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We would like to acknowledge the financial support by the China Scholarship Council (Grant No. 202208140019) , which funded the PhD grant for Shuqin Geng, the leading author of this work, and CNRS for the funding CPJ OPERANDO 278487. Finally, XAS experiments were performed at the CLESS beamline at ALBA Synchrotron (Proposal No. 2022035799) with the collaboration of ALBA staff.

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Towards the development of smart nickel/carbon-based materials for lignin electrolysis: First steps for unravelling the influence of nickel loading and catalyst morphology on lignin electrooxidation

Publicat a:Applied Catalysis B-Environmental. 365 124947- - 2025-05-15 365(), DOI: 10.1016/j.apcatb.2024.124947

Autors: Geng, Shuqin; Gonzalez-Cobos, Jesus; Perez-Carcelen, Lorena; Blanco-Gutierrez, Veronica; Marini, Carlo; Dos Santos-Garcia, Antonio Juan; Caravaca, Angel

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The production of H2 through the electrolysis of lignin is a promising technology, which offers several theoretical advantages compared to the state-of-the-art electrolysis of water, such as: i) the possibility to work under lower electrical polarizations on account of the favoured thermodynamics, and ii) the valorisation of a biomass-waste. The electrooxidation of lignin seems to be the limiting reaction for the overall electrolysis process. Therefore, the development of efficient/smart catalysts for such reaction is of paramount importance. The aim of this study is to get more insights into understanding the influence of the catalyst morphology and physicochemical properties for the desired electrochemical process. Hence, we developed a variety of nickel/carbon materials with nominal nickel loadings from 1 % to 20 %. The thorough characterization of those materials indicated that the catalysts with low nickel loading exhibited small needle-like nanostructures in strong interaction with the carbon support. However, as the loading increased, we observed a coexistence of such small nickel-based nanostructures with much bigger nanosheet-like structures covering the support (with weaker interactions). The electrochemical results were discussed together with the assessment of in-situ characterization techniques (Raman and XANES), and we propose a global model where the electrochemical activity towards the electrooxidation of lignin was mainly attributed to the synergic effect between the high-surface-area carbon support containing oxygen functional groups and the small nickel-based nanostructures, while the bigger nanosheet-like structures were rendered ineffective for such electrochemical process. Thus, this study opens a new window towards the development of advanced/smart materials for lignin-electrooxidation.

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