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构建直接Z型CeO/UiO-66-NH异质结以提高光催化有机污染物降解和析氢性能。

Construction of a direct Z-scheme CeO/UiO-66-NH heterojunction for boosting photocatalytic organic pollutant degradation and H evolution performance.

作者信息

Zhang Heling, Wan Yuqi, Shang Simin, Cheng Qingrong, Pan Zhiquan

机构信息

School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan, 430205, PR China.

Department of Electrical and Electronic Engineering, The University of Hong Kong, Hong Kong, 99907, PR China.

出版信息

Dalton Trans. 2023 Apr 4;52(14):4562-4573. doi: 10.1039/d2dt03797a.

Abstract

In this study, hollow CeO nanospheres were grown on UIO-66-NH nanosheets to form a novel CeO/UiO-66-NH (abbreviation, CU) Z-scheme heterojunction photocatalyst by calcination and hydrothermal method for hydrogen production and photocatalytic degradation of organic pollutants. Under visible light, the H generation rate of the CU composite was 5662.1 μmol g h, which was 22 and 7 fold than that of pure CeO and pure UiO-66-NH, respectively. In addition, compared with CeO and UiO-66-NH, the as-prepared CU composites exhibited enhanced photo-degradation efficiencies for tetracycline (TC) and 2,4-dichlorophenol (DCP) under simulated solar light irradiation. Among them, the CU composite demonstrated the highest photocatalytic performance and reached 91.5% for TC, and 94.3% for DCP. In addition, a logical solid-state Z-type electron transfer mechanism is presented with the results of radical scavenging and ESR experiments to illustrate the intensive decomposed ability of the photocatalytic system. The enhanced photocatalytic performance of CU heterostructures can be attributed to the formation of a band-position-matched hollow structure heterojunction between CeO and UIO-66-NH, which can effectively inhibit the recombination of carriers and increase the specific surface area as well as the light absorption. Moreover, the oxidation and reduction ability of the charge carriers was also increased. This work resulted in a feasible idea for removing organic pollutants and hydrogen production by traditional inorganic semiconductor/MOF-based heterostructured photocatalysts.

摘要

在本研究中,通过煅烧和水热法在UIO-66-NH纳米片上生长中空CeO纳米球,以形成一种新型的CeO/UiO-66-NH(缩写为CU)Z型异质结光催化剂,用于制氢和光催化降解有机污染物。在可见光下,CU复合材料的H生成速率为5662.1 μmol g⁻¹ h⁻¹,分别是纯CeO和纯UiO-66-NH的22倍和7倍。此外,与CeO和UiO-66-NH相比,所制备的CU复合材料在模拟太阳光照射下对四环素(TC)和2,4-二氯苯酚(DCP)表现出增强的光降解效率。其中,CU复合材料表现出最高的光催化性能,对TC的光催化降解率达到91.5%,对DCP的光催化降解率达到94.3%。此外,通过自由基清除和电子顺磁共振(ESR)实验结果提出了一种合理的固态Z型电子转移机制,以说明光催化系统的强分解能力。CU异质结构光催化性能的增强可归因于CeO和UIO-66-NH之间形成了带位置匹配的中空结构异质结,这可以有效抑制载流子的复合,增加比表面积以及光吸收。此外,电荷载流子的氧化和还原能力也得到了提高。这项工作为通过传统无机半导体/基于金属有机框架(MOF)的异质结构光催化剂去除有机污染物和制氢提供了一个可行的思路。

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