Bi4Ti3O12纳米片表面有意引入氧空位和Ti3+缺陷促进CO2光还原为CH3OH,ACS Applied Nano Materials

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Bi4Ti3O12纳米片表面有意引入氧空位和Ti3+缺陷促进CO2光还原为CH3OH
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2024-01-29 , DOI: 10.1021/acsanm.3c05346
Yuxuan Wang ₁ , Chenhui Qiu ₁ , Yujing Xie ₁ , Lei Wang ₁ , Jing Ding ₁ , Jinfeng Zhang ₂ , Hui Wan ₁ , Guofeng Guan ₁

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利用钙钛矿光催化还原CO ₂和H ₂ O生产碳氢化合物燃料为解决能源危机和温室效应提供了一种有吸引力的方法。 Bi ₄ Ti ₃ O ₁₂ (BTO)因其独特的层状结构而在光催化领域备受关注，但仍面临着光响应弱、光生载流子复合严重等诸多挑战。本文采用熔盐法和NaBH ₄高温还原法(HBTO)制备了具有不同浓度表面氧空位(V _O )和Ti ^{3+缺陷的Bi}₄ Ti ₃ O ₁₂纳米片。表面缺陷在HBTO表面形成明显的载流子陷阱，降低了光生电子和空穴的复合率，并调整了带隙结构（从3.09 eV到2.62 eV），提高了HBTO的可见光利用率。光致载流子复合率的降低和可见光响应的提高显着增强了HBTO在可见光下的光催化CO ₂还原活性。优化后的HBTO-4（NaBH ₄ :Bi ₄ Ti ₃ O ₁₂ = 1:5）的CH ₃ OH产率为4.90 μmol·g ^–1 ·h ^–1，约为原始BTO的3.5倍。同时，通过密度泛函理论（DFT）计算了带隙结构、电子态密度（DOS）和功函数。该研究为设计和制备富含表面缺陷的钙钛矿光催化剂以实现太阳能的高效转换提供了有效的策略。

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Intentionally Introducing Oxygen Vacancies and Ti3+ Defects on the Surface of Bi4Ti3O12 Nanosheets for Promoting the Photoreduction of CO2 to CH3OH

Using perovskite photocatalytic reduction of CO₂ and H₂O to produce hydrocarbon fuels offers an attractive method to solve the energy crisis and the greenhouse effect. Bi₄Ti₃O₁₂ (BTO) has received much attention in the field of photocatalysis due to its unique layered structure, but it still faces many challenges such as weak photoresponse and severe photogenerated carrier recombination. In this paper, Bi₄Ti₃O₁₂ nanosheets with different concentrations of surface oxygen vacancies (V_O) and Ti³⁺ defect were prepared by the molten salt method and NaBH₄ high-temperature reduction method (HBTO). Surface defects formed obvious carrier traps on the HBTO surface, reduced the recombination rate of photogenerated electrons and holes, and adjusted the band gap structure (from 3.09 to 2.62 eV), which improved the visible light utilization of HBTO. The decrease of photoinduced carrier recombination rate and the improvement of visible light response significantly enhanced the photocatalytic CO₂ reduction activity of HBTO under visible light. The CH₃OH yield with the optimized HBTO-4 (NaBH₄:Bi₄Ti₃O₁₂ = 1:5) was 4.90 μmol·g^–1·h^–1, which was about 3.5 times that of the original BTO. Meanwhile, the band gap structure, electronic density of states (DOS), and work function were calculated by the density functional theory (DFT). This study provided an effective strategy for designing and preparing perovskite photocatalysts rich in surface defects for the efficient conversion of solar energy.

更新日期：2024-01-29

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