目的:对比三维多回波恢复梯度回波(3D MERGE)、三维可变反转角快速自旋回波(3D SPACE STIR)序列在腰椎间盘突出症(LDH)检查中的应用效果。方法:选择2020年1月~2022年11月收治的135例LDH患者,回顾性分析患者临床和磁共振成像(MRI)资料,...目的:对比三维多回波恢复梯度回波(3D MERGE)、三维可变反转角快速自旋回波(3D SPACE STIR)序列在腰椎间盘突出症(LDH)检查中的应用效果。方法:选择2020年1月~2022年11月收治的135例LDH患者,回顾性分析患者临床和磁共振成像(MRI)资料,所有患者均接受常规MRI扫描及3D MERGE、3D SPACE STIR序列扫描,对比3D MERGE、3D SPACE STIR序列测量神经根直径的一致性,评价两种序列的图像质量参数[信噪比(SNR)、对比噪声比(CNR)]、图像清晰度评分。结果:3D MERGE和3D SPACE STIR序列测量的L3~S1神经根直径比较差异无统计学意义(P>0.05),且两组序列测量的L3、L4、L5和S1直径均显示出较高相关性(r=0.957,0.986,0.975,0.972,P<0.05);3D MERGE序列的SNR及CNR均高于3D SPACE STIR序列,神经根显示分级、图像清晰度评分优于3D SPACE STIR序列,差异有统计学意义(P<0.05)。结论:3D MERGE、3D SPACE STIR序列在LDH神经根直径测量中具有极高一致性,3D MERGE序列较3D SPACE STIR序列能够更清晰显示神经跟的解剖形态,图像质量更好。展开更多
在循证医学时代下,依托规范的技术方法和标准化的操作规程发掘中医药独特优势,是实现中医药现代化、国际化发展并惠泽人类的必由之路。中医理论、人用经验和研究证据三结合证据体系的提出标志着中医药特色评价体系思维方法取得了重要进...在循证医学时代下,依托规范的技术方法和标准化的操作规程发掘中医药独特优势,是实现中医药现代化、国际化发展并惠泽人类的必由之路。中医理论、人用经验和研究证据三结合证据体系的提出标志着中医药特色评价体系思维方法取得了重要进步,经过恰当方法整合后的多元证据体是中医药临床指南推荐意见和循证卫生决策的有力支撑。本文基于当前国际证据合成与分级方法学前沿进展,初步提出中医药多元证据整合的方法学框架——MERGE(Merge Evidence-based Research and artificial intelliGence to support smart dEcision)框架,以期为中医药循证医学方法学体系的完善和发展提供借鉴和参考。展开更多
Due to the considerable uncertainties inherent in the datasets describing the spatiotemporal distributions of precipitation in the drylands of China,this study presents a new merged monthly precipitation product with ...Due to the considerable uncertainties inherent in the datasets describing the spatiotemporal distributions of precipitation in the drylands of China,this study presents a new merged monthly precipitation product with a spatial resolution of approximately 0.2°×0.2°during 1980–2019.The newly developed precipitation product was validated at different temporal scales(e.g.,monthly,seasonally,and annually).The results show that the new product consistently aligns with the spatiotemporal distributions reported by the Chinese Meteorological Administration Land Data Assimilation System(CLDAS)product and Multi-Source Weighted Ensemble Precipitation(MSWEP).The merged product exhibits exceptional quality in describing the drylands of China,with a bias of–2.19 mm month^(–1)relative to MSWEP.In addition,the annual trend of the merged product(0.09 mm month^(–1)yr^(−1))also closely aligns with that of the MSWEP(0.11 mm month^(–1)yr^(−1))during 1980–2019.The increasing trend indicates that the water cycle and wetting process intensified in the drylands of China during this period.In particular,there was an increase in wetting during the period from 2001–2019.Generally,the merged product exhibits potential value for improving our understanding of the climate and water cycle in the drylands of China.展开更多
Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the ...Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.展开更多
Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by ...Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.展开更多
This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abun...This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.展开更多
The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure ...The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure of the d-orbitals of CoP using cerium doping in this paper,thus significantly improving the intrinsic property and conductivity of CoP for water splitting.As a result,the as-synthesize porous Ce-doped CoP micro-polyhedron composite derived from Ce-ZIF-67 as bifunctional electrocatalytic materials exhibits excellent electrocatalytic performance in both the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),overpotentials of about 152 mV for HER at 10 mA cm^(-2)and about 352 mV for OER at 50 mA cm^(-2),and especially it shows outstanding long-term stability.Besides,an alkaline electrolyzer,using Ce0.04Co0.96P electrocatalyst as both the anode and cathode,delivers a cell voltage value of1.55 V at the current density of 10 mA cm^(-2).The calculation results of the density functional theory(DFT)demonstrate that the introduction of an appropriate amount of Ce into CoP can enhance the conductivity,and can induce the electronic modulation to regulate the selective adsorption of reaction intermediates on catalytic surface and the formation of O*intermediates(CoOOH),which exhibits an excellent electrocatalytic performance.This study provides novel insights into the design of an extraordinary performance water-splitting of the multicomponent electrocatalysts.展开更多
Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water spl...Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water splitting.In this study,we constructed a superior Ti-doped hematite photoanode(TiFeO)by employing SnOx as an electron transfer mediator,partially oxidized graphene(pGO)as a hole transfer mediator,and molecular Co cubane as a water oxidation catalyst.The Co/pGO/TiFeO/SnO_(x)integrated system achieves a photocurrent density of 2.52 mA cm–2 at 1.23 VRHE,which is 2.4 times higher than bare photoanode(1.04 mA cm^(-2)),with operational stability up to 100 h.Kinetic measurements indicate that pGO can promote charge transfer from TiFeO to the Co cubane catalyst.In contrast,SnOx reduces charge recombination at the interface between TiFeO and the fluorinated tin oxide substrate.In-situ infrared spectroscopy shows the formation of an O–O bonded intermediate during water oxidation.This study highlights the crucial role of incorporating dual charge-transfer mediators into photoelectrodes for efficient solar energy conversion.展开更多
Using natural gas(NG)as the primary fuel helps alleviate the fossil fuel crisis while reducing engine soot and nitrogen oxide(NO_(X))emissions.In this paper,the influences of a novel split injection concept on an NG h...Using natural gas(NG)as the primary fuel helps alleviate the fossil fuel crisis while reducing engine soot and nitrogen oxide(NO_(X))emissions.In this paper,the influences of a novel split injection concept on an NG high pressure direct injection(HPDI)engine are examined.Four typical split injection strategies,namely split pre-injection of pilot diesel(PD)and NG,split post-injection of PD and NG,split pre-injection of NG,and split post-injection of PD,were developed to investigate the influences on combustion and emissions.Results revealed that split pre injection of NG enhanced the atomization of PD,whereas the split post-injection of NG lowered the temperature in the core region of the PD spray,resulting in the deterioration of combustion.The effect of the split injection strategy on indicated thermal efficiency exceeded 7.5%.Split pre-injection was favorable to enhancing thermal efficiency,whereas split post-injection was not.Ignition delay,combustion duration,and premixed combustion time proportion were affected by injection strategies by 3.8%,50%,and 19.7%,respectively.Split pre-injection increased CH_(4) emission in the exhaust.Split post-injection,especially split post-injection of PD and NG,reduced the unburned CH_(4) emission by approximately 30%.When the split post-injection ratio was less than 30%,the trade-off between NO_(X) and soot was interrupted.The distribution range of hydroxyl radicals was expanded by pre-injection,and NO_(X) was generated in the region where the NG jet hit the wall.This paper provides valuable insights into the optimization of HPDI injection parameters.展开更多
Photocatalytic seawater splitting is an attractive way for producing green hydrogen.Significant progresses have been made recently in catalytic efficiencies,but the activity of catalysts can only maintain stable for a...Photocatalytic seawater splitting is an attractive way for producing green hydrogen.Significant progresses have been made recently in catalytic efficiencies,but the activity of catalysts can only maintain stable for about 10 h.Here,we develop a vacancy-engineered Ag_(3)PO_(4)/CdS porous microreactor chip photocatalyst,operating in seawater with a performance stability exceeding 300 h.This is achieved by the establishment of both catalytic selectivity for impurity ions and tailored interactions between vacancies and sulfur species.Efficient transport of carriers with strong redox ability is ensured by forming a heterojunction within a space charge region,where the visualization of potential distribution confirms the key design concept of our chip.Moreover,the separation of oxidation and reduction reactions in space inhibits the reverse recombination,making the chip capable of working at atmospheric pressure.Consequently,in the presence of Pt co-catalysts,a high solar-to-hydrogen efficiency of 0.81%can be achieved in the whole durability test.When using a fully solar-driven 256 cm2 hydrogen production prototype,a H_(2) evolution rate of 68.01 mmol h−1 m−2 can be achieved under outdoor insolation.Our findings provide a novel approach to achieve high selectivity,and demonstrate an efficient and scalable prototype suitable for practical solar H_(2) production.展开更多
Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to th...Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.展开更多
Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water spli...Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water splitting stands out as a promising approach for direct solar-driven hydrogen production.Enhancing the efficiency and stability of photoelectrodes is a key focus in PEC water-splitting research.Tantalum nitride(Ta_(3)N_(5)),with its suitable band gap and band-edge positions for PEC water splitting,has emerged as a highly promising photoanode material.This review begins by introducing the history and fundamental characteristics of Ta_(3)N_(5),emphasizing both its advantages and challenges.It then explores methods to improve light absorption efficiency,charge separation and transfer efficiency,surface reaction rate,and the stability of Ta_(3)N_(5) photoanodes.Additionally,the review discusses the progress of research on tandem PEC cells incorporating Ta_(3)N_(5) photoanodes.Finally,it looks ahead to future research directions for Ta_(3)N_(5) photoanodes.The strategic approach outlined in this review can also be applied to other photoelectrode materials,providing guidance for their development.展开更多
The progress of modern industry has given rise to great requirements for network transmission latency and reliability in domains such as smart grid and intelligent driving.To address these challenges,the concept of Ti...The progress of modern industry has given rise to great requirements for network transmission latency and reliability in domains such as smart grid and intelligent driving.To address these challenges,the concept of Time-sensitive networking(TSN)is proposed by IEEE 802.1TSN working group.In order to achieve low latency,Cyclic queuing and forwarding(CQF)mechanism is introduced to schedule Timetriggered(TT)flows.In this paper,we construct a TSN model based on CQF and formulate the flow scheduling problem as an optimization problem aimed at maximizing the success rate of flow scheduling.The problem is tackled by a novel algorithm that makes full use of the characteristics and the relationship between the flows.Firstly,by K-means algorithm,the flows are initially partitioned into subsets based on their correlations.Subsequently,the flows within each subset are sorted by a new special criteria extracted from multiple features of flow.Finally,a flow offset selecting method based on load balance is used for resource mapping,so as to complete the process of flow scheduling.Experimental results demonstrate that the proposed algorithm exhibits significant advantages in terms of scheduling success rate and time efficiency.展开更多
文摘目的:对比三维多回波恢复梯度回波(3D MERGE)、三维可变反转角快速自旋回波(3D SPACE STIR)序列在腰椎间盘突出症(LDH)检查中的应用效果。方法:选择2020年1月~2022年11月收治的135例LDH患者,回顾性分析患者临床和磁共振成像(MRI)资料,所有患者均接受常规MRI扫描及3D MERGE、3D SPACE STIR序列扫描,对比3D MERGE、3D SPACE STIR序列测量神经根直径的一致性,评价两种序列的图像质量参数[信噪比(SNR)、对比噪声比(CNR)]、图像清晰度评分。结果:3D MERGE和3D SPACE STIR序列测量的L3~S1神经根直径比较差异无统计学意义(P>0.05),且两组序列测量的L3、L4、L5和S1直径均显示出较高相关性(r=0.957,0.986,0.975,0.972,P<0.05);3D MERGE序列的SNR及CNR均高于3D SPACE STIR序列,神经根显示分级、图像清晰度评分优于3D SPACE STIR序列,差异有统计学意义(P<0.05)。结论:3D MERGE、3D SPACE STIR序列在LDH神经根直径测量中具有极高一致性,3D MERGE序列较3D SPACE STIR序列能够更清晰显示神经跟的解剖形态,图像质量更好。
文摘在循证医学时代下,依托规范的技术方法和标准化的操作规程发掘中医药独特优势,是实现中医药现代化、国际化发展并惠泽人类的必由之路。中医理论、人用经验和研究证据三结合证据体系的提出标志着中医药特色评价体系思维方法取得了重要进步,经过恰当方法整合后的多元证据体是中医药临床指南推荐意见和循证卫生决策的有力支撑。本文基于当前国际证据合成与分级方法学前沿进展,初步提出中医药多元证据整合的方法学框架——MERGE(Merge Evidence-based Research and artificial intelliGence to support smart dEcision)框架,以期为中医药循证医学方法学体系的完善和发展提供借鉴和参考。
基金supported by the National Natural Science Foundation of China the National Natural Science Foundation of China(Grant No.41991231)the Fundamental Research Funds for the Central Universities(lzujbky-2022-kb11).
文摘Due to the considerable uncertainties inherent in the datasets describing the spatiotemporal distributions of precipitation in the drylands of China,this study presents a new merged monthly precipitation product with a spatial resolution of approximately 0.2°×0.2°during 1980–2019.The newly developed precipitation product was validated at different temporal scales(e.g.,monthly,seasonally,and annually).The results show that the new product consistently aligns with the spatiotemporal distributions reported by the Chinese Meteorological Administration Land Data Assimilation System(CLDAS)product and Multi-Source Weighted Ensemble Precipitation(MSWEP).The merged product exhibits exceptional quality in describing the drylands of China,with a bias of–2.19 mm month^(–1)relative to MSWEP.In addition,the annual trend of the merged product(0.09 mm month^(–1)yr^(−1))also closely aligns with that of the MSWEP(0.11 mm month^(–1)yr^(−1))during 1980–2019.The increasing trend indicates that the water cycle and wetting process intensified in the drylands of China during this period.In particular,there was an increase in wetting during the period from 2001–2019.Generally,the merged product exhibits potential value for improving our understanding of the climate and water cycle in the drylands of China.
基金support by National Key Research and Development Program of China(2022YFB3803502)National Natural Science Foundation of China(52103076)+5 种基金Science and Technology Commission of Shanghai Municipality(23ZR1400300)special fund of Beijing Key Laboratory of Indoor Air Quality Evaluat ion and Control(NO.BZ0344KF21-02)State Key Laboratory of Electrical Insulation and Power Equipment(EIPE22203)JLF is a member of LSRE-LCM–Laboratory of Separation and Reaction Engineering-Laboratory of Catalysis and Materials,supported by national funds through FCT/MCTES(PIDDAC):LSRE-LCM,UIDB/50020/2020(DOI:10.54499/UIDB/50020/2020)UIDP/50020/2020(DOI:10.54499/UIDP/50020/2020)ALiCE,LA/P/0045/2020(DOI:10.54499/LA/P/0045/2020).
文摘Direct seawater splitting has emerged as a popular and promising research direction for synthesising clean,green,non-polluting,and sustainable hydrogen energy without depending on high-purity water in the face of the world’s shortage of fossil energy.However,efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria,microorganisms,and stray ions in seawater.Additionally,producing hydrogen on an industrial scale is challenging due to the high production cost.The present review addresses these challenges from the catalyst point of view,namely,that designing catalysts with high catalytic activity and stability can directly affect the rate and effect of seawater splitting.From the ion transfer perspective,designing membranes can block harmful ions,improving the stability of seawater splitting.From the energy point of view,mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting.Finally,ideas and directions for further research on direct seawater splitting in the future are pointed out,with the aim of achieving low-cost and high-efficiency hydrogen production.
基金support from the Czech Science Foundation,project EXPRO,No 19-27454Xsupport by the European Union under the REFRESH—Research Excellence For Region Sustainability and High-tech Industries project number CZ.10.03.01/00/22_003/0000048 via the Operational Programme Just Transition from the Ministry of the Environment of the Czech Republic+1 种基金Horizon Europe project EIC Pathfinder Open 2023,“GlaS-A-Fuels”(No.101130717)supported from ERDF/ESF,project TECHSCALE No.CZ.02.01.01/00/22_008/0004587).
文摘Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.
基金National Programs for NanoKey Project(2022YFA1504002)National Natural Science Foundation of China(22078233)。
文摘This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides(M/SLDH)through spontaneous redox and sulfurization processes.The developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm^(-2)in 1 M KOH,respectively.As both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm^(-2)and exhibited high structural robustness,maintaining stability at 1000 mA cm^(-2)for 300 h.In-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water oxidation.Additionally,ultraviolet photoelectron spectroscopy(UPS)and density functional theory(DFT)analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER activities.This study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.
基金supported by the National Natural Science Foundation of China(No.12162023&52268042)Key R&D Program of Gansu Province-International Cooperation Project(No.20YF8WA064)Natural Science Foundation of Gansu Province(No.22JR5RA253).
文摘The reasonable design of material morphology and eco-friendly electrocatalysts are essential to highly efficient water splitting.It is proposed that a promising strategy effectively regulates the electronic structure of the d-orbitals of CoP using cerium doping in this paper,thus significantly improving the intrinsic property and conductivity of CoP for water splitting.As a result,the as-synthesize porous Ce-doped CoP micro-polyhedron composite derived from Ce-ZIF-67 as bifunctional electrocatalytic materials exhibits excellent electrocatalytic performance in both the oxygen evolution reaction(OER)and the hydrogen evolution reaction(HER),overpotentials of about 152 mV for HER at 10 mA cm^(-2)and about 352 mV for OER at 50 mA cm^(-2),and especially it shows outstanding long-term stability.Besides,an alkaline electrolyzer,using Ce0.04Co0.96P electrocatalyst as both the anode and cathode,delivers a cell voltage value of1.55 V at the current density of 10 mA cm^(-2).The calculation results of the density functional theory(DFT)demonstrate that the introduction of an appropriate amount of Ce into CoP can enhance the conductivity,and can induce the electronic modulation to regulate the selective adsorption of reaction intermediates on catalytic surface and the formation of O*intermediates(CoOOH),which exhibits an excellent electrocatalytic performance.This study provides novel insights into the design of an extraordinary performance water-splitting of the multicomponent electrocatalysts.
文摘Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water splitting.In this study,we constructed a superior Ti-doped hematite photoanode(TiFeO)by employing SnOx as an electron transfer mediator,partially oxidized graphene(pGO)as a hole transfer mediator,and molecular Co cubane as a water oxidation catalyst.The Co/pGO/TiFeO/SnO_(x)integrated system achieves a photocurrent density of 2.52 mA cm–2 at 1.23 VRHE,which is 2.4 times higher than bare photoanode(1.04 mA cm^(-2)),with operational stability up to 100 h.Kinetic measurements indicate that pGO can promote charge transfer from TiFeO to the Co cubane catalyst.In contrast,SnOx reduces charge recombination at the interface between TiFeO and the fluorinated tin oxide substrate.In-situ infrared spectroscopy shows the formation of an O–O bonded intermediate during water oxidation.This study highlights the crucial role of incorporating dual charge-transfer mediators into photoelectrodes for efficient solar energy conversion.
基金Supported by the National Natural Science Foundation of China(No.51909154)Shanghai Engineering Research Center of Ship Intelligent Maintenance and Energy Efficiency(No.20DZ2252300).
文摘Using natural gas(NG)as the primary fuel helps alleviate the fossil fuel crisis while reducing engine soot and nitrogen oxide(NO_(X))emissions.In this paper,the influences of a novel split injection concept on an NG high pressure direct injection(HPDI)engine are examined.Four typical split injection strategies,namely split pre-injection of pilot diesel(PD)and NG,split post-injection of PD and NG,split pre-injection of NG,and split post-injection of PD,were developed to investigate the influences on combustion and emissions.Results revealed that split pre injection of NG enhanced the atomization of PD,whereas the split post-injection of NG lowered the temperature in the core region of the PD spray,resulting in the deterioration of combustion.The effect of the split injection strategy on indicated thermal efficiency exceeded 7.5%.Split pre-injection was favorable to enhancing thermal efficiency,whereas split post-injection was not.Ignition delay,combustion duration,and premixed combustion time proportion were affected by injection strategies by 3.8%,50%,and 19.7%,respectively.Split pre-injection increased CH_(4) emission in the exhaust.Split post-injection,especially split post-injection of PD and NG,reduced the unburned CH_(4) emission by approximately 30%.When the split post-injection ratio was less than 30%,the trade-off between NO_(X) and soot was interrupted.The distribution range of hydroxyl radicals was expanded by pre-injection,and NO_(X) was generated in the region where the NG jet hit the wall.This paper provides valuable insights into the optimization of HPDI injection parameters.
基金support from the Industry-University Cooperation Project of Fujian Province(2023H6003)F.L.gratefully acknowledges financial support from the Fuzhou Fuzhi Photocatalysis Research Center+1 种基金Q.C.gratefully acknowledges financial support from the National Natural Science Foundation of China(22022205,22372193)the CAS Project for Young Scientists in Basic Research(YSBR-054).
文摘Photocatalytic seawater splitting is an attractive way for producing green hydrogen.Significant progresses have been made recently in catalytic efficiencies,but the activity of catalysts can only maintain stable for about 10 h.Here,we develop a vacancy-engineered Ag_(3)PO_(4)/CdS porous microreactor chip photocatalyst,operating in seawater with a performance stability exceeding 300 h.This is achieved by the establishment of both catalytic selectivity for impurity ions and tailored interactions between vacancies and sulfur species.Efficient transport of carriers with strong redox ability is ensured by forming a heterojunction within a space charge region,where the visualization of potential distribution confirms the key design concept of our chip.Moreover,the separation of oxidation and reduction reactions in space inhibits the reverse recombination,making the chip capable of working at atmospheric pressure.Consequently,in the presence of Pt co-catalysts,a high solar-to-hydrogen efficiency of 0.81%can be achieved in the whole durability test.When using a fully solar-driven 256 cm2 hydrogen production prototype,a H_(2) evolution rate of 68.01 mmol h−1 m−2 can be achieved under outdoor insolation.Our findings provide a novel approach to achieve high selectivity,and demonstrate an efficient and scalable prototype suitable for practical solar H_(2) production.
基金supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization(NEDO),the JST Fusion Oriented Research for disruptive Science and Technology Program(JPMJFR213D)JSPS KAKENHI(JP24K17774)Domen for his guidance during their PhD studies at the University of Tokyo,as well as for his ongoing support,encouragement,and mentorship.
文摘Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.
文摘Harnessing solar energy for renewable fuel production through artificial photosynthesis offers an ideal solution to the current energy and environmental crises.Among various methods,photoelectrochemical(PEC)water splitting stands out as a promising approach for direct solar-driven hydrogen production.Enhancing the efficiency and stability of photoelectrodes is a key focus in PEC water-splitting research.Tantalum nitride(Ta_(3)N_(5)),with its suitable band gap and band-edge positions for PEC water splitting,has emerged as a highly promising photoanode material.This review begins by introducing the history and fundamental characteristics of Ta_(3)N_(5),emphasizing both its advantages and challenges.It then explores methods to improve light absorption efficiency,charge separation and transfer efficiency,surface reaction rate,and the stability of Ta_(3)N_(5) photoanodes.Additionally,the review discusses the progress of research on tandem PEC cells incorporating Ta_(3)N_(5) photoanodes.Finally,it looks ahead to future research directions for Ta_(3)N_(5) photoanodes.The strategic approach outlined in this review can also be applied to other photoelectrode materials,providing guidance for their development.
基金supported by Science and Technology Project of State Grid Corporation Headquarters under Grant 5108-202218280A-2-170-XG(Development and Application of Power Time-Sensitive Network Switching Chip。
文摘The progress of modern industry has given rise to great requirements for network transmission latency and reliability in domains such as smart grid and intelligent driving.To address these challenges,the concept of Time-sensitive networking(TSN)is proposed by IEEE 802.1TSN working group.In order to achieve low latency,Cyclic queuing and forwarding(CQF)mechanism is introduced to schedule Timetriggered(TT)flows.In this paper,we construct a TSN model based on CQF and formulate the flow scheduling problem as an optimization problem aimed at maximizing the success rate of flow scheduling.The problem is tackled by a novel algorithm that makes full use of the characteristics and the relationship between the flows.Firstly,by K-means algorithm,the flows are initially partitioned into subsets based on their correlations.Subsequently,the flows within each subset are sorted by a new special criteria extracted from multiple features of flow.Finally,a flow offset selecting method based on load balance is used for resource mapping,so as to complete the process of flow scheduling.Experimental results demonstrate that the proposed algorithm exhibits significant advantages in terms of scheduling success rate and time efficiency.
