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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

Supramolecular systems for bioapplications:recent research progress in China

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Science China chemistry 2024年第5期67卷 1397-1441页

作者： Yue-Yang Liu Xiao-Yong Yu Yu-Chen Pan Hang Yin Shuang Chao Yujie Li He Ma Minzan Zuo Kun-Xu Teng Jun-Li Hou Yong Chen Dong-Sheng Guo Ruibing Wang Yuxin Pei Zhichao Pei Jiang-Fei Xu Xiao-Yu Hu Chunju Li Qing-Zheng Yang Leyong Wang Yu Liu Zhan-Ting Li State Key Laboratory of Organometallic chemistry Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional MoleculesShanghai Institute of Organic ChemistryChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai 200032China department of chemistry Fudan UniversityShanghai 200438China College of chemistry State Key Laboratory of Elemento-Organic ChemistryCollaborative Innovation Center of Chemical Science and EngineeringNankai UniversityTianjin 300071China State Key Laboratory of Quality research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao 999078China College of chemistry&Pharmacy Northwest A&F UniversityYangling 712100China Key Lab of organic Optoelectronics&Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China College of Materials Science and Technology Nanjing University of Aeronautics and AstronauticsNanjing 211106China Key Laboratory of Radiopharmaceuticals Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China Tianjin Key Laboratory of Structure and Performance for Functional molecules College of ChemistryTianjin Normal UniversityTianjin 300387China State Key Laboratory of Analytical chemistry for Life Science Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Supramolecular systems feature dynamic,reversible and stimuli-responsive characteristics,which are not easily achieved by molecular *** last decade has witnessed tremendous advances in the investigations of supramolecular systems for various bioapplications,which include drug delivery,anticancer therapy,antibacterial therapy,photodynamic therapy,photothermal therapy,combination therapy,antidotes for residual drugs or toxins,and bioimaging and ***-guest chemistry has played a key role in the development of such bioactive supramolecular systems,and natural macrocycles(such as cyclodextrins),synthetic macrocycles(such as calixarenes,cucurbit[n]urils,and pillararenes),and porous framework polymers(such as supramolecular organic frameworks and flexible organic frameworks)have been most successfully used as hosts to build different kinds of host-guest systems for attaining designed *** self-assembly of rationally designed amphiphilic molecules,macromolecules and polymers represent another important approach for the construction of supramolecular architectures with advanced *** this review,we summarize the important contributions made by Chinese researchers in this field,with emphasis on those reported in the past five years.

关键词： host-guest chemistry drug delivery anticancer and antibacterial photodynamic therapy photothermal therapy antidote transmembrane channel bioimaging and biosensing

Cr-catalyzed allylic C(sp^(3))–H addition to aldehydes enabled by photoinduced ligand-to-metal charge transfer

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Science China chemistry 2024年第5期67卷 1589-1595页

作者： Xianrong Zeng Feng-Hua Zhang Runchen Lai Xiaoyu Lin Zhaobin Wang Key Laboratory of Precise Synthesis of Functional molecules of Zhejiang Province Department of ChemistrySchool of Science and Research Center for Industries of the FutureWestlake UniversityHangzhou 310030China Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024China Key Laboratory of Precise Synthesis of Functional molecules of Zhejiang Province Instrumentation and Service Center for Molecular SciencesWestlake UniversityHangzhou 310024China

Photoinduced ligand-to-metal charge transfer(LMCT) has emerged as an effective strategy for synthesizing organic molecules in a sustainable manner. However, the majority of existing reports on selective C(sp^(3))–H bond functionalization via photoinduced LMCT focus on the use of late transition metals or rare-earth metals for radical additions or cross-couplings. In contrast, the utilization of photoinduced LMCT with 3d early transition metals poses a significant challenge. Herein, we describe an unprecedented approach to allylic C(sp^(3))–H addition to aldehydes, employing chromium(Cr) complexes as catalysts through visible-light-induced LMCT. By investigating the reaction pathway through various mechanistic studies, including radical trapping, kinetic isotope effect(KIE) analysis, and transient absorption spectroscopy, valuable insights have been gained. The proposed mechanism suggests the intermediacy of bromine radicals through homolysis of the Cr–Br bond. Notably, this protocol expands our understanding of the photochemical properties of earth-abundant Cr complexes.

关键词： Cr catalysis photoinduced ligand-to-metal charge transfer hydrogen-atom transfer carbonyl addition

Oxidative cyclization of allyl compounds and isocyanide: A facile entry to polysubstituted 2-cyanopyrroles

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Chinese Chemical Letters 2024年第4期35卷 330-335页

作者： Yaping Zhang Wei Zhou Mingchun Gao Tianqi Liu Bingxin Liu Chang-Hua Ding Bin Xu department of chemistry Affiliated Nantong Hospital of Shanghai University(The Sixth People's Hospital of Nantong)Shanghai Engineering Research Center of Organ RepairInnovative Drug Research CenterSchool of MedicineShanghai UniversityShanghai 200444China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

A facile Tf OH-catalyzed oxidative cyclization of allyl compounds and isocyanide has been developed with the assistance of DDQ, where isocyanide is used as the crucial "N" and "CN" sources. Highly functionalized 2-cyanopyrroles are constructed efficiently through a new formal [3 + 2] mode, demonstrating diverse reactivity and synthetic utility in organic chemistry. 2-Cyanopyrrole is converted into a nucleobase analogue of Remdesivir and 5H-pyrrolo[2,1-a]isoindole through a three-step or a two-step sequence, respectively. This protocol features broad substrate scope, operational simplicity and good functional group tolerance.

关键词： Isocyanide Cyanopyrrole Insertion Allyl compound Bronsted acid catalysis

STING agonist-conjugated metal-organic framework induces artificial leukocytoid structures and immune hotspots for systemic antitumor responses

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National Science Review 2024年第7期11卷 189-204页

作者： Taokun Luo Xiaomin Jiang Yingjie Fan Eric Yuan Jinhong Li Langston Tillman Wenbin Lin department of chemistry University of Chicago department of Radiation and Cellular Oncology and the Ludwig center for Metastasis research University of Chicago

Radiotherapy is widely used for cancer treatment, but its clinical utility is limited by radioresistance and its inability to target metastases. Nanoscale metal-organic frameworks(MOFs) have shown promise as high-Z nanoradiosensitizers to enhance radiotherapy and induce immunostimulatory regulation of the tumor microenvironment. We hypothesized that MOFs could deliver small-molecule therapeutics to synergize with radiotherapy for enhanced antitumor efficacy. Herein, we develop a robust nanoradiosensitizer,GA-MOF, by conjugating a STING agonist, 2,3-cyclic guanosine monophosphate–adenosine monophosphate(GA), on MOFs for synergistic radiosensitization and STING activation. GA-MOF demonstrated strong anticancer efficacy by forming immune-cell-rich nodules(artificial leukocytoid structures) and transforming them into immunostimulatory hotspots with radiotherapy. Further combination with an immune checkpoint blockade suppressed distant tumors through systemic immune activation. Our work not only demonstrates the potent radiosensitization of GA-MOF, but also provides detailed mechanisms regarding MOF distribution, immune regulatory pathways and long-term immune effects.

关键词： metal-organic framework radiosensitization STING agonist artificial leukocytoid structures immune hotspots immunotherapy nanomedicine

Confined Mn^(2+) enables effective aerobic oxidation catalysis

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Science China chemistry 2024年第5期67卷 1545-1553页

作者： Desheng Yuan Sicong Ma Xiao Kong Chi Zhang Lin Chen Chengsheng Yang Lihua Wang Zhen Liu Lin Ye Yongmei Liu Rui Ma Zhi-Pan Liu Yifeng Zhu Yong Cao Xinhe Bao department of Chemical Physics University of Science and Technology of ChinaHefei 230026China department of chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollaborative Innovation Center of Chemistry for Energy MaterialsFudan UniversityShanghai 200438China Key Laboratory of Synthetic and Self-Assembly chemistry for organic Functional molecules Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Institute of Advanced Fluorine-Containing Materials Zhejiang Normal UniversityJinhua 321004China State Key Laboratory of Catalysis National Laboratory for Clean EnergyCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Effective and mild activation of O_(2) is essential but challenging for aerobic oxidation. In heterogeneous catalysis, high-valence manganese oxide(e.g., +4) is known to be active for the oxidation, whereas divalent MnO is ineffective due to its limited capacity to supply surface oxygen and its thermodynamically unstable structure when binding O_(2) in reaction conditions. Inspired by natural enzymes that rely on divalent Mn^(2+), we discovered that confining Mn^(2+) onto the Mn_(2)O_(3) surface through a dedicated calcination process creates highly active catalysts for the aerobic oxidation of 5-hydroxymethylfurfural, benzyl alcohol, and *** Mn_(2)O_(3)-confined Mn^(2+) is undercoordinated and efficiently mediates O_(2) activation, resulting in 2–3 orders of magnitude higher activity than Mn_(2)O_(3) alone. Through low-temperature infrared spectroscopy, we distinguished low-content Mn^(2+) sites at Mn_(2)O_(3) surface, which are difficult to be differentiated by X-ray photoelectron spectroscopy. The combination of in-situ energydispersive X-ray absorption spectroscopy and X-ray diffraction further provides insights into the formation of the newly identified active Mn^(2+) sites. By optimizing the calcination step, we were able to increase the catalytic activity threefold *** finding offers promising frontiers for exploring active oxidation catalysts by utilizing the confinement of Mn^(2+)and oftenignored calcination skills.

关键词： confinement catalysis manganese oxide aerobic oxidation divalent Mn^(2+) operando spectroscopies

Synthesis of hierarchically porous carbon materials by zinc salts-assisted carbonization of biomass and organic solid wastes

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Particuology 2024年第1期84卷 45-52页

作者： Le-Le Zhang Lei Tong Yanwei Ding Wanqun Zhang Hai-Wei Liang Hefei National research center for Physical Sciences at the Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei230026China

Hierarchically porous carbons(HPCs)with multimodal pores have attracted considerable attention due to their unique physical and chemical properties and various application potentials in heterogeneous catalysis,environmental treatment,and energy storage and ***,we report a general and simple zinc salts-assisted method for the synthesis of HPCs with varied porosity and chemical func-tionalities by the direct carbonization of diverse biomass and *** the carbonization,zinc salts are thermally decomposed into nanoparticles that serve as in-situ templates to introduce nanopores in *** prepared HPCs exhibit high specific surface areas(up to 2432 m2 g-1),large pore volumes(up to 4.30 cm^(3)g^(-1)),and broad pore size ***,the zinc salts can be recovered and recycled,supporting the sustainable production of HPCs on large *** prepared HPCs-supported catalysts with atomically dispersed metal sites exhibit promising electrocatalytic performance for the oxygen reduction reaction.

关键词： Hierarchical porous carbon Zinc salts Biomass Wastes Electrocatalysis

Photoinduced copper-catalyzed alkoxyl radical-triggered ring-expansion/aminocarbonylation cascade

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Chinese Chemical Letters 2024年第6期35卷 331-336页

作者： Jing-Qi Tao Shuai Liu Tian-Yu Zhang Hong Xin Xu Yang Xin-Hua Duan Li-Na Guo department of chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an 710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an 710049China State Key Laboratory of Applied organic chemistry Lanzhou UniversityLanzhou 730000China

A photoinduced copper-catalyzed alkoxyl triggered C-C bond cleavage/aminocarbonylation cascade is *** adjusting the structure of alkoxyl radical precursors,functionalized lactones and ketoamides were synthesized with good yields and excellent functional group tolerance under redox-neutral ***,this protocol enables the integration of lactone fragments with many amine drugs and drug fragments.

关键词： Copper catalysis Ring-expansion Aminocarbonylatioin Macrolactones Keto-amides

Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

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Science China chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao Yujian Liu Guogang Liu Jinquan Chen Wei Jiang Zhigang Shuai Da-Hui Qu Zhaohui Wang Key Laboratory for Advanced Materials and Joint International research Laboratory of Precision chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory of organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State Key Laboratory of Precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live ***,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap ***,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 10 *** our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(128,200 cm^(-1)mol^(-1)L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently *** femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI *** calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)*** chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence