Ni-doped ZnCo2O4 atomic layers to boost the selectivity in solar-driven reduction of CO2

作     者：Katong Liu Xiaodong Li Liang Liang Ju Wu Xingchen Jiao Jiaqi Xu Yongfu Sun Yi Xie 

作者机构：Hefei National Laboratory far Physical Sciences at Microscale CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei 230026 China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2018年第11卷第6期

页      面：2897-2908页

核心收录：

学科分类：080903[工学-微电子学与固体电子学] 081704[工学-应用化学] 07[理学] 0809[工学-电子科学与技术（可授工学、理学学位）] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 070301[理学-无机化学] 

基　　金：supported by the National Key Research and Development Program of China 国家自然科学基金 Youth Innovation Promotion Association of CAS Key Research Program of Frontier Sciences of CAS the Fundamental Research Funds for the Central Universities Scientific Research Grant of Hefei Science Center of CAS 

主　　题：atomic layers Ni-doped zinc cobaltite selectivity of CO2 reduction 

摘      要：Regulating the selectivity of CO2 photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the selectivity of CO2 photoreduction. Prototypical ZnCo2O4 atomic layers with/without Ni-doping were first synthesized. Density functional theory calculations reveal that introducing Ni atoms creates several new energy levels and increases the density-of-states at the conduction band minimum. Synchrotron radiation photoemission spectroscopy demonstrates that the band structures are suitable for CO2 photoreduction, while the surface photovoltage spectra demonstrate that Ni doping increases the carrier separation efficiency. In situ diffuse reflectance Fourier transform infrared spectra disclose that the CO2^- radical is the main intermediate, while temperature-programed desorption curves reveal that the ZnCo2O4 atomic layers with/without Ni doping favor the respective CO and CH4 desorption. The Ni-doped ZnCo2O4 atomic layers exhibit a 3.5-time higher CO selectivity than the ZnCo2O4 atomic layers. This work establishes a clear correlation between elemental doping and selectivity regulation for CO2 photoreduction, opening new possibilities for tailoring solar-driven photocatalytic behaviors.