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Science China chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of Sciences Beijing 100049China Beijing National laboratory for molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom *** studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol *** the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and *** the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

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Indole-3-acetic acid,a potential therapeutic target in Alzheimer's disease

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Science Bulletin 2024年第2期69卷 146-147页

作者： Jinghong Li Department of chemistry Center for Bioanalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology(Ministry of Education)Tsinghua UniversityBeijing 100084China

Alzheimer's disease(AD)is a chronic and progressive neurodegenerative disease that is characterized by the presence of amyloid-β(Ap)plaques,hyperphosphorylated microtubule-associated tau protein(p-tau)neurofibrillary tangles and neuronal *** to recent data,AD is the most common global cause of dementia in the *** billions of dollars have been invested in research,there is still no effective drug for the treatment of AD;consequently,this disease imposes a huge burden on individuals,families,and healthcare systems[1,2].

关键词： Alzheimer tau degeneration

On-demand molecular design for efficient blue phosphorescence

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Science China chemistry 2024年第7期67卷 2124-2126页

作者： Meiqi Dai Dongpeng Yan Beijing key laboratory of Energy Conversion and Storage Materials Key Laboratory of RadiopharmaceuticalsMinistry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China

Blue luminescence(including both fluorescence and phosphorescence)is one of the core elements in solid-state lighting and full-color *** to now,ultralong room temperature phosphorescence(RTP)with a long lifetime over 0.1 s has been continuously *** ultralong phosphorescence emission bands are in the region of 500 to600 ***,high-energy blue phosphorescence remains an immense challenge[1].

关键词： blue lifetime bands

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Cationic Conjugated Oligomers for Efficient and Rapid Antibacterial Photodynamic Therapy via Both Type Ⅰ and Type Ⅱ Pathways

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Chinese Journal of chemistry 2024年第1期42卷 61-66页

作者： Huan Wang Shuwen Guo Qiong Yuan Meiqi Li Yanli Tang Country key laboratory of Analytical chemistry for Life Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'anShaanxi 710119China

Recently,photodynamic therapy(PDT)has attracted wide attention due to its less susceptibility to drug resistance,broad-spectrum biocidal activity and biosafety in normal ***,the traditional photosensitizers(Ps)face the disadvantage of poor therapeutic efficacy due to the requirement of an aerobic environment to generate ^(1)O_(2) through Type Ⅱ ***,we designed and synthesized a novel cationic conjugated oligomer oligo(phenylene vinylene)(OPV)and studied its antibacterial photodynamic activity against both Gram-negative Escherichia coli(***)and Gram-positive bacteria methicillin-resistant Staphylococcus aureus(MRSA).Importantly,the OpV can rapidly produce reactive oxygen species(ROs)through double pathways,Type Ⅰ and Ⅱ mechanism under white light irradiation,and efficiently kill *** and MRSA at a nanomolar *** dual type photosensitizing capability makes OPV promising for enhanced PDT to treat pathogens and tumors in complex environments.

关键词： Conjugated oligomers Antibacterial photodynamic therapy Oligo(phenylene vinylene) Reactive oxygen species Typelandll pathways

Progress of additives for morphology control in organic photovoltaics

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Chinese Chemical Letters 2024年第6期35卷 38-46页

作者： Zhongjie Li Xiangyue Kong Yuhao Liu Huayu Qiu Lingling Zhan Shouchun Yin key laboratory of Organosilicon chemistry and Materials Technology of ministry of education College of MaterialChemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China

The microstructure of the active layer in organic photovoltaics(OPVs),such as the size of phase separation,purity of the phases,and molecular packing within each phase,plays a crucial role in influencing the behavior of excitons and charge carriers within the active *** is also a key determinant of the photovoltaic performance of the *** the optimization of OPV devices,the use of additives has been demonstrated to be an effective strategy in microstructure control,leading to enhanced ***,the quest for stable and efficient novel additives,along with an exploration and summarization of the mechanisms underlying additive-induced microstructure control,is essential for a better understanding of the developmental trends of high-performance *** this review,we categorize additives based on their chemical structures and discuss their effects on the microstructure of the active layer from both thermodynamic and kinetic ***,we elaborate on the working mechanisms and their impact on the photovoltaic performance of the *** review provides an overview of recent advances in additives for OPVs,offering potential guidance for the future development of additives and further optimization of the active layer in photovoltaic devices.

关键词： Organic photovoltaics Additives Active layer morphology Mechanisms Photovoltaic performances

Solid Bi_(2)O_(3)-derived nanostructured metallic bismuth with high formate selectivity for the electrocatalytic reduction of CO_(2)

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International Journal of Minerals,Metallurgy and Materials 2024年第4期31卷 803-811页

作者： Xiaoyan Wang Safeer Jan Zhiyong Wang Xianbo Jin College of chemistry and molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072China Engineering Research Center of Organosilicon Compounds&Materials Ministry of EducationWuhan 430072China

CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon ***,available catalysts for CO_(2) reduction are still characterized by limited stability and ***,metallic bismuth(Bi)has emerged as a promising catalyst for CO_(2) ***,we report the solid cathode electroreduction of commercial micronized Bi2O3as a straightforward approach for the preparation of nanostructured ***-1.1 V versus reversible hydrogen electrode in a KHCO3aqueous electrolyte,the resulting nanostructure Bi delivers a formate current density of~40 mA·cm^(-2) with a current efficiency of~86%,and the formate selectivity reaches97.6% at-0.78 *** nanosized Bi2O3as the precursor can further reduce the primary particle sizes of the resulting Bi,leading to a significantly increased formate selectivity at relatively low *** high catalytic activity of nanostructured Bi is attributable to the ultrafine and interconnected Bi nanoparticles in the nanoporous structure,which exposes abundant active sites for CO_(2) electrocatalytic reduction.

关键词： bismuth carbon dioxide electrocatalysis formate solid electroreduction

Sulfate-assisted Ni/Fe-based electrodes for anion exchange membrane saline splitting

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Nano Research 2024年第7期17卷 5985-5995页

作者： Yujun Han Li Shao Yuhang Liu Guodong Li Tongzhou Wang Xuerong Zheng Jihong Li Xiaopeng Han Wenbin Hu Yida Deng School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China State key laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China State key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China key laboratory of Advanced Energy Materials chemistry(ministry of education) Nankai UniversityTianjin 300071China

Saline water electrolysis is an appealing strategy for hydrogen production,attracting more attention in recent ***-based electrodes exhibit promise as catalysts for saline water ***,they suffer from the inferior service life of the oxygen evolution reaction(OER).Herein,we report an oxygen-evolution electrode consisting of a sulfate-modulated nickel-iron hydroxide(NiFeOOH)affording as the catalytic active layer and Fe-Ni3S2 as the corrosion-proof *** developed electrode only requires overpotentials of 220 and 292 mV to deliver the current density of 10 and 500 mA·cm^(−2),*** importantly,it presents long-term stability exceeding 140 and 100 h in 1 M KOH at high current densities of 500 and 1000 mA·cm^(−2),respectively,as well as 120 h for saline water electrolysis at 100 mA·cm^(−2).Experimental results reveal that the generated sulfate plays an indispensable role in improving stability and corrosion *** assembled and tested an anion exchange membrane electrolyzer with Pt/C and NiFeS/NIF as the cathode and anode,respectively,under industrial *** overall water-splitting electrolyzer achieves an impressive energy conversion efficiency of 75%±0.5%.This report offers fresh insights into the design of stable NiFe-based electrodes,which may further promote its practical applications for saline water electrolysis.

关键词： saline water electrolysis oxygen evolution reaction anode material water splitting

Recent advances in protein conformation sampling by combining machine learning with molecular simulation

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Chinese Physics B 2024年第3期33卷 80-87页

作者：唐一鸣杨中元姚逸飞周运谈圆王子超潘瞳熊瑞孙俊力韦广红 Department of Physics State Key Laboratory of Surface Physicsand Key Laboratory for Computational Physical Sciences (Ministry of Education)Shanghai 200438China

The rapid advancement and broad application of machine learning(ML)have driven a groundbreaking revolution in computational *** of the most cutting-edge and important applications of ML is its integration with molecular simulations to improve the sampling efficiency of the vast conformational space of large *** review focuses on recent studies that utilize ML-based techniques in the exploration of protein conformational *** first highlight the recent development of ML-aided enhanced sampling methods,including heuristic algorithms and neural networks that are designed to refine the selection of reaction coordinates for the construction of bias potential,or facilitate the exploration of the unsampled region of the energy ***,we review the development of autoencoder based methods that combine molecular simulations and deep learning to expand the search for protein ***,we discuss the cutting-edge methodologies for the one-shot generation of protein conformations with precise Boltzmann ***,this review demonstrates the promising potential of machine learning in revolutionizing our insight into the complex conformational ensembles of proteins.

关键词： machine learning molecular simulation protein conformational space enhanced sampling

Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides

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Chinese Journal of chemistry 2024年第10期42卷 1093-1099页

作者： Ying-Xia Wang Fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng Xian-Ming Zhang key laboratory of Magnetic Molecules and Magnetic Information Materials(ministry of education) Schoolof Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi 030006China key laboratory of Interface Science and Engineering in Advanced Material(ministry of education) College of ChemistryTaiyuan University of TechnologyTaiyuanShanxi 030024China

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the *** and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult *** overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal *** results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关键词： Triphenylamine Metal-organic frameworks Strontium Photooxidation Thiols Disulfides

Polyphenol-mediated interfacial deposition strategy for supported manganese oxide catalysts with excellent pollutant degradation performance

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Chinese Chemical Letters 2024年第5期35卷 493-498页

作者： Dong Cheng Youyou Feng Bingxi Feng Ke Wang Guoxin Song Gen Wang Xiaoli Cheng Yonghui Deng Jing Wei The key laboratory of Biomedical Information Engineering of ministry of education State Key Lab of Transducer TechnologySchool of Life Science and TechnologyXi’an Jiaotong UniversityXi’an 710049China School of Environmental and Municipal Engineering Xi’an University of Architecture and TechnologyXi’an 710055China Department of chemistry State Key Laboratory of Molecular Engineering of PolymersState Key Laboratory of Transducer TechnologyFudan UniversityShanghai 200433China key laboratory of Functional Inorganic Material chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical ***,it is still challenging to develop a versatile strategy for the deposition of metal oxide nanocatalysts on various substrates with different physicochemical ***,polyphenols are utilized as a“molecular glue”and reductant to mediate the interfacial deposition of MnO_(2) nanocatalysts on different ***_(2) nanocatalysts were in-situ grown on macroscope mineral substrates(e.g.,airstone)via an interfacial redox strategy between tannic acid(TA)and oxidized KMnO4,and then employed as a fixed catalyst of peroxymonosulfate(PMS)activation for treating pharmaceutical and personal care products(PPCPs)in *** fixed MnO_(2) exhibited superior catalytic performance toward different PPCPS via a singlet oxygen(^(1)O_(2))-dominated nonradical oxidation *** in the secondary effluent of wastewater treatment plants could be effectively removed by a fixed-bed column of the fixed MnO_(2) with long term *** cycle of Mn^(4+)/Mn^(3+)and surface hydroxyl group of the fixed MnO_(2) was proved to be responsible for the activation of *** work provides a new avenue for developing fixed metal oxides for sustainable water treatment.

关键词： Redox strategy Manganese oxides Fixed catalyst Peroxymonosulfate PPCPs