HPW-Anchored UiO-66 Metal-Organic Framework: A Promising Photocatalyst Effective toward Tetracycline Hydrochloride Degradation and H2 Evolution via Z-Scheme Charge Dynamics.
HPW-Anchored UiO-66 Metal-Organic Framework: A Promising Photocatalyst Effective toward Tetracycline Hydrochloride Degradation and H2 Evolution via Z-Scheme Charge Dynamics.
复制标题
DOI：
10.1021/acs.inorgchem.8b03544
复制
发表时间：
2019-03
影响因子：
4.6
通讯作者：
Satyabrata Subudhi;Sriram Mansingh;G. Swain;Arjun Behera;Dharitri Rath;K. Parida
中科院分区：
文献类型：
--
作者：
Satyabrata Subudhi;Sriram Mansingh;G. Swain;Arjun Behera;Dharitri Rath;K. Parida
消除环境污染物和使用多相光催化剂从水中生产氢(H2)是解决现代生活中日益严重的环境污染和全球能源灾难的当前情景的一项苛刻的科学。为了验证这一目的，设计低成本、耐用、光吸收能力强的半导体基光催化剂成为研究人员面临的最具挑战性的问题。对此，本文采用水热法制备了磷钨酸(HPW)锚定的金属有机骨架(MOF)，即HPW@UIO-66，它是高效、稳定的，并且能够在牺牲供体存在的情况下利用太阳能降解盐酸四环素(TCH)和产生氢气。HPW与UIO-66之间的离子相互作用对复合材料的光稳定性和电荷转移机理起着关键作用，并用X射线衍射、紫外漫反射光谱、傅立叶变换红外光谱和X射线光电子能谱对其进行了表征。30wt%HPW@UIO-66在60min的太阳光照射下，对20ppm TCH溶液的最大降解率约为87.24%，产氢量约为353.89μ。通过Mott-Schottky测量和电化学阻抗谱的延迟电荷复合过程，很好地表征了导带和价带电位。所提出的无介体Z方案取向的电子-空穴迁移路径得到了光致发光的很好支持，清除剂测试很好地解释了所制备的复合材料具有更好的电荷-载流子分离和高催化性能。这项研究将为制备新型和具有挑战性的光催化剂提供有利的蓝图，用于环境污染物的光催化处理和放氢。
The abolition of environmental pollutants and production of hydrogen (H2) from water using a heterogeneous photocatalyst is a demanding science of the current scenario to solve the increasing environmental pollution and worldwide energy catastrophe in modern life. To validate this purpose, the design of low-cost and durable semiconductor-based photocatalysts with great light absorption capacity becomes the most challenging issue for researchers. Regarding this, herein the phosphotungstic acid (HPW)-anchored Zr6O4(OH)4(BDC)6 (UiO-66) metal-organic framework (MOF), i.e., HPW@UiO-66, has been prepared by a hydrothermal method and is efficient, stable, and capable of harvesting solar energy toward the degradation of tetracycline hydrochloride (TCH) and H2 production in the presence of a sacrificial donor. The ionic interaction between HPW and UiO-66 plays a key role toward the photostability and charge-transfer mechanism of the composite and is well characterized with X-ray diffraction, UV diffuse-reflectance spectroscopy, Fourier transform infrared, and X-ray photoelectron spectroscopy. A total of 30 wt % HPW@UiO-66 shows a maximum degradation of about 87.24% of a 20 ppm TCH solution in 60 min of solar-light irradiation and about 353.89 μmol/h of H2 production. The conduction- and valence-band potentials are well characterized with Mott-Schottky measurement and a delay charge recombination process through electrochemical impedance spectroscopy. The proposed mediator-free Z-scheme-oriented electron-hole migration route is well supported by photoluminescence, and the scavenger test well explains the better charge-carrier separation and high catalytic performance of the prepared composite. This research will bestow an advantageous blueprint to fabricate novel and challenging photocatalysts toward the photocatalytic treatment of environmental pollutants and H2 evolution.