Fe-N-C oxygen reduction catalysts with full utilization of dense Fe-N4 sites

Li Jiao et al.

Summary: Replacing scarce and expensive platinum with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has been impeded by the low active site density and site utilization of M-N-C. These limitations have now been overcome by implementing trans-metalation of Zn-N-4 sites into Fe-N-4 sites.

NATURE MATERIALS (2021)

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Article Energy & Fuels

High-performing commercial Fe-N-C cathode electrocatalyst for anion-exchange membrane fuel cells

Horie Adabi et al.

Summary: This study presents a high-performing commercial oxygen reduction catalyst that can replace platinum group metal catalysts, resulting in improved performance and reduced cost for anion-exchange membrane fuel cells.

NATURE ENERGY (2021)

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Article Chemistry, Physical

Flash Bottom-Up Arc Synthesis of Nanocarbons as a Universal Route for Fabricating Single-Atom Electrocatalysts

Jae Young Jung et al.

Summary: The study presents a universal strategy for fabricating nanocarbon based-SACs using a flash bottom-up arc discharge method, which successfully achieves the synthesis of various metals and nanocarbons. The post-treatment with NH3 allows modulation of the coordination environment around Co atoms in Co-1/CNH, resulting in excellent oxygen reduction reaction activity.

SMALL METHODS (2021)

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Article Chemistry, Multidisciplinary

Nano-geometric deformation and synergistic Co nanoparticles-Co-N4 composite sites for proton exchange membrane fuel cells

Xiaoyang Cheng et al.

Summary: A novel strategy was developed to enhance the ORR activity of Co single-atom catalysts by introducing a deformed CoN4 site and Co nanoparticle-CoN4 composite sites, which effectively replenished the total density of CoN4. The resulting concave nanocube-like catalyst exhibited excellent ORR performance and high power density in acidic media, with theoretical studies confirming the enhanced O-2 activation and reduced carbon layer erosion. This research not only provides a new approach to develop ORR catalysts, but also contributes to a deeper understanding of ORR fundamentals.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Article Chemistry, Multidisciplinary

Single-Atom Catalysts: A Perspective toward Application in Electrochemical Energy Conversion

Florian D. Speck et al.

Summary: Single-atom catalysts show promise for applications in renewable energy conversion, but face challenges in scaling up synthesis, performance evaluation in real devices like fuel cells, and degradation control.

JACS AU (2021)

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Article Chemistry, Multidisciplinary

Quantification of Active Site Density and Turnover Frequency: From Single-Atom Metal to Nanoparticle Electrocatalysts

Geunsu Bae et al.

Summary: This study presents an in situ method for quantifying SD using cyanide as a probe molecule, which allows precise measurement of the decrease in cyanide concentration triggered by adsorption on metal-based active sites. This analytical strategy shows versatile applicability to various SACs and Pt nanoparticles across a broad pH range, providing insights into the structure-activity relationship in electrocatalysts.

JACS AU (2021)

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Article Chemistry, Physical

Single-atom oxygen reduction reaction electrocatalysts of Fe, Si, and N co-doped carbon with 3D interconnected mesoporosity

Hee Soo Kim et al.

Summary: This study reports a novel FeSiNC catalyst with excellent oxygen reduction reaction activity in zinc-air and fuel cells, comparable to the most efficient non-Pt-based catalysts, and exhibits outstanding performance in single-cell devices.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Article Green & Sustainable Science & Technology

Active Site Identification in FeNC Catalysts and Their Assignment to the Oxygen Reduction Reaction Pathway by In Situ Fe-57 Mossbauer Spectroscopy

Lingmei Ni et al.

Summary: This study identified the active site species in different FeNC catalysts prepared through various routes, revealing common spectral changes during the direct electroreduction of oxygen. However, changes in selectivity were attributed to variations within additional species. Density functional theory calculations provided insights into the nature of nitrogen coordination in FeN4 moieties involved in the oxygen reduction reaction.

ADVANCED ENERGY AND SUSTAINABILITY RESEARCH (2021)

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Article Chemistry, Multidisciplinary

Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN4 for Ultraefficient Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells

Mengfei Qiao et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

A General Strategy to Atomically Dispersed Precious Metal Catalysts for Unravelling Their Catalytic Trends for Oxygen Reduction Reaction

Jae Hyung Kim et al.

ACS NANO (2020)

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Article Chemistry, Multidisciplinary

Zinc-Mediated Template Synthesis of Fe-N-C Electrocatalysts with Densely Accessible Fe-Nx Active Sites for Efficient Oxygen Reduction

Guangbo Chen et al.

ADVANCED MATERIALS (2020)

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Article Chemistry, Multidisciplinary

Edge-Rich Fe-N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis

Wang Xin et al.

ADVANCED MATERIALS (2020)

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Article Chemistry, Physical

Catalytic Advantages, Challenges, and Priorities in Alkaline Membrane Fuel Cells

Horie Adabi Firouzjaie et al.

ACS CATALYSIS (2020)

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Article Chemistry, Physical

Stabilizing Single-Atom Iron Electrocatalysts for Oxygen Reduction via Ceria Confining and Trapping

Jin-Cheng Li et al.

ACS CATALYSIS (2020)

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Review Chemistry, Physical

Molecular Design of Single-Atom Catalysts for Oxygen Reduction Reaction

Chengzhang Wan et al.

ADVANCED ENERGY MATERIALS (2020)

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Article Nanoscience & Nanotechnology

Design and Preparation of Fe-N5 Catalytic Sites in Single-Atom Catalysts for Enhancing the Oxygen Reduction Reaction in Fuel Cells

Ye-Min Zhao et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

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Article Materials Science, Coatings & Films

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