Construction of Dual Active-Site NH2-MIL-125(Ti) for Efficient Selective Oxidation of Cyclohexylamine to Cyclohexanone Oxime

环己胺 环己酮 环己酮肟 化学 环己醇 活动站点 无机化学 催化作用 有机化学
作者
Weijian Ni,Xiang Liu,Qian Yang,Zhongliang Li,Jinfeng Fu,Liang Tan,Jiaming Zhang,Jian Liu
出处
期刊:Langmuir [American Chemical Society]
标识
DOI:10.1021/acs.langmuir.4c04786
摘要

In this work, dual active-site Ti-incorporated metal-organic frameworks (MIL-125 and NH2-MIL-125) were synthesized by a simple solvothermal process and applied to prepare cyclohexanone oxime from cyclohexylamine oxidation. A low-temperature thermal calcination strategy was used for the modulation of surface properties while maintaining the crystal structure and morphology. The results demonstrated that novel bifunctional NH2-MIL-125@250 °C obtained from thermal calcination possessed a large surface area with both oxygen vacancies and surface hydroxyl-active sites, promoting the adsorption and activation of cyclohexylamine and oxygen molecules, respectively. Under the optimum conditions, the cyclohexylamine conversion was 44.3%, and the selectivity to cyclohexanone oxime was 83.0%. By comparison, the stability of MIL-125 and NH2-MIL-125 was investigated separately in cyclic tests, and the crystal structure and catalytic properties of NH2-MIL-125 have been shown to be more stable than those of MIL-125. Combined with density functional theory, it was further shown that NH2-MIL-125 displayed a higher adsorption and activation ability toward cyclohexylamine and oxygen than MIL-125 and had a more stable metal-organic ligand structure. Finally, a plausible reaction pathway for selective cyclohexylamine oxidation to cyclohexanone oxime was proposed. This work can give new insights into designing novel dual active-site catalysts for the efficient catalytic transformation of organic primary amines to corresponding oximes.
最长约 10秒,即可获得该文献文件

科研通智能强力驱动
Strongly Powered by AbleSci AI
更新
PDF的下载单位、IP信息已删除 (2025-6-4)

科研通是完全免费的文献互助平台,具备全网最快的应助速度,最高的求助完成率。 对每一个文献求助,科研通都将尽心尽力,给求助人一个满意的交代。
实时播报
welch完成签到,获得积分10
1秒前
FashionBoy应助要减肥的香芦采纳,获得10
1秒前
dudu发布了新的文献求助10
1秒前
欣喜的书芹完成签到 ,获得积分10
2秒前
2秒前
doby完成签到,获得积分10
2秒前
今后应助Cookies采纳,获得10
3秒前
斯文败类应助gaomingquan采纳,获得10
3秒前
3秒前
3秒前
大模型应助cj采纳,获得10
3秒前
今后应助英勇的滑板采纳,获得10
4秒前
情怀应助林月采纳,获得10
4秒前
4秒前
马明旋完成签到,获得积分20
5秒前
镜花水月发布了新的文献求助20
5秒前
充电宝应助小巧雁菱采纳,获得10
5秒前
TH发布了新的文献求助10
5秒前
zzzz发布了新的文献求助10
6秒前
6秒前
Gaia发布了新的文献求助10
7秒前
今后应助陈成采纳,获得10
7秒前
兴奋笑阳发布了新的文献求助10
7秒前
7秒前
Akim应助panda采纳,获得10
7秒前
成成发布了新的文献求助10
8秒前
Banbor2021完成签到,获得积分10
8秒前
8秒前
abc123发布了新的文献求助10
8秒前
cgliuhx发布了新的文献求助10
8秒前
自信板栗发布了新的文献求助10
9秒前
吃鸡腿吗完成签到,获得积分10
9秒前
10秒前
苯二氮卓发布了新的文献求助20
10秒前
菜头完成签到,获得积分10
10秒前
binxman发布了新的文献求助10
10秒前
成功应助jiajia采纳,获得10
11秒前
我爱Chem发布了新的文献求助10
12秒前
14秒前
17完成签到,获得积分10
14秒前
高分求助中
Picture Books with Same-sex Parented Families: Unintentional Censorship 700
ACSM’s Guidelines for Exercise Testing and Prescription, 12th edition 500
Nucleophilic substitution in azasydnone-modified dinitroanisoles 500
不知道标题是什么 500
Indomethacinのヒトにおける経皮吸収 400
Phylogenetic study of the order Polydesmida (Myriapoda: Diplopoda) 370
Effective Learning and Mental Wellbeing 300
热门求助领域 (近24小时)
化学 材料科学 医学 生物 工程类 有机化学 生物化学 物理 内科学 纳米技术 计算机科学 化学工程 复合材料 遗传学 基因 物理化学 催化作用 冶金 细胞生物学 免疫学
热门帖子
关注 科研通微信公众号,转发送积分 3974882
求助须知:如何正确求助?哪些是违规求助? 3519431
关于积分的说明 11198315
捐赠科研通 3255698
什么是DOI,文献DOI怎么找? 1797904
邀请新用户注册赠送积分活动 877237
科研通“疑难数据库(出版商)”最低求助积分说明 806219