Pulsed Electrolysis with a Nickel Molecular Catalyst Improves Selectivity for Carbon Dioxide Reduction



Greenwell, Francesca, Siritanaratkul, Bhavin, Sharma, Preetam K, Yu, Eileen H and Cowan, Alexander J
(2023) Pulsed Electrolysis with a Nickel Molecular Catalyst Improves Selectivity for Carbon Dioxide Reduction. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 145 (28). pp. 15078-15083.

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Abstract

Pulsed electrolysis can significantly improve carbon dioxide reduction on metal electrodes, but the effect of short (millisecond to seconds) voltage steps on molecular electrocatalysts is largely unstudied. In this work, we investigate the effect pulse electrolysis has on the selectivity and stability of the homogeneous electrocatalyst [Ni(cyclam)]<sup>2+</sup> at a carbon electrode. By tuning the potential and pulse duration, we achieve a significant improvement in CO Faradaic efficiencies (85%) after 3 h, double that of the system under potentiostatic conditions. The improved activity is due to in situ catalyst regeneration from an intermediate that occurs as part of the catalyst's degradation pathway. This study demonstrates the wider opportunity to apply pulsed electrolysis to molecular electrocatalysts to control activity and improve selectivity.

Item Type: Article
Uncontrolled Keywords: 40 Engineering, 4016 Materials Engineering, 34 Chemical Sciences, 7 Affordable and Clean Energy
Divisions: Faculty of Science and Engineering > School of Physical Sciences
Depositing User: Symplectic Admin
Date Deposited: 30 Jun 2023 13:46
Last Modified: 20 Jun 2024 16:59
DOI: 10.1021/jacs.3c04811
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3171385