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|Title:||Molecule confined isolated metal sites enable the electrocatalytic synthesis of hydrogen peroxide||Authors:||Li, Xiaogang
Fan, Hong Jin
Choksi, Tej S.
|Keywords:||Engineering::Chemical engineering||Issue Date:||2022||Source:||Li, X., Tang, S., Dou, S., Fan, H. J., Choksi, T. S. & Wang, X. (2022). Molecule confined isolated metal sites enable the electrocatalytic synthesis of hydrogen peroxide. Advanced Materials, 34(25), 2104891-. https://dx.doi.org/10.1002/adma.202104891||Project:||M4012076RG118/18
|Journal:||Advanced Materials||Abstract:||The direct synthesis of hydrogen peroxide (H2 O2 ) through the two-electron oxygen reduction reaction is a promising alternative to the industrial anthraquinone oxidation process. Selectivity to H2 O2 is however limited by the four-electron pathway during oxygen reduction. Herein, it is reported that aminoanthraquinone confined isolated metal sites on carbon supports selectively steer oxygen reduction to H2 O2 through the two-electron pathway. Confining isolated NiNx sites under aminoanthraquinone increases the selectivity to H2 O2 from below 55% to above 80% over a wide potential range. Spectroscopy characterization and density functional theory calculations indicate that isolated NiNx sites are confined within a nanochannel formed between the molecule and the carbon support. The confinement reduces the thermodynamic barrier for OOH* desorption versus further dissociation, thus increasing the selectivity to H2 O2 . It is revealed how tailoring noncovalent interactions beyond the binding site can empower electrocatalysts for the direct synthesis of H2 O2 through oxygen reduction.||URI:||https://hdl.handle.net/10356/160708||ISSN:||0935-9648||DOI:||10.1002/adma.202104891||Schools:||School of Chemical and Biomedical Engineering
School of Physical and Mathematical Sciences
|Organisations:||Cambridge Centre for Advanced Research and Education in Singapore||Rights:||© 2021 Wiley-VCH GmbH. All rights reserved.||Fulltext Permission:||none||Fulltext Availability:||No Fulltext|
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