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新型可见光活性 P-g-CN 基 α-BiO/WO 三元光催化剂具有双 Z 型异质结构,用于高效分解难降解紫外滤光剂和环境激素:二苯甲酮。

Novel visible-light-active P-g-CN-based α-BiO/WO ternary photocatalysts with a dual Z-scheme heterostructure for the efficient decomposition of refractory ultraviolet filters and environmental hormones: Benzophenones.

机构信息

International Ph.D. Program in Environmental Science and Technology, National Yang Ming Chiao Tung University, Taipei, 11221, Taiwan; Institute of Environmental and Occupational Health Sciences, National Yang Ming Chiao Tung University, Taipei, 11221, Taiwan; Department of Chemistry, College of Natural and Computational Sciences, Arba Minch University, Arbaminch, Ethiopia.

International Ph.D. Program in Environmental Science and Technology, National Yang Ming Chiao Tung University, Taipei, 11221, Taiwan; Institute of Environmental and Occupational Health Sciences, National Yang Ming Chiao Tung University, Taipei, 11221, Taiwan.

出版信息

Environ Res. 2023 Oct 1;234:116553. doi: 10.1016/j.envres.2023.116553. Epub 2023 Jul 3.

DOI:10.1016/j.envres.2023.116553
PMID:37406722
Abstract

The ubiquitous and refractory benzophenone (BP)-type ultraviolet filters, which are also endocrine disruptors, were commonly detected in the aquatic matrix and could not be efficiently removed by conventional wastewater treatment processes, thus causing extensive concern. Herein, a novel ternary nanocomposite, P-g-CN/α-BiO/WO (P-gBW), was successfully fabricated by mixing cocalcinated components and applied to the decomposition of BP-type ultraviolet filters. The dual-Z-scheme heterostructure of P-gBW enhances visible-light absorption, efficiently facilitates separation and mobility, and prolongs the lifetime of photoinduced charge carriers via double charge transfer mechanisms. The optimum 95 wt% P-gBW exhibited excellent photocatalytic activity, degrading 96% 4-hydroxy benzophenone (4HBP) within 150 min and 93% 2,2',4,4'-tetrahydroxybenzophenone (BP-2) within 100 min under visible-light illumination, respectively. The pseudo-first-order rate constant of 4HBP (1.15 h) was 6.8-, 3.1-, 3.3- and 2.2-fold higher than those of WO, P-g-CN, α-BiO, and P-g-CN/α-BiO, respectively, while that of BP-2 (1.71 h) was 5.2-, 2.2-, 3.2- and 1.5-fold higher, respectively. The improved photocatalytic degradation was attributed to efficient photoinduced charge carrier separation and migration and prevented the recombination of electron holes, as verified by photoluminescence, transient photocurrent response, and electrochemical impedance spectroscopy. Trapping experiments, electron paramagnetic resonance, and band energy position indicated an efficient dual-Z-scheme heterostructure.

摘要

无处不在且难以去除的二苯甲酮(BP)型紫外线吸收剂也是内分泌干扰物,它们通常在水基质中被检测到,而且不能通过传统的废水处理工艺有效地去除,因此引起了广泛的关注。在此,通过混合共沉淀成分成功制备了一种新型三元纳米复合材料 P-g-CN/α-BiO/WO(P-gBW),并将其应用于 BP 型紫外线吸收剂的分解。P-gBW 的双 Z 型异质结构增强了可见光吸收,通过双电荷转移机制有效地促进了分离和迁移,并延长了光生载流子的寿命。最佳的 95wt% P-gBW 在可见光照射下分别在 150 分钟内和 100 分钟内表现出优异的光催化活性,降解 96%的 4-羟基二苯甲酮(4HBP)和 93%的 2,2',4,4'-四羟基二苯甲酮(BP-2)。4HBP 的拟一级速率常数(1.15 h)分别比 WO、P-g-CN、α-BiO 和 P-g-CN/α-BiO 高 6.8、3.1、3.3 和 2.2 倍,而 BP-2(1.71 h)分别高 5.2、2.2、3.2 和 1.5 倍。改进的光催化降解归因于高效的光生载流子分离和迁移,防止了电子空穴的复合,这通过光致发光、瞬态光电流响应和电化学阻抗谱得到了验证。捕获实验、电子顺磁共振和能带能量位置表明存在有效的双 Z 型异质结构。

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