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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key Laboratory of materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University advanced Membranes and Porous materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology institute of Sustainability for chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Single atom catalyst Synergy effect Carbon catalyst Electrocatalysis

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Recent advances in new-type molecular switches

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Science China Chemistry 2015年第6期58卷 916-921页

作者： Hong Li Da-Hui Qu Key Laboratory for advanced materials and institute of Fine chemicals East China University of Science & Technology

Molecular switches that can undergo reversible switching between two or more different states in response to external stimuli have been used in the fabrication of various optoelectronic devices and smart materials for many decades, and also found many applications in sensing, molecular self-assembly and photo-controlled biological systems. Recently, mechanically interlocked molecules, such as rotaxanes and catenanes, and molecular rotary motors based on overcrowded alkenes have emerged as two new kinds of molecular switches. Some novel applications of above-mentioned molecular switches have been discovered. In this mini review, we mainly highlight noticeable achievements over the past decade in this field, and summarize the applications of new types of molecular switches, for instance, controlling the chiral space to regulate catalytic reaction as organocatalysts, controlling molecular motions, synthesizing a peptide in a sequence-specific manner and modulating the wettability of the self-assembled monolayers.

关键词： molecular switches rotaxane molecular motor stimuli-responsive function

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Electrochemical impedance spectroscopy study on the corrosion of the weld zone of 3Cr steel welded joints in CO_2 environments

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International Journal of Minerals,Metallurgy and materials 2015年第5期22卷 500-508页

作者： Li-ning Xu Jin-yang Zhu Min-xu Lu Lei Zhang Wei Chang Corrosion and Protection Center Key Laboratory for Environmental Fracture (MOE) Institute for Advanced Materials and Technology University of Science and Technology Beijing cnooc Research institute

The welded joints of 3Cr pipeline steel were fabricated with commercial welding wire using the gas tungsten arc welding （GTAW） technique. Potentiodynamic polarization curves, linear polarization resistance （LPR）, electrochemical impedance spectroscopy （EIS）, scan- ning electron microscopy （SEM）, and energy-dispersive spectrometry （EDS） were used to investigate the corrosion resistance and the growth of a corrosion film on the weld zone （WZ）. The changes in electrochemical characteristics of the film were obtained through fitting of the EIS data. The results showed that the average corrosion rate of the WZ in CO2 environments first increased, then fluctuated, and finally de- creased gradually. The formation of the film on the WZ was divided into three stages： dynamic adsorption, incomplete-coverage layer forma- tion, and integral layer formation.

关键词： petroleum pipelines steel corrosion welded joints carbon dioxide electrochemical impedance spectroscopy

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Triggering a [2]rotaxane molecular shuttle through hydrogen sulfide

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Science China Chemistry 2018年第3期61卷 306-310页

作者： Shun Yang Zhoulin Luan Chuan Gao Jingjing Yu Dahui Qu Key Laboratory for advanced materials and institute of Fine chemicals East China University of Science and Technology

A novel chemically-controlled [2]rotaxane molecular shuttle was successfully designed and synthesized. A H_2 S-responsive bulk barrier was introduced between the two identical recognition stations of the [2]rotaxane to prevent dynamic shuttling of the macrocycle. Upon addition of H_2 S, the complete intramolecular cascade reaction occurs in a controllable manner, resulting in removal of the bulk barrier and the shuttling motion of the macrocycle between the two stations recovers.

关键词： rotaxane molecular shuttle chemically-controlled hydrogen sulfide stimuli-responsive

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Synthesis and Crystal Structure of 4,4′-Diamino-N,N′-diethyl Bisbenzenesulfamide

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Chinese Journal of Structural Chemistry 2007年第2期26卷 177-183页

作者： WANG Li-Min PAN Xiao-Juan FAN Zhao-Yu YANG Liu-Bo LIU Lian TIAN He Laboratory for advanced materials Institute of Fine ChemicalsEast China University of Science and Technology Shanghai 200237 China

A new compound of 4,4＇-diamino-N,V＇-diethyl bisbenzenesulfamide （C18H26N4O4S2, Fw = 426.55） has been synthesized and its structure was determined by X-ray crystallography method. The crystal belongs to the monoclinic system, space group P21/c with a = 10.0623（9）, b = 13.6759（13）, c =15.5309（14） A, β = 100.482（2）°, V= 2101.6（3） A^3, Dc = 1.348 g/cm^3, F（000） = 904, μ = 0.285 mm^-1, Z = 4, the final R = 0.0512 and wR = 0.1363 for 3485 observed reflections with I 〉 2σ（I）. The structure of the title compound is pseudo secondary axisymmetric, and the two sulfamide-groups show distorted tetrahedral configurations.

关键词： 4,4'-diamino-N,V'-diethyl bisbenzenesulfamide synthesis crystal structure

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A cucurbit [8] uril recognized rigid supramolecular polymer with photo-stimulated responsiveness

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Chinese Chemical Letters 2015年第7期26卷 867-871页

作者： Tian-Tian Cao Xu-Yang Yao Jing Zhang Qiao-Chun Wang Xiang Ma Key Laboratory for advanced materials and institute of Fine chemicals East China University of Science and Technology

A rigid supramolecular polymer was constructed in aqueous solution via cucurbit[8]uril （CB[8]） host recognition with a rigid monomer containing an azobenzene unit and two 4,4＇-bipyridin-l-ium （BP） moieties in the two ends, which also exhibited photo-responsiveness owing to the photoinduced trans- cis ~somerization of azobenzene group.

关键词： Supramolecular polymerPhoto-responsivenessHost-guest recognitionCucurbituril

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Copper-catalyzed direct oxidation and N-arylation of benzylamines with diaryliodonium salts

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Science China Chemistry 2014年第8期57卷 1132-1136页

作者： LIU Xin MAO Dan WU ShengYing YU JianJun HONG Gang ZHAO Qiao WANG LiMin Key Laboratory for advanced materials and institute of Fine chemicals East China University of Science and Technology

An efficient approach for the synthesis of N-arylated amides was developed via copper(Ⅱ) triflate-catalyzed direct oxidation of(aryl)methylamines to primary arylamides by air and subsequent N-arylation by diaryliodonium salts. Various substituted benzylamines could be applied in the reaction, providing a series of N-arylated amides in moderate to good yields. This method showed convenient, practical, and environment friendly advantages.

关键词： copper(Ⅱ) triflate diaryliodonium salts N-arylated amides oxidation

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Magnetic separation of metal sulfides/oxides by Fe3O4 at room temperature and atmospheric pressure

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Rare Metals 2019年第5期38卷 379-389页

作者： Jia-Hui Ji Yi-Fei Xiao Bin Shen Qiu-Ying Yi Jin-Long Zhang Ming-Yang Xing Key Laboratory for advanced materials and institute of Fine chemicals School of Chemistry and Molecular Engineering East China University of Science and Technology

The recovery of heterogeneous catalysts can save costs and avoid secondary pollution,but its separation efficiency and recovery cost are limited by conventional separation methods such as precipitation–flocculation,centrifugation and *** this paper,we found that surface-defective metal sulfides/oxides(WS2,CuS,ZnS,MoS2,CdS,TiO2,MoO2 and ZnO)commonly used in advanced oxidation processes(AOPs)could be magnetically recovered at room temperature and atmospheric pressure by mechanically mixing with *** potential,Raman,X-ray photoelectron spectroscopy(XPS)and electro-spin resonance(ESR)spectra were measured to explore the mechanism of the magnetic separation *** exposed active metal sites on the surface of defective metal sulfides/oxides are beneficial for the formation of chemical bonds,which are combined with electrostatic force to be responsible for the magnetic ***,other factors affecting the magnetic separation were also investigated,such as the addition of amount of Fe3O4,different solvents and particle ***,WS2 was chosen to be applied as a co-catalyst in Fenton reaction,which could be well separated by the magnetic Fe3O4 to achieve the recycle of catalyst in Fenton *** research provides a general strategy for the recycle of metal sulfides/oxides in the catalytic applications.

关键词： Magnetic separation Metal sulfides/oxides Recycle Fenton reaction

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Supramolecular gelator based on a [c2]daisy chain rotaxane:efficient gel-solution transition by ring-sliding motion

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Science China Chemistry 2019年第2期62卷 245-250页

作者： Rongrong Tao Qi Zhang Sijia Rao Xiuli Zheng Mingming Li Dahui Qu Key Laboratory for advanced materials and institute of Fine chemicals School of Chemistry and Molecular EngineeringEast China University of Science & Technology

A supramolecular gelator based on the bistable [c2]daisy chain rotaxane is designed and synthesized. The reversible actuation of the [c2]daisy chain renders the formed supramolecular gel with acid/base-responsive switching between gel and monomer solution. The efficient switching process is attributed to the ring-sliding effect of the rotaxane in response to acid/base *** ring-inhibited hydrogen bonding stacking results in a nearly quantitatively disassembly of the gel network after addition of base which is hard to be realized by traditional heating strategy in hydrogen-bonding-supported gel.

关键词： supramolecular polymer hydrogen bond stimuli-responsive gel

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Artificial molecular machines that can perform work

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Science China Chemistry 2018年第10期61卷 1261-1273页

作者： Qiaochun Wang Dizhi Chen He Tian Key Laboratory for advanced materials and institute of Fine chemicals School of Chemistry and Molecular Engineering East China University of Science and Technology

An artificial molecular machine consists of molecule or substituent components jointed together in a specific way so that their mutual displacements could be initiated using appropriate outside stimuli. Such an ability of performing mechanical motions by consuming external energy has endowed these tiny machines with vast fascinating potential applications in areas such as actuators, manipulating atoms/molecules, drug delivery, molecular electronic devices, etc. To date, although vast kinds of molecular machine archetypes have been synthesized in facile ways, they are inclined to be defined as switches but not true machines in most cases because no useful work has been done during a working cycle. More efforts need to be devoted on the utilization and amplification of the nanoscale mechanical motions among synthetic molecular machines to accomplish useful tasks. Here we highlight some of the recent advances relating to molecular machines that can perform work on different length scales, ranging from microscopic levels to macroscopic ones.

关键词： molecular machines molecular motors rotaxanes catenanes switches

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