In-situ polymerization induced atomically dispersed manganese sites as cocatalyst for CO2 photoreduction into synthesis gas

被引:70
作者
Yang, Jia [1 ]
Wang, Zhiyuan [1 ]
Jiang, Jianchao [2 ,3 ,4 ]
Chen, Wenxing [5 ]
Liao, Fan [1 ]
Ge, Xiao [1 ]
Zhou, Xiao [1 ]
Chen, Min [1 ]
Li, Ruilong [1 ]
Xue, Zhenggang [1 ]
Wang, Gang [6 ]
Duan, Xuezhi [6 ]
Zhang, Guoqing [1 ]
Wang, Yang-Gang [2 ,3 ]
Wu, Yuen [1 ]
机构
[1] Univ Sci & Technol China, Sch Chem & Mat Sci, Natl Synchrotron Radiat Lab, Hefei Natl Lab Phys Sci Microscale,Collaborat Inn, Hefei 230026, Anhui, Peoples R China
[2] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
[3] Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalysis, Shenzhen 518055, Guangdong, Peoples R China
[4] Shaanxi Univ Technol, Inst Graphene, Sch Mat Sci & Engn, Shaanxi Key Lab Catalysis, Hanzhong 723001, Peoples R China
[5] Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Construct Tailorable Adv Funct Ma, Beijing 100081, Peoples R China
[6] East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Single atom catalyst; Mn-N-C; Polypyrrole; Photocatalysis; CO2; reduction; METAL-ORGANIC-FRAMEWORKS; ATOM CATALYSTS; SINGLE; REDUCTION; EVOLUTION; INSIGHTS;
D O I
10.1016/j.nanoen.2020.105059
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Developing highly-active single atom catalyst to realize visible light driven photocatalytic CO2 reduction into value-added chemicals is an appealing route toward utilizing CO2 as the only carbon source for a sustainable future. Herein, we have successfully synthesized the atomically dispersed manganese sites in nitrogen doped carbon via an in-situ polymerization approach. The in-situ oxidative polymerization of pyrrole monomer directly catalyzed by manganese dioxide could extract the Mn atoms from MnO2 and stabilize them within the as generated polymer skeleton in one step. After high-temperature pyrolysis, atomically dispersed Mn sites are obtained, firmly and homogeneously anchored by the as-generated N-doped carbon support. The as obtained catalyst can act as cocatalyst to realize photocatalytic CO2 reduction to produce synthesis gas under visible light using [Ru(bpy)(3)]Cl-2 (bpy: 2,20-bipyridine) as photosensitizer and triethanolamine as sacrifacial agent, with gas evolution rate of CO 1470 mu mol/h/g, H-2 1310 mu mol/h/g and tunable CO/H-2 ratio from 1.12 to 0.43. Our approach is versatile to prepare a variety of morphology-controllable single atom catalysts from metal oxides for important industrial applications.
引用
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页数:7
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