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用于光催化产氢并与有机污染物降解同步进行的包裹有ZnCdS纳米颗粒的UiO-66立方体直接Z型体系。

Direct Z-scheme system of UiO-66 cubes wrapped with ZnCdS nanoparticles for photocatalytic hydrogen generation synchronized with organic pollutant degradation.

作者信息

Hou Dongfang, Zhu Qian, Wang Junjie, Deng Min, Qiao Xiu-Qing, Sun Bojing, Han Qingwen, Chi Ruan, Li Dong-Sheng

机构信息

College of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, Hubei 443002, PR China; Hubei Three Gorges Laboratory, Yichang, Hubei 443007, PR China.

College of Materials and Chemical Engineering, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang, Hubei 443002, PR China.

出版信息

J Colloid Interface Sci. 2024 Jul;665:68-79. doi: 10.1016/j.jcis.2024.03.111. Epub 2024 Mar 17.

DOI:10.1016/j.jcis.2024.03.111
PMID:38513409
Abstract

Optimized fabrication of Z-scheme photocatalyst based on MOF materials offers sustainable energy generation and environmental improvement due to their attractive properties. The Z-scheme heterojunctions consisting of UiO-66 cubes covered with ZnCdS nanoparticles were fabricated by a facile solvothermal method. Thanks to the Z-scheme carrier transport under simulated sunlight irradiation, UiO-66@ZnCdS exhibited enhanced photocatalytic performance of H generation synchronized with organic pollutant degradation in fluoroquinolone antibiotic wastewater. Synergistically, the highest comprehensive performance was obtained in ciprofloxacin solution. The H yield reached 224 μmol∙ g∙ h and simultaneously the removal efficiency was up to 83.6 %. The degradation pathways revealed that the process of piperazine ring cleavage and decarboxylation also generates H protons, further promoting the production of H. Therefore, the effective spatial separation and transfer of the photoinduced carriers are attributed to the good band structure, large specific surface area, and cooperative reduction and oxidation reactions of UiO-66@ZnCdS, resulting in significant photocatalytic activity. The toxicity assessment of antibiotics and intermediate products during the photocatalytic reaction also verifies the reduction of environmental risk. This study highlights a promising way to expand the application of the MOFs-based photocatalyst in clean energy conversion coupling with water remediation.

摘要

基于金属有机框架(MOF)材料的Z型光催化剂的优化制备,因其具有吸引力的特性而提供了可持续的能源生成和环境改善。由覆盖有ZnCdS纳米颗粒的UiO-66立方体组成的Z型异质结通过简便的溶剂热法制备。由于在模拟太阳光照射下的Z型载流子传输,UiO-66@ZnCdS在氟喹诺酮抗生素废水中表现出增强的光催化产氢性能,同时与有机污染物降解同步。协同地,在环丙沙星溶液中获得了最高的综合性能。产氢量达到224 μmol∙ g∙ h,同时去除效率高达83.6%。降解途径表明,哌嗪环裂解和脱羧过程也产生H质子,进一步促进了H的产生。因此,光生载流子的有效空间分离和转移归因于UiO-66@ZnCdS良好的能带结构、大比表面积以及协同还原和氧化反应,从而产生显著的光催化活性。光催化反应过程中抗生素和中间产物的毒性评估也验证了环境风险的降低。这项研究突出了一种有前景的方法,可扩大基于MOF的光催化剂在清洁能源转换与水修复耦合方面的应用。

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