Rational Design of Diatomic Active Sites for Elucidating Oxygen Evolution Reaction Performance Trends

Diatomic catalysts, especially those with heteronuclear active sites, have recently attracted significant attention for their advantages over single-atom catalysts in reactions with relatively high energy barrier, e.g. oxygen evolution reaction. Rational design and synthesis of heteronuclear diatomic catalysts are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report macrocyclic precursor constrained strategy to fabricate series of transition metal (M<sup>T</sup>, Ni, Co, Fe, Mn, or Cu)-noble (M<sup>N</sup>, Ir or Ru) centers in carbon material. One notable performance trend is observed in the order of Cu-M<sup>N</sup><Mn-M<sup>N</sup><Fe-M<sup>N</sup><M<sup>N</sup><Co-M<sup>N</sup><Ni-M<sup>N</sup>. Meanwhile, the pathway has been not altered, still following the traditional adsorption reaction mechanism. The effect of the M<sup>T</sup> atoms on the performances could possibly originate from the distinct adsorption/desorption behaviors of key intermediates (i.e. *OH, *O and/or *OOH), strongly implying that ΔG<sub>*OOH</sub>-ΔG<sub>*OH</sub> could be used as the performance descriptor. We believe that our work provides useful strategy for synthesis of diatomic active sites with sole coordination configuration and varied composition, and in-depth insight to their catalytic mechanism, which could be used for further optimization of diatomic catalysts towards oxygen electrocatalysis.

Authors

Institutions

Publication Details

Journal
Angewandte Chemie International Edition
Published
2024-10-04
DOI
https://doi.org/10.1002/anie.202413749
Citations
8
Primary Topic
Electrocatalysts for Energy Conversion
Type
article
Field-Weighted Citation Impact
0.82

Funders

Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Rational Design of Diatomic Active Sites for Elucidating Oxygen Evolution Reaction Performance Trends

Yuxiang Jin, Wei Tu, Zhangquan Peng, Zhigang Geng et al.
8 citations
Angewandte Chemie International Edition
Electrocatalysts for Energy Conversion
0.82
article

Rational Design of Diatomic Active Sites for Elucidating Oxygen Evolution Reaction Performance Trends

Yuxiang Jin, Wei Tu, Zhangquan Peng, Zhigang Geng, Fangyi Cheng, Qiunan Liu, Erhong Song, Nanfeng Xu, Kazu Suenaga, Junyuan Xu, Xiao Wang, Zhirong Zhang, Meng Yu, Chao Wang
article en
8 citations

Abstract

Diatomic catalysts, especially those with heteronuclear active sites, have recently attracted significant attention for their advantages over single-atom catalysts in reactions with relatively high energy barrier, e.g. oxygen evolution reaction. Rational design and synthesis of heteronuclear diatomic catalysts are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report macrocyclic precursor constrained strategy to fabricate series of transition metal (M<sup>T</sup>, Ni, Co, Fe, Mn, or Cu)-noble (M<sup>N</sup>, Ir or Ru) centers in carbon material. One notable performance trend is observed in the order of Cu-M<sup>N</sup><Mn-M<sup>N</sup><Fe-M<sup>N</sup><M<sup>N</sup><Co-M<sup>N</sup><Ni-M<sup>N</sup>. Meanwhile, the pathway has been not altered, still following the traditional adsorption reaction mechanism. The effect of the M<sup>T</sup> atoms on the performances could possibly originate from the distinct adsorption/desorption behaviors of key intermediates (i.e. *OH, *O and/or *OOH), strongly implying that ΔG<sub>*OOH</sub>-ΔG<sub>*OH</sub> could be used as the performance descriptor. We believe that our work provides useful strategy for synthesis of diatomic active sites with sole coordination configuration and varied composition, and in-depth insight to their catalytic mechanism, which could be used for further optimization of diatomic catalysts towards oxygen electrocatalysis.

Angewandte Chemie International EditionVol. 64(1)
University of Science and Technology of China (CN), Dalian Institute of Chemical Physics (CN), Chinese Academy of Sciences (CN), Nankai University (CN), Yanshan University (CN), Hefei National Center for Physical Sciences at Nanoscale (CN), Osaka Research Institute of Industrial Science and Technology (JP), Nano Energy (South Africa) (ZA), Shanghai Institute of Ceramics (CN), State Key Laboratory of Metastable Materials Science and Technology, State Key Laboratory of High Performance Ceramics and Superfine Microstructure, The University of Osaka (JP)
National Natural Science Foundation of China, Chinese Academy of Sciences, Science and Technology Commission of Shanghai Municipality, Shanghai Jiao Tong University, Japan Society for the Promotion of Science, National Key Research and Development Program of China
Affordable and clean energy
Openalex Percentile: Top 32%
Electrocatalysts for Energy Conversion
0.82
DOIOpen Access PDFOpenAlex
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.