Activity origins and design principles of nickel-based catalysts for nucleophile electrooxidation
學年 109
學期 1
出版（發表）日期 2020-11-05
作品名稱 Activity origins and design principles of nickel-based catalysts for nucleophile electrooxidation
作品名稱（其他語言）
著者 W. Chen; C. Xie; Y. Wang; Y. Zou; C. L. Dong; Y. C. Huang; Z. Xiao; Z. Wei; S. Du; C. Chen; B. Zhou; J. Ma; S. Wang
單位
出版者
著錄名稱、卷期、頁數 Chem 6(11), p.2974-2993
摘要 Understanding how electrocatalysts function in a nucleophile oxidation reaction (NOR) on anode, replacing the oxygen evolution reaction (OER) of water splitting, is vital to the development of hydrogen generation and organic electrosynthesis. Here, we propose that for β-Ni(OH)2 and NiO, the NOR activity origins are β-Ni(OH)O containing electrophilic lattice oxygen and NiO(OH)ads containing electrophilic adsorption oxygen, respectively. For β-Ni(OH)2, NOR is a two-step, one-electron reaction, including an electrogenerated catalyst dehydrogenation reaction and a spontaneous nucleophile dehydrogenation reaction. Therefore, the NOR activity of β-Ni(OH)2 can be markedly regulated by tuning the lattice oxygen ligand environment. For β-Co0.1Ni0.9(OH)2, the onset potential of NOR with different nucleophiles is ∼1.29 V (1 M KOH), which breaks the bottleneck of ∼1.35 V for most nickel-based catalysts. Overall, we identify the activity origins and propose the design principles of nickel-based catalysts for NOR. These provide theoretical guidance for the development of NOR and organic electrosynthesis in practical industrial applications.
關鍵字 electrocatalysis;nucleophile oxidation reaction;nickel hydroxide;activity origin;multiple in situ measurements;catalyst oxidation;reaction interface analysis;isotope labeling experiment;organic electrosynthesis;electrophilic lattice oxygen
語言 en_US
ISSN 2451-9294
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 是
國別 USA
公開徵稿
出版型式 ,電子版
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