Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynam...Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.展开更多
The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify t...The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify the sulfonamide scaffold identified in our previous work,and resulting in the synthesis of 40 novel sulfonamide derivatives not previously reported in the literature.The insecticidal activities of these compounds against the Mythimna separata and Plutella xylostella were assessed.Our findings indicate that the pyridine sulfonamide structure significantly enhances insecticidal efficacy.Specifically,compound 7c exhibited LC 50 values of 0.157 and 0.256 mg/mL against the M.separata and P.xylostella,which significantly increased 97-and 41-fold compared to celangulin V,respectively.The experimental results revealed that pyridine sulfonamide analogues could serve as potential green insecticides.展开更多
The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid ...The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid syntheses of aromatic scaffolds that contains deuterium remain an important yet elusive task.State-of-the-art approaches mainly relied on the transition metal-catalyzed C-H deuteration via the assistance of directing groups(DGs),which often suffered from over-deuteration and lengthy step counts required for installation and/or removal of DG.Herein,we report a generalizable synthetic linchpin strategy for the facile preparation of the ortho-deuterated aromatic core.Through capture of aryne-derived 1,3-zwitterion with heavy water,we synthesized an array of ortho-deuterated aryl sulfonium salts.These novel linchpins not only participated the transition metal catalyzed cross-coupling reaction as nucleophiles,but also served as aryl radical reservoirs under photochemical or electrochemical conditions,enabling facile and precise access to structurally diverse deuterated aromatics.Moreover,we have disclosed a novel EDA complex enabled direct arylation of phosphines under visible-light irradiation,further expanding the utility of our platform approach.展开更多
α-Chiral amides are common in pharmaceuticals,agrochemicals,natural products,and peptides,prompting the need for new synthetic methods.Here,we introduce a nickel-catalyzed asymmetric reductive amidation method to syn...α-Chiral amides are common in pharmaceuticals,agrochemicals,natural products,and peptides,prompting the need for new synthetic methods.Here,we introduce a nickel-catalyzed asymmetric reductive amidation method to synthesizeα-chiral amides from benzyl ammonium salts and isocyanates.The key to success is using a chiral 2,2-bipyridine ligand(-)-Ph-SBpy,enabling high yield(up to 95%)and enantiomeric ratio(up to 98:2 er)under mild conditions.Addition of phenol prevents isocyanate polymerization by reversibly forming a carbamate intermediate,enhancing selectivity and efficiency.The synthetic utility is showcased through transformations of the enantioenriched amides,and the mechanism and enantioselectivity are supported by experimental and computational studies.展开更多
High temperature stress (HT) significantly reduces maize yield by impairing starch accumulation in kernels.However,the mechanism by which HT affects starch synthesis remains controversial-whether through reduced assim...High temperature stress (HT) significantly reduces maize yield by impairing starch accumulation in kernels.However,the mechanism by which HT affects starch synthesis remains controversial-whether through reduced assimilate supply or direct inhibition on kernel metabolism.To clarify these mechanisms,a heat-sensitive maize hybrid,Xianyu 335 (XY),was exposed to 30℃/20℃ (maximum/minimum temperature,control) and 40℃/30℃ for seven consecutive days during the seed setting stage.Synchronous pollination (SP),apical pollination (AP),and shading treatments were applied to manipulate the inherent source–sink ratio in maize plants.Results showed that apical kernel weight decreased by 11.9%under 40℃ in the SP treatment.The ^(13)C content,starch accumulation,and cell-wall invertase (CWIN) activity also declined by 15.9,36.7,and 16.4%,respectively,under HT.In the shading treatment,40℃/30℃ caused even greater reductions in^(13)C content,starch accumulation,and CWIN activity due to diminished assimilate supply.Conversely,in the AP treatment,starch content and CWIN activity increased by 22.0 and 18.5%,respectively,under 40℃/30℃,resulting in kernel weight and ^(13)C content similar to those in SP and shading treatments regardless of temperature.Consistent with apical kernels under AP,HT did not negatively affect middle kernels in either SP or shading treatments,as kernel weight and starch content remained unchanged under HT.Although all kernels were exposed to the same HT or control environment,their responses varied a lot.The impaired starch synthesis in apical kernels under HT was rescued by increasing carbon supply via AP treatment.The contrasting performance among middle kernels,apical kernels under AP,and apical kernels under SP or shading indicates that reduced carbon supply is a critical factor underlying inhibited starch accumulation.Our findings provide a theoretical basis for further understanding kernel abortion under HT.展开更多
Five novel sulfur-containing benzyl metabolites, designated as gastrabenzylsulfoxides A and B(1 and 2), gastrabenzylsulfinate A(3) and gastrabenzylsulfides A and B(4 and 5), along with four known compounds(6-9), were ...Five novel sulfur-containing benzyl metabolites, designated as gastrabenzylsulfoxides A and B(1 and 2), gastrabenzylsulfinate A(3) and gastrabenzylsulfides A and B(4 and 5), along with four known compounds(6-9), were isolated from the aqueous extracts of Gastrodia elata.Compounds 1 and 4 are 4-hydroxy-3-(4′-hydroxybenzyl)benzyl-substituted sulfoxide and sulfide, respectively, which are unprecedented in natural products. Compound 3 represents a rare sulfinate. Several isolates and their sulfone and disulfide analogs(10-13) were synthesized to evaluate their anti-inflammatory activity. Notably, the synthesized sulfone 10 demonstrated significant alleviation of symptoms in multiple in vivo inflammatory models.展开更多
For decades,the central dogma of oncology has been that a cancer’s identity is inextricably linked to its anatomical origin.This principle underpins the entire diagnostic and therapeutic framework,from histology-base...For decades,the central dogma of oncology has been that a cancer’s identity is inextricably linked to its anatomical origin.This principle underpins the entire diagnostic and therapeutic framework,from histology-based classification to site-specific treatment guidelines.Yet,this framework catastrophically fails for a substantial population of patients diagnosed with cancer of unknown primary(CUP).These patients present metastatic disease,yet their primary tumors remain elusive despite exhaustive clinical workup1.CUP,accounting for 1%-3%of all cancer diagnoses,is an enigma with devastating consequences;the median overall survival is only 2-12 months2-4.The inability to pinpoint an origin forces clinicians to rely on broad-spectrum empirical chemotherapy,such as taxane-carboplatin regimens,which have limited efficacy and exclude patients from the promise of targeted therapies and clinical trials5.CUP is not only a diagnostic challenge but also an indictment of the siloed approach to understanding malignancy:this cancer highlights the limitations of origin-based diagnostic frameworks.However,the confluence of high-dimensional biological data and advanced artificial intelligence(AI)is now poised to address this long-standing diagnostic limitation and to herald a new era for not only CUP but also oncology as a whole(Figure 1).展开更多
Rare earth(RE)Y-type zeolite was synthesized in situ by acidic co-hydrolysis route and hydrothermal method.The key process parameters were optimized based on the RE utilization rate.The effect of inducing a rotating p...Rare earth(RE)Y-type zeolite was synthesized in situ by acidic co-hydrolysis route and hydrothermal method.The key process parameters were optimized based on the RE utilization rate.The effect of inducing a rotating packed bed(RPB)in premixing and crystallization on crystallinity and RE utilization rate was further investigated.The results indicate that lanthanide(La)cations are successfully introduced into the sodalite cage of Y-type zeolite.The optimized conditions are that the molar ratio of Si/La is 150,premixing for 5 h,crystallization at 90℃ for 18 h,and calcination at 550℃ for 3.5 h.At this stage,the RE utilization rate reaches 74.5%.Compared with the conventional stirred tank reactor(STR),RPB can effectively shorten the premixing time and crystallization time by 4.3 h and 6 h,improve the crystallinity by 23%and RE utilization rate by 7.5%.The RE utilization rate is more than 80%by RPB,surpassing the effectiveness of using the one-exchange one-calcination process in the traditional liquid ion exchange process.It is expected to provide a reference for the in-situ efficient and green synthesis of RE zeolite.展开更多
Post-exercise whey protein isolate(WPI)supplement is beneficial for skeletal muscle recovery due to the stimulation of branched chain amino acids(BCAAs).This implies us that intake slow digestion rate of protein to su...Post-exercise whey protein isolate(WPI)supplement is beneficial for skeletal muscle recovery due to the stimulation of branched chain amino acids(BCAAs).This implies us that intake slow digestion rate of protein to sustain BCAAs releasing rate may facilitate muscle protein synthesis.To examine this hypothesis,we conducted a series of protein supplements including modified slow-digesting whey(SDW),whey,hydrolyzed whey and casein,orally to mice undergoing endurance running.Our results showed that the SDW gavage constant supplied BCAAs in the serum of mice within 6 h and significantly enhanced(P<0.01)endurance exercise capacity,compared to other groups.In addition,the SDW supplementation increased the crosssectional area of mice gastrocnemius fibers,as well as their muscle and liver glycogen content.It also increased the testosterone/cortisol ratio in serum and interleukin-6(IL-6)levels in muscle,while it decreased the tumor necrosis factor-alpha(TNF-α)levels and oxidative stress in muscle.Moreover,it may activate mechanistic target of rapamycin signaling by upregulating mRNA(bcat-1 and pgc-1α)expression.Thus,our findings illustrate that prolonged BCAAs supply duration promotes mice endurance running capacity and skeletal muscle growth,contributing to the advancement of sports nutrition practices.展开更多
Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge....Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.展开更多
Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive st...Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.展开更多
Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,a...Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,as an environmentally friendly method for synthesizing ammonia,not only mitigates the reliance on current ammonia synthesis processes fed by traditional fossil fuels but also effectively reduces nitrate pollution resulting from agricultural and industrial activities.This review explores the fundamental principles of electrocata lytic nitrate reduction,focusing on the key steps of electron transfer and ammonia formation.Additionally,it summarizes the critical factors influencing the performance and selectivity of the reaction,including the properties of the electrolyte,operating voltage,electrode materials,and design of the electrolytic cell.Further discussion of recent advances in electrocatalysts,including pure metal catalysts,metal oxide catalysts,non-metallic catalysts,and composite catalysts,highlights their significant roles in enhancing both the efficiency and selectivity of electrocata lytic nitrate to ammonia(NRA)reactions.Critical challenges for the industrial NRA trials and further outlooks are outlined to propel this strategy toward real-world applications.Overall,the review provides an in-depth overview and comprehensive understanding of electrocata lytic NRA technology,thereby promoting further advancements and innovations in this domain.展开更多
Converting CO_(2)with green hydrogen to methanol as a carbon-neutral liquid fuel is a promising route for the long-term storage and distribution of intermittent renewable energy.Nevertheless,attaining highly efficient...Converting CO_(2)with green hydrogen to methanol as a carbon-neutral liquid fuel is a promising route for the long-term storage and distribution of intermittent renewable energy.Nevertheless,attaining highly efficient methanol synthesis catalysts from the vast composition space remains a significant challenge.Here we present a machine learning framework for accelerating the development of high space-time yield(STY)methanol synthesis catalysts.A database of methanol synthesis catalysts has been compiled,consisting of catalyst composition,preparation parameters,structural characteristics,reaction conditions and their corresponding catalytic performance.A methodology for constructing catalyst features based on the intrinsic physicochemical properties of the catalyst components has been developed,which significantly reduced the data dimensionality and enhanced the efficiency of machine learning operations.Two high-precision machine learning prediction models for the activities and product selectivity of catalysts were trained and obtained.Using this machine learning framework,an efficient search was achieved within the catalyst composition space,leading to the successful identification of high STY multielement oxide methanol synthesis catalysts.Notably,the CuZnAlTi catalyst achieved high STYs of 0.49 and 0.65 g_(MeOH)/(g_(catalyst)h)for CO_(2)and CO hydrogenation to methanol at 250℃,respectively,and the STY was further increased to 2.63 g_(Me OH)/(g_(catalyst)h)in CO and CO_(2)co-hydrogenation.展开更多
Urbanization and industrialization have escalated water pollution,threatening ecosystems and human health.Water pollution not only degrades water quality but also poses long-term risks to human health through the food...Urbanization and industrialization have escalated water pollution,threatening ecosystems and human health.Water pollution not only degrades water quality but also poses long-term risks to human health through the food chain.The development of efficient wastewater detection and treatment methods is essential for mitigating this environmental hazard.Carbon dots(CDs),as emerging carbon-based nanomaterials,exhibit properties such as biocompatibility,photoluminescence(PL),water solubility,and strong adsorption,positioning them as promising candidates for environmental monitoring and management.Particularly in wastewater treatment,their optical and electron transfer properties make them ideal for pollutant detection and removal.Despite their potential,comprehensive reviews on CDs'role in wastewater treatment are scarce,often lacking detailed insights into their synthesis,PL mechanisms,and practical applications.This review systematically addresses the synthesis,PL mechanisms,and wastewater treatment applications of CDs,aiming to bridge existing research gaps.It begins with an overview of CDs structure and classification,essential for grasping their properties and uses.The paper then explores the pivotal PL mechanisms of CDs,crucial for their sensing capabilities.Next,comprehensive synthesis strategies are presented,encompassing both top-down and bottom-up strategies such as arc discharge,chemical oxidation,and hydrothermal/solvothermal synthesis.The diversity of these methods highlights the potential for tailored CDs production to suit specific environmental applications.Furthermore,the review systematically discusses the applications of CDs in wastewater treatment,including sensing,inorganic removal,and organic degradation.Finally,it delves into the research prospects and challenges of CDs,proposing future directions to enhance their role in wastewater treatment.展开更多
Natural products,with their remarkable structural and biological diversity,have historically served as a vital bridge between chemistry,the life sciences,and medicine.They not only provide essential scaffolds for drug...Natural products,with their remarkable structural and biological diversity,have historically served as a vital bridge between chemistry,the life sciences,and medicine.They not only provide essential scaffolds for drug discovery but also inspire innovative strategies in drug development.The biomimetic synthesis of natural products employs principles from biomimicry,applying inspiration from biogenetic processes to design synthetic strategies that mimic biosynthetic processes.Biomimetic synthesis is a highly efficient approach in synthetic chemistry,as it addresses critical challenges in the synthesis of structurally complex natural products with significant biological and medicinal importance.It has gained widespread attention from researchers in chemistry,biology,pharmacy,and related fields,underscoring its interdisciplinary impact.In this perspective,we present recent advances and challenges in the biomimetic synthesis of natural products,along with the significance and prospects of this field,highlighting the transformative potential of biomimetic synthesis strategies for both chemical and biosynthetic approaches to natural product synthesis in the pursuit of novel therapeutic agents.展开更多
Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional sy...Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional synthetic strategies involve the use of toxic organic nitrogenous precursors or expensive heterogeneous catalysts under elevated temperatures and pressurized oxygen.Heterogeneous electrocatalysis can initiate the activation of inorganic N sources(i.e.,NH_(3)and NO^(-)_(x))under ambient reactions in liquid phase by applying a small bias,thus allowing the synthesis of value?added nitrogenous compounds from carbonyls,alkenes,keto acids,and even carbon dioxide in a sustainable manner without the use of oxidants/reductants.This review outlines recent de-velopments in electrosynthesis of nitrogenous compounds using inorganic N sources,focusing on reaction mechanisms understanding,the design and optimization of efficient electrocatalysts,and the advances in cell configurations for various C‒N coupling reactions.The limitations and challenges in applications are also discussed.展开更多
Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded...Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded organic frameworks(HOFs)have promising application potential for embedding enzymes.In fact,no metal involvement is required,and HOFs exhibit superior biocompatibility,and free access to substrates in mesoporous channels.Herein,a facile in situ growth approach was proposed for the self-assembly of alcohol dehydrogenase encapsulated in HOF.The micron-scale bio-catalytic composite was rapidly synthesized under mild conditions(aqueous phase and ambient temperature)with a controllable embedding rate.The high crystallinity and periodic arrangement channels of HOF were preserved at a high enzyme encapsulation efficiency of 59%.This bio-composite improved the tolerance of the enzyme to the acid-base environment and retained 81%of its initial activity after five cycles of batch hydrogenation involving NADH coenzyme.Based on this controllably synthesized bio-catalytic material and a common lipase,we further developed a two-stage cascade microchemical system and achieved the continuous production of chiral hydroxybutyric acid(R-3-HBA).展开更多
Fischer-Tropsch synthesis offers a promising route to convert carbon-rich resources such as coal,natural gas,and biomass into clean fuels and high-value chemicals via syngas.Catalyst development is crucial for optimiz...Fischer-Tropsch synthesis offers a promising route to convert carbon-rich resources such as coal,natural gas,and biomass into clean fuels and high-value chemicals via syngas.Catalyst development is crucial for optimizing the process,with cobalt-and iron-based catalysts being widely used in industrial applications.Iron-based catalysts,in particular,are favored due to their low cost,broad temperature range,and high water-gas shift reaction activity,making them ideal for syngas derived from coal and biomass with a low H_(2)/CO ratio.However,despite their long history of industrial use,iron-based catalysts face two significant challenges.First,the presence of multiple iron phases-metallic iron,iron oxides,and iron carbides-complicates the understanding of the reaction mechanism due to dynamic phase transformations.Second,the high water-gas shift activity of these catalysts leads to increased CO_(2) selectivity,thereby reducing overall carbon efficiency.In Fischer-Tropsch synthesis,CO_(2) can arise as primary CO_(2) from CO disproportionation(the Boudouard reaction)and as secondary CO_(2) from the water-gas shift reaction.The accumulation of CO_(2) formation further compromises overall carbon efficiency,which is particularly undesirable given the current focus on minimizing carbon emissions and achieving carbon neutrality.This review focus on the ongoing advancements of iron-based catalysts for Fischer-Tropsch synthesis,with particular emphasis on overcoming these two critical challenges for iron-based catalysts:regulating the active phases and minimizing CO_(2) selectivity.Addressing these challenges is essential for enhancing the overall catalytic efficiency and selectivity of iron-based catalysts.In this review,recent efforts to suppress CO_(2) selectivity of iron-based catalysts,including catalyst hydrophobic modification and graphene confinement,are explored for their potential to stabilize active phases and prevent unwanted side reactions.This innovative approach offers new opportunities for developing catalysts with high activity,low CO_(2) selectivity,and enhanced stability,which are key factors for enhancing both the efficiency and sustainability for Fischer-Tropsch synthesis.Such advancements are crucial for advancing more efficient and sustainable Fischer-Tropsch synthesis technologies,supporting the global push for net-zero emissions goals,and contributing to carbon reduction efforts worldwide.展开更多
The first total synthesis of marine sesquiterpene(hydro)quinone meroterpenoids dysideanones A and E–G(1 and 4–6)has been accomplished in an enantioselective and divergent way.The sesquiterpene fragment and the aroma...The first total synthesis of marine sesquiterpene(hydro)quinone meroterpenoids dysideanones A and E–G(1 and 4–6)has been accomplished in an enantioselective and divergent way.The sesquiterpene fragment and the aromatic moiety were efficiently connected via a site-selective and diastereoselective intermolecular alkylation of Wieland–Miescher ketone derivative 9 and benzyl bromide 10.The core 6/6/6/6-fused backbone of dysideanones was efficiently constructed through an intramolecular radical cyclization reaction.Dysideanone G(6)was easily prepared on a gram-scale and dysideanones A,E,and F(1,4,and 5)were divergently transformed from dysideanone G(6)in one or two steps.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.52293472,22473096 and 22471164)。
文摘Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.
基金supported by the National Natural Science Foundation of China[Grant No.21977083].
文摘The single-atom replacement strategy is a typical approach which just converts elements in lead compounds into their analogues with very small chemical changes.In this research,we implemented this strategy to modify the sulfonamide scaffold identified in our previous work,and resulting in the synthesis of 40 novel sulfonamide derivatives not previously reported in the literature.The insecticidal activities of these compounds against the Mythimna separata and Plutella xylostella were assessed.Our findings indicate that the pyridine sulfonamide structure significantly enhances insecticidal efficacy.Specifically,compound 7c exhibited LC 50 values of 0.157 and 0.256 mg/mL against the M.separata and P.xylostella,which significantly increased 97-and 41-fold compared to celangulin V,respectively.The experimental results revealed that pyridine sulfonamide analogues could serve as potential green insecticides.
基金supported by the National Natural Science Foundation of China (Nos.22271010 and 21702013)。
文摘The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid syntheses of aromatic scaffolds that contains deuterium remain an important yet elusive task.State-of-the-art approaches mainly relied on the transition metal-catalyzed C-H deuteration via the assistance of directing groups(DGs),which often suffered from over-deuteration and lengthy step counts required for installation and/or removal of DG.Herein,we report a generalizable synthetic linchpin strategy for the facile preparation of the ortho-deuterated aromatic core.Through capture of aryne-derived 1,3-zwitterion with heavy water,we synthesized an array of ortho-deuterated aryl sulfonium salts.These novel linchpins not only participated the transition metal catalyzed cross-coupling reaction as nucleophiles,but also served as aryl radical reservoirs under photochemical or electrochemical conditions,enabling facile and precise access to structurally diverse deuterated aromatics.Moreover,we have disclosed a novel EDA complex enabled direct arylation of phosphines under visible-light irradiation,further expanding the utility of our platform approach.
基金the National Natural Science Foundation of China(Nos.22150410339,W2432012,22301233 and 22171218)the Ministry of Science and Technology China(No.wgxz2022188)。
文摘α-Chiral amides are common in pharmaceuticals,agrochemicals,natural products,and peptides,prompting the need for new synthetic methods.Here,we introduce a nickel-catalyzed asymmetric reductive amidation method to synthesizeα-chiral amides from benzyl ammonium salts and isocyanates.The key to success is using a chiral 2,2-bipyridine ligand(-)-Ph-SBpy,enabling high yield(up to 95%)and enantiomeric ratio(up to 98:2 er)under mild conditions.Addition of phenol prevents isocyanate polymerization by reversibly forming a carbamate intermediate,enhancing selectivity and efficiency.The synthetic utility is showcased through transformations of the enantioenriched amides,and the mechanism and enantioselectivity are supported by experimental and computational studies.
基金financially supported by the National Natural Science Foundation of China (32071978)the National Key Research and Development Program of China (2022YFD2300901 and 2022YFD2300905)。
文摘High temperature stress (HT) significantly reduces maize yield by impairing starch accumulation in kernels.However,the mechanism by which HT affects starch synthesis remains controversial-whether through reduced assimilate supply or direct inhibition on kernel metabolism.To clarify these mechanisms,a heat-sensitive maize hybrid,Xianyu 335 (XY),was exposed to 30℃/20℃ (maximum/minimum temperature,control) and 40℃/30℃ for seven consecutive days during the seed setting stage.Synchronous pollination (SP),apical pollination (AP),and shading treatments were applied to manipulate the inherent source–sink ratio in maize plants.Results showed that apical kernel weight decreased by 11.9%under 40℃ in the SP treatment.The ^(13)C content,starch accumulation,and cell-wall invertase (CWIN) activity also declined by 15.9,36.7,and 16.4%,respectively,under HT.In the shading treatment,40℃/30℃ caused even greater reductions in^(13)C content,starch accumulation,and CWIN activity due to diminished assimilate supply.Conversely,in the AP treatment,starch content and CWIN activity increased by 22.0 and 18.5%,respectively,under 40℃/30℃,resulting in kernel weight and ^(13)C content similar to those in SP and shading treatments regardless of temperature.Consistent with apical kernels under AP,HT did not negatively affect middle kernels in either SP or shading treatments,as kernel weight and starch content remained unchanged under HT.Although all kernels were exposed to the same HT or control environment,their responses varied a lot.The impaired starch synthesis in apical kernels under HT was rescued by increasing carbon supply via AP treatment.The contrasting performance among middle kernels,apical kernels under AP,and apical kernels under SP or shading indicates that reduced carbon supply is a critical factor underlying inhibited starch accumulation.Our findings provide a theoretical basis for further understanding kernel abortion under HT.
基金supported by the National Natural Science Foundation of China (No. 82293680)the National Science and CAMS Innovation Fund for Medical Science (No. 2021-I2M-1-028)the Nonprofit Central Research Institute Fund of Chinese Academy of Medical Sciences (No. 2021-RC350-009)。
文摘Five novel sulfur-containing benzyl metabolites, designated as gastrabenzylsulfoxides A and B(1 and 2), gastrabenzylsulfinate A(3) and gastrabenzylsulfides A and B(4 and 5), along with four known compounds(6-9), were isolated from the aqueous extracts of Gastrodia elata.Compounds 1 and 4 are 4-hydroxy-3-(4′-hydroxybenzyl)benzyl-substituted sulfoxide and sulfide, respectively, which are unprecedented in natural products. Compound 3 represents a rare sulfinate. Several isolates and their sulfone and disulfide analogs(10-13) were synthesized to evaluate their anti-inflammatory activity. Notably, the synthesized sulfone 10 demonstrated significant alleviation of symptoms in multiple in vivo inflammatory models.
基金supported by the National Natural Science Foundation of China(Grant Nos.32270688,31801117,and 82430107 to X.L.,and 32500589 to H.S.)the China Postdoctoral Science Foundation(Grant Nos.BX20240253 and 2024M762384 to H.S.)+1 种基金the Natural Science Foundation of Tianjin(Grant No.24JCQNJC01280 to H.S.)Tianjin Key Medical Discipline(Specialty)Construction Project(Grant No.TJYXZDXK-3-003A).
文摘For decades,the central dogma of oncology has been that a cancer’s identity is inextricably linked to its anatomical origin.This principle underpins the entire diagnostic and therapeutic framework,from histology-based classification to site-specific treatment guidelines.Yet,this framework catastrophically fails for a substantial population of patients diagnosed with cancer of unknown primary(CUP).These patients present metastatic disease,yet their primary tumors remain elusive despite exhaustive clinical workup1.CUP,accounting for 1%-3%of all cancer diagnoses,is an enigma with devastating consequences;the median overall survival is only 2-12 months2-4.The inability to pinpoint an origin forces clinicians to rely on broad-spectrum empirical chemotherapy,such as taxane-carboplatin regimens,which have limited efficacy and exclude patients from the promise of targeted therapies and clinical trials5.CUP is not only a diagnostic challenge but also an indictment of the siloed approach to understanding malignancy:this cancer highlights the limitations of origin-based diagnostic frameworks.However,the confluence of high-dimensional biological data and advanced artificial intelligence(AI)is now poised to address this long-standing diagnostic limitation and to herald a new era for not only CUP but also oncology as a whole(Figure 1).
基金supported by the NationalKey Research and Development Program of China(2023YFA1507701)National Natural Science Foundation of China(U22B6011,22288102)“Announcement and Challenge”Science and Technology Project of Xinjiang Uygur Autonomous Region(XJKJTJBGS-2023).
文摘Rare earth(RE)Y-type zeolite was synthesized in situ by acidic co-hydrolysis route and hydrothermal method.The key process parameters were optimized based on the RE utilization rate.The effect of inducing a rotating packed bed(RPB)in premixing and crystallization on crystallinity and RE utilization rate was further investigated.The results indicate that lanthanide(La)cations are successfully introduced into the sodalite cage of Y-type zeolite.The optimized conditions are that the molar ratio of Si/La is 150,premixing for 5 h,crystallization at 90℃ for 18 h,and calcination at 550℃ for 3.5 h.At this stage,the RE utilization rate reaches 74.5%.Compared with the conventional stirred tank reactor(STR),RPB can effectively shorten the premixing time and crystallization time by 4.3 h and 6 h,improve the crystallinity by 23%and RE utilization rate by 7.5%.The RE utilization rate is more than 80%by RPB,surpassing the effectiveness of using the one-exchange one-calcination process in the traditional liquid ion exchange process.It is expected to provide a reference for the in-situ efficient and green synthesis of RE zeolite.
基金financially supported by the Fundamental Research Funds for the Central Universities(JUSRP622014)Collaborative Innovation Center of Food Safety and Quality Control in Jiangsu Province,Jiangnan University(2022-3-2)National Key Research and Development Program of China(2022YFF1100300).
文摘Post-exercise whey protein isolate(WPI)supplement is beneficial for skeletal muscle recovery due to the stimulation of branched chain amino acids(BCAAs).This implies us that intake slow digestion rate of protein to sustain BCAAs releasing rate may facilitate muscle protein synthesis.To examine this hypothesis,we conducted a series of protein supplements including modified slow-digesting whey(SDW),whey,hydrolyzed whey and casein,orally to mice undergoing endurance running.Our results showed that the SDW gavage constant supplied BCAAs in the serum of mice within 6 h and significantly enhanced(P<0.01)endurance exercise capacity,compared to other groups.In addition,the SDW supplementation increased the crosssectional area of mice gastrocnemius fibers,as well as their muscle and liver glycogen content.It also increased the testosterone/cortisol ratio in serum and interleukin-6(IL-6)levels in muscle,while it decreased the tumor necrosis factor-alpha(TNF-α)levels and oxidative stress in muscle.Moreover,it may activate mechanistic target of rapamycin signaling by upregulating mRNA(bcat-1 and pgc-1α)expression.Thus,our findings illustrate that prolonged BCAAs supply duration promotes mice endurance running capacity and skeletal muscle growth,contributing to the advancement of sports nutrition practices.
基金supported by National Natural Science Foundation of China(52302034,52402060,52202201,52021006)Beijing National Laboratory for Molecular Sciences(BNLMS-CXTD202001)+1 种基金Shenzhen Science and Technology Innovation Commission(KQTD20221101115627004)China Postdoctoral Science Foundation(2024T170972)。
文摘Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.
基金Joint Project of Dalian University of Technology-Dalian Institute of Chemical Physics (HX20230236)。
文摘Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.
基金supported by the National Key Research and Development Program of China(2023YFE0120900)the National Natural Science Foundation of China(52377160)+2 种基金the National Natural Science Foundation of China National Young Talents Project(GYKP010)Shaanxi Provincial Natural Science Program(2023-JCYB-425)Xi’an Jiaotong University Young Top Talents Program。
文摘Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,as an environmentally friendly method for synthesizing ammonia,not only mitigates the reliance on current ammonia synthesis processes fed by traditional fossil fuels but also effectively reduces nitrate pollution resulting from agricultural and industrial activities.This review explores the fundamental principles of electrocata lytic nitrate reduction,focusing on the key steps of electron transfer and ammonia formation.Additionally,it summarizes the critical factors influencing the performance and selectivity of the reaction,including the properties of the electrolyte,operating voltage,electrode materials,and design of the electrolytic cell.Further discussion of recent advances in electrocatalysts,including pure metal catalysts,metal oxide catalysts,non-metallic catalysts,and composite catalysts,highlights their significant roles in enhancing both the efficiency and selectivity of electrocata lytic nitrate to ammonia(NRA)reactions.Critical challenges for the industrial NRA trials and further outlooks are outlined to propel this strategy toward real-world applications.Overall,the review provides an in-depth overview and comprehensive understanding of electrocata lytic NRA technology,thereby promoting further advancements and innovations in this domain.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(LDT23E06012E06)National Key R&D Program of China(2023YFC3710800)+3 种基金the National EnergySaving and Low-Carbon Materials Production and Application Demonstration Platform Program(TC220H06N)Pioneer R&D Program of Zhejiang Province-China(2024SSYS0066,2023C03016)National Natural Science Foundation of China(42341208)Zhejiang Energy Group Research Fund(ZNKJ-2023-100)。
文摘Converting CO_(2)with green hydrogen to methanol as a carbon-neutral liquid fuel is a promising route for the long-term storage and distribution of intermittent renewable energy.Nevertheless,attaining highly efficient methanol synthesis catalysts from the vast composition space remains a significant challenge.Here we present a machine learning framework for accelerating the development of high space-time yield(STY)methanol synthesis catalysts.A database of methanol synthesis catalysts has been compiled,consisting of catalyst composition,preparation parameters,structural characteristics,reaction conditions and their corresponding catalytic performance.A methodology for constructing catalyst features based on the intrinsic physicochemical properties of the catalyst components has been developed,which significantly reduced the data dimensionality and enhanced the efficiency of machine learning operations.Two high-precision machine learning prediction models for the activities and product selectivity of catalysts were trained and obtained.Using this machine learning framework,an efficient search was achieved within the catalyst composition space,leading to the successful identification of high STY multielement oxide methanol synthesis catalysts.Notably,the CuZnAlTi catalyst achieved high STYs of 0.49 and 0.65 g_(MeOH)/(g_(catalyst)h)for CO_(2)and CO hydrogenation to methanol at 250℃,respectively,and the STY was further increased to 2.63 g_(Me OH)/(g_(catalyst)h)in CO and CO_(2)co-hydrogenation.
基金supported by the Natural Science Foundation of Hebei Province(No.E2022208046)National Science Foundation of China(No.52004080)+2 种基金Key project of National Natural Science Foundation of China(No.U20A20130)Key research and development project of Hebei Province(No.22373704D)2023 Central Government Guide Local Science and Technology Development Fund Project(No.236Z1812 G)。
文摘Urbanization and industrialization have escalated water pollution,threatening ecosystems and human health.Water pollution not only degrades water quality but also poses long-term risks to human health through the food chain.The development of efficient wastewater detection and treatment methods is essential for mitigating this environmental hazard.Carbon dots(CDs),as emerging carbon-based nanomaterials,exhibit properties such as biocompatibility,photoluminescence(PL),water solubility,and strong adsorption,positioning them as promising candidates for environmental monitoring and management.Particularly in wastewater treatment,their optical and electron transfer properties make them ideal for pollutant detection and removal.Despite their potential,comprehensive reviews on CDs'role in wastewater treatment are scarce,often lacking detailed insights into their synthesis,PL mechanisms,and practical applications.This review systematically addresses the synthesis,PL mechanisms,and wastewater treatment applications of CDs,aiming to bridge existing research gaps.It begins with an overview of CDs structure and classification,essential for grasping their properties and uses.The paper then explores the pivotal PL mechanisms of CDs,crucial for their sensing capabilities.Next,comprehensive synthesis strategies are presented,encompassing both top-down and bottom-up strategies such as arc discharge,chemical oxidation,and hydrothermal/solvothermal synthesis.The diversity of these methods highlights the potential for tailored CDs production to suit specific environmental applications.Furthermore,the review systematically discusses the applications of CDs in wastewater treatment,including sensing,inorganic removal,and organic degradation.Finally,it delves into the research prospects and challenges of CDs,proposing future directions to enhance their role in wastewater treatment.
基金financially supported by the National Key Research and Development Program of China(2023YFC3503902)the National Natural Science Foundation of China(82430108,82293681(82293680),and 82321004)+2 种基金the Guangdong Basic and Applied Basic Research Foundation(2022B1515120015 and 2024A1515030103)the Guangdong Major Project of Basic and Applied Basic Research(2023B0303000026)the Science and Technology Projects in Guangzhou(202102070001)。
文摘Natural products,with their remarkable structural and biological diversity,have historically served as a vital bridge between chemistry,the life sciences,and medicine.They not only provide essential scaffolds for drug discovery but also inspire innovative strategies in drug development.The biomimetic synthesis of natural products employs principles from biomimicry,applying inspiration from biogenetic processes to design synthetic strategies that mimic biosynthetic processes.Biomimetic synthesis is a highly efficient approach in synthetic chemistry,as it addresses critical challenges in the synthesis of structurally complex natural products with significant biological and medicinal importance.It has gained widespread attention from researchers in chemistry,biology,pharmacy,and related fields,underscoring its interdisciplinary impact.In this perspective,we present recent advances and challenges in the biomimetic synthesis of natural products,along with the significance and prospects of this field,highlighting the transformative potential of biomimetic synthesis strategies for both chemical and biosynthetic approaches to natural product synthesis in the pursuit of novel therapeutic agents.
基金the NSFC(No.22472112)the Suzhou Foreign Academician Workstation(No.SWY2022001)for financial supportsthe Soochow Municipal Laboratory for Low Carbon Technologies and Industries.
文摘Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional synthetic strategies involve the use of toxic organic nitrogenous precursors or expensive heterogeneous catalysts under elevated temperatures and pressurized oxygen.Heterogeneous electrocatalysis can initiate the activation of inorganic N sources(i.e.,NH_(3)and NO^(-)_(x))under ambient reactions in liquid phase by applying a small bias,thus allowing the synthesis of value?added nitrogenous compounds from carbonyls,alkenes,keto acids,and even carbon dioxide in a sustainable manner without the use of oxidants/reductants.This review outlines recent de-velopments in electrosynthesis of nitrogenous compounds using inorganic N sources,focusing on reaction mechanisms understanding,the design and optimization of efficient electrocatalysts,and the advances in cell configurations for various C‒N coupling reactions.The limitations and challenges in applications are also discussed.
基金supported by the National Key Research and Development Program of China(2019YFA0905100)the National Natural Science Foundation of China(21991102,22378227).
文摘Constructing a framework carrier to stabilize protein conformation,induce high embedding efficiency,and acquire low mass-transfer resistance is an urgent issue in the development of immobilized enzymes.Hydrogen-bonded organic frameworks(HOFs)have promising application potential for embedding enzymes.In fact,no metal involvement is required,and HOFs exhibit superior biocompatibility,and free access to substrates in mesoporous channels.Herein,a facile in situ growth approach was proposed for the self-assembly of alcohol dehydrogenase encapsulated in HOF.The micron-scale bio-catalytic composite was rapidly synthesized under mild conditions(aqueous phase and ambient temperature)with a controllable embedding rate.The high crystallinity and periodic arrangement channels of HOF were preserved at a high enzyme encapsulation efficiency of 59%.This bio-composite improved the tolerance of the enzyme to the acid-base environment and retained 81%of its initial activity after five cycles of batch hydrogenation involving NADH coenzyme.Based on this controllably synthesized bio-catalytic material and a common lipase,we further developed a two-stage cascade microchemical system and achieved the continuous production of chiral hydroxybutyric acid(R-3-HBA).
文摘Fischer-Tropsch synthesis offers a promising route to convert carbon-rich resources such as coal,natural gas,and biomass into clean fuels and high-value chemicals via syngas.Catalyst development is crucial for optimizing the process,with cobalt-and iron-based catalysts being widely used in industrial applications.Iron-based catalysts,in particular,are favored due to their low cost,broad temperature range,and high water-gas shift reaction activity,making them ideal for syngas derived from coal and biomass with a low H_(2)/CO ratio.However,despite their long history of industrial use,iron-based catalysts face two significant challenges.First,the presence of multiple iron phases-metallic iron,iron oxides,and iron carbides-complicates the understanding of the reaction mechanism due to dynamic phase transformations.Second,the high water-gas shift activity of these catalysts leads to increased CO_(2) selectivity,thereby reducing overall carbon efficiency.In Fischer-Tropsch synthesis,CO_(2) can arise as primary CO_(2) from CO disproportionation(the Boudouard reaction)and as secondary CO_(2) from the water-gas shift reaction.The accumulation of CO_(2) formation further compromises overall carbon efficiency,which is particularly undesirable given the current focus on minimizing carbon emissions and achieving carbon neutrality.This review focus on the ongoing advancements of iron-based catalysts for Fischer-Tropsch synthesis,with particular emphasis on overcoming these two critical challenges for iron-based catalysts:regulating the active phases and minimizing CO_(2) selectivity.Addressing these challenges is essential for enhancing the overall catalytic efficiency and selectivity of iron-based catalysts.In this review,recent efforts to suppress CO_(2) selectivity of iron-based catalysts,including catalyst hydrophobic modification and graphene confinement,are explored for their potential to stabilize active phases and prevent unwanted side reactions.This innovative approach offers new opportunities for developing catalysts with high activity,low CO_(2) selectivity,and enhanced stability,which are key factors for enhancing both the efficiency and sustainability for Fischer-Tropsch synthesis.Such advancements are crucial for advancing more efficient and sustainable Fischer-Tropsch synthesis technologies,supporting the global push for net-zero emissions goals,and contributing to carbon reduction efforts worldwide.
基金Financial support for this work was provided by the National Natural Science Foundation of China(Nos.22171146,21971121,and 22188101)the Fundamental Research Funds for the Central Universities,Nankai University(No.63231199)the State Key Laboratory of Medicinal Chemical Biology。
文摘The first total synthesis of marine sesquiterpene(hydro)quinone meroterpenoids dysideanones A and E–G(1 and 4–6)has been accomplished in an enantioselective and divergent way.The sesquiterpene fragment and the aromatic moiety were efficiently connected via a site-selective and diastereoselective intermolecular alkylation of Wieland–Miescher ketone derivative 9 and benzyl bromide 10.The core 6/6/6/6-fused backbone of dysideanones was efficiently constructed through an intramolecular radical cyclization reaction.Dysideanone G(6)was easily prepared on a gram-scale and dysideanones A,E,and F(1,4,and 5)were divergently transformed from dysideanone G(6)in one or two steps.
