Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction

Yan，Chunliu1; Luo，Wen2; Yuan，Huimin2; Liu，Guiyu2; Hao，Rui2; Qin，Ning2; Wang，Zhiqiang2; Liu，Kun2; Wang，Zhenyu2; Cui，Dehu1; Hu，Zhuofeng3; Lan，Yangchun1; Lu，Zhouguang2

2022-07-05

10.1016/j.apcatb.2022.121191

APPLIED CATALYSIS B-ENVIRONMENTAL   影响因子和分区

0926-3373

1873-3883

Appropriate adsorption strength and modes of intermediates on catalysts and the reaction kinetic energy barrier directly determine the selectivity and productivity of final products during CO electroreduction. This work systematically reveals the mechanisms for enhanced CO electroreduction on nitrogen-doped CuO (N-CuO) catalyst by in-situ surface enhanced Raman spectroscopy (SERS) and theoretical calculation. The introduction of N into CuO can significantly enhance the CO adsorption capacity, binding strength of key intermediates and increase the local pH value, resulting in two-fold enhancement of CO and CH production as compared to bare CuO. Meanwhile, the protonation step is promoted, making the formation of COOH quickly and earlier. Therefore, the adsorbed CO intermediate formation is produced more rapidly, and the rate-determining step is transferred, continually facilitating the electroreduction of CO. This study is inspiring in designing high-performance electrocatalysts for CO reduction.

CO2 electroreduction In-situ surface enhanced Raman spectroscopy (SERS) Intermediates adsorption Nitrogen doping copper oxides Reaction kinetic

SCI ; EI

英语

ESI高被引

第一 ; 通讯

Shenzhen NSQKJJ[K20799112] ; Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[ZDSYS20200421111401738] ; National Natural Science Foundation of China["2019B121205001","2019A1515012143"] ; Leading Talents of Guangdong Province[21875097] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[2016LJ06C536] ; Guangdong-Hong Kong-Macao Joint Laboratory[51902357] ; Natural Science Foundation of Guangdong Province, China[38000-18841209] ; Start-up Funds for High-Level Talents of Sun Yatsen University[38000-31610622] ; Fundamental Research Funds for the Central Universities[JCYJ20200109141640095]

Chemistry ; Engineering

Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical

WOS:000787894400003

ELSEVIER

20220811677858

Catalyst selectivity ; Copper oxides ; Doping (additives) ; Electrocatalysts ; Electrolytic reduction ; Gas adsorption ; Indium compounds ; Kinetic energy ; Kinetics ; Reaction intermediates ; Reaction kinetics

Ore Treatment:533.1 ; Fluid Flow, General:631.1 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Classical Physics; Quantum Theory; Relativity:931

CHEMISTRY

2-s2.0-85124715390

Scopus

1.School of Microelectronics,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Materials Science and Engineering,Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials,Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China
3.School of Environmental Science and Engineering,Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology,Sun Yat-sen University,Guangzhou,510275,China

Yan，Chunliu,Luo，Wen,Yuan，Huimin,et al. Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2022,308.

Yan，Chunliu.,Luo，Wen.,Yuan，Huimin.,Liu，Guiyu.,Hao，Rui.,...&Lu，Zhouguang.(2022).Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction.APPLIED CATALYSIS B-ENVIRONMENTAL,308.

Yan，Chunliu,et al."Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction".APPLIED CATALYSIS B-ENVIRONMENTAL 308(2022).