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 vs.Ag/AgCl)和光照条件下...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 vs.Ag/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.展开更多
基金supported by the National Basic Research Program of China(973 Program2013CB632402)+7 种基金the National Natural Science Foundation of China(513201050015137219051402025and 21433007)the Natural Science Foundation of Hubei Province(2015CFA001)the Fundamental Research Funds for the Central Universities(WUT:2014-VII-010)the Self-Determined and Innovative Research Funds of State Key Laboratory of Advanced Technology for Material Synthesis and ProcessingWuhan University of Technology(2013-ZD-1)~~
基金the National Key R&D Program of China(2017YFA0207301)National Natural Science Foundation of China(21725102,91961106,U1832156)+3 种基金CAS Key Research Program of Frontier Sciences(QYZDB-SSW-SLH018)CAS Interdisciplinary Innovation Team,Chinese Academy of Sciences President's International Fellowship Initiative(2019PC0114)China Postdoctoral Science Foundation(2019M652190)Chinese Universities Scientific Fund(WK2310000067,WK2060190096).
基金the National Natural Science Foundation of China (NSFC) (20906034)the project (2015KF-7) supported by State Key Laboratory of Advanced Technology for Material Synthesis and Processing (Wuhan University of Technology)+4 种基金the Key Academic Program of the 3rd phase "211 Project" of South China Agricultural University (2009B010100001) for their supportthe State Key Project of Fundamental Research for Nanoscience and Nanotechnology (2013CB632402)NSFC (51272199, 51320105001 and 21433007)Deanship Of Scientific Research (DSR) of King Abdulaziz University (90-130-35-Hi Ci)NSFC (20963002 and 21173088) for their support
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)+5 种基金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)
文摘光电化学(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 vs.Ag/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.