ORCID Profile
0000-0003-2246-4466
Current Organisation
University of Nottingham
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Publisher: American Chemical Society (ACS)
Date: 17-05-2021
Publisher: Wiley
Date: 26-04-2023
Abstract: Herein, we report the synthesis and characterization of a new class of hybrid Wells–Dawson polyoxometalate (POM) containing a diphosphoryl group (P 2 O 6 X) of the general formula [P 2 W 17 O 57 (P 2 O 6 X)] 6− (X=O, NH, or CR 1 R 2 ). Modifying the bridging unit X was found to impact the redox potentials of the POM. The ease with which a range of α‐functionalized diphosphonic acids (X=CR 1 R 2 ) can be prepared provides possibilities to access erse functionalized hybrid POMs. Compared to existing phosphonate hybrid Wells–Dawson POMs, diphosphoryl‐substituted POMs offer a wider tunable redox window and enhanced hydrolytic stability. This study provides a basis for the rational design and synthesis of next‐generation hybrid Wells–Dawson POMs.
Publisher: Wiley
Date: 13-08-2023
Abstract: ‘Bacterial‐type’ ferredoxins host a cubane [4Fe4S] 2+/+ cluster that enables these proteins to mediate electron transfer and facilitate a broad range of biological processes. Peptide maquettes based on the conserved cluster‐forming motif have previously been reported and used to model the ferredoxins. Herein we explore the integration of a [4Fe4S]‐peptide maquette into a H 2 ‐powered electron transport chain. While routinely formed under anaerobic conditions, we illustrate by electron paramagnetic resonance (EPR) analysis that these maquettes can be reconstituted under aerobic conditions by using photoactivated NADH to reduce the cluster at 240 K. Attempts to tune the redox properties of the iron‐sulfur cluster by introducing an Fe‐coordinating selenocysteine residue were also explored. To demonstrate the integration of these artificial metalloproteins into a semi‐synthetic electron transport chain, we utilize a ferredoxin‐inspired [4Fe4S]‐peptide maquette as the redox partner in the hydrogenase‐mediated oxidation of H 2 .
Publisher: Wiley
Date: 05-2023
Abstract: Understanding and eliminating degradation of the electrolyte solution is arguably the major challenge in the development of high energy density lithium–air batteries. The use of acetonitrile provides cycle stability comparable to current state‐of‐the‐art glyme ethers and, while solvent degradation has been extensively studied, no mechanism for acetonitrile degradation has been proposed. Through the application of in situ pressure measurements and ex situ characterization to monitor the degradation of acetonitrile in the lithium–air battery, a correlation between H 2 O concentration within the cell and deviation from the idealized electron/oxygen ratio is revealed. Characterization of the cycled electrolyte solution identifies acetamide as the major degradation product under both cell and model conditions. A new degradation pathway is proposed that rationalizes the formation of acetamide, identifies the role of H 2 O in the degradation process, and confirms lithium hydroperoxide as a critical antagonistic species in lithium–air cells for the first time. These studies highlight the importance of considering the impact of atmospheric gases when exploring lithium–air cell chemistry and suggest that further exploration of the impact of hydroperoxide species on the degradation in lithium–air cells may lead to identification of more effective electrolyte solvents.
Publisher: American Chemical Society (ACS)
Date: 21-07-2023
DOI: 10.1021/JACS.3C03207
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CC02138F
Abstract: An organofunctionalised hybrid polyoxometalate bearing Ru antennae exhibits selective CO 2 electrochemical reduction to C1 feedstocks.
Publisher: Wiley
Date: 26-04-2023
Abstract: Herein, we report the synthesis and characterization of a new class of hybrid Wells–Dawson polyoxometalate (POM) containing a diphosphoryl group (P 2 O 6 X) of the general formula [P 2 W 17 O 57 (P 2 O 6 X)] 6− (X=O, NH, or CR 1 R 2 ). Modifying the bridging unit X was found to impact the redox potentials of the POM. The ease with which a range of α‐functionalized diphosphonic acids (X=CR 1 R 2 ) can be prepared provides possibilities to access erse functionalized hybrid POMs. Compared to existing phosphonate hybrid Wells–Dawson POMs, diphosphoryl‐substituted POMs offer a wider tunable redox window and enhanced hydrolytic stability. This study provides a basis for the rational design and synthesis of next‐generation hybrid Wells–Dawson POMs.
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Graham Newton.