Mechanism study of reduction of CO2 into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role

doi:10.1016/j.jechem.2017.03.013

能源化学(英文) ›› 2017, Vol. 26 ›› Issue (5): 936-941.DOI: 10.1016/j.jechem.2017.03.013

Mechanism study of reduction of CO₂ into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role

Yi Le^a, Heng Zhong^b, Yang Yang^a, Runtian He^a, Guodong Yao^a, Fangming Jin^a,c

a School of Environmental Science and Engineering, State Key Lab of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200240, China;
b Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology(AIST), Nigatake 4-2-1, Miyagino-ku, Sendai 983-8551, Japan;
c Graduate School of Environmental Studies, Tohoku University, Aoba-ku, Sendai 980-8579, Japan

收稿日期:2017-02-13 修回日期:2017-03-22 出版日期:2017-09-15 发布日期:2017-11-10
通讯作者: Guodong Yao,E-mail addresses:geode@sjtu.edu.cn;Fangming Jin,E-mail addresses:fmjin@sjtu.edu.cn
基金资助:
The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China (No. 21277091 & 51472159), the State Key Program of National Natural Science Foundation of China (No. 21436007), the Key Basic Research Projects of Science and Technology Commission of Shanghai (No. 14JC1403100) and the Chenxing-SMG Young Scholar Project of Shanghai Jiao Tong University.

Mechanism study of reduction of CO₂ into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role

Yi Le^a, Heng Zhong^b, Yang Yang^a, Runtian He^a, Guodong Yao^a, Fangming Jin^a,c

a School of Environmental Science and Engineering, State Key Lab of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200240, China;
b Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology(AIST), Nigatake 4-2-1, Miyagino-ku, Sendai 983-8551, Japan;
c Graduate School of Environmental Studies, Tohoku University, Aoba-ku, Sendai 980-8579, Japan

Received:2017-02-13 Revised:2017-03-22 Online:2017-09-15 Published:2017-11-10
Contact: Guodong Yao,E-mail addresses:geode@sjtu.edu.cn;Fangming Jin,E-mail addresses:fmjin@sjtu.edu.cn
Supported by:
The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China (No. 21277091 & 51472159), the State Key Program of National Natural Science Foundation of China (No. 21436007), the Key Basic Research Projects of Science and Technology Commission of Shanghai (No. 14JC1403100) and the Chenxing-SMG Young Scholar Project of Shanghai Jiao Tong University.

摘要/Abstract

摘要： We have previously developed a new process of highly efficient conversion of CO₂ and water into formic acid with metallic Zn without the addition of catalyst, however, its mechanism is not clear, particularly in the catalytic role of Zn/ZnO interface. Herein, the autocatalytic role of Zn/ZnO interface formed in situ during the reduction of CO₂ into formic acid with Zn in water was studied by combining high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques and experimental data. The electron microscope results show that possible defects or dislocations formed on Zn/ZnO interface, in which plays a key role for ZnH-formation. Further XPS analyses indicate that oxygen vacancies on Zn/ZnO interface increased at short reaction times (less than 10 min). These analyses and experimental results suggest that a highly efficient and rapid conversion of CO₂ and water into formic acid should involve an autocatalytic role of the Zn/ZnO interface formed in situ, particularly at the beginning of the reaction.

关键词: Mechanism, CO₂ reduction, Zinc, Water dissociation, Interface catalysis

Abstract: We have previously developed a new process of highly efficient conversion of CO₂ and water into formic acid with metallic Zn without the addition of catalyst, however, its mechanism is not clear, particularly in the catalytic role of Zn/ZnO interface. Herein, the autocatalytic role of Zn/ZnO interface formed in situ during the reduction of CO₂ into formic acid with Zn in water was studied by combining high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques and experimental data. The electron microscope results show that possible defects or dislocations formed on Zn/ZnO interface, in which plays a key role for ZnH-formation. Further XPS analyses indicate that oxygen vacancies on Zn/ZnO interface increased at short reaction times (less than 10 min). These analyses and experimental results suggest that a highly efficient and rapid conversion of CO₂ and water into formic acid should involve an autocatalytic role of the Zn/ZnO interface formed in situ, particularly at the beginning of the reaction.

Key words: Mechanism, CO₂ reduction, Zinc, Water dissociation, Interface catalysis

Yi Le, Heng Zhong, Yang Yang, Runtian He, Guodong Yao, Fangming Jin. Mechanism study of reduction of CO₂ into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role[J]. 能源化学(英文), 2017, 26(5): 936-941.

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Mechanism study of reduction of CO₂ into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role

Mechanism study of reduction of CO₂ into formic acid by in-situ hydrogen produced from water splitting with Zn:Zn/ZnO interface autocatalytic role

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