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SSRN 2022年

作者： Luo, Ji Guo, Song Chen, Feixia Jiang, Bingli Wei, Lingzhong Gong, Yongyang Zhang, Beibei Liu, Yuanli Wei, Chun Tang, Ben Zhong Guangxi Key Laboratory of Optical and Electronic Materials and Devices College of Materials Science and Engineering Guilin University of Technology No.12 Jian’gan Rd. Qixing District Guilin541004 China College of Pharmacy Guilin Medical University No. 1 Zhiyuan Rd. Lingui District Guilin541199 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization China

The design and synthesis of organic nonconventional luminescent (NL) materials with efficient emission have attracted significant attention. However, these materials usually suffer from the fact of low photoluminescent quantum efficiency ( Φ ), poor tunability of emission wavelength, and non-luminescence in dilute solution, limiting their further application. Herein, rational molecular design strategies for NL compounds with efficient and tunable emission in dilute solution were presented via theoretical calculation and practical verification. Firstly, increasing the ratio of π-π* transition in the excited state to suppress the n-π* transition, inhibit intersystem crossing, and avoid the generation of triplet excitons which can be easily quenched by water or oxygen. Secondly, introducing strong intramolecular hydrogen bonds to suppress intramolecular rotation and inhibit non-radiative transitions. Besides, D-π-A structure can effectively adjust the luminescence color. Based on the proposed design strategies, two novel compounds named LJ-1 and LJ-2 were synthesized, both compounds can emit bright green fluorescence in dilute solution with F of up to 59.8%, and their photophysical properties are pH-dependent. The results showed that pH had a great impact on the strength of intramolecular hydrogen bonds and the degree of conjugation. For example, the emission wavelength of LJ-1 exhibited red-shift as the increase of pH value. Furthermore, LJ-1 can be used for visual detection of Ag+ in water solution in naked eye and the precise localization of lysosomes. We believe that our work will greatly broaden the application range of nonconventional luminogenic compounds in future. © 2022, The Authors. All rights reserved.

关键词： Excited states

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Non-fullerene Acceptors with a Thieno[3,4-c]pyrrole-4,6-dione(TPD) Core for Efficient Organic Solar Cells

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Chinese Journal of Polymer Science 2019年第10期37卷 1005-1014,I0005页

作者： Shi-Zhe Geng Wei-Tao Yang Jian Gao Shui-Xing Li Min-Min Shi Tsz-Ki Lau Xin-Hui Lu Chang-Zhi Li Hong-Zheng Chen Key Laboratory of Macromolecular Synthesis and Functionalization(Ministry of Education) State Key Laboratory of Silicon MaterialsDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Department of Physics The Chinese University of Hong KongNew TerritoriesHong KongChina

To achieve the red-shifted absorptions and appropriate energy levels of A-D-A type non-fullerene acceptors(NFAs), in this work, we design and synthesize two new NFAs, named TPDCIC and TPDCNC, whose electron-donating(D) unit is constructed by a thieno[3,4-c]pyrrole-4,6-dione(TPD) core attached to two cyclopentadithiophene(CPDT) moieties at both sides, and the electronaccepting(A) end-groups are 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile(IC) and 2-(3-oxo-2,3-dihydro-1 H-cyclopenta[b]naphthalen-1-ylidene)malononitrile(NC), respectively. Benefiting from TPD core, which easily forms quinoid structure and O···H or O···S intramolecular noncovalent interactions, TPDCIC and TPDCNC show more delocalization of π-electrons and perfect planar molecular geometries, giving the absorption ranges extended to 822 and 852 nm, respectively. Furthermore, the highest occupied molecular orbital(HOMO) levels of TPDCIC and TPDCNC remain relatively low-lying due to the electronegativity of the carbonyl groups on TPD core. Considering that the absorptions and energy levels of the two NFAs match well with those of a widely used polymer donor, PBDB-T, we fabricate two kinds of organic solar cells(OSCs) based on the PBDB-T:TPDCIC and PBDB-T:TPDCNC blended films, respectively. Through a series of optimizations, the TPDCIC-based devices yield an impressing power conversion efficiency(PCE)of 10.12% with a large short-circuit current density(JSC) of 18.16 mA·cm-2, and the TPDCNC-based ones exhibit a comparable PCE of9.80% with a JSC of 17.40 mA·cm-2. Our work is the first report of the TPD-core-based A-D-A type NFAs, providing a good reference for the molecular design of high-performance NFAs.

关键词： Non-fullerene acceptors (NFAs) Organic solar cells (OSCs) Thieno[3,4-c]pyrrole-4,6-dione (TPD) Narrow bandgap Energy levels

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Pressure-Engineered Through-Space Conjugation for Precise Control of Clusteroluminescence

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Angewandte Chemie 2024年第8期137卷

作者： Yayun Wang Zuping Xiong Yanan Wang Dr. Aisen Li Dr. Yuanyuan Fang Prof. Lei Li Prof. Kai Wang Prof. Qian Li Prof. Haoke Zhang School of Physics Science and Information Technology Liaocheng University Liaocheng Shandong 252000 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310058 China

Clusteroluminogens (CLgens) represent an innovative class of nonconjugated luminophores that address the limitations of conventional π-conjugated molecules. Different from the through-bond conjugation mechanism in π-conjugated luminophores, through-space conjugation (TSC) plays dominant roles in CLgens. However, precisely controlling TSC to customize the optical properties of CLgens remains a significant challenge. This work proposes a novel strategy of high pressure to engineer TSC within tetraphenylalkanes (TPAs)-based CLgens at molecular level. High-pressure exploration enables accurate manipulation of clusteroluminescence and elucidates the intrinsic structure–property relationships involved. Upon initial compression, the predominant molecular distortions marked by increased interfacial angles between benzene rings diminish TSC, resulting in anomalous hypochromatic shift in emission. Subsequently, considerable structural contraction enhances TSC and suppresses molecular motion, resulting in a pronouncedly enhanced and bathochromic-shifted emission. Notably, a series of TPAs-based CLgens exhibit intense white-light emission upon pressure release, attributed to irreversible structural distortion and destruction. This study not only advances the understanding of CLgens, but also underscores the crucial structural factors for effective TSC control, paving the way for establishing new photophysical theories for aggregate science.

关键词： Diamond anvil cell Through-space conjugation Aggregation-induced emission Clusteroluminescence Structure-property relationship

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Restriction of Intramolecular Motion(RIM):Investigating AIE Mechanism from Experimental and Theoretical Studies

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Chemical Research in Chinese Universities 2021年第1期37卷 1-15页

作者： ZHANG Jianyu ZHANG Haoke LAM Jacky W.Y. TANG Ben Zhong Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Centre for Tissue Restoration and ReconstructionInstitute for Advanced Studyand Department of Chemical and Biological EngineeringThe Hong Kong University of Science&TechnologyClear Water BayKowloonHong KongP.R.China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou310027P.R.China Center for Aggregation-Induced Emission SCUT-HKUST Joint Research InstituteState Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhou510640P.R.China Guangzhou Development District AIE InstituteGuangzhou510530P.R.China

Mechanistic studies promote scientific development from phenomena to ***-induced emission(AIE),as an unusual photophysical phenomenon,builds the bridge between molecular science and aggregate *** the twenty-year development of AIE,restriction of intramolecular motion(RIM)has been verified as the working mechanism of AIE *** this review,these mechanistic works about RIM are summarized from experimental and theoretical ***,the experimental studies are introduced from three parts:external rigidification,structural modification and structural *** the theoretical part,calculations on the low-frequency motion of AIEgens have been performed to prove the RIM *** virtue of the theoretical calculations,some new mechanisms are proposed to supplement the RIM,such as restriction of access to conical intersection,suppression of Kasha transition,restriction of access to dark state,*** is foreseeable that the RIM mechanism will unify the photophysical theories for both molecules and aggregates,and inspire more progress in aggregate science.

关键词： Aggregation-induced emission(AIE) Restriction of intramolecular motion Photophysical mechanism Aggregate science

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Construction of heparin-based hydrogel incorporated with Cu_(5.4)O ultrasmall nanozymes for wound healing and inflammation inhibition

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Bioactive Materials 2021年第10期6卷 3109-3124页

作者： Yuan Peng Danfeng He Xin Ge Yifei Lu Yuanhao Chai Yixin Zhang Zhengwei Mao Gaoxing Luo Jun Deng Yan Zhang Department of Plastic and Reconstructive Surgery Shanghai Ninth People’s HospitalShanghai JiaoTong University School of Medicine639 Zhi Zao Ju RoadShanghai200011China Institute of Burn Research Southwest HospitalState Key Lab of TraumaBurn and Combined InjuryChongqing Key Laboratory for Disease ProteomicsThird Military Medical University(Army Medical University)Chongqing400038China Department of Gastroenterology The Second Affiliated Hospital of Chongqing Medical UniversityChongqing400010China McKelvey School of Engineering Washington University in Saint LouisOne Brookings Drive Saint LouisMO63130USA MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou310027China

Excessive production of inflammatory chemokines and reactive oxygen species(ROS)can cause a feedback cycle of inflammation response that has a negative effect on cutaneous wound *** use of wound-dressing materials that simultaneously absorb chemokines and scavenge ROS constitutes a novel‘weeding and uprooting’treatment strategy for inflammatory *** the present study,a composite hydrogel comprising an amine-functionalized star-shaped polyethylene glycol(starPEG)and heparin for chemokine sequestration as well as Cu_(5.4)O ultrasmall nanozymes for ROS scavenging(Cu_(5.4)O@Hep-PEG)was *** material effectively adsorbs the inflammatory chemokines monocyte chemoattractant protein-1 and interleukin-8,decreasing the migratory activity of macrophages and ***,it scavenges the ROS in wound fluids to mitigate oxidative stress,and the sustained release of Cu_(5.4)O promotes *** acute wounds and impaired-healing wounds(diabetic wounds),Cu_(5.4)O@Hep-PEG hydrogels outperform the standard-of-care product Promogram®in terms of inflammation reduction,increased epidermis regeneration,vascularization,and wound closure.

关键词： Inflammatory chemokines Reactive oxygen species Nanozymes Hydrogels Wound healing

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Highly Regioselective Sequential 1,1-Dihydrosilylation of Terminal Aliphatic Alkynes with Primary Silanes

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Chinese Journal of Chemistry 2019年第5期37卷 457-461页

作者： Zhaoyang Cheng Shipei Xing Jun Guo Biao Cheng Lan-Fang Hu Xing-Hong Zhang Zhan Lu Deportment of Chemistry Zhejiang University Hangzhou Zhejiang 310058 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 China

Summary of main observation and conclusion A regioselective double 1,1-hydrosilylation of terminal aliphatic alkynes with primary silanes catalyzed by one cobalt catalyst has been developed. gem-Bis(dihydrosilyl)alkanes containing four silicon-hydrogen bonds are efficiently constructed in an atom-economical man ner. Tolerated substrates include simplest alkyne-ethyne, a complicated drug derivative and various functi on alized terminal aliphatic alkynes. Asymmetric approach using two catalysts is achieved with excelle nt enan tioselectivities to access corresp on ding chiral products. The tra nsformations of Si—H bonds into Si—C, Si—O, and Si —F bonds and the synthesis of enantioriched a-hydroxysilane show synthetic utility.

关键词： cobalt derivative utility

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White-light emission from organic aggregates:a review

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Advanced Photonics 2022年第1期4卷 13-29页

作者： Jianyu Zhang Xueqian Zhao Hanchen Shen Jacky W.Y.Lam Haoke Zhang Ben Zhong Tang The Hong Kong University of Science and Technology Department of ChemistryHong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstructionand Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional MaterialsClear Water BayKowloonHong KongChina Zhejiang University MOE Key Laboratory of Macromolecular Synthesis and FunctionalizationDepartment of Polymer Science and EngineeringHangzhouChina ZJU-Hangzhou Global Scientific and Technological Innovation Center HangzhouChina South China University of Technology Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesGuangzhouChina The Chinese University of Hong Kong Shenzhen Institute of Aggregate Science and TechnologySchool of Science and EngineeringShenzhenChina AIE Institute Guangzhou Development DistrictGuangzhouChina

White light,which contains polychromic visible components,affects the rhythm of organisms and has the potential for advanced applications of lighting,display,and *** with traditional incandescent bulbs and inorganic diodes,pure organic materials are superior in terms of better compatibility,flexibility,structural diversity,and environmental *** the past few years,polychromic emission has been obtained based on organic aggregates,which provides a platform to achieve white-light *** white-light emitters are sporadically reported,but the underlying mechanistic picture is still not fully *** on these considerations,we will focus on the single-component and multicomponent strategies to achieve efficient white-light emission from pure organic ***,single-component strategy is introduced from four parts:dual fluorescence,fluorescence and phosphorescence,dual phosphorescence with anti-Kasha’s behavior,and ***,doping,supramolecular assembly,and cocrystallization are summarized as strategies for multicomponent *** the construction strategies of white-light emitters,their advanced representative applications,such as organic light-emitting diodes,white luminescent dyes,circularly polarized luminescence,and encryption,are also *** is expected that this review will draw a comprehensive picture of white-light emission from organic aggregates as well as their emerging applications.

关键词： aggregate white-light emission aggregation-induced emission organic mechanism

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Bending Deformable Tension-Shear Model for Nacre-Like Composites

SSRN

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SSRN 2022年

作者： Chen, Yan Liu, Huichao Pang, Kai Zhang, Chen Qin, Huasong Xu, Zhen Liu, Yilun Laboratory for multiscale mechanics and medical science SV LAB School of Aerospace Xi'an Jiaotong University Xi’an710049 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Department of Polymer Science and Engineering Zhejiang University 38 Zheda Road Hangzhou310027 China First Aircraft Institute of Aviation Industry Corporation Xi’an710089 China

The nacre-like structures widely exist in biomaterials and bioinspired composites, where the tension-shear load transfer is the common load carrying mode due to the discontinuous platelet. However, under bending deformation the local tension-shear load transfer is coupled with the global bending deformation which can’t be described by the widely-adopted theoretical models in nacre-like composites, like the tension-shear chain (TSC) model and deformable tension-shear (DTS) model. In this work, a bending deformable tension-shear model (BDTS) model was developed to capture the tension-shear load transfer under bending configuration. In order to obtain a closed-form solution of BDTS model, the bending deformation of equal curvature was first studied, based on which two failure modes were defined, i.e., intralayer failure (Mode G) and interlayer failure (Mode I). Then, the effective bending rigidity of nacre-like structure, defined as the ratio of the average moment to curvature, was obtained, indicating the influence of material and geometrical parameters can be unified to a dimensionless parameter L/l_t, where L is the length of platelet and l_t=√((E_h h_h h_s)⁄G_s ) is the characteristic length parameter of tension-shear load transfer (E_h and G_s are Young’s modulus of hard layer and shear modulus of soft layer, h_h and h_s are the thickness of hard and soft layers, respectively). Furthermore, a general beam theory of nacre-like structures was constructed by introducing the effective bending rigidity to the modified Timoshenko beam model, which can predict the deflection of nacre-like structures well. This work first explores the two coupled deformations of local tension-shear and global bending-shear in nacre-like composites, which may guide the design of nacre-like artificial nanocomposites toward various applications where bending deformation is inevitable. © 2022, The Authors. All rights reserved.

关键词： Geometry

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Inhibition of furin by bone targeting superparamagnetic iron oxide nanoparticles alleviated breast cancer bone metastasis

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Bioactive Materials 2021年第3期6卷 712-720页

作者： Yichuan Pang Li Su Yao Fu Fan Jia Chenxi Zhang Xiankun Cao Wenxin He Xueqian Kong Jiake Xu Jie Zhao An Qin Shanghai Key Laboratory of Orthopedic Implants Department of OrthopaedicsShanghai Ninth People's HospitalShanghai Jiaotong University School of MedicineShanghai200011China Department of Nuclear Medicine Shanghai Tenth People's HospitalTongji University School of MedicineShanghai200072China Hongqiao International Institute of Medicine Shanghai Jiaotong University School of Medicine201103China Center for Chemistry of High-Performance&Novel Materials Department of ChemistryZhejiang UniversityHangzhou310027China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou310027China School of Biomedical Sciences The University of Western AustraliaPerthWestern Australia6009Australia

Breast cancer bone metastasis poses significant challenge for therapeutic *** the metastatic environment,osteoclasts and tumor cells interact synergistically to promote cancer *** this study,the proprotein convertase furin is targeted due to its critical roles in both tumor cell invasion and osteoclast ***,the furin inhibitor is specifically delivered by bone targeting superparamagnetic iron oxide(SPIO)*** in vitro and in vivo data demonstrate that this system can effectively inhibit both osteoclastic bone resorption and breast cancer invastion,leading to alleviated ***,the bone targeting&furin inhibition nanoparticle system is a promising therapeutic and diagnostic strategy for breast cancer bone metastasis.

关键词： Breast cancer metastasis Osteoclast Furin Bone targeting Iron oxide nanoparticles

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Thermo-sensitive Microgels Supported Gold Nanoparticles as Temperature-mediated Catalyst

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Chinese Journal of Polymer Science 2019年第3期37卷 235-242页

作者： Xian-Jing Zhou Hai-Peng Lu Ling-Li Kong Dong Zhang Wei Zhang Jing-Jing Nie Jia-Yin Yuan Bin-Yang Du Xin-Ping Wang Department of Chemistry Zhejiang Sci-Tech University Department of Chemistry Zhejiang University Department of Materials and Environmental Chemistry Stockholm University Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science & Engineering Zhejiang University

Microgels with a thermo-sensitive poly(N-isopropylacrylamide)(polyNIPAm) backbone and bis-imidazolium(VIM) ionic cross-links, denoted as poly(NIPAm-co-VIM), were successfully prepared. The as-synthesized ionic microgels were converted to nanoreactors, denoted as Au@PNI MGs, upon generation and immobilization of gold nanoparticles(Au NPs) of 5–8 nm in size into poly(NIPAm-co-VIM). The content of Au NPs in microgels could be regulated by controlling the 1,6-dibromohexane/vinylimidazole molar ratio in the quaternization reaction. The microgel-based nanoreactors were morphologically spherical and uniform in size, and presented reversible thermo-sensitive behavior with volume phase transition temperatures(VPTTs) at 39–40 °C. The Au@PNI MGs were used for the reduction of 4-nitrophenol, of which the catalytic activity could be modulated by temperature.

关键词： Microgel Thermo-sensitive Gold nanoparticle Catalyst

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