A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficie...A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.展开更多
A three component one-pot protocol was investigated for the synthesis of methylene bis isoxazolo[4,5-b]-pyridine-N-oxides from commercially available materials.
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
An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][B...An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][BF4] is described in this paper. Advantages of the method presented here include mild conditions, high yields together with a green nature and ease of recovery and reuse of the reaction medium.展开更多
A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-（carboxymethyl）uracil via a multi-component reaction is described. The reactive 1：1 intermediate produced from the r...A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-（carboxymethyl）uracil via a multi-component reaction is described. The reactive 1：1 intermediate produced from the reaction of tert-butyl isocyanide and dialkyl acetylenedicarboxylates was trapped at room temperature by 1-（carboxymethyl）uracil derivatives to yield polyfunctio- nalized furan rings in fairly good yields.展开更多
Oxonium ylide intermediates generated from α-diazocarbonyl compounds and water were trapped by Zn（Ⅱ）-activated α- dicarbonyl compounds. The reaction gave α,β-dihydroxyl acid derivatives in moderate yield.
The multi-component oxide (Al0.88Fe0.67Zn0.28O3)) surface (abbreviated as MCOS) was prepared to optimize the effectiveness of the elimination of As (III) from aqueous solution. The oxide surface was synthe-sized by co...The multi-component oxide (Al0.88Fe0.67Zn0.28O3)) surface (abbreviated as MCOS) was prepared to optimize the effectiveness of the elimination of As (III) from aqueous solution. The oxide surface was synthe-sized by co-precipitation method using corresponding metal carbonates. It was characterized by XRD, TGA and DSC. The surface morphology of MCOS was observed in SEM and the elemental analysis was accomplished by EDX. The composition of Al2O3, Fe2O3 & ZnO was 23.6, 39.9 and 20.6 wt% respectively in XRF analysis. The specific surface area was found 389.85 m2 g-1. Batch experiments were performed to remove As (III) from aqueous solution considering various parameters such as effect of pH, contact time, initial arsenic concentration, temperature and sor-bent dosage. The maximum sorption capacity of the surface was almost steady from pH 4 to pH 9. Kinetic study shows that As (III) sorption is following second order rate equation with the rate constant of 80×10-2 g mg-1 min-1 at room temperature and this rate was increased with increasing temperature which indicates the sorption was endothermic process. The free energy change, ΔGo was negative which proves that the sorption was spontaneous and thermodynamically favorable. Sorption isotherm was interpreted by Langmuir equation and the maximum sorption capacity of oxide monolayer was 13×10-2 mg g-1.展开更多
Caffeine was applied as a green and natural catalyst for the one-pot,four-component sequential condensation between 2-hydroxy-1,4-naphthoquinone,aromatic 1,2-diamines,ammonium thiocyanate and acid chlorides in the pre...Caffeine was applied as a green and natural catalyst for the one-pot,four-component sequential condensation between 2-hydroxy-1,4-naphthoquinone,aromatic 1,2-diamines,ammonium thiocyanate and acid chlorides in the presence of a basic ionic liquid（l-butyl-3-methylimidazolium hydroxide） to afford the corresponding benzo[a][1,3]oxazino[6,5-c]phenazine derivatives.In this one-pot transformation,five bonds and two new rings are efficiently formed.This protocol has the advantages of operational simplicity,high yields,easy workup,avoidance of hazardous or toxic catalysts and organic solvents and high chemo-and regioselectivities.展开更多
An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been devel...An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been developed by domino three-component condensation reaction between 2-hydroxynaphthalene-1,4-dione,benzene-1,2-diamines and acetylenic esters in the presence of a catalytic amount of DABCO as an expedient,eco-friendly and reusable base catalyst in water.This green process produces biologically and pharmacologically significant heterocycles in a one-pot single operation and offers considerable advantages such as：operational simplicity,short reaction time,high yields,reusability of catalyst,absence of any tedious workup or purification and avoids hazardous reagents/solvents.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
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
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
Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and m...Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and metabolic events,which need to be carried out at the right place,time,and intensity.Such mechanisms include axonal transport,local synthesis,and liquid-liquid phase separations.Alterations and malfunctions in these processes are correlated to neurodegenerative diseases such as amyotrophic lateral sclerosis(ALS).展开更多
Background Milk synthesis is an energy-intensive process influenced by oxygen availability.This study investigates how hypoxia affects milk synthesis in BMECs,focusing on key genes involved in lactation and energy met...Background Milk synthesis is an energy-intensive process influenced by oxygen availability.This study investigates how hypoxia affects milk synthesis in BMECs,focusing on key genes involved in lactation and energy metabolism.Methods BMECs were cultured in a normoxic environment and then transferred to a hypoxia chamber with 1%O2 for specified durations.The study evaluated cellular responses through various molecular experiments and RNA sequencing.Small interfering RNA was employed to knock down HIF-1αto investigate whether the lactation-related phenotype alteration depends on HIF-1α.Results Hypoxia disrupted milk protein production by reducing mTOR/P70S6K/4EBP1 signaling and downregulating genes critical for amino acid transport and protein synthesis.Triglyceride synthesis increased due to enhanced fatty acid uptake and the upregulation of regulatory proteins,including FASN and PPARγ.Although glucose uptake was elevated under hypoxia,key enzymes for lactose synthesis were downregulated,suggesting a redirection of glucose toward energy production.Mitochondrial function was impaired under hypoxia,with reduced gene expression in TCA cycle,ETC,cytosol-mitochondrial transport,decreased ATP levels,increased ROS levels,and structural alterations.Additionally,lipid synthesis and glucose uptake depend on HIF-1α,while milk protein synthesis alterations occurred independently of HIF-1α.Conclusions Hypoxia alters milk synthesis in BMECs by disrupting milk protein synthesis,enhancing lipid metabolism,and impairing energy production.These findings provide valuable insights into the molecular mechanisms underlying the effect of oxygen deprivation on lactation efficiency,offering potential targets for mitigating hypoxic stress in the mammary glands of dairy animals.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
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
Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face si...Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face significant challenges in terms of energy consumption and environmental impact.As a sustainable alternative,photocatalytic H_(2)O_(2) production,driven by solar energy,has emerged as a promising approach.This review discusses the key advancements in photocatalytic H_(2)O_(2) synthesis,focusing on overcoming challenges such as charge recombination,selectivity for the two-electron oxygen reduction reaction(2e^(-)ORR),and catalyst stability.Recent innovations in photocatalyst design,including high-entropy materials,single-atom catalysts,and covalent organic frameworks(COFs),have significantly enhanced efficiency and stability.Furthermore,novel strategies for optimizing charge separation,light harvesting,and mass transfer are explored.The integration of artificial intelligence and bioinspired systems holds potential for accelerating progress in this field.This review provides a comprehensive overview of current challenges and cutting-edge solutions,offering valuable insights for the development of scalable,decentralized H_(2)O_(2) production systems that contribute to a more sustainable future.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
The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectr...The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective.Here,we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived Cd In_(2)S_(4)/In_(2)S_(3)heterojunction that exhibited stable and high selectivity.Multiple characterizations of the Cd In_(2)S_(4)/In_(2)S_(3)heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites,a high visible-light utilization rate(λ<600 nm),efficient charge separation,and a prolonged charge-carrier lifetime.Moreover,an S-scheme charge transfer mechanism,based on the interleaved band between the two components,improved the reduction capability of the electrons.Benefiting from the compositional and structural synergy,the yield CO by Cd In_(2)S_(4)/In_(2)S_(3)-250(CI-250)reached 135.62μmol·g^(-1)·h^(-1),which was 49.32 times and 32.88 times higher than that of In_(2)S_(3)and Cd In_(2)S_(4),respectively.The Cd In_(2)S_(4)/In_(2)S_(3)heterojunction exhibited a quantum efficiency of 4.23%with a CO selectivity of 71%.Four cycle tests confirmed the good stability and recyclability of the CI-250.This work provides a new approach for designing and preparing high-performance hollow MOFsbased photocatalysts for scalable and sustainable CO_(2)reduction.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
基金supported by Sichuan Science and Technology Program(No.2023NSFSC0101)the 2024 Provincial platform project of Chengdu Normal University(No.GNFZ202404)+1 种基金Natural Science Foundation of Shandong Province(No.ZR2021MB065)National Natural Science Foundation of China(No.22101237)。
文摘A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.
文摘A three component one-pot protocol was investigated for the synthesis of methylene bis isoxazolo[4,5-b]-pyridine-N-oxides from commercially available materials.
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the National Natural Science Foundation of China(No.20573034).
文摘An efficient and novel procedure for the preparation of pyrazolo[3,4-b]pyridine derivatives through multi-component reaction of aldehyde, 5-amino-3-methyl-1-phenylpyrazole and malononitrile or cyanoacetate in [bmim][BF4] is described in this paper. Advantages of the method presented here include mild conditions, high yields together with a green nature and ease of recovery and reuse of the reaction medium.
基金supported by the Research Council of the University of Mazandaran,Iran
文摘A simple synthesis of highly functionalized 2,5-diaminofurans based pyrimidine derivatives from 1-（carboxymethyl）uracil via a multi-component reaction is described. The reactive 1：1 intermediate produced from the reaction of tert-butyl isocyanide and dialkyl acetylenedicarboxylates was trapped at room temperature by 1-（carboxymethyl）uracil derivatives to yield polyfunctio- nalized furan rings in fairly good yields.
基金supported by National Science Foundation of China(No.20772033)China postdoctoral Science Foundation(No.20080440607)
文摘Oxonium ylide intermediates generated from α-diazocarbonyl compounds and water were trapped by Zn（Ⅱ）-activated α- dicarbonyl compounds. The reaction gave α,β-dihydroxyl acid derivatives in moderate yield.
文摘The multi-component oxide (Al0.88Fe0.67Zn0.28O3)) surface (abbreviated as MCOS) was prepared to optimize the effectiveness of the elimination of As (III) from aqueous solution. The oxide surface was synthe-sized by co-precipitation method using corresponding metal carbonates. It was characterized by XRD, TGA and DSC. The surface morphology of MCOS was observed in SEM and the elemental analysis was accomplished by EDX. The composition of Al2O3, Fe2O3 & ZnO was 23.6, 39.9 and 20.6 wt% respectively in XRF analysis. The specific surface area was found 389.85 m2 g-1. Batch experiments were performed to remove As (III) from aqueous solution considering various parameters such as effect of pH, contact time, initial arsenic concentration, temperature and sor-bent dosage. The maximum sorption capacity of the surface was almost steady from pH 4 to pH 9. Kinetic study shows that As (III) sorption is following second order rate equation with the rate constant of 80×10-2 g mg-1 min-1 at room temperature and this rate was increased with increasing temperature which indicates the sorption was endothermic process. The free energy change, ΔGo was negative which proves that the sorption was spontaneous and thermodynamically favorable. Sorption isotherm was interpreted by Langmuir equation and the maximum sorption capacity of oxide monolayer was 13×10-2 mg g-1.
基金financial support from the Research Council of Young Researchers and Elite Club,Yazd Branch,Islamic Azad University,Yazd,Iran and University of Science and Arts of Yazd,Iran
文摘Caffeine was applied as a green and natural catalyst for the one-pot,four-component sequential condensation between 2-hydroxy-1,4-naphthoquinone,aromatic 1,2-diamines,ammonium thiocyanate and acid chlorides in the presence of a basic ionic liquid（l-butyl-3-methylimidazolium hydroxide） to afford the corresponding benzo[a][1,3]oxazino[6,5-c]phenazine derivatives.In this one-pot transformation,five bonds and two new rings are efficiently formed.This protocol has the advantages of operational simplicity,high yields,easy workup,avoidance of hazardous or toxic catalysts and organic solvents and high chemo-and regioselectivities.
基金financial support from the Research Council of Young ResearchersElite Club of the Islamic Azad University of YazdUniversity of Sistan and Baluchestan
文摘An efficient,convenient and environmentally benign procedure for the synthesis of novel 3-oxo-3Hbenzo[a]pyrano[2.3-c]phenazine-l-carboxylate and 3-（5-hydroxybenzo[a]phenazin-6-yl） acrylate derivatives has been developed by domino three-component condensation reaction between 2-hydroxynaphthalene-1,4-dione,benzene-1,2-diamines and acetylenic esters in the presence of a catalytic amount of DABCO as an expedient,eco-friendly and reusable base catalyst in water.This green process produces biologically and pharmacologically significant heterocycles in a one-pot single operation and offers considerable advantages such as：operational simplicity,short reaction time,high yields,reusability of catalyst,absence of any tedious workup or purification and avoids hazardous reagents/solvents.
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.
文摘Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and metabolic events,which need to be carried out at the right place,time,and intensity.Such mechanisms include axonal transport,local synthesis,and liquid-liquid phase separations.Alterations and malfunctions in these processes are correlated to neurodegenerative diseases such as amyotrophic lateral sclerosis(ALS).
基金supported by grants from the National Natural Science Foundation of China(grant number:32072756)Agricultural Research System of China(grant number:CARS-36).
文摘Background Milk synthesis is an energy-intensive process influenced by oxygen availability.This study investigates how hypoxia affects milk synthesis in BMECs,focusing on key genes involved in lactation and energy metabolism.Methods BMECs were cultured in a normoxic environment and then transferred to a hypoxia chamber with 1%O2 for specified durations.The study evaluated cellular responses through various molecular experiments and RNA sequencing.Small interfering RNA was employed to knock down HIF-1αto investigate whether the lactation-related phenotype alteration depends on HIF-1α.Results Hypoxia disrupted milk protein production by reducing mTOR/P70S6K/4EBP1 signaling and downregulating genes critical for amino acid transport and protein synthesis.Triglyceride synthesis increased due to enhanced fatty acid uptake and the upregulation of regulatory proteins,including FASN and PPARγ.Although glucose uptake was elevated under hypoxia,key enzymes for lactose synthesis were downregulated,suggesting a redirection of glucose toward energy production.Mitochondrial function was impaired under hypoxia,with reduced gene expression in TCA cycle,ETC,cytosol-mitochondrial transport,decreased ATP levels,increased ROS levels,and structural alterations.Additionally,lipid synthesis and glucose uptake depend on HIF-1α,while milk protein synthesis alterations occurred independently of HIF-1α.Conclusions Hypoxia alters milk synthesis in BMECs by disrupting milk protein synthesis,enhancing lipid metabolism,and impairing energy production.These findings provide valuable insights into the molecular mechanisms underlying the effect of oxygen deprivation on lactation efficiency,offering potential targets for mitigating hypoxic stress in the mammary glands of dairy animals.
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financial support from the National Natural Science Foundation of China(No.22279143).
文摘Hydrogen peroxide(H_(2)O_(2))is a crucial,eco-friendly oxidizing agent with a wide range of industrial,environmental,and biomedical applications.Traditional production methods,such as the anthraquinone process,face significant challenges in terms of energy consumption and environmental impact.As a sustainable alternative,photocatalytic H_(2)O_(2) production,driven by solar energy,has emerged as a promising approach.This review discusses the key advancements in photocatalytic H_(2)O_(2) synthesis,focusing on overcoming challenges such as charge recombination,selectivity for the two-electron oxygen reduction reaction(2e^(-)ORR),and catalyst stability.Recent innovations in photocatalyst design,including high-entropy materials,single-atom catalysts,and covalent organic frameworks(COFs),have significantly enhanced efficiency and stability.Furthermore,novel strategies for optimizing charge separation,light harvesting,and mass transfer are explored.The integration of artificial intelligence and bioinspired systems holds potential for accelerating progress in this field.This review provides a comprehensive overview of current challenges and cutting-edge solutions,offering valuable insights for the development of scalable,decentralized H_(2)O_(2) production systems that contribute to a more sustainable future.
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).
基金financially supported by the Program for the Development of Science and Technology of Jilin Province(Nos.20240601047RC and YDZJ202201ZYTS629)Hainan Province Science and Technology Special Fund(No.ZDYF2022SHFZ090)+1 种基金the National Natural Science Foundation(Nos.22466017 and 22061014)the specific research fund of the Innovation Platform for Academicians of Hainan Province。
文摘The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective.Here,we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived Cd In_(2)S_(4)/In_(2)S_(3)heterojunction that exhibited stable and high selectivity.Multiple characterizations of the Cd In_(2)S_(4)/In_(2)S_(3)heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites,a high visible-light utilization rate(λ<600 nm),efficient charge separation,and a prolonged charge-carrier lifetime.Moreover,an S-scheme charge transfer mechanism,based on the interleaved band between the two components,improved the reduction capability of the electrons.Benefiting from the compositional and structural synergy,the yield CO by Cd In_(2)S_(4)/In_(2)S_(3)-250(CI-250)reached 135.62μmol·g^(-1)·h^(-1),which was 49.32 times and 32.88 times higher than that of In_(2)S_(3)and Cd In_(2)S_(4),respectively.The Cd In_(2)S_(4)/In_(2)S_(3)heterojunction exhibited a quantum efficiency of 4.23%with a CO selectivity of 71%.Four cycle tests confirmed the good stability and recyclability of the CI-250.This work provides a new approach for designing and preparing high-performance hollow MOFsbased photocatalysts for scalable and sustainable CO_(2)reduction.
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.
