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p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction

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p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction. / Li, Simin; Lu, Xiuyuan; Zhao, Siqi et al.

In: ACS Catalysis, Vol. 12, No. 12, 06.2022, p. 7386-7395.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

Harvard

Li, S, Lu, X, Zhao, S, Ceccato, M, Hu, X-M, Roldan, A, Liu, M & Daasbjerg, K 2022, 'p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction', ACS Catalysis, vol. 12, no. 12, pp. 7386-7395. https://doi.org/10.1021/acscatal.2c01805

APA

Li, S., Lu, X., Zhao, S., Ceccato, M., Hu, X-M., Roldan, A., Liu, M., & Daasbjerg, K. (2022). p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction. ACS Catalysis, 12(12), 7386-7395. https://doi.org/10.1021/acscatal.2c01805

CBE

Li S, Lu X, Zhao S, Ceccato M, Hu X-M, Roldan A, Liu M, Daasbjerg K. 2022. p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction. ACS Catalysis. 12(12):7386-7395. https://doi.org/10.1021/acscatal.2c01805

MLA

Li, Simin et al. "p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction". ACS Catalysis. 2022, 12(12). 7386-7395. https://doi.org/10.1021/acscatal.2c01805

Vancouver

Li S, Lu X, Zhao S, Ceccato M, Hu X-M, Roldan A et al. p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction. ACS Catalysis. 2022 Jun;12(12):7386-7395. doi: 10.1021/acscatal.2c01805

Author

Li, Simin ; Lu, Xiuyuan ; Zhao, Siqi et al. / p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction. In: ACS Catalysis. 2022 ; Vol. 12, No. 12. pp. 7386-7395.

Bibtex

@article{79d373993efd4330a3379d09999c4eb7,
title = "p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction",
abstract = "Electrochemical CO2 reduction represents a promising path toward the production of value-added chemicals. Atomically dispersed metal sites on nitrogen-doped carbon have demonstrated outstanding catalytic performance in this reaction. However, challenges remain in developing such catalysts beyond transition metals. Herein, we present two types of p-block indium single-atom catalysts: one with four nitrogen coordinated (In-N-4) and another with three nitrogen coordinated with one vacancy nearby (In-N-3-V). In electrochemical CO2 reduction, the In-N-3-V site can achieve maximum CO Faradic efficiency (FECO) of 95% at -0.57 V vs reversible hydrogen electrode (RHE) in an aqueous medium. This outperforms the intact In-N-4 catalyst with the maximum FE(CO )of 80% at -0.47 V vs RHE. Density functional theory calculations on the mechanism suggest that structural change from In-N-4 to In-N-3-V brings the In orbital (s and pz) energies closer to the Fermi energy. These hybridized orbitals are responsible for lowering the energy barrier for COOH* intermediate formation, thus enhancing the catalytic performance. This work sheds light on the relationship between catalytic performance and structure of In single-atom sites, highlighting the importance of tailoring the electron state of s and P-z orbitals in developing efficient p-block single-atom catalysts for electrochemical CO2 reduction.",
keywords = "CO2 reduction, indium single atoms, metal-organic frameworks, coordination environment, electrocatalysis, CARBON, FORMATE, ELECTROREDUCTION, ELECTROCATALYST, CONVERSION, METAL",
author = "Simin Li and Xiuyuan Lu and Siqi Zhao and Marcel Ceccato and Xin-Ming Hu and Alberto Roldan and Min Liu and Kim Daasbjerg",
year = "2022",
month = jun,
doi = "10.1021/acscatal.2c01805",
language = "English",
volume = "12",
pages = "7386--7395",
journal = "A C S Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "12",

}

RIS

TY - JOUR

T1 - p-Block Indium Single-Atom Catalyst with Low-Coordinated In-N Motif for Enhanced Electrochemical CO2 Reduction

AU - Li, Simin

AU - Lu, Xiuyuan

AU - Zhao, Siqi

AU - Ceccato, Marcel

AU - Hu, Xin-Ming

AU - Roldan, Alberto

AU - Liu, Min

AU - Daasbjerg, Kim

PY - 2022/6

Y1 - 2022/6

N2 - Electrochemical CO2 reduction represents a promising path toward the production of value-added chemicals. Atomically dispersed metal sites on nitrogen-doped carbon have demonstrated outstanding catalytic performance in this reaction. However, challenges remain in developing such catalysts beyond transition metals. Herein, we present two types of p-block indium single-atom catalysts: one with four nitrogen coordinated (In-N-4) and another with three nitrogen coordinated with one vacancy nearby (In-N-3-V). In electrochemical CO2 reduction, the In-N-3-V site can achieve maximum CO Faradic efficiency (FECO) of 95% at -0.57 V vs reversible hydrogen electrode (RHE) in an aqueous medium. This outperforms the intact In-N-4 catalyst with the maximum FE(CO )of 80% at -0.47 V vs RHE. Density functional theory calculations on the mechanism suggest that structural change from In-N-4 to In-N-3-V brings the In orbital (s and pz) energies closer to the Fermi energy. These hybridized orbitals are responsible for lowering the energy barrier for COOH* intermediate formation, thus enhancing the catalytic performance. This work sheds light on the relationship between catalytic performance and structure of In single-atom sites, highlighting the importance of tailoring the electron state of s and P-z orbitals in developing efficient p-block single-atom catalysts for electrochemical CO2 reduction.

AB - Electrochemical CO2 reduction represents a promising path toward the production of value-added chemicals. Atomically dispersed metal sites on nitrogen-doped carbon have demonstrated outstanding catalytic performance in this reaction. However, challenges remain in developing such catalysts beyond transition metals. Herein, we present two types of p-block indium single-atom catalysts: one with four nitrogen coordinated (In-N-4) and another with three nitrogen coordinated with one vacancy nearby (In-N-3-V). In electrochemical CO2 reduction, the In-N-3-V site can achieve maximum CO Faradic efficiency (FECO) of 95% at -0.57 V vs reversible hydrogen electrode (RHE) in an aqueous medium. This outperforms the intact In-N-4 catalyst with the maximum FE(CO )of 80% at -0.47 V vs RHE. Density functional theory calculations on the mechanism suggest that structural change from In-N-4 to In-N-3-V brings the In orbital (s and pz) energies closer to the Fermi energy. These hybridized orbitals are responsible for lowering the energy barrier for COOH* intermediate formation, thus enhancing the catalytic performance. This work sheds light on the relationship between catalytic performance and structure of In single-atom sites, highlighting the importance of tailoring the electron state of s and P-z orbitals in developing efficient p-block single-atom catalysts for electrochemical CO2 reduction.

KW - CO2 reduction

KW - indium single atoms

KW - metal-organic frameworks

KW - coordination environment

KW - electrocatalysis

KW - CARBON

KW - FORMATE

KW - ELECTROREDUCTION

KW - ELECTROCATALYST

KW - CONVERSION

KW - METAL

UR - https://pubs.acs.org/doi/pdf/10.1021/acscatal.2c01805

U2 - 10.1021/acscatal.2c01805

DO - 10.1021/acscatal.2c01805

M3 - Journal article

VL - 12

SP - 7386

EP - 7395

JO - A C S Catalysis

JF - A C S Catalysis

SN - 2155-5435

IS - 12

ER -