Efficient CO_(2) electroreduction coupled with semi-dehydrogenation of tetrahydroisoquinoline by MOFs modified electrodes  

作　　者：Zi-Hao Zhu Ze-Long Liang Sheng-Li Hou Yao Xie Yue Ma Yan Zhang Bin Zhao 

机构地区：[1]College of Chemistry,Nankai University,Tianjin 300071,China

出　　处：《Journal of Energy Chemistry》2021年第12期328-335,I0008,共9页能源化学（英文版）

基　　金：supported by the National Nature Science Foundation of China (21625103 and 21971125);the China Postdoctoral Science Foundation (2019M660978 and 2020T130319);the 111 Project (B12015)。

摘　　要：Electroreduction of CO_(2) into formate catalyzed by metal-organic frameworks(MOFs) is a promising avenue to promote the carbon cycle,but the oxygen evolution reaction(OER) process in anode usually limited the reaction efficiency.Here,a new framework {(Me_(2) NH_(2))[Bi(L)]·4 DMF·2 H_(2) O}_n(V12) was constructed and structurally characterized(L=5,5'-(1,3,6,8-tetraoxo-1,3,6,8-tetrahydrobenzo [lmn][3,8]phenanthroline-2,7-diyl) dibenzene-1,3-dicarboxylic acid;DMF=N,N-dimethylformamide).V12 possesses large one-dimensional channels with the size of 1.5 × 0.7 nm and exhibits good stability in common solvents.After V12 was modified on electrode via electrodeposition,as-synthesized sample exhibits impressive catalytic performance for the transformation of CO_(2) into formate with Faraday efficiency of93.2% and current density of 11.78 mA cm^(-2) at-0.9 V(vs.RHE).Control experiments revealed that the MOFs electrodeposition strategy significantly improves the charge transfer rate and introduces more structural defects,which promotes the reaction activity.Moreover,tetra hydroisoquinoline is added as an accelerant in the anode to achieve the simultaneous generation of formate and dihydroisoquinoline.More importantly,the cell voltage is reduced from 2.79 to 2.52 V at 10 mA cm^(-2) in a two-electrode system due to more positive reaction kinetics.This work provides an enlightening strategy for using MOFs to establish an effective system to achieve CO_(2) reduction while obtaining high value-added oxidation products.

关 键 词：MOFS Carbon dioxide electroreduction Electrocatalysis Semi-dehydrogenation Electrodeposition 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]