{"title":"在TiO2-g-C3N4-rGO的间隙原子线上采用新型双Co和W单金属原子氧化物增强光催化产氢和降解性能","authors":"Annamalai Raja, Rama Krishna Chava, Misook Kang","doi":"10.1016/j.cej.2025.163000","DOIUrl":null,"url":null,"abstract":"In this study, a TiO<sub>2</sub>–g-C<sub>3</sub>N<sub>4</sub>–ethylene diamine-reduced graphene oxide photocatalyst incorporating dissolved heteropolyacid-cobalt (HPA-Co) was successfully synthesized using the hydrothermal method. The surface-dispersed CoW single atom molecules were generated as co-catalysts utilizing the HPA-Co in the presence of ethylene diamine and ethylene glycol. Notably, the use of HPA-Co as a molecular precursor enables the controlled formation of well-dispersed single CoW atoms on the hybrid, offering a unique approach not commonly reported in previous studies. The developed atomic-level engineering photocatalyst achieved a high H<sub>2</sub> generation rate of 27.40 mmol g<sup>−1</sup> h<sup>−1</sup> and a sulfathiazole (STZ) degradation efficiency of 99.7 %. Furthermore, it demonstrated excellent stability and reusability over five successive cycles of H<sub>2</sub> production and STZ photodegradation. The synthesized hybrid catalyst exhibits high photocatalytic effectiveness, enabling the purification of strongly contaminated (30 L of 50 mg/L Rhodamine B) saltwater using a specially designed wastewater treatment apparatus within about 5 h of direct sunlight radiation. Mass spectrometry was employed to identify photodegradation intermediates. The composite exhibits enhanced photocatalytic performance, attributed to synergistic effects among the components, improved charge separation, and extended light absorption. This atomic-level engineering introduces abundant active sites and facilitates interfacial charge transfer, resulting in a significantly higher hydrogen evolution rate. A potential Z-scheme approach was suggested for photocatalytic hydrogen generation efficiency. These findings contribute to the development of cost-effective, durable photocatalysts with rapid reaction kinetics and high H<sub>2</sub> generation and photodegradation efficiency.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"52 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced photocatalytic hydrogen generation and degradation performance using a novel design of dual Co and W single metal atom oxides on the interstitial atomic line of TiO2–g-C3N4–rGO\",\"authors\":\"Annamalai Raja, Rama Krishna Chava, Misook Kang\",\"doi\":\"10.1016/j.cej.2025.163000\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"In this study, a TiO<sub>2</sub>–g-C<sub>3</sub>N<sub>4</sub>–ethylene diamine-reduced graphene oxide photocatalyst incorporating dissolved heteropolyacid-cobalt (HPA-Co) was successfully synthesized using the hydrothermal method. The surface-dispersed CoW single atom molecules were generated as co-catalysts utilizing the HPA-Co in the presence of ethylene diamine and ethylene glycol. Notably, the use of HPA-Co as a molecular precursor enables the controlled formation of well-dispersed single CoW atoms on the hybrid, offering a unique approach not commonly reported in previous studies. The developed atomic-level engineering photocatalyst achieved a high H<sub>2</sub> generation rate of 27.40 mmol g<sup>−1</sup> h<sup>−1</sup> and a sulfathiazole (STZ) degradation efficiency of 99.7 %. Furthermore, it demonstrated excellent stability and reusability over five successive cycles of H<sub>2</sub> production and STZ photodegradation. The synthesized hybrid catalyst exhibits high photocatalytic effectiveness, enabling the purification of strongly contaminated (30 L of 50 mg/L Rhodamine B) saltwater using a specially designed wastewater treatment apparatus within about 5 h of direct sunlight radiation. Mass spectrometry was employed to identify photodegradation intermediates. The composite exhibits enhanced photocatalytic performance, attributed to synergistic effects among the components, improved charge separation, and extended light absorption. This atomic-level engineering introduces abundant active sites and facilitates interfacial charge transfer, resulting in a significantly higher hydrogen evolution rate. A potential Z-scheme approach was suggested for photocatalytic hydrogen generation efficiency. These findings contribute to the development of cost-effective, durable photocatalysts with rapid reaction kinetics and high H<sub>2</sub> generation and photodegradation efficiency.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"52 1\",\"pages\":\"\"},\"PeriodicalIF\":13.3000,\"publicationDate\":\"2025-04-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2025.163000\",\"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":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.163000","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 hydrogen generation and degradation performance using a novel design of dual Co and W single metal atom oxides on the interstitial atomic line of TiO2–g-C3N4–rGO
In this study, a TiO2–g-C3N4–ethylene diamine-reduced graphene oxide photocatalyst incorporating dissolved heteropolyacid-cobalt (HPA-Co) was successfully synthesized using the hydrothermal method. The surface-dispersed CoW single atom molecules were generated as co-catalysts utilizing the HPA-Co in the presence of ethylene diamine and ethylene glycol. Notably, the use of HPA-Co as a molecular precursor enables the controlled formation of well-dispersed single CoW atoms on the hybrid, offering a unique approach not commonly reported in previous studies. The developed atomic-level engineering photocatalyst achieved a high H2 generation rate of 27.40 mmol g−1 h−1 and a sulfathiazole (STZ) degradation efficiency of 99.7 %. Furthermore, it demonstrated excellent stability and reusability over five successive cycles of H2 production and STZ photodegradation. The synthesized hybrid catalyst exhibits high photocatalytic effectiveness, enabling the purification of strongly contaminated (30 L of 50 mg/L Rhodamine B) saltwater using a specially designed wastewater treatment apparatus within about 5 h of direct sunlight radiation. Mass spectrometry was employed to identify photodegradation intermediates. The composite exhibits enhanced photocatalytic performance, attributed to synergistic effects among the components, improved charge separation, and extended light absorption. This atomic-level engineering introduces abundant active sites and facilitates interfacial charge transfer, resulting in a significantly higher hydrogen evolution rate. A potential Z-scheme approach was suggested for photocatalytic hydrogen generation efficiency. These findings contribute to the development of cost-effective, durable photocatalysts with rapid reaction kinetics and high H2 generation and photodegradation efficiency.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.