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Oxygen Vacancy-Mediated Z-Scheme Charge Transfer in a 2D/1D B-Doped g-C3N4/rGO/TiO2 Heterojunction Visible Light-Driven Photocatalyst for Simultaneous/Efficient Oxygen Reduction Reaction and Alcohol Oxidation
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-08-01 , DOI: 10.1021/acs.inorgchem.2c01899
Arjun Behera 1 , Ashish Kumar Kar 1 , Rajendra Srivastava 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-08-01 , DOI: 10.1021/acs.inorgchem.2c01899
Arjun Behera 1 , Ashish Kumar Kar 1 , Rajendra Srivastava 1
Affiliation
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Hydrogen peroxide (H2O2) is a powerful oxidant that directly or indirectly oxidizes many organic and inorganic contaminants. The photocatalytic generation of H2O2 is achieved by using a semiconductor photocatalyst in the presence of alcohol as a proton source. Herein, we have synthesized oxygen vacancy (Ov)-mediated TiO2/B-doped g-C3N4/rGO (TBCN@rGO) ternary heterostructures by a simple hydrothermal technique. Several characterization techniques were employed to explore the existence of oxygen vacancies in the crystal structure and investigate their impact on the optoelectronic properties of the catalyst. Oxygen vacancies offered additional sites for adsorbing molecular oxygen, activating alcohols, and facilitating electron migration from TBCN@rGO to the surface-adsorbed O2. The defect creation (oxygen vacancy) and Z-scheme mechanistic pathways create a suitable platform for generating H2O2 by two-electron reduction processes. The optimized catalyst showed the highest photocatalytic H2O2 evolution rate of 172 μmol/h, which is 1.9 and 2.5 times greater than that of TBCN and BCN, respectively. The photocatalytic oxidation of various lignocellulose-derived alcohols (such as furfural alcohol and vanillyl alcohol) and benzyl alcohol was also achieved. Photocatalytic activity data, physicochemical and optoelectronic features, and trapping experiments were conducted to elucidate the structure–activity relationships. The TBCN@rGO acts as a multifunctional Z-scheme photocatalyst having an oxygen vacancy, modulates surface acidity–basicity required for the adsorption and activation of the reactant molecules, and displays excellent photocatalytic performance due to the formation of a large number of active surface sites, increased electrical conductivity, improved charge transfer properties, outstanding photostability, and reusability. The present study establishes a unique strategy for improving H2O2 generation and alcohol oxidation activity and also provides insights into the significance of a surface vacancy in the semiconductor photocatalyst.
中文翻译：
2D/1D B 掺杂 g-C3N4/rGO/TiO2 异质结可见光驱动光催化剂中氧空位介导的 Z 型电荷转移用于同时/高效的氧还原反应和醇氧化
过氧化氢 (H 2 O 2 ) 是一种强氧化剂，可直接或间接氧化许多有机和无机污染物。H 2 O 2的光催化产生是通过在醇作为质子源的存在下使用半导体光催化剂来实现的。在此，我们合成了氧空位（O v）介导的 TiO 2 /B 掺杂 gC 3 N 4/rGO (TBCN@rGO) 三元异质结构通过简单的水热技术。采用几种表征技术来探索晶体结构中氧空位的存在，并研究它们对催化剂光电性能的影响。氧空位为吸附分子氧、活化醇和促进电子从 TBCN@rGO 迁移到表面吸附的 O 2提供了额外的位点。缺陷产生（氧空位）和Z-方案机制途径为通过双电子还原过程产生H 2 O 2创建了合适的平台。优化后的催化剂表现出最高的光催化 H 2 O 2析出速率为 172 μmol/h，分别是 TBCN 和 BCN 的 1.9 倍和 2.5 倍。还实现了各种木质纤维素衍生醇（如糠醛醇和香草醇）和苯甲醇的光催化氧化。进行了光催化活性数据、物理化学和光电特性以及捕获实验以阐明结构-活性关系。TBCN@rGO 充当多功能Z-具有氧空位的方案光催化剂，调节反应物分子吸附和活化所需的表面酸碱度，并由于形成大量活性表面位点、增加电导率、改善电荷转移性能而显示出优异的光催化性能，出色的光稳定性和可重复使用性。本研究建立了一种独特的策略来提高 H 2 O 2的生成和醇氧化活性，并为半导体光催化剂中表面空位的重要性提供了见解。
更新日期：2022-08-01
中文翻译：
2D/1D B 掺杂 g-C3N4/rGO/TiO2 异质结可见光驱动光催化剂中氧空位介导的 Z 型电荷转移用于同时/高效的氧还原反应和醇氧化
过氧化氢 (H 2 O 2 ) 是一种强氧化剂，可直接或间接氧化许多有机和无机污染物。H 2 O 2的光催化产生是通过在醇作为质子源的存在下使用半导体光催化剂来实现的。在此，我们合成了氧空位（O v）介导的 TiO 2 /B 掺杂 gC 3 N 4/rGO (TBCN@rGO) 三元异质结构通过简单的水热技术。采用几种表征技术来探索晶体结构中氧空位的存在，并研究它们对催化剂光电性能的影响。氧空位为吸附分子氧、活化醇和促进电子从 TBCN@rGO 迁移到表面吸附的 O 2提供了额外的位点。缺陷产生（氧空位）和Z-方案机制途径为通过双电子还原过程产生H 2 O 2创建了合适的平台。优化后的催化剂表现出最高的光催化 H 2 O 2析出速率为 172 μmol/h，分别是 TBCN 和 BCN 的 1.9 倍和 2.5 倍。还实现了各种木质纤维素衍生醇（如糠醛醇和香草醇）和苯甲醇的光催化氧化。进行了光催化活性数据、物理化学和光电特性以及捕获实验以阐明结构-活性关系。TBCN@rGO 充当多功能Z-具有氧空位的方案光催化剂，调节反应物分子吸附和活化所需的表面酸碱度，并由于形成大量活性表面位点、增加电导率、改善电荷转移性能而显示出优异的光催化性能，出色的光稳定性和可重复使用性。本研究建立了一种独特的策略来提高 H 2 O 2的生成和醇氧化活性，并为半导体光催化剂中表面空位的重要性提供了见解。
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