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S-Scheme-Heterojunction LaNiO3/CdLa2S4 Photocatalyst for Solar-Driven CO2-to-CO Conversion
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-05-09 , DOI: 10.1021/acsanm.3c01443 Jiwu Zhao 1 , Fengkai Liu 1 , Wenjing Wang 1 , Ying Wang 1 , Na Wen 1, 2 , Zizhong Zhang 1 , Wenxin Dai 1 , Rusheng Yuan 1 , Zhengxin Ding 1 , Jinlin Long 1
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-05-09 , DOI: 10.1021/acsanm.3c01443 Jiwu Zhao 1 , Fengkai Liu 1 , Wenjing Wang 1 , Ying Wang 1 , Na Wen 1, 2 , Zizhong Zhang 1 , Wenxin Dai 1 , Rusheng Yuan 1 , Zhengxin Ding 1 , Jinlin Long 1
Affiliation
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Visible-light-driven semiconductor-catalyzed CO2 conversion into valuable chemicals and industrial feedstocks is one of the superior pathways to address the excess carbon emissions and energy shortages. Herein, an innovative step-scheme (S-scheme) heterojunction assembled from bulk CdLa2S4 and surface rare-earth perovskite-type oxide LaNiO3 with precisely engineered suitable band alignment is employed for the selective photocatalytic conversion of CO2 to CO. The optimized 8%-LaNiO3/CdLa2S4 photocatalyst exhibits an outstanding CO output of up to 102.43 μmol h–1 with a selectivity of about 83.4%, rivaling all of the similar incumbent photocatalytic reaction systems for CO2-to-CO conversion. It highlights the effectiveness of the S-scheme heterojunction LaNiO3/CdLa2S4 in hindering the recombination of the photogenerated electron–hole pairs. Meanwhile, a remarkable apparent quantum efficiency (AQE) of as high as 6.76% is achieved, as well as the CO output is still maintained at 99.5% of the initial value after five cycle tests, revealing the superior repeatability and reliability of the 8%-LaNiO3/CdLa2S4 photocatalyst for solar-to-chemical conversion. In addition, an experimentally verified band alignment-boosted reaction mechanism is proposed. This study highlights the construction of structurally flexible and highly designable S-scheme heterojunctions, demonstrating potential application in carbon-negative energy conversion.
中文翻译：
S型异质结LaNiO3/CdLa2S4光催化剂用于太阳能驱动的CO2-to-CO转化
可见光驱动的半导体催化CO 2转化为有价值的化学品和工业原料是解决过度碳排放和能源短缺的最佳途径之一。在此，一种由块状 CdLa 2 S 4和表面稀土钙钛矿型氧化物 LaNiO 3组装而成的创新阶梯式（S 式）异质结具有精确设计的合适的能带排列，用于将 CO 2选择性光催化转化为 CO。优化的 8%-LaNiO 3 /CdLa 2 S 4光催化剂表现出高达 102.43 μmol h –1的出色 CO 输出具有约 83.4% 的选择性，可与所有类似的现有光催化反应系统相媲美，用于 CO 2到 CO 的转化。它突出了 S 型异质结 LaNiO 3 /CdLa 2 S 4在阻碍光生电子-空穴对复合方面的有效性。同时，实现了高达6.76%的显着表观量子效率（AQE），并且经过五次循环测试，CO输出仍保持在初始值的99.5%，显示出8%的卓越重复性和可靠性-LaNiO 3 /CdLa 2 S 4用于太阳能-化学转化的光催化剂。此外，还提出了一种经过实验验证的带对齐增强反应机制。本研究重点介绍了结构灵活且高度可设计的 S 型异质结的构建，展示了在碳-负能量转换中的潜在应用。
更新日期：2023-05-09
中文翻译：
S型异质结LaNiO3/CdLa2S4光催化剂用于太阳能驱动的CO2-to-CO转化
可见光驱动的半导体催化CO 2转化为有价值的化学品和工业原料是解决过度碳排放和能源短缺的最佳途径之一。在此，一种由块状 CdLa 2 S 4和表面稀土钙钛矿型氧化物 LaNiO 3组装而成的创新阶梯式（S 式）异质结具有精确设计的合适的能带排列，用于将 CO 2选择性光催化转化为 CO。优化的 8%-LaNiO 3 /CdLa 2 S 4光催化剂表现出高达 102.43 μmol h –1的出色 CO 输出具有约 83.4% 的选择性，可与所有类似的现有光催化反应系统相媲美，用于 CO 2到 CO 的转化。它突出了 S 型异质结 LaNiO 3 /CdLa 2 S 4在阻碍光生电子-空穴对复合方面的有效性。同时，实现了高达6.76%的显着表观量子效率（AQE），并且经过五次循环测试，CO输出仍保持在初始值的99.5%，显示出8%的卓越重复性和可靠性-LaNiO 3 /CdLa 2 S 4用于太阳能-化学转化的光催化剂。此外，还提出了一种经过实验验证的带对齐增强反应机制。本研究重点介绍了结构灵活且高度可设计的 S 型异质结的构建，展示了在碳-负能量转换中的潜在应用。
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