文献类型：期刊文献

英文题名：Dopant- and Surfactant-Tuned Electrode-Electrolyte Interface Enabling Efficient Alkynol Semi-Hydrogenation

作者：Zhao, Yuan[1,2];Xu, Jipeng[3];Huang, Kai[3];Ge, Wangxin[2];Liu, Zhen[1];Liu, Honglai[3];Lian, Cheng[3];Jiang, Hongliang[1];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2023

卷号：145

期号：11

起止页码：6516

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20231113739739);WOS:【SCI-EXPANDED(收录号:WOS:000957289400001)】；

基金：This work was supported by the National Natural Science Foundation of China (22222804, U22B20143, 21978278, 21838003, 91834301, 21803063, and 21978087), the National Key R&D program (2022YFB3808400), the Shanghai Scientific and Technological Innovation Project (18JC1410500 and 19JC1410400), the Science and Technology Commission of Shanghai Municipality (22dz1205900), and the Shanghai Municipal Science and Technology Major Project. The authors thank the Shanghai Synchrotron Radiation Facility (14W1, SSRF).

语种：英文

外文关键词：Additives - Catalyst selectivity - Cationic surfactants - Dyes - Electrocatalysts - Electrodes - Electrolytes

摘要：Electrochemical alkynol semi-hydrogenation has emerged as a sustainable and environmentally benign route for the production of high-value alkenols, featuring water as the hydrogen source instead of H2. It is highly challenging to design the electrode-electrolyte interface with efficient electrocatalysts and their matched electro-lytes to break the selectivity-activity stereotype. Here, boron-doped Pd catalysts (PdB) and surfactant-modified interface are proposed to enable the simultaneous increase in alkenol selectivity and alkynol conversion. Typically, compared to pure Pd and commercial Pd/C catalysts, the PdB catalyst achieves both higher turnover frequency (139.8 h-1) and specific selectivity (above 90%) for the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). Quaternary ammonium cationic surfactants that are employed as electrolyte additives are assembled at the electrified interface in response to applied bias potential, establishing an interfacial microenvironment that can facilitate alkynol transfer and hinder water transfer suitably. Eventually the hydrogen evolution reaction is inhibited and alkynol semi-hydrogenation is promoted, without inducing the decrease of alkenol selectivity. This work offers a distinct perspective on creating a suitable electrode-electrolyte interface for electrosynthesis.