Activated Ni-OH bond in a catalyst facilitates nucleophile oxidation reaction

doi:10.1002/adma.202105320

機構典藏 > College of Engineering > Graduate Institute & Department of Electrical Engineering > Journal Article > Item 987654321/124101

Please use this identifier to cite or link to this item: https://tkuir.lib.tku.edu.tw/dspace/handle/987654321/124101

Title:	Activated Ni-OH bond in a catalyst facilitates nucleophile oxidation reaction
Authors:	Chen, Wei;Wang, Yanyong;Wu, Binbin;Shi, Jianqiao;Li, Yingying;Xu, Leitao;Xie, Chao;Zhou, Wang;Huang, Yu-Cheng;Wang, Tehua;Du, Shiqian;Song, Minglei;Wang, Dongdong;Chen, Chen;Zheng, Jianyun;Liu, Jilei;Dong, Chung-Li;Zou, Yuqin;Chen, Jun;Wang, Shuangyin
Keywords:	electrocatalysis;layered double hydroxides;nucleophile oxidation reaction;organic electrosynthesis;space-confinement-induced synthesis
Date:	2022-07-07
Issue Date:	2023-05-15 12:10:23 (UTC+8)
Publisher:	Wiley Online Library
Abstract:	The nucleophile oxidation reaction (NOR) is of enormous significance for organic electrosynthesis and coupling for hydrogen generation. However, the nonuniform NOR mechanism limits its development. For the NOR, involving electrocatalysis and organic chemistry, both the electrochemical step and non-electrochemical process should be taken into account. The NOR of nickel-based hydroxides includes the electrogenerated dehydrogenation of the Ni2+–OH bond and a spontaneous non-electrochemical process; the former determines the electrochemical activity, and the nucleophile oxidation pathway depends on the latter. Herein, the space-confinement-induced synthesis of Ni3Fe layered double hydroxide intercalated with single-atom-layer Pt nanosheets (Ni3Fe LDH-Pt NS) is reported. The synergy of interlayer Pt nanosheets and multiple defects activates Ni–OH bonds, thus exhibiting an excellent NOR performance. The spontaneous non-electrochemical steps of the NOR are revealed, such as proton-coupled electron transfer (PCET; Ni3+–O + X–H = Ni2+–OH + X•), hydration, and rearrangement. Hence, the reaction pathway of the NOR is deciphered, which not only helps to perfect the NOR mechanism, but also provides inspiration for organic electrosynthesis.
Relation:	Advanced Materials 34(27), 2105320
DOI:	10.1002/adma.202105320
Appears in Collections:	[Graduate Institute & Department of Electrical Engineering] Journal Article

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