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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao key {1. of Advanced Energy material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1.2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1.was synthesized,exhibiting 1. channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1.x(x=1.2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1.3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1.h-1.nder eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1.3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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

Rational modulation of electronic structure in PtAuCuNi alloys boosts efficient electrocatalytic ethanol oxidation assisted with energy-saving hydrogen evolution

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Journal of Energy chemistry 2024年第6期93卷 557-567,I0014页

作者： Hu Yao Yinan Zheng Xin Yu Songjie Hu Baolian Su Xiaohui Guo key Lab of Synthetic and Natural {1. Molecule chemistry of Ministry of Education The College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069ShaanxiChina Department of inorganic {1. University of NamurBruxellesB-5000 NamurBelgium

Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient ***,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.21. V at 1. mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 1. mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and *** electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and ***,in the ethanol-assisted overall water splitting(E-OWS),a current density of 1. mA cm^(-2)was achieved at 0.28 ***,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was ***,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS *** interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.

关键词： Pt-based alloy Electronic structure Ethanol oxidation Self-powered system Overall water splitting

Polyoxometalate-based flexible conductive materials with superionic conductivity

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Science China chemistry 2024年第10期67卷 3299-3309页

作者： Yuxin Wang Shuping Xue Jun Geng Ying Lu Teng Li Xiaozheng Duan Xue Bai Yanli Yang Jingqi Yang Shuxia Liu key {1. of Polyoxometalate and Reticular material chemistry of Ministry of Education College of ChemistryNortheast Normal UniversityChangchun 130024China State key {1. of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Flexible ion-conductive materials exhibit intriguing advantages for applications in flexible electronic ***,the further enhancement of their conductivity within environmental limitations is an urgent demand for the development of flexible electronic devices,yet remains as a great ***,we report a“dual-acid”strategy,via the encapsulation of two acids,H_(3)PW_(1.)O_(40)(HPW) and NH_(2)SO_(3)H(SA),with synergistic interaction into poly(vinyl alcohol)-glycerol(PVA-Gly) hydrogel,to achieve polyoxometalate(POM)-based flexible materials with superionic conductivity under various environmental *** a representative example,the prepared PVA-Gly/HPW-SA-20% hydrogel presents an ultrahigh proton conductivity ranging from -30℃(3.33×1.^(-2)S cm^(-1.) to room temperature(2.78×1.^(-1.S cm^(-1.) under ambient ***,the PVA-Gly/HPW-SA-20% hydrogel exhibits remarkable advantages in anti-freezing,mechanical flexibility and self-adhesiveness,making it a promising multifunctional electrolyte for flexible electronic *** experimental results and molecular dynamics(MD) simulations jointly demonstrate that SA bridges HPW clusters to form a dense proton transport pathway induced by multiple electrostatic and hydrogen bonding interactions between SA and HPW counterparts,which contributes to the high-level proton conductivity of the PVA-Gly/HPW-SA-20% *** work provides new insights into the design of POM-based flexible materials with superionic conductivity.

关键词： polyoxometalates proton conduction dual-acid effect hydrogel molecular dynamics simulation

Recent advances in heterogeneous hydrosilylation of unsaturated carbon-carbon bonds

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Chinese Chemical Letters 2024年第6期35卷 71-85页

作者： Heng Yang Zhijie Zhou Conghui Tang Feng Chen School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China key {1. of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The hydrosilylation of unsaturated carbon-carbon bonds is one of the most critical reactions in silicone industrial *** homogeneous Speier's catalyst,Karstedt's catalyst,and other noble metal-based catalysts are widely ***,simplifying the separation of the homogeneous catalyst from reaction products and reducing the high cost of precious metals is still *** review describes the recent development of heterogeneous catalysts for alkene,alkyne,and allene hydrosilylations,which can effectively solve problems in homogeneous hydrosilylation.

关键词： Hydrosilylation Heterogeneous catalysis Alkenes Alkynes Silanes

A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su key {1. of Polyoxometalate and Reticular material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State key {1. of Supramolecular Structure and materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(1.)(NH_(4))_(4)H_(1.)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(1.)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×1.^(-2)S cm^(-1.) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

Regulation of Tumor Microenvironment Under Malignant Conditions:Application of nMOFs in Sonodynamic Therapy

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Chemical Research in Chinese Universities 2024年第4期40卷 611-626页

作者： YANG Yilin YAN Fei SHI Zhan State key {1. of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun130012P.R.China

In this review,we delve into the intricate regulation of the tumor microenvironment(TME)under malignant conditions and explore the transformative potential of nanoscale metal-organic frameworks(nMOFs)in the realm of sonodynamic therapy(SDT).The TME serves as a dynamic milieu influencing tumor progression and therapeutic response,presenting formidable challenges,such as hypoxia,acidity,excess hydrogen peroxide,high expression of glutathione,and *** the exceptional attributes of nMOFs,including their tunable structures and biocompatibility,holds immense promise for enhancing SDT efficacy and reshaping the TME *** integrating nMOFs with SDT,researchers aim to assemble multiple functionalities in a single platform that enhance tumor cell eradication while counteracting unfavorable TME conditions and immune *** potential of nMOFs to revolutionize tumor therapies by precisely targeting TME and overcoming therapeutic barriers is underscored by an in-depth analysis of recent breakthroughs in the use of nMOFs-based sonosensitizers to remodulate TME to amplify the efficacy of SDT.

关键词： Sonodynamic therapy Metal-organic framework Tumor microenvironment Modification of sonosensitizer

Controlled fluorescent switch based on a cation grease/brake rotor system of pillar[5]arene

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Chinese Chemical Letters 2024年第3期35卷 5-7页

作者： Wei-Lei Zhou Siwei Wang Yong Chen College of chemistry and {1. Science Inner Mongolia Key Laboratory of Chemistry for Nature Products and Synthesis for Functional MoleculesInnovation Team of Optical Functional Molecular DevicesInner Mongolia Minzu UniversityTongliao 028000China College of chemistry Nankai UniversityTianjin 300071China

In recent years,molecular shuttles,motors,pumps,and elevators,*** specifically respond external physical or chemical stimuli including light,temperature,pH,redox,solvent and chemical additive to change the structure a... 详细信息

关键词： additive system showing

Bright dual-color electrochemiluminescence of a structurally determined Pt1.g1. nanocluster

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Aggregate 2024年第1期5卷 345-352页

作者： Bing Yin Lirong Jiang Xiaojian Wang Ying Liu Kaiyang Kuang Mengmeng Jing Chunmin Fang Chuanjun Zhou Shuang Chen Manzhou Zhu Institutes of Physical Science and Information Technology and Centre for Atomic Engineering of Advanced materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationDepartment of Chemistry and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefeiChina

Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1.g1. nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic ***^(1.Ag_(1.)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,*** the presence of tripropylamine(TPrA)as a coreactant,solid Pt1.g1. shows unprecedented ECL efficiency,which is more than nine times higher than that of 1.mM Ru(bpy)32+with the same TPrA ***-resolved ECL spectra reveal two ECL emission bands in the presence of *** ECL emission centered at 650 nm is assigned to the solid Pt_(1.Ag_(1.)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid *** ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon *** electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 1.0 in comparison to that without *** on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1.g1. and CDs are *** findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.

关键词： AIECLE AIEE electrochemiluminescence nanocluster photoluminescence structure