Sub-2 nm mixed metal oxide for electrochemical reduction of carbon dioxide to carbon monoxide  

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作  者:Devina Thasia Wijaya Andi Haryanto Hyun Woo Lim Kyoungsuk Jin Chan Woo Lee 

机构地区:[1]Department of Chemistry,Kookmin University,Seoul 02707,Republic of Korea [2]Department of Materials Science and Engineering,Seoul National University,Seoul 08826,Republic of Korea [3]Department of Chemistry,Korea University,Seoul 02841,Republic of Korea

出  处:《Journal of Energy Chemistry》2023年第9期303-310,共8页能源化学(英文版)

基  金:supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (RS-2023-00210114);supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (NRF-2021R1C1C1004264 and NRF2021R1A4A1032114);supported by the National Research Foundation of Korea (NRF) Grant funded by the Korean Government (MSIT) (NRF-2022R1A4A1019296);supported by the National R&D Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (2021M3D1A2051636)。

摘  要:Mixed metal oxide(MMO) represents a critical class of materials that can allow for obtaining a dynamic interface between its components:reduced metal and its metal oxide counterpart during an electrocatalytic reaction.Here,a synthetic method utilizing a MOF-derived micro/mesoporous carbon as a template to prepare sub-2 nm MMO catalysts for CO_(2) electro reduction is reported.Starting from the zeolite imidazolate framework(ZIF-8),the pyrolyzed derivatives were used to synthesize sub-2 nm Pd-Ni MMO with different compositions.The Ni-rich(Pd_(20)-Ni_(80)/ZC) catalyst exhibits unexpectedly superior performance for CO production with an improved Faradaic efficiency(FE) of 95.3% at the current density of 200 mA cm^(-2) at-0.56 V vs.reversible hydrogen electrode(RHE) compared to other Pd-Ni compositions.X-ray photoelectron spectroscopy(XPS) analysis confirms the presence of Ni^(2+) and Pd^(2+) in all compositions,demonstrating the presence of MMO.Density functional theory(DFT) calculation reveals that the lower CO binding energy on the surface of the Pd_(20)-Ni_(80) cluster eases CO desorption,thus increasing its production.This work provides a general synthetic strategy for MMO electrocatalysts and can pave a new way for screening multimetallic catalysts with a dynamic electrochemical interface.

关 键 词:Carbon dioxide reduction Mixed metal oxide NANOALLOY Carbon monoxide Metal-organic framework 

分 类 号:X701[环境科学与工程—环境工程] TQ426[化学工程]

 

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