Electrocatalytic Water Oxidation by a Phosphorus-Nitrogen O=PN3-Pincer Cobalt Complex

被引:15
作者
Das, Pradip K. [1 ,2 ]
Bhunia, Sarmistha [3 ]
Chakraborty, Priyanka [1 ,2 ]
Chatterjee, Sudipta [1 ,2 ]
Rana, Atanu [3 ]
Peramaiah, Karthik [1 ,2 ]
Alsabban, Merfat M. [1 ,2 ]
Dutta, Indranil [1 ,2 ]
Dey, Abhishek [3 ]
Huang, Kuo-Wei [1 ,2 ]
机构
[1] King Abdullah Univ Sci & Technol, KAUST Catalysis Ctr, Thuwal 239556900, Saudi Arabia
[2] King Abdullah Univ Sci & Technol, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia
[3] Indian Assoc Cultivat Sci, Sch Chem Sci, Kolkata 700032, India
关键词
OXYGEN-EVOLUTION ELECTROCATALYSTS; MOLECULAR CATALYSTS; PORPHYRINS; COOX; IDENTIFICATION; HYDROGENATION; REACTIVITY; CONVERSION; REDUCTION; CHEMISTRY;
D O I
10.1021/acs.inorgchem.0c02376
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Water oxidation is a primary step in natural as well as artificial photosynthesis to convert renewable solar energy into chemical energy/fuels. Electrocatalytic water oxidation to evolve O-2, utilizing suitable low-cost catalysts and renewable electricity, is of fundamental importance considering contemporary energy and environmental issues, yet it is kinetically challenging owing to the complex multiproton/electron transfer processes. Herein, we report the first cobalt-based pincer catalyst for catalytic water oxidation at neutral pH with high efficiency under electrochemical conditions. Most importantly, ligand (pseudo)aromaticity is identified to play an important role during electrocatalysis. A significant potential jump (similar to 300 mV) was achieved toward a lower positive value when the aromatized cobalt complex was transformed into a (pseudo)-dearomatized cobalt species. The dearomatized species catalyzes the water oxidation reaction to evolve oxygen at a much lower overpotential (similar to 340 mV) on the basis of the onset potential (at a current density of 0.5 mA/cm(2)) of catalysis at pH 10.5, outperforming other Co-based molecular catalysts reported to date. These observations may provide a new strategy for the judicious design of earth-abundant transition-metal-based water oxidation catalysts.
引用
收藏
页码:615 / 623
页数:9
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