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Nanoengineering Metal–organic frameworks and Derivatives for Electrosynthesis of Ammonia

纳微快报:英文版 2023年第11期15卷 205-240页

作者： Daming Feng Lixue Zhou Timothy J.White Anthony K.Cheetham Tianyi Ma Fengxia Wei College of Chemistry Liaoning UniversityShenyang 110036People’s Republic of China School of Materials Science and Engineering Nanyang Technological University50 Nanyang AvenueSingapore 639798Singapore Materials Research Laboratory University of CaliforniaSanta BarbaraCA 93106USA School of Science RMIT UniversityMelbourneVIC 3000Australia Institute of Materials Research and Engineering(IMRE) Agency for ScienceTechnology and Research(A^(*)STAR)2 Fusionopolis WayInnovis 08‑03Singapore 138634Singapore

Electrocatalytic synthesis under mild conditions has become increasingly important as one of the practical alternatives for industrial applications,especially for the green ammonia(NH_(3))industry.A properly engineered electrocatalyst plays a vital role in the realization of superior catalytic performance.Among various types of promising nanomaterials,Metal–organic frameworks(MOFs)are competitive candidates for developing efficient electrocatalytic NH_(3) synthesis from simple nitrogen-containing molecules or ions,such as N_(2) and NO_(3)^(−).In this review,recent advances in the development of electrocatalysts derived from MOFs for the electrosynthesis of NH_(3) are collected,categorized,and discussed,including their application in the N_(2) reduction reaction(NRR)and the NO_(3)^(−)reduction reaction(NO3RR).Firstly,the fundamental principles are illustrated,such as plausible mechanisms of NH_(3) generation from N_(2) and NO_(3)^(−),the apparatus of corresponding electrocatalysis,parameters for evaluation of reaction efficiency,and detection methods of yielding NH_(3).Then,the electrocatalysts for NRR processes are discussed in detail,including pristine MOFs,MOF-hybrids,MOF-derived N-doped porous carbons,single atomic catalysts from pyrolysis of MOFs,and other MOF-related materials.Subsequently,MOF-related NO3RR processes are also listed and discussed.Finally,the existing challenges and prospects for the rational design and fabrication of electrocatalysts from MOFs for electrochemical NH_(3) synthesis are presented,such as the evolution of investigation methods with artificial intelligence,innovation in synthetic methods of MOF-related catalysts,advancement of characterization techniques,and extended electrocatalytic reactions.

关键词： Metal–organic frameworks Electrosynthesis of ammonia Nitrogen reduction reactions Nitrate reduction reactions

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Large-scale computational screening of Metal–organic frameworks for D_(2)/H_(2) separation

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Chinese Journal of Chemical Engineering 2023年第2期54卷 323-330页

作者： Fei Wang Zhiyuan Bi Lifeng Ding Qingyuan Yang State Key Laboratory of organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China College of Information Science and Technology Beijing University of Chemical TechnologyBeijing 100029China Department of Chemistry Xi'an Jiaotong-Liverpool UniversitySuzhou 215123China

Deuterium(D_(2)) is one of the important fuel sources that power nuclear fusion reactors. The existing D_(2)/H_(2) separation technologies that obtain high-purity D_(2) are cost-intensive. Recent research has shown that metal-organic frameworks(MOFs) are of good potential for D_(2)/H_(2) separation application. In this work, a high-throughput computational screening of 12020 computation-ready experimental MOFs is carried out to determine the best MOFs for hydrogen isotope separation application. Meanwhile, the detailed structure-performance correlation is systematically investigated with the aid of machine learning. The results indicate that the ideal D_(2)/H_(2) adsorption selectivity calculated based on Henry coefficient is strongly correlated with the 1/ΔAD feature descriptor;that is, inverse of the adsorbility difference of the two adsorbates. Meanwhile, the machine learning(ML) results show that the prediction accuracy of all the four ML methods is significantly improved after the addition of this feature descriptor. In addition, the ML results based on extreme gradient boosting model also revealed that the 1/ΔAD descriptor has the highest relative importance compared to other commonly-used descriptors. To further explore the effect of hydrogen isotope separation in binary mixture, 1548 MOFs with ideal adsorption selectivity greater than 1.5 are simulated at equimolar conditions. The structure-performance relationship shows that high adsorption selectivity MOFs generally have smaller pore size(0.3-0.5 nm) and lower surface area. Among the top 200 performers, the materials mainly have the sql, pcu, cds, hxl, and ins topologies.Finally, three MOFs with high D_(2)/H_(2) selectivity and good D_(2) uptake are identified as the best candidates,of all which had one-dimensional channel pore. The findings obtained in this work may be helpful for the identification of potentially promising candidates for hydrogen isotope separation.

关键词： Metal–organic frameworks Computational screening Hydrogen isotope separation

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Recent advances in the synthesis of nanoscale hierarchically porous Metal–organic frameworks

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Nano Materials Science 2022年第4期4卷 351-365页

作者： Chongxiong Duan Kuan Liang Zena Zhang Jingjing Li Ting Chen Daofei Lv Libo Li Le Kang Kai Wang Han Hu Hongxia Xi School of Materials Science and Hydrogen Engineering Foshan UniversityFoshan528231China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou510640China State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringInstitute of New EnergyChina University of Petroleum(East China)Qingdao266580China School of Materials Science and Engineering Xi'an University of Science and TechnologyXi'an710054China School of Electrical Engineering Qingdao UniversityQingdao266061China

Nanoscale hierarchically porous Metal–organic frameworks(NHP-MOFs)have received unprecedented attention in many fields owing to their integration of the strengths of nanoscale size(metal ions(e.g.,Cu,Fe,Co,Zn,Al,Zr,and Cr),including the template method,composite technology,post-synthetic modification,in situ growth and the grind method.In addition,the mechanisms of synthesis,regulation techniques and the advantages and disadvantages of various methods are discussed.Finally,the challenges and prospects of the commercialisation of promising NHP-MOFs are also presented.The purpose of this review is to provide a road map for future design and development of NHP-MOFs for practical application.

关键词： Metal–organic frameworks Nanoscale Hierarchically porous structure Synthesis strategies

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A ternary mechanism for the facilitated transfer of metal ions onto Metal–organic frameworks: implications for the "versatility" of these materials as solid sorbents

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1632-1642页

作者： Xiyuan Bu Ming Tian Hongqing Wang Lin Wang Liyong Yuan Weiqun Shi Laboratory of Nuclear Energy Chemistry Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Although Metal–organic frameworks offer a new platform for developing versatile sorption materials,yet coordinating the functionality,structure and component of these materials remains a great challenge.It depends on a comprehensive knowledge of a“real sorption mechanism”.Herein,a ternary mechanism for U(Ⅵ)uptake in Metal–organic frameworks was reported.Analogous MIL-100s(Al,Fe,Cr)were prepared and studied for their ability to sequestrate U(Ⅵ)from aqueous solutions.As a result,MIL-100(Al)performed the best among the tested materials,and MIL-100(Cr)performed the worst.The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(Ⅵ)uptake in the three Metal–organic frameworks involves different mechanisms.Specifically,hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s(Al,Fe)by exchanging with hydrogen ions of terminal hydroxyl groups(Al-OH_(2),Fe-OH_(2)),and/or,hydrated uranyl ions are bound directly to Al(Ⅲ)center in MIL-100(Al)through a strong inner-sphere coordination.For MIL-100(Cr),however,the U(Ⅵ)uptake is attributed to electrostatic attraction.Besides,the sorption mechanism is also pH and ionic strength dependent.The present study suggests that changing metal center of Metal–organic frameworks and sorption conditions alters sorption mechanism,which helps to construct effective Metal–organic frameworks-based sorbents for water purification.

关键词： U(Ⅵ) Metal–organic frameworks adsorption mechanism metal node

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Hierarchically porous Metal–organic frameworks:synthetic strategies and applications

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National Science Review 2020年第11期7卷 1743-1758页

作者： Liang Feng Kun-Yu Wang Xiu-Liang Lv Tian-Hao Yan Hong-Cai Zhou Department of Chemistry Texas A&M UniversityCollege Station Department of Materials Science and Engineering Texas A&M UniversityCollege Station

Despite numerous advantages, applications of conventional microporous Metal–organic frameworks (MOFs) are hampered by their limited pore sizes, such as in heterogeneous catalysis and guest delivery,which usually involve large molecules. Construction of hierarchically porous MOFs (HP-MOFs) is vital to achieve the controllable augmentation of MOF pore size to mesopores or even macropores, which can enhance the diffusion kinetics of guests and improve the storage capacity. This review article focuses on recent advances in the methodology of HP-MOF synthesis, covering preparation of HP-MOFs with intrinsic hierarchical pores, and modulated, templated and template-free synthetic strategies for HP-MOFs.The key factors which affect the formation of HP-MOF architectures are summarized and discussed,followed by a brief review of their applications in heterogeneous catalysis and guest encapsulation. Overall,this review presents a roadmap that will guide the future design and development of HP-MOF materials with molecular precision and mesoscopic complexity.

关键词： Metal–organic frameworks hierarchical design synthesis application

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Pore-Directed Solid-State Selective Photoinduced E–Z Isomerization and Dimerization within Metal–organic frameworks

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CCS Chemistry 2023年第5期5卷 1225-1232页

作者： Shu-Li Chen Yan Mi Fei-Long Hu David James Young Jianping Lang Key Laboratory of Chemistry and Engineering of Forest Products State Ethnic Affairs CommissionGuangxi Minzu UniversityNanning 530006Guangxi College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123Jiangsu College of Engineering IT and EnvironmentCharles Darwin UniversityDarwin 0909Northern Territory

Design and construction of suitable pore microenvironments for selective catalytic reactions of small guest molecules is a major goal for chemists.Herein,we report control of competitive E–Z photoisomerization and photodimerization within porous Metal–organic frameworks(MOFs)by fine-tuning the pore microenvironments using different dicarboxylate linkers.MOFs with small pores((E)-X_(MOF_(1))and(E)-X_(MOF_(1))′)favor the photoinduced E–Z isomerization of one encapsulated diaryl alkene substrate while those with large pores(((E)-X)_(2MOF_(2)))prefer the photodimerization of two encapsulated alkene substrates.Both reactions show broad functional group compatibility and proceed stereospecifically in good yields under mild conditions.High local concentration of diaryl alkene ligands and their preorientation within pores facilitate stereoselective dimerization.This pore engineering strategy is applicable to control and create pore microenvironemnts for other photoinduced organic reactions within porous MOFs.

关键词： pore engineering E–Z photoisomerization photodimerization Metal–organic frameworks solid-state reaction

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Synthesis of zinc-carboxylate metal-organic frameworks for the removal of emerging drug contaminant(amodiaquine)from aqueous solution

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Journal of Environmental Sciences 2018年第2期30卷 264-275页

作者： Adedibu C.Tella Samson O.Owalude Sunday J.Olatunji Vincent O.Adimula Sunday E.Elaigwu Lukman O.Alimi Peter A.Ajibade Oluwatobi S.Oluwafemi Department of Chemistry University of Ilorin Department of Chemistry and Polymer Science Stellenbosch University School of Chemistry and Physics University of Kwa Zulu-Natal Department of Applied Chemistry University of Johannesburg Doornfontein Campus Centre for Nanomaterials Science Research University of Johannesburg

We herein report the removal of amodiaquine, an emerging drug contaminant from aqueous solution using [Zn2（fum）2（bpy）] and [Zn4 O（bdc）3]（fum = fumaric acid; bpy =4,4-bipyridine; bdc = benzene-1,4-dicarboxylate） Metal–organic frameworks（MOFs） as adsorbents. The adsorbents were characterized by elemental analysis, Fourier transform infrared（FT-IR） spectroscopy, and powder X-ray diffraction（PXRD）. Adsorption process for both adsorbents were found to follow the pseudo-first-order kinetics, and the adsorption equilibrium data fitted best into the Freundlich isotherm with the R2 values of 0.973 and0.993 obtained for [Zn2（fum）2（bpy）] and [Zn4 O（bdc）3] respectively. The maximum adsorption capacities foramodiaquine in this study were found to be 0.478 and 47.62 mg/g on the[Zn2（fum）2（bpy）] and [Zn4 O（bdc）3] MOFs respectively, and were obtained at p H of 4.3 for both adsorbents. FT-IR spectroscopy analysis of the MOFs after the adsorption process showed the presence of the drug. The results of the study showed that the prepared MOFs could be used for the removal of amodiaquine from wastewater.

关键词： Adsorption Metal–organic frameworks Amodiaquine Wastewater

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Tuning Atomically Dispersed Fe Sites in Metal–organic frameworks Boosts Peroxidase‑Like Activity for Sensitive Biosensing

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Nano-Micro Letters 2020年第12期12卷 392-403页

作者： Weiqing Xu Yikun Kang Lei Jiao Yu Wu Hongye Yan Jinli Li Wenling Gu Weiyu Song Chengzhou Zhu Key Laboratory of Pesticide and Chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079People’s Republic of China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249People’s Republic of China

Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant challenges.Herein,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the Metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active sites.Benefiting from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like activity.As a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−1.Moreover,the detection of organophosphorus pesticides was also achieved.This work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.

关键词： Nanozymes Metal–organic frameworks Atomically dispersed sites Peroxidase-like activity Biosensors

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Precise Construction of Stable Bimetallic Metal–organic frameworks with Single-Site Ti(IV) Incorporation in Nodes for Efficient Photocatalytic Oxygen Evolution

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CCS Chemistry 2022年第8期4卷 2782-2792页

作者： Lan Li Zhi-Bin Fang Wenzhuo Deng Jun-Dong Yi Rui Wang Tian-Fu Liu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of Chinese Academy of Sciences Beijing 100049 CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

Assembling the reactive low-cost Co clusters and photoresponsive ligands in the form of Metal–organic frameworks(MOFs)is a promising strategy to construct efficient water-oxidizing photocatalysts,but it is restricted by poor water stability.Introducing high valent cations in the clusters to build heterometallic Co-MOFs might be a solution,yet a precise fabrication strategy is still challenging.

关键词： cobalt catalyst Metal–organic frameworks single-site Ti incorporation stability photocatalytic O_(2)evolution

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Chemical chaperone delivered nanoscale Metal–organic frameworks as inhibitor of endoplasmic reticulum for enhanced sensitization of thermo-chemo therapy

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Chinese Chemical Letters 2022年第3期33卷 1604-1608页

作者： Xiaoyan Ma Qiong Wu Longfei Tan Changhui Fu Xiangling Ren Qijun Du Lufeng Chen Xianwei Meng Laboratory of Controllable Preparation and Application of Nanomaterials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China Graduate School of Bio-Applications and Systems Engineering Tokyo University of Agriculture and TechnologyKokyo 184-8588Japan CAS Key Laboratory of Cryogenics Technical Institute of Physics and ChemistryBeijing 100190China First Clinical Medical School and First Hospital Shanxi Medical UniversityTaiyuan 030001China

Thermotherapy and chemotherapy have received extensive attention to tumor treatment. However, thermal tolerance and drug resistance severely limit clinical effect of tumor therapy owing to endoplasmic reticulum(ER) stress. Reducing thermal tolerance and drug resistance of tumors is an urgent challenge to be solved. In this work, we design a nanoplatform of PBA-Dtxl@MIL-101 as an ER inhibitor. Amino functionalized Fe-metal organic framework(MIL-101) nanoparticles are synthesized as p H and microwave(MW) dual stimuli-responsive drug delivery system. Then, the chemical chaperones of 4-phenylbutyric acid(PBA) and antineoplastic drug Docetaxel(Dtxl) were successfully loaded into MIL-101 nanoparticles to form PBA-Dtxl@MIL-101 nanoparticles. Furthermore, PBA-Dtxl@MIL-101 nanoparticles exhibit inhibitor effect of ER stress through upregulating caspase 9 proteins and reduce thermal tolerance by downregulating HSP 90. It was demonstrated that the therapy sensitized by PBA-Dtxl@MIL-101 nanoparticles obviously destroyed tumor cells, showing simultaneously enhanced thermo-chemo therapy.

关键词： Metal–organic frameworks Biodegradable Chemotherapy Thermotherapy Microwave

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