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银@氧化锌光电化学界面原位电荷转移对析氢和罗丹明B降解高光催化性能的影响

In Situ Charge Transfer at the Ag@ZnO Photoelectrochemical Interface toward the High Photocatalytic Performance of H Evolution and RhB Degradation.

作者信息

Trang Ton Nu Quynh, Phan Thang Bach, Nam Nguyen Dang, Thu Vu Thi Hanh

机构信息

Faculty of Physics and Physics Engineering, University of Science, 227 Nguyen Van Cu Street, District 5, Ho Chi Minh City 700000, Vietnam.

Vietnam National University, Ho Chi Minh City 700000, Vietnam.

出版信息

ACS Appl Mater Interfaces. 2020 Mar 11;12(10):12195-12206. doi: 10.1021/acsami.9b15578. Epub 2020 Feb 27.

DOI:10.1021/acsami.9b15578
PMID:32013392
Abstract

Designing an efficient hybrid structure photocatalyst for photocatalytic decomposition and hydrogen (H) evolution has been considered a great choice to develop renewable technologies for clean energy production and environmental remediation. Enhanced charge transfer (CT) based on the interaction between a noble metal and a semiconductor is a crucial factor influencing the movement of photogenerated electron-hole pairs. Herein, we focus on the recent advances related to plasmon-enhanced noble metals and the semiconductor nature to drive the photocatalytic H production and photodegradation of the organic dye rhodamine B (RhB) under UV and visible light irradiation. Specifically, the combination of concerted catalysis and green nanoengineering strategies to design ZnO-based composite photocatalysts and their decoration with metallic Ag have been realized by the radio frequency (RF) sputtering technique at room temperature. This simultaneity enhances the interface coupling between Ag and ZnO and reduces the energy threshold. The creation of charge transfer in the heterojunction and Schottky barrier changes the photoelectronic properties of the as-synthesized Al-doped ZnO (AZO); afterward, these effects promote the migration, transportation, and separation of photoinduced charge carriers and enhance the light-harvesting efficiency. As a result, the as-synthesized AZO-20 hybrid nanostructure exhibits a photocurrent density of 2.5 mA/cm vs Ag/AgCl, which is improved by almost 12 times compared with that of bare ZnO (0.2 mA/cm). The hydrogen evolution rates of AZO-20 were ∼38 and ∼24 μmol/h under UV and visible light exposure, which are almost five- and tenfold higher than those of pristine ZnO, respectively. Additionally, the RhB degradation efficacies of the obtained AZO-20 were greater than almost 97 and 82% under UV and visible light illumination, respectively. The achieved apparent rate constant for the photocatalytic RhB decomposition was 0.014 min, indicating that it is 14-fold than that in pristine ZnO (0.001 min). Heterostructure AZO photocatalysts possess excellent practical stability in the water-splitting reaction and photocatalytic RhB decomposition, posing as promising candidates in practical works for pollution and energy challenges.

摘要

设计一种高效的混合结构光催化剂用于光催化分解和析氢,被认为是开发可再生清洁能源生产和环境修复技术的绝佳选择。基于贵金属与半导体之间相互作用的增强电荷转移(CT)是影响光生电子 - 空穴对移动的关键因素。在此,我们聚焦于与等离子体增强贵金属和半导体性质相关的最新进展,以驱动在紫外光和可见光照射下的光催化产氢以及有机染料罗丹明B(RhB)的光降解。具体而言,通过室温下的射频(RF)溅射技术,实现了协同催化和绿色纳米工程策略相结合来设计基于ZnO的复合光催化剂及其用金属Ag进行修饰。这同时增强了Ag与ZnO之间的界面耦合并降低了能量阈值。异质结和肖特基势垒中电荷转移的产生改变了合成的Al掺杂ZnO(AZO)的光电性质;随后,这些效应促进了光生电荷载流子的迁移、传输和分离,并提高了光捕获效率。结果,合成的AZO - 20混合纳米结构相对于Ag/AgCl的光电流密度为2.5 mA/cm²,与裸ZnO(0.2 mA/cm²)相比提高了近12倍。在紫外光和可见光照射下,AZO - 20的析氢速率分别约为38和24 μmol/h,分别比原始ZnO高出近五倍和十倍。此外,所获得的AZO - 20在紫外光和可见光照射下对RhB的降解效率分别大于97%和82%。光催化RhB分解的表观速率常数为0.014 min⁻¹,表明它是原始ZnO(0.001 min⁻¹)的14倍。异质结构AZO光催化剂在水分解反应和光催化RhB分解中具有出色的实际稳定性,是应对污染和能源挑战实际工作中有前景的候选材料。

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