N, O-coordinated Zn-MOFs for selective conversion of CO2 to formate
N, O-coordinated Zn-MOFs for selective conversion of CO2 to formate
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DOI：
10.1016/j.apsusc.2023.156664
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发表时间：
2023-02
影响因子：
6.7
通讯作者：
Ying Yang;Jiali Huang;Yingbing Zou;Yunbin Li;Tingting Zhan;Limei Huang;Xiuling Ma;Zhangjing Zhang;S. Xiang
中科院分区：
文献类型：
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作者：
Ying Yang;Jiali Huang;Yingbing Zou;Yunbin Li;Tingting Zhan;Limei Huang;Xiuling Ma;Zhangjing Zhang;S. Xiang
金属有机骨架(MOF)电化学还原CO2生成甲酸盐是目前能源转化领域中最有前景的温室气体减排途径之一。本文以3-氨基-1，2，4-三氮唑(ATRZ)与2-甲基对苯二甲酸(BDC-CH3)或2-氨基对苯二甲酸(BDC-NH2)为原料，合成了两种新的N，O配位的锌金属氧化物分子筛(FJU-127-CH3和FJU-127-NH2)，用于二氧化碳的电化学还原反应(CO2RR)。与已报道的以CO或CH4为主要产物的N配位或O配位的锌-MOF催化剂不同，这两个N，O配位的锌-MOF催化剂对甲酸盐具有比选择性和活性，法拉第效率(FE)超过60%。尤其是自侵彻的FJU-127-CH3在−为1.57VVS时具有90.2%的优越性能。RHE与普通柱层FJU-127-NH_2的比较。本工作提出了一种改变电催化CO2RR选择性的有效策略。
Electrochemical reduction of CO2to formate by metal-organic frameworks (MOFs) is one of the promising routes to mitigate greenhouse gas emissions in the energy conversion field. Herein, two new N,O-coordinated Zn-MOFs (FJU-127-CH3and FJU-127-NH2) were constructed from 3-amino-1,2,4-triazole (ATRZ) with 2-methyl-terephthalic acid (BDC-CH3) or 2-amino-terephthalic acid (BDC-NH2) for electrochemical CO2reduction reaction (CO2RR). Different from all the reported N- or O-coordinated Zn-MOFs catalysts with the main product of CO or CH4, the two N,O-coordinated Zn-MOFs exhibit specific selectivity and activity for formate with faradaic efficiency (FE) more than 60%. Especially, self-penetration FJU-127-CH3possesses superior FEformateof 90.2% at −1.57 Vvs. RHE in comparison with common pillared-layer FJU-127-NH2. This work proposes an effective strategy to alter the selectivity of electrocatalytic CO2RR.