The introduction of SCF2 motif into organic molecules would increases the bioactivity significantly.A silver-catalyzed tandem decarboxylative cyclization of 2,2-difluoro-2-(phenylthio)acetic acids with 2-aryl-N-acryla...The introduction of SCF2 motif into organic molecules would increases the bioactivity significantly.A silver-catalyzed tandem decarboxylative cyclization of 2,2-difluoro-2-(phenylthio)acetic acids with 2-aryl-N-acrylamide indoles is described,furnishing 28 examples of SCF2-substituted indolo[2,1-a]isoquinoline derivatives in moderate to good yields.Mechanistic studies reveal that a radical pathway is proposed in this transformation.展开更多
Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The a...Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The applicability and antimicrobial efficacy of these nanomaterials were systematically investigated for metal ion sensing.Experimental evidence demonstrated that the Ag‑CDs exhibited a pronounced fluorescence quenching response toward ferric ions(Fe^(3+)),enabling their quantitative determination via a linear concentration‑dependent relationship.These Ag‑CDs exhibited significant inhibitory effects on biofilm growth and disruption for both Escherichia coli and Staphylococcus aureus.Mechanism investigations indicate that Ag‑CDs induced the death of Escherichia coli and Pseudomonas aeruginosa by disrupting their bacterial morphology and structure,triggering the generation of intracellular reactive oxygen species(ROS),and impairing their antioxidant defense system.展开更多
Atomically precise silver nanoclusters(AgNCs)offer unique opportunities to correlate structure and photophysical properties,yet enhancing their photoluminescence emission remains challenging due to dominance of non-ra...Atomically precise silver nanoclusters(AgNCs)offer unique opportunities to correlate structure and photophysical properties,yet enhancing their photoluminescence emission remains challenging due to dominance of non-radiative decay pathways.Here,we report a ligand-engineering strategy to modulate the optical properties of high-nuclearity Ag_(56) NCs.The synthesized two NCs,Ag_(56)S_(12)(^(t)BuS)_(20)(CF_(3)CO_(2))_(12)(MeCN)_(3)(NC-I) and Ag_(56)S_(12)(^(t)BuS)_(20)(^(n)BuSO_(3))_(12)(NC-II),possess a similar hexagonal-close-packed Ag_(14) kernel,which is encapsulated by a similar icosahedral S_(12) middle-shell and an outer Ag_(42) shell,but differ in overall symmetry and outer Ag-ligand shell connectivity.Replacement of bidentate CF_(3) CO_(2)^(−)with tridentaten BuSO_(3)^(−) ligands increases overall Ag-X(X=O,S,and Ag)bonding interactions,resulting in not only a more rigid and compact outer Ag_(42) shell structure but also contraction of cationic Ag_(14) core and anionic icosahedral S_(12) middle-shell.These structural modifications enhance radiative decay and suppress non-radiative pathways,leading to a 17-fold increase in photoluminescence quantum yield and extended average emission lifetime.Computational analysis confirms that ligand-induced geometric stabilization and electronic delocalization govern the excited-state dynamics.This work demonstrates that rational ligand design can synergistically tune cluster geometry,rigidity,and electronic structure,providing a general strategy to improve the photophysical performance of high-nuclearity AgNCs.展开更多
The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the...The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the form of S—P bond.The ADD adsorption on argentite and sphalerite surface in Ag^(+)system was revealed by ICP,Zeta potential and XPS analyses.It is shown that the dissolved Ag^(+)from argentite surface can be absorbed on sphalerite surface in the form of silver hydroxide,and AgOH hydrophilic colloid prevents the adsorption of ADD on sphalerite surface.The ADD adsorption on argentite and sphalerite surface in the pulp containing silver and zinc ions was revealed by adsorption capacity and surface wettability analyses.It is shown that the combined Zn(OH)_(2) and AgOH hydrophilic colloid leads to greater ADD adsorption capacity on argentite surface and stronger surface hydrophobicity than sphalerite.Flotation tests demonstrate that ADD enables efficient separation of argentite from sphalerite in the pulp containing silver and zinc ions.展开更多
Electrochromic smart windows(ESWs)can significantly reduce building energy consumption,but the high cost hinders large-scale production.The in situ growth of tungsten oxide(WO_(3))films is only by a simple immersion p...Electrochromic smart windows(ESWs)can significantly reduce building energy consumption,but the high cost hinders large-scale production.The in situ growth of tungsten oxide(WO_(3))films is only by a simple immersion process,the silver nanowires(AgNWs)undergo oxidation to Ag^(+)ions through electron loss,and the liberated electrons provide driving force for the deposition of WO_(4)^(2-).Enabled the fabrication of large-area WO_(3)films and ESWs were fabricated under minimal laboratory conditions,demonstrating the economic feasibility,efficient and reliable nature of industrial production.Structural characterization and density functional theory calculations were combined to confirm that AgNWs effectively regulate oxygen vacancies of WO_(3)films and promote the in situ growth process.The optimized WO_(3)exhibits a maximum transmittance modulation of 90.8%and excellent cycling stability of 20,000 cycles.The largescale WO_(3)-based ESWs can save building energy up to 140.0 MJ m^(-2)compared to traditional windows in tropical regions,as verified by simulations more than40 global cities.This research provides a new approach for improving the performance and industrial production of ESW,providing the full understanding and development direction to short the distance of the ESW commercial production.展开更多
Understanding how genetic variation within forest species influences growth responses under climate change is essential for improving the accuracy of forest models and guiding adaptive management strategies.This study...Understanding how genetic variation within forest species influences growth responses under climate change is essential for improving the accuracy of forest models and guiding adaptive management strategies.This study models the dynamics of Italian silver fir(Abies alba)forests under varying climate change scenarios using the forest gap model FORMIND.Focusing on three distinct silver fir provenances(Western Alps,Northern Apennines,and Southern Apennines),the study simulates forest growth in the Tuscan-Emilian Apennine National Park under different representative concentration pathways(RCPs).The individual-based model FORMIND was parameterized and validated with field data for each of the provenances,demonstrating its ability to accurately reproduce key forest metrics and dynamics.Our results reveal significant differences in expected growth patterns,productivity,metabolism,and carbon storage capacity among the silver fir provenances in pure and mixed stands.In the simulations,the Northern Apennines provenance showed higher biomass production(biomass>10%±1%)and carbon uptake(net primary productivity,NPP>8%±1%)at the end of the century compared to the Western Alps provenance in the pure provenance(PP)and no regeneration scenario.Conversely,the Southern Apennines provenance showed higher biomass(biomass>5%–10%)and NPP(>15%–18%)in mixed provenance(MP)and regeneration scenarios.These results show that genetic diversity strongly affects forest growth and resilience to environmental changes.Hence,it should be included as a predictor variable in forest models.The study also demonstrates the resilience of silver fir to climatic stressors,emphasizing its potential as a robust species in multiple forest contexts.The integration of forest provenance data into the FORMIND model represents a significant advancement in forest modelling,enabling more accurate and reliable predictions under climate change scenarios.The study's findings advocate for a greater understanding and consideration of genetic diversity in forest management and conservation strategies,in support of assisted migration strategies aiming to enhance the resilience of forest ecosystems in a changing climate.展开更多
Traditional strategies for designing hyperhalogens,superatoms with exceptional electron-withdrawing capacity,rely on complex superhalogen assembly,posing significant experimental challenges.Here,we introduce a non-inv...Traditional strategies for designing hyperhalogens,superatoms with exceptional electron-withdrawing capacity,rely on complex superhalogen assembly,posing significant experimental challenges.Here,we introduce a non-invasive dual external field(DEF) approach combining solvent effects and an oriented external electric field(OEEF) to construct hyperhalogens,as demonstrated by density functional theory(DFT) calculations.Our DEF strategy proves versatile,successfully designing hyperhalogens not only in simplified Ag_n^(-) model systems but also in the experimentally synthesized Ag_(25) nanocluster.Using the 3D Ag_(19)^(-) structure as a model,we further reveal the DEF's pivotal role in O_(2) activation,where solvent-OEEF synergy induces tunable O-O bond elongation and charge transfer,proportional to field strength.Our findings establish a field-driven paradigm for hyperhalogen design that preserves native cluster composition,providing a theoretical foundation for tailoring high-performance catalysts through precise activesite modulation.展开更多
The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver n...The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver nanoclusters(Ag NCs),yet the effects of doping mode(surface vs.core)and the interface environment(e.g.,electrolyte concentration)on the electrocatalytic performance for Ag NCs toward GLY oxidation remain understood.In this work,surface-doped Ag_(4)M_(2)(SR)_(8) and core-doped Ag_(24)M(SR)_(18)(M=Ni,Pd,Pt;SR=SPhMe_(2))NCs were synthesized for electrocatalytic GLY oxidation.The results revealed a strong dependence of selectivity on doping mode and electrolyte concentration:under low KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs exhibited 100%selectivity toward oxalic acid(OA),whereas Pd-and Pt-doped Ag_(24)M NCs delivered>95%selectivity for formic acid(FA).In contrast,under high KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs gave rise to>80%FA,while Pd-and Pt-doped Ag_(24)M NCs produced>45%FA.Mechanism studies indicated that Ni doping predominantly enhanced catalytic activity via lowering the activation barrier of the initial reaction step(GLY→glyceraldehyde),whereas Pd and Pt doping modulated selectivity through reducing the energy barrier of the selective branch step(glyceric acid→OA,OA→FA).High KOH concentration promoted the oxidation by increasing the electrochemical active surface area and facilitating electron transfer of Ag NCs.This study provides clear guidance for designing high-performance Ag-based electrocatalysts for biomass valorization.展开更多
The purpose of this study is to explore the motivation,benefits and challenges of the elderly participating in e-sports,especially in the context of global population aging.E-sports has gradually become a growing glob...The purpose of this study is to explore the motivation,benefits and challenges of the elderly participating in e-sports,especially in the context of global population aging.E-sports has gradually become a growing global phenomenon.With the development of science and technology,more and more elderly people begin to participate in digital games to get fun and social interaction opportunities.The goal of the study is to deeply understand the motivation of the elderly to participate in e-sports,explore the cognitive,social and psychological benefits of this activity,and the challenges in the process of participation.Research methods include literature review,qualitative interviews and case studies.Through the analysis of existing research results and cases,we can comprehensively understand the performance and experience of the elderly in E-sports.The results show that the elderly's participation in E-sports can bring significant cognitive benefits,including improving memory,reaction speed and problem solving ability.In addition,E-sports provides a social platform for the elderly,promotes social interaction and emotional connection,and thus improves mental health.However,the elderly also face challenges such as technical barriers,health restrictions and social acceptance in the process of participation.The conclusion part points out that with the arrival of an aging society,Yinfa E-sports has broad prospects for development.Future research can focus on how E-sports can help the elderly cope with loneliness,promote cross generational communication,and how to optimize game design to meet the needs of the elderly.展开更多
Silver nanoparticles(Ag NPs)have attracted attention in the field of biomaterials due to their excellent antibacterial property.However,the reducing and stabilizing agents used for the chemical reduction of Ag NPs are...Silver nanoparticles(Ag NPs)have attracted attention in the field of biomaterials due to their excellent antibacterial property.However,the reducing and stabilizing agents used for the chemical reduction of Ag NPs are usually toxic and may cause water pollution.In this work,Ag NPs(31.2 nm in diameter)were prepared using the extract of straw,an agricultural waste,as the reducing and stabilizing agent.Experimental analysis revealed that the straw extract contained lignin,the structure of which possesses phenolic hydroxyl and methoxy groups that facilitate the reduction of silver salts into Ag NPs.The surfaces of Ag NPs were negatively charged due to the encapsulation of a thin layer of lignin molecules that prevented their aggregation.After the prepared Ag NPs were added to the precursor solution of acrylamide,free radical polymerization was triggered without the need for extra heating or light irradiation,resulting in the rapid formation of an Ag NP-polyacrylamide composite hydrogel.The inhibition zone test proved that the composite hydrogel possessed excellent antibacterial ability due to the presence of Ag NPs.The prepared hydrogel may have potential applications in the fabrication of biomedical materials,such as antibacterial dressings.展开更多
The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge...The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.展开更多
The potent antibacterial activity of silver nanoparticles is primarily attributed to the release of silver ions,which disrupt cell membranes and inactivate essential enzymes through Ag−S bonding formation.[Objective]T...The potent antibacterial activity of silver nanoparticles is primarily attributed to the release of silver ions,which disrupt cell membranes and inactivate essential enzymes through Ag−S bonding formation.[Objective]To explore silver ion immobilization to minimize silver release.[Methods]A macrocyclic cryptand with nitrogen bridgeheads was prepared and subsequently chelated with silver ions to produce Cage silver(I),which was then coordinated with different ratios of sulfonated chitosan(SCS)to form SCS/Cage Ag(I)complexes(SCA1,SCA2,and SCA3).The antioxidant activities of the complexes were assessed by reducing power and 1,1-diphenyl-2-picrylhydrazyl(DPPH)free radical and hydrogen peroxide scavenging assays.The antibacterial activities of the complexes were evaluated based on the minimum inhibitory concentrations(MICs)and minimum bactericidal concentrations(MBCs)against Staphylococcus aureus ATCC 6538 and Escherichia coli O157:H7 and the inhibition rate on biofilm formation.[Results]Cage silver(I)exhibited strong antibacterial activity,with the MIC of 0.015 mg/mL and MBC of 0.031 mg/mL against S.aureus ATCC 6538,and the MIC of 0.031 mg/mL and MBC of 0.120 mg/mL against E.coli O157:H7.Significant antioxidant properties of Cage silver(I)were also observed,as demonstrated by the DPPH free radical scavenging rates of 42.2%and 53.1%at 326 nm and 517 nm,respectively.Cage silver(I)exhibited the highest antibacterial and antioxidant activities,followed by SCA1,SCA2,SCA3,and SCS,because the content of silver ions in Cage silver(I)was 10-fold higher than that in SCA1.The antibacterial and antioxidant activities of SCA1 were better than those of Cage silver(I),which further indicated that the sulfonic groups of SCS may intensely coordinate with silver ions to exert synergistic effects.[Conclusion]Combining the merits of silver ions and SCS improves the bioavailability of the agent at microbicidal concentrations,minimizes the accumulation in the environment,and reduces treatment costs.The method developed herein offers a sustainable approach to enhance microbial control while minimizing the impact on the environment.展开更多
The Zijinshan ore field located in southwestern Fujian Province,China,is a representative porphyry-epithermal ore system hosting diverse mineralization types(Mao et al.,2013).The ore field comprises of the Zijinshan h...The Zijinshan ore field located in southwestern Fujian Province,China,is a representative porphyry-epithermal ore system hosting diverse mineralization types(Mao et al.,2013).The ore field comprises of the Zijinshan highsulfidation Cu-Au deposit,the Luoboling porphyry Cu-Mo deposit,the transitional style Cu deposit(Longjiangting and Wuziqilong)and the Yueyang low-sulfidation Agpolymetallic deposit(Zhang,2013;Zhang et al.,2003)展开更多
As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(H...As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.展开更多
The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is impera...The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is imperative to develop NO_(2)and CO_(2)sensors for ambient conditions,that can be used in indoor air quality monitoring,breath analysis,food spoilage detection,etc.In the present study,two thin film nanocomposite(nickel oxide-graphene and nickel oxide-silver nanowires)gas sensors are fabricated using direct ink writing.The nano-composites are investigated for their structural,optical,and electrical properties.Later the nano-composite is deposited on the interdigitated electrode(IDE)pattern to form NO_(2)and CO_(2)sensors.The deposited films are then exposed to NO_(2)and CO_(2)gases separately and their response and recovery times are determined using a custom-built gas sensing setup.Nickel oxide-graphene provides a good response time and recovery time of 10 and 9 s,respectively for NO_(2),due to the higher electron affinity of graphene towards NO_(2).Nickel oxide-silver nanowire nano-composite is suited for CO_(2)gas because silver is an excellent electrocatalyst for CO_(2)by giving response and recovery times of 11 s each.This is the first report showcasing NiO nano-composites for NO_(2)and CO_(2)sensing at room temperature.展开更多
Silver paste is widely used in power electronics as a die-attach material owing to its low-temperature sinterability,high melting point,and excellent electrical and thermal conductivities in sintered joints.However,ow...Silver paste is widely used in power electronics as a die-attach material owing to its low-temperature sinterability,high melting point,and excellent electrical and thermal conductivities in sintered joints.However,owing to the mismatch in the coefficient of thermal expansion(CTE)between the joints and chip,the high Young's modulus of sintered silver hinders the mitigation of the high thermal stress generated during the operation of power modules,which increases the susceptibility of sintered joints to cracking,thereby leading to potential failure.This study developed a facile approach to synthesizing bayberry-like Ag microparticles(AgMPs)through the in situ assembly of silver nanorods,resulting in a uniform distribution of nanoscale structures and mesopores on the particle surface.These particles exhibited a high specific surface area of 2.5389 m^(2)·g^(-1),which enhanced theirsintering activity,enabling sintering to occur at 149.7℃.Furthermore,the porous structure of the AgMPs effectively reduced the density of joints formed by sintering AgMP paste,thereby lowering the Young's modulus of the joints.The small grain size and intricate internal substructure of the joints yielded high shear strength,which reached112.50 MPa at 250℃.The Young's modulus could be adjusted,and the pores provided by the AgMPs maintained the Young's modulus within a low range(15.11-29.61GPa),effectively mitigating thermal stress.These new bayberry-like porous AgMPs offer a promising option for die-attach materials in electronic packaging.展开更多
2024年6月10日,《自然·通讯》(Nature Communications)在线发表了重庆大学光电工程学院臧志刚教授团队题为“Silver Coordination-Induced n-Doping of PCBM Enables Highly Efficient and Stable Inverted Perovskite Solar Cell...2024年6月10日,《自然·通讯》(Nature Communications)在线发表了重庆大学光电工程学院臧志刚教授团队题为“Silver Coordination-Induced n-Doping of PCBM Enables Highly Efficient and Stable Inverted Perovskite Solar Cells”的研究成果。该团队提出了一种银配位诱导的n型掺杂策略,成功解决了钙钛矿太阳能电池中卤化物与银电极的双向迁移问题,为提升器件长期稳定性提供了创新性解决方案。钙钛矿太阳能电池因其高效率和低成本成为光伏领域的研究热点,但卤化物离子(如碘)与银电极的不可逆化学腐蚀严重制约其实际应用。展开更多
Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMO...Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMOS)technology still suffer from substantially larger energy consumption than biological synapses,due to the slow kinetics of forming conductive paths inside the memristive units.Here we report wafer-scale Ag_(2)S-based MCAs realized using CMOS-compatible processes at temperatures below 160℃.Ag_(2)S electrolytes supply highly mobile Ag+ions,and provide the Ag/Ag_(2)S interface with low silver nucleation barrier to form silver filaments at low energy costs.By further enhancing Ag+migration in Ag_(2)S electrolytes via microstructure modulation,the integrated memristors exhibit a record low threshold of approximately−0.1 V,and demonstrate ultra-low switching-energies reaching femtojoule values as observed in biological synapses.The low-temperature process also enables MCA integration on polyimide substrates for applications in flexible electronics.Moreover,the intrinsic nonidealities of the memristive units for deep learning can be compensated by employing an advanced training algorithm.An impressive accuracy of 92.6%in image recognition simulations is demonstrated with the MCAs after the compensation.The demonstrated MCAs provide a promising device option for neuromorphic computing with ultra-high energy-efficiency.展开更多
A Silver-catalyzed enantioselective[3+2]cycloaddition of azomethine ylides with activated alkenes by using a P-stereogenic ligand Ganphos is reported.The method provides an efficient strategy for the effective synthes...A Silver-catalyzed enantioselective[3+2]cycloaddition of azomethine ylides with activated alkenes by using a P-stereogenic ligand Ganphos is reported.The method provides an efficient strategy for the effective synthesis of spirocyclic scaffolds containing a pyrroline motif.Notable features of this approach include good yields,remarkable enantioselectivity,as well as a broad substrate scope and significant step efficiency.展开更多
文摘The introduction of SCF2 motif into organic molecules would increases the bioactivity significantly.A silver-catalyzed tandem decarboxylative cyclization of 2,2-difluoro-2-(phenylthio)acetic acids with 2-aryl-N-acrylamide indoles is described,furnishing 28 examples of SCF2-substituted indolo[2,1-a]isoquinoline derivatives in moderate to good yields.Mechanistic studies reveal that a radical pathway is proposed in this transformation.
文摘Herein,antibacterial silver‑doped fluorescent carbon dots(Ag‑CDs)were synthesized through a stepwise hydrothermal method,with polyethyleneimine(PEI),citric acid(CA),and silver nitrate(AgNO3)serving as precursors.The applicability and antimicrobial efficacy of these nanomaterials were systematically investigated for metal ion sensing.Experimental evidence demonstrated that the Ag‑CDs exhibited a pronounced fluorescence quenching response toward ferric ions(Fe^(3+)),enabling their quantitative determination via a linear concentration‑dependent relationship.These Ag‑CDs exhibited significant inhibitory effects on biofilm growth and disruption for both Escherichia coli and Staphylococcus aureus.Mechanism investigations indicate that Ag‑CDs induced the death of Escherichia coli and Pseudomonas aeruginosa by disrupting their bacterial morphology and structure,triggering the generation of intracellular reactive oxygen species(ROS),and impairing their antioxidant defense system.
基金support of the JSPS KAKENHI(Grant Numbers 23H00289 and 22K19012)Scientific Research on Innovative Areas“Aquatic Functional Materials”(Grant Number 22H04562)+2 种基金the Yazaki Memorial Foundation for Science and Technology,and the Ogasawara Foundation for the Promotion of Science and Engineeringsupport from the JSPS grant(Transformative Research Areas[A],22H05133,22H05131)for M.E.,the JSPS grant(21J00210)for T.S.the JSPS grant(24K17663)for P.Z.The computations were partly performed at the Research Center for Computational Science,Okazaki,Japan(24-IMS-C194 and 25-IMS-C224).
文摘Atomically precise silver nanoclusters(AgNCs)offer unique opportunities to correlate structure and photophysical properties,yet enhancing their photoluminescence emission remains challenging due to dominance of non-radiative decay pathways.Here,we report a ligand-engineering strategy to modulate the optical properties of high-nuclearity Ag_(56) NCs.The synthesized two NCs,Ag_(56)S_(12)(^(t)BuS)_(20)(CF_(3)CO_(2))_(12)(MeCN)_(3)(NC-I) and Ag_(56)S_(12)(^(t)BuS)_(20)(^(n)BuSO_(3))_(12)(NC-II),possess a similar hexagonal-close-packed Ag_(14) kernel,which is encapsulated by a similar icosahedral S_(12) middle-shell and an outer Ag_(42) shell,but differ in overall symmetry and outer Ag-ligand shell connectivity.Replacement of bidentate CF_(3) CO_(2)^(−)with tridentaten BuSO_(3)^(−) ligands increases overall Ag-X(X=O,S,and Ag)bonding interactions,resulting in not only a more rigid and compact outer Ag_(42) shell structure but also contraction of cationic Ag_(14) core and anionic icosahedral S_(12) middle-shell.These structural modifications enhance radiative decay and suppress non-radiative pathways,leading to a 17-fold increase in photoluminescence quantum yield and extended average emission lifetime.Computational analysis confirms that ligand-induced geometric stabilization and electronic delocalization govern the excited-state dynamics.This work demonstrates that rational ligand design can synergistically tune cluster geometry,rigidity,and electronic structure,providing a general strategy to improve the photophysical performance of high-nuclearity AgNCs.
基金the support from the National Key Research and Development Program of China (No. 2022YFC2904504)the Science and Technology Research Project of Jiangxi Provincial Department of Education, China (No. GJJ2200864)the Gansu Provincial Key Research and Development Project, China (No. 22YF7GA073)。
文摘The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the form of S—P bond.The ADD adsorption on argentite and sphalerite surface in Ag^(+)system was revealed by ICP,Zeta potential and XPS analyses.It is shown that the dissolved Ag^(+)from argentite surface can be absorbed on sphalerite surface in the form of silver hydroxide,and AgOH hydrophilic colloid prevents the adsorption of ADD on sphalerite surface.The ADD adsorption on argentite and sphalerite surface in the pulp containing silver and zinc ions was revealed by adsorption capacity and surface wettability analyses.It is shown that the combined Zn(OH)_(2) and AgOH hydrophilic colloid leads to greater ADD adsorption capacity on argentite surface and stronger surface hydrophobicity than sphalerite.Flotation tests demonstrate that ADD enables efficient separation of argentite from sphalerite in the pulp containing silver and zinc ions.
基金the National Natural Science Foundation of China(grant No.52163022,62305076)Sichuan Science and Technology Program(2024ZYD0196)+1 种基金China Postdoctoral Science Foundation(2023M740505)Sichuan Postdoctoral Science Special Foundation(No.TB2023010)。
文摘Electrochromic smart windows(ESWs)can significantly reduce building energy consumption,but the high cost hinders large-scale production.The in situ growth of tungsten oxide(WO_(3))films is only by a simple immersion process,the silver nanowires(AgNWs)undergo oxidation to Ag^(+)ions through electron loss,and the liberated electrons provide driving force for the deposition of WO_(4)^(2-).Enabled the fabrication of large-area WO_(3)films and ESWs were fabricated under minimal laboratory conditions,demonstrating the economic feasibility,efficient and reliable nature of industrial production.Structural characterization and density functional theory calculations were combined to confirm that AgNWs effectively regulate oxygen vacancies of WO_(3)films and promote the in situ growth process.The optimized WO_(3)exhibits a maximum transmittance modulation of 90.8%and excellent cycling stability of 20,000 cycles.The largescale WO_(3)-based ESWs can save building energy up to 140.0 MJ m^(-2)compared to traditional windows in tropical regions,as verified by simulations more than40 global cities.This research provides a new approach for improving the performance and industrial production of ESW,providing the full understanding and development direction to short the distance of the ESW commercial production.
基金the University of Milan for funding the“ProForesta”project through the 2020 Research Support Planthe“Ente Parco Nazionale dell'Appennino Tosco-Emiliano”for having financed the project“First urgent measures to promote the adaptation of the silver fir forests of the Tuscan-Emilian Apennine National Park to the effects of climate change”。
文摘Understanding how genetic variation within forest species influences growth responses under climate change is essential for improving the accuracy of forest models and guiding adaptive management strategies.This study models the dynamics of Italian silver fir(Abies alba)forests under varying climate change scenarios using the forest gap model FORMIND.Focusing on three distinct silver fir provenances(Western Alps,Northern Apennines,and Southern Apennines),the study simulates forest growth in the Tuscan-Emilian Apennine National Park under different representative concentration pathways(RCPs).The individual-based model FORMIND was parameterized and validated with field data for each of the provenances,demonstrating its ability to accurately reproduce key forest metrics and dynamics.Our results reveal significant differences in expected growth patterns,productivity,metabolism,and carbon storage capacity among the silver fir provenances in pure and mixed stands.In the simulations,the Northern Apennines provenance showed higher biomass production(biomass>10%±1%)and carbon uptake(net primary productivity,NPP>8%±1%)at the end of the century compared to the Western Alps provenance in the pure provenance(PP)and no regeneration scenario.Conversely,the Southern Apennines provenance showed higher biomass(biomass>5%–10%)and NPP(>15%–18%)in mixed provenance(MP)and regeneration scenarios.These results show that genetic diversity strongly affects forest growth and resilience to environmental changes.Hence,it should be included as a predictor variable in forest models.The study also demonstrates the resilience of silver fir to climatic stressors,emphasizing its potential as a robust species in multiple forest contexts.The integration of forest provenance data into the FORMIND model represents a significant advancement in forest modelling,enabling more accurate and reliable predictions under climate change scenarios.The study's findings advocate for a greater understanding and consideration of genetic diversity in forest management and conservation strategies,in support of assisted migration strategies aiming to enhance the resilience of forest ecosystems in a changing climate.
基金supported by the National Natural Science Foundation of China (NSFC,Nos.12474274,92161101)the Innovation Project of Jinan Science and Technology Bureau(No.2021GXRC032)the Natural Science Foundation of Shandong Province (No.ZR2024MA091)。
文摘Traditional strategies for designing hyperhalogens,superatoms with exceptional electron-withdrawing capacity,rely on complex superhalogen assembly,posing significant experimental challenges.Here,we introduce a non-invasive dual external field(DEF) approach combining solvent effects and an oriented external electric field(OEEF) to construct hyperhalogens,as demonstrated by density functional theory(DFT) calculations.Our DEF strategy proves versatile,successfully designing hyperhalogens not only in simplified Ag_n^(-) model systems but also in the experimentally synthesized Ag_(25) nanocluster.Using the 3D Ag_(19)^(-) structure as a model,we further reveal the DEF's pivotal role in O_(2) activation,where solvent-OEEF synergy induces tunable O-O bond elongation and charge transfer,proportional to field strength.Our findings establish a field-driven paradigm for hyperhalogen design that preserves native cluster composition,providing a theoretical foundation for tailoring high-performance catalysts through precise activesite modulation.
基金support from the Jiangsu Natural Science Foundation of China(BK20230329)the National Natural Science Foundation of China(22401147,22361132540,and 22178161)the Russian Science Foundation(23-73-30007).
文摘The efficient electrocatalytic oxidation of glycerol(GLY)is one of the most promising routes for the valorization of GLY.Doping has emerged as a powerful strategy to tailor the electrocatalytic performance of silver nanoclusters(Ag NCs),yet the effects of doping mode(surface vs.core)and the interface environment(e.g.,electrolyte concentration)on the electrocatalytic performance for Ag NCs toward GLY oxidation remain understood.In this work,surface-doped Ag_(4)M_(2)(SR)_(8) and core-doped Ag_(24)M(SR)_(18)(M=Ni,Pd,Pt;SR=SPhMe_(2))NCs were synthesized for electrocatalytic GLY oxidation.The results revealed a strong dependence of selectivity on doping mode and electrolyte concentration:under low KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs exhibited 100%selectivity toward oxalic acid(OA),whereas Pd-and Pt-doped Ag_(24)M NCs delivered>95%selectivity for formic acid(FA).In contrast,under high KOH concentration,Pd-and Pt-doped Ag_(4)M_(2) NCs gave rise to>80%FA,while Pd-and Pt-doped Ag_(24)M NCs produced>45%FA.Mechanism studies indicated that Ni doping predominantly enhanced catalytic activity via lowering the activation barrier of the initial reaction step(GLY→glyceraldehyde),whereas Pd and Pt doping modulated selectivity through reducing the energy barrier of the selective branch step(glyceric acid→OA,OA→FA).High KOH concentration promoted the oxidation by increasing the electrochemical active surface area and facilitating electron transfer of Ag NCs.This study provides clear guidance for designing high-performance Ag-based electrocatalysts for biomass valorization.
文摘The purpose of this study is to explore the motivation,benefits and challenges of the elderly participating in e-sports,especially in the context of global population aging.E-sports has gradually become a growing global phenomenon.With the development of science and technology,more and more elderly people begin to participate in digital games to get fun and social interaction opportunities.The goal of the study is to deeply understand the motivation of the elderly to participate in e-sports,explore the cognitive,social and psychological benefits of this activity,and the challenges in the process of participation.Research methods include literature review,qualitative interviews and case studies.Through the analysis of existing research results and cases,we can comprehensively understand the performance and experience of the elderly in E-sports.The results show that the elderly's participation in E-sports can bring significant cognitive benefits,including improving memory,reaction speed and problem solving ability.In addition,E-sports provides a social platform for the elderly,promotes social interaction and emotional connection,and thus improves mental health.However,the elderly also face challenges such as technical barriers,health restrictions and social acceptance in the process of participation.The conclusion part points out that with the arrival of an aging society,Yinfa E-sports has broad prospects for development.Future research can focus on how E-sports can help the elderly cope with loneliness,promote cross generational communication,and how to optimize game design to meet the needs of the elderly.
基金financially supported by the National Natural Science Foundation of China(No.52203209)the State Key Laboratory of Solid Waste Reuse for Building Materials,China(No.SWR-2022-009)the Fundamental Research Funds for the Central Universities,China(No.FRF-IDRY22-012)。
文摘Silver nanoparticles(Ag NPs)have attracted attention in the field of biomaterials due to their excellent antibacterial property.However,the reducing and stabilizing agents used for the chemical reduction of Ag NPs are usually toxic and may cause water pollution.In this work,Ag NPs(31.2 nm in diameter)were prepared using the extract of straw,an agricultural waste,as the reducing and stabilizing agent.Experimental analysis revealed that the straw extract contained lignin,the structure of which possesses phenolic hydroxyl and methoxy groups that facilitate the reduction of silver salts into Ag NPs.The surfaces of Ag NPs were negatively charged due to the encapsulation of a thin layer of lignin molecules that prevented their aggregation.After the prepared Ag NPs were added to the precursor solution of acrylamide,free radical polymerization was triggered without the need for extra heating or light irradiation,resulting in the rapid formation of an Ag NP-polyacrylamide composite hydrogel.The inhibition zone test proved that the composite hydrogel possessed excellent antibacterial ability due to the presence of Ag NPs.The prepared hydrogel may have potential applications in the fabrication of biomedical materials,such as antibacterial dressings.
文摘The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.
文摘The potent antibacterial activity of silver nanoparticles is primarily attributed to the release of silver ions,which disrupt cell membranes and inactivate essential enzymes through Ag−S bonding formation.[Objective]To explore silver ion immobilization to minimize silver release.[Methods]A macrocyclic cryptand with nitrogen bridgeheads was prepared and subsequently chelated with silver ions to produce Cage silver(I),which was then coordinated with different ratios of sulfonated chitosan(SCS)to form SCS/Cage Ag(I)complexes(SCA1,SCA2,and SCA3).The antioxidant activities of the complexes were assessed by reducing power and 1,1-diphenyl-2-picrylhydrazyl(DPPH)free radical and hydrogen peroxide scavenging assays.The antibacterial activities of the complexes were evaluated based on the minimum inhibitory concentrations(MICs)and minimum bactericidal concentrations(MBCs)against Staphylococcus aureus ATCC 6538 and Escherichia coli O157:H7 and the inhibition rate on biofilm formation.[Results]Cage silver(I)exhibited strong antibacterial activity,with the MIC of 0.015 mg/mL and MBC of 0.031 mg/mL against S.aureus ATCC 6538,and the MIC of 0.031 mg/mL and MBC of 0.120 mg/mL against E.coli O157:H7.Significant antioxidant properties of Cage silver(I)were also observed,as demonstrated by the DPPH free radical scavenging rates of 42.2%and 53.1%at 326 nm and 517 nm,respectively.Cage silver(I)exhibited the highest antibacterial and antioxidant activities,followed by SCA1,SCA2,SCA3,and SCS,because the content of silver ions in Cage silver(I)was 10-fold higher than that in SCA1.The antibacterial and antioxidant activities of SCA1 were better than those of Cage silver(I),which further indicated that the sulfonic groups of SCS may intensely coordinate with silver ions to exert synergistic effects.[Conclusion]Combining the merits of silver ions and SCS improves the bioavailability of the agent at microbicidal concentrations,minimizes the accumulation in the environment,and reduces treatment costs.The method developed herein offers a sustainable approach to enhance microbial control while minimizing the impact on the environment.
基金financially supported by Zijin Mining Group(No.01612216)the Ministry of Natural Resources,China(No.ZKKJ202426)。
文摘The Zijinshan ore field located in southwestern Fujian Province,China,is a representative porphyry-epithermal ore system hosting diverse mineralization types(Mao et al.,2013).The ore field comprises of the Zijinshan highsulfidation Cu-Au deposit,the Luoboling porphyry Cu-Mo deposit,the transitional style Cu deposit(Longjiangting and Wuziqilong)and the Yueyang low-sulfidation Agpolymetallic deposit(Zhang,2013;Zhang et al.,2003)
基金supported by the National Research Foundation(NRF)of Korea,funded by the Korean Government(MSIT)(Grant No.RS-2023-00240043).
文摘As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.
文摘The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is imperative to develop NO_(2)and CO_(2)sensors for ambient conditions,that can be used in indoor air quality monitoring,breath analysis,food spoilage detection,etc.In the present study,two thin film nanocomposite(nickel oxide-graphene and nickel oxide-silver nanowires)gas sensors are fabricated using direct ink writing.The nano-composites are investigated for their structural,optical,and electrical properties.Later the nano-composite is deposited on the interdigitated electrode(IDE)pattern to form NO_(2)and CO_(2)sensors.The deposited films are then exposed to NO_(2)and CO_(2)gases separately and their response and recovery times are determined using a custom-built gas sensing setup.Nickel oxide-graphene provides a good response time and recovery time of 10 and 9 s,respectively for NO_(2),due to the higher electron affinity of graphene towards NO_(2).Nickel oxide-silver nanowire nano-composite is suited for CO_(2)gas because silver is an excellent electrocatalyst for CO_(2)by giving response and recovery times of 11 s each.This is the first report showcasing NiO nano-composites for NO_(2)and CO_(2)sensing at room temperature.
基金financially supported by the National Natural Science Foundation of China(Nos.52075125 and 52105331)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010591)Shenzhen Science and Technology Innovation Committee(Nos.JCYJ20210324124203009,JSGG20201102154600003,GXWD20231130103814001,GXWD20220721182229001)
文摘Silver paste is widely used in power electronics as a die-attach material owing to its low-temperature sinterability,high melting point,and excellent electrical and thermal conductivities in sintered joints.However,owing to the mismatch in the coefficient of thermal expansion(CTE)between the joints and chip,the high Young's modulus of sintered silver hinders the mitigation of the high thermal stress generated during the operation of power modules,which increases the susceptibility of sintered joints to cracking,thereby leading to potential failure.This study developed a facile approach to synthesizing bayberry-like Ag microparticles(AgMPs)through the in situ assembly of silver nanorods,resulting in a uniform distribution of nanoscale structures and mesopores on the particle surface.These particles exhibited a high specific surface area of 2.5389 m^(2)·g^(-1),which enhanced theirsintering activity,enabling sintering to occur at 149.7℃.Furthermore,the porous structure of the AgMPs effectively reduced the density of joints formed by sintering AgMP paste,thereby lowering the Young's modulus of the joints.The small grain size and intricate internal substructure of the joints yielded high shear strength,which reached112.50 MPa at 250℃.The Young's modulus could be adjusted,and the pores provided by the AgMPs maintained the Young's modulus within a low range(15.11-29.61GPa),effectively mitigating thermal stress.These new bayberry-like porous AgMPs offer a promising option for die-attach materials in electronic packaging.
文摘2024年6月10日,《自然·通讯》(Nature Communications)在线发表了重庆大学光电工程学院臧志刚教授团队题为“Silver Coordination-Induced n-Doping of PCBM Enables Highly Efficient and Stable Inverted Perovskite Solar Cells”的研究成果。该团队提出了一种银配位诱导的n型掺杂策略,成功解决了钙钛矿太阳能电池中卤化物与银电极的双向迁移问题,为提升器件长期稳定性提供了创新性解决方案。钙钛矿太阳能电池因其高效率和低成本成为光伏领域的研究热点,但卤化物离子(如碘)与银电极的不可逆化学腐蚀严重制约其实际应用。
基金supported by the Swedish Strategic Research Foundation(SSF FFL15-0174 to Zhen Zhang)the Swedish Research Council(VR 2018-06030 and 2019-04690 to Zhen Zhang)+1 种基金the Wallenberg Academy Fellow Extension Program(KAW 2020-0190 to Zhen Zhang)the Olle Engkvist Foundation(Postdoc grant 214-0322 to Zhen Zhang).
文摘Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic computing.However,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMOS)technology still suffer from substantially larger energy consumption than biological synapses,due to the slow kinetics of forming conductive paths inside the memristive units.Here we report wafer-scale Ag_(2)S-based MCAs realized using CMOS-compatible processes at temperatures below 160℃.Ag_(2)S electrolytes supply highly mobile Ag+ions,and provide the Ag/Ag_(2)S interface with low silver nucleation barrier to form silver filaments at low energy costs.By further enhancing Ag+migration in Ag_(2)S electrolytes via microstructure modulation,the integrated memristors exhibit a record low threshold of approximately−0.1 V,and demonstrate ultra-low switching-energies reaching femtojoule values as observed in biological synapses.The low-temperature process also enables MCA integration on polyimide substrates for applications in flexible electronics.Moreover,the intrinsic nonidealities of the memristive units for deep learning can be compensated by employing an advanced training algorithm.An impressive accuracy of 92.6%in image recognition simulations is demonstrated with the MCAs after the compensation.The demonstrated MCAs provide a promising device option for neuromorphic computing with ultra-high energy-efficiency.
文摘A Silver-catalyzed enantioselective[3+2]cycloaddition of azomethine ylides with activated alkenes by using a P-stereogenic ligand Ganphos is reported.The method provides an efficient strategy for the effective synthesis of spirocyclic scaffolds containing a pyrroline motif.Notable features of this approach include good yields,remarkable enantioselectivity,as well as a broad substrate scope and significant step efficiency.
