Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability cau...Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.展开更多
Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a s...Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) production.Operating within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.展开更多
The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reporte...The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reported as a highly active OER electrocatalyst in alkaline seawater,requiring only overpotentials of 303 and 332 mV to achieve 100 and 300 mA·cm^(-2),respectively.Moreover,it shows strong long-term electrochemical durability for at least 50 h.展开更多
Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nano...Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nanosheet array on Ni foam(Co-Ni_(3)S_(2)/NF)as a high-efficiency OER electrocatalyst for seawater.In alkaline conditions,Co-Ni_(3)S_(2)/NF requires an overpotential of only 368 mV to drive 100 mA·cm^(–2),superior to Ni_(3)S_(2)/NF(385 mV).Besides,it exhibits at least 50-h continuous electrolysis.展开更多
Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited a...Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.展开更多
The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a ...The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and amine.This innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing field.This review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen species.Additionally,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding reactions.This critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.展开更多
Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In t...Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In this communication,we report the application of Mo_(2)C nanosheets-decorated carbon sheets(Mo_(2)C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea electrosynthesis.In CO_(2)-saturated 0.2 mol/L Na_(2)SO_(4)solution containing 0.05 mol/L NO_(3)^(-),the Mo_(2)C/C catalyst achieves an impres-sive urea yield of 579.13μg h^(-1)mg^(-1)with high Faradaic efficiency of 44.80%at-0.5 V versus the reversible hydrogen electrode.Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of^(∗)CO and^(∗)NH_(2)intermediates and facilitate their C-N coupling.This research propels the use of Mo_(2)C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.展开更多
It is of great importance to design and develop electrocatalysts that are both long-lasting and efficient for seawater oxidation.Herein,a three-dimensional porous cauliflower-like Ni_(3)S_(2) foam on Ni foam(Ni_(3)S_(...It is of great importance to design and develop electrocatalysts that are both long-lasting and efficient for seawater oxidation.Herein,a three-dimensional porous cauliflower-like Ni_(3)S_(2) foam on Ni foam(Ni_(3)S_(2) foam/NF)is proposed as a high-performance electrocatalyst for the oxygen evolution reaction in alkaline seawater.The as-synthesis Ni_(3)S_(2) foam/NF achieves exceptional efficacy,achieving a current density of 100 mA·cm^(−2)at mere overpotential of 369 mV.Notably,its electrocatalytic stability extends up to 1000 h at 500 mA·cm^(−2).展开更多
Background Studies show tranexamic acid can reduce the risk of death and early neurological deterioration after intracranial haemorrhage.We aimed to assess whether tranexamic acid reduces haematoma expansion and impro...Background Studies show tranexamic acid can reduce the risk of death and early neurological deterioration after intracranial haemorrhage.We aimed to assess whether tranexamic acid reduces haematoma expansion and improves outcome in intracerebral haemorrhage patients susceptible to haemorrhage expansion.Methods We did a prospective,double-blind,randomised,placebo-controlled trial at 10 stroke centres in China.Acute supratentorial intracerebral haemorrhage patients were eligible if they had indication of haemorrhage expansion on admission imaging(eg,spot sign,black hole sign or blend sign),and were treatable within 8 hours of symptom onset.Patients were randomly assigned(1:1)to receive either tranexamic acid or a matching placebo.The primary outcome was intracerebral haematoma growth(>33% relative or>6 mL absolute)at 24 hours.Clinical outcomes were assessed at 90 days.Results Of the 171 included patients,124(72.5%)were male,and the mean age was 55.9±11.6 years.89 patients received tranexamic acid and 82 received placebo.The primary outcome did not differ significantly between the groups:36(40.4%)patients in the tranexamic acid group and 34(41.5%)patients in the placebo group had intracranial haemorrhage growth(OR 0.96,95% CI 0.52 to 1.77,p=0.89).The proportion of death was lower in the tranexamic acid treatment group than placebo group(8.1%vs 10.0%),but there were no significant differences in secondary outcomes including absolute intracranial haemorrhage growth,death and dependency.Conclusions Among patients susceptible to haemorrhage expansion treated within 8 hours of stroke onset,tranexamic acid did not significantly prevent intracerebral haemorrhage growth.Larger studies are needed to assess safety and efficacy of tranexamic acid in intracerebral haemorrhage patients.展开更多
Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issu...Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issues of electrode poisoning and corrosion will occur during the seawater electrolysis process,and active and stable electrocatalysts for the hydrogen evolution reaction(HER)are thus highly desired.In this work,N,O-doped carbon foam in-situ derived from commercial melamine foam is proposed as a high-active metal-free HER electrocatalyst for seawater splitting.In acidic seawater,our catalyst shows high hydrogen generation performance with small overpotential of 161 mV at 10 mA·cm^(−2),a low Tafel slop of 97.5 mV·dec^(−1),and outstanding stability.展开更多
Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with cataly...Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with catalytic activity of heterogeneous catalysts.Nanoribbon is attractive nanostructure,which possesses the flexibility of one-dimensional nanomaterials,the large surface area of two-dimensional nanomaterials,and lateral size confinement effects.In this work,Cu_(3)P nanoribbon is proposed as a highly efficient electrocatalyst for N_(2)-to-NH_(3)conversion under benign conditions.When measured in N_(2)-saturated 0.1 M HCl,such Cu_(3)P nanoribbon achieves high performance with an excellent Faradaic efficiency as high as 37.8%and a large yield of 18.9μg·h^(−1)·mgcat.−1 at−0.2 V.It also demonstrates outstanding stability in long-term electrolysis test at least for 45 h.展开更多
Background and purpose Current randomised controlled trials(RCTs)showed an uncertain benefit of haemostatic therapy on preventing haematoma expansion and improving the outcome in patients with intracerebral haemorrhag...Background and purpose Current randomised controlled trials(RCTs)showed an uncertain benefit of haemostatic therapy on preventing haematoma expansion and improving the outcome in patients with intracerebral haemorrhage(ICH).This meta-analysis aims to systematically evaluate the effect of haemostatic agents on the prevention of haemorrhage growth in patients with high-risk spontaneous ICH predicted by CT signs in RCTs.Methods A comprehensive search of PubMed,EMBASE and Cochrane library from 1 January 2005 to 30 June 2021 was conducted.RCTs that compared haemostatic agents with placebo for the treatment of spontaneous patients with ICH with high-risk haemorrhage growth were included.The primary endpoint was haematoma expansion at 24 hours.Other major endpoints of interest included 90-day functional outcome and mortality.Results The meta-analysis included four RCTs that randomised 2666 patients with ICH with high-risk haemorrhage growth.Haemostatic therapy reduced the rate of haematoma expansion at a marginally statistically significant level when compared with placebo(OR 0.84;95% CI 0.70 to 1.00;p=0.051).Subgroup analysis for patients with black hole sign on CT revealed a significant reduction of haematoma expansion with haemostatic therapy(OR 0.61;95% CI 0.39 to 0.94;p=0.03).However,both the primary analysis and subgroup analyses showed that haemostatic therapy could not reduce the rate of poor functional outcome(modified Rankin Scale>3)or death.Conclusions Haemostatic therapy showed a marginally significant benefit in reducing early haematoma expansion in patients with high-risk spontaneous ICH predicted by markers on CT scan.However,no significant improvement in functional outcome or reduction of mortality was observed.展开更多
Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decora...Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decorated N-doped carbon nanorods on graphite paper(CeO_(2)−x@NC/GP)were demonstrated as a highly efficient NO_(3)−RR electrocatalyst.The CeO_(2)−x@NC/GP catalyst manifests a significant NH_(3 )yield up to 712.75μmol·h^(−1)·cm^(−2) at−0.8 V vs.reversible hydrogen electrode(RHE)and remarkable Faradaic efficiency of 92.93%at−0.5 V vs.RHE under alkaline conditions,with excellent durability.Additionally,an assembled Zn-NO_(3)−battery with CeO_(2)−x@NC/GP as cathode accomplishes a high-power density of 3.44 mW·cm^(−2) and a large NH3 yield of 145.08μmol·h^(−1)·cm^(−2).Density functional theory results further expose the NO_(3)−reduction mechanism on CeO_(2)(111)surface with VO.展开更多
Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our rec...Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth(BZ-NiFe-LDH/CC)behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation,affords enlarged interlayer spacing of LDH,inhibits chlorine(electro)chemistry,and alleviates local pH drop of the electrode.It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm^(−2)in 1 M KOH.In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis,BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm^(−2)in alkaline seawater.Operando Raman spectroscopy studies further identify structural changes of disorderedδ(NiIII-O)during the seawater oxidation process.展开更多
Computational simulation provides an effective way of understanding the disordered structure and structureproperty relationships for metallic glass systems.Here,we systematically investigated the finite-size effects o...Computational simulation provides an effective way of understanding the disordered structure and structureproperty relationships for metallic glass systems.Here,we systematically investigated the finite-size effects of the static structure and dynamical behaviors in a three-dimensional Cu50Zr50 model metallic glass via classical molecular dynamics(MD)simulations.It was found that the local structure is insensitive to the system size while the dynamical properties present evident finite-size effects.The decoupling between local structure and relaxation dynamics in the investigated supercooling emerges when the system contains less than~2000 atoms.However,the collapse can be observed between the structural relaxation time and the dynamical heterogeneity for different sized systems across the whole range of our investigation.Our results support the intrinsic link between the structural relaxation time and dynamic heterogeneity and reveal the critical simulated system size for representing the structural origins of dynamics in bulk metallic glass with ignorable surface effects.展开更多
Background:Secondary central nervous system lymphoma(SCNSL)is defined as lymphoma involvement within the central nervous system(CNS)that originated elsewhere,or a CNS relapse of systemic lymphoma.Prognosis of SCNSL is...Background:Secondary central nervous system lymphoma(SCNSL)is defined as lymphoma involvement within the central nervous system(CNS)that originated elsewhere,or a CNS relapse of systemic lymphoma.Prognosis of SCNSL is poor and the most appropriate treatment is still undetermined.Methods:We conducted a retrospective study to assess the feasibility of an R-MIADD(rituximab,high-dose methotrexate,ifosfamide,cytarabine,liposomal formulation of doxorubicin,and dexamethasone)regimen for SCNSL patients.Results:Nineteen patients with newly diagnosed CNS lesions were selected,with a median age of 58(range 20 to 72)years.Out of 19 patients,11(57.9%)achieved complete remission(CR)and 2(10.5%)achieved partial remission(PR);the overall response rate was 68.4%.The median progression-free survival after CNS involvement was 28.0 months(95%confidence interval 11.0–44.9),and the median overall survival after CNS involvement was 34.5 months.Treatment-related death occurred in one patient(5.3%).Conclusions:These single-centered data underscore the feasibility of an R-MIADD regimen as the induction therapy of SCNSL,further investigation is warranted.展开更多
When the face of the inspected person and the photograph on their identification(ID)card cannot be clearly matched,the individual is undocumented,or the ID is forged,it is often difficult for the on‑site police to res...When the face of the inspected person and the photograph on their identification(ID)card cannot be clearly matched,the individual is undocumented,or the ID is forged,it is often difficult for the on‑site police to respond in time.This study proposes a number of key technologies for collecting fingerprints at mobile terminals for fast comparison using an automated fingerprint ID system(AFIS).These technologies ensure intelligent mobile fingerprint collection and allow the transmission of fingerprint information from the terminal to AFIS,over a wireless public security network for real‑time fingerprint comparison.This study also analyzes the feasibility and effectiveness of the proposed technologies for system design and the applicability of fingerprint ID algorithms.The system achieved good results in a test by the Shanghai Public Security Bureau Criminal Investigation Corps.展开更多
The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into val...The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into valuable resources.The process of converting NO_(3)^(-)to NH_(3)is complex,involving eight electron transfers and multiple intermediates,making the choice of electrocatalyst critical.In this study,we report a cobalt selenide(Co Se_(2))nanowire array on carbon cloth(CoSe_(2)/CC)as an effective electrocatalyst for the NO_(3)^(-)to NH_(3)conversion.In an alkaline medium with 0.1 mol/L NO_(3)^(-),CoSe_(2)/CC demonstrates exceptional NH_(3)Faradaic efficiency of 97.6%and a high NH_(3)yield of 517.7μmol h^(-1)cm^(-2)at-0.6 V versus the reversible hydrogen electrode.Furthermore,insights into the reaction mechanism of CoSe_(2)in the electrocatalytic NO_(3)^(-)reduction are elucidated through density functional theory calculations.展开更多
基金support from the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811)。
文摘Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.
文摘Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) production.Operating within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.
基金The authors extend their appreciation to the Deanship of Scientific Research at King Khalid University for funding support through large group Research Project(No.RGP2/257/44).
文摘The development of highly efficient and durable oxygen evolution reaction(OER)catalysts for seawater electrolysis is of great importance for applications.Here,an amorphous FeMoO_(4) nanorod array on Ni foam is reported as a highly active OER electrocatalyst in alkaline seawater,requiring only overpotentials of 303 and 332 mV to achieve 100 and 300 mA·cm^(-2),respectively.Moreover,it shows strong long-term electrochemical durability for at least 50 h.
基金This research was funded by Deputy for Research&Innovation,Ministry of Education through Initiative of Institutional Funding at University of Ha’il–Saudi Arabia through project number IFP-22098.
文摘Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nanosheet array on Ni foam(Co-Ni_(3)S_(2)/NF)as a high-efficiency OER electrocatalyst for seawater.In alkaline conditions,Co-Ni_(3)S_(2)/NF requires an overpotential of only 368 mV to drive 100 mA·cm^(–2),superior to Ni_(3)S_(2)/NF(385 mV).Besides,it exhibits at least 50-h continuous electrolysis.
基金supported by the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811).
文摘Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.
基金National Natural Science Foundation of China,Grant/Award Numbers:42277485,21976141,22272197,22102184,22102136,U22A20392Natural Science Foundation of Hubei Province,Grant/Award Numbers:2022CFB1001,2021CFA034+1 种基金Department of Education of Hubei Province,Grant/Award Numbers:Q20221701,Q20221704Joint Fund of Yulin University and Dalian National Laboratory for Clean Energy,Grant/Award Number:YLU-DNL Fund 2022008。
文摘The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and amine.This innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing field.This review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen species.Additionally,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding reactions.This critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.
基金support from the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province(No.JC2018004).
文摘Electrocatalytic synthesis of urea through C-N bond formation,converting carbon dioxide(CO_(2))and ni-trate(NO_(3)^(-)),presents a promising,less energy-intensive alternative to industrial urea production process.In this communication,we report the application of Mo_(2)C nanosheets-decorated carbon sheets(Mo_(2)C/C)as a highly efficient electrocatalyst for facilitating C-N coupling in ambient urea electrosynthesis.In CO_(2)-saturated 0.2 mol/L Na_(2)SO_(4)solution containing 0.05 mol/L NO_(3)^(-),the Mo_(2)C/C catalyst achieves an impres-sive urea yield of 579.13μg h^(-1)mg^(-1)with high Faradaic efficiency of 44.80%at-0.5 V versus the reversible hydrogen electrode.Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of^(∗)CO and^(∗)NH_(2)intermediates and facilitate their C-N coupling.This research propels the use of Mo_(2)C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in C-N coupling reactions.
基金the Deanship of Scientific Research at King Khalid University for funding support through large group Research Project under grant(No.RGP2/119/45).
文摘It is of great importance to design and develop electrocatalysts that are both long-lasting and efficient for seawater oxidation.Herein,a three-dimensional porous cauliflower-like Ni_(3)S_(2) foam on Ni foam(Ni_(3)S_(2) foam/NF)is proposed as a high-performance electrocatalyst for the oxygen evolution reaction in alkaline seawater.The as-synthesis Ni_(3)S_(2) foam/NF achieves exceptional efficacy,achieving a current density of 100 mA·cm^(−2)at mere overpotential of 369 mV.Notably,its electrocatalytic stability extends up to 1000 h at 500 mA·cm^(−2).
基金supported by the National Key R&D program of China(2016YFC1307301)National Natural Science Foundation of China(81820108012)+2 种基金National Natural Science Foundation of China(81870913)National Natural Science Foundation of China(81971614)Beijing Science and Technology Commission(D141100000114002).
文摘Background Studies show tranexamic acid can reduce the risk of death and early neurological deterioration after intracranial haemorrhage.We aimed to assess whether tranexamic acid reduces haematoma expansion and improves outcome in intracerebral haemorrhage patients susceptible to haemorrhage expansion.Methods We did a prospective,double-blind,randomised,placebo-controlled trial at 10 stroke centres in China.Acute supratentorial intracerebral haemorrhage patients were eligible if they had indication of haemorrhage expansion on admission imaging(eg,spot sign,black hole sign or blend sign),and were treatable within 8 hours of symptom onset.Patients were randomly assigned(1:1)to receive either tranexamic acid or a matching placebo.The primary outcome was intracerebral haematoma growth(>33% relative or>6 mL absolute)at 24 hours.Clinical outcomes were assessed at 90 days.Results Of the 171 included patients,124(72.5%)were male,and the mean age was 55.9±11.6 years.89 patients received tranexamic acid and 82 received placebo.The primary outcome did not differ significantly between the groups:36(40.4%)patients in the tranexamic acid group and 34(41.5%)patients in the placebo group had intracranial haemorrhage growth(OR 0.96,95% CI 0.52 to 1.77,p=0.89).The proportion of death was lower in the tranexamic acid treatment group than placebo group(8.1%vs 10.0%),but there were no significant differences in secondary outcomes including absolute intracranial haemorrhage growth,death and dependency.Conclusions Among patients susceptible to haemorrhage expansion treated within 8 hours of stroke onset,tranexamic acid did not significantly prevent intracerebral haemorrhage growth.Larger studies are needed to assess safety and efficacy of tranexamic acid in intracerebral haemorrhage patients.
基金supported by the National Natural Science Foundation of China(No.22072015).
文摘Seawater electrolysis is the most promising technology for large scale hydrogen production due to the abundance and low cost of seawater in nature.However,compared with the traditional freshwater electrolysis,the issues of electrode poisoning and corrosion will occur during the seawater electrolysis process,and active and stable electrocatalysts for the hydrogen evolution reaction(HER)are thus highly desired.In this work,N,O-doped carbon foam in-situ derived from commercial melamine foam is proposed as a high-active metal-free HER electrocatalyst for seawater splitting.In acidic seawater,our catalyst shows high hydrogen generation performance with small overpotential of 161 mV at 10 mA·cm^(−2),a low Tafel slop of 97.5 mV·dec^(−1),and outstanding stability.
基金the National Natural Science Foundation of China(No.22072015)the Opening Fund of Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research(Hunan Normal University),Ministry of Education(No.2020-02)+2 种基金Young Elite Scientist Sponsorship Program by CAST(No.YESS20210226)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020354)Deanship of Scientific Research at King Khalid University,Abha,Saudi Arabia for funding this work through the Research Group Program under No.RGP.2/79/43.
文摘Ambient electroreduction of nitrogen(N_(2))is considered as a green and feasible approach for ammonia(NH_(3))synthesis,which urgently demands for efficient electrocatalyst.Morphology has close relationship with catalytic activity of heterogeneous catalysts.Nanoribbon is attractive nanostructure,which possesses the flexibility of one-dimensional nanomaterials,the large surface area of two-dimensional nanomaterials,and lateral size confinement effects.In this work,Cu_(3)P nanoribbon is proposed as a highly efficient electrocatalyst for N_(2)-to-NH_(3)conversion under benign conditions.When measured in N_(2)-saturated 0.1 M HCl,such Cu_(3)P nanoribbon achieves high performance with an excellent Faradaic efficiency as high as 37.8%and a large yield of 18.9μg·h^(−1)·mgcat.−1 at−0.2 V.It also demonstrates outstanding stability in long-term electrolysis test at least for 45 h.
基金The study is funded by grants from the Beijing Science and Technology Commission(D141100000114002)National Natural Science Foundation of China(81820108012,81971614)National Key R&D Program of China(2016YFC1307301,2018YFC1312402).
文摘Background and purpose Current randomised controlled trials(RCTs)showed an uncertain benefit of haemostatic therapy on preventing haematoma expansion and improving the outcome in patients with intracerebral haemorrhage(ICH).This meta-analysis aims to systematically evaluate the effect of haemostatic agents on the prevention of haemorrhage growth in patients with high-risk spontaneous ICH predicted by CT signs in RCTs.Methods A comprehensive search of PubMed,EMBASE and Cochrane library from 1 January 2005 to 30 June 2021 was conducted.RCTs that compared haemostatic agents with placebo for the treatment of spontaneous patients with ICH with high-risk haemorrhage growth were included.The primary endpoint was haematoma expansion at 24 hours.Other major endpoints of interest included 90-day functional outcome and mortality.Results The meta-analysis included four RCTs that randomised 2666 patients with ICH with high-risk haemorrhage growth.Haemostatic therapy reduced the rate of haematoma expansion at a marginally statistically significant level when compared with placebo(OR 0.84;95% CI 0.70 to 1.00;p=0.051).Subgroup analysis for patients with black hole sign on CT revealed a significant reduction of haematoma expansion with haemostatic therapy(OR 0.61;95% CI 0.39 to 0.94;p=0.03).However,both the primary analysis and subgroup analyses showed that haemostatic therapy could not reduce the rate of poor functional outcome(modified Rankin Scale>3)or death.Conclusions Haemostatic therapy showed a marginally significant benefit in reducing early haematoma expansion in patients with high-risk spontaneous ICH predicted by markers on CT scan.However,no significant improvement in functional outcome or reduction of mortality was observed.
基金supported by the National Natural Science Foundation of China(No.22072015).
文摘Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decorated N-doped carbon nanorods on graphite paper(CeO_(2)−x@NC/GP)were demonstrated as a highly efficient NO_(3)−RR electrocatalyst.The CeO_(2)−x@NC/GP catalyst manifests a significant NH_(3 )yield up to 712.75μmol·h^(−1)·cm^(−2) at−0.8 V vs.reversible hydrogen electrode(RHE)and remarkable Faradaic efficiency of 92.93%at−0.5 V vs.RHE under alkaline conditions,with excellent durability.Additionally,an assembled Zn-NO_(3)−battery with CeO_(2)−x@NC/GP as cathode accomplishes a high-power density of 3.44 mW·cm^(−2) and a large NH3 yield of 145.08μmol·h^(−1)·cm^(−2).Density functional theory results further expose the NO_(3)−reduction mechanism on CeO_(2)(111)surface with VO.
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth(BZ-NiFe-LDH/CC)behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation,affords enlarged interlayer spacing of LDH,inhibits chlorine(electro)chemistry,and alleviates local pH drop of the electrode.It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm^(−2)in 1 M KOH.In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis,BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm^(−2)in alkaline seawater.Operando Raman spectroscopy studies further identify structural changes of disorderedδ(NiIII-O)during the seawater oxidation process.
基金supported by the Science Challenge Project (TZ2018004)the NSAF joint Program (U1930402)computational support from Beijing Computational Research Center (CSRC)
文摘Computational simulation provides an effective way of understanding the disordered structure and structureproperty relationships for metallic glass systems.Here,we systematically investigated the finite-size effects of the static structure and dynamical behaviors in a three-dimensional Cu50Zr50 model metallic glass via classical molecular dynamics(MD)simulations.It was found that the local structure is insensitive to the system size while the dynamical properties present evident finite-size effects.The decoupling between local structure and relaxation dynamics in the investigated supercooling emerges when the system contains less than~2000 atoms.However,the collapse can be observed between the structural relaxation time and the dynamical heterogeneity for different sized systems across the whole range of our investigation.Our results support the intrinsic link between the structural relaxation time and dynamic heterogeneity and reveal the critical simulated system size for representing the structural origins of dynamics in bulk metallic glass with ignorable surface effects.
基金This study was supported by the Capital’s Funds for Health Improvement and Research(2020-2-2049)。
文摘Background:Secondary central nervous system lymphoma(SCNSL)is defined as lymphoma involvement within the central nervous system(CNS)that originated elsewhere,or a CNS relapse of systemic lymphoma.Prognosis of SCNSL is poor and the most appropriate treatment is still undetermined.Methods:We conducted a retrospective study to assess the feasibility of an R-MIADD(rituximab,high-dose methotrexate,ifosfamide,cytarabine,liposomal formulation of doxorubicin,and dexamethasone)regimen for SCNSL patients.Results:Nineteen patients with newly diagnosed CNS lesions were selected,with a median age of 58(range 20 to 72)years.Out of 19 patients,11(57.9%)achieved complete remission(CR)and 2(10.5%)achieved partial remission(PR);the overall response rate was 68.4%.The median progression-free survival after CNS involvement was 28.0 months(95%confidence interval 11.0–44.9),and the median overall survival after CNS involvement was 34.5 months.Treatment-related death occurred in one patient(5.3%).Conclusions:These single-centered data underscore the feasibility of an R-MIADD regimen as the induction therapy of SCNSL,further investigation is warranted.
文摘When the face of the inspected person and the photograph on their identification(ID)card cannot be clearly matched,the individual is undocumented,or the ID is forged,it is often difficult for the on‑site police to respond in time.This study proposes a number of key technologies for collecting fingerprints at mobile terminals for fast comparison using an automated fingerprint ID system(AFIS).These technologies ensure intelligent mobile fingerprint collection and allow the transmission of fingerprint information from the terminal to AFIS,over a wireless public security network for real‑time fingerprint comparison.This study also analyzes the feasibility and effectiveness of the proposed technologies for system design and the applicability of fingerprint ID algorithms.The system achieved good results in a test by the Shanghai Public Security Bureau Criminal Investigation Corps.
基金funding support through large group research project(No.RGP2/119/45)。
文摘The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into valuable resources.The process of converting NO_(3)^(-)to NH_(3)is complex,involving eight electron transfers and multiple intermediates,making the choice of electrocatalyst critical.In this study,we report a cobalt selenide(Co Se_(2))nanowire array on carbon cloth(CoSe_(2)/CC)as an effective electrocatalyst for the NO_(3)^(-)to NH_(3)conversion.In an alkaline medium with 0.1 mol/L NO_(3)^(-),CoSe_(2)/CC demonstrates exceptional NH_(3)Faradaic efficiency of 97.6%and a high NH_(3)yield of 517.7μmol h^(-1)cm^(-2)at-0.6 V versus the reversible hydrogen electrode.Furthermore,insights into the reaction mechanism of CoSe_(2)in the electrocatalytic NO_(3)^(-)reduction are elucidated through density functional theory calculations.