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Design and synthesis of thiol-terminated imidothioether oligomer as thermally latent hardener and modifier for high-performance epoxy/thiol thermosets

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Science China Chemistry 2024年第2期67卷 632-641页

作者： Xing Liu Jianjun Zhou Shumei Liu Jianqing Zhao School of Materials Science and Engineering South China University of TechnologyGuangzhou510640China Key Lab Guangdong high Property&Functional Polymer Materials Key Laboratory of Polymer Processing EngineeringMinistry of EducationGuangzhou510640China

Conventional base-catalyzed epoxy/aliphatic thiol systems have a poor storage stability,and are impossible to be one-pot systems.A widely accepted solution is to use the latent catalysts,which are usually insoluble anionic initiators sensitive to impurities and moisture,and have many limitations in practical use.In this work,a soluble thiol-terminated imidothioether oligomer(TPI) was synthesized and used as a latent hardener and modifier to prepare one-pot epoxy/thiol systems without the latent catalysts.The latent behavior and curing mechanism of epoxy systems(EP/TPI series),consisted of bisphenol A diglycidyl ether(DGEBA),pentaerythritol tetrakis(mercaptoacetate)(PETMP) and TPI,were proposed.The thiol exchange reaction between TPI and PETMP preceded the curing reaction of DGEBA,and produced aromatic thiols,which were unreactive at ambient conditions and reacted with DGEBA to form the thermosets at temperatures above 130 ℃.At the loading of 24.4 wt%TPI,the epoxy system(EP/TPI-3) had a shelf life of 13 days and was completely cured within 20 min at 180 ℃.Meanwhile,the catalyst-free curing process of EP/TPI-3 system was insensitive to impurities and moisture.Furthermore,the thermal and mechanical properties of EP/TPI-3 thermoset were simultaneously improved,thereinto,the glass transition temperature,Young's modulus and ultimate tensile strength were increased by 16.7 ℃,12.9%,and 13.6%,respectively,compared with those of the commercial DGEBA/PETMP thermoset.This work shows that TPI has the potential to be a powerful alternative to commercial latent catalysts,and EP/TPI thermosets with High performance have broad application prospects.

关键词： thiol-terminated imidothioether oligomer epoxy systems thiol exchange reaction thermal latency High performance

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Mechanical behavior and permeability properties of sustainable and high-performance anisotropic three-dimensional printable concrete

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Frontiers of Structural and Civil Engineering 2023年第11期17卷 1662-1674页

作者： Fatih OZALP Civil Engineering Department Istanbul Medeniyet UniversityIstanbul 34700Turkey

Three-dimensional printable concrete requires further development owing to the challenges encountered,including its brittle behavior,high cement requirement for the buildability of layers,and anisotropic behavior in different directions.The aim of this study is to overcome these challenges.First,three-dimensional printable concrete mixtures were prepared using silica fume,ground blast furnace slag,and metakaolin,instead of cement,to reduce the amount of cement.Subsequently,the rheological and mechanical behaviors of these concretes were investigated.Second,threedimensional printable concrete mixtures were prepared using 6-mm-long steel and synthetic fibers to eliminate brittleness and determine the effect of those fibers on the anisotropic behavior of the concrete.As a result of this study,it is understood that printable concretes with extremely low permeability and high buildability can be achieved using mineral additives.In addition,results showed that three-dimensional concrete samples containing short steel fibers achieve fracture energies up to 36 times greater than that of plain concrete.Meanwhile,its characteristic length values,as indicators of ductility,are 22 times higher than those of plain concrete.The weakest strength was recorded at the interfaces between layers.The bending and splitting tensile strengths of three-dimensional printed plain concrete samples were 15%and 19%lower than those of casted samples,respectively.However,the addition of fibers improved the mechanical strength of the interfaces significantly.

关键词： three-dimensional concrete printing rheology High performance mineral additives anisotropy fiber

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A nonchlorinated solvent-processed polymer semiconductor for high-performance ambipolar transistors

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National Science Review 2022年第4期9卷 139-147页

作者： Jie Yang Yaqian Jiang Zhiyuan Zhao Xueli Yang Zheye Zhang Jinyang Chen Junyu Li Wei Shi Shuai Wang Yunlong Guo Yunqi Liu Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of Sciences School of Chemistry and Chemical Engineering Huazhong University of Science and Technology

Ambipolar polymer semiconductors are potentially serviceable for logic circuits, light-emitting field-effect transistors(LFETs) and polymer solar cells(PSCs). Although several high-performance ambipolar polymers have been developed, their optoelectronic devices are generally processed from toxic chlorinated solvents. To achieve the commercial applications of organic FETs(OFETs), the polymers should be processed from nonchlorinated solvents, instead of chlorinated solvents. However, most conjugated polymers show poor solubility in nonchlorinated solvents. It is of great importance to develop ambipolar polymers that can be processed from nonchlorinated solvents. Here, we develop a nonchlorinated solvent processed polymer named poly[7-fluoro-N, N′-di(4-decyltetradecyl)-7′-azaisoindigo-6′,6′′-(thieno[3,2-b]thiophene-2,5-diyl)-7′′′-fluoro-N′′, N′′′-di(4-decyltetradecyl)-7′′-azaisoindigo-6,6′′′-([2,2′′-bithiophene]-5,5′′-diyl)](PITTI-BT) by designing a monomer with a large molar mass. The polymer displays good solubility in p-xylene(PX). Well-aligned films of PITTI-BT are achieved by an off-center spin-coating(SC) method. Based on the high-quality films, the OFETs fabricated from PX solution achieve record ambipolar performance with hole and electron mobilities of 3.06 and2.81 cm~2 V-1s-1, respectively. The combination of nonchlorinated solvents and good alignment process offers an effective and eco-friendly approach to obtain high-performance ambipolar transistors.

关键词： nonchlorinated solvent High performance ambipolar transistor alignment

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high-performance lithium-ion batteries based on polymer/graphene hybrid cathode material

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中国科学:化学英文版 2023年第9期66卷 2683-2689页

作者： Yang Zhao Minghan Ni Nuo Xu Chenxi Li Yanfeng Ma Hongtao Zhang Yongsheng Chen The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China Renewable Energy Conversion and Storage Center(RECAST) Nankai UniversityTianjin 300071China

Organic and carbon-based lithium-ion batteries possess abundant resources,nontoxicity,environmental friendliness,and High performance,and they have been widely studied in the past decades.However,it remains a challenge to construct such batteries with high capacity,high cycling stability,and high conductivity simultaneously.Here,we elaborately design and integrate organic polymer(p-FcPZ) with graphene network to create a hybrid material(p-FcPZ@G) for high-performance lithium-ion batteries(LIBs).The bi-polar polymer p-FcPZ containing multiple redox-active sites endows p-FcPZ@G with both remarkable cycling stability and high capacity.The porous conductive graphene network with a large surface area facilitates rapid ions/electrons transportation,resulting in superior rate performance.Therefore,the half-cell based on p-FcPZ@G cathode exhibits simultaneously high capacity(~250 mA h g^(-1) at 50 mA g^(-1)),excellent cycling stability(retention of 99.999% per cycle for 10,000 cycles at 2,000 mA g^(-1)) and superior rate performance.Additionally,the graphene-based full cell assembled with p-FcPZ@G cathode and graphene anode also demonstrates comprehensively high electrochemical performance.

关键词： lithium-ion batteries organic electrode graphene hybrid material High performance full cells

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3D MoS_(2) foam integrated with carbon paper as binder-free anode for High performance sodium-ion batteries

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Journal of Energy Chemistry 2022年第2期31卷 26-33页

作者： Fangying Zheng Zeyu Wei Huicong Xia Yunchuan Tu Xiangyu Meng Kaixin Zhu Jiao Zhao Yimin Zhu Jianan Zhang Yan Yang Dehui Deng Institute of Environmental Remediation Dalian Maritime UniversityDalian 116026LiaoningChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina Zhang Dayu School of Chemistry Dalian University of TechnologyDalian 116024LiaoningChina

Molybdenum sulfide(MoS_(2))with well-designed porous structure has the potential to be great electrode materials in sodium-ion batteries due to its high theoretical capacity and abundant resource,however,hindered by its intrinsic low conductivity and stability.Herein,MoS_(2) with 3 D macroporous foam structure and high conductivity was obtained through SiO_(2) templates and integrated with carbon paper(3 D FMoS_(2)/CP).It has showed superior specific capacity(225 m A h g^(-1),0.4–3 V)and cycling stability(1000 cycles)at high rate(2000 m A g^(-1)),with a low decay rate(0.033%per cycle)in sodium-ion batteries.The excellent electrochemical performance may originate from its unique integrated structure:3 D MoS_(2) macropores providing high surface area and abundant transfer channels while carbon paper enhancing the conductivity of MoS_(2) and avoiding unnecessary side reactions brought by binder addition.

关键词： 3D MoS_(2)foam Carbon paper Binder-free electrode High performance Sodium-ion batteries

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PdSe_(2)/MoSe_(2) vertical heterojunction for self-powered photodetector with High performance

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Nano Research 2022年第3期15卷 2489-2496页

作者： Jiahong Zhong Biao Wu Yassine MADOUNE Yunpeng Wang Zongwen Liu Yanping Liu School of Physics and Electronics Hunan Key Laboratory for Super-microstructure and Ultrafast ProcessCentral South UniversityChangsha 410083China State Key Laboratory of high-performance Complex Manufacturing Central South UniversityChangsha 410083China School of Chemical and Biomolecular Engineering The University of SydneyNSW 2006Australia The University of Sydney Nano Institute The University of SydneyNSW 2006Australia Shenzhen Research Institute of Central South University A510aVirtual University BuildingSouthern DistrictHigh-tech Industrial ParkYuehai StreetNanshan DistrictShenzhen 518057China

Van der Waals’two-dimensional(2D)material heterostructure engineering offers an effective strategy for the design of multifunctional and high-performance optoelectronic devices.However,2D heterostructure photodetectors with a photoconductive effect tend to suffer from high driving source-drain voltages and significant dark noise currents.Herein,a self-powered photodetector with High performance was fabricated based on vertically stacked graphene/MoSe_(2)/PdSe_(2)/graphene heterojunctions through a dry transfer method.The fabricated device displays current rectification characteristics in darkness(on/off ratio>10^(3))and superior photovoltaic behaviors under illumination.In addition,benefitting from the strong built-in field,the Gr/PdSe_(2)/MoSe_(2)/Gr heterojunction photodetector is able to respond to a broad spectrum from visible to near-infrared(NIR)with a remarkable responsivity of 651 mA·W^(−1),a high specific detectivity of 5.29×10^(11) Jones and a fast response speed of 41.7/62.5μs.Moreover,an enhanced responsivity of 1.16 A·W^(−1) has been obtained by a reverse voltage(−1 V)and further evaluation on image recognition has also demonstrated the great application potential of the Gr/MoSe_(2)/PdSe_(2)/Gr heterojunction photodetector.The findings are expected to bring new opportunities for the development of highly sensitive,high-speed and energy-efficient photodetectors for comprehensive applications.

关键词： heterostructure MoSe_(2) PdSe_(2) self-powered photodetector High performance

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D-π-D molecular layer electronically bridges the NiO_(x) hole transport layer and the perovskite layer towards High performance photovoltaics

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Journal of Energy Chemistry 2022年第4期31卷 797-804页

作者： Rongguo Xu Xiuwen Xu Ruixi Luo Yu Li Gaopeng Wang Tongfa Liu Ning Cai Shihe Yang Guangdong Provincial Key Lab of Nano-Micro Materials Research School of Chemical Biology and BiotechnologyShenzhen Graduate SchoolPeking UniversityShenzhen 518055GuangdongChina School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006GuangdongChina Institute of Biomedical Engineering Shenzhen Bay LaboratoryShenzhen 518107GuangdongChina

Nickel oxide (NiO_(x)) has significant cost and stability advantages over poly[bis (4-phenyl)(2,4,6-trimethyl phenyl)amine](PTAA) for inverted p-i-n perovskite solar cells (PSCs),but the poor NiO_(x)/perovskite contact stemming from some reactive species at the interface led to suboptimal device performance.To solve this problem,we take a multiple donor molecule approach,using 3,3’-(4,8-bis(hexylthio)benzo[1,2-b:4,5-b’]dithiophene-2,6-diyl)bis(10-(6-bromohexyl)-10H-phenoxazine)(BDT-POZ) as an example,to modify the NiO_(x)/perovskite interface.The primary goal was to reduce the under-coordinated Ni^(≥3+) cations via electron transfer from the donor molecules to NiO_(x),thus mitigating the detrimental reactions between perovskite and NiO_(x).Equally importantly,the hole extraction at the interface was greatly enhanced after the organic donor modification,since the hydrophobic species atop NiO_(x) not only enabled pinhole-free crystallization of the perovskite but also properly tuned the interfacial energy level alignment.Consequently,the PSCs with NiO_(x)/BDT-POZ HTL achieved a high power conversion efficiency (PCE) up to 20.16%,which compared excellently with that of the non-modified devices (17.83%).This work provides a new strategy to tackle the exacting issues that have so far impeded the development of NiO_(x) based PSCs.

关键词： Perovskite solar cells NiO_(x)modification Hole transport Energy level alignment High performance

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Low-cost all-iron flow battery with High performance towards long-duration energy storage

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Journal of Energy Chemistry 2022年第10期31卷 445-451,I0011页

作者： Xiaoqi Liu Tianyu Li Zhizhang Yuan Xianfeng Li Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Long duration energy storage(LDES)technologies are vital for wide utilization of renewable energy sources and increasing the penetration of these technologies within energy infrastructures.Herein,we propose a low-cost alkaline all-iron flow battery by coupling ferri/ferro-cyanide redox couple with ferric/ferrous-gluconate complexes redox couple.The designed all-iron flow battery demonstrates a coulombic efficiency of above 99%and an energy efficiency of~83%at a current density of80 m A cm^(-2),which can continuously run for more than 950 cycles.Most importantly,the battery demonstrates a coulombic efficiency of more than 99.0%and an energy efficiency of~83%for a long duration(~12,16 and 20 h per cycle)charge/discharge process.Benefiting from the low cost of iron electrolytes,the overall cost of the all-iron flow battery system can be reached as low as$76.11 per k Wh based on a10 h system with a power of 9.9 k W.This work provides a new option for next-generation cost-effective flow batteries for long duration large scale energy storage.

关键词： Long-duration energy storage All-iron flow battery Iron-based complexes High performance Gluconate

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High performance Zn-I_(2)battery with acetonitrile electrolyte working at low temperature

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Nano Research 2022年第4期15卷 3170-3177页

作者： Chunlai Song Zongshuai Gong Chong Bai Fengshi Cai Zhihao Yuan Xizheng Liu School of Materials Science and Engineering Tianjin Key Laboratory of Photoelectric Materials&DevicesKey Laboratory of Display Materials and Photoelectric Devices of Ministry of EducationTianjin University of TechnologyNo.391 Binshuixi RoadTianjin 300384China

Large scale applications of metal-iodine batteries working at sub-zero degree have been challenged by the limited capacity and performance degradation.Herein,we firstly propose a Zn-I_(2)battery working at low temperature with a carbon composite material/iodine(CCM-I_(2))cathode,a Zn anode and an environmentally tolerable Zn(ClO4)2-ACN electrolyte.The CCM framework with hierarchical porous structure endows a powerful iodine-anchoring to overcome undesirable dissolution of iodine in organic electrolyte,and the Zn(ClO4)2-ACN electrolyte with low freezing point and high ionic conductivity enhances the low temperature performance.The synergies enable an efficiently reversible conversion of Zn-I_(2)battery even at-40℃.Therefore,the resultant Zn-I_(2)battery delivers a high specific capacity of 200 mAh·g^(-1),which is fairly approximate to the theoretical capacity of I_(2)(211 mAh·g^(-1))and a superior cycling stability with minimal capacity fading of 0.00043%per cycle over 7,000 times under 2C at-20℃.Furthermore,even at-40℃,this Zn-I_(2)battery still exhibits a good capacity retention of 68.7%compared to the capacity at 25℃ and a rapid capacity-recover ability with elevating temperature change.Our results distinctly indicate this Zn-I_(2)battery can be 1competent for the practical application under low temperature operation.

关键词： Zn-I_(2)battery low temperature acetonitrile electrolyte carbon composite material High performance

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Cascading V_(2)O_(3)/N-doped carbon hybrid nanosheets as high-performance cathode materials for aqueous zinc-ion batteries

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Chinese Chemical Letters 2022年第3期33卷 1430-1434页

作者： Yue Niu Denghui Wang Yingjie Ma Linjie Zhi CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100039China

In recent years, especially when there is increasing concern about the safety issue of lithium-ion batteries (LIBs), aqueous Zn-ion batteries (ZIBs) have been getting a lot of attention because of their cost-effectiveness, materials abundance, high safety, and ecological friendliness. Their working voltage and specific capacity are mainly determined by their cathode materials. Vanadium oxides are promising cathode materials for aqueous ZIBs owing to their low cost, abundant resources, and multivalence. However, vanadium oxide cathodes still suffer from unsatisfactory capacity, poor stability, and low electrical conductivity. In this work, cascading V_(2)O_(3)/nitrogen doped carbon (V_(2)O_(3)/NC) hybrid nanosheets are prepared for high-performance aqueous ZIBs by pyrolyzing pentyl viologen dibromide (PV) intercalated V_(2)O5 nanosheets. The unique structure features of V_(2)O_(3)/NC nanosheets, including thin sheet-like morphology, small crystalline V_(2)O_(3) nanoparticles, and conductive NC layers, endow V_(2)O_(3)/NC with superior performance compared to most of the reported vanadium oxide cathode materials for aqueous ZIBs. The V_(2)O_(3)/NC cathode exhibits the discharge capacity of 405 mAh/g at 0.5 A/g, excellent rate capability (159 mAh/g at 20 A/g), and outstanding cycling stability with 90% capacity retention over 4000 cycles at 20 A/g.

关键词： Aqueous zinc ion batteries Cathode materials Vanadium oxides Nitrogen doped carbon 2D nanosheets High performance

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