Against the backdrop of escalating global climate change and energy crises,the resource utilization of carbon dioxide(CO_(2)),a major greenhouse gas,has become a crucial pathway for achieving carbon peaking and carbon...Against the backdrop of escalating global climate change and energy crises,the resource utilization of carbon dioxide(CO_(2)),a major greenhouse gas,has become a crucial pathway for achieving carbon peaking and carbon neutrality goals.The hydrogenation of CO_(2)to methanol not only enables carbon sequestration and recycling,but also provides a route to produce high value-added fuels and basic chemical feedstocks,holding significant environmental and economic potential.However,this conversion process is thermodynamically and kinetically limited,and traditional catalyst systems(e.g.,Cu/ZnO/Al_(2)O_(3))exhibit inadequate activity,selectivity,and stability under mild conditions.Therefore,the development of novel high-performance catalysts with precisely tunable structures and functionalities is imperative.Metal-organic frameworks(MOFs),as crystalline porous materials with high surface area,tunable pore structures,and diverse metal-ligand compositions,have the great potential in CO_(2)hydrogenation catalysis.Their structural design flexibility allows for the construction of well-dispersed active sites,tailored electronic environments,and enhanced metal-support interactions.This review systematically summarizes the recent advances in MOF-based and MOF-derived catalysts for CO_(2)hydrogenation to methanol,focusing on four design strategies:(1)spatial confinement and in situ construction,(2)defect engineering and ion-exchange,(3)bimetallic synergy and hybrid structure design,and(4)MOF-derived nanomaterial synthesis.These approaches significantly improve CO_(2)conversion and methanol selectivity by optimizing metal dispersion,interfacial structures,and reaction pathways.The reaction mechanism is further explored by focusing on the three main reaction pathways:the formate pathway(HCOO*),the RWGS(Reverse Water Gas Shift reaction)+CO*hydrogenation pathway,and the trans-COOH pathway.In situ spectroscopic studies and density functional theory(DFT)calculations elucidate the formation and transformation of key intermediates,as well as the roles of active sites,metal-support interfaces,oxygen vacancies,and promoters.Additionally,representative catalytic performance data for MOFbased systems are compiled and compared,demonstrating their advantages over traditional catalysts in terms of CO_(2)conversion,methanol selectivity,and space-time yield.Future perspectives for MOF-based CO_(2)hydrogenation catalysts will prioritize two main directions:structural design and mechanistic understanding.The precise construction of active sites through multi-metallic synergy,defect engineering,and interfacial electronic modulation should be made to enhance catalyst selectivity and stability.In addition,advanced in situ characterization techniques combined with theoretical modeling are essential to unravel the detailed reaction mechanisms and intermediate behaviors,thereby guiding rational catalyst design.Moreover,to enable industrial application,challenges related to thermal/hydrothermal stability,catalyst recyclability,and cost-effective large-scale synthesis must be addressed.The development of green,scalable preparation methods and the integration of MOF catalysts into practical reaction systems(e.g.,flow reactors)will be crucial for bridging the gap between laboratory research and commercial deployment.Ultimately,multi-scale structure-performance optimization and catalytic system integration will be vital for accelerating the industrialization of MOF-based CO_(2)-to-methanol technologies.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
Hydrogen energy development is transitioning from vision and plan-ning to widespread application.To date,more than 60 countries and regions have announced hydrogen energy development strategies focused on accelerating...Hydrogen energy development is transitioning from vision and plan-ning to widespread application.To date,more than 60 countries and regions have announced hydrogen energy development strategies focused on accelerating demonstration projects and real-world deployment.展开更多
A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)...A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)S,metallic copper converts chalcopyrite into bornite(Cu_(5)FeS_(4)).However,the introduction of H_(2)S promotes the formation of chalcocite(Cu_(2)S)by altering the oxidation pathway of copper.Electrochemical analysis demonstrates that the presence of H₂S significantly reduces the corrosion potential of copper from 0.251 to−0.223 V(vs SHE),reaching the threshold necessary for the formation of Cu_(2)S.Nevertheless,excessive H_(2)S triggers sulfate reduction via the reaction of 8Cu+H_(2)SO_(4)+3H_(2)S=4Cu_(2)S+4H_(2)O(ΔG=−519.429 kJ/mol at 50℃),leading to inefficient copper utilization.展开更多
Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphou...Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt%H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).展开更多
Molecular hydrogen(H2)demonstrates selective antioxidant and anti-inflammatory properties with therapeutic potential across musculoskeletal conditions including osteoarthritis,rheumatoid arthritis,exercise-induced mus...Molecular hydrogen(H2)demonstrates selective antioxidant and anti-inflammatory properties with therapeutic potential across musculoskeletal conditions including osteoarthritis,rheumatoid arthritis,exercise-induced muscle damage,chronic pain syndromes,tendinopathies,and muscle atrophy.This review critically evaluates preclinical and clinical evidence for H2 therapy and identifies research gaps.A comprehensive search of PubMed,EMBASE,and Cochrane Library(up to April 2025)yielded 45 eligible studies:25 preclinical and 20 clinical trials.Preclinical models consistently showed reductions in reactive oxygen species,inflammatory cytokines,and improved cell viability.Clinical trials reported symptomatic relief in osteoarthritis,decreased Disease Activity Score 28 in rheumatoid arthritis,and accelerated clearance of muscle damage markers.Delivery methods varied-hydrogen-rich water,gas inhalation,and saline infusion-hindering direct comparison.Mechanistic biomarkers were inconsistently reported,limiting understanding of target engagement.Common limitations included small sample sizes,short durations,and protocol heterogeneity.Despite these constraints,findings suggest H2 may serve as a promising adjunctive therapy via antioxidant,anti-inflammatory,and cytoprotective mechanisms.Future research should prioritize standardized delivery protocols,robust mechanistic endpoints,and longer-term randomized trials to validate clinical efficacy and optimize therapeutic strategies.展开更多
Electrosynthesis of hydrogen peroxide through the two-electron oxygen reduction pathway provides a crucial alternative to the energy-intensive anthraquinone process.Nevertheless,the efficicency for hydrogen peroxide g...Electrosynthesis of hydrogen peroxide through the two-electron oxygen reduction pathway provides a crucial alternative to the energy-intensive anthraquinone process.Nevertheless,the efficicency for hydrogen peroxide generation is limited by the competitive four-electron pathway.In this work,we report a noncovalent modulation strategy for the isolated CoN_(4) sites by metal-phthalocyanine molecules confinement,which boosts the two-electron oxygen reduction towards generating hydrogen peroxide.The confined Co-phthalocyanine molecules on CoN_(4) sites through π-π interactions induce the competitive*OOH adsorption between the two Co sites formed nanochannel.This noncovalent modulation contributes to the weakened*OOH binding on CoN_(4) sites and thus suppresses its further dissociation,achieving the maximum selectivity of 95% with high activity for H_(2)O_(2)production.This work shows that tailoring noncovalent interactions beyond the binding sites is a promising approach to modulate the local structure of isolated metal sites and related catalytic performance.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
Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in ...Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in the total hydrogen storage capacity due to“dead weight.”Here,we synthesize an optimized N-doped porous carbon(rN-pC)without heavy metal as supporting scaffold to confine Mg/MgH_(2) nanoparticles(Mg/MgH_(2)@rN-pC).rN-pC with 60 wt%loading capacity of Mg(denoted as 60 Mg@rN-pC)can adsorb and desorb 0.62 wt%H_(2) on the rN-pC scaffold.The nanoconfined MgH_(2) can be chemically dehydrided at 175℃,providing~3.59 wt%H_(2) with fast kinetics(fully dehydrogenated at 300℃ within 15 min).This study presents the first realization of nanoconfined Mg-based system with adsorption-active scaffolds.Besides,the nanoconfined MgH_(2) formation enthalpy is reduced to~68 kJ mol^(−1) H_(2) from~75 kJ mol^(−1) H_(2) for pure MgH_(2).The composite can be also compressed to nanostructured pellets,with volumetric H_(2) density reaching 33.4 g L^(−1) after 500 MPa compression pressure,which surpasses the 24 g L^(−1) volumetric capacity of 350 bar compressed H_(2).Our approach can be implemented to the design of hybrid H_(2) storage materials with enhanced capacity and desorption rate.展开更多
The integration of wind power and natural gas for hydrogen production forms a Green and Blue Hydrogen Integrated Energy System(GBH-IES),which is a promising cogeneration approach characterized by multienergy complemen...The integration of wind power and natural gas for hydrogen production forms a Green and Blue Hydrogen Integrated Energy System(GBH-IES),which is a promising cogeneration approach characterized by multienergy complementarity,flexible dispatch,and efficient utilization.This system can meet the demands for electricity,heat,and hydrogen while demonstrating significant performance in energy supply,energy conversion,economy,and environment(4E).To evaluate the GBH-IES system effectively,a comprehensive performance evaluation index system was constructed from the 4E dimensions.The fuzzy DEMATEL method was used to quantify the causal relationships between indicators,establishing a scientific input-output assessment system.The DEA model was then employed for preliminary performance evaluation of the hydrogen storage system,followed by the entropy weight TOPSIS method to enhance the accuracy and reliability of the assessment results.The study also conducted a comprehensive benefit evaluation and sensitivity analysis for different cases involving blue hydrogen,green hydrogen,and their synergistic effects under varying carbon emission factors(CEFs)and hydrogen blending ratios(HBRs).The results indicate that combining green and blue hydrogen can achieve higher comprehensive benefits for the hydrogen storage system,providing valuable insights for hydrogen storage development and demonstrating the effectiveness of themulti-criteria decision-making methods used.展开更多
To simultaneously improve the critical factors in photocatalytic H_(2)production,the population of active photogenerated electrons,the adsorption and activation of H_(2)O molecules,and the surface dehydrogenation effi...To simultaneously improve the critical factors in photocatalytic H_(2)production,the population of active photogenerated electrons,the adsorption and activation of H_(2)O molecules,and the surface dehydrogenation efficiency,we propose a synergistic strategy for TiO_(2)modification by combining transition metal(TM)doping and N-doped carbon(N-C)coating.The targeted Cr-TiO_(2)@N-C heterojunction exhibits dramatically enhanced H_(2)production under blue light irradiation,contrasting sharply with a negligible production by pristine TiO_(2).Comprehensive structural characterization and theoretical calculations confirm the uniform substitution of Cr into the TiO_(2)lattice,promoting the formation of adjacent oxygen vacancies(VO).The synergistic effect of Cr doping and VO extends the light absorption range into the visible region.The coated N-C layer facilitates the efficient separation of photogenerated charge carriers,boosting the population of active electrons.Critically,the combined action of VO and N-C layer enhances the adsorption and activation of H_(2)O molecules while effectively improving the subsequent surface dehydrogenation efficiency.Significantly,this strategy demonstrates broad universality:Analogous TM-TiO_(2)@N-C heterojunctions(TM=Mn,Co,Ni,Cu,and Zn)synthesized via the same approach all show substantially improved H_(2)production performance over pristine TiO_(2).展开更多
3D printing,as a versatile additive manufacturing technique,offers high design flexibility,rapid prototyping,minimal material waste,and the capability to fabricate complex,customized geometries.These attributes make i...3D printing,as a versatile additive manufacturing technique,offers high design flexibility,rapid prototyping,minimal material waste,and the capability to fabricate complex,customized geometries.These attributes make it particularly well-suited for low-temperature hydrogen electrochemical conversion devices—specifically,proton exchange membrane fuel cells,proton exchange membrane electrolyzer cells,anion exchange membrane electrolyzer cells,and alkaline electrolyzers—which demand finely structured components such as catalyst layers,gas diffusion layers,electrodes,porous transport layers,and bipolar plates.This review provides a focused and critical summary of the current progress in applying 3D printing technologies to these key components.It begins with a concise introduction to the principles and classifications of mainstream 3D printing methods relevant to the hydrogen energy sector and proceeds to analyze their specific applications and performance impacts across different device architectures.Finally,the review identifies existing technical challenges and outlines future research directions to accelerate the integration of 3D printing in nextgeneration low-temperature hydrogen energy systems.展开更多
Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via lo...Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.展开更多
The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges rem...The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges remain in achieving broad visiblelight absorption and suppressing charge recombination.In this work,we developed a series of photocatalysts through in situ embedding of red-emissive CDs(R-CDs)into g-C_(3)N_(4)(RCN)with precisely controlled loading amounts.Systematic characterization revealed that the R-CDs incorporation simultaneously addresses two fundamental limitations:(1)extending the light absorption edge to 800 nm,and(2)acting as an electron acceptor,facilitating charge separation.The optimized RCN composite demonstrates exceptional H_(2)evolution activity(1.87 mmol·g^(-1)·h^(-1),wavelength(λ)≥420 nm),representing a 3.3-fold enhancement over pristine g-C_(3)N_(4).Remarkably,the apparent quantum efficiency(AQE)reaches 9.1% at 420 nm,while maintaining measurable activity beyond 475 nm,where unmodified g-C_(3)N_(4)shows negligible response.This study provides fundamental insights into band structure engineering and charge carrier management through rational design of CDs-modified semiconductor heterostructures.展开更多
Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Pre-chamber ignition technology can address the issue of uneven in-cylinder mixture combustion in large-bore marine engines.The impact of various pre-chamber structures on the formation of the mixture and jet flames w...Pre-chamber ignition technology can address the issue of uneven in-cylinder mixture combustion in large-bore marine engines.The impact of various pre-chamber structures on the formation of the mixture and jet flames within the pre-chamber is explored.This study performed numerical simulations on a large-bore marine ammonia/hydrogen pre-chamber engine prototype,considering pre-chamber volume,throat diameter,the distance between the hydrogen injector and the spark plug,and the hydrogen injector angle.Compared with the original engine,when the pre-chamber volume is 73.4 ml,the throat diameter is 14 mm,the distance ratio is 0.92,and the hydrogen injector angle is 80°.Moreover,the peak pressure in the pre-chamber increased by 23.1%,and that in the main chamber increased by 46.3%.The results indicate that the performance of the original engine is greatly enhanced by altering its fuel and pre-chamber structure.展开更多
In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperat...In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperature(T_(c))of 1D superconductors is low.In this work,we theoretically investigate the possible high T_(c) superconductivity of(5,5)carbon nanotube(CNT).The pristine(5,5)CNT is a Dirac semimetal and can be modulated into a semiconductor by full hydrogenation.Interestingly,by further hole doping,it can be regulated into a metallic state with the sp3-hybridized𝜎electrons metalized,and a giant Kohn anomaly appears in the optical phonons.The two factors together enhance the electron–phonon coupling,and lead to high-T_(c) superconductivity.When the hole doping concentration of hydrogenated-(5,5)CNT is 2.5 hole/cell,the calculated T_(c) is 82.3 K,exceeding the boiling point of liquid nitrogen.Therefore,the predicted hole-doped hydrogenated-(5,5)CNT provides a new platform for 1D high-T_(c) superconductivity and may have potential applications in 1D nanodevices.展开更多
Atomically ordered precious intermetallic nanoparticles have garnered significant attention for diverse applications due to their well-defined surface atomic arrangements and exceptional electronic and geometric prope...Atomically ordered precious intermetallic nanoparticles have garnered significant attention for diverse applications due to their well-defined surface atomic arrangements and exceptional electronic and geometric properties.However,synthesizing non-precious ordered intermetallics that exhibit high stability under operating conditions remains a formidable challenge,primarily owing to their strong oxyphilicity,highly negative reduction potentials,and low corrosion resistance.In this work,we report a facile yet versatile seed-mediated solid-phase approach for fabricating uniform Ni_(3)Ga_(1) intermetallic nanocubes(NCs)fully encapsulated within N-doped carbon layers(denoted as Ni_(3)Ga_(1)@NC-800).Extensive characterization confirms the formation of a unique core-shell architecture,with atomic-resolution structural analysis and X-ray absorption fine structure measurements unequivocally verifying the atomically ordered Ni_(3)Ga_(1) intermetallic phase.The Ni_(3)Ga_(1)@NC-800 catalyst demonstrates exceptional performance in the 1,4-hydrogenation of α,β-unsaturated carbonyl compounds,exhibiting both remarkable activity and exclusive selectivity while maintaining high stability over multiple reaction cycles without observable performance decay.Combined experimental and theoretical calculations reveal that the strong interatomic p-d orbital hybridization facilitates electron transfer from Ga to Ni atoms,resulting in electron localization on ordered Ni atoms.This electronic configuration positively influences H_(2)activation and optimizes substrate adsorption strength,thereby substantially improving catalytic efficiency.Furthermore,this synthetic strategy proves generalizable,successfully extending to the synthesis of other non-precious ordered Ni_(1)Sn_(1) and Ni_(2)In_(3) intermetallics confined within N-doped carbon matrices.展开更多
The vip-host chemistry in polymer electrolytes plays a crucial role for all-solid-state Li metal batteries,where the stable operation of such batteries heavily relies on high ion conductivity,strong mechanical prope...The vip-host chemistry in polymer electrolytes plays a crucial role for all-solid-state Li metal batteries,where the stable operation of such batteries heavily relies on high ion conductivity,strong mechanical properties,and stable interfaces of the electrolyte.While traditional ceramic fillers can boost ion conductivity,they fail to improve interfacial stability.In this study,we introduce intermolecular hydrogen bonding into a polyethylene oxide(PEO)-based polymer electrolyte through the incorporation of metal organic framework(MOF)and lithium nitrate additives.The hydrogen on the PEO chain is found to be tightly interacted with the oxygen nodes of UiO-66 MOF and nitrate anions,creating a cross-linked framework that reduces the crystallinity of the PEO and enhances the integrity of composite.This interaction induces a beneficial Li3N and LiF-rich solid electrolyte interphase,ensuring 2000 h of stable lithium metal operation without short-circuits.The strong polysulfide adsorption enables compatibility with high-capacity sulfur cathodes,resulting in solidstate Li-S batteries that can achieve a high capacity of 913.8 mAh·g^(-1)and exhibit stable cycling performance.This work demonstrates the deep understanding of vip-host chemistry in polymer electrolytes and their potential in developing energy-dense solid-state Li metal batteries.展开更多
A hydrogen energy storage system(HESS)is one of the many risingmodern green innovations,using excess energy to generate hydrogen and storing it for various purposes.With that,there have been many discussions about com...A hydrogen energy storage system(HESS)is one of the many risingmodern green innovations,using excess energy to generate hydrogen and storing it for various purposes.With that,there have been many discussions about commercializing HESS and improving it further.However,the design and sizing process can be overwhelming to comprehend with various sources to examine,and understanding optimal design methodologies is crucial to optimize a HESS design.With that,this review aims to collect and analyse a wide range of HESS studies to summarise recent studies.Two different collections of studies are studied,one was sourced by the main author for preliminary readings,and another was obtained via VOSViewer.The findings from the Web of Science platform were also examined for amore comprehensive understanding.Major findings include the People’sRepublic of China has been active in HESS research,as most works and active organizations originate from this country.HESS has been mainly researched to support power generation and balance load demands,with financial analysis being the common scope of analysis.MATLAB is a common tool used for HESS design,modelling,and optimization as it can handle complex calculations.Artificial neural network(ANN)has the potential to be used to model the HESS,but additional review is required as a formof future work.From a commercialization perspective,pressurized hydrogen tanks are ideal for hydrogen storage in a HESS,but other methods can be considered after additional research and development.From this review,it can be implied that modelling works will be the way forward for HESS research,but extensive collaborations and additional review are needed.Overall,this review summarized various takeaways that future research works on HESS can use.展开更多
基金Supported by the National Key Research and Development Program of China(2023YFB4104500,2023YFB4104502)the National Natural Science Foundation of China(22138013)the Taishan Scholar Project(ts201712020).
文摘Against the backdrop of escalating global climate change and energy crises,the resource utilization of carbon dioxide(CO_(2)),a major greenhouse gas,has become a crucial pathway for achieving carbon peaking and carbon neutrality goals.The hydrogenation of CO_(2)to methanol not only enables carbon sequestration and recycling,but also provides a route to produce high value-added fuels and basic chemical feedstocks,holding significant environmental and economic potential.However,this conversion process is thermodynamically and kinetically limited,and traditional catalyst systems(e.g.,Cu/ZnO/Al_(2)O_(3))exhibit inadequate activity,selectivity,and stability under mild conditions.Therefore,the development of novel high-performance catalysts with precisely tunable structures and functionalities is imperative.Metal-organic frameworks(MOFs),as crystalline porous materials with high surface area,tunable pore structures,and diverse metal-ligand compositions,have the great potential in CO_(2)hydrogenation catalysis.Their structural design flexibility allows for the construction of well-dispersed active sites,tailored electronic environments,and enhanced metal-support interactions.This review systematically summarizes the recent advances in MOF-based and MOF-derived catalysts for CO_(2)hydrogenation to methanol,focusing on four design strategies:(1)spatial confinement and in situ construction,(2)defect engineering and ion-exchange,(3)bimetallic synergy and hybrid structure design,and(4)MOF-derived nanomaterial synthesis.These approaches significantly improve CO_(2)conversion and methanol selectivity by optimizing metal dispersion,interfacial structures,and reaction pathways.The reaction mechanism is further explored by focusing on the three main reaction pathways:the formate pathway(HCOO*),the RWGS(Reverse Water Gas Shift reaction)+CO*hydrogenation pathway,and the trans-COOH pathway.In situ spectroscopic studies and density functional theory(DFT)calculations elucidate the formation and transformation of key intermediates,as well as the roles of active sites,metal-support interfaces,oxygen vacancies,and promoters.Additionally,representative catalytic performance data for MOFbased systems are compiled and compared,demonstrating their advantages over traditional catalysts in terms of CO_(2)conversion,methanol selectivity,and space-time yield.Future perspectives for MOF-based CO_(2)hydrogenation catalysts will prioritize two main directions:structural design and mechanistic understanding.The precise construction of active sites through multi-metallic synergy,defect engineering,and interfacial electronic modulation should be made to enhance catalyst selectivity and stability.In addition,advanced in situ characterization techniques combined with theoretical modeling are essential to unravel the detailed reaction mechanisms and intermediate behaviors,thereby guiding rational catalyst design.Moreover,to enable industrial application,challenges related to thermal/hydrothermal stability,catalyst recyclability,and cost-effective large-scale synthesis must be addressed.The development of green,scalable preparation methods and the integration of MOF catalysts into practical reaction systems(e.g.,flow reactors)will be crucial for bridging the gap between laboratory research and commercial deployment.Ultimately,multi-scale structure-performance optimization and catalytic system integration will be vital for accelerating the industrialization of MOF-based CO_(2)-to-methanol technologies.
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Hydrogen energy development is transitioning from vision and plan-ning to widespread application.To date,more than 60 countries and regions have announced hydrogen energy development strategies focused on accelerating demonstration projects and real-world deployment.
基金financially supported by the National Key Research and Development Program of China (No. 2022YFC2105300)。
文摘A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)S,metallic copper converts chalcopyrite into bornite(Cu_(5)FeS_(4)).However,the introduction of H_(2)S promotes the formation of chalcocite(Cu_(2)S)by altering the oxidation pathway of copper.Electrochemical analysis demonstrates that the presence of H₂S significantly reduces the corrosion potential of copper from 0.251 to−0.223 V(vs SHE),reaching the threshold necessary for the formation of Cu_(2)S.Nevertheless,excessive H_(2)S triggers sulfate reduction via the reaction of 8Cu+H_(2)SO_(4)+3H_(2)S=4Cu_(2)S+4H_(2)O(ΔG=−519.429 kJ/mol at 50℃),leading to inefficient copper utilization.
基金supported by the National Natural Science Foundation of China(22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009).
文摘Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt%H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).
文摘Molecular hydrogen(H2)demonstrates selective antioxidant and anti-inflammatory properties with therapeutic potential across musculoskeletal conditions including osteoarthritis,rheumatoid arthritis,exercise-induced muscle damage,chronic pain syndromes,tendinopathies,and muscle atrophy.This review critically evaluates preclinical and clinical evidence for H2 therapy and identifies research gaps.A comprehensive search of PubMed,EMBASE,and Cochrane Library(up to April 2025)yielded 45 eligible studies:25 preclinical and 20 clinical trials.Preclinical models consistently showed reductions in reactive oxygen species,inflammatory cytokines,and improved cell viability.Clinical trials reported symptomatic relief in osteoarthritis,decreased Disease Activity Score 28 in rheumatoid arthritis,and accelerated clearance of muscle damage markers.Delivery methods varied-hydrogen-rich water,gas inhalation,and saline infusion-hindering direct comparison.Mechanistic biomarkers were inconsistently reported,limiting understanding of target engagement.Common limitations included small sample sizes,short durations,and protocol heterogeneity.Despite these constraints,findings suggest H2 may serve as a promising adjunctive therapy via antioxidant,anti-inflammatory,and cytoprotective mechanisms.Future research should prioritize standardized delivery protocols,robust mechanistic endpoints,and longer-term randomized trials to validate clinical efficacy and optimize therapeutic strategies.
基金financially supported by the National Natural Science Foundation of China(No.U21A2077)the Natural Science Foundation of Shandong Province(Nos.ZR2022JQ08 and 2023HWYQ-028)+4 种基金the Taishan Scholar Project Foundation of Shandong Province(Nos.tsqn202211028 and tsqn202306080)the City University of Hong Kong(Nos.9020005,9610663,and 7020103)ITF-RTH-Global STEM Professorship(No.9446008)Hong Kong Branch of National Precious Metals Material Engineering Research Center—ITC FundGeneral Research Fund(No.9043720)from the Research Grants Council of Hong Kong SAR,China.
文摘Electrosynthesis of hydrogen peroxide through the two-electron oxygen reduction pathway provides a crucial alternative to the energy-intensive anthraquinone process.Nevertheless,the efficicency for hydrogen peroxide generation is limited by the competitive four-electron pathway.In this work,we report a noncovalent modulation strategy for the isolated CoN_(4) sites by metal-phthalocyanine molecules confinement,which boosts the two-electron oxygen reduction towards generating hydrogen peroxide.The confined Co-phthalocyanine molecules on CoN_(4) sites through π-π interactions induce the competitive*OOH adsorption between the two Co sites formed nanochannel.This noncovalent modulation contributes to the weakened*OOH binding on CoN_(4) sites and thus suppresses its further dissociation,achieving the maximum selectivity of 95% with high activity for H_(2)O_(2)production.This work shows that tailoring noncovalent interactions beyond the binding sites is a promising approach to modulate the local structure of isolated metal sites and related catalytic performance.
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 Key R&D Program of China(2022YFB3803700)National Natural Science Foundation of China(52171186)+1 种基金Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)support from“Zhiyuan Honor Program”for doctoral students,Shanghai Jiao Tong University.
文摘Nanoconfinement is a promising approach to simultaneously enhance the thermodynamics,kinetics,and cycling stability of hydrogen storage materials.The introduction of supporting scaffolds usually causes a reduction in the total hydrogen storage capacity due to“dead weight.”Here,we synthesize an optimized N-doped porous carbon(rN-pC)without heavy metal as supporting scaffold to confine Mg/MgH_(2) nanoparticles(Mg/MgH_(2)@rN-pC).rN-pC with 60 wt%loading capacity of Mg(denoted as 60 Mg@rN-pC)can adsorb and desorb 0.62 wt%H_(2) on the rN-pC scaffold.The nanoconfined MgH_(2) can be chemically dehydrided at 175℃,providing~3.59 wt%H_(2) with fast kinetics(fully dehydrogenated at 300℃ within 15 min).This study presents the first realization of nanoconfined Mg-based system with adsorption-active scaffolds.Besides,the nanoconfined MgH_(2) formation enthalpy is reduced to~68 kJ mol^(−1) H_(2) from~75 kJ mol^(−1) H_(2) for pure MgH_(2).The composite can be also compressed to nanostructured pellets,with volumetric H_(2) density reaching 33.4 g L^(−1) after 500 MPa compression pressure,which surpasses the 24 g L^(−1) volumetric capacity of 350 bar compressed H_(2).Our approach can be implemented to the design of hybrid H_(2) storage materials with enhanced capacity and desorption rate.
基金The Key Research andDevelopment Project of Xinjiang Uygur Autonomous Region,with the grant number 2024B04025The General Programof Natural Science Foundation of Xinjiang Uygur Autonomous Region,with the grant number 2022D01C366.
文摘The integration of wind power and natural gas for hydrogen production forms a Green and Blue Hydrogen Integrated Energy System(GBH-IES),which is a promising cogeneration approach characterized by multienergy complementarity,flexible dispatch,and efficient utilization.This system can meet the demands for electricity,heat,and hydrogen while demonstrating significant performance in energy supply,energy conversion,economy,and environment(4E).To evaluate the GBH-IES system effectively,a comprehensive performance evaluation index system was constructed from the 4E dimensions.The fuzzy DEMATEL method was used to quantify the causal relationships between indicators,establishing a scientific input-output assessment system.The DEA model was then employed for preliminary performance evaluation of the hydrogen storage system,followed by the entropy weight TOPSIS method to enhance the accuracy and reliability of the assessment results.The study also conducted a comprehensive benefit evaluation and sensitivity analysis for different cases involving blue hydrogen,green hydrogen,and their synergistic effects under varying carbon emission factors(CEFs)and hydrogen blending ratios(HBRs).The results indicate that combining green and blue hydrogen can achieve higher comprehensive benefits for the hydrogen storage system,providing valuable insights for hydrogen storage development and demonstrating the effectiveness of themulti-criteria decision-making methods used.
基金supported by the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.24KJA150003)the Xuzhou Key Research and Development Program(Social Development)(No.KC23298)+1 种基金the National Natural Science Foundation of China(No.22271122)Basic Research Program of Jiangsu(No.BK20253049).
文摘To simultaneously improve the critical factors in photocatalytic H_(2)production,the population of active photogenerated electrons,the adsorption and activation of H_(2)O molecules,and the surface dehydrogenation efficiency,we propose a synergistic strategy for TiO_(2)modification by combining transition metal(TM)doping and N-doped carbon(N-C)coating.The targeted Cr-TiO_(2)@N-C heterojunction exhibits dramatically enhanced H_(2)production under blue light irradiation,contrasting sharply with a negligible production by pristine TiO_(2).Comprehensive structural characterization and theoretical calculations confirm the uniform substitution of Cr into the TiO_(2)lattice,promoting the formation of adjacent oxygen vacancies(VO).The synergistic effect of Cr doping and VO extends the light absorption range into the visible region.The coated N-C layer facilitates the efficient separation of photogenerated charge carriers,boosting the population of active electrons.Critically,the combined action of VO and N-C layer enhances the adsorption and activation of H_(2)O molecules while effectively improving the subsequent surface dehydrogenation efficiency.Significantly,this strategy demonstrates broad universality:Analogous TM-TiO_(2)@N-C heterojunctions(TM=Mn,Co,Ni,Cu,and Zn)synthesized via the same approach all show substantially improved H_(2)production performance over pristine TiO_(2).
基金the support from the National Natural Science Foundation of China(Nos.22208376,UA22A20429)the Qingdao New Energy Shandong Laboratory Open Project(QNESL OP 202303)+3 种基金Shandong Provincial Natural Science Foundation(Nos.ZR2024QB175,ZR2023LFG005)Fundamental Research Funds for the Central Universities(No.25CX07002A)National Natural Science Foundation of China(Z202401390008)The Hunan Provincial Natural Science Foundation(2025JJ60301)。
文摘3D printing,as a versatile additive manufacturing technique,offers high design flexibility,rapid prototyping,minimal material waste,and the capability to fabricate complex,customized geometries.These attributes make it particularly well-suited for low-temperature hydrogen electrochemical conversion devices—specifically,proton exchange membrane fuel cells,proton exchange membrane electrolyzer cells,anion exchange membrane electrolyzer cells,and alkaline electrolyzers—which demand finely structured components such as catalyst layers,gas diffusion layers,electrodes,porous transport layers,and bipolar plates.This review provides a focused and critical summary of the current progress in applying 3D printing technologies to these key components.It begins with a concise introduction to the principles and classifications of mainstream 3D printing methods relevant to the hydrogen energy sector and proceeds to analyze their specific applications and performance impacts across different device architectures.Finally,the review identifies existing technical challenges and outlines future research directions to accelerate the integration of 3D printing in nextgeneration low-temperature hydrogen energy systems.
基金the National Nature Science Foundation of China for Excellent Young Scientists Fund(32222058)Fundamental Research Foundation of CAF(CAFYBB2022QB001).
文摘Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.
基金financially supported by the National Key R&D Program of China(No.2023YFB3810800)the National Natural Science Foundation of China(Nos.22579008,22502012,22301013,and 22272003)+3 种基金Key Project of the National Natural Science Foundation of China(No.21936001)R&D Program of Beijing Municipal Education Commission(No.KZ20231000506)Beijing Outstanding Young Scientists Program(No.BJJWZYJH01201910005017)the Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(No.11000024T000003219982).
文摘The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges remain in achieving broad visiblelight absorption and suppressing charge recombination.In this work,we developed a series of photocatalysts through in situ embedding of red-emissive CDs(R-CDs)into g-C_(3)N_(4)(RCN)with precisely controlled loading amounts.Systematic characterization revealed that the R-CDs incorporation simultaneously addresses two fundamental limitations:(1)extending the light absorption edge to 800 nm,and(2)acting as an electron acceptor,facilitating charge separation.The optimized RCN composite demonstrates exceptional H_(2)evolution activity(1.87 mmol·g^(-1)·h^(-1),wavelength(λ)≥420 nm),representing a 3.3-fold enhancement over pristine g-C_(3)N_(4).Remarkably,the apparent quantum efficiency(AQE)reaches 9.1% at 420 nm,while maintaining measurable activity beyond 475 nm,where unmodified g-C_(3)N_(4)shows negligible response.This study provides fundamental insights into band structure engineering and charge carrier management through rational design of CDs-modified semiconductor heterostructures.
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
基金Supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions under Grant No.014000319/2018-00391.
文摘Pre-chamber ignition technology can address the issue of uneven in-cylinder mixture combustion in large-bore marine engines.The impact of various pre-chamber structures on the formation of the mixture and jet flames within the pre-chamber is explored.This study performed numerical simulations on a large-bore marine ammonia/hydrogen pre-chamber engine prototype,considering pre-chamber volume,throat diameter,the distance between the hydrogen injector and the spark plug,and the hydrogen injector angle.Compared with the original engine,when the pre-chamber volume is 73.4 ml,the throat diameter is 14 mm,the distance ratio is 0.92,and the hydrogen injector angle is 80°.Moreover,the peak pressure in the pre-chamber increased by 23.1%,and that in the main chamber increased by 46.3%.The results indicate that the performance of the original engine is greatly enhanced by altering its fuel and pre-chamber structure.
基金supported by the National Natural Science Foundation of China (Grant Nos.12074213 and 11574108)the Major Basic Program of Natural Science Foundation of Shandong Province (Grant No.ZR2021ZD01)the Natural Science Foundation of Shandong Province (Grant No.ZR2023MA082)。
文摘In recent years,the research on superconductivity in one-dimensional(1D)materials has been attracting increasing attention due to its potential applications in low-dimensional nanodevices.However,the critical temperature(T_(c))of 1D superconductors is low.In this work,we theoretically investigate the possible high T_(c) superconductivity of(5,5)carbon nanotube(CNT).The pristine(5,5)CNT is a Dirac semimetal and can be modulated into a semiconductor by full hydrogenation.Interestingly,by further hole doping,it can be regulated into a metallic state with the sp3-hybridized𝜎electrons metalized,and a giant Kohn anomaly appears in the optical phonons.The two factors together enhance the electron–phonon coupling,and lead to high-T_(c) superconductivity.When the hole doping concentration of hydrogenated-(5,5)CNT is 2.5 hole/cell,the calculated T_(c) is 82.3 K,exceeding the boiling point of liquid nitrogen.Therefore,the predicted hole-doped hydrogenated-(5,5)CNT provides a new platform for 1D high-T_(c) superconductivity and may have potential applications in 1D nanodevices.
基金financially supported by the program of the National Natural Science Foundation of Shandong Province(No.ZR2023ZD23)the Shandong Province Key Research and Development Plan(No.2023CXGC010607).
文摘Atomically ordered precious intermetallic nanoparticles have garnered significant attention for diverse applications due to their well-defined surface atomic arrangements and exceptional electronic and geometric properties.However,synthesizing non-precious ordered intermetallics that exhibit high stability under operating conditions remains a formidable challenge,primarily owing to their strong oxyphilicity,highly negative reduction potentials,and low corrosion resistance.In this work,we report a facile yet versatile seed-mediated solid-phase approach for fabricating uniform Ni_(3)Ga_(1) intermetallic nanocubes(NCs)fully encapsulated within N-doped carbon layers(denoted as Ni_(3)Ga_(1)@NC-800).Extensive characterization confirms the formation of a unique core-shell architecture,with atomic-resolution structural analysis and X-ray absorption fine structure measurements unequivocally verifying the atomically ordered Ni_(3)Ga_(1) intermetallic phase.The Ni_(3)Ga_(1)@NC-800 catalyst demonstrates exceptional performance in the 1,4-hydrogenation of α,β-unsaturated carbonyl compounds,exhibiting both remarkable activity and exclusive selectivity while maintaining high stability over multiple reaction cycles without observable performance decay.Combined experimental and theoretical calculations reveal that the strong interatomic p-d orbital hybridization facilitates electron transfer from Ga to Ni atoms,resulting in electron localization on ordered Ni atoms.This electronic configuration positively influences H_(2)activation and optimizes substrate adsorption strength,thereby substantially improving catalytic efficiency.Furthermore,this synthetic strategy proves generalizable,successfully extending to the synthesis of other non-precious ordered Ni_(1)Sn_(1) and Ni_(2)In_(3) intermetallics confined within N-doped carbon matrices.
基金financially supported by the National Natural Science Foundation of China(Nos.22272080(M.Y.)and 52272218(H.X.))the Fundamental Research Funds for the Central Universities(No.2242024k30047).
文摘The vip-host chemistry in polymer electrolytes plays a crucial role for all-solid-state Li metal batteries,where the stable operation of such batteries heavily relies on high ion conductivity,strong mechanical properties,and stable interfaces of the electrolyte.While traditional ceramic fillers can boost ion conductivity,they fail to improve interfacial stability.In this study,we introduce intermolecular hydrogen bonding into a polyethylene oxide(PEO)-based polymer electrolyte through the incorporation of metal organic framework(MOF)and lithium nitrate additives.The hydrogen on the PEO chain is found to be tightly interacted with the oxygen nodes of UiO-66 MOF and nitrate anions,creating a cross-linked framework that reduces the crystallinity of the PEO and enhances the integrity of composite.This interaction induces a beneficial Li3N and LiF-rich solid electrolyte interphase,ensuring 2000 h of stable lithium metal operation without short-circuits.The strong polysulfide adsorption enables compatibility with high-capacity sulfur cathodes,resulting in solidstate Li-S batteries that can achieve a high capacity of 913.8 mAh·g^(-1)and exhibit stable cycling performance.This work demonstrates the deep understanding of vip-host chemistry in polymer electrolytes and their potential in developing energy-dense solid-state Li metal batteries.
文摘A hydrogen energy storage system(HESS)is one of the many risingmodern green innovations,using excess energy to generate hydrogen and storing it for various purposes.With that,there have been many discussions about commercializing HESS and improving it further.However,the design and sizing process can be overwhelming to comprehend with various sources to examine,and understanding optimal design methodologies is crucial to optimize a HESS design.With that,this review aims to collect and analyse a wide range of HESS studies to summarise recent studies.Two different collections of studies are studied,one was sourced by the main author for preliminary readings,and another was obtained via VOSViewer.The findings from the Web of Science platform were also examined for amore comprehensive understanding.Major findings include the People’sRepublic of China has been active in HESS research,as most works and active organizations originate from this country.HESS has been mainly researched to support power generation and balance load demands,with financial analysis being the common scope of analysis.MATLAB is a common tool used for HESS design,modelling,and optimization as it can handle complex calculations.Artificial neural network(ANN)has the potential to be used to model the HESS,but additional review is required as a formof future work.From a commercialization perspective,pressurized hydrogen tanks are ideal for hydrogen storage in a HESS,but other methods can be considered after additional research and development.From this review,it can be implied that modelling works will be the way forward for HESS research,but extensive collaborations and additional review are needed.Overall,this review summarized various takeaways that future research works on HESS can use.
