催化作用
甲醇
镍
电化学
格式化
氧化还原
阳极
无机化学
化学
氧阴离子
化学工程
组合化学
材料科学
电极
有机化学
物理化学
工程类
作者
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,Yuandong Wang
标识
DOI:10.1038/s41467-022-30670-4
摘要
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.
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