Compositionally engineered Cd–Mo–Se alloyed QDs toward photocatalytic H2O2 production and Cr(vi) reduction with a detailed mechanism and influencing parameters†

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR
Jyotirmayee Sahu, Sriram Mansingh, Bhagyashree Priyadarshini Mishra, Deeptimayee Prusty and Kulamani Parida
{"title":"Compositionally engineered Cd–Mo–Se alloyed QDs toward photocatalytic H2O2 production and Cr(vi) reduction with a detailed mechanism and influencing parameters†","authors":"Jyotirmayee Sahu, Sriram Mansingh, Bhagyashree Priyadarshini Mishra, Deeptimayee Prusty and Kulamani Parida","doi":"10.1039/D3DT02555A","DOIUrl":null,"url":null,"abstract":"<p >With the exceptional advantages of safety, greenness, and low cost, photocatalytic H<small><sub>2</sub></small>O<small><sub>2</sub></small> generation has kindled a wonderful spark, although being severely hampered by the terrible photoinduced exciton recombination, migration, and surface decomposition. Here, employing reflux method, the Cd–Mo–Se quantum dots of varying molar ratios of Cd and Mo were synthesized using thioglycolic acid as the capping ligand to regulate their growth. This type of metal alloying promotes rapid charge migration, improves light harvesting, and reduces the rate of charge recombination. The improved optoelectronic properties and boosted activity of Cd-rich ternary CMSe-1 QDs led to the observed exceptional photocatalytic H<small><sub>2</sub></small>O<small><sub>2</sub></small> yield of 1403.5 μmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small> (solar to chemical conversion efficiency, 0.27%) under visible light, outperforming the other ternary and Se-based QD photocatalysts. Additionally, CMSe-1 shows 93.6% (2 h) hazardous Cr(<small>VI</small>) photoreduction. The enhanced catalytic performance of CMSe-1 corresponds to effective charge carrier separation and transfer efficiency, well supported by PL, TRPL, and electrochemical measurements. Photocatalytic H<small><sub>2</sub></small>O<small><sub>2</sub></small> production was also studied under varying experimental conditions and the scavenger test suggests a superoxide radical intermediate 2-step single electron reduction pathway. The catalyst-assisted Cr(<small>VI</small>) reduction is substantiated by the zero-order kinetics as well as the determination of the pH<small><sub>PZC</sub></small> value. The catalyst can be employed for a maximum of four times while retaining its activity, according to the photostability and reusability test outcomes. This research presents interesting approaches for producing ternary QDs and modified systems for efficient photocatalytic H<small><sub>2</sub></small>O<small><sub>2</sub></small> production and Cr(<small>VI</small>) reduction.</p>","PeriodicalId":71,"journal":{"name":"Dalton Transactions","volume":" 44","pages":" 16525-16537"},"PeriodicalIF":3.5000,"publicationDate":"2023-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/dt/d3dt02555a?page=search","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Dalton Transactions","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2023/dt/d3dt02555a","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0

Abstract

With the exceptional advantages of safety, greenness, and low cost, photocatalytic H2O2 generation has kindled a wonderful spark, although being severely hampered by the terrible photoinduced exciton recombination, migration, and surface decomposition. Here, employing reflux method, the Cd–Mo–Se quantum dots of varying molar ratios of Cd and Mo were synthesized using thioglycolic acid as the capping ligand to regulate their growth. This type of metal alloying promotes rapid charge migration, improves light harvesting, and reduces the rate of charge recombination. The improved optoelectronic properties and boosted activity of Cd-rich ternary CMSe-1 QDs led to the observed exceptional photocatalytic H2O2 yield of 1403.5 μmol g−1 h−1 (solar to chemical conversion efficiency, 0.27%) under visible light, outperforming the other ternary and Se-based QD photocatalysts. Additionally, CMSe-1 shows 93.6% (2 h) hazardous Cr(VI) photoreduction. The enhanced catalytic performance of CMSe-1 corresponds to effective charge carrier separation and transfer efficiency, well supported by PL, TRPL, and electrochemical measurements. Photocatalytic H2O2 production was also studied under varying experimental conditions and the scavenger test suggests a superoxide radical intermediate 2-step single electron reduction pathway. The catalyst-assisted Cr(VI) reduction is substantiated by the zero-order kinetics as well as the determination of the pHPZC value. The catalyst can be employed for a maximum of four times while retaining its activity, according to the photostability and reusability test outcomes. This research presents interesting approaches for producing ternary QDs and modified systems for efficient photocatalytic H2O2 production and Cr(VI) reduction.

Abstract Image

组成工程化Cd-Mo-Se合金量子点用于光催化H2O2生成和Cr(VI)还原,详细的机理和影响参数。
尽管受到可怕的光诱导激子复合、迁移和表面分解的严重阻碍,但光催化H2O2的产生凭借其安全、绿色和低成本的独特优势,点燃了奇妙的火花。本文以巯基乙酸为封端配体,采用回流法合成了不同Cd和Mo摩尔比的Cd-Mo-Se量子点,以调节其生长。这种类型的金属合金化促进了电荷的快速迁移,改善了光捕获,并降低了电荷复合的速率。富镉三元CMSe-1量子点的光电性能和活性的提高导致在可见光下观察到的优异的光催化H2O2产率为1403.5μmol g-1 h-1(太阳能到化学转化效率,0.27%),优于其他三元和Se基量子点光催化剂。此外,CMSe-1显示93.6%(2小时)的有害Cr(VI)光还原。CMSe-1增强的催化性能对应于有效的电荷载流子分离和转移效率,PL、TRPL和电化学测量很好地支持了这一点。在不同的实验条件下还研究了光催化H2O2的产生,清除剂测试表明超氧化物自由基中间体是两步单电子还原途径。催化剂辅助的Cr(VI)还原通过零级动力学以及pHPZC值的测定得到证实。根据光稳定性和可重复使用性测试结果,该催化剂最多可使用四次,同时保持其活性。这项研究为生产三元量子点提供了有趣的方法,并为有效的光催化H2O2生产和Cr(VI)还原提供了改性系统。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
×
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
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
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 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信