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
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 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
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
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
Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this st...Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this study,Ni,Ru,and Pt ternary metals were embedded into nitrogen-doped hollow carbon spheres(NHCSs)by hydrothermal tandem heat treatment to form ternary supported metal nanoparticles with high dispersion and ultra-small particle size(~1.3 nm),which realized efficient hydrogen evolution from multi-scenario electrocatalytic water splitting.In the whole pH range,the performance of NiRuPt/NHCSs is better than that of commercial Pt/C catalyst,and the overpotentials under alkaline,neutral,and acidic conditions are as low as 15.5,20.0,and 29.5 mV,respectively.Under industrial conditions,NiRuPt/NHCSs also have excellent hydrogen evolution reaction(HER)performance,achieving efficient electrolysis of seawater for hydrogen production,and achieving Ampere-level hydrogen production at low voltage(~1.76 V)on integrated membrane electrode assemblies.Density functional theory(DFT)calculations show that in the NiRuPt ternary metal,the Pt site is conducive to promoting the desorption of*H to form H_(2),the Ru site is conducive to promoting the capture of H_(2)O,and the Ni site is conducive to promoting the dissociation of H_(2)O.Therefore,the formed NiRuPt ternary metal synergistically promotes multi-scenario efficient electrolysis of water to produce hydrogen.This study provides a new idea for the design of multi-component metal/carbon-based composite catalysts,and promotes the development of non-noble metal/noble metal composite catalysts in hydrogen production by electrolysis of water.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
Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/...Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/SnO_(2)heterojunction catalyst synthesized via an ion-exchange vulcanization method,which achieves exceptional activity and selectivity for CO_(2)-toformate conversion.Through in-situ Raman spectroscopy,ex-situ X-ray diffraction(XRD),and X-ray photoelectron spectroscopy(XPS),we demonstrate that the octahedral SnS_(2)/SnO_(2)heterojunction dynamically restructures into a sulfur-doped Sn/SnO_(2)(Sn(S)/SnO_(2))heterostructure under operating conditions.Density functional theory(DFT)calculations reveal that the Sn(S)/SnO_(2)interface facilitates electron transfer from SnO_(2)to metallic Sn(S),generating a built-in electric field that stabilizes Sn^(4+)in SnO_(2)and accelerates proton-coupled electron transfer to*OCHO intermediates.Consequently,the catalyst achieves a formate Faradaic efficiency exceeding 90% over a broad potential window(-0.6 to -1.0 V vs.reversible hydrogen electrode(RHE))with a high partial current density of -280 mA·cm^(-2),surpassing most reported Sn-based catalysts.This work elucidates the structural dynamics and interfacial enhancement mechanisms of heterojunction catalysts,offering a rational design principle for advanced CO_(2)RR electrocatalysts.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
Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the li...Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the linear scaling relationship,thereby exhibiting large overpotentials.In the lattice oxygen mechanism(LOM),the OER can be enhanced by enabling direct O_(2)formation.However,this enhancement is accompanied by the generation of oxygen vacancies,which presents a significant challenge to the long-term stability of LOMOER,particularly when operating at high current densities.Recently,the*O-*O coupling mechanism(OCM)has emerged as a promising alternative;it not only breaks the linear scaling relationship but also ensures catalytic stability.This review encapsulates the cutting-edge advancements in electrocatalysts that are grounded in the OCM,offering a detailed interpretation on the foundational principles guiding the design of OCM-OER catalysts.It also highlights recent theoretical investigations combining machine learning(ML)with density functional theory(DFT)calculations to reveal OER mechanisms.At the end of this review,the challenges and opportunities associated with OCM-OER electrocatalysts are discussed.展开更多
This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionar...This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionary processes.By representing agents and their defined environments with probabilistic interactions,ABM allows the assessment of the effects of individual behavior at the micro level on the greater social phenomena at the macro level.The review looks into the applications of ABM in portraying some of the key components of emotions and cognition-empathy,cooperation,decision making,and emotional transmission-and analyzes the problems including scalability,empirical validation,and description of sensitive emotional states.The most important conclusion is that merging ABM with information neurobiological data and artificial intelligence(AI)techniques would allow for deepening the interactions within the system and enhancing its responsiveness to stimuli.This review highlights approaches that aim to exploit the ABM methodology more fully and integrates methods from biology,neuroscience,and engineering.This integration could contribute to our understanding of the human behavior evolution and adaptation within systems relevant to policymaking,healthcare,and education.展开更多
This paper is about the transformation process of theoretical frameworks used in educational research on teaching evolution. To this end, some authors' claims, findings and suggestions offered via particular studi...This paper is about the transformation process of theoretical frameworks used in educational research on teaching evolution. To this end, some authors' claims, findings and suggestions offered via particular studies are evaluated. While the evaluated authors have represented secularism as a barrier to teaching evolution in the United States, they have also offered pedagogically theistic or agnostic evolution as the best choice for the reconciliation of religion and evolution. This paper is particularly concerned with one of the explanatory theoretical frameworks—religious cultural competence in evolution education(ReCCEE), which is derived from the cultural competence framework—although others are visited as well. Even though the schools or authors who have applied ReCCEE do not directly reference constructivism, their studies are built upon constructivist pedagogy and epistemological idealism. They often have problematic issues such as obscurantism, ad hominem attacks, cherry-picking and an ill-formed appeal to authority. Besides, these papers present biased or uncritical views and ill-informed definitions of some terms, such as secularism and agnosticism.展开更多
The globin superfamily,central to oxygen(O_(2))cascade dynamics,exemplifies how canalization—evolutionary stabilization of phenotypic traits—enables vertebrates to thrive in extreme environments.In birds,hemoglobins...The globin superfamily,central to oxygen(O_(2))cascade dynamics,exemplifies how canalization—evolutionary stabilization of phenotypic traits—enables vertebrates to thrive in extreme environments.In birds,hemoglobins(Hbs)serve as a paradigm of this process,with structural and functional canalization underpinning their exceptional aerobic capacity and elevational diversification.Despite significant advances of globins in our understanding of avian aerobic adaptation,a comprehensive synthesis of functional diversity,molecular evolution,and structural innovation is essential to fully elucidate their canalized roles in O_(2)homeostasis.Integrating perspectives on globin functional diversity and structural evolution,this review examines how chance(mutation/fixation biases)and contingency(historical genetic/epistatic constraints)shape Hb divergence and parallelism,thereby bridging molecular mechanisms with physiological adaptation in birds.We highlight how avian Hbs,canalized through compensatory substitutions and allosteric regulation,achieves a balance between evolutionary robustness and adaptive plasticity.However,critical gaps remain persist:the roles of understudied globins(e.g.,neuroglobin,globin E)and the mechanisms of genetic assimilation in migratory taxa.We propose an integrative framework that incorporates ecological divergence(elevation,flight endurance),phylogenetic timescales,and systems biology to unravel how canalization directs adaptive compromise.By focusing on birds within the amniotes,this synthesis advances a cohesive model for vertebrate evolution,wherein canalized globins reconcile metabolic precision with ecological innovation.Ultimately,this review refines hypotheses of O_(2)cascade evolution and calls for cross-disciplinary studies to decode the genetic and physiological architecture underlying adaptive canalization in extreme environments.展开更多
Addressing the kinetic limitations of oxygen evolution reaction(OER)is paramount for advancing rechargeable Zn-air batteries,thus it is extremely urgent to drive the development of effective and affordable electrocata...Addressing the kinetic limitations of oxygen evolution reaction(OER)is paramount for advancing rechargeable Zn-air batteries,thus it is extremely urgent to drive the development of effective and affordable electrocatalysts.This work constructs the interfacial structure of cobalt-iron alloys@phosphates(denoted as CoFe/CoFePO)as OER catalyst through a two-step approach using water-bath and hydrothermal methods,which demonstrated significant OER activity in alkaline media,requiring a low overpotential of 271 mV to achieve 10 mA cm^(−2) and exhibiting a competitive Tafel slope of 65 mV dec^(-1),alongside sustained operational stability.The enhanced performance can be attributed to the improved electrical conductivity due to the participation of CoFe alloys and the increased number of active sites through partial phosphorylation,which synergistically enhances charge transfer processes and accelerates OER kinetics.Moreover,dynamic structural evolution during OER process was thoroughly probed,and the results show that alloys@phosphates gradually evolve into phosphate radicalmodified CoFe hydroxyoxides that act as the actual active phase.Highlighting its practical applicability,the integration of prepared catalyst into zinc-air batteries leads to markedly improved performance,thereby offering promising new strategic directions for the development of next-generation OER electrocatalysts.展开更多
Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru ...Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.展开更多
This study reconstructs the lithofacies and paleogeographic evolution of North Africa during the Cambrian to Devonian periods,emphasizing the influence of tectonic events,sea-level fluctuations,and climatic changes on...This study reconstructs the lithofacies and paleogeographic evolution of North Africa during the Cambrian to Devonian periods,emphasizing the influence of tectonic events,sea-level fluctuations,and climatic changes on the region's depositional systems and basin development.Integrating seismic,well log,and core data,we identify key depositional patterns and their implications for hydrocarbon exploration.During sedimentation of diverse stages,the source-to-sink systems underwent significant transitions under provenance variation.During the Cambrian-Ordovician periods,intracratonic sag basins dominated,with braided river systems transitioning into glacial deposits in response to climatic cooling and glaciation.Under the control of the source-to-sink system,Silurian witnessed the opening of the Paleo-Tethys Ocean,leading to extensive marine transgressions and the deposition of organic-rich shales of the Lower Silurian,a primary hydrocarbon source rock.Regression during the Late Silurian introduced deltaic and fluvial systems,influenced by tectonic uplifting.During the Devonian period,the Hercynian Orogeny significantly impacted basin architecture,facilitating the development of passive margin basins.Braided and meandering river systems transitioned into deltaic and shallow marine environments,with Late Devonian anoxic conditions fostering the formation of additional hydrocarbon source rocks.This research highlights the interplay of tectonics,climate,and sea-level changes in shaping North Africa's sedimentary history.The findings provide critical insights into the distribution of hydrocarbon source and reservoir rocks,offering valuable guidance for exploration and development in the region.展开更多
Efficient industrial hydrogen production via water splitting hinges on the development of highly effective oxygen evolution catalysts and a clear understanding of their catalytic mechanisms.Among various strategies,ex...Efficient industrial hydrogen production via water splitting hinges on the development of highly effective oxygen evolution catalysts and a clear understanding of their catalytic mechanisms.Among various strategies,exploiting the synergistic effects of transition metals has shown great promise,although the underlying mechanisms remain elusive.Here,we investigate bi-transition metal borides,Mo_(2)MB_(2)(M=Co and Ni),as a model system to unravel these synergistic effects and the evolution of active species during the oxygen evolution reaction(OER).Using combined in-situ and ex-situ characterization techniques,we monitor the structural and valence changes of constituent elements in real time.We find that Mo and B undergo oxidation and dissolution at the anode,initiating distinct evolutionary pathways.In Mo_(2)MB_(2),rapid structural collapse leads to the formation ofγ-CoOOH as the active species.In contrast,Mo_(2)MB_(2) exhibits a more gradual surface-driven transformation,producingγ-NiOOH and Ni–O–Mo species.Chronopotentiometry testing reveals continued Mo and B dissolution,culminating in the transition ofγ-phases to amorphous states,followed by recrystallization intoβ-phases.This study provides critical insights into dissolution-induced structural evolution,active species dynamics,and the synergistic interactions between Mo/B and Co/Ni during OER catalysis.展开更多
Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong...Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong acid in PEMWE systems pose a major challenge to the stability of electrocatalysts,and the development of efficient and corrosion-resistant catalysts is urgently needed.Currently,iridium(Ir)-based catalysts have gained great attention due to their promising activity and stability,while the extremely low reserves of Ir in the earth seriously hinder the commercialization of PEMWE.Therefore,a systematic understanding of the latest advances in Ir-based catalysts is necessary to guide their rational design to meet the industrial requirements.In this review,the general reaction mechanisms and advanced characterization techniques for mechanism recognition are first introduced.Afterwards,the systematic design strategies and performances of Ir-based catalysts,including metallic Ir,Ir oxides,and Ir-based perovskites,are summarized in detail.Finally,the conclusions,challenges,and prospects for Ir-based electrocatalysts are presented.展开更多
An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-...An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-doped CoP electrocatalysts in the alkaline hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The introduction of Br modulates the electronic structure of the Co site,endowing Br-CoP with a more metallic character.In addition,P ion leaching promotes the in situ reconstruction of Br-CoOOH,which is the real active site for the OER reaction.Meanwhile,the HER situation is different.On the basis of P ion leaching,the leaching of Br ions promotes the formation of CoP-Co(OH)_(2) active species.In addition,Br doping enhances the adsorption of^(*)H,showing excellent H adsorption free energy,thereby greatly improving the HER activity.Simultaneously,it also enhances the adsorption of OOH^(*),effectively facilitating the occurrence of OER reactions.Br-CoP only needs 261 and 76 mV overpotential to drive the current density of 20 mA cm^(-2) and 10 mA^(-2),which can be maintained unchanged for 100 h.This study provides new insights into anion doping strategies and catalyst reconstruction mechanisms.展开更多
CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on cat...CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on catalyst performance.In this study,CoFe BMH nanoflowers(CoFe BMH NFs),CoFe BMH nanosheets(CoFe BMH NSHs),CoFe BMH nanorods(CoFe BMH NRs),and CoFe BMH nanospheres(CoFe BMH NSPs)were prepared on nickel foam via a hydrothermal method.CoFe BMH NSHs exhibited the most beneficial catalytic activity.At a current density of 100 mA·cm^(-2),its overpotential for oxygen evolution reaction(OER)was 282 mV,and the overall water splitting voltage was 2.05 V.The double-layer charging capacitance(Cdl)value of CoFe BMH NSHs was the largest in CoFe BMHs,which proves that CoFe BMH NSHs have the largest active area.Furthermore,the active site in the OER process was metal oxyhydroxide(MOOH)through in situ Raman characterization,and the generation of the active substance was an irreversible process.This work provides important insights into the design of catalyst morphologies and offers valuable guidelines for the enhancement of the performance of other catalysts.展开更多
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 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.
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 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financially supported by the Yunnan Fundamental Research Projects(Nos.202401CF070026 and 202501AT070017)the Scientific Research Fund Project of Yunnan Provincial Education Department(No.2024J0134)+1 种基金the Xingdian Talent Program of Yunnan Province,and the Scientific and Technological Project of Yunnan Precious Metals Laboratory(No.YPML-20240502065)Xinjiang Key Laboratory of Novel Functional Materials Chemistry Open Science Project(No.XJLNFMC-202406).
文摘Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this study,Ni,Ru,and Pt ternary metals were embedded into nitrogen-doped hollow carbon spheres(NHCSs)by hydrothermal tandem heat treatment to form ternary supported metal nanoparticles with high dispersion and ultra-small particle size(~1.3 nm),which realized efficient hydrogen evolution from multi-scenario electrocatalytic water splitting.In the whole pH range,the performance of NiRuPt/NHCSs is better than that of commercial Pt/C catalyst,and the overpotentials under alkaline,neutral,and acidic conditions are as low as 15.5,20.0,and 29.5 mV,respectively.Under industrial conditions,NiRuPt/NHCSs also have excellent hydrogen evolution reaction(HER)performance,achieving efficient electrolysis of seawater for hydrogen production,and achieving Ampere-level hydrogen production at low voltage(~1.76 V)on integrated membrane electrode assemblies.Density functional theory(DFT)calculations show that in the NiRuPt ternary metal,the Pt site is conducive to promoting the desorption of*H to form H_(2),the Ru site is conducive to promoting the capture of H_(2)O,and the Ni site is conducive to promoting the dissociation of H_(2)O.Therefore,the formed NiRuPt ternary metal synergistically promotes multi-scenario efficient electrolysis of water to produce hydrogen.This study provides a new idea for the design of multi-component metal/carbon-based composite catalysts,and promotes the development of non-noble metal/noble metal composite catalysts in hydrogen production by electrolysis of water.
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.
基金the Natural Science Foundation of Jiangsu Province(No.BK20253049)the Science and Technology Program of Xuzhou(No.KC25028)+3 种基金the Basic Science(Natural Science)Research Project of Higher Education Institutions in Jiangsu Province(No.25KJB430013)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.24KJA150003)the National Natural Science Foundation of China(No.22271122)the Xuzhou Key Research and Development Program(Social Development)(No.KC23298).
文摘Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/SnO_(2)heterojunction catalyst synthesized via an ion-exchange vulcanization method,which achieves exceptional activity and selectivity for CO_(2)-toformate conversion.Through in-situ Raman spectroscopy,ex-situ X-ray diffraction(XRD),and X-ray photoelectron spectroscopy(XPS),we demonstrate that the octahedral SnS_(2)/SnO_(2)heterojunction dynamically restructures into a sulfur-doped Sn/SnO_(2)(Sn(S)/SnO_(2))heterostructure under operating conditions.Density functional theory(DFT)calculations reveal that the Sn(S)/SnO_(2)interface facilitates electron transfer from SnO_(2)to metallic Sn(S),generating a built-in electric field that stabilizes Sn^(4+)in SnO_(2)and accelerates proton-coupled electron transfer to*OCHO intermediates.Consequently,the catalyst achieves a formate Faradaic efficiency exceeding 90% over a broad potential window(-0.6 to -1.0 V vs.reversible hydrogen electrode(RHE))with a high partial current density of -280 mA·cm^(-2),surpassing most reported Sn-based catalysts.This work elucidates the structural dynamics and interfacial enhancement mechanisms of heterojunction catalysts,offering a rational design principle for advanced CO_(2)RR electrocatalysts.
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supported by the National Natural Science Foundation of China(Nos.22373063 and 22302005)Fundamental Research Funds for the Central Universities of China(No.GK202203002)+1 种基金China Postdoctoral Science Foundation(No.2023M730044)Technology Innovation Leading Program of Shaanxi(Program No.2023KXJ-007).
文摘Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the linear scaling relationship,thereby exhibiting large overpotentials.In the lattice oxygen mechanism(LOM),the OER can be enhanced by enabling direct O_(2)formation.However,this enhancement is accompanied by the generation of oxygen vacancies,which presents a significant challenge to the long-term stability of LOMOER,particularly when operating at high current densities.Recently,the*O-*O coupling mechanism(OCM)has emerged as a promising alternative;it not only breaks the linear scaling relationship but also ensures catalytic stability.This review encapsulates the cutting-edge advancements in electrocatalysts that are grounded in the OCM,offering a detailed interpretation on the foundational principles guiding the design of OCM-OER catalysts.It also highlights recent theoretical investigations combining machine learning(ML)with density functional theory(DFT)calculations to reveal OER mechanisms.At the end of this review,the challenges and opportunities associated with OCM-OER electrocatalysts are discussed.
文摘This review explores the use of agent-based modeling(ABM)within the framework of study human emotion and cognition in the context of its ability to simulate complex social interactions,adaptive changes,and evolutionary processes.By representing agents and their defined environments with probabilistic interactions,ABM allows the assessment of the effects of individual behavior at the micro level on the greater social phenomena at the macro level.The review looks into the applications of ABM in portraying some of the key components of emotions and cognition-empathy,cooperation,decision making,and emotional transmission-and analyzes the problems including scalability,empirical validation,and description of sensitive emotional states.The most important conclusion is that merging ABM with information neurobiological data and artificial intelligence(AI)techniques would allow for deepening the interactions within the system and enhancing its responsiveness to stimuli.This review highlights approaches that aim to exploit the ABM methodology more fully and integrates methods from biology,neuroscience,and engineering.This integration could contribute to our understanding of the human behavior evolution and adaptation within systems relevant to policymaking,healthcare,and education.
文摘This paper is about the transformation process of theoretical frameworks used in educational research on teaching evolution. To this end, some authors' claims, findings and suggestions offered via particular studies are evaluated. While the evaluated authors have represented secularism as a barrier to teaching evolution in the United States, they have also offered pedagogically theistic or agnostic evolution as the best choice for the reconciliation of religion and evolution. This paper is particularly concerned with one of the explanatory theoretical frameworks—religious cultural competence in evolution education(ReCCEE), which is derived from the cultural competence framework—although others are visited as well. Even though the schools or authors who have applied ReCCEE do not directly reference constructivism, their studies are built upon constructivist pedagogy and epistemological idealism. They often have problematic issues such as obscurantism, ad hominem attacks, cherry-picking and an ill-formed appeal to authority. Besides, these papers present biased or uncritical views and ill-informed definitions of some terms, such as secularism and agnosticism.
基金supported by the National Natural Science Foundation of China(NSFC 31900313)to X.Z.the Central guide local science and technology development funds(XZ202301YD0007C)to L.Y.+1 种基金NSFC(32471572)National Key Research and Development Program of China(2024YFC2310303)to D.L。
文摘The globin superfamily,central to oxygen(O_(2))cascade dynamics,exemplifies how canalization—evolutionary stabilization of phenotypic traits—enables vertebrates to thrive in extreme environments.In birds,hemoglobins(Hbs)serve as a paradigm of this process,with structural and functional canalization underpinning their exceptional aerobic capacity and elevational diversification.Despite significant advances of globins in our understanding of avian aerobic adaptation,a comprehensive synthesis of functional diversity,molecular evolution,and structural innovation is essential to fully elucidate their canalized roles in O_(2)homeostasis.Integrating perspectives on globin functional diversity and structural evolution,this review examines how chance(mutation/fixation biases)and contingency(historical genetic/epistatic constraints)shape Hb divergence and parallelism,thereby bridging molecular mechanisms with physiological adaptation in birds.We highlight how avian Hbs,canalized through compensatory substitutions and allosteric regulation,achieves a balance between evolutionary robustness and adaptive plasticity.However,critical gaps remain persist:the roles of understudied globins(e.g.,neuroglobin,globin E)and the mechanisms of genetic assimilation in migratory taxa.We propose an integrative framework that incorporates ecological divergence(elevation,flight endurance),phylogenetic timescales,and systems biology to unravel how canalization directs adaptive compromise.By focusing on birds within the amniotes,this synthesis advances a cohesive model for vertebrate evolution,wherein canalized globins reconcile metabolic precision with ecological innovation.Ultimately,this review refines hypotheses of O_(2)cascade evolution and calls for cross-disciplinary studies to decode the genetic and physiological architecture underlying adaptive canalization in extreme environments.
基金supported by the National Natural Science Foundation of China(No.52002122).
文摘Addressing the kinetic limitations of oxygen evolution reaction(OER)is paramount for advancing rechargeable Zn-air batteries,thus it is extremely urgent to drive the development of effective and affordable electrocatalysts.This work constructs the interfacial structure of cobalt-iron alloys@phosphates(denoted as CoFe/CoFePO)as OER catalyst through a two-step approach using water-bath and hydrothermal methods,which demonstrated significant OER activity in alkaline media,requiring a low overpotential of 271 mV to achieve 10 mA cm^(−2) and exhibiting a competitive Tafel slope of 65 mV dec^(-1),alongside sustained operational stability.The enhanced performance can be attributed to the improved electrical conductivity due to the participation of CoFe alloys and the increased number of active sites through partial phosphorylation,which synergistically enhances charge transfer processes and accelerates OER kinetics.Moreover,dynamic structural evolution during OER process was thoroughly probed,and the results show that alloys@phosphates gradually evolve into phosphate radicalmodified CoFe hydroxyoxides that act as the actual active phase.Highlighting its practical applicability,the integration of prepared catalyst into zinc-air batteries leads to markedly improved performance,thereby offering promising new strategic directions for the development of next-generation OER electrocatalysts.
基金supported by the Development Project of Youth Innovation Team in Shandong Colleges and Universities(No.2019KJC031)the Natural Science Foundation of Shandong Province(Nos.ZR2019MB064,ZR2021MB122 and ZR2022MB137)the Doctoral Program of Liaocheng University(No.318051608).
文摘Pt-based materials are the benchmarked catalysts in the cathodic hydrogen evolution reaction(HER)of water splitting;the prohibitive cost and scarcity of Pt immensely impede the commercialization of hydrogen energy.Ru has aroused significant concern because of its Pt-like activity and much lower price.However,it’s still a top priority to minimize the Ru loading and pursue the most superior cost performance.
基金financially supported by the National Natural Science Foundation of China(Grant No.92255302).
文摘This study reconstructs the lithofacies and paleogeographic evolution of North Africa during the Cambrian to Devonian periods,emphasizing the influence of tectonic events,sea-level fluctuations,and climatic changes on the region's depositional systems and basin development.Integrating seismic,well log,and core data,we identify key depositional patterns and their implications for hydrocarbon exploration.During sedimentation of diverse stages,the source-to-sink systems underwent significant transitions under provenance variation.During the Cambrian-Ordovician periods,intracratonic sag basins dominated,with braided river systems transitioning into glacial deposits in response to climatic cooling and glaciation.Under the control of the source-to-sink system,Silurian witnessed the opening of the Paleo-Tethys Ocean,leading to extensive marine transgressions and the deposition of organic-rich shales of the Lower Silurian,a primary hydrocarbon source rock.Regression during the Late Silurian introduced deltaic and fluvial systems,influenced by tectonic uplifting.During the Devonian period,the Hercynian Orogeny significantly impacted basin architecture,facilitating the development of passive margin basins.Braided and meandering river systems transitioned into deltaic and shallow marine environments,with Late Devonian anoxic conditions fostering the formation of additional hydrocarbon source rocks.This research highlights the interplay of tectonics,climate,and sea-level changes in shaping North Africa's sedimentary history.The findings provide critical insights into the distribution of hydrocarbon source and reservoir rocks,offering valuable guidance for exploration and development in the region.
基金funding support from the National Science Fund for Distinguished Young Scholars(No.T2225027).
文摘Efficient industrial hydrogen production via water splitting hinges on the development of highly effective oxygen evolution catalysts and a clear understanding of their catalytic mechanisms.Among various strategies,exploiting the synergistic effects of transition metals has shown great promise,although the underlying mechanisms remain elusive.Here,we investigate bi-transition metal borides,Mo_(2)MB_(2)(M=Co and Ni),as a model system to unravel these synergistic effects and the evolution of active species during the oxygen evolution reaction(OER).Using combined in-situ and ex-situ characterization techniques,we monitor the structural and valence changes of constituent elements in real time.We find that Mo and B undergo oxidation and dissolution at the anode,initiating distinct evolutionary pathways.In Mo_(2)MB_(2),rapid structural collapse leads to the formation ofγ-CoOOH as the active species.In contrast,Mo_(2)MB_(2) exhibits a more gradual surface-driven transformation,producingγ-NiOOH and Ni–O–Mo species.Chronopotentiometry testing reveals continued Mo and B dissolution,culminating in the transition ofγ-phases to amorphous states,followed by recrystallization intoβ-phases.This study provides critical insights into dissolution-induced structural evolution,active species dynamics,and the synergistic interactions between Mo/B and Co/Ni during OER catalysis.
基金supported by the National Natural Science Foundation of China(22202053,22109035,52362031,and 52274297)the start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084,23068,and 23169)+4 种基金the Hainan Province Science and Technology Special Fund(ZDYF2024SHFZ074)the Collaborative Innovation Center of Marine Science and Technology,Hainan University(XTCX2022HYC04)the specific research fund of The Innovation Platform for Academicians of Hainan Province(YSPTZX202315)the Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202307)the Open Fund Project of Key Laboratory of Electrochemical Energy Storage and Energy Conversion in Hainan Province of China(KFKT2023002)。
文摘Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong acid in PEMWE systems pose a major challenge to the stability of electrocatalysts,and the development of efficient and corrosion-resistant catalysts is urgently needed.Currently,iridium(Ir)-based catalysts have gained great attention due to their promising activity and stability,while the extremely low reserves of Ir in the earth seriously hinder the commercialization of PEMWE.Therefore,a systematic understanding of the latest advances in Ir-based catalysts is necessary to guide their rational design to meet the industrial requirements.In this review,the general reaction mechanisms and advanced characterization techniques for mechanism recognition are first introduced.Afterwards,the systematic design strategies and performances of Ir-based catalysts,including metallic Ir,Ir oxides,and Ir-based perovskites,are summarized in detail.Finally,the conclusions,challenges,and prospects for Ir-based electrocatalysts are presented.
基金supported by the National Natural Science Foundation of China(62404063)the Natural Science Foundation of Heilongjiang Province(YQ2022B008,LH2023A011)+1 种基金the Basic research support plan project for outstanding young teachers in undergraduate universities of Heilongjiang Province(YQJH2023160)the Basic scientific research business expense project of Heilongjiang Provincial Department of Education(2022-KYYWF-0170).
文摘An in-depth understanding of the catalyst surface evolution is crucial for precise control of active sites,yet this aspect has often been overlooked.This study reveals the spontaneous anion regulation mechanism of Br-doped CoP electrocatalysts in the alkaline hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The introduction of Br modulates the electronic structure of the Co site,endowing Br-CoP with a more metallic character.In addition,P ion leaching promotes the in situ reconstruction of Br-CoOOH,which is the real active site for the OER reaction.Meanwhile,the HER situation is different.On the basis of P ion leaching,the leaching of Br ions promotes the formation of CoP-Co(OH)_(2) active species.In addition,Br doping enhances the adsorption of^(*)H,showing excellent H adsorption free energy,thereby greatly improving the HER activity.Simultaneously,it also enhances the adsorption of OOH^(*),effectively facilitating the occurrence of OER reactions.Br-CoP only needs 261 and 76 mV overpotential to drive the current density of 20 mA cm^(-2) and 10 mA^(-2),which can be maintained unchanged for 100 h.This study provides new insights into anion doping strategies and catalyst reconstruction mechanisms.
基金supported by the National Science Fund for Distinguished Young Scholars(No.52025041)the National Natural Science Foundation of China(Nos.52474319,52250091,U2341267,and 52450003)+1 种基金the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-02C2)supported by the Interdisciplinary Research Project for Young Teachers of USTB,China(Fundamental Research Funds for the Central Universities)(No.FRF-IDRY-GD23-003).
文摘CoFe bimetallic hydroxides(CoFe BMHs)find wide applications as excellent catalysts in the field of water splitting.However,no study has systematically investigated the influence of the morphologies of CoFe BMHs on catalyst performance.In this study,CoFe BMH nanoflowers(CoFe BMH NFs),CoFe BMH nanosheets(CoFe BMH NSHs),CoFe BMH nanorods(CoFe BMH NRs),and CoFe BMH nanospheres(CoFe BMH NSPs)were prepared on nickel foam via a hydrothermal method.CoFe BMH NSHs exhibited the most beneficial catalytic activity.At a current density of 100 mA·cm^(-2),its overpotential for oxygen evolution reaction(OER)was 282 mV,and the overall water splitting voltage was 2.05 V.The double-layer charging capacitance(Cdl)value of CoFe BMH NSHs was the largest in CoFe BMHs,which proves that CoFe BMH NSHs have the largest active area.Furthermore,the active site in the OER process was metal oxyhydroxide(MOOH)through in situ Raman characterization,and the generation of the active substance was an irreversible process.This work provides important insights into the design of catalyst morphologies and offers valuable guidelines for the enhancement of the performance of other catalysts.
