高效光电化学催化CO_(2)转化合成乙酸

作     者：王晓农 高超 刘敬祥 毛可可 段德隆 陈双明 叶润 邱云瑞 马军 郑旭升 龙冉 武晓君 宋礼 朱俊发 熊宇杰 Xiaonong Wang;Chao Gao;Jingxiang Low;Keke Mao;Delong Duan;Shuangming Chen;Run Ye;Yunrui Qiu;Jun Ma;Xusheng Zheng;Ran Long;Xiaojun Wu;Li Song;Junfa Zhu;Yujie Xiong

作者机构：Hefei National Laboratory for Physical Sciences at the MicroscaleCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Institute of EnergyHefei Comprehensive National Science CenterHefei 230031China School of Energy and Environment ScienceAnhui University of TechnologyMaanshan 243032China 

基　　金：financially supported in part by the National Key R&D Program of China (2017YFA0207301, and 2017YFA0403402) the National Natural Science Foundation of China (21725102, 91961106, U1832156, 22075267, 21803002, 91963108, 21950410514, and U1732272) CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018) Science and Technological Fund of Anhui Province for Outstanding Youth (2008085 J05) Youth Innovation Promotion Association of CAS (2019444) Young Elite Scientist Sponsorship Program by CAST, China Postdoctoral Science Foundation (2019 M652190, 2020 T130627) Chinese Universities Scientific Fund (WK2060190096), MOST (2018YFA0208603) DNL Cooperation Fund, CAS (DNL201922, DNL180201) 

出 版 物：《Science Bulletin》 (科学通报（英文版）)

年 卷 期：2021年第66卷第13期

页      码：1296-1304,M0004页

摘      要：光电化学(PEC)催化CO_(2)转化合成高附加值多碳化合物具有广阔的应用前景.本文将Au纳米晶修饰N掺杂TiO_(2)纳米片的光阳极与Zn掺杂Cu_(2)O阴极相结合,构筑了高效PECCO_(2)转化体系.该体系在较低外加偏压(0.5 V ***/AgCl)和光照条件下能够实现CO_(2)高效转化合成CH3COOH,其法拉第效率高达58.1%(碳产物的选择性为91.5%).研究人员进一步利用程序升温脱附和原位拉曼光谱发现阴极上Zn的引入能够在选择性催化CO_(2)转化合成CH3COOH过程中起到关键作用:(1)优化Cu_(2)O局部电子结构;(2)增加表面反应活性位点;(3)促进C-C偶联中间体CH2/*CH3的形成.而Au纳米晶修饰N掺杂TiO_(2)纳米片优异的光响应则能够为反应提供更多的光生电子,进而提高催化反应速率.这项工作不仅实现了高选择性光电化学催化CO_(2)向高附加值产物的转化,同时为高效PEC CO_(2)转化体系的设计提供了新的思路.

主 题 词：Ag/AgCl N掺杂 程序升温脱附 选择性催化 原位拉曼光谱 光电化学 光生电子 高选择性 

学科分类：083002[083002] 0830[工学-生物工程类] 081702[081702] 081705[081705] 08[工学] 0817[工学-轻工类] 080502[080502] 0805[工学-能源动力学] 

核心收录：

D　O　I：10.1016/j.scib.2021.04.004

馆 藏 号：203102902...