A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and...A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.展开更多
The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecul...The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an an...While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an analysis framework(expression variance decomposition,EVaDe)for comparative single-cell expression data based on phenotypic evolution theory.After decomposing the gene expression variance into separate components,we use two strategies to identify genes exhibiting large between-taxon expression divergence and small within-cell-type expression noise in certain cell types,attributing this pattern to putative adaptive evolution.In a dataset of primate prefrontal cortex,we find that such humanspecific key genes enrich with neurodevelopment-related functions,while most other genes exhibit neutral evolution patterns.Specific neuron types are found to harbor more of these key genes than other cell types,thus likely to have experienced more extensive adaptation.Reassuringly,at the molecular sequence level,the key genes are significantly associated with the rapidly evolving conserved non-coding elements.An additional case analysis comparing the naked mole-rat(NMR)with the mouse suggests that innateimmunity-related genes and cell types have undergone putative expression adaptation in NMR.Overall,the EVaDe framework may effectively probe adaptive evolution mode in single-cell expression data.展开更多
This study presents a comprehensive phylogenetic analysis on Batrachospermaceae based on key taxonomic identifiers(rbcL,psaA,psbA,and COI-5P)from some genera.To systematically explore the phylogenetic relationships an...This study presents a comprehensive phylogenetic analysis on Batrachospermaceae based on key taxonomic identifiers(rbcL,psaA,psbA,and COI-5P)from some genera.To systematically explore the phylogenetic relationships and taxonomy within Batrachospermaceae,we integrated molecular and morphological data,and explored the phylogeny,character evolution,and ancestral geographical origin and provided a theoretical support for the classification and geographic origination of Batrachospermaceae.Our findings reveal distinct relationships within the phylogenetic tree.Notably,10 genera(Sirodotia,Batrachospermum,Tuomeya,Volatus,Lympha,Nothocladus,Torularia,Sheathia,Nocturama,and Petrohua)are closely associated in the rbcL phylogenetic tree.Additionally,four genera(Kumanoa,Hoefkenia,Notohesperus,and Virescentia)exhibit high support ratios,indicating their close interrelations.Other genera,including Paludicola,Visia,Acarposporophycos,Macrosporophycos,Visioidea,Balliopsis,and Psilosiphon,exhibit clustering traits.Furthermore,the multigene sequences provide a robust support for Montagnia that forms a monophyletic group.Ancestral reconstruction of morphological characters identifies nine primitive character states,including whorl,fascicle length,cortical cells,secondary fascicles,the shape of carpogonical branch,spermatangia,carposporophyte,carpogonium and trichogyne,with Visia likely representing ancestral traits in Batrachospermaceae.Furthermore,geographical origin maps suggest a potential common ancestral of Batrachospermaceae origin in the American continent.Additional to conventional analyses,including evolutionary and ancestral reconstruction investigations into key morphological characters,we attempt to reconstruct the biogeography within the Batrachospermaceae,thus contributing to a nuanced understanding of its origin.展开更多
Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a fo...Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.展开更多
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theor...The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theoretical and practical significance for guiding oil and gas exploration.The sedimentary facies and sedimentary evolution of the high-resolution sequence framework of the Carboniferous Taiyuan Formation in the Hangjinqi area have been systematically analyzed for the first time by drilling,logging and seismic data.The results show that four types of sequence interfaces can be identified in the Taiyuan Formation:regional unconformity surfaces,scour surfaces,lithologic-lithofacies transformation surfaces and flooding surfaces.According to the sedimentary response caused by the upward and downward movements of the base level at different levels,the Taiyuan Formation can be divided into 2 long-term cycles(LSC_(1)-LSC_(2)),4 mid-term cycles(MSC_(1)-MSC4)and 7 short-term cycles(SSC_(1)-SSC7).The long-and mid-term cycles correspond to members T_(1)and T_(2)and layers T_(1)-1,T_(1-2),T_(2-1),and T_(2)-2,respectively.Long-term cycles are dominated by C_(1);mid-term cycles are dominated by C_(1)and C_(2),followed by A2;and short-term cycles are dominated by C_(1),C_(2),A1 and A2.Under the high-resolution sequence stratigraphic framework,the Hangjinqi area underwent a transformation of fan delta and tidal flat depositional systems during the Taiyuan Formation sedimentary period.In the MSC_(1)-MSC_(2)stage,owing to a large-scale paleocontinent,the fan delta sedimentary body,which was limited in scale and scope,developed only in the southeastern corner and gradually transitioned basinward to tidal flat facies.In the MSC3-MSC4 stage,as the paleocontinent continuously decreased and the sedimentary range expanded,fan-delta plain sedimentation began in the study area.Several braided distributary channels with poor connectivity developed on the fan-delta plain,and between them were floodplains and peat swamps.展开更多
The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nano...Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.展开更多
Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and ma...Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and magnetic field enhanced-electrochemical activity remains to be fully elucidated.Herein,single-domain CoFe_(2)O_(4) catalysts with tunable oxygen vacancies(CFO-V_(O)) were synthesized to probe how V_(O) mediates magnetism and OER activity under magnetic field.The introduction of V_(O) can simultaneously modulate saturation magnetization(M_(s)) and coercivity(H_(c)),where the increased M_(s) dominates the magnetic field-enhanced OER activity.Under a 14,000 G magnetic field,the optimized CFO-V_(O) exhibits up to 16.1 % reduction in overpotential and 365 % enhancement in magnetocurrent(MC).Electrochemical analyses and post-OER characterization reveal that the magnetic field synergistically improves OER kinetics through lattice distortion induction,magnetohydrodynamic effect,and spin charge transfer effect.Importantly,the magnetic field promotes additional Co^(3+) generation to compensate for charge imbalance caused by V_(O) filling,maintaining dynamic equilibrium of V_(O) and effective reactant adsorption-conversion processes.This work unveils the synergistic mechanism of V_(O) and magnetic parameters for enhancing OER performance under the magnetic field,providing new insights into the design of high-efficiency spinregulated OER catalysts.展开更多
Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philologica...Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philological and historical analysis of ST,tracing its evolution from early battlefield applications to contemporary clinical use.By critically examining classical Mongolian medical texts alongside modern case studies,we aim to systematize ST’s therapeutic methods,indications,and limitations,while exploring its mechanisms of action through both traditional theory and modern biomedical perspectives.ST has undergone significant transformation,shifting from whole-body cavity immersion in the 13th century to targeted,organ-specific applications in modern practice.Its four primary methods–Covering,Mounted,Organ Placement,and Suction–demonstrate efficacy in treating cold-natured diseases,musculoskeletal disorders,gynecological conditions,and certain emergencies.ST embodies the core principles of TMM,particularly the balance of the“Three Roots”and the correction of cold-induced pathologies through heat.Despite challenges related to standardization,cultural translation,and regulatory acceptance,ST holds translational potential for integrative medicine.Future research should prioritize mechanistic validation,clinical standardization,and the development of biocompatible thermal technologies to bridge traditional practice with modern healthcare systems.展开更多
A complex system is inherently high-dimensional.Recent studies indicate that,even without complete knowledge of its evolutionary dynamics,the future behavior of such a system can be predicted using time-series data(da...A complex system is inherently high-dimensional.Recent studies indicate that,even without complete knowledge of its evolutionary dynamics,the future behavior of such a system can be predicted using time-series data(data-driven prediction).This suggests that the essential dynamics of a complex system can be captured through a low-dimensional representation.Virus evolution and climate change are two examples of complex,time-varying systems.In this article,we show that mutations in the spike protein provide valuable data for predicting SARS-CoV-2 variants,forecasting the possible emergence of the new macro-lineage Q in the near future.Our analysis also demonstrates that carbon dioxide concentration is a reliable indicator for predicting the evolution of the climate system,extending global surface air temperature(GSAT)forecasts through 2500.展开更多
Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a...Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a series of Schreibersite-type intermetallic compounds,particularly Mo_(2)Fe_(0.8)Ru_(0.2)P,are synthesized through high-temperature solid-phase synthesis.Experimental results demonstrate that the integration of Ru significantly improves the kinetics of proton adsorption and desorption during the hydrogen evolution reaction(HER).Additionally,density functional theory(DFT)calculations and X-ray absorption near edge structure(XANES)analyses effectively corroborate the pronounced d-orbital hybridization of Fe within the structure,which facilitates the transfer of hydroxide ions and the maintenance of material durability during alkaline HER processes.Remarkably,Mo_(2)Fe_(0.8)Ru_(0.2)P exhibits superior alkaline HER activity,characterized by an overpotential of merely 48 mV at a current density of 10 mA cm^(-2).After prolonged operation of 1000 h at high current densities(1.1 A cm^(-2)),the activity decline remains minimal,under 4%(with overpotential increasing from 258 mV to 268 mV).These results demonstrate the potential of strategically combining metallic elements to design high-performance industrial-grade electrocatalysts.展开更多
As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attra...As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attracted much attention from researchers due to its operational simplicity,the high purity of the hydrogen generated,and its potential for achieving zero carbon emissions throughout the process.Numerous studies has been manipulated on platinum(Pt)-based catalysts,which exhibit superior performance in hydrogen evolution reactions.Within this category,Pt nanoclusters stand out due to their unique attributes,such as quantum size effects and unique coordination environments.These features enable them to outperform both Pt metal atoms and nanoparticles in hydrogen evolution reactions regarding activity and stability.Here,we primarily delve into the reaction mechanisms underlying Pt nanocluster-based hydrogen catalysts,with particular emphasis on the interactions between the metal catalysts and their associated support materials.We provide an exhaustive summary of the strategies employed in the synthesis,the structural analyses conducted,and the performance metrics observed for Pt nanocluster catalysts when paired with various supporting materials.In closing,we explore the future potential and challenges facing Pt nanocluster-based catalysts in the context of industrial water electrolysis,along with emerging avenues for their design and optimization.展开更多
Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the...Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.展开更多
Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to thei...Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.展开更多
Photocatalysis provides a promising solution to the worldwide shortages of energy and industrially important raw materials by utilizing sunlight for coupled hydrogen(H_(2))production with controllable organic transfor...Photocatalysis provides a promising solution to the worldwide shortages of energy and industrially important raw materials by utilizing sunlight for coupled hydrogen(H_(2))production with controllable organic transformation.Herein,we demonstrate that PtFeNiCoCu high-entropy alloy(HEA)nanocrystals can act as efficient cocatalysts for H_(2)evolution coupled with selective oxidation of cinnamyl alcohol to cinnamaldehyde by cubic cadmium sulfide(CdS)quantum dots(QDs)with uniform sizes of 4.0±0.5 nm.HEA nanocrystals were prepared via a simple solvothermal approach,and were successfully integrated with CdS QDs by an electrostatic self-assembly method to construct HEA/CdS composites.The optimized HEA/CdS sample presented an enhanced photocatalytic H_(2)production rate of 7.15 mmol g^(-1)h^(-1),which was 13 times that of pure CdS QDs.Moreover,a cinnamyl alcohol conversion of 96.2%with cinnamaldehyde selectivity of 99.5%was achieved after photoreaction for 3 h.The integration of HEA with CdS QDs extended the optical absorption edge from 475 to 484 nm.From d-band center analysis,Pt atoms in the HEA are the active sites for H_(2)evolution,exhibiting higher catalytic activity than pure Pt.Meanwhile,the band structure of the CdS QDs enables the oxidative transformation of cinnamyl alcohol to cinnamaldehyde with high selectivity.Moreover,femtosecond transient absorption spectroscopy shows that HEA can significantly promote the separation of photogenerated carriers in CdS,which is vital for achieving enhanced photocatalytic activity.This work inspires atomic-level design of photocatalytic materials for coordinated production of green energy carriers and value-added products.展开更多
Ru-based nanomaterials have been demonstrated to be highly active electrocatalysts for hydrogen evo-lution reaction(HER),yet weak water adsorption and splitting ability in neutral media thus it is rather difficult for...Ru-based nanomaterials have been demonstrated to be highly active electrocatalysts for hydrogen evo-lution reaction(HER),yet weak water adsorption and splitting ability in neutral media thus it is rather difficult for the intermediates to adsorb on the active site.Herein,we introduce a concept of the prox-imity effect,com prising adjacent Ru and RuO_(2) nanoparticles coupled on TiO_(2)(Ru/RuO_(2)-TiO_(2)),for the synergic promotion of water molecule adsorption and splitting,significantly enhancing HER electrocatal-ysis performance.The in-situ spectroscopy experiments and density function theory(DFT)simulations demonstrated that the proximity effect between the adjacent Ru nanoparticles and RuO_(2) nanoparticles can accelerate water adsorption and splitting.As a result,the as-made Ru/RuO_(2)-TiO_(2) only need overpo-tentials of 52.7,16.0,and 16.4 mV to achieve the current density of 10 mA cm-2 in neutral,acid,and alkaline media,respectively.The mass activity of Ru/RuO_(2)-TiO_(2) in neutral media is 320 and 117 times higher than that of commercial Ru/C and Pt/C at the overpotential of 100 mV,respectively.This work emphasizes the proximity effect for activation of reactants which can be extended to other electrocat-alytic reactions.展开更多
The dissimilar 2B06 and 7B04 Al alloy joints were prepared by refill friction stir spot welding(RFSSW),and the microstructural evolution and corrosion behavior of the joints were investigated.Based on microstructural ...The dissimilar 2B06 and 7B04 Al alloy joints were prepared by refill friction stir spot welding(RFSSW),and the microstructural evolution and corrosion behavior of the joints were investigated.Based on microstructural analysis,the welded joints exhibit distinct microstructural zones,including the stir zone(SZ),thermomechanically affected zone(TMAZ),and heat-affected zone(HAZ).The grain size of each zone is in the order of HAZ>TMAZ>SZ.Notably,the TMAZ and HAZ contain significantly larger secondary-phase particles compared to the SZ,with particle size in the HAZ increasing at higher rotational speeds.Electrochemical tests indicate that corrosion susceptibility follows the sequence of HAZ>TMAZ>SZ>BM,with greater sensitivity observed at increased rotational speeds.Post-corrosion mechanical performance degradation primarily arises from crevice corrosion at joint overlaps,but not from the changes in the microstructure.展开更多
文摘A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.
文摘The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
文摘While methodology for determining the mode of evolution in coding sequences has been well established,evaluation of adaptation events in emerging types of phenotype data needs further development.Here,we propose an analysis framework(expression variance decomposition,EVaDe)for comparative single-cell expression data based on phenotypic evolution theory.After decomposing the gene expression variance into separate components,we use two strategies to identify genes exhibiting large between-taxon expression divergence and small within-cell-type expression noise in certain cell types,attributing this pattern to putative adaptive evolution.In a dataset of primate prefrontal cortex,we find that such humanspecific key genes enrich with neurodevelopment-related functions,while most other genes exhibit neutral evolution patterns.Specific neuron types are found to harbor more of these key genes than other cell types,thus likely to have experienced more extensive adaptation.Reassuringly,at the molecular sequence level,the key genes are significantly associated with the rapidly evolving conserved non-coding elements.An additional case analysis comparing the naked mole-rat(NMR)with the mouse suggests that innateimmunity-related genes and cell types have undergone putative expression adaptation in NMR.Overall,the EVaDe framework may effectively probe adaptive evolution mode in single-cell expression data.
基金Supported by the National Natural Science Foundation of China(No.32170204)。
文摘This study presents a comprehensive phylogenetic analysis on Batrachospermaceae based on key taxonomic identifiers(rbcL,psaA,psbA,and COI-5P)from some genera.To systematically explore the phylogenetic relationships and taxonomy within Batrachospermaceae,we integrated molecular and morphological data,and explored the phylogeny,character evolution,and ancestral geographical origin and provided a theoretical support for the classification and geographic origination of Batrachospermaceae.Our findings reveal distinct relationships within the phylogenetic tree.Notably,10 genera(Sirodotia,Batrachospermum,Tuomeya,Volatus,Lympha,Nothocladus,Torularia,Sheathia,Nocturama,and Petrohua)are closely associated in the rbcL phylogenetic tree.Additionally,four genera(Kumanoa,Hoefkenia,Notohesperus,and Virescentia)exhibit high support ratios,indicating their close interrelations.Other genera,including Paludicola,Visia,Acarposporophycos,Macrosporophycos,Visioidea,Balliopsis,and Psilosiphon,exhibit clustering traits.Furthermore,the multigene sequences provide a robust support for Montagnia that forms a monophyletic group.Ancestral reconstruction of morphological characters identifies nine primitive character states,including whorl,fascicle length,cortical cells,secondary fascicles,the shape of carpogonical branch,spermatangia,carposporophyte,carpogonium and trichogyne,with Visia likely representing ancestral traits in Batrachospermaceae.Furthermore,geographical origin maps suggest a potential common ancestral of Batrachospermaceae origin in the American continent.Additional to conventional analyses,including evolutionary and ancestral reconstruction investigations into key morphological characters,we attempt to reconstruct the biogeography within the Batrachospermaceae,thus contributing to a nuanced understanding of its origin.
基金support from the National Natural Science Foundation of China(Nos.12305373 and 52276220)the Guangzhou Basic Research Program(No.SL2024A04J00234).
文摘Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.
基金supported by the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
基金supported by the Fundamental Research Funds for the Liaoning Universities(Grant No.LJ202410166012).
文摘The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theoretical and practical significance for guiding oil and gas exploration.The sedimentary facies and sedimentary evolution of the high-resolution sequence framework of the Carboniferous Taiyuan Formation in the Hangjinqi area have been systematically analyzed for the first time by drilling,logging and seismic data.The results show that four types of sequence interfaces can be identified in the Taiyuan Formation:regional unconformity surfaces,scour surfaces,lithologic-lithofacies transformation surfaces and flooding surfaces.According to the sedimentary response caused by the upward and downward movements of the base level at different levels,the Taiyuan Formation can be divided into 2 long-term cycles(LSC_(1)-LSC_(2)),4 mid-term cycles(MSC_(1)-MSC4)and 7 short-term cycles(SSC_(1)-SSC7).The long-and mid-term cycles correspond to members T_(1)and T_(2)and layers T_(1)-1,T_(1-2),T_(2-1),and T_(2)-2,respectively.Long-term cycles are dominated by C_(1);mid-term cycles are dominated by C_(1)and C_(2),followed by A2;and short-term cycles are dominated by C_(1),C_(2),A1 and A2.Under the high-resolution sequence stratigraphic framework,the Hangjinqi area underwent a transformation of fan delta and tidal flat depositional systems during the Taiyuan Formation sedimentary period.In the MSC_(1)-MSC_(2)stage,owing to a large-scale paleocontinent,the fan delta sedimentary body,which was limited in scale and scope,developed only in the southeastern corner and gradually transitioned basinward to tidal flat facies.In the MSC3-MSC4 stage,as the paleocontinent continuously decreased and the sedimentary range expanded,fan-delta plain sedimentation began in the study area.Several braided distributary channels with poor connectivity developed on the fan-delta plain,and between them were floodplains and peat swamps.
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.
文摘Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.
基金supported by the “Climbing Plan” of Harbin Normal University (No.XKB202301)National Natural Science Foundation of China (Nos.21871065 and 22071038)。
文摘Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and magnetic field enhanced-electrochemical activity remains to be fully elucidated.Herein,single-domain CoFe_(2)O_(4) catalysts with tunable oxygen vacancies(CFO-V_(O)) were synthesized to probe how V_(O) mediates magnetism and OER activity under magnetic field.The introduction of V_(O) can simultaneously modulate saturation magnetization(M_(s)) and coercivity(H_(c)),where the increased M_(s) dominates the magnetic field-enhanced OER activity.Under a 14,000 G magnetic field,the optimized CFO-V_(O) exhibits up to 16.1 % reduction in overpotential and 365 % enhancement in magnetocurrent(MC).Electrochemical analyses and post-OER characterization reveal that the magnetic field synergistically improves OER kinetics through lattice distortion induction,magnetohydrodynamic effect,and spin charge transfer effect.Importantly,the magnetic field promotes additional Co^(3+) generation to compensate for charge imbalance caused by V_(O) filling,maintaining dynamic equilibrium of V_(O) and effective reactant adsorption-conversion processes.This work unveils the synergistic mechanism of V_(O) and magnetic parameters for enhancing OER performance under the magnetic field,providing new insights into the design of high-efficiency spinregulated OER catalysts.
基金supported by The China Ethnic Medicine Association Research Grant(No.2023MY055-81)Science and Technology Program of the Joint Fund of Scientific Research for the Public Hospitals of Inner Mongolia Academy of Medical Sciences(2023GLLHD177,2023GLLH0174)Inner Mongolia Autonomous Region Regional Medical Center for Specialized Care(2025).
文摘Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philological and historical analysis of ST,tracing its evolution from early battlefield applications to contemporary clinical use.By critically examining classical Mongolian medical texts alongside modern case studies,we aim to systematize ST’s therapeutic methods,indications,and limitations,while exploring its mechanisms of action through both traditional theory and modern biomedical perspectives.ST has undergone significant transformation,shifting from whole-body cavity immersion in the 13th century to targeted,organ-specific applications in modern practice.Its four primary methods–Covering,Mounted,Organ Placement,and Suction–demonstrate efficacy in treating cold-natured diseases,musculoskeletal disorders,gynecological conditions,and certain emergencies.ST embodies the core principles of TMM,particularly the balance of the“Three Roots”and the correction of cold-induced pathologies through heat.Despite challenges related to standardization,cultural translation,and regulatory acceptance,ST holds translational potential for integrative medicine.Future research should prioritize mechanistic validation,clinical standardization,and the development of biocompatible thermal technologies to bridge traditional practice with modern healthcare systems.
基金Natural science foundation of Inner Mongolia(2024LHMS06018)The basic scientific research funding for directly affiliated universities in the Inner Mongolia(JY20250094)。
文摘A complex system is inherently high-dimensional.Recent studies indicate that,even without complete knowledge of its evolutionary dynamics,the future behavior of such a system can be predicted using time-series data(data-driven prediction).This suggests that the essential dynamics of a complex system can be captured through a low-dimensional representation.Virus evolution and climate change are two examples of complex,time-varying systems.In this article,we show that mutations in the spike protein provide valuable data for predicting SARS-CoV-2 variants,forecasting the possible emergence of the new macro-lineage Q in the near future.Our analysis also demonstrates that carbon dioxide concentration is a reliable indicator for predicting the evolution of the climate system,extending global surface air temperature(GSAT)forecasts through 2500.
基金supported by Research Grants of the NRF(2023R1A2C2003823,RS-2024-00405818)funded by the National Research Foundation under the Ministry of Science,ICT&Future,Korea。
文摘Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels.In this study,a series of Schreibersite-type intermetallic compounds,particularly Mo_(2)Fe_(0.8)Ru_(0.2)P,are synthesized through high-temperature solid-phase synthesis.Experimental results demonstrate that the integration of Ru significantly improves the kinetics of proton adsorption and desorption during the hydrogen evolution reaction(HER).Additionally,density functional theory(DFT)calculations and X-ray absorption near edge structure(XANES)analyses effectively corroborate the pronounced d-orbital hybridization of Fe within the structure,which facilitates the transfer of hydroxide ions and the maintenance of material durability during alkaline HER processes.Remarkably,Mo_(2)Fe_(0.8)Ru_(0.2)P exhibits superior alkaline HER activity,characterized by an overpotential of merely 48 mV at a current density of 10 mA cm^(-2).After prolonged operation of 1000 h at high current densities(1.1 A cm^(-2)),the activity decline remains minimal,under 4%(with overpotential increasing from 258 mV to 268 mV).These results demonstrate the potential of strategically combining metallic elements to design high-performance industrial-grade electrocatalysts.
基金the National Key Research and Development Program of China(No.2022YFB4102000)the National Natural Science Foundation of China(NSFC,Nos.22102018 and 52171201)+4 种基金the Huzhou Science and Technology Bureau(No.2022GZ45)the Hefei National Research Center for Physical Sciences at the Microscale(No.KF2021005)the China Postdoctoral Science Foundation-Funded Project(No.2022M710601)the Huzhou Science and Technology Bureau(No.2023GZ02)the Natural Science Foundation of Sichuan Province(No.24NSFSC5779)。
文摘As hydrogen energy technologies gain momentum,the role of renewable energy in facilitating sustainable hydrogen production is becoming increasingly critical.As a hydrogen production method,water electrolysis has attracted much attention from researchers due to its operational simplicity,the high purity of the hydrogen generated,and its potential for achieving zero carbon emissions throughout the process.Numerous studies has been manipulated on platinum(Pt)-based catalysts,which exhibit superior performance in hydrogen evolution reactions.Within this category,Pt nanoclusters stand out due to their unique attributes,such as quantum size effects and unique coordination environments.These features enable them to outperform both Pt metal atoms and nanoparticles in hydrogen evolution reactions regarding activity and stability.Here,we primarily delve into the reaction mechanisms underlying Pt nanocluster-based hydrogen catalysts,with particular emphasis on the interactions between the metal catalysts and their associated support materials.We provide an exhaustive summary of the strategies employed in the synthesis,the structural analyses conducted,and the performance metrics observed for Pt nanocluster catalysts when paired with various supporting materials.In closing,we explore the future potential and challenges facing Pt nanocluster-based catalysts in the context of industrial water electrolysis,along with emerging avenues for their design and optimization.
基金supported by the Major Science and Technology Special Plan of Yunnan Province(Nos.202302AB080012 and 202402AB080004)the National Natural Science Foundation of China(No.22264025)+1 种基金the Basic Research Foundation of Yunnan Province(Nos.202401AS070033 and 202501AT070055)the Reserve talents for young and middleaged academic and technical leaders project of Yunnan Province(No.202405AC350071).
文摘Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.
基金financial support by the National Natural Science Foundation of China(No.52102241)Doctor of Suzhou University Scientific Research Foundation(Nos.2022BSK019,2020BS015)+2 种基金the Primary Research and Development Program of Anhui Province(No.201904a05020087)the Natural Science Research Project in Universities of Anhui Province in China(Nos.2022AH051386,KJ2021A1114)the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking Qilu University of Technology。
文摘Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
文摘Photocatalysis provides a promising solution to the worldwide shortages of energy and industrially important raw materials by utilizing sunlight for coupled hydrogen(H_(2))production with controllable organic transformation.Herein,we demonstrate that PtFeNiCoCu high-entropy alloy(HEA)nanocrystals can act as efficient cocatalysts for H_(2)evolution coupled with selective oxidation of cinnamyl alcohol to cinnamaldehyde by cubic cadmium sulfide(CdS)quantum dots(QDs)with uniform sizes of 4.0±0.5 nm.HEA nanocrystals were prepared via a simple solvothermal approach,and were successfully integrated with CdS QDs by an electrostatic self-assembly method to construct HEA/CdS composites.The optimized HEA/CdS sample presented an enhanced photocatalytic H_(2)production rate of 7.15 mmol g^(-1)h^(-1),which was 13 times that of pure CdS QDs.Moreover,a cinnamyl alcohol conversion of 96.2%with cinnamaldehyde selectivity of 99.5%was achieved after photoreaction for 3 h.The integration of HEA with CdS QDs extended the optical absorption edge from 475 to 484 nm.From d-band center analysis,Pt atoms in the HEA are the active sites for H_(2)evolution,exhibiting higher catalytic activity than pure Pt.Meanwhile,the band structure of the CdS QDs enables the oxidative transformation of cinnamyl alcohol to cinnamaldehyde with high selectivity.Moreover,femtosecond transient absorption spectroscopy shows that HEA can significantly promote the separation of photogenerated carriers in CdS,which is vital for achieving enhanced photocatalytic activity.This work inspires atomic-level design of photocatalytic materials for coordinated production of green energy carriers and value-added products.
基金supported by the Young Project of the Education Department in Guizhou Province(No.2022099)the Natural Science Special of Guizhou University(No.X202220 Special Post A).
文摘Ru-based nanomaterials have been demonstrated to be highly active electrocatalysts for hydrogen evo-lution reaction(HER),yet weak water adsorption and splitting ability in neutral media thus it is rather difficult for the intermediates to adsorb on the active site.Herein,we introduce a concept of the prox-imity effect,com prising adjacent Ru and RuO_(2) nanoparticles coupled on TiO_(2)(Ru/RuO_(2)-TiO_(2)),for the synergic promotion of water molecule adsorption and splitting,significantly enhancing HER electrocatal-ysis performance.The in-situ spectroscopy experiments and density function theory(DFT)simulations demonstrated that the proximity effect between the adjacent Ru nanoparticles and RuO_(2) nanoparticles can accelerate water adsorption and splitting.As a result,the as-made Ru/RuO_(2)-TiO_(2) only need overpo-tentials of 52.7,16.0,and 16.4 mV to achieve the current density of 10 mA cm-2 in neutral,acid,and alkaline media,respectively.The mass activity of Ru/RuO_(2)-TiO_(2) in neutral media is 320 and 117 times higher than that of commercial Ru/C and Pt/C at the overpotential of 100 mV,respectively.This work emphasizes the proximity effect for activation of reactants which can be extended to other electrocat-alytic reactions.
基金supported by the National Natural Science Foundation of China (Nos. 52075449, 51975480)。
文摘The dissimilar 2B06 and 7B04 Al alloy joints were prepared by refill friction stir spot welding(RFSSW),and the microstructural evolution and corrosion behavior of the joints were investigated.Based on microstructural analysis,the welded joints exhibit distinct microstructural zones,including the stir zone(SZ),thermomechanically affected zone(TMAZ),and heat-affected zone(HAZ).The grain size of each zone is in the order of HAZ>TMAZ>SZ.Notably,the TMAZ and HAZ contain significantly larger secondary-phase particles compared to the SZ,with particle size in the HAZ increasing at higher rotational speeds.Electrochemical tests indicate that corrosion susceptibility follows the sequence of HAZ>TMAZ>SZ>BM,with greater sensitivity observed at increased rotational speeds.Post-corrosion mechanical performance degradation primarily arises from crevice corrosion at joint overlaps,but not from the changes in the microstructure.
