This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the...This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the research field of one-carbon(C1)chemistry,including catalytic conversion of C1 molecules to valuable chemicals and superclean fuels,innovative catalyst and reactor development,and the design of new catalytic reactions and processes.Organized chronologically,this review highlights Prof.Tsubaki’s academic contributions from 1990,when he studied and worked at The University of Tokyo,to his current role as a full professor at the University of Toyama.The academic section of this review is divided into three main parts,focusing on Prof.Tsubaki’s pioneering work in C1 chemistry.We believe that this review will serve as a highly valuable reference for colleagues in the fields of C1 chemistry and catalysis,and inspire the development of more original and groundbreaking research.展开更多
Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of...Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of polyfluoroarenes with alkyl halides under mild conditions is reported.Polyfluoroarenes(3~6 F)can reacted smoothly with a diverse range of alkyl halides,such as primary,secondary,and tertiary alkyl iodides.The efficient formation of C(sp2)—C(sp3)can be achieved through the combination of Ni catalysis and(Bpin)2/K2CO3 as terminal reductant.展开更多
The exsolution method has garnered significant attention owing to its high efficacy in developing highly efficient and stable metal nanocatalysts.Herein,a versatile exsolution approach is developed to embed size-tunab...The exsolution method has garnered significant attention owing to its high efficacy in developing highly efficient and stable metal nanocatalysts.Herein,a versatile exsolution approach is developed to embed size-tunable metal nanocatalysts within a conductive metal pnictogenide matrix.The gas-phase reaction of Ru-substituted Ni-Fe-layered-double-hydroxide(Ni_(2)Fe_(1-x)Ru_(x)-LDH)with pnictogenation reagents leads to the exsolution of Ru metal nanocatalysts and a phase transformation into metal pnictogenide.The variation in reactivity of pnictogenation reagents allows for control over the size of the exsolved metal nanocatalysts(i.e.,nanoclusters for nitridation and single atoms for phosphidation),underscoring the effectiveness of the pnictogenation-driven exsolution strategy in stabilizing size-tunable metal nanocatalysts.The Ru-exsolved nickel-iron nitride/phosphide demonstrates outstanding electrocatalyst activity for the hydrogen evolution reaction,exhibiting a smaller overpotential and higher stability than Ru-deposited homologs.The high efficacy of pnictogenation-assisted exsolution in optimizing the performance and stability of Ru metal nanocatalysts is ascribed to the efficient interfacial electronic interaction between Ru metals and nitride/phosphide ions assisted by the inner sphere mechanism.In situ spectroscopic analyses highlight that exsolved Ru single atoms facilitate more efficient electron transfer to the reactants than the exsolved Ru nanoclusters,which is primarily responsible for the superior impact of the phosphidation-driven exsolution approach.展开更多
Background:Chaetomorpha aerea,a marine green alga,has drawn attention because of its rich phytochemical constituents and therapeutic benefits.Using an integrated approach that combined in vitro,in vivo,and in silico a...Background:Chaetomorpha aerea,a marine green alga,has drawn attention because of its rich phytochemical constituents and therapeutic benefits.Using an integrated approach that combined in vitro,in vivo,and in silico approaches,this work examined the antioxidant,anti-inflammatory,and antidiabetic qualities of acetone extract of C.aerea(AECA).Methods:Total phenolic and flavonoid concentrations of AECA were measured.Antioxidant activity was assessed using the DPPH and ABTS free radical scavenging assays.In vitro protein denaturation and in vivo carrageenan-induced paw edema models were employed to evaluate the anti-inflammatory potential,whereas antidiabetic activity was assessed using in vitroα-amylase inhibition and in vivo oral glucose tolerance test(OGTT).Molecular docking and ADME/T analysis were employed to further analyze bioactive compounds identified using gas chromatography–mass spectrometry(GC–MS).Result:Antioxidant activity demonstrated a minimum inhibitory concentration(IC_(50))of 107.44μg/mL for DPPH and 118.23μg/mL for ABTS.In vitro anti-inflammatory assays indicated a suppression of protein denaturation at a concentration of 102μg/mL(IC_(50)),where AECA(400 mg/kg)resulted in a 27%reduction in paw edema at 6 h in the mouse model.In vitro antidiabetic test indicatedα-amylase inhibition with an IC_(50) value of 70.72μg/mL,and in the OGTT,a significant lowering of blood glucose was recorded at 120 min in mice.Strong binding affinities were observed for stigmasta-5,24(28)-dien-3-ol,identified using GC–MS,with values of−9.9 kcal/mol forα-amylase and−8.0 kcal/mol for cyclooxygenase-2.Conclusion:C.aerea serves as an effective natural remedy for oxidative stress,inflammation,and hyperglycemia.These findings advocate for further clinical and mechanistic investigations to optimize therapeutic efficacy.展开更多
The persistence of chlorinated alkanes in aquatic environments poses significant health risks due to its biotoxicity and high volatility,which contributes to both water and air pollution.This study investigates the ef...The persistence of chlorinated alkanes in aquatic environments poses significant health risks due to its biotoxicity and high volatility,which contributes to both water and air pollution.This study investigates the efficacy of carbon dioxide radical anion(CO_(2)·^(-))mediated advanced reduction processes(ARPs)for the reductive dechlorination of chlorinated alkanes using small molecular monocarboxylic acids(SMAs)under UV irradiation.The study focused on formic acid(HCOOH),acetic acid(CH_3COOH),and propionic acid(CH_3CH_(2)COOH)to generate CO_(2)·^(-),revealing that UV/HCOOH system exhibits a notably high chloroform(CF)degradation efficiency of 97.8%in 90 min.Kinetic studies indicated a linear relationship between the HCOOH concentrations and the observed reaction rate constants(k_(obs)),demonstrating that CO_(2)·^(-)production is crucial for CF degradation.Electron paramagnetic resonance spectroscopy identified CO_(2)·^(-)and hydroxyl radicals(HO·)as the active species,with the former playing a predominant role in CF degradation.The study also explored the influence of carbon chain length in SMAs on CF degradation,finding that longer chains decrease the degradation efficiency,potentially due to reduced UV activation.A higher reaction rate constant(k_(obs))under acidic conditions,with a marked decrease in efficiency as the pH exceeds 3.7,where HCOO^(-)becomes predominant.This study enhances our understanding of CO_(2)·^(-)mediated ARPs and explores potential applications in environmental remediation,providing insights into the pathways and mechanisms of CF degradation.The UV/SMAs systems offer advantages for practical applications,such as milder reaction conditions and higher efficiency compared to traditional methods.展开更多
This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due ...This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due to their distinct active sites and superior catalytic efficacy,found their applications in the fields of energy conversion and environmental protection.The review elaborated on the potential carriers,preparation methods,and characterization techniques for single-atom photocatalysts.Subsequently,the article provided an in-depth explanation of the crucial role of H_(2)O in photocatalytic reactions,serving as an important green solvent and an oxygen/proton source.The adsorption of water could also change the surface energy structure and charge distribution of the photocatalyst.Conversely,the presence of H_(2)O might also inhibit the target reaction.Additionally,the distinct roles of water in both liquid and gas phases were discussed.Furthermore,the review systematically summarized the applications of single-atom photocatalysts in H_(2)generation,CO_(2)reduction,N2fixation,H_(2)O_(2)production,and environmentalremediation.It delved into the mechanisms by which water molecules participated in photocatalytic processes and their interactions with competing pathways,thereby revealing the complexity and critical importance of water in photocatalytic reactions.Finally,the article discusses the opportunities and challenges of SACs in photocatalytic reactions with H_(2)O.This article provides a comprehensive perspective for understanding the role of SACs in waterinvolved photocatalytic reactions.展开更多
Enhancing the output capacity of semiconductor bridge(SCB) through the application of composite nano-energetic films is a subject of wide concern. Furthermore, improving the safety, reliability, and production efficie...Enhancing the output capacity of semiconductor bridge(SCB) through the application of composite nano-energetic films is a subject of wide concern. Furthermore, improving the safety, reliability, and production efficiency of energetic semiconductor bridge(ESCB) is the primary focus for large-scale engineering applications in the future. Here, the Al/CuO nano-film ESCB was efficiently fabricated using 3D direct writing. The electrostatic safety of the film is enhanced by precisely adjusting the particle size of Al, while ensuring that the SCB can initiate the film with small energy. The burst characteristics of SCB/ESCB were thoroughly investigated by employing a 100 μF tantalum capacitor to induce SCB and ESCB under an intense voltage gradient. The solid-state heating process of both SCB and ESCB was analyzed with multi physical simulation(MPS). The experimental results demonstrate that the critical burst time of both SCB and ESCB decreases with increasing voltage. Under the same voltage, the critical burst time of ESCB is longer than that of SCB, primarily due to differences in the melting to vaporization stage. The MPS results indicate that the highest temperature is observed at the V-shaped corner of SCB. Due to the thermal contact resistance between SCB and the film, heat conduction becomes more concentrated in the central region of the bridge, resulting in a faster solid-state heating process for ESCB compared to SCB.The results of the gap ignition experiments indicate that at a 19 mm gap, an ESCB with a film mass of 10 mg can ignite nickel hydrazine nitrate(NHN) and cyclotrimethylenetrinitramine(RDX). This suggests that thermite ESCB can serve as a novel, safe, and reliable energy exchange element and initiator in largescale engineering applications.展开更多
In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the ...In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the Ce-OFDC matrix,forming a CeOFDC/PCN composite material.Antibacterial assays demonstrated that Ce-OFDC/PCN had significant inhibitory effects on both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus),achieving inhibition rates of 99.5%and 94.3%,respectively.Notably,the antibacterial performance of Ce-OFDC/PCN was superior to that of Ce-OFDC or PCN alone.Furthermore,photocurrent and electrical impedance scanning measurements demonstrated that the Ce-OFDC/PCN composites showed improved photocurrent response and superior efficiency in separating photogenerated electrons and holes.The photocurrent density of Ce-OFDC/PCN reached 120μA cm^(-2),which was 1.5 times higher than that of PCN(80μA cm^(-2))and 12 times higher than that of Ce-OFDC(10μA cm^(-2)).Electron paramagnetic resonance analysis indicated that reactive oxygen species played a crucial role in the antimicrobial process,with super oxide radicals(·O_(2)^(-))and hydroxyl radical(·OH)showing the most prominent influence.We conducted reactive oxygen species(ROS)scavenging experiments to further confirm this view.After adding glutathione(GSH)to remove all ROS,the antibacterial efficiency of Ce-OFDC/PCN decreased by about 40%.Adding D-mannitol to remove·OH reduced the inhibition rate to 54.7%,and adding superoxide dismutase(SOD)to remove·O_(2)^(-)reduced the inhibition rate to 65.4%.The Ce-OFDC/PCN heterostructure increased the separation efficiency of photogenerated electrons and holes,producing increased reactive oxygen species.That,in turn,contributed to the observed superior photocatalytic antibacterial performance.This research significantly advanced the development of metal-organic framework(MOF)-based materials and provided valuable insights into the design of antimicrobial photocatalysts.展开更多
Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to th...Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.展开更多
Proton exchange membranes(PEMs)are widely employed in energy conversion and storage devices including fuel cells(FCs),redox flow batteries(RFBs)and PEM water electrolysis(PEMWE).As one of the main components of these ...Proton exchange membranes(PEMs)are widely employed in energy conversion and storage devices including fuel cells(FCs),redox flow batteries(RFBs)and PEM water electrolysis(PEMWE).As one of the main components of these devices,a high-performance PEM is always desirable considering the cost challenges from both energy utilization efficiency and production cost.From this century,governments of countries worldwide have introduced PFAS(per-and polyfluoroalkyl substances)restriction related policies,which facilitate the extensive research on non-fluorinated PEMs.Besides,non-fluorinated PEMs become hot topics of all kinds of PEMs due to the advantages including excellent conductivity,high mechanical property,reduced swelling,low cost and reduced ion permeation of electrochemically active species.In this review,various types of non-fluorinated PEMs including main-chain-type hydrocarbon membranes,microphase separation membranes and membranes with rigid-twisted structure are comprehensively summarized.The basic properties of different types of non-fluorinated PEMs including water uptake,swelling ratio,oxidative stability,tensile strength and conductivity are compared and the corresponding application performance in FCs,RFBs and PEMWE are discussed.The state-of-the-art of the structural design in both monomers and polymers is reviewed for the construction of fast ion transport channels and high resistance of free radical attacks.Also,future challenges and possibilities for the development of non-fluorinated PEMs are comprehensively forecasted.展开更多
High-entropy materials(HEMs),which are typically composed of five or more elements in near-equimolar ratios with concentrations ranging from 5%to 35%,have distinct elemental compositions and geometric properties that ...High-entropy materials(HEMs),which are typically composed of five or more elements in near-equimolar ratios with concentrations ranging from 5%to 35%,have distinct elemental compositions and geometric properties that allow for the development of advanced electrocatalysts for renewable energy conversion systems.The highentropy effect,crystal dislocations,cocktail effect,and slow diffusion in high-entropy layered double hydroxides(HE-LDHs)and amorphous materials(HE-AMs)have all been shown to boost electrocatalytic water oxidation performance significantly.These materials exhibit remarkable activity and stability in both alkaline and acidic conditions.HE-AMs,in particular,benefit from a variety of defects,including coordinatively unsaturated sites and loosely connected atoms,which are critical to their improved catalytic capabilities.HEMs engineering and precise nanostructure control can address the low intrinsic activity,restricted active sites,and poor conductivity of binary and ternary amorphous and LDH catalysts.This study discusses current advances in HE-LDHs and HE-AMs for water electrolysis,including synthesis methods,structural features,active site identification by DFT calculations,and their applications in water electrocatalysis.The presentation also covers potential problems and future directions for developing these materials in energy conversion device systems.展开更多
The discontinuation of denosumab[antibody targeting receptor activator of nuclear factor kappa B ligand(RANKL)]therapy may increase the risk of multiple vertebral fractures;however,the underlying pathophysiology is la...The discontinuation of denosumab[antibody targeting receptor activator of nuclear factor kappa B ligand(RANKL)]therapy may increase the risk of multiple vertebral fractures;however,the underlying pathophysiology is largely unknown.In patients who underwent discontinuation after multiple injections of denosumab,the levels of tartrate-resistant acid phosphatase 5b increased compared to pretreatment levels,indicating a phenomenon known as“overshoot.”The rate of decrease in bone mineral density during the withdrawal period was higher than the rate of decrease associated with aging,suggesting that the physiological bone metabolism had broken down.Overshoot and significant bone loss were also observed in mice receiving continuous administration of anti-RANKL antibody after treatment was interrupted,resembling the original pathology.In mice long out of overshoot,bone resorption recovered,but osteoblast numbers and bone formation remained markedly reduced.The bone marrow exhibited a significant reduction in stem cell(SC)antigen 1-and platelet-derived growth factor receptor alpha-expressing osteoblast progenitors(PαS cells)and alkaline phosphatase-positive early osteoblasts.Just before the overshoot phase,the osteoclast precursor cell population expands and RANKL-bearing extracellular vesicles(EVs)became abundant in the serum,leading to robust osteoclastogenesis after cessation of anti-RANKL treatment.Thus,accelerated bone resorption due to the accumulation of RANKLbearing EVs and long-term suppression of bone formation uncoupled from bone resorption leads to the severe bone loss characteristic of denosumab discontinuation.展开更多
Background:Epidemiological studies have confirmed that longer exposure to insecticides like cypermethrin(CYP)significantly increases the risk of male reproductive toxicity.Crocus sativus L.has been recognized due to i...Background:Epidemiological studies have confirmed that longer exposure to insecticides like cypermethrin(CYP)significantly increases the risk of male reproductive toxicity.Crocus sativus L.has been recognized due to its therapeutic properties,but its exact role and molecular mechanisms in treatment of reproductive dysfunction remain unclear.Methods:During this study,36 rats were randomly divided into six groups(n=6):control,CYP-induced(60 mg/kg),standard(leuprolide 3 mg/kg)and three treatment groups receiving aqueous,ethanolic,and oil extracts(50 mg/kg or 20 mL/kg)for post-toxicity induction.Results:The finding represented that exposure of CYP significantly increased oxidative stress,disrupted testicular architecture,and markedly reduced testosterone levels(P<0.05).Importantly,Crocus sativus L.treatment alleviated these changes by increasing the expression of Nrf2(nuclear factor erythroid 2-related factor 2),restoring the activity of antioxidant enzymes,and enhancing testicular histomorphology.Surprisingly,molecular docking established a high binding affinity of Crocus sativus L.phytoconstituents such as gallic acid,cinnamic acid and quercetin to the Nrf2-Keap1 complex.It is worth noting that,Crocus sativus L.exhibited a high level of protection against reproductive toxicity caused by CYP in male rats,which was mediated by the activation of Nrf2 pathway,reduction of oxidative damage,and favorable ADMET characteristics.Conclusion:Notably,this research provides a more valid,safe,and effective method of developing new drugs for reproductive disorders,however,further investigation is needed to support the research findings and implement it in clinical practice.展开更多
Radiation-induced grafting of styrene onto polytetrafluoroethylene (PTFE) membranes was studied by a simultaneous irradiation technique.Grafting was carded out usingγ-radiation from a ^(60)Co source at room temperatu...Radiation-induced grafting of styrene onto polytetrafluoroethylene (PTFE) membranes was studied by a simultaneous irradiation technique.Grafting was carded out usingγ-radiation from a ^(60)Co source at room temperature. Effects of absorbed dose,atmosphere,dose rate,and the concentration of initial monomer on the degree of grafting (DOG) were investigated and the most appropriate grafting condition was obtained.Subsequently,sulphonation of the grafted PTFE membrane (PTFE-g-PS) was carried out and a series of ion exchange membranes (PTFE-g-PSSA) was prepared.Further characterizations of FTIR,TGA,and SEM testified that grafting and sulphonation of the membranes were successfully processed;moreover,grafting of styrene not only occurred in the surface of PTFE membrane,but also in the micropores of the membrane.Ion exchange capacity (IEC) and conductivity were found increase with the grafting yield.The results suggest that at a low dose,such as 17 kGy,the ion exchange membrane (IEM) which will be suitable for vanadium redox battery (VRB) use can be obtained.展开更多
Chemistry-heated diffused permeation was used to treat POMs. ICP, IR, TG-DTA, XPS were used to characterize K_(10)H_3[Dy(SiW_4Mo_7O_(39))_2] and the sample. The result show that Sm and Gd can be permeated into the bod...Chemistry-heated diffused permeation was used to treat POMs. ICP, IR, TG-DTA, XPS were used to characterize K_(10)H_3[Dy(SiW_4Mo_7O_(39))_2] and the sample. The result show that Sm and Gd can be permeated into the body of this sample, chemical bonds forming between Sm and other components and the conductivity of K_(10)H_3[Dy(SiW_4Mo_7O_(39))_2] improves by 0 9356×10~4 times.展开更多
Soil acidification is a major threat to agricultural sustainability in tropical and subtropical regions.Biodegradable and environmentally friendly materials,such as calcium lignosulfonate(CaLS),calcium poly(aspartic a...Soil acidification is a major threat to agricultural sustainability in tropical and subtropical regions.Biodegradable and environmentally friendly materials,such as calcium lignosulfonate(CaLS),calcium poly(aspartic acid)(PASP-Ca),and calcium polyγ-glutamic acid(γ-PGA-Ca),are known to effectively ameliorate soil acidity.However,their effectiveness in inhibiting soil acidification has not been studied.This study aimed to evaluate the effect of CaLS,PASP-Ca,andγ-PGA-Ca on the resistance of soil toward acidification as directly and indirectly(i.e.,via nitrification)caused by the application of HNO_(3)and urea,respectively.For comparison,Ca(OH)_(2)and lignin were used as the inorganic and organic controls,respectively.Among the materials,γ-PGA-Ca drove the substantial improvements in the pH buffering capacity(pHBC)of the soil and exhibited the greatest potential in inhibiting HNO_(3)-induced soil acidification via protonation of carboxyl,complexing with Al~(3+),and cation exchange processes.Under acidification induced by urea,CaLS was the optimal one in inhibiting acidification and increasing exchangeable acidity during incubation.Furthermore,the sharp reduction in the population sizes of ammonia-oxidizing bacteria(AOB)and ammonia-oxidizing archaea(AOA)confirmed the inhibition of nitrification via CaLS application.Therefore,compared to improving soil pHBC,CaLS may play a more important role in suppressing indirect acidification.Overall,γ-PGA-Ca was superior to PASP-Ca and CaLS in enhancing the soil pHBC and the its resistance to acidification induced by HNO_(3) addition,whereas CaLS was the best at suppressing urea-driven soil acidification by inhibiting nitrification.In conclusion,these results provide a reference for inhibiting soil re-acidification in intensive agricultural systems.展开更多
In this study,the truncated octahedral CeO_(2)(CeO_(2)-to)with special morphology was prepared by the solvothermal method with oleic acid(OA)and oleamine(OM)as the morphology-directing agents.High-resolution transmiss...In this study,the truncated octahedral CeO_(2)(CeO_(2)-to)with special morphology was prepared by the solvothermal method with oleic acid(OA)and oleamine(OM)as the morphology-directing agents.High-resolution transmission electron microscopy(HRTEM)results show that CeO_(2)-to exposes composite{100}and{111}facets,while CeO_(2)cubic(CeO_(2)-c)and CeO_(2)octahedral(CeO_(2)-o)only expose single crystal facets of{100}plane and{111}plane,respectively.Interestingly,this CeO_(2)-to photocatalyst exhibits remarkable photooxidation performance of gaseous acetaldehyde(CH_(3)CHO)degradation,in which CO_(2)generation value reaches 1.78 and 7.97-times greater than that of CeO_(2)-c and CeO_(2)-o,respectively.In addition,the active species trapping experiment signifies that superoxide(·O_(2)^(-))and holes(h^(+))are the main reactive substances during the CH_(3)CHO degradation process,and the electron paramagnetic resonance(EPR)spectra indicates that the former is the major contributor.Notably,the electron transfer mechanism between CeO_(2)-to{100}and{111}facets and the surface oxygen adsorption ability are revealed via density functional theory(DFT)calculations.It is also confirmed that{100}facets are more conducive to the absorption of acetaldehyde than{111}facets.Finally,a reasonable mechanism for improved photocatalytic CH_(3)CHO degradation on CeO_(2)-to is proposed based on relevant experiments and DFT calculations.This study demonstrates that the systematic development of surface homojunction structured photocatalysts can efficiently increase the degradation activity for volatile organic compounds(VOCs).It also offers additional direction for optimizing the photocatalytic activity of other ceriumbased photocatalysts.展开更多
Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storag...Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storage technology for the grid-scale integration of renewable electricity.pH-neutral AORFBs that feature high safety,low corrosivity,and environmental benignity are particularly promising,and their battery performance is significantly impacted by redox-active molecules and ion-exchange membranes(IEMs).Here,representative anolytes and catholytes engineered for use in pH-neutral AORFBs are outlined and summarized,as well as their side reactions that cause irreversible battery capacity fading.In addition,the recent achievements of IEMs for pH-neutral AORFBs are discussed,with a focus on the construction and tuning of ion transport channels.Finally,the critical challenges and potential research opportunities for developing practically relevant pH-neutral AORFBs are presented.展开更多
The title compound was prepared and treated by high temperature gaseous mix rare earth permeation. ICP, IR, TG-DTA, XPS, XRD were used to characterize the title compound and the treated sample. The results confirm tha...The title compound was prepared and treated by high temperature gaseous mix rare earth permeation. ICP, IR, TG-DTA, XPS, XRD were used to characterize the title compound and the treated sample. The results confirm that Ce and La can be permeated into the body of the title compound. Four-probe method was used to measure the conductivities. A novel result that the conductivity of the permeated compound (δ=9.2×10 -3 S·cm -1)improved by 7.1×106 times than that of the title compound(δ=1.29×10 -9 S·cm -1) is received.展开更多
Rare earth co-permeation of （NH4）3[CrMo6O24H6]·7H2O was reported and the conductivity of （NH4）3[CrMo6O24H6] was improved by 6.734×10^9 times. X-ray fluorescence spectrometry （XRF）, thermogravimetry-dif...Rare earth co-permeation of （NH4）3[CrMo6O24H6]·7H2O was reported and the conductivity of （NH4）3[CrMo6O24H6] was improved by 6.734×10^9 times. X-ray fluorescence spectrometry （XRF）, thermogravimetry-differential thermal analysis （TG-DTA）, X-ray diffraction （XRD） have been used to character （NH4）3[CrMo6O24H6]·7H2O and permeated sample. Experimental results showed that Nd could be permeated into the body of this sample and the XRD patterns showed great difference between （NH4）3[CrMo6O24H6]·7H2O and permeated sample. The structure of （NH4）3[CrMo6O24H6]·7H2O was destroyed and new compound MoN perhaps formed.展开更多
基金All thanks go to the contributions from all students,postdoctoral fellows,and visiting scholars.Special thanks are extended to the contributions from Prof.Jong Wook Bae(Sungkyunkwan University),Prof.Ruiqin Yang(Zhejiang University of Science and Technology),Prof.Yisheng Tan(Institute of Coal Chemistry,Chinese Academy of Sciences),Prof.Minbo Wu(China University of Petroleum),Prof.Xingang Li(Tianjin University),et al.Jie Yao appreciates the Grant-in-Aid for JSPS Fellows(JSPS KAKENHI 22J11458 and 22KJ1456).
文摘This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the research field of one-carbon(C1)chemistry,including catalytic conversion of C1 molecules to valuable chemicals and superclean fuels,innovative catalyst and reactor development,and the design of new catalytic reactions and processes.Organized chronologically,this review highlights Prof.Tsubaki’s academic contributions from 1990,when he studied and worked at The University of Tokyo,to his current role as a full professor at the University of Toyama.The academic section of this review is divided into three main parts,focusing on Prof.Tsubaki’s pioneering work in C1 chemistry.We believe that this review will serve as a highly valuable reference for colleagues in the fields of C1 chemistry and catalysis,and inspire the development of more original and groundbreaking research.
文摘Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of polyfluoroarenes with alkyl halides under mild conditions is reported.Polyfluoroarenes(3~6 F)can reacted smoothly with a diverse range of alkyl halides,such as primary,secondary,and tertiary alkyl iodides.The efficient formation of C(sp2)—C(sp3)can be achieved through the combination of Ni catalysis and(Bpin)2/K2CO3 as terminal reductant.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(RS-2023-00208355,RS-2024-00439825,and 2022M3H4A408610313)supported by the Global Science Research Center Program(RS-2024-00411134)+1 种基金funded by the National Research Foundation of KoreaThe experiments at PAL were supported in part by MOST and POSTECH。
文摘The exsolution method has garnered significant attention owing to its high efficacy in developing highly efficient and stable metal nanocatalysts.Herein,a versatile exsolution approach is developed to embed size-tunable metal nanocatalysts within a conductive metal pnictogenide matrix.The gas-phase reaction of Ru-substituted Ni-Fe-layered-double-hydroxide(Ni_(2)Fe_(1-x)Ru_(x)-LDH)with pnictogenation reagents leads to the exsolution of Ru metal nanocatalysts and a phase transformation into metal pnictogenide.The variation in reactivity of pnictogenation reagents allows for control over the size of the exsolved metal nanocatalysts(i.e.,nanoclusters for nitridation and single atoms for phosphidation),underscoring the effectiveness of the pnictogenation-driven exsolution strategy in stabilizing size-tunable metal nanocatalysts.The Ru-exsolved nickel-iron nitride/phosphide demonstrates outstanding electrocatalyst activity for the hydrogen evolution reaction,exhibiting a smaller overpotential and higher stability than Ru-deposited homologs.The high efficacy of pnictogenation-assisted exsolution in optimizing the performance and stability of Ru metal nanocatalysts is ascribed to the efficient interfacial electronic interaction between Ru metals and nitride/phosphide ions assisted by the inner sphere mechanism.In situ spectroscopic analyses highlight that exsolved Ru single atoms facilitate more efficient electron transfer to the reactants than the exsolved Ru nanoclusters,which is primarily responsible for the superior impact of the phosphidation-driven exsolution approach.
文摘Background:Chaetomorpha aerea,a marine green alga,has drawn attention because of its rich phytochemical constituents and therapeutic benefits.Using an integrated approach that combined in vitro,in vivo,and in silico approaches,this work examined the antioxidant,anti-inflammatory,and antidiabetic qualities of acetone extract of C.aerea(AECA).Methods:Total phenolic and flavonoid concentrations of AECA were measured.Antioxidant activity was assessed using the DPPH and ABTS free radical scavenging assays.In vitro protein denaturation and in vivo carrageenan-induced paw edema models were employed to evaluate the anti-inflammatory potential,whereas antidiabetic activity was assessed using in vitroα-amylase inhibition and in vivo oral glucose tolerance test(OGTT).Molecular docking and ADME/T analysis were employed to further analyze bioactive compounds identified using gas chromatography–mass spectrometry(GC–MS).Result:Antioxidant activity demonstrated a minimum inhibitory concentration(IC_(50))of 107.44μg/mL for DPPH and 118.23μg/mL for ABTS.In vitro anti-inflammatory assays indicated a suppression of protein denaturation at a concentration of 102μg/mL(IC_(50)),where AECA(400 mg/kg)resulted in a 27%reduction in paw edema at 6 h in the mouse model.In vitro antidiabetic test indicatedα-amylase inhibition with an IC_(50) value of 70.72μg/mL,and in the OGTT,a significant lowering of blood glucose was recorded at 120 min in mice.Strong binding affinities were observed for stigmasta-5,24(28)-dien-3-ol,identified using GC–MS,with values of−9.9 kcal/mol forα-amylase and−8.0 kcal/mol for cyclooxygenase-2.Conclusion:C.aerea serves as an effective natural remedy for oxidative stress,inflammation,and hyperglycemia.These findings advocate for further clinical and mechanistic investigations to optimize therapeutic efficacy.
基金supported by the National Natural Science Foundation of China(Nos.52270165 and 51978537)the Key Laboratory of Safety for Geotechnical and Structural Engineering of Hubei Province。
文摘The persistence of chlorinated alkanes in aquatic environments poses significant health risks due to its biotoxicity and high volatility,which contributes to both water and air pollution.This study investigates the efficacy of carbon dioxide radical anion(CO_(2)·^(-))mediated advanced reduction processes(ARPs)for the reductive dechlorination of chlorinated alkanes using small molecular monocarboxylic acids(SMAs)under UV irradiation.The study focused on formic acid(HCOOH),acetic acid(CH_3COOH),and propionic acid(CH_3CH_(2)COOH)to generate CO_(2)·^(-),revealing that UV/HCOOH system exhibits a notably high chloroform(CF)degradation efficiency of 97.8%in 90 min.Kinetic studies indicated a linear relationship between the HCOOH concentrations and the observed reaction rate constants(k_(obs)),demonstrating that CO_(2)·^(-)production is crucial for CF degradation.Electron paramagnetic resonance spectroscopy identified CO_(2)·^(-)and hydroxyl radicals(HO·)as the active species,with the former playing a predominant role in CF degradation.The study also explored the influence of carbon chain length in SMAs on CF degradation,finding that longer chains decrease the degradation efficiency,potentially due to reduced UV activation.A higher reaction rate constant(k_(obs))under acidic conditions,with a marked decrease in efficiency as the pH exceeds 3.7,where HCOO^(-)becomes predominant.This study enhances our understanding of CO_(2)·^(-)mediated ARPs and explores potential applications in environmental remediation,providing insights into the pathways and mechanisms of CF degradation.The UV/SMAs systems offer advantages for practical applications,such as milder reaction conditions and higher efficiency compared to traditional methods.
基金financially supported by Guangdong Basic and Applied Basic Research Foundation(No.2024A1515010976)Shenzhen Peacock Plan(No.20210802524B)+3 种基金the Postdoctoral Research Foundation of China(Nos.GZC20241085,GZC20230562,GZC20230564)China Postdoctoral Science Foundation(No.2024M760583)the National Natural Science Foundation of China(No.52402234)Shenzhen Key Laboratory of 2D Metamaterials for Information Technology
文摘This article systematically reviewed the applications of single-atom catalysts(SACs)in the domain of photocatalytic reactions,with a particular emphasis on the indispensable role of H_(2)O in these processes.SACs,due to their distinct active sites and superior catalytic efficacy,found their applications in the fields of energy conversion and environmental protection.The review elaborated on the potential carriers,preparation methods,and characterization techniques for single-atom photocatalysts.Subsequently,the article provided an in-depth explanation of the crucial role of H_(2)O in photocatalytic reactions,serving as an important green solvent and an oxygen/proton source.The adsorption of water could also change the surface energy structure and charge distribution of the photocatalyst.Conversely,the presence of H_(2)O might also inhibit the target reaction.Additionally,the distinct roles of water in both liquid and gas phases were discussed.Furthermore,the review systematically summarized the applications of single-atom photocatalysts in H_(2)generation,CO_(2)reduction,N2fixation,H_(2)O_(2)production,and environmentalremediation.It delved into the mechanisms by which water molecules participated in photocatalytic processes and their interactions with competing pathways,thereby revealing the complexity and critical importance of water in photocatalytic reactions.Finally,the article discusses the opportunities and challenges of SACs in photocatalytic reactions with H_(2)O.This article provides a comprehensive perspective for understanding the role of SACs in waterinvolved photocatalytic reactions.
基金supported by the National Natural Science Foundation of China(Grant Nos.22275092 and 52372084)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(Grant No.KYCX24_0709)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.30923010920)the State Key Laboratory of Transient Chemical Effects and Control,China,(Grant No.6142602230201).
文摘Enhancing the output capacity of semiconductor bridge(SCB) through the application of composite nano-energetic films is a subject of wide concern. Furthermore, improving the safety, reliability, and production efficiency of energetic semiconductor bridge(ESCB) is the primary focus for large-scale engineering applications in the future. Here, the Al/CuO nano-film ESCB was efficiently fabricated using 3D direct writing. The electrostatic safety of the film is enhanced by precisely adjusting the particle size of Al, while ensuring that the SCB can initiate the film with small energy. The burst characteristics of SCB/ESCB were thoroughly investigated by employing a 100 μF tantalum capacitor to induce SCB and ESCB under an intense voltage gradient. The solid-state heating process of both SCB and ESCB was analyzed with multi physical simulation(MPS). The experimental results demonstrate that the critical burst time of both SCB and ESCB decreases with increasing voltage. Under the same voltage, the critical burst time of ESCB is longer than that of SCB, primarily due to differences in the melting to vaporization stage. The MPS results indicate that the highest temperature is observed at the V-shaped corner of SCB. Due to the thermal contact resistance between SCB and the film, heat conduction becomes more concentrated in the central region of the bridge, resulting in a faster solid-state heating process for ESCB compared to SCB.The results of the gap ignition experiments indicate that at a 19 mm gap, an ESCB with a film mass of 10 mg can ignite nickel hydrazine nitrate(NHN) and cyclotrimethylenetrinitramine(RDX). This suggests that thermite ESCB can serve as a novel, safe, and reliable energy exchange element and initiator in largescale engineering applications.
基金financially supported by the Youth Fund of the National Natural Science Foundation of China(No.22406161)“Lvyang Jinfeng Project”Funded by Yangzhou City(No.137013435)+2 种基金the Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou Universitythe Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCX23_1910)JST ACT-C program of Japan
文摘In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the Ce-OFDC matrix,forming a CeOFDC/PCN composite material.Antibacterial assays demonstrated that Ce-OFDC/PCN had significant inhibitory effects on both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus),achieving inhibition rates of 99.5%and 94.3%,respectively.Notably,the antibacterial performance of Ce-OFDC/PCN was superior to that of Ce-OFDC or PCN alone.Furthermore,photocurrent and electrical impedance scanning measurements demonstrated that the Ce-OFDC/PCN composites showed improved photocurrent response and superior efficiency in separating photogenerated electrons and holes.The photocurrent density of Ce-OFDC/PCN reached 120μA cm^(-2),which was 1.5 times higher than that of PCN(80μA cm^(-2))and 12 times higher than that of Ce-OFDC(10μA cm^(-2)).Electron paramagnetic resonance analysis indicated that reactive oxygen species played a crucial role in the antimicrobial process,with super oxide radicals(·O_(2)^(-))and hydroxyl radical(·OH)showing the most prominent influence.We conducted reactive oxygen species(ROS)scavenging experiments to further confirm this view.After adding glutathione(GSH)to remove all ROS,the antibacterial efficiency of Ce-OFDC/PCN decreased by about 40%.Adding D-mannitol to remove·OH reduced the inhibition rate to 54.7%,and adding superoxide dismutase(SOD)to remove·O_(2)^(-)reduced the inhibition rate to 65.4%.The Ce-OFDC/PCN heterostructure increased the separation efficiency of photogenerated electrons and holes,producing increased reactive oxygen species.That,in turn,contributed to the observed superior photocatalytic antibacterial performance.This research significantly advanced the development of metal-organic framework(MOF)-based materials and provided valuable insights into the design of antimicrobial photocatalysts.
基金supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization(NEDO),the JST Fusion Oriented Research for disruptive Science and Technology Program(JPMJFR213D)JSPS KAKENHI(JP24K17774)Domen for his guidance during their PhD studies at the University of Tokyo,as well as for his ongoing support,encouragement,and mentorship.
文摘Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.
基金funded by the National Key Research and Development Program of China(No.2022YFB3805300)National Natural Science Foundation of China(Grant No.22125801,22005010).
文摘Proton exchange membranes(PEMs)are widely employed in energy conversion and storage devices including fuel cells(FCs),redox flow batteries(RFBs)and PEM water electrolysis(PEMWE).As one of the main components of these devices,a high-performance PEM is always desirable considering the cost challenges from both energy utilization efficiency and production cost.From this century,governments of countries worldwide have introduced PFAS(per-and polyfluoroalkyl substances)restriction related policies,which facilitate the extensive research on non-fluorinated PEMs.Besides,non-fluorinated PEMs become hot topics of all kinds of PEMs due to the advantages including excellent conductivity,high mechanical property,reduced swelling,low cost and reduced ion permeation of electrochemically active species.In this review,various types of non-fluorinated PEMs including main-chain-type hydrocarbon membranes,microphase separation membranes and membranes with rigid-twisted structure are comprehensively summarized.The basic properties of different types of non-fluorinated PEMs including water uptake,swelling ratio,oxidative stability,tensile strength and conductivity are compared and the corresponding application performance in FCs,RFBs and PEMWE are discussed.The state-of-the-art of the structural design in both monomers and polymers is reviewed for the construction of fast ion transport channels and high resistance of free radical attacks.Also,future challenges and possibilities for the development of non-fluorinated PEMs are comprehensively forecasted.
基金supported by the Innovative Research Group Project of the National Natural Science Foundation of China(No.52021004)the Funds for Chongqing Talents Plan(No.CQYC2021059563)+1 种基金the Fundamental Research Funds for the Central Universities(No.2021CDJQY-027)the National Natural Science Foundation of China(No.52206089).
文摘High-entropy materials(HEMs),which are typically composed of five or more elements in near-equimolar ratios with concentrations ranging from 5%to 35%,have distinct elemental compositions and geometric properties that allow for the development of advanced electrocatalysts for renewable energy conversion systems.The highentropy effect,crystal dislocations,cocktail effect,and slow diffusion in high-entropy layered double hydroxides(HE-LDHs)and amorphous materials(HE-AMs)have all been shown to boost electrocatalytic water oxidation performance significantly.These materials exhibit remarkable activity and stability in both alkaline and acidic conditions.HE-AMs,in particular,benefit from a variety of defects,including coordinatively unsaturated sites and loosely connected atoms,which are critical to their improved catalytic capabilities.HEMs engineering and precise nanostructure control can address the low intrinsic activity,restricted active sites,and poor conductivity of binary and ternary amorphous and LDH catalysts.This study discusses current advances in HE-LDHs and HE-AMs for water electrolysis,including synthesis methods,structural features,active site identification by DFT calculations,and their applications in water electrocatalysis.The presentation also covers potential problems and future directions for developing these materials in energy conversion device systems.
文摘The discontinuation of denosumab[antibody targeting receptor activator of nuclear factor kappa B ligand(RANKL)]therapy may increase the risk of multiple vertebral fractures;however,the underlying pathophysiology is largely unknown.In patients who underwent discontinuation after multiple injections of denosumab,the levels of tartrate-resistant acid phosphatase 5b increased compared to pretreatment levels,indicating a phenomenon known as“overshoot.”The rate of decrease in bone mineral density during the withdrawal period was higher than the rate of decrease associated with aging,suggesting that the physiological bone metabolism had broken down.Overshoot and significant bone loss were also observed in mice receiving continuous administration of anti-RANKL antibody after treatment was interrupted,resembling the original pathology.In mice long out of overshoot,bone resorption recovered,but osteoblast numbers and bone formation remained markedly reduced.The bone marrow exhibited a significant reduction in stem cell(SC)antigen 1-and platelet-derived growth factor receptor alpha-expressing osteoblast progenitors(PαS cells)and alkaline phosphatase-positive early osteoblasts.Just before the overshoot phase,the osteoclast precursor cell population expands and RANKL-bearing extracellular vesicles(EVs)became abundant in the serum,leading to robust osteoclastogenesis after cessation of anti-RANKL treatment.Thus,accelerated bone resorption due to the accumulation of RANKLbearing EVs and long-term suppression of bone formation uncoupled from bone resorption leads to the severe bone loss characteristic of denosumab discontinuation.
文摘Background:Epidemiological studies have confirmed that longer exposure to insecticides like cypermethrin(CYP)significantly increases the risk of male reproductive toxicity.Crocus sativus L.has been recognized due to its therapeutic properties,but its exact role and molecular mechanisms in treatment of reproductive dysfunction remain unclear.Methods:During this study,36 rats were randomly divided into six groups(n=6):control,CYP-induced(60 mg/kg),standard(leuprolide 3 mg/kg)and three treatment groups receiving aqueous,ethanolic,and oil extracts(50 mg/kg or 20 mL/kg)for post-toxicity induction.Results:The finding represented that exposure of CYP significantly increased oxidative stress,disrupted testicular architecture,and markedly reduced testosterone levels(P<0.05).Importantly,Crocus sativus L.treatment alleviated these changes by increasing the expression of Nrf2(nuclear factor erythroid 2-related factor 2),restoring the activity of antioxidant enzymes,and enhancing testicular histomorphology.Surprisingly,molecular docking established a high binding affinity of Crocus sativus L.phytoconstituents such as gallic acid,cinnamic acid and quercetin to the Nrf2-Keap1 complex.It is worth noting that,Crocus sativus L.exhibited a high level of protection against reproductive toxicity caused by CYP in male rats,which was mediated by the activation of Nrf2 pathway,reduction of oxidative damage,and favorable ADMET characteristics.Conclusion:Notably,this research provides a more valid,safe,and effective method of developing new drugs for reproductive disorders,however,further investigation is needed to support the research findings and implement it in clinical practice.
基金Supported by The Scientific Research Foundation of State's Education Ministry for the Returned Overseas Chinese Scholars.
文摘Radiation-induced grafting of styrene onto polytetrafluoroethylene (PTFE) membranes was studied by a simultaneous irradiation technique.Grafting was carded out usingγ-radiation from a ^(60)Co source at room temperature. Effects of absorbed dose,atmosphere,dose rate,and the concentration of initial monomer on the degree of grafting (DOG) were investigated and the most appropriate grafting condition was obtained.Subsequently,sulphonation of the grafted PTFE membrane (PTFE-g-PS) was carried out and a series of ion exchange membranes (PTFE-g-PSSA) was prepared.Further characterizations of FTIR,TGA,and SEM testified that grafting and sulphonation of the membranes were successfully processed;moreover,grafting of styrene not only occurred in the surface of PTFE membrane,but also in the micropores of the membrane.Ion exchange capacity (IEC) and conductivity were found increase with the grafting yield.The results suggest that at a low dose,such as 17 kGy,the ion exchange membrane (IEM) which will be suitable for vanadium redox battery (VRB) use can be obtained.
文摘Chemistry-heated diffused permeation was used to treat POMs. ICP, IR, TG-DTA, XPS were used to characterize K_(10)H_3[Dy(SiW_4Mo_7O_(39))_2] and the sample. The result show that Sm and Gd can be permeated into the body of this sample, chemical bonds forming between Sm and other components and the conductivity of K_(10)H_3[Dy(SiW_4Mo_7O_(39))_2] improves by 0 9356×10~4 times.
基金supported by the Major project of Ministry of Agriculture and Rural Affairs of the People’s Republic of China(No.NK2022180401)the major project of Ministry of Agriculture and Rural Affairs of the People’s Republic of China(No.NK2022180404)。
文摘Soil acidification is a major threat to agricultural sustainability in tropical and subtropical regions.Biodegradable and environmentally friendly materials,such as calcium lignosulfonate(CaLS),calcium poly(aspartic acid)(PASP-Ca),and calcium polyγ-glutamic acid(γ-PGA-Ca),are known to effectively ameliorate soil acidity.However,their effectiveness in inhibiting soil acidification has not been studied.This study aimed to evaluate the effect of CaLS,PASP-Ca,andγ-PGA-Ca on the resistance of soil toward acidification as directly and indirectly(i.e.,via nitrification)caused by the application of HNO_(3)and urea,respectively.For comparison,Ca(OH)_(2)and lignin were used as the inorganic and organic controls,respectively.Among the materials,γ-PGA-Ca drove the substantial improvements in the pH buffering capacity(pHBC)of the soil and exhibited the greatest potential in inhibiting HNO_(3)-induced soil acidification via protonation of carboxyl,complexing with Al~(3+),and cation exchange processes.Under acidification induced by urea,CaLS was the optimal one in inhibiting acidification and increasing exchangeable acidity during incubation.Furthermore,the sharp reduction in the population sizes of ammonia-oxidizing bacteria(AOB)and ammonia-oxidizing archaea(AOA)confirmed the inhibition of nitrification via CaLS application.Therefore,compared to improving soil pHBC,CaLS may play a more important role in suppressing indirect acidification.Overall,γ-PGA-Ca was superior to PASP-Ca and CaLS in enhancing the soil pHBC and the its resistance to acidification induced by HNO_(3) addition,whereas CaLS was the best at suppressing urea-driven soil acidification by inhibiting nitrification.In conclusion,these results provide a reference for inhibiting soil re-acidification in intensive agricultural systems.
基金supported by the National Natural Science Foundation of China(Nos.21805191 and 22205084)Project funded by China Postdoctoral Science Foundation(No.2023M741039)+3 种基金Project funded by National&Local Joint Engineering Research Center for Mineral Salt Deep Utilization(SF202303)Project Funded by Yangzhou University(137013308),Guangdong Basic and Applied Basic Research Foundation(No.2020A1515010982)Shenzhen Stable Support Project(No.20200812122947002),the Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou UniversityPostgraduate Research&Practice Innovation Program of Jiangsu Province(Yangzhou University,No.XKYCX20_014)。
文摘In this study,the truncated octahedral CeO_(2)(CeO_(2)-to)with special morphology was prepared by the solvothermal method with oleic acid(OA)and oleamine(OM)as the morphology-directing agents.High-resolution transmission electron microscopy(HRTEM)results show that CeO_(2)-to exposes composite{100}and{111}facets,while CeO_(2)cubic(CeO_(2)-c)and CeO_(2)octahedral(CeO_(2)-o)only expose single crystal facets of{100}plane and{111}plane,respectively.Interestingly,this CeO_(2)-to photocatalyst exhibits remarkable photooxidation performance of gaseous acetaldehyde(CH_(3)CHO)degradation,in which CO_(2)generation value reaches 1.78 and 7.97-times greater than that of CeO_(2)-c and CeO_(2)-o,respectively.In addition,the active species trapping experiment signifies that superoxide(·O_(2)^(-))and holes(h^(+))are the main reactive substances during the CH_(3)CHO degradation process,and the electron paramagnetic resonance(EPR)spectra indicates that the former is the major contributor.Notably,the electron transfer mechanism between CeO_(2)-to{100}and{111}facets and the surface oxygen adsorption ability are revealed via density functional theory(DFT)calculations.It is also confirmed that{100}facets are more conducive to the absorption of acetaldehyde than{111}facets.Finally,a reasonable mechanism for improved photocatalytic CH_(3)CHO degradation on CeO_(2)-to is proposed based on relevant experiments and DFT calculations.This study demonstrates that the systematic development of surface homojunction structured photocatalysts can efficiently increase the degradation activity for volatile organic compounds(VOCs).It also offers additional direction for optimizing the photocatalytic activity of other ceriumbased photocatalysts.
基金funded by the National Key Research and Development Program of China(Nos.2022YFB3805303,2022YFB3805304)the National Natural Science Foundation of China(Grant/Award Numbers:22308345,U20A20127)+1 种基金the Anhui Provincial Natural Science Foundation(No.2308085QB68)the Fundamental Research Funds for the Central Universities(No.WK2060000059).
文摘Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storage technology for the grid-scale integration of renewable electricity.pH-neutral AORFBs that feature high safety,low corrosivity,and environmental benignity are particularly promising,and their battery performance is significantly impacted by redox-active molecules and ion-exchange membranes(IEMs).Here,representative anolytes and catholytes engineered for use in pH-neutral AORFBs are outlined and summarized,as well as their side reactions that cause irreversible battery capacity fading.In addition,the recent achievements of IEMs for pH-neutral AORFBs are discussed,with a focus on the construction and tuning of ion transport channels.Finally,the critical challenges and potential research opportunities for developing practically relevant pH-neutral AORFBs are presented.
文摘The title compound was prepared and treated by high temperature gaseous mix rare earth permeation. ICP, IR, TG-DTA, XPS, XRD were used to characterize the title compound and the treated sample. The results confirm that Ce and La can be permeated into the body of the title compound. Four-probe method was used to measure the conductivities. A novel result that the conductivity of the permeated compound (δ=9.2×10 -3 S·cm -1)improved by 7.1×106 times than that of the title compound(δ=1.29×10 -9 S·cm -1) is received.
基金the Key Science and Technology Foundation of Heilongjiang Province(Grant No.GB02A301) National Natural Science Foundation of China(Grant No.2037101)
文摘Rare earth co-permeation of （NH4）3[CrMo6O24H6]·7H2O was reported and the conductivity of （NH4）3[CrMo6O24H6] was improved by 6.734×10^9 times. X-ray fluorescence spectrometry （XRF）, thermogravimetry-differential thermal analysis （TG-DTA）, X-ray diffraction （XRD） have been used to character （NH4）3[CrMo6O24H6]·7H2O and permeated sample. Experimental results showed that Nd could be permeated into the body of this sample and the XRD patterns showed great difference between （NH4）3[CrMo6O24H6]·7H2O and permeated sample. The structure of （NH4）3[CrMo6O24H6]·7H2O was destroyed and new compound MoN perhaps formed.
