CF-CuO/CeO2 的原位电化学重构以高效生成活性物质,Inorganic Chemistry

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CF-CuO/CeO2 的原位电化学重构以高效生成活性物质
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-06-02 , DOI: 10.1021/acs.inorgchem.2c01338
Xuliang Pang ₁ , Huaiquan Zhao ₁ , Yifei Huang ₁ , Youchao Liu ₁ , Hongye Bai ₁ , Weiqiang Fan ₁ , Weidong Shi ₁

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通过原位电化学重建实现本征活性已成为设计催化剂的巨大挑战。在此，提出了一种有效的电化学策略来重建 CF-CuO/CeO ₂前体的表面。在氧化/还原电位的刺激下，CF-CuO/CeO ₂表面成功生成了丰富的活性位点。值得注意的是，富氧空位CeO _{2的注入协同优化了CF-CuO/CeO}₂的化学组成和电子结构，极大地促进了活性物质的产生。系统的电化学实验表明，重构的 CF-CuO/CeO _{2具有优异的催化性能}可分别归因于CuOOH/CeO ₂和Cu ₂ O/Ce ₂ O ₃活性物质。氧化/还原活化的CF-CuO/CeO ₂进一步用于配对电池中，用于协同催化羟甲基糠醛氧化与4-硝基苯酚加氢。结果，在配对系统中实现了近 100% 的法拉第效率生产呋喃二甲酸/4-氨基苯酚（-0.9 V vs Ag/AgCl，1.5 h）。因此，通过氧化/还原活化的电化学重建已被证实是一种显着激发催化剂固有活性的可行方法。

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In Situ Electrochemical Reconstitution of CF–CuO/CeO2 for Efficient Active Species Generation

Achievement of the intrinsic activity by in situ electrochemical reconstruction has been becoming a great challenge for designing a catalyst. Herein, an effective electrochemical strategy is proposed to reconstruct the surface of the CF–CuO/CeO₂ precursor. Under the stimulation of oxidative/reductive potential, abundant active sites were successfully generated on the surface of CF–CuO/CeO₂. Remarkably, the implantation of oxygen vacancy-rich CeO₂ synergistically optimizes the chemical composition and electronic structure of CF–CuO/CeO₂, greatly promoting the generation of active species. Systematic electrochemical experiments indicate that the superior catalytic performance of reconstructed CF–CuO/CeO₂ could be attributed to CuOOH/CeO₂ and Cu₂O/Ce₂O₃ active species, respectively. The oxidative-/reductive-activated CF–CuO/CeO₂ was further employed in a paired cell for the synergistic catalysis of hydroxymethylfurfural oxidation with 4-nitrophenol hydrogenation. As a result, nearly 100% Faraday efficiency for furandicarboxylic acid/4-aminophenol production was achieved in the paired system (−0.9 V vs Ag/AgCl, 1.5 h). Therefore, the electrochemical reconstruction via oxidative/reductive activation has been confirmed as a feasible approach to significantly excite the intrinsic activity of a catalyst.

更新日期：2022-06-02

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