Osteoporosis is a known risk factor for rotator cuff tears(RCTs),but the causal correlation and underlying mechanisms remain unclear.This study aims to evaluate the impact of osteoporosis on RCT risk and investigate t...Osteoporosis is a known risk factor for rotator cuff tears(RCTs),but the causal correlation and underlying mechanisms remain unclear.This study aims to evaluate the impact of osteoporosis on RCT risk and investigate their genetic associations.Using data from the UK Biobank(n=457871),cross-sectional analyses demonstrated that osteoporosis was significantly associated with an increased risk of RCTs(adjusted OR[95%CI]=1.38[1.25–1.52]).A longitudinal analysis of a subset of patients(n=268117)over 11 years revealed that osteoporosis increased the risk of RCTs(adjusted HR[95%CI]=1.56[1.29–1.87]),which is notably varied between sexes in sex-stratified analysis.Causal inference methods,including propensity score matching,inverse probability weighting,causal random forest and survival random forest models further confirmed the causal effect,both from cross-sectional and longitudinal perspectives.展开更多
Prominent cadmium(Cd)pollution and widespread phoxim(p H)use hinder the growth and medicinal value of Ligusticum chuanxiong Hort.(Chuanxiong).While bioremediation by rhizobacteria helps plants counter pollutants,the s...Prominent cadmium(Cd)pollution and widespread phoxim(p H)use hinder the growth and medicinal value of Ligusticum chuanxiong Hort.(Chuanxiong).While bioremediation by rhizobacteria helps plants counter pollutants,the specific roles of indigenous resistant consortia collected from polluted soils in immobilizing heavy metals,degrading pesticides,and enhancing plant stress tolerance remain insufficiently explored.Here,an indigenous pollutant-resistant consortium(RM)was developed from a highly Cd-polluted area(14.85 mg/kg Cd)as a bioremediation strategy to alleviate stress on Chuanxiong.The RM was specifically enriched with a Cd-p H co-resistant strain,Halomonas spp.TS2.Through16S r RNA sequencing,active microorganisms within RM was identified,including Bacillus,Acinetobacter,Enterococcus,Paraclostridium,and Staphylococcus.Pot experiments demonstrated that RM increased Chuanxiong biomass by 93.38%under Cd-contaminated and by 32.89%under Cd-p H co-contaminated.Furthermore,RM enhanced p H degradation,stabilized soil compounds,and reduced Cd bioavailability,thereby mitigating oxidative damage and altering the diversity and composition of Cd-p H-resistant organisms.These results indicate that utilizing indigenous microbial consortia as a bioremediation strategy can effectively improve soil health and enhance the sustainable cultivation of medicinal herbs in environments heavily contaminated.展开更多
Immunosuppressants currently approved for the treatment of autoimmune diseases and organ transplant rejection present diverse adverse effects that impair the life quality of patients.Therefore,the development of novel...Immunosuppressants currently approved for the treatment of autoimmune diseases and organ transplant rejection present diverse adverse effects that impair the life quality of patients.Therefore,the development of novel immunomodulators with high efficiency and low toxicity is essential.Ellagic acid(EA),a natural polyphenol compound widely distributed in berries,is metabolically transformed by gut microbiome to exert systemic health benefits.Here,we identified that intraperitoneal administration of EA with no cytotoxicity,beyond its wellknown oral metabolic fate,effectively decreased clinical severity and central nervous system(CNS)inflammation/demyelination in experimental autoimmune encephalomyelitis,a mouse model of an autoimmune disease multiple sclerosis.Interestingly,intraperitoneal EA administration at incredibly low doses(0.1 mg/(kg·day))is dose-sparing with fingolimod(FTY720),the first FDA-approved oral drug for MS.In addition,intraperitoneal EA also ameliorated the brain damage in a neuromyelitis optica(NMO)model,and significantly prevented the immune rejection of allograft skin graft.Evidence from pharmacological studies combined with RNA-seq indicate that prototype EA functions by a mechanism that involves direct inhibition of casein kinase II(CKII)to suppress the expression of IL-17 and promote the expression of Cpt1a to regulate T helper cell 17 differentiation.In conclusion,our study demonstrates that the prototype EA entering the blood circulation acts as a novel therapeutic immunomodulator for the treatment of autoimmune diseases and transplant rejection through the CKII-mediated Janus kinase/signal transducer and activator of transcription 3 Cpt1a signaling pathway.展开更多
In aerospace,BBC-Nb alloys confront notable challenges in thermal stability and toughness under cyclic fatigue at varying temperatures.Insufficient thermal stability and expedited coalescence of precipitates substanti...In aerospace,BBC-Nb alloys confront notable challenges in thermal stability and toughness under cyclic fatigue at varying temperatures.Insufficient thermal stability and expedited coalescence of precipitates substantially accelerates the degradation of alloys at elevated temperatures.Here,a Nb alloy with impressive thermal stability and mechanical properties was designed using theoretical calculations and a two-step graded heat treatment process.The superlative properties of the Nb alloy are primarily associated with the NbC hierarchical structures,i.e.,stable nanoparticles in Nb-BCC grains and discontinuous microparticles at grain boundaries(GBs).The hierarchical carbides configuration avoids continuous precipitation of carbides at GBs and preferential coarsening within the grains.The process involves precipitating ZrC nanoparticles at 1350℃,then stabilizing NbC at 1800℃ by replacing Zr with Nb.Nb-FCC nanophases enveloping NbC prevent coarsening and have strong relationships with both NbC nanoparticles and matrix.The concept of fine-tuning NbC precipitation within grains and introducing NbC at GBs with a substitution method offers a strategy for high-strength,heat-resistant materials.展开更多
Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature...Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature environments is based on contact ion pairs(CIPs)dominated solvation structure here.In detail,in the long-chain phosphate ester-based electrolyte,the spatial site-blocking effect enables the strong solvation co-solvent ether(diethylene glycol dimethyl ether,G2)to exhibit strong ion-dipole interactions,further multicomponent competitive coordination maintaining the CIP,balancing electrode kinetics,and optimizing the high-temperature interphases.High-temperature in-situ Raman spectroscopy monitors the changes in the stable solvent structure during charge/discharge processes for the first time,and time of flight secondary ion mass spectrometry(TOF-SIMS)reveals the stable solid electrolyte interphase(SEI)with full-depth enrichment of the inorganic component.Benefiting from the high-temperature interfacial chemistry-dependent solvent structure,the advanced electrolyte enables stable cycling of 1.6 Ah 18650 batterie at 100-125℃and discharging with high current pulses(~1.83 A)at 150℃,which has rarely been reported so far.In addition,pin-pricking of 18650 batteries at100%state of charge(SoC)without fire or smoke and the moderate thermal runaway temperature(187℃)tested via the accelerating rate calorimetry(ARC)demonstrate the excellent safety of the optimized electrolyte.展开更多
BACKGROUND Serum retinol-binding protein(RBP)is the primary transport protein of circulating vitamin A.RBP has a crucial role in maintaining nutrient metabolism and physiologic homeostasis.Several studies have indicat...BACKGROUND Serum retinol-binding protein(RBP)is the primary transport protein of circulating vitamin A.RBP has a crucial role in maintaining nutrient metabolism and physiologic homeostasis.Several studies have indicated that serum RBP participates in the progression of diabetes and diabetes-related complications.However,the impact of serum RBP on lower limb atherosclerosis has not been determined in individuals with type 2 diabetes mellitus(T2DM).AIM To determine the association between serum RBP and lower limb atherosclerosis in individuals with T2DM.METHODS This retrospective study enrolled 4428 eligible T2DM patients and divided the patients into non-lower limb atherosclerosis(n=1913)and lower limb atherosclerosis groups(n=2515)based on lower limb arterial ultrasonography results.At hospital admission,baseline serum RBP levels were assessed,and all subjects were categorized into three groups(Q1-Q3)based on RBP tertiles.Logistic regression,restricted cubic spline regression,subgroup analysis,and machine learning were used to assess the association between RBP levels and lower limb atherosclerosis risk.RESULTS Among 4428 individuals with T2DM,2515(56.80%)had lower limb atherosclerosis.Logistic analysis showed that lower limb atherosclerosis risk increased by 1%for every 1 unit rise in serum RBP level(odds ratio=1.01,95%confidence interval:1.00-1.02,P=0.004).Patients in the highest tertile group(Q3)had a higher lower limb atherosclerosis risk compared to the lowest tertile group(Q1)(odds ratio=1.36,95%confidence interval:1.12-1.67,P=0.002).The lower limb atherosclerosis risk gradually increased with an increase in RBP tertile(P for trend=0.005).Restricted cubic spline analysis indicated a linear correlation between serum RBP levels and lower limb atherosclerosis risk(non-linear P<0.05).Machine learning demonstrated the significance and diagnostic value of serum RBP in predicting lower limb atherosclerosis risk.CONCLUSION Elevated serum RBP levels correlate with an increased lower limb atherosclerosis risk in individuals with T2DM.展开更多
BACKGROUND Poor glycaemic control in patients with type 2 diabetes mellitus(T2DM)is often accompanied by multiple complications,including diabetic nephropathy(DN),diabetic retinopathy(DR),diabetic peripheral neuropath...BACKGROUND Poor glycaemic control in patients with type 2 diabetes mellitus(T2DM)is often accompanied by multiple complications,including diabetic nephropathy(DN),diabetic retinopathy(DR),diabetic peripheral neuropathy(DPN),and cardiac structural abnormality left ventricular hypertrophy(LVH).Early identification of high-risk populations for these complications and the implementation of intervention measures are crucial for improving patient outcomes.Serum alpha-1-microglobulin(α1-MG),a multifunctional protein synthesized by the liver and lymphocytes,has been considered a potential biomarker of diabetes-related diseases in recent years.AIM To investigate the associations of serumα1-MG with DN,DR,DPN,and LVH in T2DM patients and its predictive value.METHODS This retrospective study included 5045 T2DM patients.The study participants were stratified into quartiles according to their serumα1-MG levels.Multivariate logistic regression,restricted cubic spline,and explainable machine learning models were employed for risk assessment and feature importance evaluation.RESULTS Increasedα1-MG levels were observed in patients with DN,DR,DPN,and LVH(all P<0.001).Multivariate logistic regression revealed that each standard deviation increase inα1-MG was associated with an 84%increase in DN risk(OR:1.84,95%CI:1.62-2.10,P<0.001),a 17%increase in DR risk(OR:1.17,95%CI:1.07-1.28,P<0.001),a 14%increase in DPN risk(OR:1.14,95%CI:1.03-1.27,P=0.014),and a 28%increase in LVH risk(OR:1.28,95%CI:1.18-1.38,P<0.001).Subgroup analyses and machine learning confirmed the associations of elevatedα1-MG with these complications in T2DM patients.CONCLUSION Elevated serumα1-MG levels were independently associated with increased risks of DN,DR,DPN,and LVH in T2DM patients,suggesting its potential as a predictive biomarker.展开更多
The first-ever synthesis of the unknown furo[2,3:4,5]pyrimido[1,2-b]indazole skeleton was demonstrated based on the undiscovered tetra-functionalization of enaminones,with simple substrates and reaction conditions.The...The first-ever synthesis of the unknown furo[2,3:4,5]pyrimido[1,2-b]indazole skeleton was demonstrated based on the undiscovered tetra-functionalization of enaminones,with simple substrates and reaction conditions.The key to realizing this process lies in the multiple trapping of the in situ generated ketenimine cation by the 3-aminoindazole,which results in the formation of four new chemical bonds and two new rings in one pot.Moreover,the products of this new reaction were found to exhibit aggregationinduced emission(AIE)without modification.展开更多
Leaf color is one of the most important breeding traits,which is closely related to the growth,development,yield and quality of Chinese cabbage.Leaf color mutants are precious materials for studying the molecular mech...Leaf color is one of the most important breeding traits,which is closely related to the growth,development,yield and quality of Chinese cabbage.Leaf color mutants are precious materials for studying the molecular mechanisms of photosynthesis,chlorophyll metabolism and chloroplast signal transduction pathways.The types of mutations included dark green,virescent,xanthas,and striped leaves.Notably,light-regulated leaf color mutants such as var1,var2,im,thf1 and pvsl1 have been reported in Arabidopsis thaliana and common beans(Xu et al.,2021).展开更多
To alleviate ultrafiltration(UF) membrane fouling, the pre-coagulation of poly-aluminum chloride(PACl) with the aid of chitosan(CTS) was conducted for synthetic humic acid–kaolin water treatment. Pre-coagulation of t...To alleviate ultrafiltration(UF) membrane fouling, the pre-coagulation of poly-aluminum chloride(PACl) with the aid of chitosan(CTS) was conducted for synthetic humic acid–kaolin water treatment. Pre-coagulation of three molecular weights(MW) CTSs(50–190 kDa(CTSL), 190–310 kDa(CTSM) and 310–375 kDa(CTSH)) was optimized with slow-mixing speeds of 30, 60 and 90 r/min, respectively. The removal efficiency and floc properties as well as membrane fouling were analyzed, and were compared to results obtained by conventional coagulation with PACl. Results showed that variations in floc properties could be ascribed to the coagulation mechanisms of CTS_L/CTS_M/CTS_H at different slow-mixing speeds, resulting in reduced UF membrane fouling. Specifically, at the low speed of 30 r/min, all three CTS types produced flocs with similar properties, while CTSLresulted in the lowest removal efficiency and aggravated irreversible fouling. At the appropriate speed of 60 r/min, CTSMgenerated the most compact flocs with the combined effects of bridging and path mechanisms. The compact cake layer formed could alleviate irreversible fouling,which was beneficial for prolonging the operation of the UF membrane. At the high speed of90 r/min, CTSHformed fragile flocs and aggravated irreversible membrane fouling. We considered membrane fouling to be affected by floc properties and the resultant removal efficiency, which was governed by the MW of the CTS used and the slow-mixing speed applied as well.展开更多
Diamond,with ultrahigh hardness,high wear resistance,high thermal conductivity,and so forth,has attracted worldwide attention.However,researchers found emergent reactions at the interfaces between diamond and ferrous ...Diamond,with ultrahigh hardness,high wear resistance,high thermal conductivity,and so forth,has attracted worldwide attention.However,researchers found emergent reactions at the interfaces between diamond and ferrous materials,which significantly affects the performance of diamond-based devices.Herein,combing experiments and theoretical calculations,taking diamond–iron(Fe)interface as a prototype,the counter-diffusion mechanism of Fe/carbon atoms has been established.Surprisingly,it is identified that Fe and diamond first form a coherent interface,and then Fe atoms diffuse into diamond and prefer the carbon vacancies sites.Meanwhile,the relaxed carbon atoms diffuse into the Fe lattice,forming Fe_(3)C.Moreover,graphite is observed at the Fe_(3)C surface when Fe_(3)C is over-saturated by carbon atoms.The present findings are expected to offer new insights into the atomic mechanism for diamondferrous material's interfacial reactions,benefiting diamond-based device applications.展开更多
Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and horm...Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and hormone metabolism, nutritional balances, and results in ion toxicity in plants. To better understand the mechanisms of salt-induced growth inhibition in Chinese cabbage, RNA-seq and physiological index determination were conducted to explore the impacts of salt stress on carbon cycle metabolism and photosynthesis in Chinese cabbage. Here, we found that the number of thylakoids and grana lamellae and the content of starch granules and chlorophyll in the leaves of Chinese cabbage under salt stress showed a time-dependent response, first increasing and then decreasing. Chinese cabbage increased the transcript levels of genes related to the photosynthetic apparatus and carbon metabolism under salt stress, probably in an attempt to alleviate damage to the photosynthetic system and enhance CO_(2) fixation and energy metabolism. The transcription of genes related to starch and sucrose synthesis and degradation were also enhanced;this might have been an attempt to maintain intracellular osmotic pressure by increasing soluble sugar concentrations. Soluble sugars could also be used as potential reactive oxygen species(ROS) scavengers, in concert with peroxidase(POD)enzymes, to eliminate ROS that accumulate during metabolic processes. Our study characterizes the synergistic response network of carbon metabolism and photosynthesis under salt stress.展开更多
Chronic prostatitis/chronic pelvic pain syndrome(CP/CPPS)is highly prevalent worldwide and poses a significant threat to men’s health,particularly affecting young men.However,the exact causes and mechanisms behind CP...Chronic prostatitis/chronic pelvic pain syndrome(CP/CPPS)is highly prevalent worldwide and poses a significant threat to men’s health,particularly affecting young men.However,the exact causes and mechanisms behind CP/CPPS remain unclear,leading to challenges in its treatment.In this research,a CP/CPPS rat model was established with complete Freund’s adjuvant(CFA),and berberine hydrochloride was administered through daily gavage to assess its therapeutic effects.The alterations in the gut microbiome induced by CP/CPPS and berberine hydrochloride were investigated through 16S ribosomal RNA sequencing of cecum content and colonic epithelial cells.To investigate the impact of the gut microbiome on CP/CPPS,a pseudo germ-free rat model was established,and fecal microbiome transplantation(FMT)was performed on these rats.In all,berberine hydrochloride demonstrated effective reduction of inflammation and oxidative stress in the prostate,offering significant therapeutic advantages for CP/CPPS.Through analysis of the gut microbiome using 16S ribosome RNA sequencing,distinct differences were observed between CP/CPPS rats and control rats,and Clostridium butyricum was identified as a key bacteria.Pseudo germ-free rats that underwent FMT from CP/CPPS rats or rats treated with berberine hydrochloride displayed varying levels of inflammatory cytokine production,oxidative stress,and activity of associated signaling pathways.In conclusion,the therapeutic potential of berberine hydrochloride in addressing CP/CPPS is highly significant.The gut microbiome has emerged as a critical factor in the development of CP/CPPS and plays a pivotal role in mediating the therapeutic effects of berberine hydrochloride.展开更多
The development of passive NO_(x)adsorbers with cost-benefit and high NO_(x)storage capacity remains an on-going challenge to after-treatment technologies at lower temperatures associated with cold-start NO_(x)emissio...The development of passive NO_(x)adsorbers with cost-benefit and high NO_(x)storage capacity remains an on-going challenge to after-treatment technologies at lower temperatures associated with cold-start NO_(x)emissions.Herein,Cs_(1)Mg_(3)Al catalyst prepared by sol-gel method was cyclic tested in NO_(x)storage under 5 vol%water.At 100°C,the NO_(x)storage capacity(1219 μmol g^(-1))was much higher than that of Pt/BaO/Al_(2)O_(3)(610 μmol g^(-1)).This provided new insights for non-noble metal catalysts in low-temperature passive NO_(x)adsorption.The addition of Cs improved the mobility of oxygen species and thus improved the NO_(x)storage capacity.The XRD,XPS,IR spectra and in situ DRIFTs with NH3 probe showed an interaction between CsO_(x)and AlO_(x)sites via oxygen species formed on Cs_(1)Mg_(3)Al catalyst.The improved mobility of oxygen species inferred from O2-TPD was consistent with high NO_(x)storage capacity related to enhanced formation of nitrate and additional nitrite species by NO_(x)oxidation.Moreover,the addition of Mg might improve the stability of Cs_(1)Mg_(3)Al by stabilizing surface active oxygen species in cyclic experiments.展开更多
Vanadium disulfide(VS_(2)) as a typical two-dimensional transition metal chalcogenide has excellent competitiveness for sodium-ion storage due to its wide layer spacing(0.575 nm),high theoretical capacity of 932mAh...Vanadium disulfide(VS_(2)) as a typical two-dimensional transition metal chalcogenide has excellent competitiveness for sodium-ion storage due to its wide layer spacing(0.575 nm),high theoretical capacity of 932mAh·g^(-1) originating from multi-electron electrochemical redox.However,continuous sodiation process accompanied by crystal structural evolution and collapse cause rapid capacity decaying.Herein,novel few-layer VS_(2)nanosheets with open(001) crystal planes are in-situ constructed on reduced graphene oxide to solve these issues mentioned above.It indicates that few-layer VS_(2)provides more Na^(+) storage activity due to the low Na^(+)surface migration energy barrier on exposed crystal(001)planes.The flexible and high electronic conductivity of carbon matrix also effectively builds multi-level buffer structure and electron transport kinetics to boost the Na^(+)insertion/conversion reactive activity on VS_(2) as well as Na^(+) pseudocapacitance storage kinetics on edges and defects of nano sheets.Those coupling effects result in high rate capability and long cycling stability as a battery/capacitor anode.It delivers conspicuous high energy density of 81 and 40 Wh·kg^(-1) at power density of 118 and 10,286W·kg^(-1),as well as 80% energy retention rate after 5000cycles,confirming its great application potential in sodiumbased storage devices.展开更多
Diamond possesses excellent thermal conductivity and tunable bandgap.Currently,the high-pressure,high-temperature,and chemical vapor deposition methods are the most promising strategies for the commercial-scale produc...Diamond possesses excellent thermal conductivity and tunable bandgap.Currently,the high-pressure,high-temperature,and chemical vapor deposition methods are the most promising strategies for the commercial-scale production of synthetic diamond.Although diamond has been extensively employed in jewelry and cutting/grinding tasks,the realization of its high-end applications through microstructure engineering has long been sought.Herein,we discuss the microstructures encountered in diamond and further concentrate on cutting-edge investigations utilizing electron microscopy techniques to illuminate the transition mechanism between graphite and diamond during the synthesis and device constructions.The impacts of distinct microstructures on the electrical applications of diamond,especially the photoelectrical,electrical,and thermal properties,are elaborated.The recently reported elastic and plastic deformations revealed through in situ microscopy techniques are also summarized.Finally,the limitations,perspectives,and corresponding solutions are proposed.展开更多
Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures....Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures.Herein,a flame-retardant,low-cost and thermally stable long chain phosphate ester based(tributyl phosphate,TBP)electrolyte is reported,which can effectively enhance the cycling stability of highly loaded high-nickel LMBs with high safety through co-solvation strategy.The interfacial compatibility between TBP and electrode is effectively improved using a short-chain ether(glycol dimethyl ether,DME),and a specially competitive solvation structure is further constructed using lithium borate difluorooxalate(LiDFOB)to form the stable and inorganic-rich electrode interphases.Benefiting from the presence of the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)enriched with LiF and Li_(x)PO_(y)F_(z),the electrolyte demonstrates excellent cycling stability assembled using a 50μm lithium foil anode in combination with a high loading NMC811(15.4 mg cm^(-2))cathode,with 88%capacity retention after 120 cycles.Furthermore,the electrolyte exhibits excellent high-temperature characteristics when used in a 1-Ah pouch cell(N/P=0.26),and higher thermal runaway temperature(238℃)in the ARC(accelerating rate calorimeter)demonstrating high safety.This novel electrolyte adopts long-chain phosphate as the main solvent for the first time,and would provide a new idea for the development of extremely high safety and high-temperature electrolytes.展开更多
Electrochemical lithium extraction from salt lakes is an effective strategy for obtaining lithium at a low cost.Nevertheless,the elevated Mg:Li ratio and the presence of numerous coexisting ions in salt lake brines gi...Electrochemical lithium extraction from salt lakes is an effective strategy for obtaining lithium at a low cost.Nevertheless,the elevated Mg:Li ratio and the presence of numerous coexisting ions in salt lake brines give rise to challenges,such as prolonged lithium extraction periods,diminished lithium extraction efficiency,and considerable environmental pollution.In this work,Li FePO4(LFP)served as the electrode material for electrochemical lithium extraction.The conductive network in the LFP electrode was optimized by adjusting the type of conductive agent.This approach resulted in high lithium extraction efficiency and extended cycle life.When the single conductive agent of acetylene black(AB)or multiwalled carbon nanotubes(MWCNTs)was replaced with the mixed conductive agent of AB/MWCNTs,the average diffusion coefficient of Li+in the electrode increased from 2.35×10^(-9)or 1.77×10^(-9)to 4.21×10^(-9)cm^(2)·s^(-1).At the current density of 20 mA·g^(-1),the average lithium extraction capacity per gram of LFP electrode increased from 30.36 mg with the single conductive agent(AB)to 35.62 mg with the mixed conductive agent(AB/MWCNTs).When the mixed conductive agent was used,the capacity retention of the electrode after 30 cycles reached 82.9%,which was considerably higher than the capacity retention of 65.8%obtained when the single AB was utilized.Meanwhile,the electrode with mixed conductive agent of AB/MWCNTs provided good cycling performance.When the conductive agent content decreased or the loading capacity increased,the electrode containing the mixed conductive agent continued to show excellent electrochemical performance.Furthermore,a self-designed,highly efficient,continuous lithium extraction device was constructed.The electrode utilizing the AB/MWCNT mixed conductive agent maintained excellent adsorption capacity and cycling performance in this device.This work provides a new perspective for the electrochemical extraction of lithium using LFP electrodes.展开更多
As one promising carbon-based material,sp^(3)-hybrid carbon nitride has been predicted with various novel physicochemical properties.However,the synthesis of sp^(3)-hybrid carbon nitride is still limited by the nanaos...As one promising carbon-based material,sp^(3)-hybrid carbon nitride has been predicted with various novel physicochemical properties.However,the synthesis of sp^(3)-hybrid carbon nitride is still limited by the nanaoscale,low crystallinity,complex source,and expensive instruments.Herein,we have presented a facile approach to the sp^(3)-hybrid carbon nitride nano/micro-crystals with microwave-assisted confining growth and liquid exfoliation.Actually,the carbon nitride nano/micro-crystals can spontaneously emerge and grow in the microwave-assisted polymerization of citric acid and urea,and the liquid exfoliation can break the bulk disorder polymer to retrieve the highly crystalline carbon nitride nano/micro-crystals.The obtained carbon nitride nano/micro-crystals present superior blue light absorption strength and surprising photoluminescence quantum yields of 57.96% in ethanol and 18.05%in solid state.The experimental characterizations and density functional theory calculations reveal that the interface-trapped localized exciton may contribute to the excellent intrinsic light emission capability of carbon nitride nano/micro-crystals and the interparticle staggered stacking will prevent the aggregation-caused-quenching partially.Finally,the carbon nitride nano/micro-crystals are demonstrated to be potentially useful as the phosphor medium in light-emitting-diode for interrupting blue light-induced eye damage.This work paves new light on the synthesis strategy of sp^(3)-hybrid carbon nitride materials and thus may push forward the development of multiple carbon nitride research.展开更多
Sodium-based storage devices based on conversion-type metal sulfide anodes have attracted great atten-tion due to their multivalent ion redox reaction ability.However,they also suffer from sodium polysul-fides(NaPSs)s...Sodium-based storage devices based on conversion-type metal sulfide anodes have attracted great atten-tion due to their multivalent ion redox reaction ability.However,they also suffer from sodium polysul-fides(NaPSs)shuttling problems during the sluggish Na^(+) redox process,leading to"voltage failure"and rapid capacity decay.Herein,a metal cobalt-doping vanadium disulfide(Co-VS_(2))is proposed to simulta-neously accelerate the electrochemical reaction of VS_(2) and enhance the bidirectional redox of soluble NaPSs.It is found that the strong adsorption of NaPSs by V-Co alloy nanoparticles formed in situ during the conversion reaction of Co-VS_(2) can effectively inhibit the dissolution and shuttle of NaPSs,and ther-modynamically reduce the formation energy barrier of the reaction path to effectively drive the complete conversion reaction,while the metal transition of Co elements enhances reconversion kinetics to achieve high reversibility.Moreover,Co-VS_(2) also produce abundant sulfur vacancies and unsaturated sulfur edge defects,significantly improve ionic/electron diffusion kinetics.Therefore,the Co-VS_(2) anode exhibits ultrahigh rate capability(562 mA h g^(-1) at 5 A g^(-1)),high initial coulombic efficiency(~90%)and 12,000 ultralong cycle life with capacity retention of 90%in sodium-ion batteries(SIBs),as well as impressive energy/power density(118 Wh kg^(-1)/31,250 W kg^(-1))and over 10.000 stable cycles in sodium-ion hybrid capacitors(SIHCs).Moreover,the pouch cell-type SIHC displays a high-energy density of 102 Wh kg^(-1) and exceed 600 stable cycles.This work deepens the understanding of the electrochemical reaction mechanism of conversion-type metal sulfide anodes and provides a valuable solution to the shuttlingofNaPSs inSIBsandSIHCs.展开更多
基金the Scientific Research Innovation Capability Support Project for Young Faculty(ZYGXQNJSKYCXNLZCXM-H8)Fundamental Research Funds for the Central Universities(2024ZYGXZR077)+3 种基金Guangdong Basic and Applied Basic Research Foundation(2023B1515120006)Guangzhou Basic and Applied Basic Research Foundation(2024A04J5776)the Research Fund(2023QN10Y421)Guangzhou Talent Recruitment Team Program(2024D03J0004),all related to this study.
文摘Osteoporosis is a known risk factor for rotator cuff tears(RCTs),but the causal correlation and underlying mechanisms remain unclear.This study aims to evaluate the impact of osteoporosis on RCT risk and investigate their genetic associations.Using data from the UK Biobank(n=457871),cross-sectional analyses demonstrated that osteoporosis was significantly associated with an increased risk of RCTs(adjusted OR[95%CI]=1.38[1.25–1.52]).A longitudinal analysis of a subset of patients(n=268117)over 11 years revealed that osteoporosis increased the risk of RCTs(adjusted HR[95%CI]=1.56[1.29–1.87]),which is notably varied between sexes in sex-stratified analysis.Causal inference methods,including propensity score matching,inverse probability weighting,causal random forest and survival random forest models further confirmed the causal effect,both from cross-sectional and longitudinal perspectives.
基金supported by the National Natural Science Foundation of China(Nos.51978576,42207021 and 52370177)Sichuan Province Science and Technology Support Program(Nos.2023ZHCG0058,2025ZNSFSC0194 and 2024NSFSC0131)+1 种基金the Fundamental Research Funds for the Central Universities(No.2682024ZTPY012)the Science and Technology Project of Sichuan Tobacco Company of China National Tobacco Corporation(Nos.SCYC202109 and SCYC202409)。
文摘Prominent cadmium(Cd)pollution and widespread phoxim(p H)use hinder the growth and medicinal value of Ligusticum chuanxiong Hort.(Chuanxiong).While bioremediation by rhizobacteria helps plants counter pollutants,the specific roles of indigenous resistant consortia collected from polluted soils in immobilizing heavy metals,degrading pesticides,and enhancing plant stress tolerance remain insufficiently explored.Here,an indigenous pollutant-resistant consortium(RM)was developed from a highly Cd-polluted area(14.85 mg/kg Cd)as a bioremediation strategy to alleviate stress on Chuanxiong.The RM was specifically enriched with a Cd-p H co-resistant strain,Halomonas spp.TS2.Through16S r RNA sequencing,active microorganisms within RM was identified,including Bacillus,Acinetobacter,Enterococcus,Paraclostridium,and Staphylococcus.Pot experiments demonstrated that RM increased Chuanxiong biomass by 93.38%under Cd-contaminated and by 32.89%under Cd-p H co-contaminated.Furthermore,RM enhanced p H degradation,stabilized soil compounds,and reduced Cd bioavailability,thereby mitigating oxidative damage and altering the diversity and composition of Cd-p H-resistant organisms.These results indicate that utilizing indigenous microbial consortia as a bioremediation strategy can effectively improve soil health and enhance the sustainable cultivation of medicinal herbs in environments heavily contaminated.
基金supported by the Chinese National Natural Science Foundation(92268118,82071396,82271199)the Shaanxi Provincial Key R&D Foundation(2021ZDLSF03-09)+3 种基金the Scientific Research Program Funded by Shaanxi Provincial Education Department(22JK0550)the Fundamental Research Funds for the Central Universities(GK202201013,GK202202006,GK202305001)the Excellent Graduate Training Program of Shaanxi Normal University(LHRCYB23003)Tian Jiabing Scholar Program.
文摘Immunosuppressants currently approved for the treatment of autoimmune diseases and organ transplant rejection present diverse adverse effects that impair the life quality of patients.Therefore,the development of novel immunomodulators with high efficiency and low toxicity is essential.Ellagic acid(EA),a natural polyphenol compound widely distributed in berries,is metabolically transformed by gut microbiome to exert systemic health benefits.Here,we identified that intraperitoneal administration of EA with no cytotoxicity,beyond its wellknown oral metabolic fate,effectively decreased clinical severity and central nervous system(CNS)inflammation/demyelination in experimental autoimmune encephalomyelitis,a mouse model of an autoimmune disease multiple sclerosis.Interestingly,intraperitoneal EA administration at incredibly low doses(0.1 mg/(kg·day))is dose-sparing with fingolimod(FTY720),the first FDA-approved oral drug for MS.In addition,intraperitoneal EA also ameliorated the brain damage in a neuromyelitis optica(NMO)model,and significantly prevented the immune rejection of allograft skin graft.Evidence from pharmacological studies combined with RNA-seq indicate that prototype EA functions by a mechanism that involves direct inhibition of casein kinase II(CKII)to suppress the expression of IL-17 and promote the expression of Cpt1a to regulate T helper cell 17 differentiation.In conclusion,our study demonstrates that the prototype EA entering the blood circulation acts as a novel therapeutic immunomodulator for the treatment of autoimmune diseases and transplant rejection through the CKII-mediated Janus kinase/signal transducer and activator of transcription 3 Cpt1a signaling pathway.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52471025 and 51901252)the Natural Science Foundation of Hunan Province(Grant No.2023JJ30684)the Natural Science Foundation of Changsha Municipal(Grant No.kq2202091).
文摘In aerospace,BBC-Nb alloys confront notable challenges in thermal stability and toughness under cyclic fatigue at varying temperatures.Insufficient thermal stability and expedited coalescence of precipitates substantially accelerates the degradation of alloys at elevated temperatures.Here,a Nb alloy with impressive thermal stability and mechanical properties was designed using theoretical calculations and a two-step graded heat treatment process.The superlative properties of the Nb alloy are primarily associated with the NbC hierarchical structures,i.e.,stable nanoparticles in Nb-BCC grains and discontinuous microparticles at grain boundaries(GBs).The hierarchical carbides configuration avoids continuous precipitation of carbides at GBs and preferential coarsening within the grains.The process involves precipitating ZrC nanoparticles at 1350℃,then stabilizing NbC at 1800℃ by replacing Zr with Nb.Nb-FCC nanophases enveloping NbC prevent coarsening and have strong relationships with both NbC nanoparticles and matrix.The concept of fine-tuning NbC precipitation within grains and introducing NbC at GBs with a substitution method offers a strategy for high-strength,heat-resistant materials.
基金supported by the National Natural Science Foundation of China(grant no.52072322,52202235)the Department of Science and Technology of Sichuan Province(CN)(grant no.23GJHZ0147)the Research and Innovation Fund for Graduate Students of Southwest Petroleum University(No.:2022KYCX111)。
文摘Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature environments is based on contact ion pairs(CIPs)dominated solvation structure here.In detail,in the long-chain phosphate ester-based electrolyte,the spatial site-blocking effect enables the strong solvation co-solvent ether(diethylene glycol dimethyl ether,G2)to exhibit strong ion-dipole interactions,further multicomponent competitive coordination maintaining the CIP,balancing electrode kinetics,and optimizing the high-temperature interphases.High-temperature in-situ Raman spectroscopy monitors the changes in the stable solvent structure during charge/discharge processes for the first time,and time of flight secondary ion mass spectrometry(TOF-SIMS)reveals the stable solid electrolyte interphase(SEI)with full-depth enrichment of the inorganic component.Benefiting from the high-temperature interfacial chemistry-dependent solvent structure,the advanced electrolyte enables stable cycling of 1.6 Ah 18650 batterie at 100-125℃and discharging with high current pulses(~1.83 A)at 150℃,which has rarely been reported so far.In addition,pin-pricking of 18650 batteries at100%state of charge(SoC)without fire or smoke and the moderate thermal runaway temperature(187℃)tested via the accelerating rate calorimetry(ARC)demonstrate the excellent safety of the optimized electrolyte.
基金The study was approved by the ethics committee of Southwest Hospital,the First Affiliated Hospital of Army Medical University of Chinese People's Liberation Army(No.KY2024007).
文摘BACKGROUND Serum retinol-binding protein(RBP)is the primary transport protein of circulating vitamin A.RBP has a crucial role in maintaining nutrient metabolism and physiologic homeostasis.Several studies have indicated that serum RBP participates in the progression of diabetes and diabetes-related complications.However,the impact of serum RBP on lower limb atherosclerosis has not been determined in individuals with type 2 diabetes mellitus(T2DM).AIM To determine the association between serum RBP and lower limb atherosclerosis in individuals with T2DM.METHODS This retrospective study enrolled 4428 eligible T2DM patients and divided the patients into non-lower limb atherosclerosis(n=1913)and lower limb atherosclerosis groups(n=2515)based on lower limb arterial ultrasonography results.At hospital admission,baseline serum RBP levels were assessed,and all subjects were categorized into three groups(Q1-Q3)based on RBP tertiles.Logistic regression,restricted cubic spline regression,subgroup analysis,and machine learning were used to assess the association between RBP levels and lower limb atherosclerosis risk.RESULTS Among 4428 individuals with T2DM,2515(56.80%)had lower limb atherosclerosis.Logistic analysis showed that lower limb atherosclerosis risk increased by 1%for every 1 unit rise in serum RBP level(odds ratio=1.01,95%confidence interval:1.00-1.02,P=0.004).Patients in the highest tertile group(Q3)had a higher lower limb atherosclerosis risk compared to the lowest tertile group(Q1)(odds ratio=1.36,95%confidence interval:1.12-1.67,P=0.002).The lower limb atherosclerosis risk gradually increased with an increase in RBP tertile(P for trend=0.005).Restricted cubic spline analysis indicated a linear correlation between serum RBP levels and lower limb atherosclerosis risk(non-linear P<0.05).Machine learning demonstrated the significance and diagnostic value of serum RBP in predicting lower limb atherosclerosis risk.CONCLUSION Elevated serum RBP levels correlate with an increased lower limb atherosclerosis risk in individuals with T2DM.
文摘BACKGROUND Poor glycaemic control in patients with type 2 diabetes mellitus(T2DM)is often accompanied by multiple complications,including diabetic nephropathy(DN),diabetic retinopathy(DR),diabetic peripheral neuropathy(DPN),and cardiac structural abnormality left ventricular hypertrophy(LVH).Early identification of high-risk populations for these complications and the implementation of intervention measures are crucial for improving patient outcomes.Serum alpha-1-microglobulin(α1-MG),a multifunctional protein synthesized by the liver and lymphocytes,has been considered a potential biomarker of diabetes-related diseases in recent years.AIM To investigate the associations of serumα1-MG with DN,DR,DPN,and LVH in T2DM patients and its predictive value.METHODS This retrospective study included 5045 T2DM patients.The study participants were stratified into quartiles according to their serumα1-MG levels.Multivariate logistic regression,restricted cubic spline,and explainable machine learning models were employed for risk assessment and feature importance evaluation.RESULTS Increasedα1-MG levels were observed in patients with DN,DR,DPN,and LVH(all P<0.001).Multivariate logistic regression revealed that each standard deviation increase inα1-MG was associated with an 84%increase in DN risk(OR:1.84,95%CI:1.62-2.10,P<0.001),a 17%increase in DR risk(OR:1.17,95%CI:1.07-1.28,P<0.001),a 14%increase in DPN risk(OR:1.14,95%CI:1.03-1.27,P=0.014),and a 28%increase in LVH risk(OR:1.28,95%CI:1.18-1.38,P<0.001).Subgroup analyses and machine learning confirmed the associations of elevatedα1-MG with these complications in T2DM patients.CONCLUSION Elevated serumα1-MG levels were independently associated with increased risks of DN,DR,DPN,and LVH in T2DM patients,suggesting its potential as a predictive biomarker.
基金supported by the National Natural Science Foundation of China(Nos.21971080,22171098)supported by Chengdu Guibao Science&Technology Co.,Ltd.This work was also supported by the 111 Project(No.B17019)。
文摘The first-ever synthesis of the unknown furo[2,3:4,5]pyrimido[1,2-b]indazole skeleton was demonstrated based on the undiscovered tetra-functionalization of enaminones,with simple substrates and reaction conditions.The key to realizing this process lies in the multiple trapping of the in situ generated ketenimine cation by the 3-aminoindazole,which results in the formation of four new chemical bonds and two new rings in one pot.Moreover,the products of this new reaction were found to exhibit aggregationinduced emission(AIE)without modification.
基金supported by the Natural Science Foundation of Hebei Province(Grant No.C2024204110)the National Key Research and Development Program of China(Grant No.2023YFD1200101-08)+3 种基金the National Natural Science Foundation of China(Grant Nos.32172560,31930098)the Hebei Provincial Natural Science Fund for Distinguished Young(Grant No.C2020204063)the Science Fund for Distinguished Young Scholars of Hebei Province(Grant No.C2021204049)the Innovative Research Group Project of Hebei Natural Science Foundation(Grant No.C2020204111)。
文摘Leaf color is one of the most important breeding traits,which is closely related to the growth,development,yield and quality of Chinese cabbage.Leaf color mutants are precious materials for studying the molecular mechanisms of photosynthesis,chlorophyll metabolism and chloroplast signal transduction pathways.The types of mutations included dark green,virescent,xanthas,and striped leaves.Notably,light-regulated leaf color mutants such as var1,var2,im,thf1 and pvsl1 have been reported in Arabidopsis thaliana and common beans(Xu et al.,2021).
基金supported by the National Natural Science Foundation of China(No.51478010)
文摘To alleviate ultrafiltration(UF) membrane fouling, the pre-coagulation of poly-aluminum chloride(PACl) with the aid of chitosan(CTS) was conducted for synthetic humic acid–kaolin water treatment. Pre-coagulation of three molecular weights(MW) CTSs(50–190 kDa(CTSL), 190–310 kDa(CTSM) and 310–375 kDa(CTSH)) was optimized with slow-mixing speeds of 30, 60 and 90 r/min, respectively. The removal efficiency and floc properties as well as membrane fouling were analyzed, and were compared to results obtained by conventional coagulation with PACl. Results showed that variations in floc properties could be ascribed to the coagulation mechanisms of CTS_L/CTS_M/CTS_H at different slow-mixing speeds, resulting in reduced UF membrane fouling. Specifically, at the low speed of 30 r/min, all three CTS types produced flocs with similar properties, while CTSLresulted in the lowest removal efficiency and aggravated irreversible fouling. At the appropriate speed of 60 r/min, CTSMgenerated the most compact flocs with the combined effects of bridging and path mechanisms. The compact cake layer formed could alleviate irreversible fouling,which was beneficial for prolonging the operation of the UF membrane. At the high speed of90 r/min, CTSHformed fragile flocs and aggravated irreversible membrane fouling. We considered membrane fouling to be affected by floc properties and the resultant removal efficiency, which was governed by the MW of the CTS used and the slow-mixing speed applied as well.
基金supported by the National Natural Science Foundation of China(Grant Nos.12274371,62271450,U21A2070,21805247,12074345)Cross-Disciplinary Innovative Research Group Project of Henan Province(Grant No.232300421004).
文摘Diamond,with ultrahigh hardness,high wear resistance,high thermal conductivity,and so forth,has attracted worldwide attention.However,researchers found emergent reactions at the interfaces between diamond and ferrous materials,which significantly affects the performance of diamond-based devices.Herein,combing experiments and theoretical calculations,taking diamond–iron(Fe)interface as a prototype,the counter-diffusion mechanism of Fe/carbon atoms has been established.Surprisingly,it is identified that Fe and diamond first form a coherent interface,and then Fe atoms diffuse into diamond and prefer the carbon vacancies sites.Meanwhile,the relaxed carbon atoms diffuse into the Fe lattice,forming Fe_(3)C.Moreover,graphite is observed at the Fe_(3)C surface when Fe_(3)C is over-saturated by carbon atoms.The present findings are expected to offer new insights into the atomic mechanism for diamondferrous material's interfacial reactions,benefiting diamond-based device applications.
基金financially supported by the Natural Science Foundation of Hebei Province-Innovation Group Research Project(Grant No.C2020204111)the National Natural Science Foundation of China(Grant No.31930098)+3 种基金the Science Fund for Distinguished Young Scholars of Hebei Province(Grant No.C2021204049)the Hebei Province Outstanding Youth Fund(Grant No.BJ2021024)the Hebei Provincial Key Research Projects(21326344D)Hebei International Joint Research Base of Modern Agricultural Biotechnology.
文摘Chinese cabbage(Brassica rapa ssp. pekinensis) has a long cultivation history and is one of the vegetable crops with the largest cultivation area in China. However, salt stress severely damages photosynthesis and hormone metabolism, nutritional balances, and results in ion toxicity in plants. To better understand the mechanisms of salt-induced growth inhibition in Chinese cabbage, RNA-seq and physiological index determination were conducted to explore the impacts of salt stress on carbon cycle metabolism and photosynthesis in Chinese cabbage. Here, we found that the number of thylakoids and grana lamellae and the content of starch granules and chlorophyll in the leaves of Chinese cabbage under salt stress showed a time-dependent response, first increasing and then decreasing. Chinese cabbage increased the transcript levels of genes related to the photosynthetic apparatus and carbon metabolism under salt stress, probably in an attempt to alleviate damage to the photosynthetic system and enhance CO_(2) fixation and energy metabolism. The transcription of genes related to starch and sucrose synthesis and degradation were also enhanced;this might have been an attempt to maintain intracellular osmotic pressure by increasing soluble sugar concentrations. Soluble sugars could also be used as potential reactive oxygen species(ROS) scavengers, in concert with peroxidase(POD)enzymes, to eliminate ROS that accumulate during metabolic processes. Our study characterizes the synergistic response network of carbon metabolism and photosynthesis under salt stress.
基金supported by grants from the National Natural Science Foundation of China(NSFC,No.82370701 and No.82002701).
文摘Chronic prostatitis/chronic pelvic pain syndrome(CP/CPPS)is highly prevalent worldwide and poses a significant threat to men’s health,particularly affecting young men.However,the exact causes and mechanisms behind CP/CPPS remain unclear,leading to challenges in its treatment.In this research,a CP/CPPS rat model was established with complete Freund’s adjuvant(CFA),and berberine hydrochloride was administered through daily gavage to assess its therapeutic effects.The alterations in the gut microbiome induced by CP/CPPS and berberine hydrochloride were investigated through 16S ribosomal RNA sequencing of cecum content and colonic epithelial cells.To investigate the impact of the gut microbiome on CP/CPPS,a pseudo germ-free rat model was established,and fecal microbiome transplantation(FMT)was performed on these rats.In all,berberine hydrochloride demonstrated effective reduction of inflammation and oxidative stress in the prostate,offering significant therapeutic advantages for CP/CPPS.Through analysis of the gut microbiome using 16S ribosome RNA sequencing,distinct differences were observed between CP/CPPS rats and control rats,and Clostridium butyricum was identified as a key bacteria.Pseudo germ-free rats that underwent FMT from CP/CPPS rats or rats treated with berberine hydrochloride displayed varying levels of inflammatory cytokine production,oxidative stress,and activity of associated signaling pathways.In conclusion,the therapeutic potential of berberine hydrochloride in addressing CP/CPPS is highly significant.The gut microbiome has emerged as a critical factor in the development of CP/CPPS and plays a pivotal role in mediating the therapeutic effects of berberine hydrochloride.
基金supported by the National Natural Science Foundation of China(Grant No.51938014,Grant No.22176217,Grant No.22276215)the Fundamental Research Funds for the Central Universities and the Research Funds of Renmin University of China(No.22XNKJ28).
文摘The development of passive NO_(x)adsorbers with cost-benefit and high NO_(x)storage capacity remains an on-going challenge to after-treatment technologies at lower temperatures associated with cold-start NO_(x)emissions.Herein,Cs_(1)Mg_(3)Al catalyst prepared by sol-gel method was cyclic tested in NO_(x)storage under 5 vol%water.At 100°C,the NO_(x)storage capacity(1219 μmol g^(-1))was much higher than that of Pt/BaO/Al_(2)O_(3)(610 μmol g^(-1)).This provided new insights for non-noble metal catalysts in low-temperature passive NO_(x)adsorption.The addition of Cs improved the mobility of oxygen species and thus improved the NO_(x)storage capacity.The XRD,XPS,IR spectra and in situ DRIFTs with NH3 probe showed an interaction between CsO_(x)and AlO_(x)sites via oxygen species formed on Cs_(1)Mg_(3)Al catalyst.The improved mobility of oxygen species inferred from O2-TPD was consistent with high NO_(x)storage capacity related to enhanced formation of nitrate and additional nitrite species by NO_(x)oxidation.Moreover,the addition of Mg might improve the stability of Cs_(1)Mg_(3)Al by stabilizing surface active oxygen species in cyclic experiments.
基金financially supported by the National Natural Science Foundation of China (Nos.52072322 and 51604250)Sichuan Science and Technology Program (Nos.2022YFG0294 and 2019-GH02-00052-HZ)。
文摘Vanadium disulfide(VS_(2)) as a typical two-dimensional transition metal chalcogenide has excellent competitiveness for sodium-ion storage due to its wide layer spacing(0.575 nm),high theoretical capacity of 932mAh·g^(-1) originating from multi-electron electrochemical redox.However,continuous sodiation process accompanied by crystal structural evolution and collapse cause rapid capacity decaying.Herein,novel few-layer VS_(2)nanosheets with open(001) crystal planes are in-situ constructed on reduced graphene oxide to solve these issues mentioned above.It indicates that few-layer VS_(2)provides more Na^(+) storage activity due to the low Na^(+)surface migration energy barrier on exposed crystal(001)planes.The flexible and high electronic conductivity of carbon matrix also effectively builds multi-level buffer structure and electron transport kinetics to boost the Na^(+)insertion/conversion reactive activity on VS_(2) as well as Na^(+) pseudocapacitance storage kinetics on edges and defects of nano sheets.Those coupling effects result in high rate capability and long cycling stability as a battery/capacitor anode.It delivers conspicuous high energy density of 81 and 40 Wh·kg^(-1) at power density of 118 and 10,286W·kg^(-1),as well as 80% energy retention rate after 5000cycles,confirming its great application potential in sodiumbased storage devices.
基金supported by the National Key Research and Development Program of China (Grant No.2022YFB3608604)National Natural Science Foundation of China (Grant Nos.12274371,52072345,62271450,U21A2070,and 62027816)+1 种基金Natural Science Foundation of Henan Province (Grant Nos.222300420077,222301420037)Foundation for the Returned Overseas Researchers of Henan Province.
文摘Diamond possesses excellent thermal conductivity and tunable bandgap.Currently,the high-pressure,high-temperature,and chemical vapor deposition methods are the most promising strategies for the commercial-scale production of synthetic diamond.Although diamond has been extensively employed in jewelry and cutting/grinding tasks,the realization of its high-end applications through microstructure engineering has long been sought.Herein,we discuss the microstructures encountered in diamond and further concentrate on cutting-edge investigations utilizing electron microscopy techniques to illuminate the transition mechanism between graphite and diamond during the synthesis and device constructions.The impacts of distinct microstructures on the electrical applications of diamond,especially the photoelectrical,electrical,and thermal properties,are elaborated.The recently reported elastic and plastic deformations revealed through in situ microscopy techniques are also summarized.Finally,the limitations,perspectives,and corresponding solutions are proposed.
基金supported by the National Natural Science Foundation of China (grant No.52072322)the Department of Science and Technology of Sichuan Province (CN) (grant no.23GJHZ0147,23ZDYF0262,2022YFG0294)Research and Innovation Fund for Graduate Students of Southwest Petroleum University (No.:2022KYCX111)。
文摘Safety remains a persistent challenge for high-energy-density lithium metal batteries(LMBs).The development of safe and non-flammable electrolytes is especially important in harsh conditions such as high temperatures.Herein,a flame-retardant,low-cost and thermally stable long chain phosphate ester based(tributyl phosphate,TBP)electrolyte is reported,which can effectively enhance the cycling stability of highly loaded high-nickel LMBs with high safety through co-solvation strategy.The interfacial compatibility between TBP and electrode is effectively improved using a short-chain ether(glycol dimethyl ether,DME),and a specially competitive solvation structure is further constructed using lithium borate difluorooxalate(LiDFOB)to form the stable and inorganic-rich electrode interphases.Benefiting from the presence of the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)enriched with LiF and Li_(x)PO_(y)F_(z),the electrolyte demonstrates excellent cycling stability assembled using a 50μm lithium foil anode in combination with a high loading NMC811(15.4 mg cm^(-2))cathode,with 88%capacity retention after 120 cycles.Furthermore,the electrolyte exhibits excellent high-temperature characteristics when used in a 1-Ah pouch cell(N/P=0.26),and higher thermal runaway temperature(238℃)in the ARC(accelerating rate calorimeter)demonstrating high safety.This novel electrolyte adopts long-chain phosphate as the main solvent for the first time,and would provide a new idea for the development of extremely high safety and high-temperature electrolytes.
基金financially supported by the National Natural Science Foundation of China(No.52072322)the Department of Science and Technology of Sichuan Province,China(Nos.23GJHZ0147,23ZDYF0262,2022YFG0294,and 2019-GH02-00052-HZ)。
文摘Electrochemical lithium extraction from salt lakes is an effective strategy for obtaining lithium at a low cost.Nevertheless,the elevated Mg:Li ratio and the presence of numerous coexisting ions in salt lake brines give rise to challenges,such as prolonged lithium extraction periods,diminished lithium extraction efficiency,and considerable environmental pollution.In this work,Li FePO4(LFP)served as the electrode material for electrochemical lithium extraction.The conductive network in the LFP electrode was optimized by adjusting the type of conductive agent.This approach resulted in high lithium extraction efficiency and extended cycle life.When the single conductive agent of acetylene black(AB)or multiwalled carbon nanotubes(MWCNTs)was replaced with the mixed conductive agent of AB/MWCNTs,the average diffusion coefficient of Li+in the electrode increased from 2.35×10^(-9)or 1.77×10^(-9)to 4.21×10^(-9)cm^(2)·s^(-1).At the current density of 20 mA·g^(-1),the average lithium extraction capacity per gram of LFP electrode increased from 30.36 mg with the single conductive agent(AB)to 35.62 mg with the mixed conductive agent(AB/MWCNTs).When the mixed conductive agent was used,the capacity retention of the electrode after 30 cycles reached 82.9%,which was considerably higher than the capacity retention of 65.8%obtained when the single AB was utilized.Meanwhile,the electrode with mixed conductive agent of AB/MWCNTs provided good cycling performance.When the conductive agent content decreased or the loading capacity increased,the electrode containing the mixed conductive agent continued to show excellent electrochemical performance.Furthermore,a self-designed,highly efficient,continuous lithium extraction device was constructed.The electrode utilizing the AB/MWCNT mixed conductive agent maintained excellent adsorption capacity and cycling performance in this device.This work provides a new perspective for the electrochemical extraction of lithium using LFP electrodes.
基金the National Natural Science Foundation of China(12074348,12261141661,62204223,52072345,and 12174348)the China Postdoctoral Science Foundation(2022TQ0307)the Natural Science Foundation of Henan Province(242300421179 and 222102310664).
文摘As one promising carbon-based material,sp^(3)-hybrid carbon nitride has been predicted with various novel physicochemical properties.However,the synthesis of sp^(3)-hybrid carbon nitride is still limited by the nanaoscale,low crystallinity,complex source,and expensive instruments.Herein,we have presented a facile approach to the sp^(3)-hybrid carbon nitride nano/micro-crystals with microwave-assisted confining growth and liquid exfoliation.Actually,the carbon nitride nano/micro-crystals can spontaneously emerge and grow in the microwave-assisted polymerization of citric acid and urea,and the liquid exfoliation can break the bulk disorder polymer to retrieve the highly crystalline carbon nitride nano/micro-crystals.The obtained carbon nitride nano/micro-crystals present superior blue light absorption strength and surprising photoluminescence quantum yields of 57.96% in ethanol and 18.05%in solid state.The experimental characterizations and density functional theory calculations reveal that the interface-trapped localized exciton may contribute to the excellent intrinsic light emission capability of carbon nitride nano/micro-crystals and the interparticle staggered stacking will prevent the aggregation-caused-quenching partially.Finally,the carbon nitride nano/micro-crystals are demonstrated to be potentially useful as the phosphor medium in light-emitting-diode for interrupting blue light-induced eye damage.This work paves new light on the synthesis strategy of sp^(3)-hybrid carbon nitride materials and thus may push forward the development of multiple carbon nitride research.
基金supported by the National Natural Science Foundation of China(Grant Nos.52072322,22209137,51604250)the Department of Science and Technology of Sichuan Province(CN)(GrantNos.2022YFG0294,23GJHZ0147,23ZDYF0262)Production-Education Integration Demonstration Project of Sichuan Province"Photovoltaic Industry Production-Education Integration Comprehensive Demonstration Base of Sichuan Province"(Sichuan Financial Education[2022]No.106.n)。
文摘Sodium-based storage devices based on conversion-type metal sulfide anodes have attracted great atten-tion due to their multivalent ion redox reaction ability.However,they also suffer from sodium polysul-fides(NaPSs)shuttling problems during the sluggish Na^(+) redox process,leading to"voltage failure"and rapid capacity decay.Herein,a metal cobalt-doping vanadium disulfide(Co-VS_(2))is proposed to simulta-neously accelerate the electrochemical reaction of VS_(2) and enhance the bidirectional redox of soluble NaPSs.It is found that the strong adsorption of NaPSs by V-Co alloy nanoparticles formed in situ during the conversion reaction of Co-VS_(2) can effectively inhibit the dissolution and shuttle of NaPSs,and ther-modynamically reduce the formation energy barrier of the reaction path to effectively drive the complete conversion reaction,while the metal transition of Co elements enhances reconversion kinetics to achieve high reversibility.Moreover,Co-VS_(2) also produce abundant sulfur vacancies and unsaturated sulfur edge defects,significantly improve ionic/electron diffusion kinetics.Therefore,the Co-VS_(2) anode exhibits ultrahigh rate capability(562 mA h g^(-1) at 5 A g^(-1)),high initial coulombic efficiency(~90%)and 12,000 ultralong cycle life with capacity retention of 90%in sodium-ion batteries(SIBs),as well as impressive energy/power density(118 Wh kg^(-1)/31,250 W kg^(-1))and over 10.000 stable cycles in sodium-ion hybrid capacitors(SIHCs).Moreover,the pouch cell-type SIHC displays a high-energy density of 102 Wh kg^(-1) and exceed 600 stable cycles.This work deepens the understanding of the electrochemical reaction mechanism of conversion-type metal sulfide anodes and provides a valuable solution to the shuttlingofNaPSs inSIBsandSIHCs.
