{"title":"通过耦合 g-C3N4 和 NH2-MIL-125 提高吸附和电荷转移能力,高效降解水中的磺胺甲噁唑:特性、降解效率、影响因素和机理","authors":"Wei Guo , Mengmeng Zhang , Bingjie Yin , Haoqing Dong , Delong Meng , Guodong Zhang , Guangshan Zhang , Yanjun Xin , Qinghua Chen","doi":"10.1016/j.jphotochem.2024.116040","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalysis is an advanced oxidation process that shows excellent promise in degrading organic pollutants present in water. However, electrons and holes tend to combine easily during the transfer process, and the adsorption capacity of single-phase photocatalytic materials is weak, resulting in a low degradation rate. Therefore, a new composite semiconductor photocatalyst g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 was constructed using a two-step solvothermal method. The morphology, elemental composition, structure, photoelectric properties, and photocatalytic activity of g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 were characterized. The photocatalytic degradation of Sulfamethoxazole (SMX) in water was also carried out. Results indicated that g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 had been synthesized successfully, and g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 had a broader photoresponse range, higher adsorption capacity, and higher separation efficiency of photogenerated carriers. When pH was 4.0 and catalyst dosage was 0.15 g/L, g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 showed the highest degradation rate for SMX. It was confirmed that the main active groups in SMX degradation were <sup><img></sup>OH, h<sup>+</sup>, and <sup><img></sup>O<sub>2</sub><sup>−</sup>. 15 kinds of intermediates of SMX and the possible degradation pathways were identified by high-performance liquid chromatography-mass spectrometry and DFT calculation. Toxicity analysis revealed that the intermediate products have a lower developmental toxicity than SMX. This work demonstrated that g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 has great potential in eliminating antibiotics from water.</div></div>","PeriodicalId":16782,"journal":{"name":"Journal of Photochemistry and Photobiology A-chemistry","volume":"459 ","pages":"Article 116040"},"PeriodicalIF":4.1000,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Improved adsorption and charge transfer capacity by coupling g-C3N4 and NH2-MIL-125 for efficient degradation of sulfamethoxazole in water: Characterization, degradation efficiency, influence factors, and mechanism\",\"authors\":\"Wei Guo , Mengmeng Zhang , Bingjie Yin , Haoqing Dong , Delong Meng , Guodong Zhang , Guangshan Zhang , Yanjun Xin , Qinghua Chen\",\"doi\":\"10.1016/j.jphotochem.2024.116040\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalysis is an advanced oxidation process that shows excellent promise in degrading organic pollutants present in water. However, electrons and holes tend to combine easily during the transfer process, and the adsorption capacity of single-phase photocatalytic materials is weak, resulting in a low degradation rate. Therefore, a new composite semiconductor photocatalyst g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 was constructed using a two-step solvothermal method. The morphology, elemental composition, structure, photoelectric properties, and photocatalytic activity of g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 were characterized. The photocatalytic degradation of Sulfamethoxazole (SMX) in water was also carried out. Results indicated that g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 had been synthesized successfully, and g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 had a broader photoresponse range, higher adsorption capacity, and higher separation efficiency of photogenerated carriers. When pH was 4.0 and catalyst dosage was 0.15 g/L, g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 showed the highest degradation rate for SMX. It was confirmed that the main active groups in SMX degradation were <sup><img></sup>OH, h<sup>+</sup>, and <sup><img></sup>O<sub>2</sub><sup>−</sup>. 15 kinds of intermediates of SMX and the possible degradation pathways were identified by high-performance liquid chromatography-mass spectrometry and DFT calculation. Toxicity analysis revealed that the intermediate products have a lower developmental toxicity than SMX. This work demonstrated that g-C<sub>3</sub>N<sub>4</sub>/NH<sub>2</sub>-MIL-125 has great potential in eliminating antibiotics from water.</div></div>\",\"PeriodicalId\":16782,\"journal\":{\"name\":\"Journal of Photochemistry and Photobiology A-chemistry\",\"volume\":\"459 \",\"pages\":\"Article 116040\"},\"PeriodicalIF\":4.1000,\"publicationDate\":\"2024-09-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Photochemistry and Photobiology A-chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1010603024005847\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Photochemistry and Photobiology A-chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1010603024005847","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Improved adsorption and charge transfer capacity by coupling g-C3N4 and NH2-MIL-125 for efficient degradation of sulfamethoxazole in water: Characterization, degradation efficiency, influence factors, and mechanism
Photocatalysis is an advanced oxidation process that shows excellent promise in degrading organic pollutants present in water. However, electrons and holes tend to combine easily during the transfer process, and the adsorption capacity of single-phase photocatalytic materials is weak, resulting in a low degradation rate. Therefore, a new composite semiconductor photocatalyst g-C3N4/NH2-MIL-125 was constructed using a two-step solvothermal method. The morphology, elemental composition, structure, photoelectric properties, and photocatalytic activity of g-C3N4/NH2-MIL-125 were characterized. The photocatalytic degradation of Sulfamethoxazole (SMX) in water was also carried out. Results indicated that g-C3N4/NH2-MIL-125 had been synthesized successfully, and g-C3N4/NH2-MIL-125 had a broader photoresponse range, higher adsorption capacity, and higher separation efficiency of photogenerated carriers. When pH was 4.0 and catalyst dosage was 0.15 g/L, g-C3N4/NH2-MIL-125 showed the highest degradation rate for SMX. It was confirmed that the main active groups in SMX degradation were OH, h+, and O2−. 15 kinds of intermediates of SMX and the possible degradation pathways were identified by high-performance liquid chromatography-mass spectrometry and DFT calculation. Toxicity analysis revealed that the intermediate products have a lower developmental toxicity than SMX. This work demonstrated that g-C3N4/NH2-MIL-125 has great potential in eliminating antibiotics from water.
期刊介绍:
JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds.
All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor).
The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.