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Title: Molecule confined isolated metal sites enable the electrocatalytic synthesis of hydrogen peroxide
Authors: Li, Xiaogang
Tang, Shasha
Dou, Shuo
Fan, Hong Jin
Choksi, Tej S.
Wang, Xin
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-.
Project: M4012076RG118/18
RS 04/19
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.
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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