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A Review of Metal-Organic Framework-Based Compounds for Environmental Applications

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Energy & Environmental Materials 2023年第3期6卷 47-76页

作者： Yongteng Qian Fangfang Zhang Dae Joon Kang Huan Pang School of Chemistry and Chemical Engineering Yangzhou University Department of Physics Sungkyunkwan University Department of Interdisciplinary Course of Physics and Chemistry Sungkyunkwan University

Metal-organic framework-based compounds have recently gained great attention because of their unique porous structure,ordered porosity,and high specific surface area.Benefiting from these superior properties,metalorganic framework-based compounds have been proven to be one of the most potential candidates for environmental governance and remediation.In this review,the different types of metal-organic framework-based compounds are first summarized.Further,the various environmental applications of metal-organic framework-based compounds including organic pollutant removal,toxic and hazardous gas capture,heavy metal ion detection,gas separation,water harvesting,air purification,and carbon dioxide reduction reactions are discussed in detail.In the end,the opportunities and challenges for the future development of metal-organic framework-based compounds for environmental applications are highlighted.

关键词： air purification environmental governance and remediation metal–organic framework organic pollutant removal toxic and hazardous gas capture

Dual-ligand and hard-soft-acid-base strategies to optimize metal-organic framework nanocrystals for stable electrochemical cycling performance

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National Science Review 2022年第7期9卷 88-96页

作者： Shasha Zheng Yan Sun Huaiguo Xue Pierre Braunstein Wei huang Huan Pang School of Chemistry and Chemical Engineering Yangzhou University Institut de Chimie UMR 7177 Universite′ de StrasbourgCNRS State Key Laboratory of Organic Electronics and Information Displays and Institute of Advanced Materials (IAM)Nanjing University of Posts and Telecommunications Frontiers Science Center for Flexible Electronics (FSCFE) MIIT Key Laboratory of Flexible Electronics (KLo FE)Northwestern Polytechnical University

Most metal-organic frameworks(MOFs) hardly maintain their physical and chemical properties after exposure to acidic,neutral,or alkaline aqueous solutions,resulting in insufficient stability,therefore limiting their applications.Thus,the design and synthesis of stable size/morphology-controlled MOF nanocrystals is critical but challenging.In this study,dual-ligand and hard-soft-acid-base strategies were used to fabricate a variety of 3D pillared-layer [Ni(thiophene-2,5-dicarboxylate)(4,4’-bipyridine)]nMOF nanocrystals(1D nanofibers,2D nanosheets and 3D aggregates) with controllable morphology by varying the concentration of 4,4’-bipyridine and thus controlling the crystal growth direction.Owing to the shorter ion diffusion length,enhanced ele ctron/ion transfer and strong interactions between thiophene-2,5-dicarboxylate and4,4’-bipyridine,the 2D nanosheets showed much larger specific capacitance than 1D nanofibers and 3D aggregates.A single device with an output voltage as high as 3.0 V and exceptional cycling performance(95% of retention after 5000 cycles at 3 mA cm-2) was realized by configuring two aqueous asymmetric super capacitive devices in series.The excellent cycling property and charge-discharge mechanism are consistent with the hard-soft-acid-base theory.

关键词： metal-organic framework dual ligand hard-soft-acid-base electrochemical energy storage supercapacitor

Design and synthesis of nitrogen-doped hexagonal NiCoO nanoplates derived from Ni-Co-MOF for high-performance electrochemical energy storage

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Chinese Chemical Letters 2020年第9期31卷 2280-2286页

作者： Yan Li Yuying Shan Huan Pang School of Chemistry and Chemical Engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009China

In order to further improve the potential application of nickel-cobalt oxide(NiCoO) in supercapacitors,we use controlled calcination of diffe rent Ni-Co-MOF([NiCo(HBTC)(4,4’-bipy)]) composites to obtain five kinds of nickel doped NiCoO(N-NiCoO) with different Ni/Co molar ratio.These N-NiCoO materials with unique hexagonal nanoplates structure,high specific surface area and high porosity indicate high and stable electrochemical activity.In particular,N-NiCoO-2 with a Ni/Co molar ratio of 2:1 exhibits the highest 945.79 F/g specific capacitance at 1 A/g and a high cycle stability of only 6.7% attenuation after 5000 cycles.Apart from the certain percentage of NiCoO with higher conductivity,nitrogen doping provides more reactive sites and the specific porous hexagonal nanoplates structure of the product itself accelerate electron transfer and promote electrolyte diffusion can more effectively enhance the electrochemical performance.Therefore,N-NiCoO synthesized via a simple method exhibit exciting potential and can be used as an electrode material for supercapacitors with good performance.

关键词： Ni-Co-MOF N-NiCoO Solvothermal Supercapacitors Electrochemical performance

A 3D hierarchical electrocatalyst:Core–shell Cu@Cu(OH)_(2)nanorods/MOF octahedra supported on N-doped carbon for oxygen evolution reaction

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Nano Research 2023年第5期16卷 8012-8017页

作者： Xinran Li Yipei Li Changli Wang Huaiguo Xue Huan Pang Qiang Xu School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM) SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory(SKAEM-JIL)Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of GuangdongDepartment of ChemistryDepartment of Materials Science and Engineering and SUSTech Academy for Advanced Interdisciplinary StudiesSouthern University of Science and Technology(SUSTech)Shenzhen 518055China

Cu-based materials are seldom reported as oxygen evolution reaction(OER)electrocatalysts due to their inherent electron orbital configuration,which makes them difficult to adsorb oxygen-intermediates during OER.Reasonably engineering the hierarchical architectures and the electronic structures can improve the performance of Cu-based OER catalysts,such as constructing multilevel morphology,inducing the porous materials,improving the Cu valence,building heterostructures,doping heteroatoms,etc.In this work,copper-1,3,5-benzenetricarboxylate(HKUST-1)octahedra in-situ grow on the Cu nanorod(NR)-supported N-doped carbon microplates,meanwhile an active layer of Cu(OH)_(2)forms on the surface of the original conductive Cu NRs.The octahedral HKUST-1,serving as a spacer between the microplates,greatly improves the porosity and increases the available active sites,facilitating the mass transport and electron transfer,thus resulting in greatly enhanced OER performance.

关键词： core–shell nanorod Cu@Cu(OH)_(2) metal–organic framework oxygen evolution reaction

A highly alkaline-stable metal oxide@metal–organic framework composite for high-performance electrochemical energy storage

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National Science Review 2020年第2期7卷 305-314页

作者： Shasha Zheng Qing Li Huaiguo Xue Huan Pang Qiang Xu School of Chemistry and Chemical Engineering and Institute for Innovative Materials and Energy Yangzhou University AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory National Institute of Advanced Industrial Science and Technology

Most metal-organic frameworks(MOFs) hardly maintain their physical and chemical properties after exposure to alkaline aqueous solutions,thus precluding their use as potential electrode materials for electrochemical energy storage devices.Here,we present the design and synthesis of a highly alkaline-stable metal oxide@MOF composite,CoOnanocube@Co-MOF(CoO@Co-MOF),via a controllable and facile one-pot hydrothermal method under highly alkaline conditions.The obtained composite possesses exceptional alkaline stability,retaining its original structure in 3.0 M KOH for at least 15 days.Benefitting from the exceptional alkaline stability,unique structure,and larger surface area,the CoO@Co-MOF composite shows a specific capacitance as high as 1020 F gat 0.5 A gand a high cycling stability with only 3.3% decay after 5000 cycles at 5 A g.The as-constructed solid-state flexible device exhibits a maximum energy density of 21.6 mWh cm.

关键词： metal–organic framework metal oxide composite electrochemical energy storage flexible supercapacitor

Fluorinated pillared-layer metal-organic framework microrods for improved electrochemical cycling stability

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Chinese Chemical Letters 2021年第12期32卷 3817-3820页

作者： Shasha Zheng Yue Ru Huaiguo Xue Huan Pang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China

Developing metal-organic framework(MOF)-based materials with good cyclic stability is the key to their practical application. Fluorinated organic compounds are usually highly chemically stability due to the high electronegativity of fluorine. Also, the pillared-layer structures based on coordination bonds have better structure and thermal stability than those based on hydrogen bonds. Herein, the fluorinated pillared-layer [Ni(2,3,4,5-tetrafluorobenzoic acid)(4,4-bipyridine)]nMOF([Ni(TFBA)(Bpy)]n) materials were constructed through a facile room-temperature solution reaction and used as electrode materials for supercapacitors. Surprisingly, the size/morphology of Ni(TFBA)(Bpy)nMOFs could be adjusted by varying the synthesis time. Benefting from the short ion diffusion length, unique pillar-layer structure, and strong intercomponent synergy of organic ligands, the Ni(TFBA)(Bpy)nMOF microrods showed a higher electrochemical energy storage capability than bulk MOFs. At the same time, compared to the non-fluorinated [Ni(benzoic acid)(Bpy)]nMOFs(31.5% capacitance decay), the fluorinated Ni(TFBA)(Bpy)n MOFs have a higher cycle stability with only 2.6% capacitance loss after 5000 cycles at 3 m A/cm^(2).

关键词： Fluorinated metal-organic framework Pillar-layer structure Microrod Cyclic stability Electrochemical energy storage Supercapacitor

Nanoreactors derived from silica-protection-assisted metal-organic framework

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Chinese Chemical Letters 2020年第9期31卷 2207-2210页

作者： Ling Jin Xiaxia Li Chunsen Liu Huan Pang School of Chemistry and Chemical Engineering Guangling CollegeYangzhou UniversityYangzhou 225009China Henan Provincial Key Laboratory of Surface&Interface Science Zhengzhou University of Light IndustryZhengzhou 450002China

The construction of highly stable and regular nanoreactors is a major challenge.In this work,we use a facile template protection method to obtain ZIF-67@SiO2(JS) and to encapsulate metal oxide nanoparticles(Co3O4) into nanoreactors(SiO2).ZIF-67 crystals provide a cobalt species;SiO2 was first used as a protective layer of ZIF-67 and then as a nanoreactor for metastable metal oxide nanoparticles.On this basis,Co3O4@SiO2 with dodecahedron morphology were synthesized by calcining JS at different tempe ratures,followed by a hydrothermal reaction to obtain Co3(OH)4Si2O5.Subsequently,CoSx and CoP-SiO2 were fabricated through sulfuration and phosphorization.The results in this work show that nanoreactors derived from metal-organic frameworks(MOFs) with a rational structure have broad development prospects.

关键词： Core-shell structure Metal oxide nanoparticles Co3(OH)4Si2O5 Nanoreactors Silicon shell

Promoting performance of lithium-sulfur battery via in situ sulfur reduced graphite oxide coating

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Rare Metals 2021年第2期40卷 417-424页

作者： Yuan Li Xiao-Tian Guo Song-Tao Zhang Huan Pang Department of Pharmacy Jiangsu Food and Pharmaceutical Science CollegeHuai’an223003China School of Chemistry and Chemical Engineering Guangling CollegeYangzhou UniversityYangzhou225000China

Activated graphene/sulfur structure sheathed in a flexible graphene layer is presented as the cathode material of lithium-sulfur battery.The surface coating graphite oxide sheets are reduced by a one-step in situ sulfur reduction method under vacuum at 600℃without any additional reductant.The high reduction degree of in situ sulfur reduced graphite oxide(RGO)coating layer will facilitate the rapid charge transfer at high current rate.The flexible encapsulated RGO structure will retard the diffusion of polysulfides and adjust the volume change of sulfur in cycling.As a result,the electrochemical evaluation of the RGO-activated graphene(AG)/S electrode demonstrates superior capacity,cycling and rate performance.The RGO-AG/S electrode with 60 wt%sulfur loading achieves a stable cyclability over 2000 galvanostatic charge/discharge process(capacity-fade rate of only 0.03%per cycle at1600 mA·g^(-1)).The average Coulombic efficiency remains at~96%with no electrolyte additives(such as LiNO_(3)).The outstanding property of RGO-AG/S electrode is attributed to the distinctive in situ sulfur RGOcoated hierarchical texture.

关键词： Lithium-sulfur battery Surface coating In situ Activated graphene Long-term stability

Metal-organic framework and its composites modulate macrophage polarization in the treatment of inflammatory diseases

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Chinese Chemical Letters 2024年第5期35卷 45-56页

作者： Feifei Wang Hang Yao Xinyue Wu Yijian Tang Yang Bai Hui Chong Huan Pang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China School of Pharmacy Changzhou UniversityChangzhou 213164China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210023China

Metal-organic framework(MOF)is a periodic sexual network structure with large surface area and high porosity,which is assembled by inorganic nodes and organic ligands through coordinate covalent bond.MOFs have the advantages of controllable pore size and shape,large specific surface area,easy modification and more active sites.In addition,MOF based nanoenzymes display excellent enzyme catalytic activity due to their special structure and multiple exposed metal active sites,controlling the production of reactive oxygen species(ROS)in cells or the body,and thus regulating the polarization of macrophage.This article reviews the mechanism of MOF material regulating macrophage polarization and the function of macrophages with different phenotypes.By utilizing the excellent properties of MOFs and the advantages of combining them with bioactive materials,we have discovered their excellent applications in the treatment of inflammatory diseases.Finally,we discussed the current challenges and prospects faced by MOF based composite materials.We expect that the research in this developing field will play a more important role in combating inflammatory diseases in the field of nanomedicine.

关键词： Metal-organic framework Inflammation Macrophage polarization Reactive oxygen species Nanozyme activity