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Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon

文献类型：期刊论文

作者Ding, Yuxiao2,3; Zhang, Pengfei3; Xiong, Hailong1; Sun, Xiaoyan2,4; Klyushin, Alexander5; Zhang, Bingsen6; Liu, Zigeng7; Zhang, Jinshui3; Zhu, Huiyuan3; Qiao, Zhen-An1
刊名GREEN CHEMISTRY
出版日期2020-09-21
卷号22期号:18页码:6025-6032
ISSN号1463-9262
DOI10.1039/d0gc01717e
通讯作者Qiao, Zhen-An(qiaozhenan@jlu.edu.cn) ; Heumann, Saskia(saskia.heumann@cec.mpg.de) ; Dai, Sheng(dais@ornl.gov)
英文摘要The development of environmentally benign catalysts for highly regioselective hydroxylation of phenol remains an unsolved challenge in both industry and academia because the electrophilic substitution of phenol simultaneously occurs on both ortho- and para-positions. Herein, we report a designed atomically dispersed iron-based heterogeneous catalyst, in which the iron species is coordinated by a functionalized ionic liquid monolayer on carbon nanotubes. The catalyst exhibits an unprecedented level of regioselectivity (>99%) towards the hydroxylation of phenol and displays a much better activity (TOF towards catechol productivity, 1.79 s(-1)) compared to the homogeneous free ion system (TOF towards catechol productivity, 0.44 s(-1)). Both experimental and theoretical investigations confirm that the catalytic oxidation with hydroperoxide undergoes a non-radical addition process and substitutes only the ortho-positions of phenol. This finding provides not only a quite active and selective catalyst for industrially very important reactions, but also a promising methodology of designing biomimetic iron-based heterogeneous catalysts at the atomic level.
资助项目Max Planck Society ; National Natural Science Foundation of China[21671073] ; National Natural Science Foundation of China[21621001] ; 111 Project of the Ministry of Education of China[B17020] ; Program for JLU Science and Technology Innovative Research Team
WOS研究方向Chemistry ; Science & Technology - Other Topics
语种英语
WOS记录号WOS:000571356300033
出版者ROYAL SOC CHEMISTRY
资助机构Max Planck Society ; National Natural Science Foundation of China ; 111 Project of the Ministry of Education of China ; Program for JLU Science and Technology Innovative Research Team
源URL[http://ir.imr.ac.cn/handle/321006/140593]  
专题金属研究所_中国科学院金属研究所
通讯作者Qiao, Zhen-An; Heumann, Saskia; Dai, Sheng
作者单位1.Jilin Univ, State Key Lab Inorgan Synth & Preparat Chem, 2699 Qianjin St, Changchun 130012, Peoples R China
2.Max Planck Inst Chem Enery Convers, Stillstr 43-34, D-45470 Mulheim, Germany
3.Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA
4.Tech Univ Berlin, Inst Chem, Str 17 Juni 135, D-10623 Berlin, Germany
5.Fritz Haber Inst Max Planck Gesell, Faradayweg 4-6, D-14195 Berlin, Germany
6.Chinese Acad Sci, Inst Met Res, Shenyang 110016, Peoples R China
7.Forschungzentrum Julich, Inst Energy & Climate Res, Ostring O10, D-52425 Julich, Germany
推荐引用方式
GB/T 7714		 Ding, Yuxiao,Zhang, Pengfei,Xiong, Hailong,et al. Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon[J]. GREEN CHEMISTRY,2020,22(18):6025-6032.
APA Ding, Yuxiao.,Zhang, Pengfei.,Xiong, Hailong.,Sun, Xiaoyan.,Klyushin, Alexander.,...&Dai, Sheng.(2020).Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon.GREEN CHEMISTRY,22(18),6025-6032.
MLA Ding, Yuxiao,et al."Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon".GREEN CHEMISTRY 22.18(2020):6025-6032.

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来源：金属研究所

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