Chen, Y., Gao, R., Ji, S., Li, H., Tang, K., Jiang, P., Hu, H., Zhang, Z., Hao, H., Qu, Q., Liang, X., Chen, W., Dong, J., Wang, D., & Li, Y. (2021). Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance. Angewandte Chemie - International Edition, 60(6), 3212-3221. https://doi.org/10.1002/anie.202012798
Chen, Yuanjun ; Gao, Rui ; Ji, Shufang et al. / Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks : Enhanced Oxygen Reduction Performance. In: Angewandte Chemie - International Edition. 2021 ; Vol. 60, No. 6. pp. 3212-3221.
@article{e36edfb3fb8c4feea739ae0748ebf16b,
title = "Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance",
abstract = "Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF-derived Co single-atom catalyst with the optimal Co1-N3PS active moiety incorporated in a hollow carbon polyhedron (Co1-N3PS/HC) was designed and synthesized. Co1-N3PS/HC exhibits outstanding alkaline ORR activity with a half-wave potential of 0.920 V and superior ORR kinetics with record-level kinetic current density and an ultralow Tafel slope of 31 mV dec−1, exceeding that of Pt/C and almost all non-precious ORR electrocatalysts. In acidic media the ORR kinetics of Co1-N3PS/HC still surpasses that of Pt/C. This work offers atomic-level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.",
keywords = "cobalt, density-functional calculations, heterogeneous catalysis, metal–organic frameworks, oxygen reduction",
author = "Yuanjun Chen and Rui Gao and Shufang Ji and Haijing Li and Kun Tang and Peng Jiang and Haibo Hu and Zedong Zhang and Haigang Hao and Qingyun Qu and Xiao Liang and Wenxing Chen and Juncai Dong and Dingsheng Wang and Yadong Li",
note = "Publisher Copyright: {\textcopyright} 2020 Wiley-VCH GmbH",
year = "2021",
month = feb,
day = "8",
doi = "10.1002/anie.202012798",
language = "English",
volume = "60",
pages = "3212--3221",
journal = "Angewandte Chemie - International Edition",
issn = "1433-7851",
publisher = "John Wiley and Sons Ltd",
number = "6",
}
Chen, Y, Gao, R, Ji, S, Li, H, Tang, K, Jiang, P, Hu, H, Zhang, Z, Hao, H, Qu, Q, Liang, X, Chen, W, Dong, J, Wang, D & Li, Y 2021, 'Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance', Angewandte Chemie - International Edition, vol. 60, no. 6, pp. 3212-3221. https://doi.org/10.1002/anie.202012798
Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance. / Chen, Yuanjun; Gao, Rui; Ji, Shufang et al.
In:
Angewandte Chemie - International Edition, Vol. 60, No. 6, 08.02.2021, p. 3212-3221.
Research output: Contribution to journal › Article › peer-review
TY - JOUR
T1 - Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks
T2 - Enhanced Oxygen Reduction Performance
AU - Chen, Yuanjun
AU - Gao, Rui
AU - Ji, Shufang
AU - Li, Haijing
AU - Tang, Kun
AU - Jiang, Peng
AU - Hu, Haibo
AU - Zhang, Zedong
AU - Hao, Haigang
AU - Qu, Qingyun
AU - Liang, Xiao
AU - Chen, Wenxing
AU - Dong, Juncai
AU - Wang, Dingsheng
AU - Li, Yadong
N1 - Publisher Copyright:
© 2020 Wiley-VCH GmbH
PY - 2021/2/8
Y1 - 2021/2/8
N2 - Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF-derived Co single-atom catalyst with the optimal Co1-N3PS active moiety incorporated in a hollow carbon polyhedron (Co1-N3PS/HC) was designed and synthesized. Co1-N3PS/HC exhibits outstanding alkaline ORR activity with a half-wave potential of 0.920 V and superior ORR kinetics with record-level kinetic current density and an ultralow Tafel slope of 31 mV dec−1, exceeding that of Pt/C and almost all non-precious ORR electrocatalysts. In acidic media the ORR kinetics of Co1-N3PS/HC still surpasses that of Pt/C. This work offers atomic-level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.
AB - Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF-derived Co single-atom catalyst with the optimal Co1-N3PS active moiety incorporated in a hollow carbon polyhedron (Co1-N3PS/HC) was designed and synthesized. Co1-N3PS/HC exhibits outstanding alkaline ORR activity with a half-wave potential of 0.920 V and superior ORR kinetics with record-level kinetic current density and an ultralow Tafel slope of 31 mV dec−1, exceeding that of Pt/C and almost all non-precious ORR electrocatalysts. In acidic media the ORR kinetics of Co1-N3PS/HC still surpasses that of Pt/C. This work offers atomic-level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.
KW - cobalt
KW - density-functional calculations
KW - heterogeneous catalysis
KW - metal–organic frameworks
KW - oxygen reduction
UR - http://www.scopus.com/inward/record.url?scp=85097443409&partnerID=8YFLogxK
U2 - 10.1002/anie.202012798
DO - 10.1002/anie.202012798
M3 - Article
C2 - 33124719
AN - SCOPUS:85097443409
SN - 1433-7851
VL - 60
SP - 3212
EP - 3221
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 6
ER -
Chen Y, Gao R, Ji S, Li H, Tang K, Jiang P et al. Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance. Angewandte Chemie - International Edition. 2021 Feb 8;60(6):3212-3221. doi: 10.1002/anie.202012798
