Single-atom Rh based bipyridine framework porous organic polymer: A high active and superb stable catalyst for heterogeneous methanol carbonylation

doi:10.1016/j.jcat.2018.11.015

	Single-atom Rh based bipyridine framework porous organic polymer: A high active and superb stable catalyst for heterogeneous methanol carbonylation
	Ren, Zhou 1,3; Liu, Yang 4; Lyu, Yuan 1; Song, Xiangen 1; Zheng, Changyong 1,3; Feng, Siquan 1,3; Jiang, Zheng 4; Ding, Yunjie 1,2
刊名	JOURNAL OF CATALYSIS
	2019
卷号	369 页码:249-256
关键词	Heterogeneous methanol carbonylation Porous organic ligands Rh-N coordination bonds Five-coordinated active center Single-atom catalyst
ISSN号	0021-9517
DOI	10.1016/j.jcat.2018.11.015
通讯作者	Lyu, Yuan(luyuan@dicp.ac.cn) ; Ding, Yunjie(dyj@dicp.ac.cn)
英文摘要	A novel Rh based porous composed N polymer with hierarchical pore, high surface area and high thermal stability (Rh-POL-2BPY) was successfully obtained by impregnation of Rh-2(CO)(4)Cl-2 solution of dichloromethane. And based on Rh species as the most active carbonylation site, Rh-POL-2BPY was selected as a catalyst applied in heterogeneous methanol carbonylation system and behaved excellent carbonylation activity (TOF approximate to 1400 h(-1)) under 195 degrees C, 2.5 MPa, higher than the corresponding homogeneous system without acetic acid. In addition, contrast to the most reported unstable heterogeneous methanol carbonylation systems, Rh-POL-2BPY could maintain incredibly outstanding stability for near 400 h owing to the firm coordination bond between Rh and N and high exposed N content in the polymer. Here, POL-2BPY apart from its heat-resisting property acts as massive rivets to immobilize the Rh species in its framework solidly during carbonylation process. XPS, XANES, HAADF-STEM and EXAFS results verify the N species of bipyridine, the single atom dispersion of Rh and Rh-N coordination bond. And above all, the novel five coordinated Rh center is proposed as the real active site of methanol carbonylation by EXAFS spectra. (C) 2018 Elsevier Inc. All rights reserved.
资助项目	National Key R&D Program of China[2017YFB0602203] ; SSRF, SINAP (Shanghai, China)[BL14W1] ; National Synchrotron Radiation Laboratory (NSRL, China)
WOS关键词	FIXED-BED HYDROFORMYLATION ; LIGAND ; MICROPOROSITY ; PALLADIUM
WOS研究方向	Chemistry ; Engineering
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000460711700026
资助机构	National Key R&D Program of China ; National Key R&D Program of China ; SSRF, SINAP (Shanghai, China) ; SSRF, SINAP (Shanghai, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Key R&D Program of China ; National Key R&D Program of China ; SSRF, SINAP (Shanghai, China) ; SSRF, SINAP (Shanghai, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Key R&D Program of China ; National Key R&D Program of China ; SSRF, SINAP (Shanghai, China) ; SSRF, SINAP (Shanghai, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Key R&D Program of China ; National Key R&D Program of China ; SSRF, SINAP (Shanghai, China) ; SSRF, SINAP (Shanghai, China) ; National Synchrotron Radiation Laboratory (NSRL, China) ; National Synchrotron Radiation Laboratory (NSRL, China)
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/165790]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Lyu, Yuan; Ding, Yunjie
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Liaoning, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Liaoning, Peoples R China 3.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China 4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
推荐引用方式 GB/T 7714	Ren, Zhou,Liu, Yang,Lyu, Yuan,et al. Single-atom Rh based bipyridine framework porous organic polymer: A high active and superb stable catalyst for heterogeneous methanol carbonylation[J]. JOURNAL OF CATALYSIS,2019,369:249-256.
APA	Ren, Zhou.,Liu, Yang.,Lyu, Yuan.,Song, Xiangen.,Zheng, Changyong.,...&Ding, Yunjie.(2019).Single-atom Rh based bipyridine framework porous organic polymer: A high active and superb stable catalyst for heterogeneous methanol carbonylation.JOURNAL OF CATALYSIS,369,249-256.
MLA	Ren, Zhou,et al."Single-atom Rh based bipyridine framework porous organic polymer: A high active and superb stable catalyst for heterogeneous methanol carbonylation".JOURNAL OF CATALYSIS 369(2019):249-256.