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metal-organic framework based nanomaterials for electrocatalytic oxygen redox reaction

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Science China Chemistry 2019年第4期62卷 417-429页

作者： Kexin Zhang Wenhan Guo Zibin Liang Ruqiang Zou Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of Engineering Peking University

Due to the severe environmental issues, many advanced technologies, typically fuel cells and metal-air batteries have aroused widespread concerns and been intensively studied in recent years. However, oxygen redox reactions including oxygen evolution reaction(OER) and oxygen reduction reaction(ORR) as the core reactions suffer from sluggish kinetics of the multiple electron transfer process. Currently, Pt, RuO_2, and IrO_2 are considered to be the benchmark catalysts for ORR and OER, but their high price, scarcity and instability hinder them from large-scale application. To overcome these limits, exploring alternative electrocatalysts with low cost, high activity, long-term stability, and earth-abundance is of extreme urgency. metal-organic frameworks(MOFs) are a family of inorganic-organic hybrid materials with high surface areas and tunable structures, making them proper as catalyst candidates. Herein, the recent progress of MOFs and MOF-derived materials for ORR and OER is systematically reviewed, and the relationship between compositions and electrochemical performance is discussed. It is expected that this review can be helpful for the future development of related MOF-based materials with excellent electrochemical performance.

关键词： metal-organic frameworks oxygen evolution reaction oxygen reduction reaction earth-abundant materials electrocatalysis nanomaterials

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

metal-organic framework coated titanium dioxide nanorod array p-n heterojunction photoanode for solar water-splitting

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Nano Research 2019年第3期12卷 643-650页

作者： Hui Yang Joeseph Bright Sujan Kasani Peng Zheng Terence Musho Banglin Chen Ling Huang Nianqiang Wu Department of Mechanical and Aerospace Engineering West Virginia University Morgantown WV 26506-6106 USA C. Eugene Bennett Department of Chemistry West Virginia University Morgantown WV 26506-6045 USA Department of Pharmaceutical Science West Virginia University Morgantown WV 26506-9530 USA Lane Department of Computer Science and Electrical Engineering West Virginia University Morgantown WV 26506 USA Department of Chemistry University of Texas at San Antonio One UTSA Circle San Antonio TX 78249-1604 USA Institute of Advanced Materials (IAM) Nanjing Tech University (NanjingTech) 30 South Puzhu Road Nanjing 211816 China

This paper presents a p-n heterojunction photoanode based on a p-type porphyrin metal-organic framework (MOF) thin film and an n-type rutile titanium dioxide nanorod array for photoelectrochemical water splitting. The TiO2@MOF core-shell n anorod array is formed by coati ng an 8 nm thick MOF layer on a vertically aligned TiO2 nanorod array scaffold via a layer-by-layer self-assembly method. This vertically aligned core-shell nanorod array enables a long optical path length but a short path length for extraction of photogenerated minority charge carriers (holes) from TiO2 to the electrolyte. A p-n junction is formed between TiO2 and MOF, which improves the extraction of photogenerated electr ons and holes out of the TiO2 nano rods. In additi on, the MOF coati ng sign ificantly improves the efficie ncy of charge in jecti on at the photoanode/electrolyte interface. Introduction of Co(lll) into the MOF layer further enhances the charge extraction in the photoanode and improves the charge injection efficiency. As a result, the photoelectrochemical cell with the TiO2@Co-MOF nanorod array photoanode exhibits a photocurrent density of 2.93 mA/cm^2 at 1.23 V (vs. RHE), which is ~ 2.7 times the photocurrent achieved with bare T1O2 nanorod array under irradiation of an unfiltered 300 W Xe lamp with an output power density of 100 mW/cm^2.

关键词： metal-organic framework water-splitting p-n junction photoanode titanium dioxide

metal-organic frameworks derived flower-like Co_3O_4/nitrogen doped graphite carbon hybrid for high-performance sodium-ion batteries

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Journal of Materials Science & Technology 2019年第1期35卷 100-108页

作者： Haifeng Xu Guang Zhu Baoming Hao School of Mechanical and Electronic Engineering Suzhou University Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou University

In this work, a novel flower-like cobalt-based metal organic frameworks(MOFs) self-assembled by Co^(2+) and nicotinic acid have been designed and synthesized. After a simple annealing treatment, Co_3O_4 nanoparticles in-situ decorating on nitrogen doped graphite carbon-sheet(Co_3O_4/NC) were obtained. The resultant Co_3O_4/NC hybrid with unique flower-like structure and ration combination of Co_3O_4 nanoparticles and nitrogen doped graphite carbon, endowing the hybrid with enhanced electrical conductivity,short ion diffusion pathways and rich porosity to the materials, which can largely alleviate the problems of Co_3O_4 such as inferior intrinsic electrical conductivity, sluggish ion kinetics and large volume change upon cycling. When evaluated as anode material for sodium-ion batteries(SIBs), the Co_3O_4/NC hybrid exhibits satisfied reversible capacity(213.9 mAh g^(-1) after 100 cycles at 0.1 A g^(-1) ), excellent rate capability(145.4 m Ah g^(-1) at 2 A g^(-1) and 130.1 mAh g^(-1) at 4 A g^(-1) ) and robust long-term cycling stability(120.1 m Ah g^(-1) after 2000 cycles at 0.5 A g^(-1) ), showing great potential for high-performance SIBs.

关键词： Co3O4/NC hybrid metal-organic frameworks Sodium-ion batteries High-performance

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 ***,MOF-based batteries are facing challenges such as poor electronic conductivity and inferior long-cycle stability that limit their further *** 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

metal-organic frameworks-derived nitrogen-doped carbon supported nanostructured PtNi catalyst for enhanced hydrosilylation of 1-octene

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Nano Research 2019年第10期12卷 2584-2588页

作者： Junfeng Wen Yuanjun Chen Shufang Ji Jian Zhang Dingsheng Wang and Yadong Li School of chemistry and chemical engineering Yulin UniversityYulin 719000China Department of Chemistry Tsinghua UniversityBeijing 100084China

Here,we successfully developed nano structured PtNi particles supported on n itroge rrdoped carbon(NC),which were obtai ned by carbon izati on of metal-organic frameworks under different temperatures,forming the nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 and nano-PtNi/NC-1000 *** hydrosilylation of 1-octene,we found that the nano-PtNi/NC-1000 catalyst exhibits higher activity for anti-Markovnikov hydrosilylation of 1-octene than those of nano-PtNi/NC-600,nano-PtNi/NC-800,nano-PtNi/NC-900 *** have verified that benefiting from obvious charge transfer from nano-PtNi particles to NC support carbonized at 1,000℃,the nano-PtNi/NC-1000 catalyst achieved almost complete conversion and produce exclusive adduct for anti-Markovnikov hydrosilylation of ***,the nano-PtNi/NC-1000 catalyst exhibited good reusability for the hydrosilylation *** work provides a new path to optimize electronic structure of catalysts by support modification to enhance electron transfer between metal active species and supports for highly catalytic performance.

关键词： metal-organic frameworks nanostructured PtNi particles hydrosilylation nitrogen-doped carbon

Co3O4 nanocage derived from metal-organic frameworks: An excellent cathode catalyst for rechargeable Li-O2 battery

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Nano Research 2019年第7期12卷 1555-1562页

作者： Zhuoliang Jiang Hui Sun Wenke Shi Tianhang Zhou Jianyong Hu Jingyang Cheng Pengfei Hu Shigang Sun State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of biogas upgrading utilizationCollege of New Energy and MaterialsChina University of Petroleum-BeijingBeijing 102249China State Key Lab of PCOSS Xiamen UniversityXiamen 361005China Eduard-Zintl-Institut fur Anorganische und Physikalische Chemie Technische UniversitatDarmstadtAlarich-Weiss-Strasse 8D-64287 DarmstadtGermany

Rechargeable non-aqueous Li-O2 battery is regarded as one of the most promising energy-storage technologies on account of its high energy *** is believed that the rational design of three-dimensional (3D) architecture for catalyst is a key factor for the remarkable ***-organic frameworks (MOFs) derived materials possess excellent architecture,which is beneficial for Li-O2 *** this work,ZIF-67 is used as precursor template and calcinated under different temperature to produce Co3O4 *** the anneal treatment is under 350℃,the derived Co3O4 nanocage holds the most complete skeleton,which provides better charge transfer ability as well as O2 and Li^+ ***,the Co3O4 nanocage owns more oxygen vacancies,offering more active *** the synergistic effect of nanocage structure and active sites,the Co3O4 nanocage stably delivers a large specific capacity of 15,500 mAh·g^-1 as well as a long cycle-life of 132 cycles at limited discharge capacity of 1,000 mAh·g^-1 under discharge/charge current density of 0.5 A·g^-1.

关键词： U-O2 batteries metal-organic framework (MOF)-derived Co3O4 nanocage Co3O4 polyhedron Co3O4 particle

Co-delivery of PARP and PI3K inhibitors by nanoscale metal-organic frameworks for enhanced tumor chemoradiation

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Nano Research 2019年第12期12卷 3003-3017页

作者： Megan J.Neufeld Allison N.DuRoss Madeleine R.Landry Hayden Winter Andrea M.Goforth Conroy Sun Department of Pharmaceutical Sciences College of PharmacyOregon State UniversityPortlandOregon 97201USA Department of Chemistry Portland State University1719 SW 10th AvePortlandOregon 97201USA Department of Radiation Medicine Oregon Health&Science University3181 S.W.Sam Jackson Park RdPortlandOregon 97239USA

Due to their complementary activity,the use of DNA damage repair(DDR)inhibitors during radiotherapy(RT)has yielded promising ***,this approach is often hindered by toxicity and poor in vivo stability of the DDR in *** scale metal-organic frameworks(nMOFs)represent an emerging class of crystalline materials which exhibit advantageous properties over traditional nanomaterials and demonstrate great potential in ***,a unique,synergistic treatment strategy for enhancing the therapeutic efficacy of RT vianMOF-mediated drug delivery and RT enhancement was evaluated.A nMOF containing the high-Zelement Hf and the ligand 1,4-dicarboxybenzene(Hf-BDC)was synthesized and loaded with the two DDR inhibitor drugs,talazoparib and buparlisib(TB@Hf-BDC-PEG).TB@Hf-BDC-PEGaugmented RT by increasing reactive oxygen species generation and thus DNA damage of which repair was inhibited *** enhancement was demonstrated in vivo where the combination of concurrent radiation with in travenous TB@Hf-BDC-PEG administration resulted in improved tumor control and increased ***,no apparent toxicity was observed with nMOF treatment,supporting its potential as an attractive candidate over traditional nano *** work provides the first report of nMOFs employed to enhance thetherapeutic response to RT through DDR inhibitor delivery and physical radiation dose enhancement.

关键词： nano scale metal-organic frameworks chemoradiotherapy DNA damage repair inhibitors drug delivery radiation dose enhancement

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 ***,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 *** 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 *** mechanistic insights into photoreduction of CO2 have been studied based on thermodynamical,electrochemical,and spectroscopic investigation,together with density functional theory(DFT)*** 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