Selectively converting CO_(2) to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells  

作　　者：Jiwu Zhao Liang Huang Lan Xue Zhenjie Niu Zizhong Zhang Zhengxin Ding Rusheng Yuan Xu Lu Jinlin Long 

机构地区：[1]State Key Laboratory of Photocatalysis on Energy and Environment,College of Chemistry,Fuzhou University,Fuzhou 350116,Fujian,China [2]Clean Combustion Research Center(CCRC),Division of Physical Sciences and Engineering,King Abdullah University of Science and Technology(KAUST),Thuwal 23955-6900,Saudi Arabia

出　　处：《Journal of Energy Chemistry》2023年第4期601-610,共10页能源化学（英文版）

基　　金：financially supported by the National Key R&D Program of China (2018YFE0208500);the National Natural Science Foundation of China (Grants No. 22072022);funded by King Abdullah University of Science and Technology (KAUST) through the baseline funding (BAS/1/1413-01-01)。

摘　　要：The integration of electrochemical CO_(2)reduction(CO_(2)RR) and photoelectrochemical water oxidation offers a sustainable access to valuable chemicals and fuels. Here, we develop a rapidly annealed hematite photoanode with a photocurrent density of 2.83 mA cm^(-2)at 1.7 VRHEto drive the full-reaction. We also present Cu-alloys electrocatalysis extended from CuInSnS4, which are superior in both activity and selectivity for CO_(2)RR. Specifically, the screened CuInSn achieves a CO_(2)to HCOOH Faradaic efficiency of 93% at a cell voltage of-2.0 V by assembling into artificial photosynthesis cell. The stability test of IT exhibits less than 3% degradation over 24 h. Furthermore, in-situ Raman spectroscopy reveals that both CO_(3)^(-2)and CO_(2)are involved in CO_(2)RR as reactants. The preferential affinity of C for H in the ^(*)HCO_(2)intermediate enables an improved HCOOH-selectivity, highlighting the role of multifunctional Cu in reducing the cell voltage and enhancing the photocurrent density.

关 键 词：CO_(2)reduction Rapid annealing Fe_(2)O_(3)photoanode CuInSnS_(4) In-situ spectroscopy 

分 类 号：X701[环境科学与工程—环境工程] TQ225.121[化学工程—有机化工]