Synergistic Integration of AuCu Co-Catalyst with Oxygen Vacancies on TiO2 for Efficient Photocatalytic Conversion of CO2 to CH4,ACS Applied Materials & Interfaces

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Synergistic Integration of AuCu Co-Catalyst with Oxygen Vacancies on TiO2 for Efficient Photocatalytic Conversion of CO2 to CH4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-09-24 , DOI: 10.1021/acsami.1c14371
Deli Jiang ₁ , Yimeng Zhou ₁ , Qianxiao Zhang ₁ , Qi Song ₁ , Changjian Zhou ₂ , Xiangli Shi ₂ , Di Li ₂

Affiliation

Photocatalytic reduction of CO₂ toward eight-electron CH₄ 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 TiO₂ nanosheet photocatalyst simultaneously equipped with AuCu alloy co-catalyst and oxygen vacancies (AuCu-TiO_2–x NSs) was rationally designed and fabricated for the selective conversion of CO₂ into CH₄. 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 CO₂. The oxygen vacancies in TiO₂ contribute to the separation of charge carriers and, more importantly, promote the oxidation of H₂O, thus providing rich protons to promote the deep reduction of CO₂ to CH₄. Consequently, the optimal AuCu-TiO_2–x nanosheets (NSs) photocatalyst achieves a CO₂ reduction selectivity toward CH₄ up to 90.55%, significantly higher than those of TiO_2–x NSs (31.82%), Au-TiO_2–x NSs (38.74%), and Cu-TiO_2–x NSs (66.11%). Furthermore, the CH₄ evolution rate over the AuCu-TiO_2–x NSs reaches 22.47 μmol·g^–1·h^–1, which is nearly twice that of AuCu-TiO₂ NSs (12.10 μmol·g^–1·h^–1). 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 CO₂.

中文翻译：

AuCu 助催化剂与 TiO2 上的氧空位协同整合，以实现 CO2 到 CH4 的高效光催化转化

由于缓慢的电荷分离和转移动力学以及缺乏用于吸附和活化反应物的活性位点，将CO ₂光催化还原为八电子 CH ₄产物并同时具有高转化效率和选择性仍然具有很大的挑战性。在此，合理设计和制造了同时配备 AuCu 合金助催化剂和氧空位的缺陷 TiO ₂纳米片光催化剂（AuCu-TiO _{2– x} NSs），用于将 CO ₂选择性转化为 CH ₄. 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，而且还充当了还原 CO _{2 的}协同活性位点。TiO _{2 中}的氧空位有助于电荷载流子的分离，更重要的是促进H ₂ O的氧化，从而提供丰富的质子以促进CO ₂深度还原为CH ₄。因此，最佳的AuCu-TiO _{2– x}纳米片（NSs）光催化剂对CH ₄的CO ₂还原选择性高达90.55%，明显高于TiO _2–_xNSs (31.82%)、Au-TiO _{2– x} NSs (38.74%) 和 Cu-TiO _{2– x} NSs (66.11%)。此外，AuCu-TiO _2–_x NSs 上的 CH ₄析出速率达到 22.47 μmol·g ^–1 ·h ^–1，几乎是 AuCu-TiO ₂ NSs (12.10 μmol·g ^–1 ·h ^–1）。这项研究对设计和合成具有氧空位和合金金属的光催化剂作为高选择性深度还原 CO ₂的助催化剂提出了独特的见解。

更新日期：2021-10-06

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