{"title":"钨酸盐(WO3·H2O)在微孔和介孔二氧化硅上原位生长以增强出氧光催化","authors":"Oussama Oulhakem*, and , Boutaina Rezki, ","doi":"10.1021/acs.jpcc.5c0182810.1021/acs.jpcc.5c01828","DOIUrl":null,"url":null,"abstract":"<p >Developing an efficient photocatalytic water-splitting system requires enhancing the intrinsic activities of both the oxygen evolution photocatalyst (OEP) and the hydrogen evolution photocatalyst (HEP). While recent studies have shown that tungstite (WO<sub>3</sub>·H<sub>2</sub>O) can stably oxidize water to O<sub>2</sub> using a broader spectrum of visible light compared to WO<sub>3</sub>, further improvements in its photocatalytic performances as an OEP are needed. One alternative is the use of supported photocatalysts; a uniform suspension of WO<sub>3</sub>·H<sub>2</sub>O on inert SiO<sub>2</sub> spheres reduces the amount of photocatalysts and provides more active sites. In this work, we report the impregnation of WO<sub>3</sub>·H<sub>2</sub>O onto the surface of two types of amorphous silica (microporous and mesoporous) in a one-pot synthesis using Pluronic P123 (P123) and Pluronic F127 (F127) templates. Structural characterization revealed that the resulting composites (SiOHW-P123 and SiOHW-F127) are single-phase materials, with WO<sub>3</sub>·H<sub>2</sub>O nanoparticles anchored to the silica’s surface via hydrogen bonding. Additionally, the conduction band minimum (CBM) of silica-impregnated WO<sub>3</sub>·H<sub>2</sub>O exhibited a significant positive shift compared to lone tungstite, which could be attributed to the increased tilt angle of W─O─W bonds induced by interactions with the amorphous silica framework. The SiOHW-F127 composite displayed a more uniform dispersion of tungstite across the surface, leading to a higher number of electrocatalytic sites, as confirmed by electrochemical impedance measurements. As a result, both composites demonstrated stable O<sub>2</sub> generation in aqueous Ag<sup>+</sup> solutions. Precisely, results demonstrate that O<sub>2</sub> production rates over SiOHW-P123 and SiOHW-F127 were two and three times higher, respectively, than over lone WO<sub>3</sub>·H<sub>2</sub>O. These findings highlight the potential of these composites as promising building blocks for photocatalytic water-splitting systems.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"129 23","pages":"10518–10530 10518–10530"},"PeriodicalIF":3.2000,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In Situ Growth of Tungstite (WO3·H2O) on Microporous and Mesoporous Silicas for Enhanced Oxygen-Evolving Photocatalysis\",\"authors\":\"Oussama Oulhakem*, and , Boutaina Rezki, \",\"doi\":\"10.1021/acs.jpcc.5c0182810.1021/acs.jpcc.5c01828\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Developing an efficient photocatalytic water-splitting system requires enhancing the intrinsic activities of both the oxygen evolution photocatalyst (OEP) and the hydrogen evolution photocatalyst (HEP). While recent studies have shown that tungstite (WO<sub>3</sub>·H<sub>2</sub>O) can stably oxidize water to O<sub>2</sub> using a broader spectrum of visible light compared to WO<sub>3</sub>, further improvements in its photocatalytic performances as an OEP are needed. One alternative is the use of supported photocatalysts; a uniform suspension of WO<sub>3</sub>·H<sub>2</sub>O on inert SiO<sub>2</sub> spheres reduces the amount of photocatalysts and provides more active sites. In this work, we report the impregnation of WO<sub>3</sub>·H<sub>2</sub>O onto the surface of two types of amorphous silica (microporous and mesoporous) in a one-pot synthesis using Pluronic P123 (P123) and Pluronic F127 (F127) templates. Structural characterization revealed that the resulting composites (SiOHW-P123 and SiOHW-F127) are single-phase materials, with WO<sub>3</sub>·H<sub>2</sub>O nanoparticles anchored to the silica’s surface via hydrogen bonding. Additionally, the conduction band minimum (CBM) of silica-impregnated WO<sub>3</sub>·H<sub>2</sub>O exhibited a significant positive shift compared to lone tungstite, which could be attributed to the increased tilt angle of W─O─W bonds induced by interactions with the amorphous silica framework. The SiOHW-F127 composite displayed a more uniform dispersion of tungstite across the surface, leading to a higher number of electrocatalytic sites, as confirmed by electrochemical impedance measurements. As a result, both composites demonstrated stable O<sub>2</sub> generation in aqueous Ag<sup>+</sup> solutions. Precisely, results demonstrate that O<sub>2</sub> production rates over SiOHW-P123 and SiOHW-F127 were two and three times higher, respectively, than over lone WO<sub>3</sub>·H<sub>2</sub>O. These findings highlight the potential of these composites as promising building blocks for photocatalytic water-splitting systems.</p>\",\"PeriodicalId\":61,\"journal\":{\"name\":\"The Journal of Physical Chemistry C\",\"volume\":\"129 23\",\"pages\":\"10518–10530 10518–10530\"},\"PeriodicalIF\":3.2000,\"publicationDate\":\"2025-05-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry C\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpcc.5c01828\",\"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":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpcc.5c01828","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
In Situ Growth of Tungstite (WO3·H2O) on Microporous and Mesoporous Silicas for Enhanced Oxygen-Evolving Photocatalysis
Developing an efficient photocatalytic water-splitting system requires enhancing the intrinsic activities of both the oxygen evolution photocatalyst (OEP) and the hydrogen evolution photocatalyst (HEP). While recent studies have shown that tungstite (WO3·H2O) can stably oxidize water to O2 using a broader spectrum of visible light compared to WO3, further improvements in its photocatalytic performances as an OEP are needed. One alternative is the use of supported photocatalysts; a uniform suspension of WO3·H2O on inert SiO2 spheres reduces the amount of photocatalysts and provides more active sites. In this work, we report the impregnation of WO3·H2O onto the surface of two types of amorphous silica (microporous and mesoporous) in a one-pot synthesis using Pluronic P123 (P123) and Pluronic F127 (F127) templates. Structural characterization revealed that the resulting composites (SiOHW-P123 and SiOHW-F127) are single-phase materials, with WO3·H2O nanoparticles anchored to the silica’s surface via hydrogen bonding. Additionally, the conduction band minimum (CBM) of silica-impregnated WO3·H2O exhibited a significant positive shift compared to lone tungstite, which could be attributed to the increased tilt angle of W─O─W bonds induced by interactions with the amorphous silica framework. The SiOHW-F127 composite displayed a more uniform dispersion of tungstite across the surface, leading to a higher number of electrocatalytic sites, as confirmed by electrochemical impedance measurements. As a result, both composites demonstrated stable O2 generation in aqueous Ag+ solutions. Precisely, results demonstrate that O2 production rates over SiOHW-P123 and SiOHW-F127 were two and three times higher, respectively, than over lone WO3·H2O. These findings highlight the potential of these composites as promising building blocks for photocatalytic water-splitting systems.
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.