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Thiazoloisoindigo-based Polymer Semiconductors: Synthesis,Structure-Property Relationship, Charge Carrier Polarity, and Field-Effect Transistor Performance

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Chinese Journal of Polymer Science 2024年第1期42卷 24-31,I0006页

作者： Bo-Wen Li Miao Xiong Mei-Hua Liu Zhi-Gao Li Long Sang Zi-Han Xiong Biao Xiao Jian Pei Xiao-Bo Wan key laboratory of Optoelectronic Chemical Materials and Devices Ministry of EducationSchoolofOptoelectronic Materials&TechnologyJianghan UniversityWuhan430056China Bejing National laboratoryfor molecular Sciences the Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Developing new polymeric semiconductors with excellent device performance is essential for organic electronics. Herein, we synthesized two new thiazoloisoindigo(Tz II)-based polymers, namely, P(Tz II-d Th-d Th) and P(Tz II-d Th-d Tz), by copolymerizing thiophene-flanked Tz II with bithiophene and bithiazole, respectively. Owing to the more electron-deficient nature of bithiazole than bithiophene, P(Tz II-d Th-d Tz)possesses deeper LUMO/HOMO levels of-3.45/-5.47 e V than P(Tz II-d Th-d Th)(-3.34/-5.32 e V). The organic field-effect transistor(OFET) devices based on P(Tz II-d Th-d Th) exhibited p-type behaviors with an average hole mobility value as high as 1.43 cm^(2)·V^(-1)·s^(-1), while P(Tz II-d Th-d Tz)showed typical ambipolar characteristics with average hole and electron mobilities of 0.38 and 0.56 cm^(2)·V^(-1)·s^(-1). In addition, we compared the performances of both polymers with other Tz II-based polymers reported in our previous work, and showed that the charge carrier polarity can be manipulated by adjusting the number of the thiophene units between the acceptor unit. As the increase of the number of thiophene rings,charge carrier polarity shifts from electron-dominated ambipolar transport to hole-dominated ambipolar transport and then to unipolar hole transport in OFETs, which provides an effective molecular design strategy for further optimization of polymer OFET performance.

关键词： Field-effect transistor Charge carrier polarity Thiazoloisoindigo

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Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu key laboratory of Organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China key laboratory of Organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for *** this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction ***3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 *** a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film ***3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer ***,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 *** work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor

Integrated multi-scale approach combining global homogenization and local refinement for multi-field analysis of high-temperature superconducting composite magnets

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Applied Mathematics and Mechanics(English Edition) 2024年第5期45卷 747-762页

作者： Hanxiao GUO Peifeng GAO Xingzhe WANG key laboratory of Mechanics on Western Disaster and Environment of ministry of education Key Laboratory of Special Function Materials and Structure Design of Ministry of EducationCollege of Civil Engineering and MechanicsLanzhou UniversityLanzhou 730000China

Second-generation high-temperature superconducting(HTS)conductors,specifically rare earth-barium-copper-oxide(REBCO)coated conductor(CC)tapes,are promising candidates for high-energy and high-field superconducting *** respect to epoxy-impregnated REBCO composite magnets that comprise multilayer components,the thermomechanical characteristics of each component differ considerably under extremely low temperatures and strong electromagnetic *** numerical models include homogenized orthotropic models,which simplify overall field calculation but miss detailed multi-physics aspects,and full refinement(FR)ones that are thorough but computationally ***,we propose an extended multi-scale approach for analyzing the multi-field characteristics of an epoxy-impregnated composite magnet assembled by HTS pancake *** approach combines a global homogenization(GH)scheme based on the homogenized electromagnetic T-A model,a method for solving Maxwell's equations for superconducting materials based on the current vector potential T and the magnetic field vector potential A,and a homogenized orthotropic thermoelastic model to assess the electromagnetic and thermoelastic properties at the macroscopic *** then identify“dangerous regions”at the macroscopic scale and obtain finer details using a local refinement(LR)scheme to capture the responses of each component material in the HTS composite tapes at the mesoscopic *** results of the present GH-LR multi-scale approach agree well with those of the FR scheme and the experimental data in the literature,indicating that the present approach is accurate and *** proposed GH-LR multi-scale approach can serve as a valuable tool for evaluating the risk of failure in large-scale HTS composite magnets.

关键词： epoxy-impregnated high-temperature superconducting(HTS)magnet multi-scale method global homogenization(GH) local refinement(LR) multi-field analysis

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Light/pH dual-responsive magnetic metal-organic frameworks composites for phosphorylated peptide enrichment

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Chinese Chemical Letters 2024年第7期35卷 222-226页

作者： Rui Wang He Qi Haijiao Zheng Qiong Jia College of Chemistry Jilin UniversityChangchun 130012China key laboratory for molecular enzymology and engineering of ministry of education School of Life SciencesJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)combined with specific ligands are highly adaptable smart materials that can respond to external and physiological *** this study,we introduced a pyridinyl zwitterionic ligand with light/pH dual response into magnetic MOF composite(Fe_(3)O_(4)@ZW-MOF)for enrichment of phosphorylated peptides for the first *** introduction of the developed ligand gives MOF material dual response *** stimulation affects the generation/disappearance of free radicals of the pyridine derivative,resulting in a change in the charge gradient of the zwitterion,and zwitterion can also regulate the p H of the solution by adding acid or ***,the reversible capture and release of phosphorylated peptides can be easily achieved by adjusting light and *** established phosphorylated peptide enrichment platform exhibits high sensitivity(detection limit of 1 fmol),high selectivity(β-casein:BSA,1:1000),and good reusability(7 cycles).In addition,the method was applied to the enrichment of phosphorylated peptides in complex systems(non-fat milk and human serum),demonstrating the feasibility of this method for phosphoproteom *** conclusion,the synthesized Fe_(3)O_(4)@ZW-MOF is a promising MOF material,which provides the possibility to advance the application of responsive MOFs materials in proteomics.

关键词： Light pH Dual-response Metal-organic frameworks Phosphorylated peptide

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Ultrafast micro/nano-manufacturing of metastable materials for energy

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National Science Review 2024年第4期11卷 283-298页

作者： Xiaoya Cui Yanchang Liu Yanan Chen School of Materials Science and engineering Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) and Tianjin Key Laboratory of Composite and Functional MaterialsTianjin University ministry of education key laboratory of Protein Sciences School of Life SciencesTsinghua University

The structural engineering of metastable nanomaterials with abundant defects has attracted much attention in energy-related fields. The high-temperature shock(HTS) technique, as a rapidly developing and advanced synthesis strategy, offers significant potential for the rational design and fabrication of high-quality nanocatalysts in an ultrafast, scalable, controllable and eco-friendly way. In this review, we provide an overview of various metastable micro-and nanomaterials synthesized via HTS, including single metallic and bimetallic nanostructures, high entropy alloys, metal compounds(e.g. metal oxides) and carbon nanomaterials. Note that HTS provides a new research dimension for nanostructures, i.e. kinetic modulation. Furthermore, we summarize the application of HTS—as supporting films for transmission electron microscopy grids—in the structural engineering of 2D materials, which is vital for the direct imaging of metastable materials. Finally, we discuss the potential future applications of high-throughput and liquid-phase HTS strategies for non-equilibrium micro/nano-manufacturing beyond energy-related *** is believed that this emerging research field will bring new opportunities to the development of nanoscience and nanotechnology in both fundamental and practical aspects.

关键词： high-temperature shock technique defect engineering metastable phase kinetic modulation non-equilibrium micro/nano-manufacturing

Comparison of Measurements for Enhanced Diffusion Problem in Chemical Reaction Systems

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Chinese Journal of Chemistry 2024年第14期42卷 1659-1664页

作者： Ah-Young Jee Ziyang Wen Huan Wang Beijing National laboratory for molecular Sciences College of Chemistry and Molecular EngineeringBeijing Key Laboratory of Polymer Chemistry&Physics of Ministry of EducationPeking UniversityBeijing100871 China

The problem of molecular diffusion in the soup of chemical reactions attracts mounting interest across fields ranging from chemistry to biophysics to material *** reactions involve bond breakup and formation,whose time scale is typically on the orders of fs to ps,while molecular diffusion occurs at time scales ofμs to *** two processes are often considered orthogonal,given the vastly different *** serial results show that the enzyme's diffusion is enhanced in a substrate-dependent manner,which was further extended to small molecule reaction systems,challenging this classical ***,the results from different groups using different techniques do not quantitatively agree,and a general mechanism is yet to be *** summarize experimental studies on diffusion problems and seek to reconcile the interpretation with understanding the limits of measurement tools and the chemical nature of reaction *** molecular diffusion in chemical reactions will provide fresh thoughts in designing chemical systems such as molecular machines that harvest work at the nanoscale in a controllable manner.

关键词： molecular diffusion Chemical reactions Enzyme reactions Active matter Diffusion measurements Single-molecule studies Fluorescence Time-resolved spectroscopy

In situ embedded bismuth nanoparticles among highly porous carbon fibers for efficient carbon dioxide reduction

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Rare Metals 2024年第9期43卷 4312-4320页

作者： Wei-Jian Guo Ao Zhou Wen-Wen Cai Jin-Tao Zhang key laboratory for Colloid and Interface Chemistry (ministry of education) School of Chemistry and Chemical EngineeringShandong University

Electrocatalysis provides an optimal approach for the conversion of carbon dioxide(CO2) into high-value chemicals, thereby presenting a promising avenue toward achieve carbon neutrality. However, addressing the selectivity and stability challenges of metal catalysts in electrolytic reduction remains a daunting task. In this study, the electrospinning method is employed to fabricate porous carbon nanofibers loaded with bismuth nanoparticles with the help of in situ pyrolysis. The porous carbon nanofibers as conductive support would facilitate the dispersion of bismuth active sites while inhibiting their aggregation and promoting the mass transfer, thus enhancing their electrocatalytic activity and stability. Additionally, nitrogen doping induces electron delocalization in bismuth atoms through metal-support interactions, thus enabling efficient adsorption of intermediates for improving selectivity based on the theoretical calculation. Consequently, Bi@PCNF-500 exhibits the exceptional selectivity and stability across a wide range of potential windows. Notably, its faradaic efficiency(FE) of formate reaches 92.7% in H-cell and94.9% in flow cell, respectively, with good electrocatalytic stability. The in situ characterization and theoretical calculations elucidate the plausible reaction mechanism to obtain basic rules for designing efficient electrocatalyst.

关键词： Carbon dioxide reduction Electron delocalization N-doping Porous carbon nanofiber

Cross-linkedα-amylase aggregates on Fe3O4 magnetic nanoparticles modified with polydopamine/polyethyleneimine for efficient hydrolysis of starch

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Particuology 2024年第7期90卷 98-105页

作者： Jiandong Cui Xiuming Tang Qingqing Ma Yuyan Chang Qunli Zhang Shiru Jia State key laboratory of Food Nutrition and Safety Laboratory of Industrial Fermentation MicrobiologyMinistry of EducationTianjin University of Science and TechnologyTianjin 300457China key laboratory of Biomass Chemical engineering of ministry of education Zhejiang UniversityHangzhou 310027China

In this workα-amylase was immobilized on magnetic Fe3O4 nanoparticles with polyethylenimine(PEI)/polydopamine(PDA)coating or 3-aminopropyl triethoxysilane(APTES)for the first time via adsorption–precipitation–*** with the freeα-amylase,the resultant magnetic cross-linkedα-amylase aggregates(PEI/PDA-M-CLEAs and N-M-CLEAs)exhibited excellent thermal and storage stability as well as pH *** storage at 25°C for 60 days,freeα-amylase only retained 60%of its initial activity,while PEI/PDA-M-CLEAs and N-M-CLEAs retained 80%and 78%of their initial activities,***,N-M-CLEAs and PEI/PDA-M-CLEAs showed good *** 6 repeated uses,PEI/PDA-M-CLEAs and N-M-CLEAs still maintained 65%and 62%of their initial activities,***,PEI/PDA-M-CLEAs and N-M-CLEAs exhibited higher starch hydrolysis efficiency than freeα-*** maximum dextrose equivalent(DE)values of starch hydrolysis by PEI/PDA-M-CLEAs and N-M-CLEAs reached 29.24%and 28.79%within 90 min,***,the maximum DE values of starch hydrolysis by the freeα-amylase was only 27.89%even in 150 *** magnetic cross-linkedα-amylase aggregates could be introduced as effective biocatalyst for industrial applications in production of maltose syrups.

关键词： α-amylase Magnetic nanoparticles Functional modification Magnetic cross-linked enzyme aggregates Hydrolysis of starch

Spontaneous anchoring Cl into α-Co（OH）2 as efficient and stable oxygen reduction electrocatalysts for seawater battery

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Rare Metals 2024年第7期43卷 3074-3083页

作者： Wang Zheng Xue-Rong Zheng Qi Lu Yan-Hui Cao Yang Wang Hai-Peng Fu Jin-Feng Zhang Yi-Da Deng Wen-Bin Hu School of Materials Science and engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin University State key laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan University key laboratory of Electromagnetic Processing of Materials Ministry of EducationNortheastern University

Seawater battery is an advanced energy storage system that enables conversion of chemical energy to electricity by consuming metals,dissolved oxygen and seawater in anode,cathode and electrolyte,***,the oxygen reduction reaction（ORR） activity and stability of electrocatalysts can be easily deactivated due to the severe Cl-permeation and corrosion in seawater ***,we developed a structural buffer engineering strategy by spontaneously anchoring Cl-into α-Co（OH）2as efficient and stable ORR electrocatalysts,in which the ultrathin α-Co（OH）2nanosheets were synthesized using an ultrafast solution high-temperature shock（SHTS） *** large lattice space（～ 0.8 nm） of layered α-Co（OH）2ensured the spontaneously penetration of Cl-into the lattice structure and replaced part of OH-to form α-Co（OH）*** continuous leaching and compensating of saturated Cl in α-Co（OH）2-xClxcould enhance the Cl-corrosion resistance and modulate electronic structure of Co metallic sites,thus improving the ORR electrocatalytic activity and stability in seawater *** α-Co（OH）2-xClxseawater batteries display superior onset and half-wave potentials of 0.71 and 0.66 V,respectively,which are much better than the counterparts of α-Co（OH）2and of β-Co（OH）2with no Cl-penetrating and no buffer *** α-Co（OH）2-xClx-based seawater batteries display stable open-circuit potential of 1.69 V and outstanding specific capacity of 1345 mAh·g-1.

关键词： Seawater battery Oxygen reduction electrocatalyst Solution high-temperature shock Structural buffer engineering