期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 334, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.122851
关键词
Dual active sites; Rearrangement of electrons; Site distance effect; Driving effect; Electrocatalytic reduction of As(III)
In the field of electrocatalytic reduction, single atom catalysts (SACs) have been extensively researched. However, the metal active sites are easily weakened or poisoned during complex multi-step proton-electron reactions. Therefore, it remains a great challenge to improve the adsorption-desorption capacity and enhance rapid surface reactions for superior electrocatalytic performance. In this study, the electron synergism of neighbouring Fe and Co diatoms on graphene (FeCoN6-Gra) was found to promote the electrocatalytic reduction of arsenious acid (As(III)), surpassing single-atomic catalysts containing only Fe or Co. The electron allocation mechanism associated with Co injection was observed to trigger two-site adsorption and efficiently regulate electron transport between surface sites and As(III). Furthermore, the dynamic migration of As(III) driven by Co during the reduction process was emphasized, playing a crucial role in breaking the As-O bond and achieving efficient catalysis of the diatomic model.
Single atom catalysts (SACs) have been widely studied in the field of electrocatalytic reduction, but in the complex multi-step proton-electron reactions, the metal active site is easy to be weakened or even poisoned. Therefore, how to improve the adsorption-desorption capacity and rapid surface reaction to obtain superior electrocatalytic performance remains a great challenge. We indicate the electron synergism of neighbouring Fe and Co diatoms on graphene (FeCoN6-Gra) to promote the electrocatalytic reduction of arsenious acid (As(III)), which is superior to single-atomic catalysts containing only Fe or Co. It is found that the new electron allocation mechanism associated with the injection of Co is beneficial to trigger the two-site adsorption and effectively regulate electron transport between surface sites and As(III). Moreover, the dynamic migration of As(III) driven by Co atom during the reduction process is emphasized, which contributes to break the As-O bond, thus achieving efficient catalysis of the diatomic model.
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