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具有氧空位的AuCu助催化剂与TiO协同集成用于CO高效光催化转化为CH₄ 。

Synergistic Integration of AuCu Co-Catalyst with Oxygen Vacancies on TiO for Efficient Photocatalytic Conversion of CO to CH.

作者信息

Jiang Deli, Zhou Yimeng, Zhang Qianxiao, Song Qi, Zhou Changjian, Shi Xiangli, Li Di

机构信息

School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.

Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang 212013, China.

出版信息

ACS Appl Mater Interfaces. 2021 Oct 6;13(39):46772-46782. doi: 10.1021/acsami.1c14371. Epub 2021 Sep 24.

Abstract

Photocatalytic reduction of CO toward eight-electron CH product with simultaneously high conversion efficiency and selectivity remains great challenging owing to the sluggish charge separation and transfer kinetics and lack of active sites for the adsorption and activation of reactants. Herein, a defective TiO nanosheet photocatalyst simultaneously equipped with AuCu alloy co-catalyst and oxygen vacancies (AuCu-TiO NSs) was rationally designed and fabricated for the selective conversion of CO into CH. The experimental results demonstrated that the AuCu alloy co-catalyst not only effectively promotes the separation of photogenerated electron-hole pairs but also acts as synergistic active sites for the reduction of CO. The oxygen vacancies in TiO contribute to the separation of charge carriers and, more importantly, promote the oxidation of HO, thus providing rich protons to promote the deep reduction of CO to CH. Consequently, the optimal AuCu-TiO nanosheets (NSs) photocatalyst achieves a CO reduction selectivity toward CH up to 90.55%, significantly higher than those of TiO NSs (31.82%), Au-TiO NSs (38.74%), and Cu-TiO NSs (66.11%). Furthermore, the CH evolution rate over the AuCu-TiO NSs reaches 22.47 μmol·g·h, which is nearly twice that of AuCu-TiO NSs (12.10 μmol·g·h). This research presents a unique insight into the design and synthesis of photocatalyst with oxygen vacancies and alloy metals as the co-catalyst for the highly selective deep reduction of CO.

摘要

将CO光催化还原为具有高转化效率和选择性的八电子CH产物仍然极具挑战性,这是由于电荷分离和转移动力学缓慢以及缺乏用于反应物吸附和活化的活性位点。在此,我们合理设计并制备了一种同时配备AuCu合金助催化剂和氧空位的缺陷TiO纳米片光催化剂(AuCu-TiO NSs),用于将CO选择性转化为CH。实验结果表明,AuCu合金助催化剂不仅有效地促进了光生电子-空穴对的分离,还作为还原CO的协同活性位点。TiO中的氧空位有助于电荷载流子的分离,更重要的是,促进了HO的氧化,从而提供丰富的质子以促进CO深度还原为CH。因此,最佳的AuCu-TiO纳米片(NSs)光催化剂对CH的CO还原选择性高达90.55%,显著高于TiO NSs(31.82%)、Au-TiO NSs(38.74%)和Cu-TiO NSs(66.11%)。此外,AuCu-TiO NSs上的CH析出速率达到22.47 μmol·g·h,几乎是AuCu-TiO NSs(12.10 μmol·g·h)的两倍。这项研究为设计和合成以氧空位和合金金属作为助催化剂用于CO高选择性深度还原的光催化剂提供了独特的见解。

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