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Chinese Journal of Chemical Engineering 2021年第5期34卷 167-174页

作者： Huan Li Yao Zhong Luxi Wang Qiang Deng Jun Wang Zheling Zeng Xinxiang Cao Shuguang Deng Key Laboratory of Poyang Lake Environment and Resource Utilization(Nanchang University)of the Ministry of Education School of ResourceEnvironmental and ChemicalEngineeringNanchang UniversityNanchang 330031China Laboratory for Development&Application of Cold Plasma Technology College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471022China School for Engineering of Matter Transport and EnergyArizona State University551 E.Tyler MallTempeAZ 85287United States

In the dehydration of fructose to 5-hydroxymethyl furfural(HMF),in situ produced water weakens the acid strength of the catalyst and causes the rehydration of HMF,causing unsatisfactory catalytic activity and selectivity.In this work,a class of benzenesulfonic acid-grafted metal-organic frameworks with strong acidity and hydrophobicity is obtained by the direct sulfonation method using 4-chlorobenzenesulfonic acid as sulfonating agent.The resultant MOFs have a specific surface area of greater than 250 m^(2)·g^(-1),acid density above 1.0 mmol·g^(-1),and water contact angle up to 129°.The hydrophobic MOF-PhSO_(3)H exhibits both higher catalytic activity and selectivity than MOF-SO_(3)H in the HMF synthesis due to its better hydrophobicity and olephilicity.Moreover,the catalyst has a high recycled stability.At last,fructose is completely converted,and 98.0%yield of HMF is obtained under 120℃ in a DMSO solvent system.The successful preparation of the hydrophobic acidic MOF provides a novel hydrophobic catalyst for the synthesis of HMF.

关键词： Catalysis Catalyst Biomass metal-organic framework Fructose 5-Hydroxymethylfurfural

2-Methylimidazole assisted ultrafast synthesis of carboxylate-based metal–organic framework nano-structures in aqueous medium at room temperature

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Science Bulletin 2019年第15期64卷 1103-1109页

作者： Shaheed Ullah Bilal Akram Hassan Ali Hao Zhang Haozhou Yang Qingda Liu Xun Wang Key Laboratory of organic Opteoelectronics and Molecular Engineering Department of Chemistry Tsinghua University

Carboxylate-based metal–organic frameworks(CMOFs)have received considerable attentions for their high stability,catalytic activity,and porosity.However,synthesis of CMOFs requires high temperature,pressure,and long reaction time.Here,we explored the activity of 2-methylimidazole(2-MIM)for ultrafast synthesis of CMOF nanostructures(CMOFNs),in aqueous medium at room temperature and reaction time of 10 min.Seven CMOFNs have been synthesized by using Al3+,Cr3+,Cu2+,Fe3+,In3+,or Cd2+salt and1,4-bezenedicarboxylic acid,or 1,3,5-benzenetricarboxylic acid.Through this technique,the CMOFs with space time yield 181–501 kgcrystal sizes of ca.200–700 nm was obtained.

关键词： metal-organic framework Carboxylate 2-Methylimidazole Room temperature synthesis Nanostructures

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金属-有机骨架材料水相合成路线研究进展

Science China Materials 2020年第5期63卷 667-685页

作者：段崇雄余仪肖静张雪莲李理波阳鹏飞吴军良奚红霞 School of Materials Science and Energy Engineering Foshan UniversityFoshan 528231China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640China School of Environment and Energy South China University of TechnologyGuangzhou 510006China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

金属-有机骨架材料具有优异的物理化学性质,因而在气体储存、吸附分离、药物传输、超级电容器、催化等领域具有广阔的应用前景.然而大多数金属-有机骨架材料的合成通常需要用到大量的有机溶剂,而这些有机溶剂的使用不仅会增加金属-有机... 详细信息

金属-有机骨架材料具有优异的物理化学性质,因而在气体储存、吸附分离、药物传输、超级电容器、催化等领域具有广阔的应用前景.然而大多数金属-有机骨架材料的合成通常需要用到大量的有机溶剂,而这些有机溶剂的使用不仅会增加金属-有机骨架材料的生产成本,且极易对环境造成影响.基于此,理想的合成路线是用水代替有害的有机溶剂,以降低成本及减轻其对环境的影响.本文总结了近期金属-有机骨架材料水相合成路线的研究进展,重点概括了不同水相合成法制备金属-有机骨架材料的机理,并分析了各种方法的优缺点.此外,还讨论了当前绿色且低成本工业化生产金属-有机骨架材料存在的问题以及未来可能的发展方向.

关键词： metal-organic frameworks water-based routes industrial production

metal-organic framework UiO-66 membranes

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Frontiers of Chemical Science and Engineering 2020年第2期14卷 216-232页

作者： Xinlei Liu Catalysis Engineering Department of Chemical EngineeringDelft University of Technology2629 HZ DelftThe Netherlands

metal-organic frameworks(MOFs)have emerged as a class of promising membrane materials.UiO-66 is a prototypical and stable MOF material with a number of analogues.In this article,we review five approaches for fabricating UiO-66 polycrystalline membranes including synthesis,secondary synthesis,biphase synthesis,gas-phase deposition and electrochemical deposition,as well as their applications in gas separation,pervaporation,nanofiltration and ion separation.On this basis,we propose possible methods for scalable synthesis of UiO-66 membranes and their potential separation applications in the future.

关键词： membrane metal-organic framework UiO-66 separation

Ultrafast laser dynamics of metal organic frameworks/TiO_2 nano-arrays hybrid composites for energy conversion applications

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Journal of Energy Chemistry 2019年第2期28卷 88-94页

作者： Fatma M.Ismail Daniel O'Neil Tareq Youssef Souad A.Elfeky The National Institute of Laser Enhanced Sciences Cairo University Zewail City of Science and Technology Georgia Institute of Technology

Herein,we report the victorious synthesis of metal-organic frameworks(MOFs) on TiO_2 nanotubes(NTs)using a layer-by-layer(LbL) approach.Highly crystalline and homogenous thin films of MOFs were grown and characterized using XRD,SEM,FT-IR and UV/Vis spectroscopy.Moreover,the utilization of the MOF films as sensitizers was probed in bespoke Graetzel type liquid junction solar cells.The constructed cell performance revealed an I_(sc) of 1.16 mA cm^(–2),Vocof 0.63 V,FF of 0.33,and E_(ff) of 0.42%.Further,pumpprobe transient laser spectroscopy was performed to investigate the energy and charge transfer dynamics of the MOFs/TiO_2 NTs interface.The results indicated 86% injection efficiency.The ultrafast pump-probe spectroscopy allows the investigation of this process and the differences between MOFs.It also showed that the relaxation of the MOF chromophores is in competition with electron injection in the Ti O2 motif.Thus this study provides a new insight into electron transfer from photoexcited metal-organic frameworks(MOFs) into titanium dioxide.

关键词： Ultrafast laser dynamics metal-organic frameworks TiO2 nano-arrays Energy conversion Thin film

Encapsulating a Ni（Ⅱ） molecular catalyst in photoactive metal–organic framework for highly efficient photoreduction of CO2

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Science Bulletin 2019年第14期64卷 976-985页

作者： Zhi-Hao Yan Bo Ma Shu-Rong Li Junxue Liu Rong Chen Ming-Hao Du Shengye Jin Gui-Lin Zhuang La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China State Key Laboratory of Molecular Reaction Dynamics and Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China College of Chemical Engineering Zhejiang University of Technology Hangzhou 310032 China

Photocatalytic reduction of CO2 to CO is a promising strategy for reducing atmospheric CO2 levels and storing solar radiation as chemical energy.Here,we demonstrate that a molecular catalyst[NiⅡ(bpet)(H2O)2]successfully encapsulated into a highly robust and visible-light responsive metal–organic framework(Ru-UiO-67)to fabricate composite catalysts for photocatalytic CO2 reduction.The composite Ni@Ru-UiO-67 photocatalysts show efficient visible-light-driven CO2 reduction to CO with a TON of 581 and a selectivity of 99% after 20-h illumination,because of the facile electron transfer from Ru-photosensitizer to Ni(Ⅱ)active sites in Ni@Ru-UiO-67 system.The mechanistic insights into photoreduction of CO2 have been studied based on thermodynamical,electrochemical,and spectroscopic investigation,together with density functional theory(DFT)calculations.This work shows that encapsulating molecular catalyst into photoactive MOF highlights opportunities for designing efficient,stable and recyclable photocatalysts.

关键词： metal-organic frameworks CO2 reduction Transient absorption Photocatalysis DFT calculations

metal-organic frameworks for CO2 photoreduction

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Frontiers in Energy 2019年第2期13卷 221-250页

作者： Lei ZHANG Junqing ZHANG Department of Mechanical Engineering University of Alaska Fairbanks Fairbanks AK 99775 USA

metal-organic frameworks (MOFs) have attracted much attention because of their large surface areas, tunable structures, and potential applications in many areas. In recent years, MOFs have shown much promise in CO2 photoreduction. This review summarized recent research progresses in MOF-based photocatalysts for photocatalytic reduction of CO2. Besides, it discussed strategies in rational design of MOF-based photocatalysts (functionalized pristine MOFs, MOF-photosensitizer, MOF-semiconductor, MOF-metal, and MOF-carbon materials composites) with enhanced performance on CO2 reduction. Moreover, it explored challenges and outlook on using MOF-based photocatalysts for CO2 reduction.

关键词： metal-organic frameworks (MOFs) photoca-talysis CO2 photoreduction composite

Multistep evolution from a metal–organic framework to ultrathin nanosheets

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Science Bulletin 2019年第14期64卷 964-967页

作者： Yun Li Jin Huang Zong-Wen Mo Xue-Wen Zhang Xiao-Ning Cheng Li Gong Dong-Dong Zhou Jie-Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China Instrumental Analysis and Research Center Sun Yat-Sen University Guangzhou 510275 China

Two-dimensional (2D) materials and ultrathin nanosheets have attracted tremendous research interests [1-4]. Exfoliation of porous coordination polymers (PCPs) or metal-organic frameworks (MOFs) with 2D coordination structures is emerging as a viable strategy for preparation of new types of 2D materials [5-8]. The relatively weak bonding within and strong interactions between 2D coordination networks are the main problems for successful exfoliation [9]. Pretreatments of the layered MOFs to expand the interlayer distances can be helpful [10-12]. Capturing the exfoliation intermediates and visualizing their structures are valuable for understanding the exfoliation mechanism and confirming the structures of the final 2D materials [11,12].

关键词： Two-dimensional (2D) porous coordination polymers (PCPs) metal-organic frameworks (MOFs)

metal-organic frameworks and their derivatives for Li-air batteries

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Chinese Chemical Letters 2020年第3期31卷 635-642页

作者： Yu Dong Siwu Li Shanshan Hong Lu Wang Bo Wang Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials Key Laboratory of Cluster ScienceMinistry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

metal-organic frameworks(MOFs)are a class of outstanding materials in Li-air batteries because of their high surface areas,tailorable pore sizes and diverse catalytic centers.However,MOF-based batteries are facing challenges such as poor electronic conductivity and inferior long-cycle stability that limit their further development.This review first summarizes the progress of pristine MOFs and MOF-derived materials in Li-air batteries in the past 5 years,then provides a perspective for subsequent development of MOFs and their derivatives in this emerging field.

关键词： metal-organic frameworks MOF-derived materials Li-air batteries Li-O2 batteries Li-CO2 batteries

Recent advances in metal-organic frameworks for lithium metal anode protection

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Chinese Chemical Letters 2020年第3期31卷 609-616页

作者： Ying Du Xing Gao Siwu Li Lu Wang Bo Wang Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials Key Laboratory of Cluster ScienceMinistry of EducationSchool of Chemistryand Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

The lithium metal battery has been considered as a promising candidate for next generation batteries.However,safety concerns caused by uncontrollable lithium dendrite growth on lithium anode are severely hampering the commercial application.metal-organic frameworks(MOFs)become one of the most attractive materials due to the high porosity,structural designability and tunability.With unique open channels and pores as well as functional components in MOFs,the transportation and deposition of lithium ions can be regulated,which leads to enhanced electrochemical prope rties.Various strategies for lithium metal protection are proposed in recent wo rks on applications of MOFs in lithium metal batteries.In this review,we highlight latest key approaches in this field and discuss the prospects for MOFs in advanced Li anodes.

关键词： metal-organic frameworks Li anode Lithium metal batteries Li dendrite Protection