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Impact of Polymer Matrix on Polymer Mechanochromism from Excited state Intramolecular Proton Transfer

Chinese Journal of Chemistry 2024年第6期42卷 611-616页

作者： Yu Wu Xin Cheng Huan Hu Shui Hu Zhimin Ma Zhiyong Ma beijing advanced innovation center for soft matter science and engineering Beijing State Key Laboratory of Organic-Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing100029 China center of advanced Elastomer Materials College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing100029 China College of engineering Peking UniversityBeijing100871 China

Mechanochromic polymers based on non-covalent changes have attracted much attention recently.Herein,we report the impact of inter/intramolecular hydrogen bonds on polymer mechanochromism from the excited state intramolecular proton transfer (ESIPT) process.PhMz-NH2-OH and PhMz=2A are designed and obtained by simple and high-yield synthesis,and are connected into polyurethane and poly(methyl acrylate-co-2-ethylhexyl acrylate),respectively.In the initial state,the PhMz-NH2-OH@PU sample shows blue fluorescence from the excited enol form (E*) excitons,owing to intermolecular hydrogen bonds that interrupt the ESIPT reactions but the PhMz=2A@PMA-2-EA sample expresses cyan fluorescence belonging to the excited keto form (K*) emission,implying that the intramolecular hydrogen bonds matter.Furthermore,under stretching,external force can tune the emission of the PhMz=2A@PMA-2-EA sample from K* to E* state.Though external force can putatively still promote a bond rotation,ESIPT reactions remain equivalently interrupted in both the relaxed and stressed states in a hydrogen-bond donating environment.DFT calculation confirms the force-induced increase in dihedral angle for the transition of ESIPT-on/off.Thus,PhMz-NH2-OH@PU and PhMz=2A@PMA-2-EA showed disparate initial ESIPT states and further different responses/sensitivity to force.This study reports a novel and efficient strategy for enriching mechanochromic investigation and extending the applications of ESIPT reactions.

关键词： Polymer mechanochromism Excited state intramolecular proton transfer Hydrogen bonding Supramolecular chemistry Elastomers

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Electrochemical converting ethanol to hydrogen and acetic acid for large scale green hydrogen production

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Nano Research 2024年第3期17卷 1542-1551页

作者： Yufeng Zhang Wei Zhu Jinjie Fang Zhiyuan Xu Yanrong Xue Jiajing Pei Rui Sui Xingdong Wang Xuejiang Zhang Zhongbin Zhuang state key Lab of organic-inorganic composites and beijing advanced innovation center for soft matter science and engineering Beijing University of Chemical TechnologyBeijing 100029China laboratory of advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171China beijing key laboratory of Energy Environmental Catalysis Beijing University of Chemical TechnologyBeijing 100029China

Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.

关键词： selective ethanol electrooxidation gold alloy catalyst electrochemical-coupled hydrogen production market assessment interfacial water activation

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Matrix-Mediated Color-Tunable Ultralong organic Room Temperature Phosphorescence of 7H-Benzo[c]carbazole Derivatives

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CCS Chemistry 2024年第3期6卷 798-811页

作者： Chen Qian Xue Zhang Zhimin Ma Xiaohua Fu Zewei Li Huiwen Jin Mingxing Chen Hong Jiang Zhiyong Ma beijing advanced innovation center for soft matter science and engineering State Key Laboratory of Organic–Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029 beijing National laboratory for Molecular sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Building on the recent systematic research on 1Hbenzo[f]indole(Bd),an important advancement in constructing ultralong organic room temperature(UORTP)materials with a universal strategy via a readily obtained unit(7H-Benzo[c]carbazole,BCz)is proposed in this work.Pure powders of BCz and its derivatives merely exhibit blue fluorescence at ambient condition.However,when BCz and its derivatives are dispersed into polymer or powder matrixes,strong photo-activated green UORTP can be observed from their doped systems at room temperature.Moreover,the UORTP color can be tuned between green and yellow depending on the matrix.The ultralong phosphorescence originates from the generation of charge-separated states via radicals.The matrixes play a key role in both stabilizing charge-separated states and controlling UORTP color.More interestingly,when using polymethyl methacrylate as matrix,the doped films achieve stronger photo-activated ultralong phosphorescence underwater than in air at room temperature.Comparedwith Bd,BCz achieves better performance not only in ultralong phosphorescence properties but also in practical applications.This work gains a deeper insight into the mechanism of UORTP and paves a new approach to applying organic phosphorescent materials to underwater coating and imaging.

关键词： 7H-Benzo[c]carbazole ultralong organic room temperature phosphorescence ion radical matrix-mediated color tunning underwater application

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Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano Research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song state key laboratory of Chemical Resource engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)process.We herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) themselves.The surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) conversion.For example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V vs.RHE,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl chains.By virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and aerophilic.In this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed HER.This work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

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Interface catalytic reduction of alumina by nickle for the aluminum nanowire growth: Dynamics observed by in situ TEM

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Nano Research 2024年第3期17卷 1225-1231页

作者： Zichun Wang Dan Wang Ang Li Lizhuo Wang Xiaodong Han Yijiao Jiang Jianfeng Chen Jun Huang beijing advanced innovation center for soft matter science and engineering State Key Laboratory of Organic–Inorganic CompositesBeijing University of Chemical TechnologyBeijing 100029China laboratory for Catalysis engineering School of Chemical and Biomolecular EngineeringThe University of SydneyNew South Wales 2006Australia beijing key laboratory of Microstructure and Property of advanced Materials Beijing University of TechnologyBeijing 100024China Department of engineering Macquarie UniversitySydneyNew South Wales 2109Australia

Metal nanowires show promise in a broad range of applications and can be fabricated via a number of methods,such as vapor–liquid–solid process and template-based electrodeposition.However,the synthesis of Al nanowires(NWs)is still challenging from the stable alumina substrate.In this work,the Ni-catalyzed fabrication of Al NWs has been realized using various Al_(2)O_(3) substrates.The growth dynamics of Al NWs on Ni/Al_(2)O_(3) was studied using in situ transmission electron microscopy(TEM).The effect of alumina structures,compositions,and growth temperature were investigated.The growth of Al NWs correlates with the Na addition to the alumina support.Since no eutectic mixture of nickel aluminide was formed,a mechanism of Ni-catalyzed reduction of Al_(2)O_(3) for Al NWs growth has been proposed instead of the vapor–liquid–solid mechanism.The key insights reported here are not restricted to Ni-catalyzed Al NWs growth but can be extended to understanding the dynamic change and catalytic performance of Ni/Al_(2)O_(3) under working conditions.

关键词： in situ transmission electron microscopy(TEM) Al nanowires alumina reduction nanowire growth

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Central aromatic-core fluorination in non-fullerene acceptor advances binary organic solar cells to a record efficiency of 19.7%

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science China Materials 2024年

作者： Ming Zhang Zhi-Guo Zhang state key laboratory of organic/inorganic composites Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology

organic solar cells(OSCs) hold great promise for the conversion of solar energy into electricity, showing advantages such as lightweight, flexibility, semi-transparency, and solution processability. The field has witnessed significant advancements,notably with the transition from fullerene acceptors to nonfullerene acceptors(NFAs).

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Near-infrared double-cable conjugated polymers based on alkyl linkers with tunable length for single-component organic solar cells

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Chinese Chemical Letters 2024年第4期35卷 452-456页

作者： Yikun Wang Qiaomei Chen Shijie Liang Dongdong Xia Chaowei Zhao Christopher R.McNeill Weiwei Li beijing advanced innovation center for soft matter science and engineering&state key laboratory of organic-inorganic composites Beijing University of Chemical TechnologyBeijing 100029China Institute of Applied Chemistry Jiangxi Academy of SciencesNanchang 330096China Department of Materials science and engineering Monash UniversityWellington RoadClaytonVictoria 3800Australia

The photovoltaic properties of double-cable conjugated polymers are significantly influenced by the length of the alkyl linkers that connect donor backbones and acceptor side units. In this study, a series of 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile(IC)-based double-cable polymers with alkyl linkers ranging from C_8H_(16)to C_(16)H_(32)(Px, x = 8, 10, 12, 14, 16) were synthesized for single-component organic solar cells(SCOSCs). Among these, the linker length x = 12(P12) is found to optimize the power conversion efficiencies(PCEs) in SCOSCs. Specifically, PCEs increase from P8 to P12 and then decline from P12to P16. Detailed investigations of optical absorption, charge transport, and morphology provide insights into the underlying factors contributing to these PCE variations. The findings indicate that the exceptional photovoltaic properties observed in P12 can be attributed to three key factors: A delicate balance between enhanced charge separation facilitated by the increased spacer length and reduced crystallinity resulting from longer spacers, higher charge mobilities, and well-balanced hole/electron transport characteristics. This study highlights the critical role of linker length in determining the photovoltaic properties of double-cable conjugated polymer-based SCOSCs and offers valuable guidance for the design of novel double-cable conjugated polymers.

关键词： Single-component organic solar cells Double-cable conjugated polymers Photovoltaic properties Alkyl linkers

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Aggregation-induced Emission Probe for Fluorescence/Photoacoustic Dual-modality Imaging and Photodynamic/Photothermal Treatment

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Chemical Research in Chinese Universities 2024年第2期40卷 293-304页

作者： CHEN Peiyu ZHANG Guoyang LI Jiguang MA Lijun ZHOU Jiaying ZHU Mingguang LI Shuo WANG Zhuo state key laboratory of Chemical Resource engineering College of ChemistryBeijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing100029P.R.China

The combination of near-infrared(NIR)fluorescence imaging(FLI)and photoacoustic imaging(PAI)can effectively compensate for each other’s inherent limitations,which can provide reliable and rich information on tumor biology.Therefore,the development of FL/PA dual-modality imaging probes is beneficial for achieving precision cancer diagnosis and treatment.Herein,we designed an efficient phototherapy agent methoxy bithiophene indene(OTIC),which was based on aggregation-induced emission(AIE)active fluorophores.To improve the water dispersion and enrichment of OTIC at the tumor site,OTIC nanoparticles(OTIC NPs)were prepared by a nanoprecipitation method.The balance between radiation and non-radiation energy dissipation was regulated by the strong donor-acceptor interaction and intramolecular motion.So OTIC NPs exhibited bright NIR fluorescence,photoacoustic signals,efficient generation of reactive oxygen species,and high photothermal conversion efficiency under NIR irradiation.Accurate imaging of the tumor and mice sentinel lymph nodes(SLNs)with OTIC NPs was visualized by NIR FL/PA dual-modal imaging.With the comprehensive imaging information provided by OTIC NPs in vivo,tumors were ablated under laser irradiation,which greatly improved the therapeutic efficacy.OTIC NPs would be possible to realize the precise guidance of FL/PA imaging for tumor treatment in the future clinical application.

关键词： Aggregation-induced emission Dual-modality imaging Photodynamic/photothermal treatment

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Hydrothermal synthesis of polyimide-linked covalent organic frameworks towards ultrafast and stable cathodic sodium storage

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science China Chemistry 2024年第4期67卷 1300-1310页

作者： Xiya Yang Lei Gong Zhixin Liu Qianjun Zhi Baoqiu Yu Xin Chen Kang Wang Xiaofeng Li Dongdong Qi Jianzhuang Jiang beijing advanced innovation center for Materials Genome engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China state key laboratory of organic-inorganic composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Redox-active organic materials are capturing growing attention as cathode materials for sustainable alkaline metal ion batteries.However,the storage of Na+in most organic materials-based cathodes is plagued by low capacity and unsatisfying rate performance due to their low active site densities and limited exposed active sites.Herein,two polyimide-linked covalent organic frameworks(COFs),namely HATN-PD-COF and HATN-TAB-COF,were fabricated from hydrothermal synthesis with redoxactive triphenylene-2,3,6,7,10,11-hexacarboxylic acid and aromatic amines as starting materials.Powder X-ray diffraction and electron microscopy analysis indicate the high crystalline nature of these COFs with AA stacking configuration and orderly mesoporous tunnel.N_(2) sorption measurement discloses the permanent porosity of these two COFs with a Brunauer-EmmettTeller surface area of 1,065-1,200 m^(2)g^(-1)and a large pore size of 2.0-3.1 nm.Galvanostatic intermittent titration technique and density functional theory calculations reveal the facile Na+ion diffusion along the mesoporous tunnel of these COFs with a small energy barrier of 0.13-0.40 e V.In particular,the as-prepared COFs based-cathodes show ultrafast and stable Na+storage associated with their conjugated electronic structure,highly ordered mesoporous tunnel,robust structure,and redox-active C=N/C=O-rich framework as exemplified by the high reversible capacity of 210 m A h g^(-1)at 200 m A g^(-1),record-high rate performance(195 m A h g^(-1)at a high current density of 10,000 m A g^(-1))among organic electrodes and the capacity retention of nearly 91%at 10,000 m A g^(-1)after 7,000 cycles for HATN-PD-COF.

关键词： covalent organic framework sodium ion battery cathode high rate organic electrode

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

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Nano-Micro Letters 2024年第7期16卷 402-440页

作者： Yizhe Li Yajie Li Hao Sun Liyao Gao Xiangrong Jin Yaping Li Zhi LV Lijun Xu Wen Liu Xiaoming Sun state key laboratory of Chemical Resource engineering Beijing Advanced Innovation Center for Soft Matter Science EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Xinjiang Coal Mine Mechanical and Electrical engineering Technology Research center Xinjiang Institute of EngineeringUrumqi 830023Xinjiang Uygur Autonomous RegionPeople’s Republic of China

The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.

关键词： Dual-atom catalysts Synergetic effect Electrocatalysis Oxygen reduction reaction CO_(2)reduction reaction Hydrogen evolution reaction N2 reduction reaction

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