Interwoven Molecular Chains Obtained by Ionic Self-Assembly of Two Iron(III) Porphyrins with Opposite and Mismatched Charges

doi:10.1021/acsami.9b07460

	Interwoven Molecular Chains Obtained by Ionic Self-Assembly of Two Iron(III) Porphyrins with Opposite and Mismatched Charges
	Xie, Yan 2,3; Zhong, Qinglu 1,4; Lv, Yang 2; Li, Jia 2; Hao, Zhiqiang 2; Tang, Chizhou 3,4; Wei, Xuming 3; Su, Yang 3; Huang, Jiahui 3; Wang, Anjie 2
刊名	ACS APPLIED MATERIALS & INTERFACES
	2019-09-18
卷号	11 期号:37 页码:34203-34211
关键词	porphyrin electrocatalysts ionic self-assembly oxygen reduction reaction molecular dynamics simulation
ISSN号	1944-8244
DOI	10.1021/acsami.9b07460
通讯作者	Li, Guohui(ghli@dicp.ac.cn) ; Song, Yujiang(yjsong@dlut.edu.cn)
英文摘要	We report ionic self-assembly of positively charged Fe-III meso-tetra(N-methyl-4-pyridyl) porphyrin ((FeNMePyP)-N-III) with negatively charged Fe-III meso-tetra(4-sulfonatophenyl) porphyrin ((FeTPPS4)-T-III), leading to the formation of flower-like nanostructures composed of unprecedented three-dimensional (3D) entangled chains of porphyrin dimers. Molecular dynamics (MD) simulations show that the 3D entanglement of porphyrin chains closely correlates to mismatched charges present in porphyrin dimers like [Fe-III(H2O)(2) NMePyP](5+)/[Fe-III(H2O)(2)TPPS4](3-) that requires extra interactions or entanglement with neighboring ones to achieve electric neutrality. Interestingly, the inter- woven chains bring in excellent thermal stability as evidenced by well maintenance of the flower-like morphology after pyrolysis at 775 degrees C in argon, which is in good agreement of high-temperature MD simulations. Meanwhile, heat treatment of the flower-like porphyrin nanostructure leads to the formation of a non-noble metal electrocatalyst (NNME) with largely inherited morphology. This exemplifies a new approach by combining ionic self-assembly with subsequent pyrolysis for the synthesis of NNMEs with desired control over the morphology of template-free NNMEs that has rarely been achieved prior to this study. Furthermore, our electrocatalyst exhibits excellent activity and durability toward oxygen reduction reaction as well as much better methanol tolerance compared with commercial Pt/C in alkaline solutions.
资助项目	National Key Research & Development Program of China[2016YFB0101307] ; National Natural Science Fund of China[91430110] ; National Natural Science Fund of China[21606219] ; Liaoning BaiQianWan Talents Program[201519] ; Program for Liaoning Excellent Talents in University[LR2015014] ; Dalian Excellent Young Scientific and Technological Talents[2015R006] ; Fundamental Research Funds for the Central Universities[DUT19ZD208] ; Fundamental Research Funds for the Central Universities[DUT1SRC(3)001] ; Fundamental Research Funds for the Central Universities[DUT1SZD225]
WOS关键词	OXYGEN REDUCTION REACTION ; N-DOPED CARBON ; ELECTROCATALYSTS ; GRAPHENE ; PERFORMANCE ; DURABILITY ; CATALYST ; OXIDE ; NANOPARTICLES ; DESIGN
WOS研究方向	Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000487179900074
资助机构	National Key Research & Development Program of China ; National Key Research & Development Program of China ; National Natural Science Fund of China ; National Natural Science Fund of China ; Liaoning BaiQianWan Talents Program ; Liaoning BaiQianWan Talents Program ; Program for Liaoning Excellent Talents in University ; Program for Liaoning Excellent Talents in University ; Dalian Excellent Young Scientific and Technological Talents ; Dalian Excellent Young Scientific and Technological Talents ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research & Development Program of China ; National Key Research & Development Program of China ; National Natural Science Fund of China ; National Natural Science Fund of China ; Liaoning BaiQianWan Talents Program ; Liaoning BaiQianWan Talents Program ; Program for Liaoning Excellent Talents in University ; Program for Liaoning Excellent Talents in University ; Dalian Excellent Young Scientific and Technological Talents ; Dalian Excellent Young Scientific and Technological Talents ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research & Development Program of China ; National Key Research & Development Program of China ; National Natural Science Fund of China ; National Natural Science Fund of China ; Liaoning BaiQianWan Talents Program ; Liaoning BaiQianWan Talents Program ; Program for Liaoning Excellent Talents in University ; Program for Liaoning Excellent Talents in University ; Dalian Excellent Young Scientific and Technological Talents ; Dalian Excellent Young Scientific and Technological Talents ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research & Development Program of China ; National Key Research & Development Program of China ; National Natural Science Fund of China ; National Natural Science Fund of China ; Liaoning BaiQianWan Talents Program ; Liaoning BaiQianWan Talents Program ; Program for Liaoning Excellent Talents in University ; Program for Liaoning Excellent Talents in University ; Dalian Excellent Young Scientific and Technological Talents ; Dalian Excellent Young Scientific and Technological Talents ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/172881]
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	Li, Guohui; Song, Yujiang
作者单位	1.Chinese Acad Sci, Lab Mol Modeling & Design, State Key Lab Mol React Dynam, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 4.Univ Chinese Acad Sci, 19 A Yuquan Rd, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Xie, Yan,Zhong, Qinglu,Lv, Yang,et al. Interwoven Molecular Chains Obtained by Ionic Self-Assembly of Two Iron(III) Porphyrins with Opposite and Mismatched Charges[J]. ACS APPLIED MATERIALS & INTERFACES,2019,11(37):34203-34211.
APA	Xie, Yan.,Zhong, Qinglu.,Lv, Yang.,Li, Jia.,Hao, Zhiqiang.,...&Song, Yujiang.(2019).Interwoven Molecular Chains Obtained by Ionic Self-Assembly of Two Iron(III) Porphyrins with Opposite and Mismatched Charges.ACS APPLIED MATERIALS & INTERFACES,11(37),34203-34211.
MLA	Xie, Yan,et al."Interwoven Molecular Chains Obtained by Ionic Self-Assembly of Two Iron(III) Porphyrins with Opposite and Mismatched Charges".ACS APPLIED MATERIALS & INTERFACES 11.37(2019):34203-34211.