4.8 Article

d-Orbital Electron Delocalization Realized by Axial Fe4C Atomic Clusters Delivers High-Performance Fe-N-C Catalysts for Oxygen Reduction Reaction

Related references

Note: Only part of the references are listed.
Article Chemistry, Physical

Regulating the Fe-spin state by Fe/Fe3C neighbored single Fe-N4 sites in defective carbon promotes the oxygen reduction activity

Guijun Li et al.

Summary: By pre-preparing a 3D nitrogen-doping carbon-sheet network from in situ gas-molecule cutting of bulk MOF and then adsorbing iron into defects and pores of this preformed matrix, we achieve a Fe-N-C catalyst with 14.78 wt.% iron existed as single-atom Fe-N-4 sites neighboured Fe/Fe3C nanostructures. This catalyst delivers excellent ORR activity and the primary ZAB performance with excellent durability. These results highlight the importance of metal-atoms spin-state modulation by coupled active metal-species in hybrid catalysts for electrochemical energy devices.

ENERGY STORAGE MATERIALS (2023)

Review Chemistry, Physical

Electrocatalysis Mechanism and Structure-Activity Relationship of Atomically Dispersed Metal-Nitrogen-Carbon Catalysts for Electrocatalytic Reactions

Long-Ji Yuan et al.

Summary: This review provides a systematic introduction to the research methods of M-N-C catalysts, reveals their electrocatalytic mechanism and structure-activity relationship, and points out future research directions.

SMALL METHODS (2023)

Article Chemistry, Multidisciplinary

Tuning the spin state of Fe single atoms by Pd nanoclusters enables robust oxygen reduction with dissociative pathway

Xiaoqian Wei et al.

Summary: Here, we report an unprecedented oxygen reduction reaction catalyst consisting of Pd nanoclusters and Fe single atoms. Experimental investigations and theoretical calculations reveal that the enhanced activity of this catalyst is due to the spin-state transition induced by Pd nanoclusters, leading to the activation of O-O bond and a transition from associative to dissociative process. This Fe-N-C/PdNC catalyst exhibits excellent ORR performance in acid conditions, surpassing the performance of Pt/C catalyst.
Article Chemistry, Multidisciplinary

Architecting FeNx on High Graphitization Carbon for High-Performance Oxygen Reduction by Regulating d-Band Center

Lingfeng Li et al.

Summary: An effective phase-transition strategy is reported to enhance the stability of Fe-N-C catalysts, while preserving their activity, by increasing the graphitization degree and incorporating Fe nanoparticles encapsulated by a graphitic carbon layer. The resulting Fe@Fe-N-C catalysts exhibit excellent oxygen reduction reaction (ORR) activity and stability, making them promising alternatives to platinum group metals.

SMALL (2023)

Article Materials Science, Multidisciplinary

Boost the Utilization of Dense FeN4 Sites for High-Performance Proton Exchange Membrane Fuel Cells

Yanrong Li et al.

Summary: This study reports a melamine-assisted vapor deposition approach to enhance the performance of Fe-N-C catalysts for the oxygen reduction reaction (ORR). Melamine not only compensates for nitrogen loss during pyrolysis, but also etches the carbon substrate, increasing its surface area and porosity for subsequent vapor deposition. The treated 0.20Mela-FeNC catalyst shows significantly improved active site density and utilization, resulting in high ORR activity and power density.

ENERGY & ENVIRONMENTAL MATERIALS (2023)

Article Nanoscience & Nanotechnology

Abrading bulk metal into single atoms

Gao-Feng Han et al.

Summary: A solvent-free and zero-waste method for synthesizing single-atom catalysts from bulk metals has been reported. This method is applicable to different metals and supports, and it offers a green and efficient approach for the commercialization of single-atom catalysts.

NATURE NANOTECHNOLOGY (2022)

Article Chemistry, Multidisciplinary

Single-Atom Fe Catalysts for Fenton-Like Reactions: Roles of Different N Species

Yu Xiong et al.

Summary: Recognizing and controlling the structure-activity relationships of single-atom catalysts is crucial for manipulating their catalytic properties. The study on Fe single-atom catalysts supported on nitrogen-doped carbon reveals high catalytic reactivity, stability, and wide pH suitability in Fenton-like reactions, with the roles of different N species further explored both experimentally and theoretically. Density functional theory calculations highlight how the location of d-band center of Fe sites affects the generation of Fe-oxo intermediates, leading to excellent catalytic properties.

ADVANCED MATERIALS (2022)

Article Multidisciplinary Sciences

Iron atom-cluster interactions increase activity and improve durability in Fe-N-C fuel cells

Xin Wan et al.

Summary: This study demonstrates the high activity and stability of an Fe-N-C catalyst for oxygen reduction reaction in acidic fuel cells by introducing nitrogen-coordinated iron clusters and closely surrounding Fe-N-4 active sites. The strong electronic interaction between the iron clusters and the Fe-N-4 sites optimizes the adsorption strength of reaction intermediates and enhances the catalyst's turnover frequency and demetalation resistance.

NATURE COMMUNICATIONS (2022)

Article Chemistry, Physical

Understanding the structure-performance relationship of active sites at atomic scale

Runze Li et al.

Summary: This article discusses the key factors affecting the catalytic performance of metal-based atomically dispersed catalysts and their relationship with the active sites. It first introduces the effectiveness of active site design through coordination effects, then discusses the role of chemical bonds in the active sites and the influence of the spacing of active atoms in intermetallic compounds on catalytic behavior. Additionally, the importance of synergistic effects in catalyst design is emphasized, and the key parameters affecting catalytic performance at the atomic scale are summarized.

NANO RESEARCH (2022)

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)

Review Chemistry, Physical

Are Fe-N-C Electrocatalysts an Alternative to Pt-Based Electrocatalysts for the Next Generation of Proton Exchange Membrane Fuel Cells?

Xiong Zhang et al.

Summary: This review summarizes the notable progress in the development of low Pt-based and Fe-N-C electrocatalysts for proton exchange membrane fuel cell (PEMFC) applications. The research focuses on the design and optimization of Fe-N-C's as a cost-effective alternative to platinum-based catalysts. By comparing the performance of Fe-N-C's with that of commercial Pt/C catalysts, it is suggested that Fe-N-C's have the potential to be alternative candidates in PEMFCs. The review discusses various aspects including the mechanism, active sites, catalyst layer design, performance, and durability of Fe-N-C's in PEMFCs, aiming to provide insights into their potential as replacements for Pt-based catalysts and pointing out future research directions.

ACS CATALYSIS (2022)

Article Chemistry, Multidisciplinary

Role of Pyridinic Nitrogen in the Mechanism of the Oxygen Reduction Reaction on Carbon Electrocatalysts

Kotaro Takeyasu et al.

Summary: The introduction of pyridinic nitrogen (pyri-N) into carbon-based electrocatalysts for the oxygen reduction reaction is considered to create new active sites. In this study, it was found that catalysts containing pyri-N molecules exhibited highest activity in acidic electrolytes, with 1,10-phenanthroline/CB showing the best performance.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

Article Chemistry, Physical

Identification of durable and non-durable FeNx sites in Fe-N-C materials for proton exchange membrane fuel cells

Jingkun Li et al.

Summary: Fe-N-C materials show promise as an alternative to platinum in acidic polymer fuel cells, but limited understanding of their operando degradation hinders rational approaches to improved durability. Two distinct FeNx sites in the catalysts degrade differently during the oxygen reduction reaction, with one site substantially contributing after 50 hours of operation.

NATURE CATALYSIS (2021)

Article Chemistry, Multidisciplinary

Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres

Cheng Tang et al.

Summary: This study demonstrates that the molecular-level local structure, including first and second coordination spheres, plays a critical role in determining the selectivity of catalytic reactions. By modifying the first and second coordination spheres of Co-SACs, it is possible to tailor the oxygen reduction reaction selectivity. The unique selectivity change originates from the structure-dependent shift of active sites, leading to improved activity and selectivity for acidic H2O2 electrosynthesis.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

Article Energy & Fuels

The design space for long-duration energy storage in decarbonized power systems

Nestor A. Sepulveda et al.

Summary: Wind and solar energy need to be supplemented by energy storage and firm generating capacity. Long-duration energy storage is seen as a potential solution to intermittency in renewable energy generation. The key parameters for the performance of energy storage are energy capacity cost and discharge efficiency. Storage systems with durations exceeding 100 hours have the greatest impact on electricity cost and firm generation.

NATURE ENERGY (2021)

Article Chemistry, Multidisciplinary

Improving the Stability of Non-Noble-Metal M-N-C Catalysts for Proton-Exchange-Membrane Fuel Cells through M-N Bond Length and Coordination Regulation

Zhengpei Miao et al.

Summary: An effective strategy is developed to enhance the stability of non-noble-metal catalysts in fuel cells by improving the bonding strength between metal ions and chelating polymers. The optimized catalyst exhibits outstanding activity and stability in both half-cell and fuel cell cathodes, with near 100% retention of current density for an extended period. The study suggests that the Fe-N-4/C site can strongly stabilize Fe centers against demetalation, providing insights for further catalyst design.

ADVANCED MATERIALS (2021)

Article Multidisciplinary Sciences

Designing the next generation of proton-exchange membrane fuel cells

Kui Jiao et al.

Summary: The rapid growth of proton-exchange membrane fuel cell technology is driving the demand for clean and sustainable global energy applications. Increasing PEMFC power density is critical for commercialization, with ambitious goals set globally. Future high-power-density PEMFCs will focus on improving membrane electrode assembly components, water and thermal management, and materials.

NATURE (2021)

Article Chemistry, Physical

Synergistically enhanced single-atomic site Fe by Fe3C@C for boosted oxygen reduction in neutral electrolyte

Xiaoqian Wei et al.

Summary: This study constructed exceptional single-atomic site Fe catalyst boosted by adjacent graphene-encapsulated Fe3C nanocrystals (Fe3C@C-Fe SAS) for oxygen reduction reaction (ORR), showing robust performance and outstanding peak power density in the neutral electrolyte system. Density functional theory (DFT) calculations revealed that the introduction of Fe3C@C nanocrystals accelerates the activation of O2 molecules and desorption of OH* on Fe single-atomic sites, leading to promising ORR activity.

NANO ENERGY (2021)

Article Multidisciplinary Sciences

Iron phthalocyanine with coordination induced electronic localization to boost oxygen reduction reaction

Kejun Chen et al.

NATURE COMMUNICATIONS (2020)

Article Materials Science, Multidisciplinary

Fe3C nanoparticles for magnetic hyperthermia application

A. Gangwar et al.

JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS (2019)

Article Chemistry, Multidisciplinary

Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN4 Sites for Oxygen Reduction

Jiazhan Li et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019)

Article Chemistry, Multidisciplinary

Engineering Energy Level of Metal Center: Ru Single-Atom Site for Efficient and Durable Oxygen Reduction Catalysis

Meiling Xiao et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2019)

Article Chemistry, Multidisciplinary

High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites

Hanguang Zhang et al.

ENERGY & ENVIRONMENTAL SCIENCE (2019)

Article Chemistry, Multidisciplinary

Adsorbed Intermediates in Oxygen Reduction on Platinum Nanoparticles Observed by In Situ IR Spectroscopy

Simantini Nayak et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2018)

Review Chemistry, Multidisciplinary

Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction

Ambarish Kulkarni et al.

CHEMICAL REVIEWS (2018)

Article Chemistry, Physical

Synthesis of highly-active Fe-N-C catalysts for PEMFC with carbide-derived carbons

Sander Ratso et al.

JOURNAL OF MATERIALS CHEMISTRY A (2018)

Article Chemistry, Multidisciplinary

Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation

Hanguang Zhang et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2017)

Article Chemistry, Multidisciplinary

Discriminating Catalytically Active FeNx Species of Atomically Dispersed Fe-N-C Catalyst for Selective Oxidation of the C-H Bond

Wengang Liu et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2017)

Article Chemistry, Physical

EPR study of a novel [Fe-porphyrin] catalyst

K. C. Christoforidis et al.

MOLECULAR PHYSICS (2007)

Article Materials Science, Multidisciplinary

A fast and robust algorithm for Bader decomposition of charge density

Graeme Henkelman et al.

COMPUTATIONAL MATERIALS SCIENCE (2006)

Article Multidisciplinary Sciences

Sustainable hydrogen production

JA Turner

SCIENCE (2004)