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González Calatayud, DavidAuthorRecio, F JavierAuthorMendiola, M AntoniaAuthorLopez-Torres, ElenaCorresponding Author

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March 10, 2025
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Nickel(II) Benzil Bis(Thiosemicarbazonato) Complexes as Electrocatalysts for Hydrogen Evolution Reaction

Publicated to: Applied Organometallic Chemistry. 39 (4): e70094- - 2025-04-01 39(4), DOI: 10.1002/aoc.70094

Authors: Lizcano-Vaquero, Ruben; Buron, Rodrigo; Recio, F Javier; Jimenez-Gomez, Daniel; Calatayud, David G; Iglesias-Juez, Ana; Fresno, Fernando; Mendiola, M Antonia; Lopez-Torres, Elena

Affiliations

CSIC, Inst Catalisis & Petroleoquim, Madrid, Spain - Author
Univ Autonoma Madrid, Dept Quim Fis Aplicada, Madrid, Spain - Author
Univ Autonoma Madrid, Dept Quim Inorgan, Madrid, Spain - Author
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Abstract

We report the electrocatalytic performance in hydrogen evolution reaction (HER) of three Ni(II) complexes based on benzil bis(thiosemicarbazone) ligands derived from 1,2-diphenylethanedione and 4-isopropyl-3-thiosemicarbazide ((LH2)-H-1), 4-methyl-3-thiosemicarbazide ((LH2)-H-2) or 3-thiosemicarbazide ((LH2)-H-3). Cyclic voltammetry in dimethylformamide (DMF) exhibit two diffusion-controlled reversible processes at negative potentials, corresponding to [(NiL3)-L-II]/[(NiL3)-L-II](-) and Ni-II/Ni-I reduction processes. The catalytic activity in DMF was evaluated using acetic acid as proton source, showing the appearance of a catalytic cathodic current associated with the Ni-II/I redox couple. Analysis of the gas evolved from controlled potential coulometry (CPC) confirmed that the three complexes can effectively catalyse hydrogen evolution and that the catalytic activity depends on the substituent attached to the terminal amine. Electrolysis induces electrodeposition of the complexes on the electrode surface forming a film, which were also tested as HER catalysts. The results showed that the total charge produced by the films is, in all cases, lower than with the dissolved complex, but they exhibit higher faradaic efficiencies. DFT calculations were made to establish the catalytic route, and the results support an ECEC mechanism, in which E represents an electrochemical step and C is a chemical one (protonation), centred in the metal assisted by the ligand.

Keywords

Bifunctional electrocatalystBis(thiosemicarbazone)DerivativesEfficienElectrocatalysiElectrocatalysisHydrogen evolution reactionNickel(ii) complexesOxygenReduction

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal Applied Organometallic Chemistry due to its progression and the good impact it has achieved in recent years, according to the agency Scopus (SJR), it has become a reference in its field. In the year of publication of the work, 2025, it was in position , thus managing to position itself as a Q2 (Segundo Cuartil), in the category Inorganic Chemistry.

Independientemente del impacto esperado determinado por el canal de difusión, es importante destacar el impacto real observado de la propia aportación.

Según las diferentes agencias de indexación, el número de citas acumuladas por esta publicación hasta la fecha 2025-12-06:

  • Scopus: 3

Impact and social visibility

From the perspective of influence or social adoption, and based on metrics associated with mentions and interactions provided by agencies specializing in calculating the so-called "Alternative or Social Metrics," we can highlight as of 2025-12-06:

  • The use of this contribution in bookmarks, code forks, additions to favorite lists for recurrent reading, as well as general views, indicates that someone is using the publication as a basis for their current work. This may be a notable indicator of future more formal and academic citations. This claim is supported by the result of the "Capture" indicator, which yields a total of: 6 (PlumX).

It is essential to present evidence supporting full alignment with institutional principles and guidelines on Open Science and the Conservation and Dissemination of Intellectual Heritage. A clear example of this is:

  • The work has been submitted to a journal whose editorial policy allows open Open Access publication.
  • Assignment of a Handle/URN as an identifier within the deposit in the Institutional Repository: https://repositorio.uam.es/handle/10486/719969

Leadership analysis of institutional authors

There is a significant leadership presence as some of the institution’s authors appear as the first or last signer, detailed as follows: First Author (Lizcano-Vaquero, Ruben) and Last Author (LOPEZ TORRES, ELENA SOFIA).

the author responsible for correspondence tasks has been LOPEZ TORRES, ELENA SOFIA.

Awards linked to the item

FJR acknowledges financial support from Grant TED2021-131042B-I00 funded by MCIN/AEI/10.13039/501100011033 and by "ERDF A way of making Europe."