Boosting hydrogen peroxide production via establishment and reconstruction of single-metal sites in covalent organic frameworks
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作者
Yang, Shuai; Lu, Lanlu; Li, Ji; Cheng, Qingqing; Mei, Bingbao; Li, Xuewen; Mao, Jianing; Qiao, Panzhe; Sun, Fanfei; Ma, Jingyuan; Xu, Qing; Jiang, Zheng
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刊物名称
SUSMAT
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年、卷、文献号
2023, 3, 2692-4552
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关键词
Yang, Shuai; Lu, Lanlu; Li, Ji; Cheng, Qingqing; Mei, Bingbao; Li, Xuewen; Mao, Jianing; Qiao, Panzhe; Sun, Fanfei; Ma, Jingyuan; Xu, Qing; Jiang, Zheng
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摘要
Covalent organic frameworks (COFs) have been well developed in electrocatalytic systems owing to their controllable skeletons, porosities, and functions. However, the catalytic process in COFs remains underexplored, hindering an in-depth understanding of the catalytic mechanism. In this work, uniform Pt-N1O1Cl4 sites chelated via C-N and C=O bonds along the one-dimensional and open channels of TP-TTA-COF were established. Different from conventional single-metal sites constructed for the near-free platinum for hydrogen evolution, the as-constructed PtCl-COF showed 2e(-) oxygen reduction for H2O2 production. We tracked the dynamic evolution process of atomic Pt sites in which Pt-N1O1Cl4 was transformed into Pt-N1O1(OH)(2) using in situ X-ray adsorption. The theoretical calculations revealed that the strong Pt-support interaction in Pt-N1O1(OH)(2) facilitated *OOH formation and thus led to higher selectivity and activity for the oxygen reduction reaction in the 2e(-) pathway. This work can expand the applications of COFs through the regulation of their local electronic states for the manipulation of the metal center.
