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molecular engineering of Y-series acceptors for nonfullerene organic solar cells

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SusMat 2022年第5期2卷 591-606页

作者： Qiao He Petr Ufimkin Filip Aniés Xiantao Hu Panagiota Kafourou Martina Rimmele Charlotte L.Rapley Bowen Ding Department of Chemistry and Centre for Processable Electronics Imperial College LondonLondonUK

The power conversion efficiencies(PCEs)of single-junction organic solar cells(OSCs)have surpassed 19%,owing to the emerging Y-series nonfullerene acceptors(NFAs).Undoubtedly,the power and flexibility of chemical design has been a strong driver for this rapid efficiency improvement in the OSC field.Over the course of the past 3 years,a variety of modifications have been made to the structure of the Y6 acceptor,and a large number of Y-series NFAs have been reported to further improve performance.Herein,we present our insights into the rationale behind the Y6 acceptor and discuss the design principles toward high-performance Y-series NFAs.It is clear that structural modifications through choice of heteroatom,soluble chains,πspacers,central cores,and end groups alter the material characteristics and properties,contributing to distinctive photovoltaic performance.Subsequently,we analyze various design strategies of Y-series-containing materials,including polymerized small-molecule acceptors(PSMA),non-fused-ring acceptors(NFRA),and all-fused-ring acceptors(AFRA).This review is expected to be of value in providing effective molecular design strategies for high-performance NFAs in future innovations.

关键词： molecular engineering narrow bandgap nonfullerene organic solar cell Y-series acceptor

molecular engineering of antibodies for site-specific conjugation to lipid polydopamine hybrid nanoparticles

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Acta Pharmaceutica Sinica B 2020年第11期10卷 2212-2226页

作者： Hobin Yang Quoc-Viet Le Gayong Shim Yu-Kyoung Oh Young Kee Shin Laboratory of molecular Pathology and Cancer Genomics College of Pharmacy and Research Institute of Pharmaceutical SciencesSeoul National UniversitySeoul 08826Republic of Korea College of Pharmacy and Research Institute of Pharmaceutical Sciences Seoul National UniversitySeoul 08826Republic of Korea Bio-MAX Seoul National UniversitySeoul 08826Republic of Korea

Conjugation of antibodies to nanoparticles allows specific cancer targeting,but conventional conjugation methods generate heterogeneous conjugations that cannot guarantee the optimal orientation and functionality of the conjugated antibody.Here,a molecular engineering technique was used for sitespecific conjugation of antibodies to nanoparticles.We designed an anti-claudin 3(CLDN3)antibody containing a single cysteine residue,h4 G3 cys,then linked it to the maleimide group of lipid polydopamine hybrid nanoparticles(LPNs).Because of their negatively charged lipid coating,LPNs showed high colloidal stability and provided a functional surface for site-specific conjugation of h4 G3 cys.The activity of h4 G3 cys was tested by measuring the binding of h4 G3 cys-conjugated LPNs(C-LPNs)to CLDN3-positive tumor cells and assessing its subsequent photothermal effects.C-LPNsspecifically recognized CLDN3-overexpressing T47 D breast cancer cells but not CLDN3-negative Hs578 T breast cancer cells.High binding of C-LPNs to CLDN3-overexpressing T47 D cells resulted in significantly higher temperature generation upon NIR irradiation and potent anticancer photothermal efficacy.Consistent with this,intravenous injection of C-LPNsin a T47 D xenograft mouse model followed by NIR irradiation caused remarkable tumor ablation compared with other treatments through high temperature increases.Our results establish an accurate antibody-linking method and demonstrate the possibility of developing therapeutics using antibody-guided nanoparticles.

关键词： molecular engineering Site-specific conjugation Lipid polydopamine hybrid nanoparticles Claudin 3 Photothermal therapy

CsPbBr_(3) quantum dots photodetectors boosting carrier transport via molecular engineering strategy

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Nano Research 2021年第11期14卷 4038-4045页

作者： Wei Yan Jianhua Shen Yihua Zhu Yiqing Gong Jingrun Zhu Zheng Wen Chunzhong Li Shanghai engineering Research Centre of Hierarchical Nanomaterials Key Laboratory for Ultrafine Materials of Ministry of EducationFrontiers Science Centre for Materiobiology and Dynamic ChemistrySchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou215123China Shanghai engineering Research Centre of Hierarchical Nanomaterials School of Chemical EngineeringEast China University of Science and TechnologyShanghai200237China

Perovskite quantum dots (PQDs) require ligands on their surfaces to passivate defects and prevent aggregation. However, the ligands construct the interface relationship between the PQDs, which may seriously hinder the carrier transport. Hence, we propose a molecular engineering strategy of using 3,4-ethylenedioxythiophene (EDOT) to perfectly solve this problem, benefiting from its high conjugation and passivation ability to CsPbBr_(3) PQDs. Furthermore, EDOT on the surface of PQDs can be in-situ polymerized under the photocurrent of the photodetector, thus interconnecting the PQDs which enhanced the performance of the photodetectors up to 178% of its initial performance. We have thoroughly investigated the electropolymerization process of EDOT and its passivation effect on PQDs. The simple lateral photodetector based on EDOT PQDs exhibits a high responsivity of 11.96 A/W, which is 104 times higher than that of oleic acid caped PQDs. Due to the protection of poly(3,4-ethylenedioxythiophene) (PEDOT), the photodetector prepared from EDOT PQDs exhibited very high stability, retaining 94% of its performance after six months in air. This strategy provides a solution for the application of PQDs in high performances and stable optoelectronic devices.

关键词： perovskite quantum dots molecular engineering photodetector interface 3,4-ethylenedioxythiophene

Hydrophobic 1-octadecanethiol functionalized copper catalyst promotes robust high-current CO_(2) gas-diffusion electrolysis

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Nano Research 2022年第2期15卷 1393-1398页

作者： Liangyao Xue Xuefeng Wu Yuanwei Liu Beibei Xu Xuelu Wang Sheng Dai Pengfei Liu Huagui Yang Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China Physics Department and Shanghai Key Laboratory of Magnetic Resonance School of Physics and Materials ScienceEast China Normal UniversityShanghai 200062China Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool oj Chemistry and Molecular EngineeringEast China University of Science and Technology130 Meilong RoadShanghai 200237China

The electrocatalytic reduction of CO_(2) presents a promising strategy in addressing environmental and energy crisis.Significant progress has been achieved via CO_(2) gas diffusion electrolysis,to react at high selectivity and high rate.However,the gas diffusion layer(GDL)of the gas diffusion electrode(GDE)still suffers from low tolerance and limited active sites.Here,the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE,which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.The resultant GDE exhibits multi-carbon(C_(2+))product selectivity over faradaic efficiency(FE)of 70.0%in the range of 100 to 800 mA·cm^(-2),with the peak FE^(c2+)of 85.2%at 800 mA·cm^(-2).Notably,the strengthened GDE could continuously drive high-current electrolysis for more than 100 h without flooding.This work opens a new way to improve CO_(2) gas diffusion electrolysis via surface molecular engineering.

关键词： CO_(2)reduction reaction gas diffusion electrolysis multi-carbon products molecular engineering hydrophobicity

molecular design of an ultra-strong tissue adhesive hydrogel with tunable multifunctionality

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Bioactive Materials 2023年第11期29卷 214-229页

作者： Yuting Zheng Avijit Baidya Nasim Annabi Department of Chemical and Biomolecular engineering University of Californi1Los AngelesLos AngelesCA90095United States Department of Bioengineering University of Californi1Los AngelesLos AngelesCA90095United States

Designing adhesive hydrogels with optimal properties for the treatment of injured tissues is challenging due to the tradeoff between material stiffness and toughness while maintaining adherence to wet tissue surfaces. In most cases, bioadhesives with improved mechanical strength often lack an appropriate elastic compliance, hindering their application for sealing soft, elastic, and dynamic tissues. Here, we present a novel strategy for engineering tissue adhesives in which molecular building blocks are manipulated to allow for precise control and optimization of the various aforementioned properties without any tradeoffs. To introduce tunable mechanical properties and robust tissue adhesion, the hydrogel network presents different modes of covalent and noncovalent interactions using N-hydroxysuccinimide ester (NHS) conjugated alginate (Alg-NHS), poly (ethylene glycol) diacrylate (PEGDA), tannic acid (TA), and Fe^(3+) ions. Through combining and tuning different molecular interactions and a variety of crosslinking mechanisms, we were able to design an extremely elastic (924%) and tough (4697 kJ/m3) multifunctional hydrogel that could quickly adhere to wet tissue surfaces within 5 s of gentle pressing and deform to support physiological tissue function over time under wet conditions. While Alg-NHS provides covalent bonding with the tissue surfaces, the catechol moieties of TA molecules synergistically adopt a mussel-inspired adhesive mechanism to establish robust adherence to the wet tissue. The strong adhesion of the engineered bioadhesive patch is showcased by its application to rabbit conjunctiva and porcine cornea. Meanwhile, the engineered bioadhesive demonstrated painless detachable characteristics and in vitro biocompatibility. Additionally, due to the molecular interactions between TA and Fe3+, antioxidant and antibacterial properties required to support the wound healing pathways were also highlighted. Overall, by tuning various molecular interactions, we were able to develop a single-hydrogel platform wit

关键词： molecular engineering Tough hydrogel Bioadhesive Multifunctionality

Vacuum residue coking process simulation using molecular-level kinetic model coupled with vapor-liquid phase separation

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Chinese Journal of Chemical engineering 2022年第1期35卷 301-310页

作者： Zhengyu Chen Xinhui Yao Dong Guan Suoqi Zhao Linzhou Zhang Chunming Xu State Key Laboratory of Heavy Oil Processing Petroleum Molecular Engineering Center(PMEC)China University of PetroleumBeijing 102249China

In this work,a molecular-level kinetic model was built to simulate the vacuum residue(VR)coking process in a semi-batch laboratory-scale reaction kettle.A series of reaction rules for heavy oil coking were summarized and formulated based on the free radical reaction mechanism.Then,a large-scale molecularlevel reaction network was automatically generated by applying the reaction rules on the vacuum residue molecules.In order to accurately describe the physical change of each molecule in the reactor,we coupled the molecular-level kinetic model with a vapor–liquid phase separation model.The vapor–liquid phase separation model adopted the Peng-Robinson equation of state to calculate vapor–liquid equilibrium.A separation efficiency coefficient was introduced to represent the mass transfer during the phase separation.We used six sets of experimental data under various reaction conditions to regress the model parameters.The tuned model showed that there was an excellent agreement between the calculated values and experimental data.Moreover,we investigated the effect of reaction temperature and reaction time on the product yields.After a comprehensive evaluation of the reaction temperature and reaction time,the optimal reaction condition for the vacuum residue coking was also obtained.

关键词： Kinetic modeling molecular engineering Vapor-liquid equilibrium Vacuum residue coking

Spectral and biodistributional engineering of deep near-infrared chromophore

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中国化学快报:英文版 2023年第9期34卷 176-182页

作者： Yan Dong Xicun Lu Yi Li Weichao Chen Lei Yin Jie Zhao Xinru Hu Xinran Li Zuhai Lei Yuyang Wu Hao Chen Xiao Luo Xuhong Qian Youjun Yang State Key Laboratory of Bioreactor engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China Shanghai engineering Research Center of molecular Therapeutics and New Drug Development School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200241China molecular Imaging Center Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China

Fluorescence-guided surgery calls for development of near-infrared fluorophores.Despite the wide-spread application and a safe clinical record of Indocyanine Green(ICG),its maximal absorption wavelength at780 nm is rather short and longer-wavelength dyes are desired to exploit such benefits as low phototoxicity and deep penetration depth.Here,we report ECY,a stable deep near-infrared(NIR)fluorochromic scaffold absorbing/emitting at 836/871 nm with a fluorescence quantum yield of 16%in CH_(2)Cl_(2).ECY was further rationally engineered for biological distribution specificity.Analogous bearing different numbers of sulfonate group or a polyethylene glycol chain were synthesized.By screening this focused library upon intravenous injection to BALB/c mice,ECYS2 was identified to be a suitable candidate for bioimaging of organs involved in hepatobiliary excretion,and ECYPEG was found to be a superior candidate for vasculature imaging.They have potentials in intraoperative imaging.

关键词： Near infrared fluorophore In vivo imaging molecular engineering Biological distribution Angiography

engineering Mechanical Strong Biomaterials Inspired by Structural Building Blocks in Nature

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Chemical Research in Chinese Universities 2023年第1期39卷 92-106页

作者： LI Jiahe MA Chao ZHANG Hongjie LIU Kai engineering Research Center of Advanced Rare Earth Materials Ministry of EducationDepartment of ChemistryTsinghua UniversityBeijing100084P.R.China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022P.R.China

The intricate multiscale architectures in natural structural building blocks provide many sources of inspiration for the designs of artificial biomaterials.In nature,the assembly of highly ordered molecular crystals and amorphous aggregates often derives from inter-and intra-molecular interactions of biomacromolecules,e.g.,proteinaceous materials.The structural biomaterials derived from the protein self-assembly behave with remarkable mechanical performance.However,there is still a grand challenge to mimic the mechanical properties of natural protein-based biomaterials in a rational design fashion to yield comparable man-made synthetic ensembles.In this review,a brief perspective on current challenges and advances in terms of bioinspired structural materials is presented.We outline a framework for mimicking protein self-assembly of natural building blocks across multiscale and highlight the critical role of synthetic biology and chemical modifications in material biosynthesis.Particularly,we focus on the design and promising applications of protein-based fibers,adhesives,dynamic hydrogels and engineered living materials,in which natural mechanical functions are effectively reproduced.

关键词： Bioinspired material Protein self-assembly Mechanical property Synthetic biology molecular engineering

Theory-Driven Design of Electrocatalysts for the Two-Electron Oxygen Reduction Reaction Based on Dispersed Metal Phthalocyanines

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CCS Chemistry 2022年第1期4卷 228-236页

作者： Yang Wang Zisheng Zhang Xiao Zhang Yubo Yuan Zhan Jiang Hongzhi Zheng Yang-Gang Wang Hua Zhou Yongye Liang Department of Materials Science and engineering Southern University of Science and TechnologyShenzhen 518055 Department of Chemistry Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055 State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027 X-Ray Science Division Advanced Photon SourceArgonne National LaboratoryLemontIL 60439 Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices Southern University of Science and TechnologyShenzhen 518055

The two-electron electrochemical reduction of oxygen is an appealing approach to produce hydrogen peroxide.Metal and heteroatom-doped carbon(M–X/C)materials have recently been recognized as compelling catalysts for this process,but their performance improvement is generally hindered by the ill-defined structures of active sites.Herein,we demonstrate a theory-driven design of catalysts for oxygen reduction reactions based on molecularly dispersed electrocatalysts(MDEs)with metal phthalocyanines on carbon nanotubes.Density functional theory calculations suggest that nickel phthalocyanine(NiPc)favors the formation of*H_(2)O_(2) over*O,thus acting as a selective catalyst for peroxide production.NiPc MDE shows high peroxide yields of∼83%,superior to the aggregated NiPc and pyrolyzed Ni–N/C catalysts.The performance is further enhanced by the introduction of the cyano group(CN).NiPc–CN MDE exhibits∼92%peroxide yields and good stability.Our studies provide a new perspective for the development of heterogeneous electrocatalysts for hydrogen peroxide production from metal macrocyclic complexes.

关键词： metal phthalocyanine oxygen reduction reaction peroxide theory-driven design molecular engineering