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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu Department of chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real active species, but also provide an approach to design the specific active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Phosphine-Catalyzed [4+3] Annulation Reaction of Indole Derivatives with MBH Carbonates:A Facile Access to Indole-1,2-fused 1,4-Diazepinones and Azepines

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Chinese Journal of chemistry 2024年第3期42卷 271-275页

作者： Yannan Zhu Haoran Jiang Yi-Ning Wang Faculty of chemistry and Chemical Engineering Yancheng Institute of TechnologyYanchengJiangsu224051 China

A phosphine-catalyzed [4+3] annulation between dinucleophilic indole derivatives and Morita−Baylis−Hillman (MBH) carbonates was discovered by using the N1 and N4′/C4′ nucleophilicities of the indole precursors,in which indoles act as four atom synthons. This protocol provides an efficient and facile access to indole-1,2-fused 1,4-diazepinones and azepines in good to high yields in one step,which illustrates potential synthetic utilities in drug discovery.

关键词： Phosphine catalysis [4+3]Annulation Indole derivatives Nitrogen heterocycles Organocatalysis

Facile synthesis of accordion-like porous carbon from waste PET bottles-based MIL-53(Al) and its application for high-performance Zn-ion capacitor

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Green Energy & Environment 2024年第7期9卷 1138-1150页

作者： Jiaxin Li Shuai Zhang Yumeng Hua Yichao Lin Xin Wen Ewa Mijowska Tao Tang Xuecheng Chen Rodney S.Ruoff Faculty of Chemical Technology and Engineering West Pomeranian University of Technology Key State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Safety Engineering China University of Mining and Technology institute of Advanced Electrical Materials Qingdao University of Science and Technology institute for Basic Science Center for Multiple Dimensional Carbon Materials Department of chemistry Ulsan National Institute of Science and Technology (UNIST) Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST)

It is of great scientific and economic value to recycle waste poly（ethylene terephthalate）(PET) into high-value PET-based metal organic frameworks（MOFs） and further convert it into porous carbon for green energy storage applications. In the present study, a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53（Al） with a 100% conversation, then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors. The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m2g-1and unique accordion-like structure with hierarchical porosity. Benefit to these advantageous characters, the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g-1at the current density of 0.5 A g-1and good rate capability of 73.6% capacitance retention at 20 A g-1in 6 mol L-1KOH electrolyte. Furthermore, the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g-1at 0.1 A g-1, excellent cycling stability of 92.2% capacitance retention after 10 000 cycles and ultra-high energy density of 150.3 Wh kg-1at power density of 90 W kg-1in 3 mol L-1ZnSO4electrolyte. It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF, and further expands the applications of MOF-derived carbons for high-performance energy storage devices, so it is conducive to both pollution alleviation and sustainable economic development.

关键词： PET Recycling Porous carbon Supercapacitor Energy storage

Asymmetric side-chain engineering of organic semiconductor for ultrasensitive gas sensing

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Chinese Chemical Letters 2024年第3期35卷 428-433页

作者： Xiaoying Ma Xiaojuan Dai Lanyi Xiang Jiajun Chang Danfeng Zhi Haozhen Zhao Zhenjie Ni Ye Zou Xike Gao Fengjiao Zhang School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190China Key Laboratory of Synthetic and Self-Assembly chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Binzhou institute of Technology Binzhou 256606China

Molecular structure of organic semiconductor plays a critical role in determining the performance and functionality of organic electronic devices,by optimizing the electrical,optical and physicochemical *** alkyl chains are fundamental units in tailering the solubility and assemblability,among which the asymmetric properties have been reported as key element for controlling the packing motifs and intrinsic charge ***,we expanded the scope of molecular asymmetry dependent sensing features based on a new series of naphthalene diimides(NDI)-based derivatives substituted with a same branching alkyl chain but various linear-shaped alkyl chains(Cn-).A clear molecular stacking change,from head-to-head bilayer to head-to-tail monolayer packing model,is observed based on the features of anisotropic molecular interactions with the change in the chain *** importantly,a unique LUMO level shift of 0.17 eV is validated for NDI-PhC4,providing a record sensitivity up to 150%to 0.01 ppb ammonia,due to the desired molecular reactivity and device amplification *** results indicate that asymmetric side-chain engineering opens a route for breath healthcare.

关键词： Organic thin film transistor Asymmetric side chain Gas sensing Molecular stacking Energy level manipulating

Co/Fe Dual Catalysis for Sequential Hydrosilylation-Isomerization:Access to Trisubstituted(E)-Alkenyl Silanes from Terminal Alkynes

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Chinese Journal of chemistry 2024年第16期42卷 1860-1866页

作者： Zhihao Guo Guixia Liu Zheng Huang Chang-Kung Chuang institute East China Normal UniversityShanghai 200062China The State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChineseAcademyof SciencesShanghai200032China School of chemistry and Materials Science Hangzhou Institute of Advanced StudyUniversity of Chinese Academy of SciencesHangzhouZhejiang310024China

By rational modification of electronic and steric properties of pincer ligands,a Co/Fe dual catalyst system is developed for one-pot sequential Markovnikov alkyne hydrosilylation and stereoselective alkene *** protocol provides an atom-economical and efficient approach to trisubstituted(E)-alkenyl silanes from widely accessible terminal alkynes with high regio-and stereoselectivities under mild *** utility of this reaction was demonstrated by gram-scale synthesis and derivatization of bioactive *** radical clock and trapping experiments indicated that radical pathway might be operative in the alkene isomerization step.

关键词： Cobalt Dual catalysis Hydrosilylation Iron Isomerization Trisubstituted alkenyl silanes

Cobalt(Ⅲ)hydride HAT mediated enantioselective intramolecular hydroamination access to chiral pyrrolidines

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Science China chemistry 2024年第6期67卷 2002-2008页

作者： Qi Meng Tao Qin Huanran Miao Ge Zhang Qian Zhang Jilin Province Key Laboratory of Organic Functional Molecular Design&Synthesis Department of ChemistryNortheast Normal UniversityChangchun130024China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China

Enantioenriched pyrrolidines and derivatives are ubiquitous substructures in compounds of importance to medicinal and biological ***,we report an efficient cobalt-catalyzed intramolecular asymmetric hydroamination reaction that produces chiral pyrrolidines with good to excellent yield and *** with previously reported radicalinvolved methodologies for enantioenriched pyrrolidines,these conditions feature two elegant versatilities,enabling(1)the use of cobalt-catalyzed hydrogen atom transfer(HAT)to generate organocobalt intermediates that bring radical reaction to organometallic chemistry,and(2)enantioselective intramolecular C-N bond forging through an S_(N)2-like displacement involving dynamic kinetic resolution(DKR).This approach provides a new alternative and efficient methodology for enantioselective radical-involved C-N bond construction that can be used in the synthesis of both chiral pyrrolidines and homologous nitrogen heterocycles.

关键词： asymmetric catalysis radical hydroamination cobalt catalysis hydrogen atom transfer

Defect mediated losses and degradation of perovskite solar cells:Origin impacts and reliable characterization techniques

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Journal of Energy chemistry 2024年第7期94卷 217-253页

作者： Himangshu Baishy Ramkrishna Das Adhikari Mayur Jagdishbhai Patel Deepak Yadav Tapashi Sarmah Mizanur Alam Manab Kalita Parameswar Krishnan lyer Centre for Nanotechnology Indian Institute of Technology GuwahatiGuwahati 781039AssamIndia Department of chemistry Indian Institute ofTechnology GuwahatGuwahati739AssamIndi

The rapid advancement of halide-based hybrid perovskite materials has garnered significant research attention,particularly in the domain of photovoltaic *** to their exceptional optoelec-tronic properties,they demonstrated power conversion efficiency(PcE)of over 25%in single junction solar *** the notable progress in PCE over the past decade,the inherent high defect density pre-senting in perovskite materials gives rise to several loss mechanisms and associated ion migration in per-ovskite solar cells(PsCs)during operational *** factors collectively contribute to a significant stability challenge in PsCs,placing their longevity far behind for *** numerous reports have explored defects,ion migration,and their impacts on device performance,a com-prehensive correlation between the types of defects and the degradation kinetics of perovskite materials and PsCs has been *** this context,this review aims to provide a comprehensive overview of the origins of defects and ion migration,emphasizing their correlation with the degradation kinetics of per-ovskite materials and PsCs,leveraging reliable characterization ***,these charac-terization techniques are intended to comprehend loss mechanisms by different passivation approaches to enhance the durability and PCE of PSCs.

关键词： Perovskite solar cells Defects lon migration Degradation Stability

Preparation of Chemically Recyclable Poly(ether-alt-ester) by the Ring Opening Polymerization of Cyclic Monomers Synthesized by Coupling Glycolide and Epoxides

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Chinese Journal of Polymer Science 2024年第2期42卷 168-175,I0006页

作者： Feng Ren Zhuang-Zhuang Liang Ming-Xin Niu Chen-Yang Hu Xuan Pang Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei230026China

Polyester and polyether are two key oxygenated polymers, and completely alternative sequence of poly(ester-alt-ether) could efficiently combine the advantages(including flexibility, degradability, etc.) of both segments. Currently, despite their copolymers could be synthesized from one-pot mixture of cyclic esters and epoxides, perfectly alternative microstructure is very challenging to realize and typically restricted to certain monomer pairs. Moving forward, synthesizing poly(ester-alt-ether) from commercially available and largescale monomers would be a significant advance. For example, successfully commercialized poly(glycolic acid)(PGA), which is not easily soluble in polymers due to its high crystallinity and is brittle and difficult to control the degradation cycle, would encounter a new paradigm if engineered into poly(ester-altether). In this work, starting from the design of monomer with hybrid structures, we successfully synthesized a series of 1,4-dioxan-2-one containing different substituents based on glycolide(GA) and epoxides using commercially available Salen-Cr(III) and PPNCl catalytic *** new monomers underwent ring-opening polymerization(ROP) to form a series of poly(ester-alt-ether) with perfectly alternating glycolic acid and propylene glycol repeat units under catalytic system of thiourea/base. The poly(ester-alt-ether) have significantly lower glass-transition temperature than PGA. Additionally, the poly(ester-alt-ether) can be chemically recovered to monomer using Sn(Oct)2 or 1,8-diazabicyclo[5.4.0]undecane-7-ene(DBU) as a catalyst in solution, thus establishing a closed-loop life cycle. From monomers derived from GA and epoxides, this work furnishes a novel strategy for the synthesis of poly(ester-alt-ether) with chemical recyclability.

关键词： Polyester Polyether Alternative copolymer Ring-opening polymerization

Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo_(5)}motifs for enhanced proton conductivity

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Nano Research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China Hebei Key Laboratory of Organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction

Kinetic network models to elucidate aggregation dynamics of aggregation-induced emission systems

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Aggregate

Aggregate 2024年第1期5卷 1-8页

作者： Zige Liu Michae L.Kalin Bojun Liu Siqin Cao Xuhui Huang Theoretical chemistry institute Department of ChemistryUniversity of Wisconsin-MadisonMadisonWisconsinUSA Biophysics University of Wisconsin-MadisonMadisonWisconsinUSA

Aggregation-induced emission(AIE)is a phenomenon where a molecule that is weakly or non-luminescent in a diluted solution becomes highly emissive when *** luminogens(AIEgens)hold promise in diverse applications like bioimaging,chemical sensing,and *** in AIE luminescence is also critical for understanding aggregation kinetics as the aggregation process is an essential component of AIE *** investigation of AIEgen aggregation is challenging due to the fast timescale of the aggregation and the amorphous aggregate *** simulations such as molecular dynamics(MD)simulation provide a valuable approach to complement experiments with atomic-level knowledge to study the fast dynamics of aggregation ***,individual simulations still struggle to systematically elucidate heterogeneous kinetics of the formation of amorphous AIEgen *** network models(KNMs),constructed from an ensemble of MD simulations,hold great potential in addressing this *** these models,dynamic processes are modeled as a series ofMarkovian transitions occurring among metastable conformational states at discrete time *** this perspective article,we first review previous studies to characterize the AIEgen aggregation kinetics and their *** then introduce KNMs as a promising approach to elucidate the complex kinetics of aggregations to address these *** importantly,we discuss our perspective on linking the output of KNMs to experimental observations of time-resolved AIE *** expect that this approach can validate the computational predictions and provide great insights into the aggregation kinetics for AIEgen *** insights will facilitate the rational design of improved AIEgens in their applications in biology and materials sciences.

关键词： hydrophobic aggregation kinetic network models molecular dynamics simulations