4.5 Article

Intermediates-induced CO2 Reduction Reaction Activity at Single-Atom M-N-2 (M=Fe, Co, Ni) Sites

Related references

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

How pH Affects the Oxygen Reduction Reactivity of Fe-N-C Materials

Tianyang Liu et al.

Summary: By using first-principles microkinetic computations, we discover a pH-dependent regulation mechanism in Fe-N-C materials, which explains the significant activity difference in acidic and alkaline media. We find that FeN4 centers of Fe-N-C catalysts are covered by intrinsic intermediates *OH and *O at different pH values, forming FeN4-OH and FeN4-O centers. The activity difference of Fe-N-C catalysts can be attributed to the optimization of electronic structure and intermediate adsorption induced by *O coordination. Our work provides mechanistic insights into pH effects and contributes to more effective catalyst design.

ACS CATALYSIS (2023)

Article Nanoscience & Nanotechnology

Dual-Atom Metal and Nonmetal Site Catalyst on a Single Nickel Atom Supported on a Hybridized BCN Nanosheet for Electrochemical CO2 Reduction to Methane: Combining High Activity and Selectivity

Yuqin Zhang et al.

Summary: Using density functional theory calculations, this study investigated the electrocatalytic performance of a single transition metal (TM) atom embedded into a defective nanosheet for carbon dioxide reduction reaction (CO2RR). The results showed that the TM atom coordinated with nonmetal atoms could activate CO2 and stabilize key intermediates, resulting in selective CO2 reduction to hydrocarbons.

ACS APPLIED MATERIALS & INTERFACES (2022)

Article Chemistry, Multidisciplinary

Ligand Engineering in Nickel Phthalocyanine to Boost the Electrocatalytic Reduction of CO2

Kejun Chen et al.

Summary: A ligand-tuned strategy has been developed to enhance the catalytic performance of NiPc in the CO2 reduction reaction, highlighting the ligand effect on CO2RR. The tailored NiPc with electron-donating substituents shows ultrahigh activity and selectivity for CO formation, indicating a promising approach for efficient CO2RR.

ADVANCED FUNCTIONAL MATERIALS (2022)

Article Chemistry, Multidisciplinary

Low-Coordinated Co-N-C on Oxygenated Graphene for Efficient Electrocatalytic H2O2 Production

Haisheng Gong et al.

Summary: By simultaneously regulating the coordination number of atomically dispersed cobalt sites and nearby oxygen functional groups through a one-step microwave thermal shock, a highly selective and active Co-N-C electrocatalyst for H2O2 electrosynthesis has been obtained. This catalyst exhibits high H2O2 selectivity, outstanding mass activity, and large kinetic current density, showing great potential for the development of new electrocatalysts with unprecedented reactivity.

ADVANCED FUNCTIONAL MATERIALS (2022)

Article Chemistry, Physical

Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol

Minzhi Ma et al.

Summary: This study successfully fabricated Co/g-C3N4 single-atom catalysts for photocatalytic reduction of CO2 to methanol, showing significantly enhanced activity. The work provides a strategy to boost the photoreduction CO2 activity by loading ultrahigh surface density single atomically dispersed cobalt active sites.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

Article Chemistry, Multidisciplinary

High-curvature carbon-supported Ni single atoms with charge polarization for highly efficient CO2 reduction

Xingshun Wu et al.

Summary: High curvature carbon-supported isolated NiN4 sites with excellent CO2 reduction reaction performance were achieved through a top-down strategy. The charge polarization induced by the axial asymmetry of the carbon substrate enhances COOH* adsorption and reduces the free energy barrier of the rate-determining step.

CHEMICAL COMMUNICATIONS (2022)

Review Chemistry, Physical

Key factors for designing single-atom metal-nitrogen-carbon catalysts for electrochemical CO2 reduction

Chen Jia et al.

Summary: This article summarizes the recent achievements of M-N-C SACs for CO2RR, emphasizing the importance of key factors such as metal sites, coordination environment, and substrates in achieving high CO2RR performance. Perspective views and guidelines are provided for the future development of M-N-C SACs as CO2RR catalysts.

CURRENT OPINION IN ELECTROCHEMISTRY (2022)

Article Chemistry, Multidisciplinary

Limiting the Uncoordinated N Species in M-Nx Single-Atom Catalysts toward Electrocatalytic CO2 Reduction in Broad Voltage Range

Dawei Xi et al.

Summary: Carbon-supported Ni single-atom catalysts with precisely controlled single-atom structure achieved through joule heating strategy show superior performance in electrocatalytic carbon dioxide reduction reaction, with 80% of N dopants coordinated with metal elements, thereby avoiding unfavorable N species and demonstrating unprecedented activity, selectivity, and stability.

ADVANCED MATERIALS (2022)

Article Multidisciplinary Sciences

Insights into the activity of single-atom Fe-N-C catalysts for oxygen reduction reaction

Kang Liu et al.

Summary: This study provides a model to understand the catalytic activity of single-atom M-N-C catalysts in the oxygen reduction reaction. The authors demonstrate the regulation of divacancy defects on Fe-N-4 site ORR activity and identify the origin of Fe-N-4 ORR activity through the hybridization between Fe 3dz(2), 3dyz (3dxz) and O-2 pi* orbitals.

NATURE COMMUNICATIONS (2022)

Article Chemistry, Physical

Coordinatively Deficient Single-atom Fe-N-C Electrocatalyst with Optimized Electronic Structure for High-performance Lithium-sulfur Batteries

Jiayi Wang et al.

Summary: In this study, the deficiency coordination of single-atom Fe site was predicted and validated to enhance sulfur immobilization and catalytic activity, leading to the preparation of a high-performance catalyst for Li-S batteries. The monodispersed FeN2-NC showed excellent electrochemical performance through tuning the coordination number.

ENERGY STORAGE MATERIALS (2022)

Article Chemistry, Physical

Theoretical investigation on electrocatalytic reduction of CO2 to methanol and methane by bimetallic atoms TM1/TM2-N@Gra (TM = Fe, Co, Ni, Cu)

Xiaofei Wei et al.

Summary: This study employs density functional theory (DFT) to design ten different transition metal dual atom catalysts (DACs) and analyze their catalytic properties in electrocatalytic CO2 reduction reaction (CO2RR). Fe/Co-N@Gra and Co2-N@Gra demonstrate superior catalytic performance and product selectivity for methane.

APPLIED SURFACE SCIENCE (2022)

Article Chemistry, Physical

Molecularly Engineered Carbon Platform To Anchor Edge-Hosted Single-Atomic M-N/C (M = Fe, Co, Ni, Cu) Electrocatalysts of Outstanding Durability

Woo Yeong Noh et al.

Summary: The synthetic protocol based on molecularly engineered anchoring carbon platform (ACP) and microwave pyrolysis stabilizes concentrated edge-hosted single-atom catalytic sites, enhancing the activity and stability of the catalysts.

ACS CATALYSIS (2022)

Article Materials Science, Multidisciplinary

Axial coordination modification of M-N4 single-atom catalysts to regulate the electrocatalytic CO2 reduction reaction

Mengbo Ma et al.

Summary: The CO2 reduction reaction (CO2RR) to CO using Earth-abundant single-atom catalysts (SACs) based on Fe, Co, and Ni shows great potential, but the activity and selectivity still need improvement. Recent studies have found that axial coordination can enhance the activity of M-N-C SACs, but only limited ligands have been reported. This study systematically investigates the modification of MN4 (M = Fe, Co, Ni) SACs using a series of organic ligands and reveals that the introduction of axial ligands can significantly affect the adsorption and reaction characteristics. The findings provide new insights for the development of highly effective CO2RR catalysts.

JOURNAL OF MATERIALS CHEMISTRY C (2022)

Article Chemistry, Multidisciplinary

Why heterogeneous single-atom catalysts preferentially produce CO in the electrochemical CO2 reduction reaction

Yu Wang et al.

Summary: Using bismuth nanosheets and Bi-N-C SAC as model catalysts, this study computationally reveals the correlation between the selectivity of M-N-C SACs and the CO2 adsorption mode, providing guidance for the development of high-performance CO2RR catalysts.

CHEMICAL SCIENCE (2022)

Article Chemistry, Physical

Cu acting as Fe activity promoter in dual-atom Cu/Fe-NC catalyst in CO2RR to C1 products

Xiaofei Wei et al.

Summary: By constructing a dual-atom center (Cu/Fe-NC) through incorporating Cu into Fe single-atom catalysts, this study demonstrated efficient CO2RR generation of multi-electron products CH3OH and CH4 with low limiting potentials. The synergistic effect of Fe as the active site and Cu as the activity promoter significantly improved the catalytic performance, providing a new avenue for CO2RR research.

APPLIED SURFACE SCIENCE (2021)

Article Chemistry, Multidisciplinary

Electronic Spin Moment As a Catalytic Descriptor for Fe Single-Atom Catalysts Supported on C2N

Wenhui Zhong et al.

Summary: The study reveals that the catalytic activity of Fe single-atom supported on C2N for oxygen reduction reaction is influenced by the spin states. Manipulation of the spin states can effectively tune the catalytic activity, with the potential to design transition metal single-atom catalysts with improved performance.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

Article Chemistry, Multidisciplinary

Atomically Dispersed s-Block Magnesium Sites for Electroreduction of CO2 to CO

Qiyou Wang et al.

Summary: This study demonstrates the construction of atomically dispersed magnesium atoms embedded in graphitic carbon nitride for CO2 electroreduction to CO. Theoretical calculations and experimental results show that the desorption of CO on Mg sites is easier compared to Fe and Co sites, leading to higher CO Faradaic efficiency and activity. This work sheds new light on the use of s-block metal sites for efficient CO2RR.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

Article Engineering, Environmental

Activation of CO2 on graphitic carbon nitride supported single-atom cobalt sites

Junwei Fu et al.

Summary: This study used density functional theory to calculate the reaction pathways of CO2 to CO on pure g-C3N4 and single-atom cobalt modified g-C3N4, finding that Co-CN possesses enhanced CO2 adsorption and activation abilities.

CHEMICAL ENGINEERING JOURNAL (2021)

Article Chemistry, Multidisciplinary

Origin of the N-coordinated single-atom Ni sites in heterogeneous electrocatalysts for CO2 reduction reaction

Yu Wang et al.

Summary: The study reveals that the active Ni moieties of Ni-N-C SACs are expected to have a formula of NiN4 and display high activity for facilitating the selective CO2RR. Model results show reasonable agreement with experimental data, highlighting the crucial role of tetrapyrrolic coordination of Ni in CO2RR.

CHEMICAL SCIENCE (2021)

Article Chemistry, Multidisciplinary

Low-Valence Znδ+ (0<δ<2) Single-Atom Material as Highly Efficient Electrocatalyst for CO2 Reduction

Simin Li et al.

Summary: The nitrogen-stabilized single-atom catalyst Zn delta+-NC containing low-valence zinc atoms shows excellent catalytic performance in the electrochemical reduction of CO2 to CO. The unsaturated three-coordinate sites on Zn play a key role in reducing the energy barrier and achieving high CO selectivity. This work sheds light on the relationship between coordination number, valence state, and catalytic performance, with potential industrial applications for high current densities.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

Review Materials Science, Multidisciplinary

Product selectivity of photocatalytic CO2 reduction reactions

Junwei Fu et al.

MATERIALS TODAY (2020)

Article Chemistry, Multidisciplinary

Isolated Diatomic Ni-Fe Metal-Nitrogen Sites for Synergistic Electroreduction of CO2

Wenhao Ren et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2019)

Article Chemistry, Multidisciplinary

Self-Adjusting Activity Induced by Intrinsic Reaction Intermediate in Fe-N-C Single-Atom Catalysts

Yu Wang et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2019)

Article Multidisciplinary Sciences

Remarkable active-site dependent H2O promoting effect in CO oxidation

Shu Zhao et al.

NATURE COMMUNICATIONS (2019)

Article Chemistry, Physical

Implicit self-consistent electrolyte model in plane-wave density-functional theory

Kiran Mathew et al.

JOURNAL OF CHEMICAL PHYSICS (2019)

Article Chemistry, Multidisciplinary

Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO2

Xiaoqian Wang et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2018)

Article Chemistry, Multidisciplinary

Coordinatively unsaturated nickel-nitrogen sites towards selective and high-rate CO2 electroreduction

Chengcheng Yan et al.

ENERGY & ENVIRONMENTAL SCIENCE (2018)

Article Multidisciplinary Sciences

Heterogeneous Fe-3 single-cluster catalyst for ammonia synthesis via an associative mechanism

Jin-Cheng Liu et al.

NATURE COMMUNICATIONS (2018)

Article Energy & Fuels

Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction

Hong Bin Yang et al.

NATURE ENERGY (2018)

Article Chemistry, Physical

Theoretical Approaches to Describing the Oxygen Reduction Reaction Activity of Single-Atom Catalysts

Anjli M. Patel et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2018)

Article Chemistry, Multidisciplinary

Synergistic Effects between Atomically Dispersed Fe-N-C and C-S-C for the Oxygen Reduction Reaction in Acidic Media

Hangjia Shen et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2017)

Article Chemistry, Physical

Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways

Kiran Mathew et al.

JOURNAL OF CHEMICAL PHYSICS (2014)

Article Chemistry, Multidisciplinary

How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels

Andrew A. Peterson et al.

ENERGY & ENVIRONMENTAL SCIENCE (2010)

Article Chemistry, Physical

Origin of the overpotential for oxygen reduction at a fuel-cell cathode

JK Norskov et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2004)