Mesoporous PdAg Nanospheres for Stable Electrochemical CO2 Reduction to Formate |
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| Authors: | Yuan Zhou Rui Zhou Xiaorong Zhu Na Han Bin Song Tongchao Liu Guangzhi Hu Yafei Li Jun Lu Yanguang Li |
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| Affiliation: | 1. Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123 China;2. College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023 China;3. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439 USA;4. Institute for Ecological Research and Pollution Control of Plateau Lakes, School of Ecology and Environmental Science, Yunnan University, Kunming, 650504 China |
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| Abstract: | Palladium is a promising material for electrochemical CO2 reduction to formate with high Faradaic efficiency near the equilibrium potential. It unfortunately suffers from problematic operation stability due to CO poisoning on surface. Here, it is demonstrated that alloying is an effective strategy to alleviate this problem. Mesoporous PdAg nanospheres with uniform size and composition are prepared from the co-reduction of palladium and silver precursors in aqueous solution using dioctadecyldimethylammonium chloride as the structure-directing agent. The best candidate can initiate CO2 reduction at zero overpotential and achieve high formate selectivity close to 100% and great stability even at <-0.2 V versus reversible hydrogen electrode. The high selectivity and stability are believed to result from the electronic coupling between Pd and Ag, which lowers the d-band center of Pd and thereby significantly enhances its CO tolerance, as evidenced by both electrochemical analysis and theoretical simulations. |
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| Keywords: | electrochemical CO2 reduction formate mesoporous nanospheres palladium–silver alloys stability |
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