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Tuning Redox Active Polyoxometalates for Efficient Electron-Coupled Proton-Buffer-Mediated Water Splitting.
Lei, Jie; Yang, Jun-Jie; Liu, Ting; Yuan, Ru-Ming; Deng, Ding-Rong; Zheng, Ming-Sen; Chen, Jia-Jia; Cronin, Leroy; Dong, Quan-Feng.
Afiliación
  • Lei J; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Yang JJ; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Liu T; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Yuan RM; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Deng DR; College of Mechanical and Energy Engineering, Jimei University, Xiamen, Fujian, 361005, P. R. China.
  • Zheng MS; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Chen JJ; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Cronin L; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), Xiamen University, Xiamen, Fujian, 361005, P. R. China.
  • Dong QF; School of Chemistry, University of Glasgow, Glasgow, UK.
Chemistry ; 25(49): 11432-11436, 2019 Sep 02.
Article en En | MEDLINE | ID: mdl-31309625
We present strategies to tune the redox properties of polyoxometalate clusters to enhance the electron-coupled proton-buffer-mediated water splitting process, in which the evolution of hydrogen and oxygen can occur in different forms and is separated in time and space. By substituting the heteroatom template in the Keggin-type polyoxometalate cluster, H6 ZnW12 O40 , it is possible to double the number of electrons and protonation in the redox reactions (from two to four). This increase can be achieved with better matching of the energy levels as indicated by the redox potentials, compared to the ones of well-studied H3 PW12 O40 and H4 SiW12 O40 . This means that H6 ZnW12 O40 can act as a high-performance redox mediator in an electrolytic cell for the on-demand generation of hydrogen with a high decoupling efficiency of 95.5 % and an electrochemical energy efficiency of 83.3 %. Furthermore, the H6 ZnW12 O40 cluster also exhibits an excellent cycling behaviour and redox reversibility with almost 100 % H2 -mediated capacity retention during 200 cycles and a high coulombic efficiency >92 % each cycle at 30 mA cm-2 .
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Texto completo: 1 Bases de datos: MEDLINE Idioma: En Revista: Chemistry Asunto de la revista: QUIMICA Año: 2019 Tipo del documento: Article
Texto completo
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Texto completo: 1 Bases de datos: MEDLINE Idioma: En Revista: Chemistry Asunto de la revista: QUIMICA Año: 2019 Tipo del documento: Article