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Sequence-sorted redox-switchable hetero[3]rotaxanes

Organic Chemistry Frontiers 2022年第1期9卷 64-74页

作者： Marius Gaedke Henrik Hupatz Felix Witte Susanne M.Rupf Clara Douglas Hendrik V.Schröder Lukas Fischer Moritz Malischewski beate paulus Christoph A.Schalley Institut für Chemie und Biochemie der Freien Universität Berlin Arnimallee 2014195 BerlinGermany Institut für Chemie und Biochemie der Freien Universität Berlin Arnimallee 2214195 BerlinGermany Institut für Chemie und Biochemie der Freien Universität Berlin Fabeckstr.34/3614195 BerlinGermany

From a library of five crown ether macrocycles with different ring sizes and redox-active moieties,such as tetrathiafulvalene(TTF)and naphthalene dimiide(NDI),directional heterocircuit[3]rotaxanes were *** an axle with two binding sites with different steric accessibility,the concept of integrative self-sorting was applied to program the sequence of functional units in heteropseudo[3]*** on binding strength and ring size of the smaller macrocycles,different heteropseudo[3]rotaxane selectivities and stabilities were determined by 2D NMR spectroscopy and tandem mass spectrometry.A heteropseudo[3]rotaxane with rotaxane-like behaviour was isolated chromatographically,displaying electrochemically“frustrated”properties.A robust synthetic procedure was developed allowing the synthesis of four new hetero[3]rotaxanes incorporating specific sequences of functional *** pseudoisomeric rotaxanes which have the naphthalene diimide subunit at two different positions show distinct electrochemical *** calculations suggest that this differences could arise from a folding of the structure,in which the redox-active moieties stack with a stopper *** study presents a blueprint for the construction of hetero[3]rotaxanes with sequential control of the functional units along the track of the axle and paves the way to extend the functionality of mechanically interlocked molecules.

关键词： properties redox Sequence

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Activating coordinative conjugated polymer via interfacial electron transfer for efficient CO_(2) electroreduction

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能源化学:英文版 2023年第8期83卷 313-323,I0009页

作者： Jing Zhang Jia-Jun Dai De-Quan Cao Heng Xu Xing-Yu Ding Chun-Hua Zhen beate paulus Jin-Yu Ye Qian Liang Jun-Ke Liu Shi-Jun Xie Sai-Sai Deng Zhen Wang Jun-Tao Li Yao Zhou Shi-Gang Sun College of Energy XiamenUniversityXiamen 361005FujianChina College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005FujianChina Institute of Chemistry and Biochemistry Freie Universitat BerlinArnimallee 2214195 BerlinGermany

With tunable local electronic environment,high mass density of MN4sites,and ease of preparation,metal-organic conjugated coordinative polymer(CCP) with inherent electronic conductivity provides a promising alternative to the well-known M-N-C ***,the coordination reaction between Cu^(2+)and 1,2,4,5-tetraaminobenzene(TAB) was conducted on the surface of metallic Cu nanowires,forming a thin layer of CuN4-based CCP(Cu-TAB) on the Cu *** importantly,interfacial transfer of electrons from Cu core to the CuN4-based CCP nanoshell was observed within the resulting CuTAB@Cu,which was found to enrich the local electronic density of the *** such,the CuTAB@Cu demonstrates much improved affinity to the*COOH intermediate formed from the rate determining step;the energy barrier for C-C coupling,which is critical to convert CO_(2)into C2products,is also ***,it delivers a current density of-9.1 mA cm^(-2)at a potential as high as 0.558 V(***) in H-type cell and a Faraday efficiency of 46.4% for *** work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN4-based CCPs for efficient electroreduction of CO_(2).

关键词： Metal-organic solid compounds Conjugated coordinative polymer Solid-solid interfacial electron transfer MN_(4)sites Electrocatalysis

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