scholarly journals Study of Proton Coupled Electron Transfer in a Biomimetic Dimanganese Water Oxidation Catalyst with Terminal Water Ligands

2010 ◽  
Vol 6 (8) ◽  
pp. 2395-2401 ◽  
Author(s):  
Ting Wang ◽  
Gary W. Brudvig ◽  
Victor S. Batista
Keyword(s):  
Electron Transfer ◽  
Water Oxidation ◽  
Oxidation Catalyst ◽  
Proton Coupled Electron Transfer ◽  
Water Ligands

scholarly journals Design and synthesis of benzimidazole phenol-porphyrin dyads for the study of bioinspired photoinduced proton-coupled electron transfer

2019 ◽  
Vol 23 (11n12) ◽  
pp. 1336-1345
Author(s):  
S. Jimena Mora ◽  
Daniel A. Heredia ◽  
Emmanuel Odella ◽  
Uma Vrudhula ◽  
Devens Gust ◽  
...  
Keyword(s):  
Electron Transfer ◽  
Excited State ◽  
Photosystem Ii ◽  
Proton Transfer ◽  
Water Oxidation ◽  
Oxidation Catalyst ◽  
Design And Synthesis ◽  
Proton Coupled Electron Transfer ◽  
Anchoring Groups ◽  
High Redox Potential

Benzimidazole phenol-porphyrin dyads have been synthesized to study proton-coupled electron transfer (PCET) reactions induced by photoexcitation. High-potential porphyrins have been chosen to model P680, the photoactive chlorophyll cluster of photosynthetic photosystem II (PSII). They have either two or three pentafluorophenyl groups at the meso positions to impart the high redox potential. The benzimidazole phenol (BIP) moiety models the Tyr[Formula: see text]-His190 pair of PSII, which is a redox mediator that shuttles electrons from the water oxidation catalyst to P680[Formula: see text]. The dyads consisting of a porphyrin and an unsubstituted BIP are designed to study one-electron one-proton transfer (E1PT) processes upon excitation of the porphyrin. When the BIP moiety is substituted with proton-accepting groups such as imines, one-electron two-proton transfer (E2PT) processes are expected to take place upon oxidation of the phenol by the excited state of the porphyrin. The bis-pentafluorophenyl porphyrins linked to BIPs provide platforms for introducing a variety of electron-accepting moieties and/or anchoring groups to attach semiconductor nanoparticles to the macrocycle. The triads thus formed will serve to study the PCET process involving the BIPs when the oxidation of the phenol is achieved by the photochemically produced radical cation of the porphyrin.

scholarly journals Introducing a closed system approach for the investigation of chemical steps involving proton and electron transfer; as illustrated by a copper-based water oxidation catalyst

2017 ◽  
Vol 19 (6) ◽  
pp. 4208-4215 ◽  
Author(s):  
Jessica M. de Ruiter ◽  
Francesco Buda
Keyword(s):  
Molecular Dynamics ◽  
Electron Transfer ◽  
Reaction Mechanism ◽  
Ab Initio ◽  
Closed System ◽  
Water Oxidation ◽  
System Approach ◽  
Oxidation Catalyst ◽  
Proton Coupled Electron Transfer

We present an ab initio molecular dynamics approach to characterize proton-coupled electron transfer catalytic steps and identify the preferred reaction mechanism.

The role of proton coupled electron transfer in water oxidation

2012 ◽  
Vol 5 (7) ◽  
pp. 7704 ◽  
Author(s):  
Christopher J. Gagliardi ◽  
Aaron K. Vannucci ◽  
Javier J. Concepcion ◽  
Zuofeng Chen ◽  
Thomas J. Meyer
Keyword(s):  
Electron Transfer ◽  
Water Oxidation ◽  
Proton Coupled Electron Transfer

scholarly journals Atomically manipulated proton transfer energizes water oxidation on silicon carbide photoanodes

2018 ◽  
Vol 6 (47) ◽  
pp. 24358-24366 ◽  
Author(s):  
Hao Li ◽  
Huan Shang ◽  
Yuchen Shi ◽  
Rositsa Yakimova ◽  
Mikael Syväjärvi ◽  
...  
Keyword(s):  
Silicon Carbide ◽  
Electron Transfer ◽  
Proton Transfer ◽  
Water Oxidation ◽  
Proton Coupled Electron Transfer ◽  
Rate Limiting Step ◽  
Limiting Step ◽  
Rate Limiting

Preferential exposure of Si-face of SiC will mechanistically shift the rate limiting step of water oxidation from sluggish proton-coupled electron transfer on C-face to a more energy-favorable electron transfer.

Aligning Electronic and Protonic Energy Levels of Proton-Coupled Electron Transfer in Water Oxidation on Aqueous TiO2

2014 ◽  
Vol 126 (45) ◽  
pp. 12242-12246 ◽  
Author(s):  
Jun Cheng ◽  
Xiandong Liu ◽  
John A. Kattirtzi ◽  
Joost VandeVondele ◽  
Michiel Sprik
Keyword(s):  
Electron Transfer ◽  
Water Oxidation ◽  
Energy Levels ◽  
Proton Coupled Electron Transfer

scholarly journals Frontispiece: Aligning Electronic and Protonic Energy Levels of Proton-Coupled Electron Transfer in Water Oxidation on Aqueous TiO2

2014 ◽  
Vol 53 (45) ◽  
pp. n/a-n/a
Author(s):  
Jun Cheng ◽  
Xiandong Liu ◽  
John A. Kattirtzi ◽  
Joost VandeVondele ◽  
Michiel Sprik
Keyword(s):  
Electron Transfer ◽  
Water Oxidation ◽  
Energy Levels ◽  
Proton Coupled Electron Transfer

scholarly journals A bio-inspired coordination polymer as outstanding water oxidation catalyst via second coordination sphere engineering

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Wenlong Li ◽  
Fusheng Li ◽  
Hao Yang ◽  
Xiujuan Wu ◽  
Peili Zhang ◽  
...  
Keyword(s):  
Coordination Polymer ◽  
Proton Transfer ◽  
Water Oxidation ◽  
Isotope Effects ◽  
Oxidation Catalyst ◽  
Amino Acid Residues ◽  
Hydrogen Electrode ◽  
Proton Coupled Electron Transfer ◽  
Rate Determining Step ◽  
Iron Nickel

Abstract First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials (η) significantly above thermodynamic requirements. Here, we report an iron/nickel terephthalate coordination polymer on nickel form (NiFeCP/NF) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis. NiFeCP/NF exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm−2 in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of NiFeCP/NF on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate.

scholarly journals The mechanism for proton–coupled electron transfer from tyrosine in a model complex and comparisons with Y Z oxidation in photosystem II

2002 ◽  
Vol 357 (1426) ◽  
pp. 1471-1479 ◽  
Author(s):  
Martin Sjödin ◽  
Stenbjörn Styring ◽  
Björn Åkermark ◽  
Licheng Sun ◽  
Leif Hammarström
Keyword(s):  
Electron Transfer ◽  
Photosystem Ii ◽  
Water Oxidation ◽  
Oxidation Mechanism ◽  
Model System ◽  
Proton Coupled Electron Transfer ◽  
Tyrosine Oxidation ◽  
Model Complex ◽  
Primary Donor ◽  
Mn Cluster

In the water–oxidizing reactions of photosystem II (PSII), a tyrosine residue plays a key part as an intermediate electron–transfer reactant between the primary donor chlorophylls (the pigment P 680 ) and the water–oxidizing Mn cluster. The tyrosine is deprotonated upon oxidation, and the coupling between the proton reaction and electron transfer is of great mechanistic importance for the understanding of the water–oxidation mechanism. Within a programme on artificial photosynthesis, we have made and studied the proton–coupled tyrosine oxidation in a model system and been able to draw mechanistic conclusions that we use to interpret the analogous reactions in PSII.

Sign in / Sign up

Export Citation Format

Share Document