通过基于 S-Scheme 的 2D-2D WS2/掺硫 g-C3N4 异质结改善电荷载流子分离,实现卓越的光催化氧气还原反应

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL ACS Applied Energy Materials Pub Date : 2024-08-01 DOI:10.1021/acsaem.4c0106110.1021/acsaem.4c01061
Kundan Kumar Das, Upali Aparajita Mohanty, Ritik Mohanty, Preeti Prabha Sarangi, Dipti Prava Sahoo and Kulamani Parida*, 
{"title":"通过基于 S-Scheme 的 2D-2D WS2/掺硫 g-C3N4 异质结改善电荷载流子分离,实现卓越的光催化氧气还原反应","authors":"Kundan Kumar Das,&nbsp;Upali Aparajita Mohanty,&nbsp;Ritik Mohanty,&nbsp;Preeti Prabha Sarangi,&nbsp;Dipti Prava Sahoo and Kulamani Parida*,&nbsp;","doi":"10.1021/acsaem.4c0106110.1021/acsaem.4c01061","DOIUrl":null,"url":null,"abstract":"<p >Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation via a photocatalytic O<sub>2</sub> reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H<sub>2</sub>O<sub>2</sub> production is restricted because of sluggish reaction kinetics and fast recombination of photoinduced excitons. Therefore, a superior two-dimensional (2D)–2D WS<sub>2</sub>/sulfur-doped g-C<sub>3</sub>N<sub>4</sub> (WSCN) hybrid material was successfully fabricated to address the associated limitations through a combination of wet impregnation and calcination techniques for H<sub>2</sub>O<sub>2</sub> production. The effective anchoring of WS<sub>2</sub> nanoplates onto sulfur-doped g-C<sub>3</sub>N<sub>4</sub> (SCN) nanosheets facilitates effective separation of photoinduced excitons with sturdy redox properties, which is attributable to the establishment of S-scheme heterojunctions between WS<sub>2</sub> and SCN through W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. The W–S bond at the interface acts as a bridge for effective charge segregation pathways. Among all, 2.5 WSCN displays an exceptional H<sub>2</sub>O<sub>2</sub> production of 817 μmol, which was 7.9- and 2.68-fold higher than those of pristine WS<sub>2</sub> and SCN, respectively. The solar-to-chemical conversion efficiency was found to be 0.24%, whereas the apparent quantum yield was estimated to be 3.19% at 420 nm irradiation. The improved photocatalytic activity was figured out by a higher cathodic photocurrent of −1.51 mA cm<sup>–2</sup> and delayed recombination of excitons, as supported by photoluminescence and electrochemical impedance spectroscopy measurements. The S-scheme charge-transfer pathway was well validated by a radical scavenging experiment and work function, which was evaluated from VB-XPS analysis and in situ XPS measurement. This research offers a paradigmatic idea for constructing an S-scheme photocatalyst for H<sub>2</sub>O<sub>2</sub> generation.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Improving Charge Carrier Separation through S-Scheme-Based 2D–2D WS2/Sulfur-Doped g-C3N4 Heterojunctions for a Superior Photocatalytic O2 Reduction Reaction\",\"authors\":\"Kundan Kumar Das,&nbsp;Upali Aparajita Mohanty,&nbsp;Ritik Mohanty,&nbsp;Preeti Prabha Sarangi,&nbsp;Dipti Prava Sahoo and Kulamani Parida*,&nbsp;\",\"doi\":\"10.1021/acsaem.4c0106110.1021/acsaem.4c01061\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation via a photocatalytic O<sub>2</sub> reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H<sub>2</sub>O<sub>2</sub> production is restricted because of sluggish reaction kinetics and fast recombination of photoinduced excitons. Therefore, a superior two-dimensional (2D)–2D WS<sub>2</sub>/sulfur-doped g-C<sub>3</sub>N<sub>4</sub> (WSCN) hybrid material was successfully fabricated to address the associated limitations through a combination of wet impregnation and calcination techniques for H<sub>2</sub>O<sub>2</sub> production. The effective anchoring of WS<sub>2</sub> nanoplates onto sulfur-doped g-C<sub>3</sub>N<sub>4</sub> (SCN) nanosheets facilitates effective separation of photoinduced excitons with sturdy redox properties, which is attributable to the establishment of S-scheme heterojunctions between WS<sub>2</sub> and SCN through W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. The W–S bond at the interface acts as a bridge for effective charge segregation pathways. Among all, 2.5 WSCN displays an exceptional H<sub>2</sub>O<sub>2</sub> production of 817 μmol, which was 7.9- and 2.68-fold higher than those of pristine WS<sub>2</sub> and SCN, respectively. The solar-to-chemical conversion efficiency was found to be 0.24%, whereas the apparent quantum yield was estimated to be 3.19% at 420 nm irradiation. The improved photocatalytic activity was figured out by a higher cathodic photocurrent of −1.51 mA cm<sup>–2</sup> and delayed recombination of excitons, as supported by photoluminescence and electrochemical impedance spectroscopy measurements. The S-scheme charge-transfer pathway was well validated by a radical scavenging experiment and work function, which was evaluated from VB-XPS analysis and in situ XPS measurement. This research offers a paradigmatic idea for constructing an S-scheme photocatalyst for H<sub>2</sub>O<sub>2</sub> generation.</p>\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-08-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsaem.4c01061\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsaem.4c01061","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

通过光催化氧化还原反应生成过氧化氢(H2O2)一直被认为是一种经济高效且环保的合成方法。然而,由于反应动力学迟缓以及光诱导激子的快速重组,H2O2 的生产率受到了限制。因此,为了解决相关的局限性,我们通过湿法浸渍和煅烧技术相结合的方法,成功制备了一种优异的二维(2D)-2D WS2/掺硫 g-C3N4 (WSCN)杂化材料,用于生产 H2O2。WS2 纳米板有效地锚定在掺硫 g-C3N4 (SCN) 纳米片上,促进了光诱导激子的有效分离,并具有坚固的氧化还原特性,这归功于 WS2 和 SCN 之间通过 W-S 键建立的 S 型异质结,X 射线光电子能谱 (XPS) 分析证实了这一点。界面上的 W-S 键充当了有效电荷隔离途径的桥梁。其中,2.5 WSCN 的 H2O2 生成量高达 817 μmol,分别是原始 WS2 和 SCN 的 7.9 倍和 2.68 倍。在 420 纳米波长的照射下,太阳能到化学物质的转化效率为 0.24%,而表观量子产率估计为 3.19%。光致发光和电化学阻抗光谱测量结果表明,阴极光电流为 -1.51 mA cm-2,激子延迟重组,从而提高了光催化活性。通过自由基清除实验和功函数,以及 VB-XPS 分析和原位 XPS 测量评估,S 型电荷转移途径得到了很好的验证。这项研究为构建用于生成 H2O2 的 S 型光催化剂提供了一个范例。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Improving Charge Carrier Separation through S-Scheme-Based 2D–2D WS2/Sulfur-Doped g-C3N4 Heterojunctions for a Superior Photocatalytic O2 Reduction Reaction

Hydrogen peroxide (H2O2) generation via a photocatalytic O2 reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H2O2 production is restricted because of sluggish reaction kinetics and fast recombination of photoinduced excitons. Therefore, a superior two-dimensional (2D)–2D WS2/sulfur-doped g-C3N4 (WSCN) hybrid material was successfully fabricated to address the associated limitations through a combination of wet impregnation and calcination techniques for H2O2 production. The effective anchoring of WS2 nanoplates onto sulfur-doped g-C3N4 (SCN) nanosheets facilitates effective separation of photoinduced excitons with sturdy redox properties, which is attributable to the establishment of S-scheme heterojunctions between WS2 and SCN through W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. The W–S bond at the interface acts as a bridge for effective charge segregation pathways. Among all, 2.5 WSCN displays an exceptional H2O2 production of 817 μmol, which was 7.9- and 2.68-fold higher than those of pristine WS2 and SCN, respectively. The solar-to-chemical conversion efficiency was found to be 0.24%, whereas the apparent quantum yield was estimated to be 3.19% at 420 nm irradiation. The improved photocatalytic activity was figured out by a higher cathodic photocurrent of −1.51 mA cm–2 and delayed recombination of excitons, as supported by photoluminescence and electrochemical impedance spectroscopy measurements. The S-scheme charge-transfer pathway was well validated by a radical scavenging experiment and work function, which was evaluated from VB-XPS analysis and in situ XPS measurement. This research offers a paradigmatic idea for constructing an S-scheme photocatalyst for H2O2 generation.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
期刊最新文献
Issue Editorial Masthead Issue Publication Information Organic Battery Materials Fe-Induced Surface Regulation and Accelerated Hydrogen Evolution Kinetics in γ-MnS Three-Dimensional Microarchitectures Unprecedented InOOH Hexagonal Nanoplates for Highly Selective Synthesis of Methanol via Moderately Photothermal CO2 Hydrogenation
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1