金/氧化锌催化剂上氧空位促进的乙二醇氧化酯化反应生成乙醇酸甲酯

IF 6.3 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Applied Surface Science Pub Date : 2024-11-21 DOI:10.1016/j.apsusc.2024.161855
Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren
{"title":"金/氧化锌催化剂上氧空位促进的乙二醇氧化酯化反应生成乙醇酸甲酯","authors":"Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren","doi":"10.1016/j.apsusc.2024.161855","DOIUrl":null,"url":null,"abstract":"Au/ZnO-<em>x</em> with different morphologies were prepared by controlling the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> (<em>x</em>) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-<em>x</em> firstly increases and then decreases with the increase of the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub>, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (V<sub>o</sub><sup>+</sup>) accompanied with the highest <em>I</em><sub>100</sub>/<em>I</em><sub>101</sub> ratio at moderate (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> dosage, promoting the adsorption and dissociation of O<sub>2</sub> molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the V<sub>o</sub><sup>+</sup> and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"13 1","pages":""},"PeriodicalIF":6.3000,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Oxygen vacancies-promoted oxidative esterification of ethylene glycol to methyl glycolate over Au/ZnO catalyst\",\"authors\":\"Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren\",\"doi\":\"10.1016/j.apsusc.2024.161855\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Au/ZnO-<em>x</em> with different morphologies were prepared by controlling the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> (<em>x</em>) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-<em>x</em> firstly increases and then decreases with the increase of the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub>, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (V<sub>o</sub><sup>+</sup>) accompanied with the highest <em>I</em><sub>100</sub>/<em>I</em><sub>101</sub> ratio at moderate (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> dosage, promoting the adsorption and dissociation of O<sub>2</sub> molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the V<sub>o</sub><sup>+</sup> and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"13 1\",\"pages\":\"\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2024-11-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apsusc.2024.161855\",\"RegionNum\":2,\"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":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.apsusc.2024.161855","RegionNum":2,"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

利用沉积沉淀法,通过控制(NH4)2CO3(x)的用量制备了不同形貌的 Au/ZnO-x,并将其应用于甲醇和乙二醇(EG)一步氧化酯化制乙醇酸甲酯(MG)。Au/ZnO-x 的催化性能随着(NH4)2CO3 量的增加先增大后减小,在 Au/ZnO-4 中达到最大,EG 转化率为 89.6%,对 MG 的选择性为 96.4%,明显高于已报道的金基催化剂。这种优异的催化性能主要源于在中等(NH4)2CO3 用量下,氧空位浓度(Vo+)最高,同时 I100/I101 比值最大,促进了 O2 分子的吸附和解离。具体而言,(100)和(101)晶面之间不同的优先生长比分别导致 Au/ZnO-2、Au/ZnO-4 和 Au/ZnO-6 具有片状堆叠形态、有序层结构和不规则团簇。值得注意的是,研究发现 Vo+ 与 EG 转化率之间存在线性正相关。创新性地提出了氧空位催化 EG 氧化酯化反应的机理,为设计该反应的高效催化剂提供了新思路。
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
Oxygen vacancies-promoted oxidative esterification of ethylene glycol to methyl glycolate over Au/ZnO catalyst
Au/ZnO-x with different morphologies were prepared by controlling the amount of (NH4)2CO3 (x) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-x firstly increases and then decreases with the increase of the amount of (NH4)2CO3, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (Vo+) accompanied with the highest I100/I101 ratio at moderate (NH4)2CO3 dosage, promoting the adsorption and dissociation of O2 molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the Vo+ and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.
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
Applied Surface Science
Applied Surface Science 工程技术-材料科学:膜
CiteScore
12.50
自引率
7.50%
发文量
3393
审稿时长
67 days
期刊介绍: Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.
期刊最新文献
Synthesis and potent antibacterial activity of nano-CuFe2O4/MoS2@Ag composite under visible light Non-Fourier thermal spike effect on nanocrystalline Cu phase engineering Fully hot Air-Processed All-Inorganic CsPbI2Br perovskite solar cells for outdoor and indoor applications Designing core–shell LiNi0.5Mn1.5O4-based cathode materials with enhanced rate capability and improved cycling stability Fe/Co bimetallic borides with modified electronic structure for Efficient oxygen evolution reaction
×
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