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cu cluster embedded porous nanofibers for high-performance CO_(2) electroreduction

Chinese Chemical Letters 2023年第4期34卷 542-546页

作者： Zhifeng Xin Zibo Yuan Jingjing Liu Xinjian Wang Kejing Shen Yifa Chen Ya-Qian Lan Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa’anshan 243002China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Metal-doped carbon materials, as one of the most important electrocatalytic catalysts for CO_(2)reduction reaction(CO_(2)RR), have attracted increasing attention. Herein, a series of cu cluster embedded highly porous nanofibers have been prepared through the carbonization of electro-spun MOF/PAN nanofibers.The obtained cu cluster doped porous nanofibers possessed fibrous morphology, high porosity, conductivity, and uniformly dispersed cu clusters, which could be applied as promising CO_(2)RR catalysts. Specifically, best of them, MCP-500 exhibited high catalytic performance for CO_(2)RR, in which the Faradaic efficiency of CO(FECO) was as high as 98% at-0.8 V and maintained above 95% after 10 h continuous electrocatalysis. The high performance might be attributed to the synergistic effect of tremendously layered graphene skeleton and uniformly dispersed cu clusters that could largely promote the electron conductivity, mass transfer and catalytic activity during the electrocatalytic CO_(2)RR process. This attempt will provide a new idea to design highly active CO_(2)RR electrocatalyst.

关键词： Electrocatalysis cu cluster Porous nanofiber Electrospinning CO_(2)RR

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过一硫酸盐体系中铜分布模式控制活性物种的产生和污染物降解路径

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Engineering 2024年第4期35卷 168-179页

作者： Ning Li Haoxi Dai Mengting He Jun Wang Zhanjun Cheng Beibei Yan Wenchao Peng Guanyi Chen School of Environmental Science and Engineering&Tianjin Engineering Research Center of Bio Gas/Oil Technology Tianjin UniversityTianjin 300072China Department of Chemical Engineering Tianjin UniversityTianjin 300350China School of Mechanical Engineering Tianjin University of CommerceTianjin 300134China School of Science Tibet UniversityLhasa 850012China

The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate(PMS)activation and contaminants degradation.Herein,atomic layer deposition is applied to prepare cu single atom(SA-cu),cluster(C-cu),and film(F-cu)decorated MXene catalysts by regulating the number of deposition cycles.In comparison with SA-cu-MXene(adsorption energy(E_(ads))=-4.236 eV)and F-cu-MXene(E_(ads)=-3.548 eV),PMS is shown to adsorb preferably on the C-cu-MXene surface for activation(E_(ads)=-5.435 eV),realizing higher utilization efficiency.More SO_(4)^(·-)are generated in C-cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-cu-MXene and F-cu-MXene activated PMS systems.Particularly,the contribution of SO_(4)^(·-)oxidation to sulfamethoxazole(SMX)degradation followed the order,C-cu-MXene(97.3%)>SA-cu-MXene(90.4%)>Fcu-MXene(71.9%),realizing the larger SMX degradation rate in the C-cu-MXene/PMS system with the degradation rate constants(k)at 0.0485 min^(-1).Additionally,SMX degradation routes in C-cu-MXene/PMS system are found with fewer toxic intermediates.Through this work,we highlighted the importance of guided design of heterogeneous catalysts in the PMS system.Appropriate metal distribution patterns need to be selected according to the actual water treatment demand.Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.

关键词： cu cluster Distribution pattern Peroxymonosulfate Active species Degradation routes

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Rational designing MOFs from novel multi-dentate ligands

Rational designing MOFs from novel multi-dentate ligands

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中国化学会第十五届固态化学与无机合成学术会议

作者： Yili Dong Shufang Li Lei Xu Zaiyong Zhang Zhi Su Min Fang Hongke Liu School of chemistry and materials Nanjing normal university

Metal organic frameworks is composed of metal ion or metal cluster and organic ligands through self-assembly method forming multi network structure, which has been widely applied in the adsorption gas, selective catalysis, fluorescence and other fields. With porphyrin ligand as a building unit of the MOFs has a wide range of applications such as catalysis, sensing, optical absorption. Single-crystal-to-single-crystal（SCSC） transformation and MOFs which based polyoxometalates（POMs） have been paid widespread attention, and flexibility for the coordination complexes is a hot research field, which is highly related to the chemical and physical properties. We have used both tripodal and porphyrin ligands to design MOFs with various metal ions. We have synthesized a number of MOFs based on copper clusters by the reaction of copper（II） and multidentate ligands via the solvothermal synthesis, the optical and electrionic properties, the factors that facilitate the simple metal ions to be the complex clusters, have been characterized and discussed. And a dissolution-recrystallization structural transformation（DRST） process from 2D（NJNU-100） to 3D（NJNU-101） structure has been studied by various techniques. We have also obtained a number of MOFs with 2D or 3D structures constructed from meso-tetra（4-imidazoyl）porphyrin（TImP） ligand. These MOFs have exhibited ultrahigh chemical stability（stable in saturated（～27.5 M） NaOH solutions for weeks）, unique coordination model or large distortion of porphyrin plane that had not been found before in porphyrinic MOFs, and the catalytic property that can catalyze the oxidation of styrene. These works have provided a insight view for the structural transformation, and illustrated that the unsaturated coordination nodes would be a great driving force for the structural transformation and will facilitate further study of porphyrinic and metal cluster based MOFs.

关键词： MOFs porphyrin ligand cu cluster 2D or 3D SCSC ultrahigh chemical stability catalytic optical and electrionic properties

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