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Enhanced stability of highly-dispersed copper catalyst supported by hierarchically porous carbon for long term selective hydrogenation

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催化学报 2020年第7期41卷 1081-1090页

作者： Hu Nian Li Xiaoyun Liu Siming Wang Zhao He Xiaoke Hou Yuexin Wang Yuxiang Deng Zhao Chen Lihua Su Baolian Laboratory of Living Materials Wuhan University of Technology the State Key Laboratory of Advanced Technology for Material Synthesis and Processing Hubei Wuhan 430070 Wuhan University of Technology State Key Laboratory of Silicate Materials for Architectures Hubei Wuhan 430070 Laboratory of Inorganic Materials Chemistry (CMI) University of Namur Belgium Namur B-5000 Clare Hall University of Cambridge Cambridge CB3 9AL

Copper based catalysts have high potential for the substituent of noble-metal based catalysts as their high selectivity and moderate activity for selective hydrogenation reaction; however, achieving further high catalytic stability is very difficult. In this work, the carbonization process of Cu-based organic frameworks was explored for the synthesis of highly-dispersed Cu supported by hierarchically porous carbon with high catalytic performance for selective hydrogenation of 1,3-butadiene. The porous hierarchy of carbon support and the dispersion of copper nanoparticles can be precisely tuned by controlling the carbonization process. The resultant catalyst carbonized at 600 °C exhibits a rather low reaction temperature at 75 °C for 100% butadiene conversion with 100% selectivity to butenes, due to its reasonable porous hierarchy and highly-dispersed copper sites. More importantly, unprecedentedly stability of the corresponding Cu catalyst was firstly observed for selective 1,3-butadiene hydrogenation, with both 100% butadiene conversion and 100% butenes selectivity over 120 h of reaction at 75 °C. This study verifies that a simply control the carbonization process of metal organic frameworks can be an effective way to obtain Cu-based catalysts with superior catalytic performance for selective hydrogenation reaction.

关键词： Hierarchically porous structure Catalyst Cu/C Selective hydrogenation Metal organic frameworks

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Molecularly Tunable Heterostructured Co-Polymers Containing Electron-Deficient and -Rich Moieties for Visible-Light and Sacrificial-Agent-Free H2O2Photosynthesis

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Angewandte Chemie 2024年第29期136卷

作者： Jingzhao Cheng Wang Wang Jianjun Zhang Sijie Wan Prof. Bei Cheng Prof. Jiaguo Yu Prof. Shaowen Cao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Hubei Technology Innovation Center for Advanced Composites Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China

As an alternative to hydrogen peroxide (H 2 O 2 ) production by complex anthraquinone oxidation process, photosynthesis of H 2 O 2 from water and oxygen without sacrificial agents is highly demanded. Herein, a covalently connected molecular heterostructure is synthesized via sequential C−H arylation and Knoevenagel polymerization reactions for visible-light and sacrificial-agent-free H 2 O 2 synthesis. The subsequent copolymerization of the electron-deficient benzodithiophene-4,8-dione (BTD) and the electron-rich biphenyl (B) and p -phenylenediacetonitrile (CN) not only expands the π-conjugated domain but also increases the molecular dipole moment, which largely promotes the separation and transfer of the photoinduced charge carriers. The optimal heterostructured BTDB-CN 0.2 manifested an impressive photocatalytic H 2 O 2 production rate of 1920 μmol g −1 h −1 , which is 2.2 and 11.6 times that of BTDB and BTDCN. As revealed by the femtosecond transient absorption (fs-TA) and theoretical calculations, the linkage serves as a channel for the rapid transfer of photogenerated charge carriers, enhancing the photocatalytic efficiency. Further, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) uncovers that the oxygen reduction reaction occurs through the step one-electron pathway and the mutual conversion between C=O and C−OH with the anchoring of H + during the catalysis favored the formation of H 2 O 2 . This work provides a novel perspective for the design of efficient organic photocatalysts.

关键词： molecular heterostructure H2O2 dipole moment channel reaction path

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Quasilinear dispersion in electronic band structure and high Seebeck coefficient in CuFeS2-based thermoelectric materials

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Physical Review materials 2020年第2期4卷 025405-025405页

作者： Hongyao Xie Xianli Su Shiqiang Hao Christopher Wolverton Ctirad Uher Xinfeng Tang Mercouri G. Kanatzidis State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Department of Chemistry Northwestern University Evanston Illinois 60208 USA Department of Materials Science and Engineering Northwestern University Evanston Illinois 60208 USA Department of Physics University of Michigan Ann Arbor Michigan 48109 USA

The earth-abundant natural mineral chalcopyrite CuFeS2 is a potential n-type thermoelectric material because of its large Seebeck coefficient at high carrier concentrations. For a long time, the large Seebeck coefficient of CuFeS2 has been attributed to a large electron effective mass, but the reasons for this and the unusual carrier concentration dependent behavior have rarely been discussed. Here, we systematically investigated the special transport behavior of CuFeS2 and found the classical parabolic band model to be inadequate in explaining it. Our experimental and theoretical studies indicate that there are two flat electronic pockets at the Γ and Z points of the Brillouin zone near the conduction band edge of CuFeS2 that dominate the charge transport. These electronic pockets result from nonparabolic quasilinearly dispersing bands that give rise to a linear wave vector dependent energy (E∼k) and a carrier density dependent effective mass (m*∼m0n1/3). Such a strong carrier concentration dependent carrier effective mass results in the high Seebeck coefficient of CuFeS2 compound under a large carrier density. The work demonstrates that quasilinearly dispersing bands can give strongly enhanced Seebeck coefficient, and could be useful in optimizing the properties of thermoelectric materials.

关键词： Thermoelectric effects

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Large-scale current collectors for regulating heat transfer and enhancing battery safety

Nature Chemical Engineering

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Nature Chemical Engineering 2024年 542-551页

作者： Lun Li Huazhang Zhang Xin Zhao Daping He Wei Shu Zixin Zhang Yu Zhao Xingchuan Li Zongkui Kou Yong Xiao Francis Verpoort Liqiang Mai Jinlong Yang Rui Tan CheeTong John Low Cheng Li Yajun Zhang Hewu Wang Hubei Engineering Research Center of RF-Microwave Technology and Application School of Physics and Mechanics Wuhan University of Technology Wuhan China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing State Key Laboratory of Silicate Materials for Architectures School of Materials Science and Engineering Wuhan University of Technology Wuhan China Guangdong Provincial Key Laboratory of New Energy Materials Service Safety College of Materials Science and Engineering Shenzhen University Shenzhen China Department of Chemical Engineering Swansea University Swansea UK Warwick Electrochemical Engineering Group WMG Energy Innovation Centre University of Warwick Warwick UK School of Vehicle and Mobility Tsinghua University Beijing China

Thermal runaway, a major battery safety issue, is triggered when the local temperature exceeds a threshold value resulting from slower heat dissipation relative to heat generation inside the cell. However, improving internal heat transfer is challenged by the low thermal conductivity of metal current collectors (CCs) and challenges in manufacturing nonmetal CC foils at large scales. Here we report a rapid temperature-responsive nonmetallic CC that can substitute benchmark Al and Cu foils to enhance battery safety. The nonmetallic CC was fabricated through a continuous thermal pressing process to afford a highly oriented Gr foil on a hundred-meter scale. This Gr foil demonstrates a high thermal conductivity of 1,400.8 W m−1K−1, about one order of magnitude higher than those of Al and Cu foils. Importantly, LiNi0.8Co0.1Mn0.1O2||graphite cells integrated with these temperature-responsive foils show faster heat dissipation, eliminating the local heat concentration and circumventing the fast exothermic aluminothermic and hydrogen-evolution reactions, which are critical factors causing the thermal failure propagation of lithium-ion battery packs.

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Electrochemical Hydrophobic Tri-layer Interface Rendered Mechanically Graded Solid Electrolyte Interface for Stable Zinc Metal Anode

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Angewandte Chemie 2024年第9期136卷

作者： Dr. Chaozheng Liu Dr. Wangwang Xu Dr. Lei Zhang Daotong Zhang Dr. Weina Xu Dr. Xiaobin Liao Weimin Chen Dr. Yizhong Cao Prof. Mei-Chun Li Prof. Changtong Mei Dr. Kangning Zhao Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and Engineering Nanjing Forestry University Nanjing 210000 China Mechanical & Industrial Engineering Department Louisiana State University Baton Rouge LA-70803 USA State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China School of Materials Science and Engineering Dongguan University of Technology Guangdong 523808 China College of Chemistry and Materials Engineering Zhejiang A&F University Hangzhou 311300 China Laboratory of Advanced Separations (LAS) École Polytechnique Fédérale de Lausanne (EPFL) Sion 1950 Lausanne Switzerland

The aqueous zinc-ion battery is promising as grid scale energy storage device, but hindered by the instable electrode/electrolyte interface. Herein, we report the lean-water ionic liquid electrolyte for aqueous zinc metal batteries. The lean-water ionic liquid electrolyte creates the hydrophobic tri-layer interface assembled by first two layers of hydrophobic OTF − and EMIM + and third layer of loosely attached water, beyond the classical Gouy–Chapman–Stern theory based electrochemical double layer. By taking advantage of the hydrophobic tri-layer interface, the lean-water ionic liquid electrolyte enables a wide electrochemical working window (2.93 V) with relatively high zinc ion conductivity (17.3 mS/cm). Furthermore, the anion crowding interface facilitates the OTF − decomposition chemistry to create the mechanically graded solid electrolyte interface layer to simultaneously suppress the dendrite formation and maintain the mechanical stability. In this way, the lean-water based ionic liquid electrolyte realizes the ultralong cyclability of over 10000 cycles at 20 A/g and at practical condition of N/P ratio of 1.5, the cumulated areal capacity reach 1.8 Ah/cm 2 , which outperforms the state-of-the-art zinc metal battery performance. Our work highlights the importance of the stable electrode/electrolyte interface stability, which would be practical for building high energy grid scale zinc-ion battery.

关键词： Electrochemical Tri-Layer Interface Hydrophobic Ionic Liquid Mechanically Graded Solid Electrolyte Interface Zinc Battery

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A Blinking Mesoporous TiO2−x Composed of Nanosized Anatase with Unusually Long-Lived Trapped Charge Carriers

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Angewandte Chemie 2020年第35期132卷 15110-15117页

作者： Zhang T. Low J. Yu J. Tyryshkin A.M. Mikmeková E. Asefa T. Department of Chemical and Biochemical Engineering Rutgers The State University of New Jersey 98 Brett Road Piscataway NJ 08854 United States State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan Hubei 430070 China Department of Chemistry and Chemical Biology Rutgers The State University of New Jersey 610 Taylor Road Piscataway NJ 08854 United States Institute of Scientific Instruments of the ASCR Czech Academy of Sciences Královopolská 147 Brno 612 64 Czech Republic

A mesoporous TiO2−x material comprised of small, crystalline, vacancy-rich anatase nanoparticles (NPs) shows unique optical, thermal, and electronic properties. It is synthesized using polymer-derived mesoporous carbon (PDMC) as a template. The PDMC pores serve as physical barriers during the condensation and pyrolysis of a titania precursor, preventing the titania NPs from growing beyond 10 nm in size. Unlike most titania nanomaterials, during pyrolysis the NPs undergo no transition from the anatase to rutile phase and they become catalytically active reduced TiO2−x. When exposed to a slow electron beam, the NPs exhibit a charge/discharge behavior, lighting up and fading away for an average period of 15 s for an extended period of time. The NPs also show a 50 nm red-shift in their UV/Vis absorption and long-lived charge carriers (electrons and holes) at room temperature in the dark, even long after UV irradiation. The NPs as photocatalysts show a good activity for CO2 reduction. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

关键词： blinking nanoparticles carbon dioxide reduction long-lived charge carriers photocatalytic energy conversions titanium dioxide

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Scalable microfabrication of three-dimensional porous interconnected graphene scaffolds with carbon spheres for high-performance all carbon-based micro-supercapacitors

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Journal of Materiomics 2019年第2期5卷 303-312页

作者： Yiming Chen Minghao Guo Liang He Wei Yang Lin Xu Jiashen Meng Xiaocong Tian Xinyu Ma Qiang Yu Kaichun Yang Xufeng Hong Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and EngineeringWuhan University of TechnologyWuhan430070China Department of Materials Science and NanoEngineering Rice UniversityHoustonTX77005United States Faculty of Materials Science&Chemistry China University of GeosciencesWuhan430074China Department of Civil Engineering Rice UniversityHoustonTX77005United States

As one of the most important micro energy storage devices(MESDs),graphene-based micro-supercapacitors(G-MSCs)possess the advantages of excellent flexibility,long cycle life,affordability and high *** most cases,constructing three-dimensional(3D)graphene networks is widely utilized to promote the permeation of electrolyte and enhance the utilization of active *** this work,conventional freeze-drying process is utilized in the fabrication of G-MSCs to constitute 3D interconnected networks micro-electrodes,and further by regulating the composition of inks,carbon spheres(CSs)at different mass loadings are introduced into the graphene scaffolds to further increase the active sites of the *** fabricated all carbon-based MSC with the optimal mass loading of CSs(0.406 mg cm^(-2))exhibits a high specific areal capacitance of 17.01mF cm^(-2)at the scan rate of 10mV s^(-1)and a capacitance retention of 93.14%after 10000 cycles at the scan rate of 500 mV s^(-1).The proposed microfabrication process is facile and fully compatible with modern microtechnologies and will be highly suitable for large-scale production and integration.

关键词： Three-dimensional Injecting Freeze-drying Mass loading Supercapacitor

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Sulfur-deficient MoS2 encapsulated in hollow mesoporous carbon spheres as a functional polysulfide mediator

Sulfur-deficient MoS2 encapsulated in hollow mesoporous carb...

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中国化学会第二十次全国电化学大会

作者： Hong-En Wang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Lithium-sulfur batteries have the advantages of high theoretical energy density(2600 Wh kg-1), low-cost and environmental friendliness, which is one of the most promising secondary battery systems. However, the practical application of Li-S batteries has still been restricted by the low Coulombic efficiency and rapid capacity decay deriving from the low conductivity of sulfur cathode, large volume expansion（～80%） during discharging, and serious lithium corrosion/dendrite of anode, particularly, high dissolution of the discharge intermediate polysulfides（LiPSs） in electrolyte and shuttle effect between cathode and anode.

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Self-assembled Nanostructures and Derived Nanocarbon materials for Electrochemical Energy Storage

Self-assembled Nanostructures and Derived Nanocarbon Materia...

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中国化学会第二十次全国电化学大会

作者： Qi Li Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Self-assembly of functional units represents an important synthetic approach in the rational design of nanomaterials with precisely-controlled chemical compositions, nanostructures and desired properties, and hence finds vast applications in areas including but not limited to biomedical engineering, separation, energy storage and conversion. The functional units which can be used in self-assembly range from small molecules, metal ions, clusters, nanoparticles to large polymeric molecules. Finely tuning the functional groups of assembly units and the bonding/interactions between the units can generate versatile materials with unique structures and properties, thus leading to the desired performances for various applications. Notably, under varied external conditions, the chemical bonding, interactions between the assembly units and the structures can also be varied, which further endows these materials with responsive properties for applications in multidisciplinary areas. In recent years, I have studied a series of self-assembled nanostructured materials which are based on metal-organic coordinative compounds constructed between metal ions and organic ligands. Nanostructuring of these materials endow them with greatly enhanced properties in electrochemical energy storage. Moreover, in combination with controlled pyrolysis and understanding of the structure-property relationship, the rational design and controlled synthesis of nanocarbon composite electrode materials towards high-performance electrochemical energy storage and conversion becomes feasible. In this talk, I will present some of our recent work on the rational design of self-assembled metal-organic nanostructures and their derived nanocarbon materials for electrochemical energy storage.

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Research on the stability of organic/inorganic hybrid perovskite materials for IEC61215 purpose

Research on the stability of organic/inorganic hybrid perovs...

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第六届新型太阳能电池材料科学与技术学术研讨会

作者： Jiang He Zhiliang Ku Yong Peng State key lab of advanced technology for materials synthesis and processing Wuhan University of Technology

Organi/Inorganic perovskite materials behavior differently under a testing condition of IEC61215. In this research, the behavior of series of perovskite materials with varied A cations under the thermal cycling testing standards were studied. We analyzed the defeating mechanisms of those materials through temperature depended XRD, SEM and AFM ***. Finally, we draw a conclusion that FACsPb（I/Br） perovskite materials could the most stable one under thermal cycling testing condition. This perovskite materials can be stable because the phase change related materials decomposition under frequent temperature change does not happen in this material, however other perovskite materials will decompose. A device with an architecture of FTO/TiO/FACsPbI/graphite electrode was then encapsulated and tested under a condition of -30℃-85℃ for 200 times. After testing, the device finally kept about 83% of its initial power conversion efficiency.

关键词： Standard stability tests Perovskite solar cells thermal cycling tests

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