Induction of Concerted Proton-Coupled Electron Transfer during Oxygen Evolution on Hematite Using Lanthanum Oxide as a Solid Proton Acceptor

ACS Catalysis ◽  
2019 ◽  
Vol 9 (10) ◽  
pp. 9212-9215 ◽  
Author(s):  
Toshihiro Takashima ◽  
Koki Ishikawa ◽  
Hiroshi Irie
2016 ◽  
Vol 52 (97) ◽  
pp. 14015-14018 ◽  
Author(s):  
Toshihiro Takashima ◽  
Koki Ishikawa ◽  
Hiroshi Irie

The oxygen evolution activity of hematite at neutral pH was enhanced by inducing the concerted proton-coupled electron transfer process.


2015 ◽  
Vol 19 (01-03) ◽  
pp. 1-8 ◽  
Author(s):  
Dilek K. Dogutan ◽  
D. Kwabena Bediako ◽  
Daniel J. Graham ◽  
Christopher M. Lemon ◽  
Daniel G. Nocera

The splitting of water into its constituent elements is an important solar fuels conversion reaction for the storage of renewable energy. For each of the half reactions of the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), multiple protons and electrons must be coupled to avoid high-energy intermediates. To understand the mechanistic details of the PCET chemistry that underpins HER and OER, we have designed hangman porphyrin and corrole catalysts. In these hangman constructs, a pendant acid/base functionality within the secondary coordination sphere is "hung" above the macrocyclic redox platform on which substrate binds. The two critical thermodynamic properties of a PCET event, the redox potential and pKa may be tuned with the macrocycle and hanging group, respectively. This review outlines the synthesis of these catalysts, as well as the examination of the PCET kinetics of hydrogen and oxygen evolution by the hangman catalysts. The insights provided by these systems provide a guide for the design of future HER and OER catalysts that use a secondary coordination sphere to manage PCET.


2020 ◽  
Vol 142 (26) ◽  
pp. 11550-11559 ◽  
Author(s):  
Astrid Nilsen-Moe ◽  
Clorice R. Reinhardt ◽  
Starla D. Glover ◽  
Li Liang ◽  
Sharon Hammes-Schiffer ◽  
...  

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