期刊
CHEMSUSCHEM
卷 9, 期 23, 页码 3361-3369出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201601286
关键词
catalysis; foot of the wave analysis; reaction mechanisms; water oxidation; water splitting
资金
- La Caixa foundation
- MINECO [CTQ-2013-49075-R, SEV-2013-0319, CTQ-2014-52974-REDC, ENE2014-52280-REDT]
- MINECO/FEDER [CTQ2015-64261-R]
- DFG [Me 1313/9-1, SFB 1073]
- international PhD program CaSuS (Catalysis for Sustainable Synthesis)
The description of the foot of the wave analysis (FOWA) applied to the electrocatalytic oxidation of water to dioxygen is reported for cases where the rate determining step is first order and second order with regard to catalyst concentration, coinciding mechanistically with the so-called water nucleophilic attack (WNA) and the interaction of two M-O units (I2M, where M represents the metal center of the catalyst), respectively. The newly adapted equations are applied to a range of relevant molecular catalysts, both in homogeneous and heterogeneous phase, and the kinetic parameters are determined, including apparent rate constants and turnover frequencies. In this respect, the application of FOWA at different catalyst concentrations allows elucidation of the reaction mechanism that operates in each case. In addition, catalytic Tafel plots are used for assessing the performance of several molecular water oxidation catalysts (WOCs) as a function of overpotential under analogous conditions, and thus can be used for benchmarking purposes. This analysis was carried out earlier for oxide-based WOCs; however, this is the first report using molecular WOCs.
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