Synergistically electronic tuning of metalloid CdSe nanorods for enhanced electrochemical CO_(2) reduction  

协同电子调控增强类金属特性CdSe纳米棒的电催化CO_(2)还原性能

作　　者：Tao Chen Tianyang Liu Xinyi Shen Wei Zhang Tao Ding Lan Wang Xiaokang Liu Linlin Cao Wenkun Zhu Yafei Li Tao Yao 陈涛;刘天阳;沈心怡;张伟;丁韬;王兰;刘潇康;曹林林;竹文坤;李亚飞;姚涛(National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;State Key Laboratory of Environmentally Friendly Energy Materials,School of National Defense Science and Technology,Southwest University of Science and Technology,Mianyang 621010,China;Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials,Jiangsu Key Laboratory of New Power Batteries,School of Chemistry and Materials Science,Nanjing Normal University,Nanjing 210023,China)

机构地区：[1]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China [2]State Key Laboratory of Environmentally Friendly Energy Materials,School of National Defense Science and Technology,Southwest University of Science and Technology,Mianyang 621010,China [3]Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials,Jiangsu Key Laboratory of New Power Batteries,School of Chemistry and Materials Science,Nanjing Normal University,Nanjing 210023,China

出　　处：《Science China Materials》2021年第12期2997-3006,共10页中国科学（材料科学（英文版）

基　　金：supported by the National Natural Science Foundation of China(12025505 and 21873050);China Ministry of Science and Technology(2017YFA0208300);the Open Fund Project of State Key Laboratory of Environmentally Friendly Energy Materials(20KFHG08);the Youth Innovation Promotion Association CAS(CX2310007007 and CX2310000091)。

摘　　要：Engineering the electronic properties of catalysts to target intermediate adsorption energy as well as harvest high selectivity represents a promising strategy to design advanced electrocatalysts for efficient CO_(2) electroreduction.Herein,a synergistical tuning on the electronic structure of the Cd Se nanorods is proposed for boosting electrochemical reduction of CO_(2) .The synergy of Ag doping coupled with Se vacancies tuned the electronic structure of the CdSe nanorods,which shows the metalloid characterization and thereby the accelerated electron transfer of CO_(2) electroreduction.Operando synchrotron radiation Fourier transform infrared spectroscopy and theoretical simulation revealed that the Ag doping and Se vacancies accelerated the CO_(2) activation process and lowered the energy barrier for the conversion from CO_(2) to;COOH;as a result,the performance of CO_(2) electroreduction was enhanced.The as-obtained metalloid Ag-doped CdSe nanorods exhibited a 2.7-fold increment in current density and 1.9-fold Faradaic efficiency of CO compared with the pristine CdSe nanorod.通过定制催化剂的电子特性以达到合适的中间体吸附能,从而获得高选择性,是一种可用于设计先进的CO_(2)电还原催化剂的有前景的策略,在本文中,我们报道了一种通过协同调控CdSe纳米棒的电子结构以促进电化学CO_(2)还原的方法.银掺杂与硒空位协同调控了CdSe纳米棒的电子结构,导致该结构显示出类金属特性,从而加速了CO_(2)电还原过程中的电子传递.此外,原位同步辐射傅里叶变换红外光谱和理论计算表明,银掺杂和硒空位的耦合加速了CO_(2)活化过程,同时降低了将CO_(2)转化为*COOH中间体的能垒,从而有效增强了电催化CO_(2)还原性能.与原始的CdSe纳米棒相比,银掺杂的CdSe纳米棒表现出2.7倍的电流密度和1.9倍的法拉第效率.

关 键 词：cadmium selenium Ag doping Se vacancies CO_(2)electroreduction 

分 类 号：O643.36[理学—物理化学] TB383.1[理学—化学]