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Donor-acceptor covalent organic frameworks-confined ultrafine bimetallic Pt-based nanoclusters for enhanced photocatalytic H_(2)generation

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Nano Research 2024年第7期17卷 5835-5844页

作者： Yu Liu Yawen Shi Hua Wang Shengbo Zhang Collaborative innovation center of chemical science and Engineering(Tianjin) Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China School of Environmental science and Engineering Tianjin Key Laboratory of Biomass/Wastes UtilizationTianjin UniversityTianjin 300350China

Photocatalytic hydrogen generation from hydrogen storage media is an effective and promising approach for the green hydrogen industry as well as for achieving carbon neutrality ***,the lower photocatalytic efficiency due to the limited light trapping capacity,low electron transfer rate,and severe aggregation of nanoparticles caused by high surface energy seriously restricts their practical ***,we constructed a series of donor–acceptor(D–A)type covalent organic frameworks to confine ultrafine bimetallic Pt-based nanoclusters for photocatalytic hydrogen generation from ammonia borane(AB)*** visible light irradiation at 20℃,PtCo_(2)@covalent organic framework(COF)showed the highest photocatalytic activity with a turnover frequency(TOF)of 486 min−*** and density functional theory(DFT)calculations reveal that the high catalytic activity is mainly attributed to the strong electronic interactions between D–A type COF and ultrafine PtCo_(2)***,the D–A type COF can significantly enhance the light-trapping ability by fine-tuning the electron-acceptor type in the framework,and accelerate the photogenerated electron transfer from D–A type COF to PtCo_(2)nanocluster,which promotes the adsorption and activation of H_(2)O and AB molecules and accelerates hydrogen ***,PtCo_(2)@COF also exhibited ultra-high durability due to the significantly enhanced resistance to nanocluster aggregation caused by the nanopore confinement effect of D–A type *** believe that this work will provide a theoretical guide for the rational design of efficient D–A COFbased catalysts for photocatalysis.

关键词： light trapping electron transfer donor-acceptor covalent organic frameworks(D-A COFs) bimetallic nanoclusters photocatalysis

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Flexible Organic Crystal with Two-Dimensional Elastic Bending and Recoverable Plastic Twisting for Circularly Polarized Luminescence

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CCS Chemistry 2024年第6期6卷 1439-1447页

作者： Wenjie Kuang Bo Jing Songgu Wu Junbo Gong State Key Laboratory of chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072 Collaborative innovation center of chemical science and Engineering Tianjin 300072

Multidimensional mechanical flexible organic crystals with tunable optoelectronic properties hold significant promise for practical application in complicated environmental ***,based on a newly designed“flexible”Schiff base small molecule with chirality,we presented a compatibly bendable and twistable organic single crystal with circularly polarized luminescence for the first ***,the twodimensional elastic bending of the chiral crystal was realized at both room and liquid nitrogen temperatures,along with recoverable plastic twisting at room ***,circular dichroism and circularly polarized luminescence spectroscopy were employed to characterize the chiral enantiomer in solution and the solid *** design strategy provides a new perspective for the future construction of chiroptical flexible crystal materials.

关键词： organic crystal multidimensional flexibility circularly polarized luminescence low-temperature resistance

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Sequence-Controlled Synthesis of Alternating Poly(ester amide)s using Water as Control Agent in One-Pot

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Chinese Journal of Polymer science 2024年第8期42卷 1015-1020页

作者： Tao Liu Fang-Fang Niu Kan Cheng Yu-Min Xia Bo-Mou Ma Xue-Li Wang Jian-Yong Yu Yong He State Key Laboratory for Modification of chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China innovation center for Textile science and Technology Donghua UniversityShanghai 201620China

Poly(ester amide)s(PEAs)attract much attention as a new kind of biodegradable ***,the synthesis of PEAs with sequence-regulated chain structures is still complicated due to the multistep polymerization,high monomer purity,as well as the usage of organic solvents,which greatly inhibits its development and ***,a one-pot strategy without solvent was developed to synthesize the alternating PEA fromα,ω-amino alcohol and dicarboxylic acid by sequential polycondensation,where water was used as the controlling agent for amidation and ***,the amidation and esterification were controlled to proceed in turn by adding or removing water,realizing the one-pot preparation of alternating *** resultant PEA is characterized by^1H-and^(13)C-NMR,and its chain structure is confirmed to be highly quasi-alternating similar to alternating PEAs prepared by classical methods The evaluations from DSC and DMA demonstrate that the properties of quasi-alternating PEA(T_(m)=102℃,ΔH_(m)=30J·g^(-1))are far superior to those of random PEA(T_(m)=72℃,ΔH_(m)<1 J·g^(-1)).

关键词： Biodegradable macromolecules Polymer architectures Sequence-controlled synthesis One-pot polymerization

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Defect engineering in transition-metal(Fe,Co,andNi)-based electrocatalysts for water splitting

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Carbon Energy 2024年第6期6卷 165-199页

作者： Kaili Wu Chaojie Lyu Jiarun Cheng Weifan Ding Jiwen Wu Qian Wang Woon-Ming Lau Jinlong Zheng Beijing Advanced innovation center for Materials Genome Engineering University of Science and Technology BeijingBeijingChina School of Chemistry and chemical Engineering Linyi UniversityLinyiChina Institute for Advanced Materials and Technology University of Science and Technology BeijingBeijingChina Shunde innovation School University of Science and Technology BeijingFoshanChina

Electrocatalytic water splitting seems to be an efficient strategy to deal with increasingly serious environmental problems and energy crises but still suffers from the lack of stable and efficient *** practical electrocatalysts by introducing defect engineering,such as hybrid structure,surface vacancies,functional modification,and structural distortions,is proven to be a dependable solution for fabricating electrocatalysts with high catalytic activities,robust stability,and good *** review is an overview of some relevant reports about the effects of defect engineering on the electrocatalytic water splitting performance of *** detail,the types of defects,the preparation and characterization methods,and catalytic performances of electrocatalysts are presented,emphasizing the effects of the introduced defects on the electronic structures of electrocatalysts and the optimization of the intermediates'adsorption energy throughout the ***,the existing challenges and personal perspectives of possible strategies for enhancing the catalytic performances of electrocatalysts are *** in-depth understanding of the effects of defect engineering on the catalytic performance of electrocatalysts will light the way to design high-efficiency electrocatalysts for water splitting and other possible applications.

关键词： defect engineering electrocatalytic water splitting element doping interfacial engineering vacancy

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Engineering Shewanella-re duce d graphene oxide aerogel biohybrid to efficiently synthesize Au nanoparticles

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Journal of Materials science & Technology 2024年第1期168卷 50-61页

作者： Baocai Zhang Shulin Shao Huan Yu Qijing Liu Sicheng Shi Qingyuan Wu Zijie Wu Yiyu Feng Yifei Wang Xi Sun Deguang Wu Feng Li Hao Song Frontier science center for Synthetic Biology and Key Laboratory of Systems Bioengineering(Ministry of Education) Tianjin UniversityTianjin 300072China Collaborative innovation center of chemical science and Engineering(Tianjin) School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Beijing Advanced innovation center for Soft Matter science and Engineering Beijing University of Chemical TechnologyBeijing 100029China School of Materials science and Engineering Tianjin UniversityTianjin 300350China College of Biological Engineering Tianjin Agricultural UniversityTianjin 300384China Department of Brewing Engineering Moutai InstituteLuban AveRenhuai 564507China

Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for ***,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ***,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of *** regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)*** eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs *** work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.

关键词： Au nanoparticles Exoelectrogenic cell(e-Cell) Shewanella Synthesis biology Extracellular electron transfer Reduced graphene oxide aerogel

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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 ***,the development of FL/PA dual-modality imaging probes is beneficial for achieving precision cancer diagnosis and ***,we designed an efficient phototherapy agent methoxy bithiophene indene(OTIC),which was based on aggregation-induced emission(AIE)active *** improve the water dispersion and enrichment of OTIC at the tumor site,OTIC nanoparticles(OTIC NPs)were prepared by a nanoprecipitation *** balance between radiation and non-radiation energy dissipation was regulated by the strong donor-acceptor interaction and intramolecular *** OTIC NPs exhibited bright NIR fluorescence,photoacoustic signals,efficient generation of reactive oxygen species,and high photothermal conversion efficiency under NIR *** imaging of the tumor and mice sentinel lymph nodes(SLNs)with OTIC NPs was visualized by NIR FL/PA dual-modal *** the comprehensive imaging information provided by OTIC NPs in vivo,tumors were ablated under laser irradiation,which greatly improved the therapeutic *** 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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A solubility limited pyrene-4,5,9,10-tetraone-based covalent organic framework for high-performance aqueous zinc-organic batteries

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Nano Research 2024年第6期17卷 5095-5103页

作者： Min Cheng Shibing Zheng Tianjiang Sun Diantao Li Weijia Zhang Zhengtai Zha Qiong Sun Jing Tian Kai Zhang Zhanliang Tao Frontiers science center for New Organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Renewable Energy Conversion and Storage CentreNankai UniversityTianjin 300071China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China

Pyrene-4,5,9,10-tetraone(PTO),with a high theoretical capacity of 408 mAh·g^(−1),is a promising candidate for rechargeable aqueous zinc-ion batteries(RAZIBs),but its zincated products during discharge process suffer from high solubility in ***,aβ-ketoenamine-linked two-dimensional(2D)covalent organic framework(COF)based on a 2,7-diaminopyrene-4,5,9,10-tetraone(4KT-BD)monomer and a 2,4,6-trihydroxy-benzene-1,3,5-tricarbaldehyde(Tp)node(4KT-Tp-COF)is synthesized to address the above *** well-designed 4KT-Tp-COF displays low solubility in 3 M Zn(CF3SO3)2 owing to the favorableπ-πstacking as well as extended ***,the ingenious structural design of the active molecule and the long-range ordered nano-channels alter the intramolecular electron distribution,which facilitates the ionic ***,the 4KT-Tp-COF cathode exhibits a stable capacity of 181 mAh·g^(−1)at 0.2 A·g^(−1),superior rate capability of 139 mAh·g^(−1)at 20 A·g^(−1),and a long lifetime of 1000 cycles without capacity loss at 30 A·g^(−1).Even at a low temperature of−20°C,the electrode also performs an ultralong cycling life of 9000 cycles with a capacity of 106 mAh·g^(−1)at 5 A·g^(−1).The comprehensive characterizations of ex-situ analyses together with the theoretical calculations validate that the groups of C=O can contribute highly accessible redox-active sites for Zn^(2+)*** ultra-stable 4KT-Tp-COF cathode provides important insights for designing robust organic electrodes for sustainable and large-scale electrochemical energy storage.

关键词： pyrene-4,5,9,10-tetraone solubility limited covalent organic framework zinc batteries

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Azocalixarenes: a scaffold of universal excipients with high efficiency

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science China Chemistry 2024年第5期67卷 1697-1706页

作者： Yu-Xin Yue Yi-Lin Lin Meng-Meng Chen Han-Wen Tian Rong Ma Ze-Han Wang Fang-Yuan Chen Yu-Chen Pan Dong-Sheng Guo College of Chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Functional Polymer Materials(Ministry of Education)Frontiers Science Center for New Organic MatterCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin 300071China

Excipients are important components of pharmaceutical preparations that affect their quality, safety, and efficacy. Macrocyclic receptors are a family of supramolecular excipients with several advantages, including molecular-level protection, small sizes,fast kinetics of host-guest recognition, and modular construction. With the continuous advances in the medical field, personalized and precision medicine requires the development of excipients with low dosages, integrated modifying effects, universality,and controlled release. To meet these requirements, we have developed a new family of macrocyclic excipients based on calixarenes by integrating their covalent(broad chemical design space) and noncovalent(wide range of substrates) ***, azocalixarenes(Azo CAs) were designed, showing high binding affinities to a broad spectrum of active pharmaceutical ingredients(APIs), selectivity to interferents, and responsiveness to hypoxic microenvironments. Due to their highly efficient and controllable recognition, Azo CAs serve as low-dose excipients for 30 APIs. Molecular encapsulation by Azo CAs results in the integrated modification of the physicochemical properties of APIs, including solubility, stability, bioavailability,and biocompatibility. Moreover, Azo CAs can be reduced by azoreductases overexpressed in hypoxic microenvironments,leading to the controlled release of APIs. Collectively, Azo CA excipients have broad application prospects for a series of diseases such as enteritis, arthritis, stroke, cancer, bacterial infection and kidney injury, with diverse therapeutic modalities,including chemotherapy, photodynamic therapy, photothermal therapy, immunotherapy, boron neutron capture therapy, radiotherapy, fluorescence imaging, and their combinations.

关键词： supramolecular chemistry host-guest systems excipient calixarene molecular recognition

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A review on vanadium extraction techniques from major vanadium-containing resources

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Rare Metals 2024年第9期43卷 4115-4131页

作者： Yin-Hui Wang Yi-Fan Wang Yu-Ting Li Chang Wu Xiu-Li Han Ning-Ning Zhao Ze-Kun Zhang Lei Dai Ling Wang Zhang-Xing He College of Mining Engineering North China University of Science and Technology Collaborative innovation center of Green Development and Ecological Restoration of Mineral Resources College of chemical Engineering North China University of Science and Technology

The critical role of vanadium in metallurgy and the increasing commercialization of vanadium redox flow batteries have contributed to a rise in market demand for vanadium, emphasizing the need to ensure the sustainability of vanadium production. Converter vanadium slag and stone coal, generated during the smelting process of vanadium–titanium magnetite, serve as primary raw materials for vanadium extraction. This paper reviews the process mineralogy of converter vanadium slag and stone coal, encompassing the chemical and physical phase compositions of the raw materials and the state of vanadium occurrence. The aim is to establish a theoretical foundation for the mechanistic study of the vanadium extraction techniques and to provide a reference for the optimization of the process afterward. This paper systematically summarizes the current vanadium extraction technology from converter vanadium slag, covering roasting,direct leaching, sub-molten salt method, and the technology and research status of vanadium extraction from stone coal. Most importantly, it identifies key issues in the current vanadium extraction techniques and challenges faced in actual production, based on the analysis of the current vanadium extraction process and mechanism research. The forward feasibility and prospects for the development of vanadium extraction technology are outlined.

关键词： Vanadium

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Non-flammable long chain phosphate ester based electrolyte via competitive solventized structures for high-performance lithium metal batteries

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Journal of Energy Chemistry 2024年第10期97卷 156-165页

作者： Li Liao Zhiqiang Han Xuanjie Feng Pan Luo Jialin Song Yin Shen Xiaoshuang Luo Xinpeng Li Xuanzhong Wen Bo Yu Junchen Chen Bingshu Guo Mingshan Wang Yun Huang Hongmei Zhang Mengmeng Yin Jiangtao Liu Yuanhua Lin Xing Li School of New Energy and Materials Southwest Petroleum University Beijing Advanced innovation center for Materials Genome Engineering Center for Green Innovation School of Mathematics and Physics University of Science and Technology Beijing State Key Laboratory of Advanced chemical Power Sources Guizhou Meiling Power Sources Co.Ltd

Safety remains a persistent challenge for high-energy-density lithium metal batteries（LMBs）.The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high ***,a flame-retardant,low-cost and thermally stable long chain phosphate ester based（tributyl phosphate,TBP） electrolyte is reported,which can effectively enhance the cycling stability of highly loaded high-nickel LMBs with high safety through co-solvation *** interfacial compatibility between TBP and electrode is effectively improved using a short-chain ether（glycol dimethyl ether,DME）,and a specially competitive solvation structure is further constructed using lithium borate difluorooxalate（LiDFOB） to form the stable and inorganic-rich electrode *** from the presence of the cathode electrolyte interphase（CEI） and solid electrolyte interphase（SEI） enriched with LiF and LixPOyFz,the electrolyte demonstrates excellent cycling stability assembled using a 50 μm lithium foil anode in combination with a high loading NMC811(15.4 mg cm-2) cathode,with 88% capacity retention after 120 ***,the electrolyte exhibits excellent high-temperature characteristics when used in a 1-Ah pouch cell（N/P=0.26）,and higher thermal runaway temperature（238℃） in the ARC（accelerating rate calorimeter） demonstrating high *** novel electrolyte adopts long-chain phosphate as the main solvent for the first time,and would provide a new idea for the development of extremely high safety and high-temperature electrolytes.

关键词： Battery safety Lithium metal batteries Long chain phosphate ester Non-flammable electrolyte Solvation structure

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