Study on the performance and mechanism of NH2-MIL-101(Fe)/CQDs@UCN composite photocatalyst with self-Fenton effect

IF 5.7 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Research Bulletin Pub Date : 2025-08-08 DOI:10.1016/j.materresbull.2025.113716

Yan Huang , Zongxue Yu , Yuwen Huang , Wei Yan , Bo Xing , Fengyan Fan , Dingmei Han , Xia Liu , Chun Xu , Chao Tang , Zhedan Yang

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Abstract

Monodisperse NH₂-MIL-101(Fe) and two-dimensional sheet-like UCN materials were synthesized using a one-pot solvothermal method and an acid treatment-ethanol intercalation-thermal exfoliation method, respectively. The heterojunction composite photocatalyst NM101/CQDs@UCN was then synthesized through electrostatic self-assembly. The heterojunction composite photocatalyst NM101/CQDs@UCN was then prepared via electrostatic self-assembly. Photocatalytic experiments and material characterization confirmed that the modified UCN and CQDs@UCN, after transitioning from the original bulk structure to a two-dimensional sheet-like structure, exhibited significantly increased BET surface area, enriched pore structure, and enhanced H₂O₂ production during photocatalytic processes. Notably, the catalyst also demonstrated excellent degradation performance for fracturing flowback fluid, achieving a COD removal rate of 72.7% under 180 minutes of visible light irradiation. Finally, capture experiments and ESR analysis revealed that the modified UCN selectively generated H₂O₂, which triggered the self-Fenton effect. This, in turn, coupled with NH₂-MIL-101(Fe) to form a surface heterojunction, promoting the directional migration and separation of photo-generated charge carriers, thus enhancing the photocatalytic degradation performance of the composite photocatalyst.

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具有自fenton效应的NH2-MIL-101(Fe)/CQDs@UCN复合光催化剂的性能及机理研究

采用一锅溶剂热法和酸处理-乙醇插层-热剥落法制备了单分散的NH₂-MIL-101（Fe）和二维片状UCN材料。然后通过静电自组装合成了异质结复合光催化剂NM101/CQDs@UCN。采用静电自组装法制备了异质结复合光催化剂NM101/CQDs@UCN。光催化实验和材料表征证实，改性后的UCN和CQDs@UCN从原来的块状结构过渡到二维片状结构后，在光催化过程中表现出明显增加的BET比表面积，丰富的孔隙结构和增强的H₂O₂产率。值得注意的是，该催化剂对压裂返排液也表现出了出色的降解性能，在可见光照射180分钟的情况下，COD去除率达到72.7%。最后，捕获实验和ESR分析表明，修饰后的UCN选择性地产生了H₂O₂，从而触发了自芬顿效应。这又与NH₂-MIL-101（Fe）耦合形成表面异质结，促进了光生载流子的定向迁移和分离，从而增强了复合光催化剂的光催化降解性能。

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来源期刊

Materials Research Bulletin 工程技术-材料科学：综合

CiteScore

9.80

自引率

5.60%

发文量

372

审稿时长

42 days

期刊介绍： Materials Research Bulletin is an international journal reporting high-impact research on processing-structure-property relationships in functional materials and nanomaterials with interesting electronic, magnetic, optical, thermal, mechanical or catalytic properties. Papers purely on thermodynamics or theoretical calculations (e.g., density functional theory) do not fall within the scope of the journal unless they also demonstrate a clear link to physical properties. Topics covered include functional materials (e.g., dielectrics, pyroelectrics, piezoelectrics, ferroelectrics, relaxors, thermoelectrics, etc.); electrochemistry and solid-state ionics (e.g., photovoltaics, batteries, sensors, and fuel cells); nanomaterials, graphene, and nanocomposites; luminescence and photocatalysis; crystal-structure and defect-structure analysis; novel electronics; non-crystalline solids; flexible electronics; protein-material interactions; and polymeric ion-exchange membranes.