Coordination environment tuning of nickel sites by oxyanions to optimize methanol electro-oxidation activity

Shanlin Li, Ruguang Ma, Jingcong Hu, Zichuang Li, Lijia Liu, Xunlu Wang, Yue Lu, George E. Sterbinsky, Shuhu Liu, Lei Zheng, Jie Liu, Danmin Liu and Jiacheng Wang ()
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Shanlin Li: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
Ruguang Ma: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
Jingcong Hu: Beijing University of Technology
Zichuang Li: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
Lijia Liu: Western University
Xunlu Wang: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
Yue Lu: Beijing University of Technology
George E. Sterbinsky: Advanced Photon Source, Argonne National Laboratory
Shuhu Liu: Institute of High Energy Physics, Chinese Academy of Sciences
Lei Zheng: Institute of High Energy Physics, Chinese Academy of Sciences
Jie Liu: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
Danmin Liu: Beijing University of Technology
Jiacheng Wang: The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract To achieve zero-carbon economy, advanced anode catalysts are desirable for hydrogen production and biomass upgrading powered by renewable energy. Ni-based non-precious electrocatalysts are considered as potential candidates because of intrinsic redox attributes, but in-depth understanding and rational design of Ni site coordination still remain challenging. Here, we perform anodic electrochemical oxidation of Ni-metalloids (NiPx, NiSx, and NiSex) to in-situ construct different oxyanion-coordinated amorphous nickel oxyhydroxides (NiOOH-TOx), among which NiOOH-POx shows optimal local coordination environment and boosts electrocatalytic activity of Ni sites towards selective oxidation of methanol to formate. Experiments and theoretical results demonstrate that NiOOH-POx possesses improved adsorption of OH* and methanol, and favors the formation of CH3O* intermediates. The coordinated phosphate oxyanions effectively tailor the d band center of Ni sites and increases Ni-O covalency, promoting the catalytic activity. This study provides additional insights into modulation of active-center coordination environment via oxyanions for organic molecules transformation.

Date: 2022
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DOI: 10.1038/s41467-022-30670-4

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