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Origin of the Improved Photoelectrochemical and Photocatalytic Activity in a ZnO-TiO2 Nanohybrid Revealed by Experimental and Density Functional Theory Studies
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-07-18 , DOI: 10.1021/acs.jpclett.4c01641 Abinash Das 1 , Dongyu Liu 2 , Yifan Wu 3 , Bayan Amer Abzakh 2 , Madhumitha R 1 , Preethi M 1 , Elena A Kazakova 4 , Andrey S Vasenko 2, 5 , Oleg V Prezhdo 3, 6
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-07-18 , DOI: 10.1021/acs.jpclett.4c01641 Abinash Das 1 , Dongyu Liu 2 , Yifan Wu 3 , Bayan Amer Abzakh 2 , Madhumitha R 1 , Preethi M 1 , Elena A Kazakova 4 , Andrey S Vasenko 2, 5 , Oleg V Prezhdo 3, 6
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Heterojunctions of metal oxides have attracted a great deal of attention as photo (electro) catalysts owing to their excellent photoactivity. While multiple fundamental studies have been dedicated to heteroaggregation, self-assembly of oppositely charged particles to obtain heterojunctions for energy applications has been underexplored. Herein, we report the synthesis of ZnO-TiO2 heterojunctions using the electrostatic self-assembly approach. The synthesized ZnO-TiO2 heterojunctions were characterized by using multiple experimental techniques. Density functional theory calculations were conducted to establish the heterojunction formation mechanism and electronic properties. The ZnO-TiO2 nanohybrid was tested for the photodegradation of rhodamine B dye and water splitting applications. The photocatalytic performance of the ZnO-TiO2 nanohybrid is 3.5 times higher than that of bare ZnO. In addition, the heterostructure exhibited an excellent photocurrent density of 2.4 mA cm–2 at a low onset potential during photoelectrochemical oxygen evolution. The performance improvements are attributed to the formation of the type II heterojunction between ZnO and TiO2, which suppresses carrier recombination and enhances carrier transport, boosting the catalytic activity.
中文翻译：
实验和密度泛函理论研究揭示了 ZnO-TiO2 纳米杂化物光电化学和光催化活性提高的根源
金属氧化物异质结作为光（电）催化剂因其优异的光活性而受到广泛关注。虽然多项基础研究致力于异质聚集，但带相反电荷的粒子自组装以获得用于能源应用的异质结的研究尚未充分。在此，我们报道了使用静电自组装方法合成ZnO-TiO 2异质结。通过使用多种实验技术对合成的ZnO-TiO 2异质结进行了表征。进行密度泛函理论计算以确定异质结形成机制和电子特性。测试了 ZnO-TiO 2纳米杂化物的罗丹明 B 染料的光降解和水分解应用。 ZnO-TiO 2纳米杂化物的光催化性能比裸ZnO高3.5倍。此外，该异质结构在光电化学析氧过程中在低起始电位下表现出2.4 mA cm –2的优异光电流密度。性能的提高归因于ZnO和TiO 2之间形成II型异质结，抑制载流子复合并增强载流子传输，从而提高催化活性。
更新日期：2024-07-18
中文翻译：
实验和密度泛函理论研究揭示了 ZnO-TiO2 纳米杂化物光电化学和光催化活性提高的根源
金属氧化物异质结作为光（电）催化剂因其优异的光活性而受到广泛关注。虽然多项基础研究致力于异质聚集，但带相反电荷的粒子自组装以获得用于能源应用的异质结的研究尚未充分。在此，我们报道了使用静电自组装方法合成ZnO-TiO 2异质结。通过使用多种实验技术对合成的ZnO-TiO 2异质结进行了表征。进行密度泛函理论计算以确定异质结形成机制和电子特性。测试了 ZnO-TiO 2纳米杂化物的罗丹明 B 染料的光降解和水分解应用。 ZnO-TiO 2纳米杂化物的光催化性能比裸ZnO高3.5倍。此外，该异质结构在光电化学析氧过程中在低起始电位下表现出2.4 mA cm –2的优异光电流密度。性能的提高归因于ZnO和TiO 2之间形成II型异质结，抑制载流子复合并增强载流子传输，从而提高催化活性。
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