期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 14, 页码 5386-5395出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c12696
关键词
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资金
- Research Center Program of the IBS in Korea [IBS-R006-D1]
- National Research Foundation of Korea (NRF) Grant - Korea government [2019R1A2C2005521]
- University of Seoul
- Ministry of Science & ICT (MSIT), Republic of Korea [IBS-R006-D1-2021-A00] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2019R1A2C2005521] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
The interaction between metals and metal-organic frameworks can significantly enhance the activity, selectivity, and stability of atomically dispersed Au on tensile-strained Pd nanoparticles, leading to improved formate production with high CO tolerance.
Pd is one of the most effective catalysts for the electrochemical reduction of CO2 to formate, a valuable liquid product, at low overpotential. However, the intrinsically high CO affinity of Pd makes the surface vulnerable to CO poisoning, resulting in rapid catalyst deactivation during CO2 electroreduction. Herein, we utilize the interaction between metals and metal-organic frameworks to synthesize atomically dispersed Au on tensile-strained Pd nanoparticles showing significantly improved formate production activity, selectivity, and stability with high CO tolerance. We found that the tensile strain stabilizes all reaction intermediates on the Pd surface, whereas the atomically dispersed Au selectively destabilizes CO* without affecting other adsorbates. As a result, the conventional COOH* versus CO* scaling relation is broken, and our catalyst exhibits 26- and 31-fold enhancement in partial current density and mass activity toward electrocatalytic formate production with over 99% faradaic efficiency, compared to Pd/C at -0.25 V versus RHE.
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