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Frontiers of chemical Science and engineering 2024年第4期18卷 97-106页

作者： Ying Li Lu Wang Junyan Xie Yong Dai Xuehong Gu Xuerui Wang State Key Laboratory of materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Quzhou Membrane material Innovation Institute Quzhou 324000China

Membrane gas separation is considered an energy-saving technique to extract He from natural gas due to no phase change and room temperature ***,the membrane performance was strongly limited by the trade-off between permeance and ***,novel 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)-2,2′-bis(3-amino-4-hydroxyphenyl)hexafluoropropane(APAF)-5-amino-2-(4-aminobenzene)benzimidazole(BIA)asymmetric membranes with a thickness of 300 nm were successfully prepared by the non-solvent induced phase separation *** membrane performance was modulated by regulating dope solution compositions(e.g.,tetrahydrofuran and polymer concentration).The ideal He/CH_(4) selectivity was 124 and the optimized He permeance reached 87 GPU,beyond the current upper ***/CH_(4) selectivity was 75 and He permeance was 73 GPU for the binary mixture feed containing 0.2 mol%*** membrane showed good resistance to CO_(2) and C_(2)H_(6),which are the typical impurities in natural *** 6FDA-APAF-BIA membranes have good stability(>160 h),which can provide great potential in He extraction from natural gas.

关键词： He separation membrane natural gas copolyimide

Controlled Synthesis of Metal-Nanoparticles Decorated Block Copolymer Hybrid Particles via Emulsion Confined Self-assembly and Their Catalytic Applications

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Chinese Journal of Chemistry 2024年第8期42卷 835-840页

作者： Xiaohua Chang Qunli Yu Dan Ji Yutian Zhu college of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhouZhejiang311121 China

Comprehensive Summary Metal nanoparticles(NPs)decorated block copolymer(BCP)hybrid nanoparticles have attracted enormous attention for their actual value in catalysis,medical therapy,and *** confined assembly of BCPs within evaporative emulsion droplet is verified as an effective method to provide polymeric scaffolds to load metal ***,to date,it remains challenging to generate different types of metal NPs decorated BCP hybrid ***,we employed the emulsion confined self-assembly of poly(styrene-b-2-vinylpyridine)(PS-b-P2VP)and the followed seed-mediated growth of Au and palladium(Pd)NPs onto well-defined BCP particles to design a series of Au/Pd decorated BCP hybrid nanoparticles,which exhibited excellent catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol with the reductant of *** work may inspire more researchers to investigate the selective decoration of different metal NPs onto the polymeric scaffolds,broadening the potential applications of the inorganic/organic hybrid nanoparticles.

关键词： Block copolymers Emulsion confined self-assembly Hybrid nanoparticles Catalytic activity Recyclability

Ultrafast Response and Threshold Adjustable Intelligent Thermoelectric Systems for Next‑Generation Self‑Powered Remote IoT Fire Warning

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Nano-Micro Letters 2024年第11期16卷 413-428页

作者： Zhaofu Ding Gang Li Yejun Wang Chunyu Du Zhenqiang Ye Lirong Liang Long‑Cheng Tang Guangming Chen college of materials Science and engineering&college of Civil and Transportation engineering Shenzhen UniversityShenzhen 518055People’s Republic of China college of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material Technology of MoEHangzhou Normal UniversityHangzhou 311121People’s Republic of China

Fire warning is vital to human life,economy and ***,the development of effective warning systems faces great challenges of fast response,adjustable threshold and remote ***,we propose an intelligent self-powered remote IoT fire warning system,by employing single-walled carbon nanotube/titanium carbide thermoelectric composite *** flexible films,prepared by a convenient solution mixing,display p-type characteristic with excellent high-temperature stability,flame retardancy and TE(power factor of 239.7±15.8μW m^(-1) K^(-2))*** comprehensive morphology and structural analyses shed light on the underlying *** the assembled TE devices(TEDs)exhibit fast fire warning with adjustable warning threshold voltages(1–10 mV).Excitingly,an ultrafast fire warning response time of~0.1 s at 1 mV threshold voltage is achieved,rivaling many state-of-the-art ***,TE fire warning systems reveal outstanding stability after 50 repeated cycles and desired durability even undergoing 180 days of air ***,a TED-based wireless intelligent fire warning system has been developed by coupling an amplifier,analogto-digital converter and Bluetooth *** combining TE characteristics,high-temperature stability and flame retardancy with wireless IoT signal transmission,TE-based hybrid system developed here is promising for next-generation self-powered remote IoT fire warning applications.

关键词： Thermoelectric Self-powered IoT fire warning Ultrafast response Threshold adjustable

Multiporphyrinic architectures:Advances in structural design for photodynamic therapy

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Aggregate 2024年第1期5卷 67-84页

作者： Yuwei Gao Yan Li Zhengwei Xu Shuangjiang Yu Junqiu Liu Hongcheng Sun college of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhouChina

Rationally designed multiporphyrinic architectures for boosting photodynamic therapy(PDT)have attracted significant attentions recently years due to their great potential for light-mediated generation of reactive oxygen ***,there is still a gap between the structure design and their PDT performance for biomedical *** tutorial review provides a historical overview on(i)the basic concept of PDT for deeply understanding the porphyrin-mediated PDT reactions,(ii)developing strategies for constructing porphyrinic architectures,like nanorings,boxes,metal-organic frameworks(MOFs),covalent-organic frameworks(COFs),vesicles,etc.,where we classified into the following three categories:multiporphyrin arrays,porphyrinic frameworks,and others porphyrin assemblies,(iii)the various application scenarios for clinical cancer therapy and antibacterial ***,the existing challenges and future perspectives on the innovation of porphyrinic architectures for clinical PDT applications are mentioned in the end ***,the porphyrinic nanomaterials with atomically precise architectures provide an ideal platform for investigating the relationship between structures and PDT outputs,design of personalized“all-in-one”theranostic agents,and the popularization and application in wider biomedical fields.

关键词： covalent-organic frameworks(COFs) metal-organic frameworks(MOFs) multiporphyrin arrays photodynamic therapy(PDT) porphyrinic architectures

Metal–ligand interfaces for well-defined gold nanoclusters

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Science China Chemistry 2024年第3期67卷 806-823页

作者： Dan Yang Yating Wu Zhaotong Yuan Chunmei Zhou Yihu Dai Xiaoyue Wan Yan Zhu Yanhui Yang Institute of Advanced Synthesis School of Chemistry and Molecular EngineeringNanjing Tech UniversityNanjing 211816China School of Chemistry and chemical engineering Nanjing UniversityNanjing 210093China college of material and chemical engineering Minjiang UniversityFuzhou 350108China

Ligand engineering for well-defined gold nanoclusters(Au NCs) is getting more extensive attention. Organizing the Au-ligand interfaces on gold NCs can achieve the structural and functional control. This review focuses on the Au-ligand interfaces including gold-phosphorus(Au-P), gold-sulfur(Au-S), gold-selenium(Au-Se), gold-carbon(Au-C), and gold-nitrogen(Au-N), derived from the bonding between Au atoms and the different ligands(e.g., organic phosphine, thiolate, selenolate, alkynyl,n-heterocyclic carbene and nitrogenous ligands). The formation mechanism of Au-ligand interfaces is well discussed. In addition, the effects of Au-ligand interfaces on the stability, optical property, and catalysis are also presented. We hope the advances in this research area can boost the development of Au NC sciences.

关键词： Au nanoclusters well-defined structures metal–ligand interfaces formation mechanism structure–property correlation

Synthesis of multifunctional additives for solid propellants:Structure,properties and mechanism

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Defence Technology（防务技术） 2024年第3期33卷 308-316页

作者： Pingan Zhang Lina Sun Jianmin Yuan Jianru Deng college of Chemistry and chemical engineering Hunan UniversityChangsha 410082PR China college of material Science and engineering Hunan UniversityChangsha 410082PR China Hu Bei Sanjiang Aerospace Jianghe chemical Technology Co. LtdYichang 444200PR China

To simplify the composite propellant formulation and address the current issue of the single-functionality present in existing additives,the multi-cyano,amine-based polybutadiene(AEHTPB-CN)was prepared based on AEHTPB by adopting appropriate synthesis *** replacing 10% of HTPB binder in the propellant formulation,it can effectively enhance the interfacial bond strength between the propellant binder matrix and solid fillers(AP(ammonium perchlorate)and RDX(cyclotrimethylene-trinitramine)),the mechanical properties of the HTPB/AP/RDX/Al propellant were superior to blank control propellant with an improvement of 35.4% in tensile strength,62.0% enhancement in elongation at break,and reduce the propellant burn rate by 10.7% with any energy *** function mechanism of AEHTPB-CN was systematically elucidated through experiments and computer simulation *** results show that the tertiary amine group in AEHTPB-CN can react with AP to form ammonium ionic bonds,and the hydroxyl and cyano groups can form hydrogen bonding interactions with AP,which enables AEHTPB-CN to be firmly adsorbed on the AP surface through chemical and physical *** RDX,the interfacial bonding effect of AEHTPB-CN is attributed to their ability to form C-H···N≡C weak hydrogen bonding interaction between the cyano group and RDX methylene group.

关键词： Hydroxyl-terminated polybutadiene(HTPB) HTPB propellant chemical modification Bonding agent Mechanism

Construction of remote cyano-substituted quaternary carbon centers via nickel-catalyzed migratory hydrocyanation of unconjugated dienes

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Science China Chemistry 2024年第10期67卷 3397-3405页

作者： Yidan Xing Rongrong Yu Mingdong Jiao Ting Wang Xianjie Fang Key Laboratory of Organosilicon Chemistry and material Technology of Ministry of Education Key Laboratory of Organosilicon Material Technology of Zhejiang ProvinceCollege of MaterialChemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China Shanghai Key Laboratory for Molecular engineering of Chiral Drugs School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The transition-metal-catalyzed migratory functionalization has emerged as a robust protocol for the building of C–C bonds remote from the“initiation”***,a similar strategy for the construction of quaternary carbon centers is still underdeveloped and only a limited number of reports ***,we report a nickel-catalyzed migratory hydrocyanation of unconjugated dienes to construct remote cyano-substituted quaternary carbon *** transformation features exceptional regioselectivity,mild reaction conditions,broad substrate scope and high *** synthetic utility of this method has been highlighted by a series of product derivatizations,and the potential of this transformation has been extended to synthesize TRPV1 antagonist and the key intermediate in the total synthesis of *** functional theory(DFT)studies unveiled that the specific catalytic pocket assumed a significant role in the selective formation of cyano-substituted quaternary carbon centers.

关键词： chain-walking regioselectivity remote cyanation quaternary carbon centers unconjugated dienes

One-Pot Stereoselective Synthesis of Different Fused Multicyclic Iminosugars Based on the Iminium-lon Intermediate

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Chinese Journal of Chemistry 2024年第2期42卷 142-150页

作者： Song Xie Jilai Wu Likai Zhou Chao Wei Xiaoliu Li Hua Chen Key Laboratoryof chemical Biology of Hebei Province College of Chemistry and Material ScienceHebei UniversityBaodingHebei 071002China college of Chemistry and chemical engineering Xingtai UniversityXingtaiHebei 054001China

Different novel fused multicyclic iminosugars were synthesized from D-ribose tosylate,aniline and vinyl ethyl ether by one-pot three-component stereoselective[4+2]reaction at different *** iminium-ion is the key intermediate for the *** a result,several complex fused iminosugars 3a were obtained by aza-Diels-Alder mechanism at 60℃,while a series of aza-C-glycosides 5a were prepared by Mannich reaction at room temperature accompanied by another tetrahydroquinoline-fused iminosugars 4a(tricyclic derivatives)through aza-Diels-Alder *** strategy will help to construct structurally diverse and bioactive iminosugar analogues.

关键词： Fused multicyclic iminosugar Aza-Diels-Alder cycloaddition Mannich reaction Tetrahydroquinoline Multicomponent reactions Enantioselectivity Cyclization

Asymmetric Zn-N_4 atomic sites embedded hollow fibers as stable Zn anode for high-performance Zn-ion hybrid capacitor

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Journal of Energy Chemistry 2024年第10期97卷 460-469,I0009页

作者： Yukun Liu Bing Li Jin Wang Caiyun Li Hongrui Yang Yang Song Sen Zhang Chao Deng Key Laboratory for Photonic and Electronic Bandgap materials Ministry of EducationCollege of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina college of material Science and chemical engineering Harbin Engineering UniversityHarbin 150001HeilongjiangChina

Zn based electrochemical energy storage systems(EES)have attracted tremendous interests owing to their low cost and high intrinsic ***,the uncontrolled growth of Zn dendrites and the side reactions of Zn metal anodes(ZMAs)severely restrict their *** address these issues,we design the asymmetric Zn-N_(4) atomic sites embedded hollow fibers(AS-IHF)as the flexible host for stable *** introducing different nitrogen resources in the synthesis,two kinds of coordination,i,***-N(pyridinic)and Zn-N(pyrrolic),are introduced in the Zn-N_(4) atomic module *** asymmetric Zn-N_(4) module with regulated micro-environment facilitates the superior zincophilic features and promotes the Zn ***,the highly porous structure of the hollow fiber effectively reduces local current density,homogenize Zn ion flux,and alleviate structure *** the advantages endow the high efficiency and good stability for Zn plating/*** theoretical and experimental results demonstrate the high reversibility,low nucleation overpotential,and dendritefree behavior of the AS-IHF@Zn anode,which afford the high stability in high-rate and long-term ***,the solid-state Zn-ion hybrid capacitor(ZIHC)based on AS-IHF@Zn anode shows the high flexibility,reliability,and superior long-term cycling capability in a wide-range of temperatures(-20-25℃).Therefore,the present work not only gives a new strategy for modulating local environments of single atomic sites,but also propels the development of flexible power sources for diverse electronics.

关键词： Asymmetric coordination Single atomic sites Zincophilic sites Dendrite free behavior Zn-ion hybrid capacitor

Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key Laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity