Charge-ordered Cu+/Cu2+ pair regulated highly-selective electroreduction of carbon monoxide to acetate

Luo，Siyuan1; Zou，Haiyuan2; Zheng，Renji1,3; Deng，Shimao1,4; Feng，Xuezhen1; Wei，Wenfei1; Wang，Ranhao1; Li，Ze5; Xu，Wei5; Duan，Lele2; Chen，Hong1

2024-07-15

10.1016/j.apcatb.2024.123887

Applied Catalysis B: Environmental   影响因子和分区

0926-3373

Selective electrochemical reduction of CO/CO to high-valuable C products is of great importance to alleviate the global warming and energy crisis problems, while the selective production of C is severely limited by the C[sbnd]C coupling pathway on the catalyst interface. Herein, by employing a Cu/Cu charge-ordered metal-organic framework (MOF) material (denoted to be Cu4BHT) as a CO electroreduction catalyst, a high acetate selectivity of 50.3% at [sbnd]0.7 V versus reversible hydrogen electrode (RHE) has been achieved. An in-depth mechanism study reveals that the charge-ordered Cu/Cu pair on Cu4BHT interface favors the C[dbnd]O bond activation, C[sbnd]C coupling, and proton-coupled electron transfer dynamics, which results in the selective formation of C products. This work illustrates the critical role of employing charge-ordered Cu/Cu catalytic site pair for C[sbnd]C coupling, which paves the way for designing highly selective catalysts to promote the formation of the C products.

Charge order CO electroreduction Electronic structure regulation Selective reduction

SCI ; EI

英语

第一 ; 通讯

20241015690618

Carbon monoxide ; Catalyst selectivity ; Copper compounds ; Crystalline materials ; Electrolytic reduction ; Energy policy ; Global warming ; Organometallics ; Product design

Atmospheric Properties:443.1 ; Energy Policy:525.6 ; Ore Treatment:533.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Production Engineering:913.1 ; Crystalline Solids:933.1

CHEMISTRY

2-s2.0-85186592799

Scopus

1.State Environmental Protection Key Laboratory of Integrated Surface Water Groundwater Pollution Control,Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,Key Laboratory of Municipal Solid Waste Recycling Technology and Management of Shenzhen City,Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (SKLISEM),School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
3.School of Minerals Processing and Bioengineering,Central South University,Changsha,410083,China
4.Eastern Institute for Advanced Study,Eastern Institute of Technology,Ningbo,China
5.Beijing National Laboratory for Molecular Sciences,Key Laboratory of Organic Solids,Institute of Chemistry,Chinese Academy of Sciences,Beijing,100190,China

Luo，Siyuan,Zou，Haiyuan,Zheng，Renji,et al. Charge-ordered Cu+/Cu2+ pair regulated highly-selective electroreduction of carbon monoxide to acetate[J]. Applied Catalysis B: Environmental,2024,349.

Luo，Siyuan.,Zou，Haiyuan.,Zheng，Renji.,Deng，Shimao.,Feng，Xuezhen.,...&Chen，Hong.(2024).Charge-ordered Cu+/Cu2+ pair regulated highly-selective electroreduction of carbon monoxide to acetate.Applied Catalysis B: Environmental,349.

Luo，Siyuan,et al."Charge-ordered Cu+/Cu2+ pair regulated highly-selective electroreduction of carbon monoxide to acetate".Applied Catalysis B: Environmental 349(2024).