通过增强 Cu-O 杂化抑制 Cu2O 的晶格氧，通过 CO2 电还原选择性稳定生产乙烯,Journal of Materials Chemistry A

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通过增强 Cu-O 杂化抑制 Cu2O 的晶格氧，通过 CO2 电还原选择性稳定生产乙烯
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-09-02 , DOI: 10.1039/d2ta05565a
Yebo Yao ₁ , Yixiang Zhou ₁ , Xia Liu ₁ , Yongjia Li ₁ , Dewei Wang ₁ , Xinyue Chi ₁ , Xiaoxuan Wang ₁ , Rui Zhao ₁ , Huiying Zhang ₁ , Yanfei Sun ₁ , Zhi-Yu Yang ₁ , Ying Wei ₁ , Yi-Ming Yan ₁

Affiliation

_{开发用于将 CO 2} (CO ₂ RR) 电化学还原为增值化工产品的高选择性和高效催化剂是实现零排放和碳中和的有希望的途径。Cu _{2 O催化剂因其在CO}₂ RR过程中增强C-C偶联的独特能力而受到广泛关注，但它仍然存在失活快和选择性差的问题。在此，我们设计了一种简单而有效的策略，通过将硼 (B) 结合到 Cu ₂ O 晶格中，成功地将活性 Cu ⁺物质稳定在高还原电位下。氧气程序升温脱附（O ₂-TPD）和理论计算证实，B掺杂有效地抑制了Cu ₂ O的晶格氧，从而加强了Cu-O键。生成的 B 掺杂 Cu ₂ O 基本上抑制了长期电解下Cu ⁺物质的还原，在 -1.2 V 下实现了至少 8 小时的 CO ₂到 C ₂ H ₄的有效生产。重要的是，我们使用了原位和非原位光谱表征研究以追踪 CO ₂ RR 过程中铜价的演变，从而确定受约束的氧晶格在稳定Cu _{2的活性 Cu}⁺中心中的作用O 催化剂。_{这项工作提供了对 Cu 2 O 催化剂的 Cu}⁺依赖性催化性能的深入理解，并为设计用于 CO ₂ RR的高效电催化剂铺平了道路。

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Restraining lattice oxygen of Cu2O by enhanced Cu–O hybridization for selective and stable production of ethylene with CO2 electroreduction

The development of highly selective and efficient catalysts for the electrochemical reduction of CO₂ (CO₂RR) to value-added chemical products is a promising pathway towards zero emissions and carbon neutrality. Cu₂O catalyst has received substantial attention due to its distinct capabilities of enhancing the C–C coupling during the CO₂RR, while it still suffers from fast deactivation and poor selectivity. Herein, we design a simple yet efficient strategy to successfully stabilize the active Cu⁺ species at highly applied reducing potential via incorporating boron (B) into the Cu₂O lattice. Oxygen temperature-programmed desorption (O₂-TPD) and theoretical calculations confirm that the B-doping effectively restrains the lattice oxygen of Cu₂O, which consequently strengthens the Cu–O bonds. The resultant B-doped Cu₂O substantially suppresses the reduction of Cu⁺ species under long-term electrolysis, achieving an efficient production of CO₂-to-C₂H₄ for at least 8 h at −1.2 V. Importantly, we used in situ and ex-situ spectroscopic characterization studies to trace the evolution of copper valence during the CO₂RR, thus identifying the role of the restrained oxygen lattice in stabilizing the active Cu⁺ centers of the Cu₂O catalyst. This work provides a deep understanding of the Cu⁺ dependent catalytic performance of the Cu₂O catalyst, and paves a novel way to design high-efficiency electrocatalysts for the CO₂RR.

更新日期：2022-09-02

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