ZIF-8 衍生的 Ag/ZnO 光催化剂具有富集的 Ag-ZnO 界面,可将甲烷有效氧化为液态含氧化合物,同时具有毫摩尔级的生产率和 ∼100 % 的选择性

Yingdong Hao, Yonghui Zhao, Chunlai Zhang, Xinqing Chen, Nannan Sun, Wei Wei
{"title":"ZIF-8 衍生的 Ag/ZnO 光催化剂具有富集的 Ag-ZnO 界面,可将甲烷有效氧化为液态含氧化合物,同时具有毫摩尔级的生产率和 ∼100 % 的选择性","authors":"Yingdong Hao, Yonghui Zhao, Chunlai Zhang, Xinqing Chen, Nannan Sun, Wei Wei","doi":"10.1016/j.apcatb.2024.124505","DOIUrl":null,"url":null,"abstract":"Achieving a high yield of oxygenates and inhibiting overoxidation remain challenging for CH photooxidation. Here, we report a catalyst with enriched Ag-ZnO interfaces by using ZIF-8 as the precursor. The resulting Ag/Z-450 photocatalysts show extraordinary efficiency in the photocatalytic oxidation of CH, a high liquid oxygenate yield of 57.88 mmol·g (28.94 mmol·g·h) and a selectivity of ∼100 % were obtained over 3.0Ag/Z-450, with HCHO as the major product (41.04 mmol·g, ∼71 % selectivity). Mechanistic studies revealed that ZnO and Ag species acted as electron donors and acceptors, respectively, which enhanced charge carriers transfer and separation. CH and O can be effectively activated to generate •CH and reactive oxygen species (ROS), their following reaction led to formation of CHOOH, which can be further converted to CHOH and HCHO. This work contributes to the development of a “two-in-one” CH photooxidation catalyst system that simultaneously achieves unparallel productivity and selectivity.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"23 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"ZIF-8 derived Ag/ZnO photocatalyst with enriched Ag-ZnO interface for effective oxidation of methane to liquid oxygenates with simultaneous mmol-scale productivity and ∼100 % selectivity\",\"authors\":\"Yingdong Hao, Yonghui Zhao, Chunlai Zhang, Xinqing Chen, Nannan Sun, Wei Wei\",\"doi\":\"10.1016/j.apcatb.2024.124505\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Achieving a high yield of oxygenates and inhibiting overoxidation remain challenging for CH photooxidation. Here, we report a catalyst with enriched Ag-ZnO interfaces by using ZIF-8 as the precursor. The resulting Ag/Z-450 photocatalysts show extraordinary efficiency in the photocatalytic oxidation of CH, a high liquid oxygenate yield of 57.88 mmol·g (28.94 mmol·g·h) and a selectivity of ∼100 % were obtained over 3.0Ag/Z-450, with HCHO as the major product (41.04 mmol·g, ∼71 % selectivity). Mechanistic studies revealed that ZnO and Ag species acted as electron donors and acceptors, respectively, which enhanced charge carriers transfer and separation. CH and O can be effectively activated to generate •CH and reactive oxygen species (ROS), their following reaction led to formation of CHOOH, which can be further converted to CHOH and HCHO. This work contributes to the development of a “two-in-one” CH photooxidation catalyst system that simultaneously achieves unparallel productivity and selectivity.\",\"PeriodicalId\":516528,\"journal\":{\"name\":\"Applied Catalysis B: Environment and Energy\",\"volume\":\"23 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-08-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environment and Energy\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apcatb.2024.124505\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environment and Energy","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1016/j.apcatb.2024.124505","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0

摘要

实现高产氧率和抑制过氧化仍然是 CH 光氧化的挑战。在此,我们报告了一种以 ZIF-8 为前驱体、具有富集 Ag-ZnO 界面的催化剂。所制备的 Ag/Z-450 光催化剂在 CH 的光催化氧化过程中表现出非凡的效率,在 3.0Ag/Z-450 上可获得 57.88 mmol-g (28.94 mmol-g-h)的高液态含氧化合物产率和 ∼100 % 的选择性,其中 HCHO 为主要产物(41.04 mmol-g,∼71 % 的选择性)。机理研究表明,氧化锌和银分别作为电子供体和受体,促进了电荷载体的转移和分离。CH 和 O 可被有效激活,生成 -CH 和活性氧(ROS),它们的后续反应导致 CHOOH 的形成,而 CHOOH 又可进一步转化为 CHOH 和 HCHO。这项工作有助于开发一种 "二合一 "的 CH 光氧化催化剂系统,该系统可同时实现无与伦比的生产率和选择性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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
ZIF-8 derived Ag/ZnO photocatalyst with enriched Ag-ZnO interface for effective oxidation of methane to liquid oxygenates with simultaneous mmol-scale productivity and ∼100 % selectivity
Achieving a high yield of oxygenates and inhibiting overoxidation remain challenging for CH photooxidation. Here, we report a catalyst with enriched Ag-ZnO interfaces by using ZIF-8 as the precursor. The resulting Ag/Z-450 photocatalysts show extraordinary efficiency in the photocatalytic oxidation of CH, a high liquid oxygenate yield of 57.88 mmol·g (28.94 mmol·g·h) and a selectivity of ∼100 % were obtained over 3.0Ag/Z-450, with HCHO as the major product (41.04 mmol·g, ∼71 % selectivity). Mechanistic studies revealed that ZnO and Ag species acted as electron donors and acceptors, respectively, which enhanced charge carriers transfer and separation. CH and O can be effectively activated to generate •CH and reactive oxygen species (ROS), their following reaction led to formation of CHOOH, which can be further converted to CHOH and HCHO. This work contributes to the development of a “two-in-one” CH photooxidation catalyst system that simultaneously achieves unparallel productivity and selectivity.
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
自引率
0.00%
发文量
0
期刊最新文献
Unusually improved peracetic acid activation for ultrafast organic compound removal through redox-inert Mg incorporation into active Co3O4 Photoelectrocatalytic allylic C–H oxidation to allylic alcohols coupled with hydrogen evolution Unveiling O2 adsorption on non-metallic active site for selective photocatalytic H2O2 production At least five: Benefit origins of potassium and sodium co-doping on carbon nitride for integrating pharmaceuticals degradation and hydrogen peroxide production Efficient and selective electroreduction of nitrate to ammonia via interfacial engineering of B-doped Cu nanoneedles
×
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