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

doi:10.1039/d0gc01717e

IMR OpenIR

	Tuning regioselective oxidation toward phenol via atomically dispersed iron sites on carbon
	Ding, Yuxiao 1,2; Zhang, Pengfei 2; Xiong, Hailong 3; Sun, Xiaoyan 1,4; Klyushin, Alexander 5; Zhang, Bingsen 6; Liu, Zigeng 7; Zhang, Jinshui 2; Zhu, Huiyuan 2; Qiao, Zhen-An 3; Heumann, Saskia 1; Dai, Sheng 2
通讯作者	Qiao, Zhen-An(qiaozhenan@jlu.edu.cn) ; Heumann, Saskia(saskia.heumann@cec.mpg.de) ; Dai, Sheng(dais@ornl.gov)
	2020-09-21
发表期刊	GREEN CHEMISTRY
ISSN	1463-9262
卷号	22 期号:18 页码:6025-6032
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.
资助者	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
DOI	10.1039/d0gc01717e
收录类别	SCI
语种	英语
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
WOS类目	Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
WOS记录号	WOS:000571356300033
出版者	ROYAL SOC CHEMISTRY
引用统计	被引频次：9[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/140594
专题	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.Max Planck Inst Chem Enery Convers, Stillstr 43-34, D-45470 Mulheim, Germany 2.Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA 3.Jilin Univ, State Key Lab Inorgan Synth & Preparat Chem, 2699 Qianjin St, Changchun 130012, Peoples R China 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.