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Facile and robust construction of a 3D-hierarchical NaNbO3-nanorod/ZnIn2S4 heterojunction towards ultra-high photocatalytic H2 production

机译:3D等级NANBO3-NANOROD/ZNIN2S4异质结的功能和强大的构造朝向超高光催化H2生产

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It is imperative but still challenging to develop heterojunction photocatalysts for efficient interfacial charge carrier separation in photocatalytic hydrogen evolution (PHE) reactions. Encouragingly, in this work, we constructed a 3D hierarchical NaNbO3/ZnIn2S4 heterojunction for the first time by in situ coating thin-layered ZnIn2S4 nanosheets on the external surface of NaNbO3 nanorods via a facile solvothermal method. A striking hydrogen evolution rate of 30.04 mmol h−1 g−1 was attained using NaNbO3/ZnIn2S4 as a photocatalyst under simulated sunlight irradiation, which is almost 110-fold and 11-fold higher than that of bare NaNbO3 and ZnIn2S4, respectively, and is the highest value obtained thus far among reported NaNbO3 and ZnIn2S4-based catalysts. This extraordinary improvement in the photocatalytic performance is mainly due to two reasons. Firstly, the difference in conduction band position and the intimate contact between NaNbO3 and ZnIn2S4 facilitate interfacial charge separation from NaNbO3 to ZnIn2S4. Secondly, the unique hierarchical heterostructure not only affords a more diffused surface area but also serves as a 3D supporting platform to generate more fruitful proton reduction sites, realizing a maximized photocatalytic activity. Additionally, density functional theory (DFT) calculations on the heterojunction further revealed the electron density distribution at the heterointerface and a close-to-neutral Gibbs free energy of hydrogen adsorption (ΔGH). Hence, the present work can provide fresh guidance for the synthesis and development of more NaNbO3 and ZnIn2S4-based composite photocatalysts for related applications in photocatalysis.
机译:势在必行,但仍然具有挑战性的是,在光催化氢进化(PHE)反应中开发出有效的界面荷载体分离的异缘光催化剂。令人鼓舞的是,在这项工作中,我们首次通过位于nanbo3纳米棒的外表面上的薄层薄层Znin2s4纳米片,首次通过宽层涂层Znin2s4纳米片构建了3D层次NANBO3/ZNIN2S4杂结。使用Nanbo3/Znin2S4作为模拟的阳光照射下的光催化剂,达到30.04 mmol H-1 G-1的惊人氢演化速率分别比Bare Nanb​​o3和Znin2s4高110倍和11倍,并且高110倍和11倍。是迄今为止在报告的Nanbo3和Znin2s4催化剂中获得的最高值。光催化性能的这种非凡改进主要是由于两个原因。首先,Nanbo3和Znin2s4之间的传导带位置的差异和亲密接触促进了界面电荷与Nanbo3到Znin2s4的分​​离。其次,独特的分层异质结构不仅提供了更具扩散的表面积,而且还可以作为一个3D支持平台,以产生更富有成果的质子还原位点,从而实现最大化的光催化活性。此外,异质结的密度功能理论(DFT)计算进一步揭示了异源面的电子密度分布和氢吸附(ΔGH)的接近中性吉布斯自由能。因此,目前的工作可以为基于NANBO3和ZNIN2S4的更多基于NANBO3和ZNIN2S4的复合光催化剂的合成和开发提供新的指导。

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