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La,Al-Codoped SrTiO3 as a Photocatalyst in Overall Water Splitting: Significant Surface Engineering Effects on Defect Engineering
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-08-31 , DOI: 10.1021/acscatal.1c02874 Yalei Qin 1 , Fan Fang 1 , Zhengzheng Xie 1 , Huiwen Lin 1 , Kai Zhang 2 , Xu Yu 3 , Kun Chang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-08-31 , DOI: 10.1021/acscatal.1c02874 Yalei Qin 1 , Fan Fang 1 , Zhengzheng Xie 1 , Huiwen Lin 1 , Kai Zhang 2 , Xu Yu 3 , Kun Chang 1
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Suppressing the formation of defects such as oxygen vacancies and Ti3+ in SrTiO3 perovskite lattice has been regarded as an effective way to improve photocatalytic performance in overall water-splitting reaction. In this work, a series of La,Al-codoped SrTiO3 catalysts are synthesized by a flux treatment method after grounding. An appropriate doping amount of La3+ and Al3+ ions into perovskite will lead to fewer defects, responsible for enhancing photocatalytic performance. Al3+ ion doping will introduce the oxygen vacancies into the perovskite, resulting in a decreasing number of Ti3+ ions. During the defect engineering, more Sr2+ will precipitate onto the perovskite surface caused by the introduction of Al3+. Hence, surface engineering is applied through appropriate La3+ ion doping contributing to the lattice distortion, allowing surficial Sr2+ to re-enter the perovskite lattice, leading to the promoted conversion of Ti3+ to Ti4+. Simultaneously, the La3+ ion doping is also beneficial to the decrease in oxygen vacancies. As a result, the essential relationship between the La3+ doping amount and photocatalytic performance in overall water splitting is revealed. The optimized 0.6% La and 1% Al codoped SrTiO3 sample loading Rh (0.1 wt %)/Cr2O3 (0.05 wt %)/CoOOH (0.05 wt %) gives the highest activity and good stability, with gas evolution rates of 1.79 mmol·h–1 (H2) and 0.91 mmol·h–1 (O2). In comparison, the apparent quantum efficiency is 78.43% under 365 nm irradiation.
中文翻译：
La,Al 共掺杂 SrTiO3 作为光催化剂在整体水分解中：表面工程对缺陷工程的显着影响
抑制SrTiO 3钙钛矿晶格中氧空位和Ti 3+等缺陷的形成被认为是提高整体水分解反应光催化性能的有效途径。在这项工作中，通过接地后的助熔剂处理方法合成了一系列La,Al 共掺杂的SrTiO 3催化剂。将适量的 La 3+和 Al 3+离子掺杂到钙钛矿中会减少缺陷，从而提高光催化性能。Al 3+离子掺杂将氧空位引入钙钛矿，导致Ti 3+离子数量减少。在缺陷工程中，更多的 Sr 2+由于引入了 Al 3+ ，将沉淀到钙钛矿表面。因此，通过适当的 La 3+离子掺杂来应用表面工程，有助于晶格畸变，使表面 Sr 2+重新进入钙钛矿晶格，从而促进 Ti 3+向 Ti 4+ 的转化。同时，La 3+离子掺杂也有利于氧空位的减少。结果，揭示了La 3+掺杂量与整体水分解中的光催化性能之间的本质关系。优化的 0.6% La 和 1% Al 共掺杂 SrTiO 3样品负载 Rh (0.1 wt %)/Cr 2O 3 (0.05 wt %)/CoOOH (0.05 wt %) 具有最高的活性和良好的稳定性，放气速率为 1.79 mmol·h –1 (H 2 ) 和 0.91 mmol·h –1 (O 2 )。相比之下，在 365 nm 照射下的表观量子效率为 78.43%。
更新日期：2021-09-17
中文翻译：
La,Al 共掺杂 SrTiO3 作为光催化剂在整体水分解中：表面工程对缺陷工程的显着影响
抑制SrTiO 3钙钛矿晶格中氧空位和Ti 3+等缺陷的形成被认为是提高整体水分解反应光催化性能的有效途径。在这项工作中，通过接地后的助熔剂处理方法合成了一系列La,Al 共掺杂的SrTiO 3催化剂。将适量的 La 3+和 Al 3+离子掺杂到钙钛矿中会减少缺陷，从而提高光催化性能。Al 3+离子掺杂将氧空位引入钙钛矿，导致Ti 3+离子数量减少。在缺陷工程中，更多的 Sr 2+由于引入了 Al 3+ ，将沉淀到钙钛矿表面。因此，通过适当的 La 3+离子掺杂来应用表面工程，有助于晶格畸变，使表面 Sr 2+重新进入钙钛矿晶格，从而促进 Ti 3+向 Ti 4+ 的转化。同时，La 3+离子掺杂也有利于氧空位的减少。结果，揭示了La 3+掺杂量与整体水分解中的光催化性能之间的本质关系。优化的 0.6% La 和 1% Al 共掺杂 SrTiO 3样品负载 Rh (0.1 wt %)/Cr 2O 3 (0.05 wt %)/CoOOH (0.05 wt %) 具有最高的活性和良好的稳定性，放气速率为 1.79 mmol·h –1 (H 2 ) 和 0.91 mmol·h –1 (O 2 )。相比之下，在 365 nm 照射下的表观量子效率为 78.43%。
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