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Granular Ionogel Particle Inks for 3D Printed Tough and Stretchable Ionotronics

Research 2024年第1期2023卷 429-442页

作者： Yuan Yao Yue Hui Zhenhua Wang Hehao Chen Heng Zhu Nanjia Zhou key laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province School of EngineeringWestlake UniversityHangzhou 310024Zhejiang ProvinceChina Institute of Advanced Technology Westlake Institute for Advanced StudyHangzhou 310024Zhejiang ProvinceChina School of Chemical Engineering and Advanced Materials the University of AdelaideAdelaide 5005South AustraliaAustralia State key laboratory of Fluid Power&Mechatronic System Key Laboratory of Soft Machines and Smart Devices of Zhejiang ProvinceCenter for X-MechanicsDepartment of Engineering MechanicsZhejiang UniversityHangzhou 310027China

Ionogels have garnered great attention as promising soft conducting materials for the fabrication of flexible energy storage devices,soft actuators,and ionotronics.However,the leakage of the ionic liquids,weak mechanical strength,and poor manufacturability have greatly limited their reliability and applications.Here,we propose a new ionogel synthesis strategy by utilizing granular zwitterionic microparticles to stabilize ionic liquids.The ionic liquids swell the microparticles and physically crosslink microparticles via either electronic interaction or hydrogen bonding.Further introducing a photocurable acrylic monomer enables the fabrication of double-network(DN)ionogels with high stretchability(>600%)and ultrahigh toughness(fracture energy>10 kJ/m^(2)).The synthesized ionogels exhibit a wide working temperature of−60 to 90℃.By tuning the crosslinking density of microparticles and physical crosslinking strength of ionogels,we synthesize DN ionogel inks and print them into three-dimensional(3D)motifs.Several ionogelbased ionotronics are 3D printed as demonstrations,including strain gauges,humidity sensors,and ionic skins made of capacitive touch sensor arrays.Via covalently linking ionogels with silicone elastomers,we integrate the ionogel sensors onto pneumatic soft actuators and demonstrate their capacities in sensing large deformation.As our last demonstration,multimaterial direct ink writing is harnessed to fabricate highly stretchable and durable alternating-current electroluminescent devices with arbitrary structures.Our printable granular ionogel ink represents a versatile platform for the future manufacturing of ionotronics.

关键词： crosslinking utilizing gauge

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The dynamic surface evolution of halide perovskites induced by external energy stimulation

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National Science Review 2024年第4期11卷 185-194页

作者： Feiyu Cheng Pengdong Wang Chenzhe Xu Qingliang Liao Suicai Zhang Haochun Sun Wenqiang Fan Guodong Liu Zhiyun Li Yaping Kong Li Wang Fangsen Li Zhuo Kang Yue Zhang Academy for Advanced Interdisciplinary Science and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing key laboratory for Advanced Energy Materials and Technologies Key Laboratory of Advanced Materials and Devices for Post-Moore ChipsMinistry of EducationBeijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology Beijing Vacuum Interconnected Nanotech Workstation(Nano-X) Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Beijing National laboratory for Condensed matter Physics Institute of Physics Chinese Academy of Sciences

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum（UHV） interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position,hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

关键词： metal halide perovskite external energy stimulation surface dynamic evolution surface electronic structure ultra-high vacuum interconnection system

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pH- and near-infrared light-responsive,biomimetic hydrogels from aqueous dispersions of carbon nanotubes

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Nano Research 2024年第4期17卷 3120-3129页

作者： Lulin Hu Xinxin Yu Jingcheng Hao Lu Xu Shandong laboratory of Yantai Advanced Materials and Green Manufacturing Yantai 264000China State key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Yantai Center for Food and Drug Control Yantai 264000China key laboratory of Colloid and Interface chemistry&key laboratory of Special Aggregated Materials Shandong UniversityJinan 250100China

Owing to their low flexibility,poor processability and a lack of responsiveness,inorganic materials are usually non-ideal for constructing a living organism.Hence,to date,lifelike materials with structural hierarchies and adaptive properties usually rely on light and soft organic molecules,although few exceptions have been acquired using two-dimensional(2D)inorganic nanosheets.Herein,with a systematic study on the gelation behavior of carbon-based 0D quantum dots,1D nanotubes,and 3D fullerenes,we find that acidified 1D carbon nanotubes(CNTs)can serve as an alternative building block for fabricating purely inorganic biomimetic soft materials.The as-prepared CNT gels exhibit not only a pH-or photothermal-triggered mechanical and tribological adaptivity,which allows them to simulate the behavior of sea cucumbers,peacock mantis shrimps,and mammalian muscles or cortical bones,but also a unique damping property that is similar to spider’s cuticular pad.Their high elasticity,effective lubrication,excellent biocompatibility,and controllable friction and wear also allow them to function as a new type of smart lubricants,whose tribological properties can be regulated either by its internal pH changes or spatiotemporally by near-infrared(NIR)light irradiations,free of any toxic and flammable base oils or additives.

关键词： biomimetic hydrogels carbon nanotubes(CNTs) mechanical and tribological adaptivity pH-and near-infrared(NIR)light responsiveness switchable lubrication

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Estimation of cancer cell migration in biomimetic random/oriented collagen fiber microenvironments

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Chinese Physics B 2024年第5期33卷 749-756页

作者：姚静如李国强姚喜耀周连杰叶志凯刘艳平郑栋天唐婷宋克纳陈果刘雳宇 Chongqing key laboratory of soft Condensed matter Physics and Smart Materials College of PhysicsChongqing UniversityChongqing 401331China Chongqing key laboratory for Resource Utilization of Heavy Metal Wastewater Aquatic Ecosystems in the Three Gorges Reservoir Region of Chongqing Observation and Research StationChongqing University of Arts and SciencesYongchuan 402160China Wenzhou Institute University of Chinese Academy of SciencesWenzhou 325000China Department of Biomedical Engineering Chongqing University of Posts and TelecommunicationsChongqing 400065China College of Medical Technology and Engineering Henan University of Science and TechnologyHenan 471023China

Increasing data indicate that cancer cell migration is regulated by extracellular matrixes and their surrounding biochemical microenvironment,playing a crucial role in pathological processes such as tumor invasion and metastasis.However,conventional two-dimensional cell culture and animal models have limitations in studying the influence of tumor microenvironment on cancer cell migration.Fortunately,the further development of microfluidic technology has provided solutions for the study of such questions.We utilize microfluidic chip to build a random collagen fiber microenvironment(RFM)model and an oriented collagen fiber microenvironment(OFM)model that resemble early stage and late stage breast cancer microenvironments,respectively.By combining cell culture,biochemical concentration gradient construction,and microscopic imaging techniques,we investigate the impact of different collagen fiber biochemical microenvironments on the migration of breast cancer MDA-MB-231-RFP cells.The results show that MDA-MB-231-RFP cells migrate further in the OFM model compared to the RFM model,with significant differences observed.Furthermore,we establish concentration gradients of the anticancer drug paclitaxel in both the RFM and OFM models and find that paclitaxel significantly inhibits the migration of MDA-MB-231-RFP cells in the RFM model,with stronger inhibition on the high concentration side compared to the low concentration side.However,the inhibitory effect of paclitaxel on the migration of MDA-MB-231-RFP cells in the OFM model is weak.These findings suggest that the oriented collagen fiber microenvironment resembling the late-stage tumor microenvironment is more favorable for cancer cell migration and that the effectiveness of anticancer drugs is diminished.The RFM and OFM models constructed in this study not only provide a platform for studying the mechanism of cancer development,but also serve as a tool for the initial measurement of drug screening.

关键词： microfluidic chip random collagen fiber microenvironment(RFM) oriented collagen fiber microenvironment(OFM) cancer cell migration

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Anisotropic s-Wave Gap in the Vicinity of a Quantum Critical Point in Superconducting BaFe_(2)(As_(1-x)P_(x))_(2) Single Crystals:A Study of Point-Contact Spectroscopy

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Chinese Physics Letters 2024年第4期41卷 118-123页

作者：詹红星林玉尺赵宇清左海艳王兴玉马肖燕李春红罗会仟陈根富李世亮任聪 School of Physics and Astronomy Yunnan UniversityKunming 650500China Beijing National laboratory for Condensed matter Physics and Institute of PhysicsChinese Academy of SciencesBeijing 100190China Yunnan key laboratory for Electromagnetic Materials and Devices Yunnan UniversityKunming 650500China

We report on soft c-axis point-contact Andreev reflection(PCAR)spectroscopy combining with resistivity measurements on BaFe_(2)(As_(0.7)P_(0.3))_(2),to elucidate the superconducting gap structure in the vicinity of the quantum critical point.A double peak at the gap edge plus a dip feature at zero-bias has been observed on the PCAR spectra,indicative of the presence of a nodeless gap in BaFe_(2)(As_(0.7)P_(0.3))_(2).Detailed analysis within a sophisticated theoretical model reveals an anisotropic gap with deep gap minima.The PCARs also feature additional structures related to the electron-bosonic coupling mode.Using the extracted superconducting energy gap value,a characteristic bosonic energy Ω_(b) and its temperature dependence are obtained,comparable with the spin-resonance energy observed in neutron scattering experiment.These results indicate a magnetism-driven quantum critical point in the BaFe_(2)(As_(1-x)P_(x))_(2) system.

关键词： quantum critical resistivity

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Room-temperature synthesis of full-component APbX_(3)perovskite nanocrystal inks for optoelectronic applications

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Journal of Energy chemistry 2024年第5期92卷 87-94页

作者： Xinyu Zhao Du Li Xuliang Zhang Hehe Huang Chenyu Zhao Wanli Ma Jianyu Yuan Institute of Functional Nano&soft Materials(FUNSOM) Soochow UniversitySuzhou 215123JiangsuChina Jiangsu key laboratory for Carbon-Based Functional Materials&Devices Soochow UniversitySuzhou 215123JiangsuChina Jiangsu key laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123JiangsuChin

Lead halide perovskite nanocrystals(PNCs)have received great research interests due to their excellent optoelectronic properties.However,high temperature,inert gas protection and insulating long-chain ligands are used during the conventional hot-injection synthesis of PNCs,which limits their practical applications.In this work,we first develop a simple and scalable polar-solvent-free method for the preparation of full-component APbX_(3)(A=Cs,methylammonium(MA),formamidinium(FA),X=Cl,Br,I)PNCs under ambient condition.Through an exothermic reaction between butylamine(BA)and propionic acid(PA)short ligands,the PbX_(2) precursors could be well dissolved without use of any polar solvent.Meanwhile,the relatively lower growth rate of PNCs in our room-temperature reaction enables us to modulate the synthetic procedure to enhance the scalability(40-fold)and achieve large-scale synthesis.The resultant short ligands passivated PNC inks are compatible with varying solution depositing technique like spray coating for large-area film.Finally,we showcase that adopting the as-prepared MAPbI_(3) PNC inks,a self-powered photodetector is fabricated and shows a high photoresponsivity.These results demonstrate that our ambient-condition synthetic approach can accelerate the preparation of tunable and ready-to-use PNCs towards commercial optoelectronic applications.

关键词： Room-temperaturesynthesis Perovskite nanocrystals Short-chainligands Large-scale Photodetector

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AI for organic and polymer synthesis

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Science China chemistry 2024年第8期 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen Fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu Huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You Department of Chemical Sciences National Natural Science Foundation of China State key laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Center of chemistry for Frontier Technologies Department of Chemistry Zhejiang University Center of Basic Molecular Science Department of Chemistry Tsinghua University Guangzhou National laboratory Center for Quantitative Biology Academy for Advanced Interdisciplinary Studies Peking University State key laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Fudan University School of Materials Science and Engineering Peking University AI for Science (AI4S)-Preferred Program Shenzhen Graduate School Peking University Beijing National laboratory for Molecular Sciences Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education College of Chemistry and Molecular Engineering Peking University State key laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

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Stretchable and self-healing conductive fibers from hierarchical silver nanowires-assembled network

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Nano Research 2024年第2期17卷 763-770页

作者： Ying-Ying Wu Hong Chen Fan Zhang Pan Guo Haili Qin Huai-Ping Cong Anhui Province key laboratory of Advanced Catalytic Materials and Reaction Engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China

Conductive fibers(CFs)with features of high conductivity,stretchability,self-healability,and electromechanical stability are key components of the increasingly popular wearable electronics.However,since the lack of structural design of conductive network and interfacial interaction between soft polymer and conductive additives,it is still hard to enable CFs to meet above requirements.Here,we describe a facial drawing method from a hydrogel reservoir which is remolded into ultrathin and stretchable CFs with excellent multi-responsive self-healability.The hydrogel reservoir was fabricated in synergy of an ice-templating method and in situ polymerization using the assembled framework as a crosslinker.Relying on the effective fabrication mechanism,the diameter of CFs could be well-tuned from 90 to 400μm by adjusting the dipping depth of the glass rod,accompanied with conductivity increased from 0.75 to 2.5 S/m.Since the hierarchical network structure was well maintained in the CFs,professional performances have been proved on the stretchability and electromechanical stability.The presence of massive hydrogen bonding and Ag–S bond enabled the CFs with excellent self-healability under the conditions of contact,electric field,and near infrared light,respectively.Excitingly,the CFs with high sensing property could be integrated into an advanced textile sensor through an effective healing-induced integration strategy,demonstrating its great potentials as superior two-dimensional(2D)electronic skins.

关键词： conductive fibers self-assembled silver nanowires Ag–S coordination self-healing flexible sensors

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Tailoring the Properties of Polyhydroxyalkanoates from Plastics to Elastomers via Stereoselective Copolymerizations of rac-β-Butyrolactone andβ-Propiolactone

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Chinese Journal of chemistry 2024年第9期42卷 963-972页

作者： Haoran Zhang JiaojiaoQin Xiaoyan Tang Beijing National laboratoryfor Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenterforSoftMatter Science and EngineeringCollegeof Chemistry andMolecularEngineeringPeking UniversityBeijing 100871China

Poly(3-hydroxybutyrate),a crucial member of the large biodegradable polyhydroxyalkanoate family,suffers from its brittleness.To enhance its performance,we employed a straightforward approach involving the ring-opening copolymerization of racemic-β-butyrolactone(rac-β-BL)andβ-propiolactone(β-PL)using the syndio-selective amino-alkoxy-bis(phenolate)-yttrium complex as a catalyst,thanks to the excellent ductility of poly(3-hydroxypropionate).Control over the rac-β-BL/β-PL feeding ratios and polymerization time yielded random or block copolymers with tunable thermal and mechanical properties comparable to traditional fossil-based plastics.Furthermore,we achieved one-pot synthesis of hard-soft-hard triblock copolymers by exploiting monomers’different copolymerization rates and a bifunctional initiator,thus transforming polyhydroxyalkanoates from hard and tough plastics to soft and ductile thermoplastic elastomers.

关键词： Ring-opening(co-)polymerization Biodegradable polymers Polyhydroxyalkanoates Copolymers Plastics Elastomers

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Tuning mechanical behaviors of highly entangled hydrogels with the random distribution of mobile entanglements

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Applied Mathematics and Mechanics(English Edition) 2024年第2期45卷 277-294页

作者： Jinlong LIU Di LU Bin CHEN Department of Engineering Mechanics Zhejiang UniversityHangzhou 310027China Beijing System Design Institute of Electro-Mechanic Engineering Beijing 100854China Intelligent Robotic Research Center Zhejiang LaboratoryHangzhou 310027China key laboratory of soft Machines and Smart Devices of Zhejiang Province Hangzhou 311100China

Highly entangled hydrogels exhibit excellent mechanical properties,including high toughness,high stretchability,and low hysteresis.By considering the evolution of randomly distributed entanglements within the polymer network upon mechanical stretches,we develop a constitutive theory to describe the large stretch behaviors of these hydrogels.In the theory,we utilize a representative volume element(RVE)in the shape of a cube,within which there exists an averaged chain segment along each edge and a mobile entanglement at each corner.By employing an explicit method,we decouple the elasticity of the hydrogels from the sliding motion of their entanglements,and derive the stress-stretch relations for these hydrogels.The present theoretical analysis is in agreement with experiment,and highlights the significant influence of the entanglement distribution within the hydrogels on their elasticity.We also implement the present developed constitutive theory into a commercial finite element software,and the subsequent simulations demonstrate that the exact distribution of entanglements strongly affects the mechanical behaviors of the structures of these hydrogels.Overall,the present theory provides valuable insights into the deformation mechanism of highly entangled hydrogels,and can aid in the design of these hydrogels with enhanced performance.

关键词： highly entangled hydrogel constitutive theory entanglement gamma distribution

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