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Green Energy & Environment 2025年第1期10卷 161-172页

作者： Meng-Ying Liu Zhe-Hui Zhang Xue-Qi Wang Qian Sun Chen Zhang Yu Li Zhuohua Sun Katalin Barta Feng Peng Tong-Qi Yuan state key laboratory of Efficient production of Forest Resources Beijing Forestry UniversityBeijing100083China Beijing key laboratory of Lignocellulosic chemistry Beijing Forestry UniversityBeijing100083China Department of chemistry Organic and Bioorganic ChemistryUniversity of GrazHeinrichstrasse 28/II8010 GrazAustria

Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent ***,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps *** key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene *** utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling *** the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.

关键词： Atmospheric reductive catalytic fractionation Corn straw Ethylene glycol Raney Ni 5-Methoxymethylfurfural

A comprehensive review on wedelolactone: natural sources, total synthesis, and pharmacological activities

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Chinese Journal of natural Medicines 2025年第02期23卷 169-181页

作者： Haiping Cai Yue Wu Xiaojin Zhang state key laboratory of natural Medicines Jiangsu Key Laboratory of Drug Design and Optimization and Department of Chemistry China Pharmaceutical University

Plant-derived natural products have long been a vital source for developing therapeutic drugs. Wedelolactone(WDL), a coumestan isolated from Eclipta prostrata, Wedelia calendulacea, Wedelia chinensis, and Sphagneticola trilobata, demonstrates a broad spectrum of therapeutic potential, including anticancer, anti-inflammatory, anti-obesity, anti-myotoxic,antimicrobial, anti-diabetic, and tissue-protective activities. This review synthesizes information on the isolation, total synthesis, pharmacological activity, underlying mechanisms, and pharmacokinetic properties of WDL. Additionally, it offers insights into potential clinical applications and future drug discovery avenues utilizing WDL or its derivatives, either independently or in combination with other pharmaceuticals.

关键词： Mechanism natural product Pharmacological activity Synthesis Wedelolactone

Highly enantioselective carbene-catalyzedδ-lactonization via radical relay cross-coupling

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Chinese Chemical Letters 2025年第1期36卷 253-257页

作者： Yuhan Liu Jingyang Zhang Gongming Yang Jian Wang School of Pharmaceutical Sciences Key Laboratory of Bioorganic Phosphorous Chemistry and Chemical Biology(Ministry of Education)Tsinghua UniversityBeijing 100084

An N-heterocyclic carbene(NHC)catalyzed enantioselective cyclisation and trifluoromethylation of olefins with cinnamaldehydes via radical relay cross-coupling in the presence of Togni reagent is reported andδ-lactones tolerated with stereogenic centers atβ-andγ-positions are obtained in moderate to high yields and with high *** computational studies explain that the radical crosscoupling step is the key to determining the *** analysis of key transition states and intermediates also provides a reasonable explanation for the difficulty of diastereoselective *** calculations also reveal that the hydrogen-bonding interaction plays a vital role in the promotion of this chemistry.

关键词： Carbene organocatalysis Radical relay cross-coupling Trifluoromethylation Cyclisation δ-Lactone

Bifunctional organocatalyst-catalyzed dynamic kinetic resolution of hemiketals for synthesis of chiral ketals via hydrogen bonding control

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Chinese Chemical Letters 2025年第1期36卷 248-252页

作者： Meng Shan Yongmei Yu Mengli Sun Shuping Yang Mengqi Wang Bo Zhu Junbiao Chang state key laboratory of Antiviral Drugs Pingyuan LaboratoryNMPA Key Laboratory for Research and Evaluation of Innovative DrugSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Herein,we report the dynamic kinetic resolution asymmetric acylation ofγ-hydroxy-γ-perfluoroalkyl butenolides/phthalides catalyzed by amino acid-derived bifunctional organocatalysts,and a series of ketals were obtained in high yields(up to 95%)and excellent enantioselectivities(up to 99%).In terms of synthetic utility,the reaction can be performed on a gram scale,and the product can be converted into potential biological nucleoside analog.

关键词： Bifunctional organocatalyst Dynamic kinetic resolution Hemiketal Chiral ketals Hydrogen bonding

Construction of N-doped copper metal-organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene

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Science China chemistry 2025年第2期68卷 601-609页

作者： Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Coordination chemistry Institute State Key Laboratory of Coordination ChemistrySchool of Chemistry and Chemical EngineeringNanjing National Laboratory of MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

Engineering nonmetallic atom-doped metal-organic framework(MOF)catalyst to promote C−C coupling and realize conversion of CO_(2) into C_(2 )multi-carbon hydrocarbon products is still ***,with 2-methylimidazole as a dopant of N element,an N-doped NH_(2)-CuBDC catalyst was obtained via a facile and simple stirring *** illumination,compared with catalytic CO_(2) reduction to C1 product of CO by original MOF,N-doped NH_(2)-CuBDC can motivate generation of C_(2)H_(4),which is difficult to achieve in photocatalytic system by MOF-based *** transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after *** importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO_(2) reduction reaction process,which further indicates the presence of Cu–N sites in the NH_(2)-CuBDC can facilitate the formation of C2H_(4) *** work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO_(2) to C_(2) products.

关键词： metal-organic frameworks C-C coupling doping photocatalytic CO_(2) reduction Cu-based catalysts

One Novel Nortriterpenoid from the Mastic(Pistacia lentiscus)and Its Anti-Inflammatory Activity

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Phyton-International Journal of Experimental Botany 2025年第1期94卷 199-207页

作者： Yan Wu Xuerui An Haofan Lv Zhiqiang Zhao Wei Liu Chunpeng Wan key Lab of natural product chemistry and Application at Universities of Education Department of Xinjiang Uygur Autonomous Region School of Chemistry and Chemical EngineeringYili Normal UniversityYining835000China Xinjiang key laboratory of Clean Conversion and High Value Utilization of Biomass Resources School of Chemistry and Chemical EngineeringYili Normal UniversityYining835000China Jiangxi key laboratory for Postharvest Technology and Nondestructive Testing of Fruits and Vegetables College of AgronomyJiangxi Agricultural UniversityNanchang330045China

A novel pair of oleanane nor-triterpenes,with compound 1 featuring a unique 18α-H structure,was isolated from mastic,and this compound represents a noteworthy new entity not previously reported in the *** absolute configurations of their structures were further determined using a combination of different analytical methods such as NMR,high-resolution mass spectrometry(HR-MS),ultraviolet(UV),infrared(IR)and single-crystal X-ray diffraction(SXRD).The compound actively mitigated inflammations by efficiently quenching nitric oxide(NO)synthesis within an ex vivo system using lipopolysaccharide activated murine macrophage RAW264.7 ***,compound 1 exhibit a better IC50 concentration of 11.69±1.39µM,surpassing the efficacy of the positive control dexamethasone,which exhibited an IC50 of 23.21±1.17μ*** compound 2 also demonstrated inhibitory activity,its potency was comparatively weaker,with an IC50 of 26.18±2.66μM.

关键词： Mastic nor-triterpene 18α-H oleanane anti-inflammatory

The transformation of nor-seco-cucurbit[10]uril to cucurbit[5]uril and cucurbit[8]uril controlled by its own concentration

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Chinese Chemical Letters 2025年第2期36卷 373-377页

作者： Shaojie Deng Peihua Ma Qinghong Bai Xin Xiao key laboratory of Macrocyclic and Supramolecular chemistry of Guizhou Province Department of Chemistry Guizhou University

Nor-seco-cucurbit[10]uril(ns-CB[10]) is a kinetic product with unique structure. The single bridged methylene in its structure makes the molecular cavity of ns-CB[10] more deformable when compared to ordinary cucurbit[n]uril, reducing its structural stability. Repeated experiments showed that ns-CB[10] gradually cracks in an acidic solution and changes the specificity of cucurbit[5]uril(CB[5]) and cucurbit[8]uril(CB[8]) under more robust acidic solutions and when heated. A series of experiments were designed to study the transformation behavior of ns-CB[10]. It was found that the concentration of ns-CB[10] was correlated with the content distribution of CB[5] and CB[8]. This study explores the influencing factors and mechanisms of the transformation of ns-CB[10] to CB[5] and CB[8]. The results are of great significance for the application of ns-CB[10], understanding the formation mechanism of cucurbit[n]urils. Furthermore,it provides a new pathway for synthesizing new cucurbit[n]urils.

关键词： Concentration control Cracking Mechanism Nor-seco-cucurbituril Transformation

The role of sulfur cycle in new particle formation:Cycloaddition reaction of SO_(3)to H_(2)S

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Journal of Environmental Sciences 2025年第2期148卷 489-501页

作者： Haijie Zhang Wei Wang Liang Fan Junling Li Yanqin Ren Hong Li Rui Gao Yisheng Xu state key laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China key laboratory of Cluster Science Ministry of Education of ChinaSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

The chemistry of sulfur cycle contributes significantly to the atmospheric nucleation process,which is the first step of new particle formation(NPF).In the present study,cycloaddition reaction mechanism of sulfur trioxide(SO_(3))to hydrogen sulfide(H_(2)S)which is a typical air pollutant and toxic gas detrimental to the environment were comprehensively investigate through theoretical calculations and Atmospheric Cluster Dynamic Code ***-phase stability and nucleation potential of the product thiosulfuric acid(H_(2)S_(2)O_(3),TSA)were further analyzed to evaluate its atmospheric *** any catalysts,the H_(2)S+SO_(3)reaction is infeasible with a barrier of 24.2 kcal/*** nucleation precursors formic acid(FA),sulfuric acid(SA),and water(H_(2)O)could effectively lower the reaction barriers as catalysts,even to a barrierless reaction with the efficiency of cis-SA>trans-FA>trans-SA>H_(2)***,the gas-phase stability of TSA was investigated.A hydrolysis reaction barrier of up to 61.4 kcal/mol alone with an endothermic isomerization reaction barrier of 5.1 kcal/mol under the catalytic effect of SA demonstrates the sufficient stability of ***,topological and kinetic analysis were conducted to determine the nucleation potential of *** clusters formed by TSA and atmospheric nucleation precursors(SA,ammonia NH_(3),and dimethylamine DMA)were thermodynamically ***,the gradually decreasing evaporation coefficients for TSA-base clusters,particularly for TSA-DMA,suggests that TSA may participate in NPF where the concentration of base molecules are relatively *** present new reaction mechanismmay contributes to a better understanding of atmospheric sulfur cycle and NPF.

关键词： New particle formation(NPF) Atmospheric sulfur cycle Nucleation process Reaction mechanism Hydrogen sulfide(H_(2)S) Atmospheric Cluster Dynamic Code (ACDC)

Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO_(2) in CO_(2)electroreduction

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Journal of Energy chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia key laboratory of chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot 010021Inner MongoliaChina state key laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina Institute of Catalysis Department of ChemistryZhejiang UniversityHangzhou 310058ZhejiangChina National key laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030Inner MongoliaChina

Conversion of CO_(2)back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO_(2)nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79%catalytic current density to hydrocarbons(excluding CO),with 49%faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO_(2)utilization.

关键词： Cu/CeO_(2)-x Oxygen vacancy Hydrocarbon production Reaction mechanism

Deciphering fungal metabolon coupling tandem inverse-electrondemand Diels-Alder reaction and semipinacol rearrangement for the biosynthesis of spiro polycyclic alkaloids

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Science China chemistry 2025年第1期68卷 288-296页

作者： Shuai Liu Wen-Qiang Xu Ying-Tong Di Man-Cheng Tang Ding-Kang Chen Ming-Ming Cao Yao-Wen Chang Hong-Yu Tang Chun-Mao Yuan Jun-Bo Yang Zhi-Li Zuo Han Guo Zi-Fei Xu Ying Zeng Yun-Dong Wu Xiao-Jiang Hao key laboratory of Phytochemistry and natural Medicines(Chinese Academy of Sciences) Kunming Institute of BotanyChinese Academy of SciencesKunming 650201China Lab of Computational chemistry and Drug Design State Key Laboratory of Chemical OncogenomicsPeking University Shenzhen Graduate SchoolShenzhen 518055China Shenzhen Bay laboratory Shenzhen 518055China University of Chinese Academy of Sciences Beijing 100049China state key laboratory of Microbial Metabolism School of Life Sciences&BiotechnologyShanghai Jiao Tong UniversityShanghai 200240China state key laboratory of Functions and Applications of Medicinal Plants Guizhou Medical UniversityGuiyang 550014China Molecular Biology Experimental Center Germplasm Bank of Wild Species in Southwest ChinaKunming Institute of BotanyChinese Academy of SciencesKunming 650201China Yunnan key laboratory for Wild Plant Resources Kunming Institute of BotanyChinese Academy of SciencesKunming 650201China Research Unit of Chemical Biology of natural Anti-Virus products Chinese Academy of Medical SciencesBeijing 100730China

In the intricate process of natural product biosynthesis,a metabolon can enhance metabolic flux by associating sequential enzymes.A fungal metabolon,comprising of flavin-dependent monooxygenase Spe F and P450 monooxygenase Spe G,is identified in the biosynthesis of spiro polycyclic alkaloids(+)-notoamide B and its diastereomer(+)-versicolamide *** notoamide E as a substance,Spe F/Spe G metabolon can control the stereoselectivity of its 2,3-epoxidation,followed by hydrogen atom ion at C-17 to generate reactive epoxide tau-m A with dienyl iminium ***,(+)-notoamide B and(+)-versicolamide B are produced via tandem nonenzymatic inverse-electron-demand Diels-Alder reaction and semipinacol *** provides the first example of metabolon in the biosynthesis of spiro-prenylated indole alkaloids.

关键词： metabolon Diels-Alder reaction semipinacol rearrangement biosynthesis notoamides spiro polycyclic alkaloids