Kunfeng Zhang , Hongxia Chen , Yifan Liu , Bo Peng , Jinxia Liang
{"title":"通过同时控制N-H键和氧的激活,增强了Ag/WO3上光催化氨氧化","authors":"Kunfeng Zhang , Hongxia Chen , Yifan Liu , Bo Peng , Jinxia Liang","doi":"10.1016/j.seppur.2025.133428","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalytic conversion of NH<sub>3</sub> into N<sub>2</sub> and H<sub>2</sub>O is a promising technology for NH<sub>3</sub> abatement. Herein, different crystal phases (hexagonal, monoclinic, and mixed crystal phases) of WO<sub>3</sub> and Ag modified monoclinic WO<sub>3</sub> (Ag/m-WO<sub>3</sub>) were synthesized for the photocatalytic oxidation of NH<sub>3</sub>. The crystal-phase transition and formation of ohmic contact accelerated charge separation and transfer, and the localized surface plasmon resonance (LSPR) effects of Ag and WO<sub>3</sub> enhanced light harvesting capacity. Accordingly, Ag/m-WO<sub>3</sub> exhibited the best photocatalytic NH<sub>3</sub> oxidation activity, and its reaction rate was 1.5 and 4.4 times higher than that of m-WO<sub>3</sub> and hexagonal WO<sub>3</sub> (h-WO<sub>3</sub>), respectively. More importantly, the photoinduced electrons of oxygen-deficient WO<sub>3</sub> could activate chemisorbed oxygen to produce superoxide radicals (•O<sub>2</sub><sup>−</sup>) without thermodynamic limitation, thus inhibiting the generation of undesirable byproducts and resulting in high N<sub>2</sub> selectivity. This work simultaneously regulates the activation of N–H bonds and the generation of •O<sub>2</sub><sup>−</sup> for NH<sub>3</sub> oxidation, contributing to the design of highly efficient photocatalysts for pollutant treatment.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"372 ","pages":"Article 133428"},"PeriodicalIF":9.0000,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced photocatalytic ammonia oxidation over Ag/WO3 via simultaneously steering the activation for N–H bonds and oxygen species\",\"authors\":\"Kunfeng Zhang , Hongxia Chen , Yifan Liu , Bo Peng , Jinxia Liang\",\"doi\":\"10.1016/j.seppur.2025.133428\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalytic conversion of NH<sub>3</sub> into N<sub>2</sub> and H<sub>2</sub>O is a promising technology for NH<sub>3</sub> abatement. Herein, different crystal phases (hexagonal, monoclinic, and mixed crystal phases) of WO<sub>3</sub> and Ag modified monoclinic WO<sub>3</sub> (Ag/m-WO<sub>3</sub>) were synthesized for the photocatalytic oxidation of NH<sub>3</sub>. The crystal-phase transition and formation of ohmic contact accelerated charge separation and transfer, and the localized surface plasmon resonance (LSPR) effects of Ag and WO<sub>3</sub> enhanced light harvesting capacity. Accordingly, Ag/m-WO<sub>3</sub> exhibited the best photocatalytic NH<sub>3</sub> oxidation activity, and its reaction rate was 1.5 and 4.4 times higher than that of m-WO<sub>3</sub> and hexagonal WO<sub>3</sub> (h-WO<sub>3</sub>), respectively. More importantly, the photoinduced electrons of oxygen-deficient WO<sub>3</sub> could activate chemisorbed oxygen to produce superoxide radicals (•O<sub>2</sub><sup>−</sup>) without thermodynamic limitation, thus inhibiting the generation of undesirable byproducts and resulting in high N<sub>2</sub> selectivity. This work simultaneously regulates the activation of N–H bonds and the generation of •O<sub>2</sub><sup>−</sup> for NH<sub>3</sub> oxidation, contributing to the design of highly efficient photocatalysts for pollutant treatment.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"372 \",\"pages\":\"Article 133428\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-05-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586625020258\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586625020258","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Enhanced photocatalytic ammonia oxidation over Ag/WO3 via simultaneously steering the activation for N–H bonds and oxygen species
Photocatalytic conversion of NH3 into N2 and H2O is a promising technology for NH3 abatement. Herein, different crystal phases (hexagonal, monoclinic, and mixed crystal phases) of WO3 and Ag modified monoclinic WO3 (Ag/m-WO3) were synthesized for the photocatalytic oxidation of NH3. The crystal-phase transition and formation of ohmic contact accelerated charge separation and transfer, and the localized surface plasmon resonance (LSPR) effects of Ag and WO3 enhanced light harvesting capacity. Accordingly, Ag/m-WO3 exhibited the best photocatalytic NH3 oxidation activity, and its reaction rate was 1.5 and 4.4 times higher than that of m-WO3 and hexagonal WO3 (h-WO3), respectively. More importantly, the photoinduced electrons of oxygen-deficient WO3 could activate chemisorbed oxygen to produce superoxide radicals (•O2−) without thermodynamic limitation, thus inhibiting the generation of undesirable byproducts and resulting in high N2 selectivity. This work simultaneously regulates the activation of N–H bonds and the generation of •O2− for NH3 oxidation, contributing to the design of highly efficient photocatalysts for pollutant treatment.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.