Ag-organic coordination polymers with multi-dimensional electron transfer channels for enhancing CO2 electroreduction

电子转移 聚合物 化学 配位聚合物 化学工程 电子 传输(计算) 纳米技术 材料科学 计算机科学 有机化学 工程类 物理 量子力学 并行计算
作者
Yingbing Zou,Tangxing Pan,Zhiwen Fan,Yunbin Li,Hao Zhang,Yan Ju,Yongfan Zhang,Xiuling Ma,Qianhuo Chen,Shengchang Xiang,Zhangjing Zhang
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:454: 140496-140496 被引量:11
标识
DOI:10.1016/j.cej.2022.140496
摘要

Two Ag-MOCPs with different dimensional electron transfer Channels were used for electrocatalytic conversion CO 2 to CO. • New Ag-MOCP materials for CO 2 RR electrocatalysts were synthesized. • CO 2 -to-CO conversion was boosted with the regulation of the electron transfer channel. • The FE CO for Ag-MOCP-2 with multi-dimensional electron transfer channels is higher than that for Ag-MOCP-1 with single channel at most given potentials. • The mechanism of its reaction was further explored by DFT calculation. Although, electrons transfer plays an important role in achieving the electrocatalytic CO 2 reduction reaction (CO 2 RR), it is scarce to regulate the electron transfer channels for enhancing the performance of CO 2 RR via rational design. Here, based on different solvothermal conditions, two metal-organic coordination polymers (MOCPs, Ag-MOCP-1 and Ag-MOCP-2 ) electrocatalyst for CO 2 RR were obtained by the same Ag ions and 5-phenyltetrazolium ligands. Single crystal X-ray diffraction showed Ag-MOCP-2 with intra-&inter-layer C–H···π and π···π interactions, while Ag-MOCP-1 with intra-layer π···π interactions. The intra-&inter-layer π interactions in Ag-MOCP-2 makes it show multi-dimensional electron transfer channels, which enable Ag-MOCP-2 with higher electron conductivities and lower band gap than Ag-MOCP-1 . And the Faradaic efficiency of CO for Ag-MOCP-2 with 78.3% is higher than that for Ag-MOCP-1 with 69.1% at -1.08 V vs . RHE, and the maximum difference can reach 22% at -1.48 V vs . RHE. Based on the same central metal and organic ligands of the two MOCPs, we believe that multi-dimensional electron transfer channels make a predominant contribution for improving CO 2 RR performance in this work.
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