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Chinese Chemical Letters 2024年第3期35卷 415-418页

作者： Chunyang Zhang Yuelan Li Zhaojun Chu Shuangzhi Yuan Yanan Qiao Jiaozhen Zhang Lin Li Yueqing Zhang Ruifeng Tian Yajie Tang Hongxiang Lou Department of natural products chemistry Key Lab of Chemical Biology(MOE)School of Pharmaceutical SciencesShandong UniversityJi'nan 250012China state key laboratory of Microbial Technology Shandong UniversityQingdao 266237China

Two distinctive rearranged 19-nor-7,8-seco-labdane diterpenoids(1 and 2)with a novel tetracyclo[5.***.1.0^(2,5.)0^(4,10)]decane skeleton,a derivative of the open tetrahydrofuran ring(7),three dimeric compounds(8-10),and four revised homologs(3-6)were obtained from Chinese liverwort Pallavicinia *** structures were identified via combined analysis of their spectroscopic data,single-crystal X-ray diffraction patterns,and ECD *** light-driven conversion of compound 5 to compounds 1-4 demonstrated that photochemically induced postmodification involved in biosynthesis is an important way to diversify natural structures.A preliminary cytotoxicity assay revealed that compound 5 showed significant inhibition in the human prostate cancer(PC-3)cell line via an apoptotic pathway.

关键词： Liverwort Pallavicinia ambigua 19-nor-7 8-seco-Labdan diterpenoid Photoinduced rearrangement Cytotoxic activity

Parallelogram 3d-4f-5d heterometallic clusters based on trilacunary tungstoantimonates with excellent proton conductivity

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Chinese Chemical Letters 2024年第3期35卷 528-531页

作者： Haiying Wang Han Xu Chaolong Chen Yingjie Zhu Yikang Zhang Dongdi Zhang Jingyang Niu Henan key laboratory of Polyoxometalate chemistry College of Chemistry and Molecular SciencesHenan UniversityKaifeng 475004China School of Pharmaceutical Science&Yunnan key laboratory of Pharmacology for natural products Kunming Medical UniversityKunming 650500China Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Two 3d-4f-5d heterometallic cluster-containing polyoxometalates,formulated as Na_(22){(SbW_(9)O_(33))_(4)[La_(3)W_(6)MO_(18)(H_(2)O)_(8)(CH_(3)COO)_(4)]_(2)}·nH_(2)O(abbreviated as La_(6)M_(2),M=Co/Mn)were synthesized and structurally ***-crystal X-ray diffraction analyses reveal that the polyanions of La_(6)Co_(2)and La_(6)Mn_(2)consist of the uncommon 3d-4f-5d clusters{La_(6)W_(12)Co_(2)}and{La_(6)W_(12)Mn_(2)},which are encapsulated by four trilacunary Keggin tungstoantimonates to form the parallelogram-shaped title ***,the polyanions can be extended into a two-dimensional(2D)frame by the linkage of peripheral Na+*** inner space of the 2D layer was filled with water molecules and thus an H-bonded network was formed,which is expected to exhibit a fascinating proton *** study of water-assisted proton conduction demonstrated that La_(6)Co_(2)and La_(6)Mn_(2)were temperature-and humiditydependent proton conductors,respectively,and the proton conductivities could reach 1.3×10^(-2)and 2.3×10^(-2)S/cm at 65℃and 90%RH conditions.

关键词： Polyoxometalate Parallelogram Heterometallic 3d-4f-5d cluster Proton conductivity

Performance enhancement and active sites identification of Cu-Cd bimetallic oxide derived catalysts for electrochemical CO_(2) reduction

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Journal of Energy chemistry 2024年第4期91卷 50-58页

作者： Cai Wang Xin Hu Bairong Chen Houan Ren Xiaoyu Wang Yilin Zhang Xinyu Chen Yuping Liu Qingxin Guan Wei Li state key laboratory of Elemento-Organic chemistry Key Laboratory of Adv.Energy Mater.Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China

The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great ***-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of ***,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 ***,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such *** results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.

关键词： CO_(2)reduction Cu-Cd bimetallic Real active sites CO production

Constituents from leaves of Macaranga hemsleyana

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Chinese Herbal Medicines 2024年第3期16卷 481-486页

作者： Joseph Sakah Kaunda Jia Liu Yaojun Xu Yuansi Chen Chenfang Yue Xingjie Zhang Ruihan Zhang Muhammad Amin Weilie Xiao Hongliang Li Xiaoli Li key laboratory of Medicinal chemistry for natural Resource Ministry of EducationYunnan Characteristic Plant Extraction LaboratoryYunnan Provincial Center for Research&Development of Natural ProductsState Key Laboratory for Conservation and Utilization of Bio-Resources in YunnanSchool of PharmacySchool of MedicineChemical Science and TechnologyYunnan UniversityKunming 650500China Yunnan key laboratory of Pharmacology for natural products Haiyuan CollegeKunming Medical UniversityKunming 650500China

Objective:To study constituents of the leaves of Macaranga hemsleyana,and evaluate their inhibitory effects against NOD-like receptor thermal protein domain associated protein 3(NLRP3)inflammasome activation,and antiproliferative ***:The constituents were isolated and purified by column chromatography on MCI gel CHP20P/P120,silica gel,Sephadex LH-20,and *** structures of compounds were determined by 1D,2D NMR,and HR-ESI-MS *** inhibitory effect of compounds on inflammasome activation was determined by lactate dehydrogenase(LDH)*** antiproliferative activity was evaluated using MTT ***:The study led to the isolation of 23 compounds,including one new compound,identified as(2Z)-3-[4-(β-D-glucopyranosyloxy)-2′-hydroxy-5′-methoxyphenyl]-2-propenoic acid(1),together with 22 known compounds recognized as 1,4-dihydro-4-oxo-3-pyridinecarbonitrile(2),methyl 4-methoxynicotinate(3),4-methoxynicotinonitrile(4),1-(3-O-β-D-glucopyranosyl-4,5-dihydroxyphenyl)-ethanone(5),neoisoastilbin(6),isoastilbin(7),aromadendrin(8),neoastilbin(9),astilbin(10),quercitrin(11),neoschaftoside(12),apigenin 6,8-bis-C-α-L-arabinoside(13),vitexin(14),bergenin(15),scopoletin(16),glucopyranoside salicyl(17),koaburside(18),benzylβ-D-glucoside(19),icariside B5(20),roseoside(21),loliolide(22),and adenosine(23).The tested compounds did not show LDH inhibition nor antiproliferative ***:Compound 1 was a new *** 2 and 3 were obtained for the first time from natural *** 22 known compounds constituted of alkaloids(2–4,23),phenolics(5,15,17,18),flavonoids(6–14),coumarin(16),benzyl glycoside(19),and norsesquiterpenes(20–22).All the compounds,1–23,were revealed from *** for the first *** is the initial uncovering of molecules 1–10,12,13,17–19,and 23 from the genus *** isolated compounds,11,14–16,and 20–22 established taxonomic classification of *** in Euphorbiaceae *** were outstanding as

关键词： antiproliferative activity chemotaxonomic significance flavonoids glycoside Macaranga hemsleyana Pax et Hoffm NLRP3 inflammasome

Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation

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Carbon Energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long state key laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great ***,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic *** exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and ***,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) *** study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

Late-stage modification of bioactive compounds:Improving druggability through efficient molecular editing

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Acta Pharmaceutica Sinica B 2024年第3期14卷 1030-1076页

作者： Tongyu Huo Xinyi Zhao Zengrui Cheng Jialiang Wei Minghui Zhu Xiaodong Dou Ning Jiao state key laboratory of natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Changping laboratory Beijing 102206China Shanghai key laboratory of Green chemistry and Chemical Processes East China Normal UniversityShanghai 200062China

Synthetic chemistry plays an indispensable role in drug discovery,contributing to hit compounds identification,lead compounds optimization,candidate drugs preparation,and so *** Nobel Prize laureate James Black emphasized,“the most fruitful basis for the discovery of a new drug is to start with an old drug”***-stage modification or functionalization of drugs,natural products and bioactive compounds have garnered significant interest due to its ability to introduce diverse elements into bioactive compounds *** modifications alter the chemical space and physiochemical properties of these compounds,ultimately influencing their potency and *** enrich a toolbox of chemical modification methods for drug discovery,this review focuses on the incorporation of halogen,oxygen,and nitrogen—the ubiquitous elements in pharmacophore components of the marketed drugs—through late-stage modification in recent two decades,and discusses the state and challenges faced in these *** also emphasize that increasing cooperation between chemists and pharmacists may be conducive to the rapid discovery of new activities of the functionalized ***,we hope this review would serve as a valuable resource,facilitating the application of late-stage modification in the construction of novel molecules and inspiring innovative concepts for designing and building new drugs.

关键词： Late-stage modification Drug space Halogenation Oxygenation Nitrogenation Synthetic chemistry

Facile and effective synthesis strategy for terbium-doped hydroxyapatite toward photoelectric devices and flexible functional fibers

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Rare Metals 2024年第4期43卷 1713-1723页

作者： Xiao-Dong Zhang Kun Nie Zi-Yao Hu Ran-Ran Zhou Xiu-Qiang Duan Wu-Bin Dai Song-Song Nie Song-Jun Yao Luo-Xin Wang Le-Fu Mei Hua Wang Yi-Yi Yao Xiao-Xue Ma Hubei key laboratory for New Textile Materials and Applications and state key laboratory of New Textile Materials and Advanced Processing Technology School of Materials Science and EngineeringWuhan Textile UniversityWuhan430200China key laboratory of Testing and Tracing of Rare Earth products for state Market Regulation Jiangxi University of Science and TechnologyGanzhou341000China Hubei key laboratory of Plasma chemistry and Advanced Materials and key laboratory of Green Chemical Engineering Process of Ministry of Education Wuhan Institute of TechnologyWuhan430205China

As a material with good biocompatibility,hydroxyapatite(HAP)can have optical properties after doping with various rare earth *** a biocompatible fluorescent material,doped HAP could have broad applications in biological probes,drug delivery,optoelectronic materials,fluorescence anti-counterfeiting,and other *** this paper,we put forward the preparation of HAP doped with terbium(Ⅲ)ions(Tb^(3+))by hydrothermal *** controlling the Tb^(3+)doping content in reaction and the reaction time,the changes in HAP's structure,morphology,and luminescence properties under different conditions were *** the doping amount of Tb^(3+)reached an optimal value,the dipole-quadrupole would occur and the concentration would be *** control experiment showed that the optimal Tb3+content was 7.5×10^(-5)mol,which showed the best fluorescence ***,a non-luminous material,was rarely used in the field of fluorescent anti-counterfeiting and photoelectric *** proposed to prepare a luminescent aramid/polyphenylene sulfide(ACFs/PPS)fiber paper and a new light-emitting diode(LED)using the Tb-doped HAP *** composite sample exhibited an excellent stability and fluorescence performance,which also demonstrated a possibility of HAP applications in anticounterfeiting and *** introduction of Tb3+dopant HAP was done to give HAP optical properties and broaden the application range of HAP.

关键词： Hydroxyapatite Rare earth luminescence Photoelectric device Aramid Polyphenylene sulfide fiber paper Luminescent fiber

Ni-catalyzed highly regio- and stereo-selective diborylative cyclization of 1,6-enynes with diboron reagent

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Science China chemistry 2024年第3期67卷 981-989页

作者： Qitao Guan Zhen Shen Yiqiang Tian Genping Huang Chun Zhang Institute of Molecular Plus Tianjin Key Laboratory of Molecular Optoelectronic ScienceDepartment of ChemistrySchool of SciencesTianjin UniversityTianjin 300072China state key laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China

The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B_2pai_2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory(DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.

关键词： nickel-catalyzed organoboron cyclization regioselectivity enantioselectivity

Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu state key laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China state key laboratory of Fine Chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China state key laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

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