The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosh...The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosheets(Vs-Ni_(2)Fe_(1)S_(2)/NF)were successfully prepared on the surface of nickel foam via solvothermal reaction of nickel-iron layered double hydroxide with sublimed sulfur added with sodium borohydride.Under the synergistic regulation of iron-doped and S-vacancies,Vs-Ni_(2)Fe_(1)S_(2)/NF shows excellent electrocatalytic performance and long-term durability.To reach current densities of 10 and500 mA cm^(-2),Vs-Ni_(2)Fe_(1)S_(2)/NF requires only 185(±5)and 248(±5)mV overpotential,respectively,and can maintain long stability for 350 h at 500 mA cm^(-2).The change of the mechanical pathway from adsorbate evolution mechanism to lattice oxygen oxidation mechanism is due to the increased acidity of the Ni site in Vs-Ni_(2)Fe_(1)S_(2)/NF,which facilitates the decouped proton and electron transfer process.Density functional calculation results show that the introduction of Fe atoms and S vacancies in Ni3S_(2)can enhance the conductivity of the intermediates by regulating the electronic structure of the intermediates,optimize the adsorption or desorption energy,and thus significantly improve the OER activity.For Vs-Ni_(2)Fe_(1)S_(2)/NF(+,-)cell,a voltage of 1.56 V is required to achieve 10 mA cm^(-2).In addition,Vs-Ni_(2)Fe_(1)S_(2)/NF catalyst also showed low overpotential(270 mV at 100 mA cm^(-2))and high alkaline tolerance(100 h at 100 mA cm^(-2))at 30 wt%KOH of 70℃.This shows that it has potential industrial application.展开更多
Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was ...Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was established to boost the catalytic activity toward water dissociation.As an experimental verification,the turnover frequency of 1.0-RTO_(V4)in hydrogen generation from ammonia borane hydrolysis reaches up to 2838 min-1(24828 min^(-1)depend on Rh dispersion),exceeding the benchmark set up by state-of-the-art catalysts.The transfer of mandated charge from O_(V)to Rh near O_(V)breaks the local symmetry of Rh nanoparticle and forms Rh^(γ-)(electron-aggregation Rh)-Rh interfacial atomic ensemble.This symmetry-broken Rh ensemble is the reason for the high activity of the catalyst.This work provides an effective electronic regulation strategy based on symmetry-broken atomic ensemble induced by mandated charge,designed to stimulate the limiting activity of metal catalyst in the field of next generation energy chemistry.展开更多
The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to amm...The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to ammonia synthesis and other reactions. Advanced catalysts have been developed for both high and low-temperature reactions and are widely used in industry. In recent years, supported metal nanoparticle catalysts have been researched due to their high metal utilization. Low-temperature catalysts have shown promising results, including high selectivity, high shift rates, and higher activity potential. Additionally, significant progress has been made in removing trace CO through the redox reaction in electrolytic cell. This paper reviews the development of WGS reaction catalysts, including the reaction mechanism, catalyst design, and innovative research methods. The catalyst plays a crucial role in the WGS reaction, and this paper provides an instant of catalyst design under different conditions. The progress of catalysts is closely related to the development of advanced characterization techniques.Furthermore, modifying the catalyst surface to enhance activity and significantly increase reaction kinetics is a current research direction. This review goals to stimulate a better understanding of catalyst design, performance optimization, and driving mechanisms, leading to further progress in this field.展开更多
Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are ...Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers.展开更多
Objective: The Qinzhi Zhudan formula(QZZD) exhibits a prominent therapeutic effect in the treatment of vascular dementia(VaD). This study combined a network pharmacology approach and experimental validation to identif...Objective: The Qinzhi Zhudan formula(QZZD) exhibits a prominent therapeutic effect in the treatment of vascular dementia(VaD). This study combined a network pharmacology approach and experimental validation to identify the underlying biological mechanism of QZZD against VaD.Methods: Male Wistar rats received bilateral common carotid artery occlusion(BCCAO) surgery, and after4 weeks of intragastric administration of QZZD, the therapeutic effect was assessed using the Morris water maze test and cerebral blood flow(CBF) assessment. Hematoxylin and eosin staining, Nissl staining, and electron microscopy were used to measure the histopathological changes in the neurons of rats. The effect of QZZD treatment on hippocampal neurotransmitters was assessed by high-performance liquid chromatography with electrochemical detection and liquid chromatography mass spectrometry.Immunofluorescence was used to observe VaD-induced microglia activation. The inflammatory cytokine levels were assessed by enzyme linked immunosorbent assay. Western blot was used to examine the TNFR1-mediated TNF pathway, which was screened out by network pharmacology analysis.Results: QZZD treatment alleviated pathological changes and neuronal damage in VaD rats and attenuated their cognitive impairment. In addition, QZZD increased CBF and the expression of acetylcholine and 5-hydroxytryptamine in the hippocampal region. Notably, QZZD inhibited microglial activation and the expression of IL-6 and TNF-a. Network pharmacology and western blot indicated that QZZD inhibited the levels of TNFR1, NF-κBp65, p-ERK, TNF-a, and IL-6, which are related to the TNFR1-mediated TNF signaling pathway.Conclusion: QZZD clearly improved learning and memory function, reduced brain pathological damage,elevated CBF and hippocampal neurotransmitter levels, and alleviated neuroinflammation of VaD rats partly by inhibiting the TNFR1-mediated TNF pathway, indicating its potential value in the clinical therapy of VaD.展开更多
Objective:To explore the therapeutic capacity of the Liangxue Xiaoban(LXXB)decoction and its disassembled prescriptions in the modulation of T cell subsets and recurrence-related indexes of psoriasis using a psoriasis...Objective:To explore the therapeutic capacity of the Liangxue Xiaoban(LXXB)decoction and its disassembled prescriptions in the modulation of T cell subsets and recurrence-related indexes of psoriasis using a psoriasis-like mouse model.Methods:The psoriasis model was generated by the treatment of BALB/c mice(n=48)with imiquimod.Mice were divided into six groups:control,psoriasis model,tripterygium glycosides,LXXB decoction,Liangxue decoction,and Qingqi decoction.After the intervention period,the interleukin(IL)-17A,IL-22,and interferon-γ levels in mice were examined and hematoxylin and eosin staining was conducted to determine pathological changes in the skin tissues.T cell subset changes in the skin-draining lymph nodes were analyzed using flow cytometry,and the expression levels of the associated transcription factors and recurrence-related indexes in the skin tissues were determined using a polymerase chain reaction.Results:LXXB decoction attenuated the levels of CD8^(+)T,Th17,and Th1 cells and induced an increase in the Th2 and Treg cell levels.The disassembled prescriptions promoted or inhibited specific subsets of T cells to improve the symptoms of psoriasis.Notably,the LXXB and Liangxue decoctions suppressed the expression of IL-22 at both the gene and protein levels and restored the CD103 and IL-15 expressions in the skin tissue to the normal range.Conclusion:LXXB decoction exerted significant immunoregulatory effects on T cell subsets and improved the recurrence-related indexes.Interestingly,the Liangxue prescription appeared to have a therapeutic advantage in terms of Th17 modulation and psoriasis recurrence,while the Qingqi prescription performed better in Treg immunoregulation.展开更多
Background:Inflammation is an essential component of liver diseases.Paeoniflorin(PF),a monoterpenoid component derived from peony root(Paeonia lactiflora Pall.),has anti-inflammatory,immunoregulatory,and hepatoprotect...Background:Inflammation is an essential component of liver diseases.Paeoniflorin(PF),a monoterpenoid component derived from peony root(Paeonia lactiflora Pall.),has anti-inflammatory,immunoregulatory,and hepatoprotective activities.However,whether PF affects liver inflammation and its underlying mechanisms is unclear.In this study,we investigated the effects of PF on lipopolysaccharide(LPS)-induced inflammation in LO2 cells and the underlying molecular mechanism.Methods:LPS was used to induce inflammation.After PF pretreatment for 2 h,the cells were treated with PF and LPS.Cell counting kit-8 was used to measure cell viability.Tumor necrosis factor-a(TNF-a)and interleukin(IL)-6 were tested by Enzyme-linked immunosorbent assay.Western blot was used to evaluate TNF-a,Ras homolog family member A(RhoA),NOD-,LRR-and pyrin domain-containing protein 3(NLRP3),apoptosis-associated speck-like protein containing a CARD(ASC),caspase-1,and IL-1b proteins expression.Results:In LPS-induced LO2 cells,PF reduced TNF-a and IL-6 inflammatory cytokine production in a dose-dependent manner.LPS-induced TNF-a expression was also suppressed by PF.In addition,PF significantly inhibited LPS-induced RhoA activation(P=.0014).Finally,PF suppressed LPS-induced NLRP3 inflammasome activation by downregulating NLRP3,ASC,caspase-1,and IL-1b expression.Conclusion:These findings suggest that PF alleviates inflammation induced by LPS and further suggest the anti-inflammatory effect of PF may follow via reduced RhoA and NLRP3 inflammasome activity.展开更多
Objective:Hospital readmission after surgery is one of the major contributors to the increased healthcare cost.Robotic-assisted hysterectomy(RAH)is an innovative surgical procedure most commonly performed within the l...Objective:Hospital readmission after surgery is one of the major contributors to the increased healthcare cost.Robotic-assisted hysterectomy(RAH)is an innovative surgical procedure most commonly performed within the last decade.The purpose of this study was to analyze the effects on hospital readmission patterns and emergency room(ER)visits within 60 days of discharge for women who had RAH versus laparoscopic hysterectomy(LH)in an academic community hospital in Texas.Method:We performed a retrospective study of women with RAH or LH.We used the univariate and multivariate logistic regression to examine the impact of patients'risk factors,the type of surgery,age,number of comorbidities,and duration of surgery on the 60-day hospital readmissions and ER visits.Results:A total of 291 cases with RAH or LH for benign and malignant indications were examined.The number of comorbidities and duration of surgery were similar between the two treatment groups(p>0.05).Patients in the RAH group were younger than the LH group(RAH:45.4±9.9 y,LH:49.8±11.5 y,p<0.05).No significant difference neither in hospital readmission or ER visits between the two groupswas observed(p?0.544 and p=0.109,respectively).Younger age and longer duration of surgery were significantly associated with a higher risk of ER visits(p<0.05).Conclusion:RAH is comparable with LH in hospital readmissions and ER visits.The younger age and longer operation time could lead to ER visits.展开更多
数据作为优质新型生产要素是数字经济发展的核心引擎.数据要素赋能中医药新质生产力是中医药事业与产业高质量发展的内在要求,在推动中医药科研范式与诊疗模式系统性变革,升级中医药传统产业,培育大量新兴未来产业中发挥重要作用.可信...数据作为优质新型生产要素是数字经济发展的核心引擎.数据要素赋能中医药新质生产力是中医药事业与产业高质量发展的内在要求,在推动中医药科研范式与诊疗模式系统性变革,升级中医药传统产业,培育大量新兴未来产业中发挥重要作用.可信数据空间(trusted data spaces,TDS)作为新型数据基础设施,是畅通数据资源循环的重要载体.面向数据要素赋能中医药传承创新发展,建设中医药可信数据空间(trusted data space for traditional Chinese medicine,TCM-TDS)具有重要的时代意义.本文从基础建设、功能架构、技术与业务流程等方面阐述了TCM-TDS建设路径,旨在形成中医药行业可推广、可复制的建设模式,支撑全国一体化数据市场需求.本文从机制体制创新、高质量数据集建设与数据基础设施完善、数智中医药理论与技术创新、多元应用场景驱动中医药数据生态体系形成与产业发展等方面提出TCM-TDS应用发展对策建议.展开更多
Reasonable design of high-activity catalytic sites for reducing the activation energy barrier of O-H bonds is significant for efficient conversion of hydrogen energy involving water dissociation.Herein,a coupling oxyg...Reasonable design of high-activity catalytic sites for reducing the activation energy barrier of O-H bonds is significant for efficient conversion of hydrogen energy involving water dissociation.Herein,a coupling oxygen vacancy(V_(o))strategy for intensifying generation and transfer of photo-induced electron for enhancing catalytic activity of water dissociation is verified.Using ammonia borane hydrolysis as a verification,the turnover frequency of Ru-TiO_(2)-V_(o)(Ru-TV_(o))catalyst reaches up to 1614 min−1 in visible light excitation condition at 298 K,exceeding the highest activity in Ru-based catalysts.Intensified generation and transfer of photo-induced electron via coupling V_(o) reduces the activation energy barrier of O-H bond on Ru sites,leading to a boosted intrinsic activity of Ru toward water dissociation.Ru sites enriched by photo-induced electrons also exhibit unprecedented performance in phenylacetylene hydrogenation.This work provides an effective strategy for water dissociation through V_(o)-intensified generation and transfer of photoinduced electron in the field of energy conversion.展开更多
This study presents an innovative dual-lock-and-key fluorescent probe engineered for the simultaneous detection of bisulfite and viscosity.The functionalized probe,(E)-2-(1-ethyl-2-(N-methylquinolinevinyl)quinolin-4(1...This study presents an innovative dual-lock-and-key fluorescent probe engineered for the simultaneous detection of bisulfite and viscosity.The functionalized probe,(E)-2-(1-ethyl-2-(N-methylquinolinevinyl)quinolin-4(1H)-ylidene)malononitrile(QC-QNM),was strategically synthesized by conjugating the quinolylmalononitrile and N-methylquinolinium through an ethylene bridge.Within this construction,the N-methylquinolinium selectively targets bisulfite,while the vinyl moiety serves as a responsive rotor for viscosity.Notably,the presence of either sulfite or viscosity alone cannot elicit significant fluorescent responses from the probe.Conversely,concurrent exposure to both bisulfite and viscosity triggers enhanced fluorescent signals,indicative of an“AND”logic gate characteristic.Quantum chemical calculations were further applied to rationalize the working mechanism of the probe.Additionally,the excellent biocompatibility of this probe in cellular imaging experiments highlights its potential for specific mitochondrial imaging by modulating both exogenous/endogenous bisulfite levels alongside viscosity induced by monensin.This novel approach thereby offers a distinctive analytical tool for monitoring the coexistence of viscosity and bisulfite in specific metabolic and physiological contexts.展开更多
Doping and compositing with conductive frameworks are adopted to increase the capacity and stability of δ-MnO_(2) used as electrode material for zinc-ion batteries(ZIB).Co-doped MnO_(2)/carbon nanotubes(CNTs)are prep...Doping and compositing with conductive frameworks are adopted to increase the capacity and stability of δ-MnO_(2) used as electrode material for zinc-ion batteries(ZIB).Co-doped MnO_(2)/carbon nanotubes(CNTs)are prepared by hydrothermally reacting MnO_(4)−and Mn^(2+) in the presence of Co^(2+),with acidified CNTs as the framework for crystallization.Characterization studies indicate that the doping with Co^(2+)does not alter the morphology of the δ-MnO_(2),but increased interplanar lattice spacing is achieved.A ZIB with Co-MnO_(2)/CNTs can deliver a high specific capacity of 365 mA h g^(−1) at a current density of 0.2 A g^(−1),and only 5.4%of specific capacity is lost after 1500 charging and discharging cycles at 1 A g^(−1),which is better than ZIBs withδ-MnO_(2) and Co-MnO_(2).For ZIBs with Co-MnO_(2)/CNTs,diffusion-controlled processes dominate.The enhanced capacity and stability originate from the increased specific surface area induced by the CNT framework,decreased charge transfer resistances,and increased ion diffusion kinetics.The insertion and extraction of both H^(+) and Zn^(2+)are involved for charge storage,with ZnSO_(4)·3Zn(OH)_(2)·5H_(2)O,MnOOH and ZnMn_(2)O_(4) detected during the discharged state and ZnMn_(3)O7·3H_(2)O identified during the charged state.展开更多
Phosphorylated modification of plant polysaccharides has emerged as an effective strategy to enhance their bioactivity.Here,we compared phosphorylated Scrophularia ningpoensis polysaccharides(PSNPs)with the native for...Phosphorylated modification of plant polysaccharides has emerged as an effective strategy to enhance their bioactivity.Here,we compared phosphorylated Scrophularia ningpoensis polysaccharides(PSNPs)with the native form(SNPs)in a cyclophosphamide(Cyp)-induced immunosuppression mouse model.In vitro,both SNPs and PSNPs scavenged hydroxyl and ABTS radicals in a dose-dependent manner,with PSNPs showing superior hydroxyl radical scavenging above 0.5 mg/mL.In vivo,Cyp administration markedly decreased superoxide dismutase(SOD)activity and increased malondialdehyde(MDA)levels in liver and serum,indicative of oxidative stress.Both SNPs and PSNPs significantly restored SOD activity and reduced MDA levels,with PSNPs showing greater efficacy.Immunohistochemical analysis further revealed that Cyp-induced suppression of hepatic nuclear factor erythroid 2-related factor 2(Nrf2)expression was effectively reversed by SNPs and more prominently by PSNPs.Immune function assessment revealed that Cyp-induced thymus and spleen atrophy was significantly reversed by SNPs or PSNPs,with PSNPs producing a more pronounced recovery.Cytokine profiling showed that both treatments elevated the anti-inflammatory cytokine IL-10 and reduced the proinflammatory cytokines TNF-αand IL-6,with PSNPs achieving stronger modulation.Immunohistochemistry confirmed nuclear factor-kappa B(NF-κB)activation in ear tissue was markedly reduced,especially by PSNPs.Furthermore,16S rRNA sequencing demonstrated that SNPs and PSNPs reshaped the gut microbiota by enriching beneficial genera and suppressing pathogenic taxa,with PSNPs inducing greater microbiota remodeling.These findings indicate PSNPs exert enhanced antioxidant,immunomodulatory,and gut microbiota-modulating activities,likely via coordinated Nrf2 activation,NF-κB inhibition,and microbial community regulation,highlighting their potential against chemotherapy-induced immunosuppression and oxidative injury.展开更多
Due to the high risk of tearing and rupture,vulnerable atherosclerotic plaques would induce serious cardiovascular and cerebrovascular diseases.Despite the available clinical methods can evaluate the vulnerability of ...Due to the high risk of tearing and rupture,vulnerable atherosclerotic plaques would induce serious cardiovascular and cerebrovascular diseases.Despite the available clinical methods can evaluate the vulnerability of plaques and specifically treat vulnerable plaques before a cardiovascular event,but the efficiency is still low and undesirable.Herein,we rationally design and engineer the low-intensity focused ultrasound(LIFU)-responsive FPD@CD nanomedicine for the highly efficient treatment of vulnerable plaques by facilely loading phase transition agent perfluorohexane(PFH)into biocompatible PLGA-PEG-PLGA nanoparticles(PPP NPs)and then attaching dextran sulphate(DS)onto the surface of PPP NPs for targeting delivery.DS,as a typical macrophages-targeted molecule,can achieve the precise vaporization of NPs and subsequently controllable apoptosis of RAW 264.7 macrophages as induced by acoustic droplet vaporization(ADV)effect.In addition,the introduction of DiR and Fe3O4 endows nanomedicine with near-infrared fluorescence(NIRF)and magnetic resonance(MR)imaging capabilities.The engineered FPD@CD nanomedicine that uses macrophages as therapeutic targets achieve the conspicuous therapeutic effect of shrinking vulnerable plaques based on in vivo and in vitro evaluation outcomes.A reduction of 49.4%of vascular stenosis degree in gross pathology specimens were achieved throughout the treatment period.This specific,efficient and biosafe treatment modality potentiates the biomedical application in patients with cardiovascular and cerebrovascular diseases based on the relief of the plaque rupture concerns.展开更多
Black phosphorus(BP) as a narrow-bandgap two-dimensional semiconductor material has been extensively studied. And the allotrope violet phosphorus(VP) exhibits wide bandgap properties extending the application in the v...Black phosphorus(BP) as a narrow-bandgap two-dimensional semiconductor material has been extensively studied. And the allotrope violet phosphorus(VP) exhibits wide bandgap properties extending the application in the visible light band. However,due to the Schottky barrier of metal/semiconductor contacts(M/S), further device application of VP is limited. Here, VP-based photodetectors with van der Waals-assisted contact were demonstrated, achieving quasi-Ohmic M/S contacts. The output characteristics in dark conditions show ultralow current at the pA level. And the device exhibits a high current on-off ratio of 10~5and a fast response speed of 8.4 ms. Furthermore, we constructed the first allotropic photodetector based on BP and VP heterojunction. The device maintains ultralow dark current(~ pA) while exhibiting faster carrier transport, with 945 μs response time and polarization detection capability. These results offer an effective way to study the optoelectronic properties of VP and promote the study of allotropic heterojunction devices.展开更多
Rational design of highly active catalysts for breaking hydrogen-oxygen bonds is of great significance in energy chemical reactions involving water.Herein,an efficient strategy for the artificial atom(RuPd)established...Rational design of highly active catalysts for breaking hydrogen-oxygen bonds is of great significance in energy chemical reactions involving water.Herein,an efficient strategy for the artificial atom(RuPd)established by d-orbital coupling and adjusted by oxygen vacancy(V_(O))is verified for water dissociation.As an experimental verification,the turnover frequency of RuPd-TiO_(2)-VO(RuPdTVO)catalyst in ammonia borane hydrolysis reaches up to 2750 min^(−1)(26,190 min−1 based on metal dispersion)in the absence of alkali,exceeding the highest active catalysts(Rh-based catalysts).The d-orbital coupling effect between Ru and Pd simulates the outer electronic structure of Rh.Electron transfer from V_(O) to(RuPd)constructs an electron-rich state of active sites that further enhances the ability of the artificial atom to dissociate water.This work provides an effective electronic regulation strategy from V_(O) and artificial atom constructed by d-orbital coupling effect for efficient water dissociation.展开更多
基金supported by the National Natural Science Foundation of China(22308206 and 22278255)the Graduate Innovation Fund of Shaanxi University of Science and Technology,China。
文摘The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosheets(Vs-Ni_(2)Fe_(1)S_(2)/NF)were successfully prepared on the surface of nickel foam via solvothermal reaction of nickel-iron layered double hydroxide with sublimed sulfur added with sodium borohydride.Under the synergistic regulation of iron-doped and S-vacancies,Vs-Ni_(2)Fe_(1)S_(2)/NF shows excellent electrocatalytic performance and long-term durability.To reach current densities of 10 and500 mA cm^(-2),Vs-Ni_(2)Fe_(1)S_(2)/NF requires only 185(±5)and 248(±5)mV overpotential,respectively,and can maintain long stability for 350 h at 500 mA cm^(-2).The change of the mechanical pathway from adsorbate evolution mechanism to lattice oxygen oxidation mechanism is due to the increased acidity of the Ni site in Vs-Ni_(2)Fe_(1)S_(2)/NF,which facilitates the decouped proton and electron transfer process.Density functional calculation results show that the introduction of Fe atoms and S vacancies in Ni3S_(2)can enhance the conductivity of the intermediates by regulating the electronic structure of the intermediates,optimize the adsorption or desorption energy,and thus significantly improve the OER activity.For Vs-Ni_(2)Fe_(1)S_(2)/NF(+,-)cell,a voltage of 1.56 V is required to achieve 10 mA cm^(-2).In addition,Vs-Ni_(2)Fe_(1)S_(2)/NF catalyst also showed low overpotential(270 mV at 100 mA cm^(-2))and high alkaline tolerance(100 h at 100 mA cm^(-2))at 30 wt%KOH of 70℃.This shows that it has potential industrial application.
基金supported by the National Natural Science Foundation of China(No.22279118,No.22309164)the China Postdoctoral Science Foundation(No.2023M733214)+1 种基金the Young Top Talent Program of Zhongyuan-Yingcai-Jihua(No.30602674)the Special Projects of Henan Province Key Research and Development and Promotion(Science and Technology Research)(No.232102241033)。
文摘Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was established to boost the catalytic activity toward water dissociation.As an experimental verification,the turnover frequency of 1.0-RTO_(V4)in hydrogen generation from ammonia borane hydrolysis reaches up to 2838 min-1(24828 min^(-1)depend on Rh dispersion),exceeding the benchmark set up by state-of-the-art catalysts.The transfer of mandated charge from O_(V)to Rh near O_(V)breaks the local symmetry of Rh nanoparticle and forms Rh^(γ-)(electron-aggregation Rh)-Rh interfacial atomic ensemble.This symmetry-broken Rh ensemble is the reason for the high activity of the catalyst.This work provides an effective electronic regulation strategy based on symmetry-broken atomic ensemble induced by mandated charge,designed to stimulate the limiting activity of metal catalyst in the field of next generation energy chemistry.
基金financially supported by the National Natural Science Foundation of China (22279118, 22279117, 22075254,31901272)the Top-Notch Talent Program of Henan Agricultural University (30501034)。
文摘The water gas shift(WGS) reaction is a standard reaction that is widely used in industrial hydrogen production and removal of carbon monoxide. The improved catalytic performance of WGS reaction also contributes to ammonia synthesis and other reactions. Advanced catalysts have been developed for both high and low-temperature reactions and are widely used in industry. In recent years, supported metal nanoparticle catalysts have been researched due to their high metal utilization. Low-temperature catalysts have shown promising results, including high selectivity, high shift rates, and higher activity potential. Additionally, significant progress has been made in removing trace CO through the redox reaction in electrolytic cell. This paper reviews the development of WGS reaction catalysts, including the reaction mechanism, catalyst design, and innovative research methods. The catalyst plays a crucial role in the WGS reaction, and this paper provides an instant of catalyst design under different conditions. The progress of catalysts is closely related to the development of advanced characterization techniques.Furthermore, modifying the catalyst surface to enhance activity and significantly increase reaction kinetics is a current research direction. This review goals to stimulate a better understanding of catalyst design, performance optimization, and driving mechanisms, leading to further progress in this field.
基金funded by the National Natural Science Foundation of China (Nos. 22279118, 31901272, 21401168, U1204203)National Science Fund for Distinguished Young of China (No. 22225202)+1 种基金Young Top Talent Program of Zhongyuan-YingcaiJihua (No. 30602674)Top-Notch Talent Program of Henan Agricultural University (No. 30501034)。
文摘Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers.
基金supported by Young Qihuang Scholars Project(90020163320001)Major National Science and Technology Projects (2019ZX09301-173)。
文摘Objective: The Qinzhi Zhudan formula(QZZD) exhibits a prominent therapeutic effect in the treatment of vascular dementia(VaD). This study combined a network pharmacology approach and experimental validation to identify the underlying biological mechanism of QZZD against VaD.Methods: Male Wistar rats received bilateral common carotid artery occlusion(BCCAO) surgery, and after4 weeks of intragastric administration of QZZD, the therapeutic effect was assessed using the Morris water maze test and cerebral blood flow(CBF) assessment. Hematoxylin and eosin staining, Nissl staining, and electron microscopy were used to measure the histopathological changes in the neurons of rats. The effect of QZZD treatment on hippocampal neurotransmitters was assessed by high-performance liquid chromatography with electrochemical detection and liquid chromatography mass spectrometry.Immunofluorescence was used to observe VaD-induced microglia activation. The inflammatory cytokine levels were assessed by enzyme linked immunosorbent assay. Western blot was used to examine the TNFR1-mediated TNF pathway, which was screened out by network pharmacology analysis.Results: QZZD treatment alleviated pathological changes and neuronal damage in VaD rats and attenuated their cognitive impairment. In addition, QZZD increased CBF and the expression of acetylcholine and 5-hydroxytryptamine in the hippocampal region. Notably, QZZD inhibited microglial activation and the expression of IL-6 and TNF-a. Network pharmacology and western blot indicated that QZZD inhibited the levels of TNFR1, NF-κBp65, p-ERK, TNF-a, and IL-6, which are related to the TNFR1-mediated TNF signaling pathway.Conclusion: QZZD clearly improved learning and memory function, reduced brain pathological damage,elevated CBF and hippocampal neurotransmitter levels, and alleviated neuroinflammation of VaD rats partly by inhibiting the TNFR1-mediated TNF pathway, indicating its potential value in the clinical therapy of VaD.
基金This experimental study was supported by the Key Research Project of the Beijing University of Chinese Medicine(2020-JYBZDGG-023)Young Qihuang Scholars Project(90020163320001).
文摘Objective:To explore the therapeutic capacity of the Liangxue Xiaoban(LXXB)decoction and its disassembled prescriptions in the modulation of T cell subsets and recurrence-related indexes of psoriasis using a psoriasis-like mouse model.Methods:The psoriasis model was generated by the treatment of BALB/c mice(n=48)with imiquimod.Mice were divided into six groups:control,psoriasis model,tripterygium glycosides,LXXB decoction,Liangxue decoction,and Qingqi decoction.After the intervention period,the interleukin(IL)-17A,IL-22,and interferon-γ levels in mice were examined and hematoxylin and eosin staining was conducted to determine pathological changes in the skin tissues.T cell subset changes in the skin-draining lymph nodes were analyzed using flow cytometry,and the expression levels of the associated transcription factors and recurrence-related indexes in the skin tissues were determined using a polymerase chain reaction.Results:LXXB decoction attenuated the levels of CD8^(+)T,Th17,and Th1 cells and induced an increase in the Th2 and Treg cell levels.The disassembled prescriptions promoted or inhibited specific subsets of T cells to improve the symptoms of psoriasis.Notably,the LXXB and Liangxue decoctions suppressed the expression of IL-22 at both the gene and protein levels and restored the CD103 and IL-15 expressions in the skin tissue to the normal range.Conclusion:LXXB decoction exerted significant immunoregulatory effects on T cell subsets and improved the recurrence-related indexes.Interestingly,the Liangxue prescription appeared to have a therapeutic advantage in terms of Th17 modulation and psoriasis recurrence,while the Qingqi prescription performed better in Treg immunoregulation.
基金This work was supported by the National Natural Science Foundation of China(81774122)the Chinese Major Scientific and Technological Special Project for Major New Drug Creation(2019ZX09301-173).
文摘Background:Inflammation is an essential component of liver diseases.Paeoniflorin(PF),a monoterpenoid component derived from peony root(Paeonia lactiflora Pall.),has anti-inflammatory,immunoregulatory,and hepatoprotective activities.However,whether PF affects liver inflammation and its underlying mechanisms is unclear.In this study,we investigated the effects of PF on lipopolysaccharide(LPS)-induced inflammation in LO2 cells and the underlying molecular mechanism.Methods:LPS was used to induce inflammation.After PF pretreatment for 2 h,the cells were treated with PF and LPS.Cell counting kit-8 was used to measure cell viability.Tumor necrosis factor-a(TNF-a)and interleukin(IL)-6 were tested by Enzyme-linked immunosorbent assay.Western blot was used to evaluate TNF-a,Ras homolog family member A(RhoA),NOD-,LRR-and pyrin domain-containing protein 3(NLRP3),apoptosis-associated speck-like protein containing a CARD(ASC),caspase-1,and IL-1b proteins expression.Results:In LPS-induced LO2 cells,PF reduced TNF-a and IL-6 inflammatory cytokine production in a dose-dependent manner.LPS-induced TNF-a expression was also suppressed by PF.In addition,PF significantly inhibited LPS-induced RhoA activation(P=.0014).Finally,PF suppressed LPS-induced NLRP3 inflammasome activation by downregulating NLRP3,ASC,caspase-1,and IL-1b expression.Conclusion:These findings suggest that PF alleviates inflammation induced by LPS and further suggest the anti-inflammatory effect of PF may follow via reduced RhoA and NLRP3 inflammasome activity.
文摘Objective:Hospital readmission after surgery is one of the major contributors to the increased healthcare cost.Robotic-assisted hysterectomy(RAH)is an innovative surgical procedure most commonly performed within the last decade.The purpose of this study was to analyze the effects on hospital readmission patterns and emergency room(ER)visits within 60 days of discharge for women who had RAH versus laparoscopic hysterectomy(LH)in an academic community hospital in Texas.Method:We performed a retrospective study of women with RAH or LH.We used the univariate and multivariate logistic regression to examine the impact of patients'risk factors,the type of surgery,age,number of comorbidities,and duration of surgery on the 60-day hospital readmissions and ER visits.Results:A total of 291 cases with RAH or LH for benign and malignant indications were examined.The number of comorbidities and duration of surgery were similar between the two treatment groups(p>0.05).Patients in the RAH group were younger than the LH group(RAH:45.4±9.9 y,LH:49.8±11.5 y,p<0.05).No significant difference neither in hospital readmission or ER visits between the two groupswas observed(p?0.544 and p=0.109,respectively).Younger age and longer duration of surgery were significantly associated with a higher risk of ER visits(p<0.05).Conclusion:RAH is comparable with LH in hospital readmissions and ER visits.The younger age and longer operation time could lead to ER visits.
文摘数据作为优质新型生产要素是数字经济发展的核心引擎.数据要素赋能中医药新质生产力是中医药事业与产业高质量发展的内在要求,在推动中医药科研范式与诊疗模式系统性变革,升级中医药传统产业,培育大量新兴未来产业中发挥重要作用.可信数据空间(trusted data spaces,TDS)作为新型数据基础设施,是畅通数据资源循环的重要载体.面向数据要素赋能中医药传承创新发展,建设中医药可信数据空间(trusted data space for traditional Chinese medicine,TCM-TDS)具有重要的时代意义.本文从基础建设、功能架构、技术与业务流程等方面阐述了TCM-TDS建设路径,旨在形成中医药行业可推广、可复制的建设模式,支撑全国一体化数据市场需求.本文从机制体制创新、高质量数据集建设与数据基础设施完善、数智中医药理论与技术创新、多元应用场景驱动中医药数据生态体系形成与产业发展等方面提出TCM-TDS应用发展对策建议.
基金supported by the National Natural Science Foundation of China(Nos.22309164 and 22279118)the China Postdoctoral Science Foundation(No.2023M733214)+1 种基金the National Science Fund for Distinguished Young Scholars of China(No.22225202)the Young Top Talent Program of Zhongyuan-Yingcai-Jihua(No.30602674).
文摘Reasonable design of high-activity catalytic sites for reducing the activation energy barrier of O-H bonds is significant for efficient conversion of hydrogen energy involving water dissociation.Herein,a coupling oxygen vacancy(V_(o))strategy for intensifying generation and transfer of photo-induced electron for enhancing catalytic activity of water dissociation is verified.Using ammonia borane hydrolysis as a verification,the turnover frequency of Ru-TiO_(2)-V_(o)(Ru-TV_(o))catalyst reaches up to 1614 min−1 in visible light excitation condition at 298 K,exceeding the highest activity in Ru-based catalysts.Intensified generation and transfer of photo-induced electron via coupling V_(o) reduces the activation energy barrier of O-H bond on Ru sites,leading to a boosted intrinsic activity of Ru toward water dissociation.Ru sites enriched by photo-induced electrons also exhibit unprecedented performance in phenylacetylene hydrogenation.This work provides an effective strategy for water dissociation through V_(o)-intensified generation and transfer of photoinduced electron in the field of energy conversion.
基金supported by the Liaoning Provincial Key Research and Development Project(Civil Science and Technology,2024JH2/102500053)the Open Fund of Key Laboratory of Biotechnology and Bioresources Utilization(Dalian Minzu University),Ministry of Education of China(KF2024009)+2 种基金the Scientific Research Project of Liaoning Provincial Department of Education(LJ212410167039,JTTMS1618)the National Natural Science Foundation of China(22278038,12374368)the Liaoning Revitalization Talents Program(XLYC2203011)。
文摘This study presents an innovative dual-lock-and-key fluorescent probe engineered for the simultaneous detection of bisulfite and viscosity.The functionalized probe,(E)-2-(1-ethyl-2-(N-methylquinolinevinyl)quinolin-4(1H)-ylidene)malononitrile(QC-QNM),was strategically synthesized by conjugating the quinolylmalononitrile and N-methylquinolinium through an ethylene bridge.Within this construction,the N-methylquinolinium selectively targets bisulfite,while the vinyl moiety serves as a responsive rotor for viscosity.Notably,the presence of either sulfite or viscosity alone cannot elicit significant fluorescent responses from the probe.Conversely,concurrent exposure to both bisulfite and viscosity triggers enhanced fluorescent signals,indicative of an“AND”logic gate characteristic.Quantum chemical calculations were further applied to rationalize the working mechanism of the probe.Additionally,the excellent biocompatibility of this probe in cellular imaging experiments highlights its potential for specific mitochondrial imaging by modulating both exogenous/endogenous bisulfite levels alongside viscosity induced by monensin.This novel approach thereby offers a distinctive analytical tool for monitoring the coexistence of viscosity and bisulfite in specific metabolic and physiological contexts.
基金funding received from the National Natural Science Foundation of China(no.22278255)the Shaanxi University of Science and Technology Scientific Research Foundation for the PhD(no.2019QNBJ 05)+2 种基金supported by the Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(no.KFKT2022-12)the Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(no.KFKT2022-12)the Graduate Innovation Fund of Shaanxi University of Science and Technology,China.
文摘Doping and compositing with conductive frameworks are adopted to increase the capacity and stability of δ-MnO_(2) used as electrode material for zinc-ion batteries(ZIB).Co-doped MnO_(2)/carbon nanotubes(CNTs)are prepared by hydrothermally reacting MnO_(4)−and Mn^(2+) in the presence of Co^(2+),with acidified CNTs as the framework for crystallization.Characterization studies indicate that the doping with Co^(2+)does not alter the morphology of the δ-MnO_(2),but increased interplanar lattice spacing is achieved.A ZIB with Co-MnO_(2)/CNTs can deliver a high specific capacity of 365 mA h g^(−1) at a current density of 0.2 A g^(−1),and only 5.4%of specific capacity is lost after 1500 charging and discharging cycles at 1 A g^(−1),which is better than ZIBs withδ-MnO_(2) and Co-MnO_(2).For ZIBs with Co-MnO_(2)/CNTs,diffusion-controlled processes dominate.The enhanced capacity and stability originate from the increased specific surface area induced by the CNT framework,decreased charge transfer resistances,and increased ion diffusion kinetics.The insertion and extraction of both H^(+) and Zn^(2+)are involved for charge storage,with ZnSO_(4)·3Zn(OH)_(2)·5H_(2)O,MnOOH and ZnMn_(2)O_(4) detected during the discharged state and ZnMn_(3)O7·3H_(2)O identified during the charged state.
基金funded by the Natural Science Foundation of China(No.81603003 and 81903829)the Natural Science Foundation of Rizhao(No.RZ2022ZR11)+2 种基金the Open Project from the State Key Labo-ratory of Traditional Chinese Medicine Syndrome(No.SKLKY2024B0006)the Department of Science and Technology of Sichuan Province(No.2024YFHZ0361)the Joint Project of Luzhou Municipal People’s Government and Southwest Medical University(No.2024LZXNYDJ026).
文摘Phosphorylated modification of plant polysaccharides has emerged as an effective strategy to enhance their bioactivity.Here,we compared phosphorylated Scrophularia ningpoensis polysaccharides(PSNPs)with the native form(SNPs)in a cyclophosphamide(Cyp)-induced immunosuppression mouse model.In vitro,both SNPs and PSNPs scavenged hydroxyl and ABTS radicals in a dose-dependent manner,with PSNPs showing superior hydroxyl radical scavenging above 0.5 mg/mL.In vivo,Cyp administration markedly decreased superoxide dismutase(SOD)activity and increased malondialdehyde(MDA)levels in liver and serum,indicative of oxidative stress.Both SNPs and PSNPs significantly restored SOD activity and reduced MDA levels,with PSNPs showing greater efficacy.Immunohistochemical analysis further revealed that Cyp-induced suppression of hepatic nuclear factor erythroid 2-related factor 2(Nrf2)expression was effectively reversed by SNPs and more prominently by PSNPs.Immune function assessment revealed that Cyp-induced thymus and spleen atrophy was significantly reversed by SNPs or PSNPs,with PSNPs producing a more pronounced recovery.Cytokine profiling showed that both treatments elevated the anti-inflammatory cytokine IL-10 and reduced the proinflammatory cytokines TNF-αand IL-6,with PSNPs achieving stronger modulation.Immunohistochemistry confirmed nuclear factor-kappa B(NF-κB)activation in ear tissue was markedly reduced,especially by PSNPs.Furthermore,16S rRNA sequencing demonstrated that SNPs and PSNPs reshaped the gut microbiota by enriching beneficial genera and suppressing pathogenic taxa,with PSNPs inducing greater microbiota remodeling.These findings indicate PSNPs exert enhanced antioxidant,immunomodulatory,and gut microbiota-modulating activities,likely via coordinated Nrf2 activation,NF-κB inhibition,and microbial community regulation,highlighting their potential against chemotherapy-induced immunosuppression and oxidative injury.
基金support from the National Natural Science Foundation of China(Grant Nos.81701650,81971608,and 82172092)the Kuanren Talents Program of the Second Affiliated Hospital of Chongqing Medical University(Grant No.2020-7)the Science&Technology Commission Foundation of Chongqing(Grant No.cstc2017jcyjAX0444).
文摘Due to the high risk of tearing and rupture,vulnerable atherosclerotic plaques would induce serious cardiovascular and cerebrovascular diseases.Despite the available clinical methods can evaluate the vulnerability of plaques and specifically treat vulnerable plaques before a cardiovascular event,but the efficiency is still low and undesirable.Herein,we rationally design and engineer the low-intensity focused ultrasound(LIFU)-responsive FPD@CD nanomedicine for the highly efficient treatment of vulnerable plaques by facilely loading phase transition agent perfluorohexane(PFH)into biocompatible PLGA-PEG-PLGA nanoparticles(PPP NPs)and then attaching dextran sulphate(DS)onto the surface of PPP NPs for targeting delivery.DS,as a typical macrophages-targeted molecule,can achieve the precise vaporization of NPs and subsequently controllable apoptosis of RAW 264.7 macrophages as induced by acoustic droplet vaporization(ADV)effect.In addition,the introduction of DiR and Fe3O4 endows nanomedicine with near-infrared fluorescence(NIRF)and magnetic resonance(MR)imaging capabilities.The engineered FPD@CD nanomedicine that uses macrophages as therapeutic targets achieve the conspicuous therapeutic effect of shrinking vulnerable plaques based on in vivo and in vitro evaluation outcomes.A reduction of 49.4%of vascular stenosis degree in gross pathology specimens were achieved throughout the treatment period.This specific,efficient and biosafe treatment modality potentiates the biomedical application in patients with cardiovascular and cerebrovascular diseases based on the relief of the plaque rupture concerns.
基金supported by the National Natural Science Foundation of China (Grant Nos. 62261136552, 62005303, and 62134001)the National Key Research and Development Program of China (Grant No. 2021YFA0715602)+2 种基金the International Partnership Program of Chinese Academy of Sciences (Grant No. 181331KYSB20200012)the Shanghai Science and Technology Committee (Grant No. 23YF1455400)the Open Research Projects of Zhejiang Lab (Grant No. 2022NK0AB01)。
文摘Black phosphorus(BP) as a narrow-bandgap two-dimensional semiconductor material has been extensively studied. And the allotrope violet phosphorus(VP) exhibits wide bandgap properties extending the application in the visible light band. However,due to the Schottky barrier of metal/semiconductor contacts(M/S), further device application of VP is limited. Here, VP-based photodetectors with van der Waals-assisted contact were demonstrated, achieving quasi-Ohmic M/S contacts. The output characteristics in dark conditions show ultralow current at the pA level. And the device exhibits a high current on-off ratio of 10~5and a fast response speed of 8.4 ms. Furthermore, we constructed the first allotropic photodetector based on BP and VP heterojunction. The device maintains ultralow dark current(~ pA) while exhibiting faster carrier transport, with 945 μs response time and polarization detection capability. These results offer an effective way to study the optoelectronic properties of VP and promote the study of allotropic heterojunction devices.
基金supported by the National Natural Science Foundation of China(Nos.22279118 and 22309164)the China Postdoctoral Science Foundation(No.2023M733214)+2 种基金the National Science Fund for Distinguished Young of China(No.22225202)the Young Top Talent Program of Zhongyuan-Yingcai-Jihua(No.30602674)Experiments were supported by Peking Nanofab.
文摘Rational design of highly active catalysts for breaking hydrogen-oxygen bonds is of great significance in energy chemical reactions involving water.Herein,an efficient strategy for the artificial atom(RuPd)established by d-orbital coupling and adjusted by oxygen vacancy(V_(O))is verified for water dissociation.As an experimental verification,the turnover frequency of RuPd-TiO_(2)-VO(RuPdTVO)catalyst in ammonia borane hydrolysis reaches up to 2750 min^(−1)(26,190 min−1 based on metal dispersion)in the absence of alkali,exceeding the highest active catalysts(Rh-based catalysts).The d-orbital coupling effect between Ru and Pd simulates the outer electronic structure of Rh.Electron transfer from V_(O) to(RuPd)constructs an electron-rich state of active sites that further enhances the ability of the artificial atom to dissociate water.This work provides an effective electronic regulation strategy from V_(O) and artificial atom constructed by d-orbital coupling effect for efficient water dissociation.
