Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles
Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles
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DOI：
10.1002/adfm.201804762
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发表时间：
2018-11-07
影响因子：
19
通讯作者：
Chen, Jingguang G.
中科院分区：
文献类型：
--
作者：
Lee, Ji Hoon;Kattel, Shyam;Chen, Jingguang G.
电化学二氧化碳还原反应（CO2RR）是将二氧化碳转化为增值化学品的有前途的策略之一。金 (Au) 催化剂被认为是 CO2RR 生产 CO 的最佳基准材料。在这项工作中，通过结合实验测量和密度泛函理论 (DFT) 计算，系统地研究了聚合物粘合剂的不同官能团对 Au 催化剂上 CO2RR 的作用。特别是，研究表明，官能团可以起到抑制不期望的析氢反应的作用，这是与CO2RR的主要竞争反应，从而使更多的催化活性位点可用于CO2RR并增强CO2RR活性。与 DFT 预测一致，富含 F 的聚四氟乙烯粘合剂中的含氟 (F) 官能团导致 CO 生产具有高法拉第效率（约 94.7%）。这项研究提出了一种通过优化选择性 CO2RR 聚合物粘合剂的新策略。
Electrochemical CO2 reduction reaction (CO2RR) is one of the promising strategies for converting CO2 to value-added chemicals. Gold (Au) catalysts are considered to be the best benchmarking materials for CO2RR to produce CO. In this work, the role of different functional groups of polymeric binders on CO2RR over Au catalysts is systematically investigated by combined experimental measurements and density functional theory (DFT) calculations. Especially, it is revealed that the functional groups can play a role in suppressing the undesired hydrogen evolution reaction, the main competing reaction against CO2RR, thus enabling more catalytic active sites to be available for CO2RR and enhancing the CO2RR activity. Consistent with the DFT prediction, fluorine (F)-containing functional groups in the F-rich polytetrafluoroethylene binder lead to a high Faradaic efficiency (approximate to 94.7%) of CO production. This study suggests a new strategy by optimizing polymeric binders for the selective CO2RR.