Supported Cobalt Polyphthalocyanine for High-Performance Electrocatalytic CO2 Reduction

被引:484
作者
Han, Na [1 ]
Wang, Yu [2 ]
Ma, Lu [3 ]
Wen, Jianguo [4 ]
Li, Jing [1 ]
Zheng, Hechuang [1 ]
Nie, Kaiqi [1 ]
Wang, Xinxia [1 ]
Zhao, Feipeng [1 ]
Li, Yafei [2 ]
Fan, Jian [1 ]
Zhong, Jun [1 ]
Wu, Tianpin [3 ]
Miller, Dean J. [4 ]
Lu, Jun [3 ]
Lee, Shuit-Tong [1 ]
Li, Yanguang [1 ]
机构
[1] Soochow Univ, Inst Funct Nano & Soft Mat, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China
[2] Nanjing Normal Univ, Coll Chem & Mat Sci, Nanjing 210023, Jiangsu, Peoples R China
[3] Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA
[4] Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA
基金
中国国家自然科学基金;
关键词
CATALYZED ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; METAL PHTHALOCYANINES; ORGANIC FRAMEWORKS; ELECTRODES; PORPHYRINS; EFFICIENCY; NANOTUBES; COMPLEXES; FILMS;
D O I
10.1016/j.chempr.2017.08.002
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical reduction of CO2 represents a possible solution for transforming atmospheric CO2 to value-added chemicals such as CO or hydrocarbons, but so far it has been hampered by the lack of suitable electrocatalysts. In this work, we design a type of organic-inorganic hybrid material by template-directed polymerization of cobalt phthalocyanine on carbon nanotubes for a high-performance CO2 reduction reaction. Compared with molecular phthalocyanines, the polymeric form of phthalocyanines supported on the conductive scaffold exhibits an enlarged electrochemically active surface area and improved physical and chemical robustness. Experimental results show that our hybrid electrocatalyst can selectively reduce CO2 to CO with a large faradic efficiency (similar to 90%), exceptional turnover frequency (4,900 hr(-1) at eta = 0.5 V), and excellent long-term durability. These metrics are superior to those of most of its organic or inorganic competitors. Its high electrocatalytic activity is also supported by density functional theory calculations.
引用
收藏
页码:652 / 664
页数:13
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