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Insight of the State for Deliberately Introduced A-Site Defect in Nanofibrous LaFeO3 for Boosting Artificial Photosynthesis of CH3OH
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-11-09 , DOI: 10.1021/acsami.3c11562 Chenhui Qiu 1 , Lei Wang 1 , Ruijie Chen 1 , Jie Zhang 1 , Jing Ding 1 , Jinfeng Zhang 2 , Hui Wan 1 , Guofeng Guan 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-11-09 , DOI: 10.1021/acsami.3c11562 Chenhui Qiu 1 , Lei Wang 1 , Ruijie Chen 1 , Jie Zhang 1 , Jing Ding 1 , Jinfeng Zhang 2 , Hui Wan 1 , Guofeng Guan 1
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Perovskite-type LaFeO3 is regarded as a potentially efficient visible-light photocatalyst owing to its narrow bandgap energy and unique photovoltaic properties. However, the insufficient active sites and the unsatisfactory utilization of photogenerated carriers severely restrict the realistic application of pure LaFeO3. Herein, we fabricated a series of LaxFeO3−δ nanofibers (x = 1.0, 0.95, 0.9, 0.85, 0.8) with an A-site defect via sol–gel combined with the electrospinning technique. Wherein, the nonstoichiometric La0.9FeO3−δ possessed the highest CH3OH yield of 5.30 μmol·g–1·h–1 with good chemical stability. A series of advanced characterizations were applied to investigate the physicochemical properties and charge-carrier behaviors of the samples. The results illustrated that the one-dimensional (1D) nanostructures combined with the appropriate concentration of vacancy defects on the surface contributed to the radial migration of photogenerated carriers, inhibited the recombination of carriers, and provided more CO2 adsorption-activation sites. Furthermore, density functional theory (DFT) calculations were employed to reveal the influence mechanism of vacancy defects on LaFeO3. This work provides a strategy to enhance the performance of photocatalytic CO2 reduction by modulating the induced oxygen vacancies caused by the A-site defect in perovskite oxides.
中文翻译：
国家对在纳米纤维 LaFeO3 中故意引入 A 位缺陷以促进 CH3OH 人工光合作用的见解
钙钛矿型LaFeO 3由于其窄带隙能量和独特的光伏特性而被认为是一种潜在高效的可见光光催化剂。然而，活性位点不足和光生载流子利用率不理想严重限制了纯LaFeO 3的实际应用。在此，我们通过溶胶-凝胶结合静电纺丝技术制备了一系列具有A位缺陷的La x FeO 3−δ纳米纤维（x = 1.0, 0.95, 0.9, 0.85, 0.8）。其中，非化学计量的La 0.9 FeO 3−δ的CH 3 OH产率最高，为5.30 μmol·g –1 ·h –1，且化学稳定性良好。应用一系列先进的表征来研究样品的物理化学性质和载流子行为。结果表明，一维（1D）纳米结构与表面适当浓度的空位缺陷相结合，有助于光生载流子的径向迁移，抑制载流子的复合，并提供更多的CO 2吸附活化位点。此外，采用密度泛函理论（DFT）计算揭示了空位缺陷对LaFeO 3的影响机制。这项工作提供了一种通过调节钙钛矿氧化物中A位缺陷引起的诱导氧空位来增强光催化CO 2还原性能的策略。
更新日期：2023-11-09
中文翻译：
国家对在纳米纤维 LaFeO3 中故意引入 A 位缺陷以促进 CH3OH 人工光合作用的见解
钙钛矿型LaFeO 3由于其窄带隙能量和独特的光伏特性而被认为是一种潜在高效的可见光光催化剂。然而，活性位点不足和光生载流子利用率不理想严重限制了纯LaFeO 3的实际应用。在此，我们通过溶胶-凝胶结合静电纺丝技术制备了一系列具有A位缺陷的La x FeO 3−δ纳米纤维（x = 1.0, 0.95, 0.9, 0.85, 0.8）。其中，非化学计量的La 0.9 FeO 3−δ的CH 3 OH产率最高，为5.30 μmol·g –1 ·h –1，且化学稳定性良好。应用一系列先进的表征来研究样品的物理化学性质和载流子行为。结果表明，一维（1D）纳米结构与表面适当浓度的空位缺陷相结合，有助于光生载流子的径向迁移，抑制载流子的复合，并提供更多的CO 2吸附活化位点。此外，采用密度泛函理论（DFT）计算揭示了空位缺陷对LaFeO 3的影响机制。这项工作提供了一种通过调节钙钛矿氧化物中A位缺陷引起的诱导氧空位来增强光催化CO 2还原性能的策略。
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