Electronic structure calculations using the tighting-binding linear muffin-tin orbital (TB-LMTO) method have been performed for Co3Ti and its hydride CO3Ti. The computed values of lattice constants and bulk moduli agr...Electronic structure calculations using the tighting-binding linear muffin-tin orbital (TB-LMTO) method have been performed for Co3Ti and its hydride CO3Ti. The computed values of lattice constants and bulk moduli agree with the experiment values. The theoritical excess enerpy and lattice staid due to hydrogen absorption consequently obtained hem the ab initio results indicate that H has the tendency to stay in Co3Ti and the ionicities of Co atomic spheres due to hydmpen absorption change from the canons to the ations. On the other hand, the changes of band structures due to hydrogenation are found to be remarkable.展开更多
By use of the self-consistent method of linear muffin-tin orbitals with the atomic sphere approximation on the basis of density functional theory, the total energies and the electron-ic sTructures ofNi, Al, and their ...By use of the self-consistent method of linear muffin-tin orbitals with the atomic sphere approximation on the basis of density functional theory, the total energies and the electron-ic sTructures ofNi, Al, and their hydrides NiH. A1H and Ni3AlH are calculated. The theoretical excess energies and the lattice strains due to hydrogen absorption consequently obtained from the ah initio results indicate that Ni is a better hydrogen absorber than Al, an. the absorptivity of Ni3Al dramatically decreases owing to the repulsion between Al and H On the other hand, the changes of band structures due to hydrogenation are found to be remparkable except that tor Al. and they are shown to be the qualitative manifestation of existing conclusions from photoemission experiments.展开更多
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an...The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.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
S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly unders...The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates.In this study,we prepared two Zn-Al spinel oxide catalysts via coprecipitation(ZnAl-C)and hydrothermal(ZnAl-H)methods,and conducted a comparative investigation in the CO_(2)hydrogenation reaction.Surprisingly,under similar conditions,ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H.Comprehensive characterizations using X-ray diffraction(XRD),Raman spectroscopy and electron paramagnetic resonance(EPR)unveiled that ZnAl-C catalyst had abundant ZnO species on its surface,and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies,which are crucial for CO_(2)adsorption and activation.Additionally,state-of-the-art solid-state nuclear magnetic resonance(NMR)techniques,including ex-situ and in-situ NMR analyses,confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species,which was readily hydrogenated to methanol and DME.These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO_(2)-to-methanol hydrogenation reaction,which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst.These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.展开更多
Green hydrogen is the most promising option and a two in one remedy that resolve the problem of both energy crisis and environmental pollution.Wide band gap semiconductors(WBG)(E_(g)>2 eV)are the most prominent and...Green hydrogen is the most promising option and a two in one remedy that resolve the problem of both energy crisis and environmental pollution.Wide band gap semiconductors(WBG)(E_(g)>2 eV)are the most prominent and leading catalytic materials in both electro and photocatalytic water splitting(WSR);two sustainable methods of green hydrogen production.WBGs guarantee long life time of photo charge carriers and thereby surface availability of electrons and holes.Therefore,WBG(with appropriate VB-CB potential)along with small band gap materials or sensitizers can yield extraordinary photocatalytic system for hydrogen production under solar light.The factors such as,free energy of hydrogen adsorption(ΔGH^(*))close to zero,high electron mobility,great thermal as well as electro chemical stability and high tunability make WBG an interesting and excellent catalyst in electrolysis too.Taking into account the current relevance and future scope,the present review article comprehends different dimensions of WBG materials as an electro/photo catalyst for hydrogen evolution reaction.Herein WBG semiconductors are presented under various classes;viz.II-VI,III-V,III-VI,lanthanide oxides,transition metal based systems,carbonaceous materials and other systems such as SiC and MXenes.Catalytic properties of WBGs favorable for hydrogen production are then reviewed.A detailed analysis on relationship between band structure and activity(electro,photo and photo-electrochemical WSR)is performed.The challenges involved in these reactions as well as the direction of advancement in WBG based catalysis are also debated.By virtue of this article authors aims to guideline and promote the development of new WBG based electro/photocatalyst for HER and other applications.展开更多
It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for elec...It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for electrocatalytic HMF oxidative reaction(e-HMFOR)have been facing low Faradaic efficiency(FE)and high water splitting voltage.Herein,we propose a strategy of the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction by constructing a Co-Ni paired site,where the Co site is in charge of adsorbing for HMF while the electrons are transferred to the Ni site,thus giving the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction superior electrocata lytic performances for e-HMFOR and water splitting.By optimizing conditions,the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction has high conversion of 99.7%,high selectivity of 99.9%,and high FE of 98.4%at 1.3 V,as well as low cell voltage of 1.31 V at 10 mA cm^(-2)in 1 M KOH+0.1 M HMF.This study offers a potential insight for e-HMFOR to high value-added FDCA coupling water splitting to produce H_(2)in an economical manner.展开更多
Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitig...Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitigate CH_(4)production and improve digestibility in cattle,we incubated substrate with rumen inoculum from yak(YRI)and cattle(CRI)in vitro in five ratios(YRI:CRI):(1)0:100(control),(2)25:75,(3)50:50,(4)75:25 and(5)100:0 for 72 h.The YRI:CRI ratios of 50:50,75:25 and 100:0 produced less total gas and CH_(4)and accumulated less hydrogen(H_(2))than0:100(control)at most time points.From 12 h onwards,there was a linear decrease(P<0.05)in carbon dioxide(CO_(2))production with increasing YRI:CRI ratio.At 72 h,the ratios of 50:50 and 75:25 had higher dry matter(+7.71%and+4.11%,respectively),as well as higher acid detergent fiber digestibility(+15.5%and+7.61%,respectively),when compared to the 0:100 ratio(P<0.05).Increasing the proportion of YRI generally increased total VFA concentrations,and,concomitantly,decreased the proportion of metabolic hydrogen([2H])incorporated into CH_(4),and decreased the recovery of[2H].The lower[2H]recovery indicates unknown[2H]sinks in the culture.Estimated Gibbs free energy changes(ΔG)for reductive acetogenesis were negative,indicating the thermodynamic feasibility of this process.It would be beneficial to identify:1)the alternative[2H]sinks,which could help mitigate CH_(4)emission,and 2)core microbes involved in fiber digestion.This experiment supported lower CH_(4)emission and greater nutrient digestibility of yaks compared to cattle.Multi-omics combined with microbial culture technologies developed in recent years could help to better understand fermentation differences among species.展开更多
Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction...Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction loss in EMW-absorbing materials and charge transfer in HB remains to be fully understood.In this study,we developed a series of deep eutectic gels to fine-tune the quantity of HB by adjusting the molar ratio of choline chloride(ChCl)and ethylene glycol(EG).Owing to the unique properties of deep eutectic gels,the effects of magnetic loss and polarization loss on EMW attenuation can be disregarded.Our results indicate that the quantity of HB initially increases and then decreases with the introduction of EG,with HB-induced conductive loss following similar pat-terns.At a ChCl and EG molar ratio of 2.4,the gel labeled G22-CE2.4 exhibited the best EMW absorption performance,characterized by an effective absorption bandwidth of 8.50 GHz and a thickness of 2.54 mm.This superior performance is attributed to the synergistic ef-fects of excellent conductive loss and impedance matching generated by the optimal number of HB.This work elucidates the role of HB in dielectric loss for the first time and provides valuable insights into the optimal design of supramolecular polymer absorbers.展开更多
Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corros...Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful chlorine.In contrast to the oxygen evolution reaction (OER)and chlorin ion oxidation reaction (ClOR),glycerol oxidation reaction (GOR) is more thermodynamically and kinetically favorable alternative.Herein,a Ru doping cobalt phosphide (Ru-CoP_(2)) is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR,for the concurrent productions of hydrogen and value-added formate.The in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP_(2)to Ru-CoOOH,accounting for the superior GOR performance.Further coupling GOR with hydrogen evolution was realized by employing Ru-CoP_(2)as both anode and cathode,requiring only a low voltage of 1.43 V at 100 mA cm^(-2),which was 250 m V lower than that in alkaline seawater.This work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.展开更多
[Objective]As hydrogen energy has gained new momentum recently,analyzing the economic and social impacts of developing a hydrogen energy sector can inform further policy formation and investment decision making in thi...[Objective]As hydrogen energy has gained new momentum recently,analyzing the economic and social impacts of developing a hydrogen energy sector can inform further policy formation and investment decision making in this regard.[Method]Considering the increasingly important role of East Asia Summit(EAS)region in both economic growth and green energy transition,this paper developed a demand-driven model for the hydrogen energy supply chains to comprehensively and quantitatively evaluate the economic and social impacts hydrogen energy development in the EAS region.[Result]This model provides estimates of the capital investment required,the number of new jobs created,the potential carbon emissions reduction,the subsidies needed in the early stages of development,and the impacts on key energy security indicators.[Conclusion]This study find that hydrogen energy development has a significant job creation effect,and that the total investment and the fiscal burden appear to be manageable for countries in the EAS region.In addition to substantial carbon emissions reduction,positive social impacts also include general improvements in energy security indicators.展开更多
Hydrogen partitioning between liquid iron alloys and silicate melts governs its distribution and cycling in Earth’s deep interior.Existing models based on simplified Fe-H systems predict strong hydrogen sequestration...Hydrogen partitioning between liquid iron alloys and silicate melts governs its distribution and cycling in Earth’s deep interior.Existing models based on simplified Fe-H systems predict strong hydrogen sequestration into the core.However,these models do not account for the modulating effects of major light elements such as oxygen and silicon in the core during Earth’s primordial differentiation.In this study,we use first-principles molecular dynamics simulations,augmented by machine learning techniques,to quantify hydrogen chemical potentials in quaternary Fe-O-Si-H systems under early core-mantle boundary conditions(135 GPa,5000 K).Our results demonstrate that the presence of 5.2 wt%oxygen and 4.8 wt%silicon reduces the siderophile affinity of hydrogen by 35%,decreasing its alloy-silicate partition coefficient from 18.2(in the case of Fe-H)to 11.8(in the case of Fe-O-Si-H).These findings suggest that previous estimates of the core hydrogen content derived from binary system models require downward revision.Our study underscores the critical role of multicomponent interactions in core formation models and provides first-principles-derived constraints to reconcile Earth’s present-day hydrogen reservoirs with its accretionary history.展开更多
Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a b...Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a binary nanophotocatalyst fabricated by blending two polymers,PS-PEG5(PS)and PBT-PEG5(PBT),with matched absorption and emission spectra,enabling a Forster resonance energy transfer(FRET)process for enhanced photocatalysis.These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation(FNP)technique with precious kinetic control over binary nanoparticle formation.The resulting nanoparticles exhibit an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g^(-1) h^(-1),2.5 times higher than that single component nanoparticles.Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles,which prolongs the excited-state lifetime and extends the namely“effective exciton diffusion length”.Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.展开更多
Hydrogen energy has gained widespread recognition for its environmentally friendly nature,high energy density and abundant resources,making it a promising energy carrier for a sustainable and clean energy society.Howe...Hydrogen energy has gained widespread recognition for its environmentally friendly nature,high energy density and abundant resources,making it a promising energy carrier for a sustainable and clean energy society.However,safe and efficient hydrogen storage remains a significant challenge due to its inherent leakiness and flammability.To overcome these challenges,alloys featuring body-centered cubic(BCC)structures have emerged as compelling candidates for hydrogen storage,owing to their exceptional capacity to achieve high-density hydrogen storage up to 3.8 wt%at ambient temperatures.Nonetheless,their practical application faces limited dehydriding capacity,complex activation processes,high costs and poor cyclic stability.Various modification strategies have been explored to overcome these limitations,including lattice regulation,element substitution,rare earth doping and heat treatment.This progress report presents an overview of the previous advancements to enhance five crucial aspects(high-V,medium-V,low-V,V-free and high-entropy alloys)in composition design and hydrogen storage properties within BCC-structured alloys.Subsequently,an in-depth analysis is conducted to examine the relationship between crystal structures and hydrogen storage properties specific to BCC-structured alloys,covering aspects such as composition,crystal structure,hydrogen storage capacity,enthalpy and entropy.Furthermore,this review explores current challenges in this field and outlines directions for future research.These insights provide valuable guidance for the design of innovative and cost-effective hydrogen storage alloys.展开更多
Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promisi...Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.展开更多
Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to thei...Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.展开更多
CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based c...CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.展开更多
Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it ...Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it is necessary for the quality of hydrogen to adhere to the standards set by ISO 14687:2019,which sets maximum limits for 14 impurities in hydrogen,aiming to prevent any degradation of fuel cell performance.Ammonia(NH_(3))is a prominent pollutant in fuel cells,and accurate measurements of its concentration are crucial for hydrogen fuel cell quantity.In this study,a novel detection platform was developed for determining NH_(3)in real hydrogen samples.The online analysis platform integrates a self-developed online dilution module with a Fourier transform infrared spectrometer(ODM-FTIR).The ODM-FTIR can be operated fully automatically with remote operation.Under the optimum conditions,this method achieved a wide linear range between(50∼1000)nmol/mol.The limit of detection(LOD)was as low as 2 nmol/mol with a relative standard deviation(RSD,n=7)of 3.6%at a content of 50 nmol/mol.To ensure that the quality of the hydrogen products meets the requirement of proton exchange membrane fuel cell vehicles(PEMFCV),the developed ODM-FTIR system was applied to monitor the NH_(3)content in Chengdu Hydrogen Energy Co.,Ltd.for 21 days during Chengdu 2021 FISU World University Games.The proposed method retains several unique advantages,including a low detection limit,excellent repeatability,high accuracy,high speed,good stability,and calibration flexibility.It is an effective analytical method for accurately quantifying NH_(3)in hydrogen,especially suitable for online analysis.It also provides a new idea for the analysis of other impurity components in hydrogen.展开更多
文摘Electronic structure calculations using the tighting-binding linear muffin-tin orbital (TB-LMTO) method have been performed for Co3Ti and its hydride CO3Ti. The computed values of lattice constants and bulk moduli agree with the experiment values. The theoritical excess enerpy and lattice staid due to hydrogen absorption consequently obtained hem the ab initio results indicate that H has the tendency to stay in Co3Ti and the ionicities of Co atomic spheres due to hydmpen absorption change from the canons to the ations. On the other hand, the changes of band structures due to hydrogenation are found to be remarkable.
文摘By use of the self-consistent method of linear muffin-tin orbitals with the atomic sphere approximation on the basis of density functional theory, the total energies and the electron-ic sTructures ofNi, Al, and their hydrides NiH. A1H and Ni3AlH are calculated. The theoretical excess energies and the lattice strains due to hydrogen absorption consequently obtained from the ah initio results indicate that Ni is a better hydrogen absorber than Al, an. the absorptivity of Ni3Al dramatically decreases owing to the repulsion between Al and H On the other hand, the changes of band structures due to hydrogenation are found to be remparkable except that tor Al. and they are shown to be the qualitative manifestation of existing conclusions from photoemission experiments.
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
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.
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.
基金financially National Key R&D Program of China(No.2022YFA1504800)National Natural Science Foundation of China(Grant No.22325405,22372160,22321002)+1 种基金Liaoning Revitalization Talents Program(XLYC1807207)DICP I202104。
文摘The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)hydrogenation.However,the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates.In this study,we prepared two Zn-Al spinel oxide catalysts via coprecipitation(ZnAl-C)and hydrothermal(ZnAl-H)methods,and conducted a comparative investigation in the CO_(2)hydrogenation reaction.Surprisingly,under similar conditions,ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H.Comprehensive characterizations using X-ray diffraction(XRD),Raman spectroscopy and electron paramagnetic resonance(EPR)unveiled that ZnAl-C catalyst had abundant ZnO species on its surface,and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies,which are crucial for CO_(2)adsorption and activation.Additionally,state-of-the-art solid-state nuclear magnetic resonance(NMR)techniques,including ex-situ and in-situ NMR analyses,confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species,which was readily hydrogenated to methanol and DME.These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO_(2)-to-methanol hydrogenation reaction,which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst.These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.
文摘Green hydrogen is the most promising option and a two in one remedy that resolve the problem of both energy crisis and environmental pollution.Wide band gap semiconductors(WBG)(E_(g)>2 eV)are the most prominent and leading catalytic materials in both electro and photocatalytic water splitting(WSR);two sustainable methods of green hydrogen production.WBGs guarantee long life time of photo charge carriers and thereby surface availability of electrons and holes.Therefore,WBG(with appropriate VB-CB potential)along with small band gap materials or sensitizers can yield extraordinary photocatalytic system for hydrogen production under solar light.The factors such as,free energy of hydrogen adsorption(ΔGH^(*))close to zero,high electron mobility,great thermal as well as electro chemical stability and high tunability make WBG an interesting and excellent catalyst in electrolysis too.Taking into account the current relevance and future scope,the present review article comprehends different dimensions of WBG materials as an electro/photo catalyst for hydrogen evolution reaction.Herein WBG semiconductors are presented under various classes;viz.II-VI,III-V,III-VI,lanthanide oxides,transition metal based systems,carbonaceous materials and other systems such as SiC and MXenes.Catalytic properties of WBGs favorable for hydrogen production are then reviewed.A detailed analysis on relationship between band structure and activity(electro,photo and photo-electrochemical WSR)is performed.The challenges involved in these reactions as well as the direction of advancement in WBG based catalysis are also debated.By virtue of this article authors aims to guideline and promote the development of new WBG based electro/photocatalyst for HER and other applications.
基金supported by the National Natural Science Foundation of China(22302019)the Changzhou Sci&Tech Program(CJ20220214).
文摘It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for electrocatalytic HMF oxidative reaction(e-HMFOR)have been facing low Faradaic efficiency(FE)and high water splitting voltage.Herein,we propose a strategy of the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction by constructing a Co-Ni paired site,where the Co site is in charge of adsorbing for HMF while the electrons are transferred to the Ni site,thus giving the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction superior electrocata lytic performances for e-HMFOR and water splitting.By optimizing conditions,the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction has high conversion of 99.7%,high selectivity of 99.9%,and high FE of 98.4%at 1.3 V,as well as low cell voltage of 1.31 V at 10 mA cm^(-2)in 1 M KOH+0.1 M HMF.This study offers a potential insight for e-HMFOR to high value-added FDCA coupling water splitting to produce H_(2)in an economical manner.
基金supported by the National Natural Science Foundation of China(32072757 and U21A20250)。
文摘Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitigate CH_(4)production and improve digestibility in cattle,we incubated substrate with rumen inoculum from yak(YRI)and cattle(CRI)in vitro in five ratios(YRI:CRI):(1)0:100(control),(2)25:75,(3)50:50,(4)75:25 and(5)100:0 for 72 h.The YRI:CRI ratios of 50:50,75:25 and 100:0 produced less total gas and CH_(4)and accumulated less hydrogen(H_(2))than0:100(control)at most time points.From 12 h onwards,there was a linear decrease(P<0.05)in carbon dioxide(CO_(2))production with increasing YRI:CRI ratio.At 72 h,the ratios of 50:50 and 75:25 had higher dry matter(+7.71%and+4.11%,respectively),as well as higher acid detergent fiber digestibility(+15.5%and+7.61%,respectively),when compared to the 0:100 ratio(P<0.05).Increasing the proportion of YRI generally increased total VFA concentrations,and,concomitantly,decreased the proportion of metabolic hydrogen([2H])incorporated into CH_(4),and decreased the recovery of[2H].The lower[2H]recovery indicates unknown[2H]sinks in the culture.Estimated Gibbs free energy changes(ΔG)for reductive acetogenesis were negative,indicating the thermodynamic feasibility of this process.It would be beneficial to identify:1)the alternative[2H]sinks,which could help mitigate CH_(4)emission,and 2)core microbes involved in fiber digestion.This experiment supported lower CH_(4)emission and greater nutrient digestibility of yaks compared to cattle.Multi-omics combined with microbial culture technologies developed in recent years could help to better understand fermentation differences among species.
基金supported by the National Nat-ural Science Foundation of China(Nos.51872238,52074227,and 21806129)the Fundamental Research Funds for the Central Universities,China(Nos.3102018zy045 and 3102019AX11)+2 种基金the Guangdong Basic and Applied Basic Research Foundation,China(No.2024A1515010298)the Natural Science Basic Research Plan in Shaanxi Province of China(Nos.2017JQ5116 and 2020JM-118)the Key Laboratory of Icing and Anti/De-icing of CARDC(No.IADL20220401).
文摘Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction loss in EMW-absorbing materials and charge transfer in HB remains to be fully understood.In this study,we developed a series of deep eutectic gels to fine-tune the quantity of HB by adjusting the molar ratio of choline chloride(ChCl)and ethylene glycol(EG).Owing to the unique properties of deep eutectic gels,the effects of magnetic loss and polarization loss on EMW attenuation can be disregarded.Our results indicate that the quantity of HB initially increases and then decreases with the introduction of EG,with HB-induced conductive loss following similar pat-terns.At a ChCl and EG molar ratio of 2.4,the gel labeled G22-CE2.4 exhibited the best EMW absorption performance,characterized by an effective absorption bandwidth of 8.50 GHz and a thickness of 2.54 mm.This superior performance is attributed to the synergistic ef-fects of excellent conductive loss and impedance matching generated by the optimal number of HB.This work elucidates the role of HB in dielectric loss for the first time and provides valuable insights into the optimal design of supramolecular polymer absorbers.
基金National Natural Science Foundation of China (Nos. 42276035, 22309030)Guangdong Basic and Applied Basic Research Foundation (Nos. 2023A1515012589,2020A1515110473)Key Plat Form Programs and Technology Innovation Team Project of Guangdong Provincial Department of Education (Nos. 2019GCZX002, 2020KCXTD011)。
文摘Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater.However,the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful chlorine.In contrast to the oxygen evolution reaction (OER)and chlorin ion oxidation reaction (ClOR),glycerol oxidation reaction (GOR) is more thermodynamically and kinetically favorable alternative.Herein,a Ru doping cobalt phosphide (Ru-CoP_(2)) is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR,for the concurrent productions of hydrogen and value-added formate.The in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP_(2)to Ru-CoOOH,accounting for the superior GOR performance.Further coupling GOR with hydrogen evolution was realized by employing Ru-CoP_(2)as both anode and cathode,requiring only a low voltage of 1.43 V at 100 mA cm^(-2),which was 250 m V lower than that in alkaline seawater.This work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.
文摘[Objective]As hydrogen energy has gained new momentum recently,analyzing the economic and social impacts of developing a hydrogen energy sector can inform further policy formation and investment decision making in this regard.[Method]Considering the increasingly important role of East Asia Summit(EAS)region in both economic growth and green energy transition,this paper developed a demand-driven model for the hydrogen energy supply chains to comprehensively and quantitatively evaluate the economic and social impacts hydrogen energy development in the EAS region.[Result]This model provides estimates of the capital investment required,the number of new jobs created,the potential carbon emissions reduction,the subsidies needed in the early stages of development,and the impacts on key energy security indicators.[Conclusion]This study find that hydrogen energy development has a significant job creation effect,and that the total investment and the fiscal burden appear to be manageable for countries in the EAS region.In addition to substantial carbon emissions reduction,positive social impacts also include general improvements in energy security indicators.
基金supported by the National Key R&D Program of China(Grant No.2022YFF0503203)National Natural Science Foundation of China(NSFC)projects(Grant Nos.42441826 and 42173041)+1 种基金the Key Research Program of the Institute of Geology and Geophysics,Chinese Academy of Sciences(Grant No.IGGCAS-202204)the computational facilities of the Computer Simulation Laboratory at IGGCAS and the Beijing Super Cloud Computing Center(BSCC).
文摘Hydrogen partitioning between liquid iron alloys and silicate melts governs its distribution and cycling in Earth’s deep interior.Existing models based on simplified Fe-H systems predict strong hydrogen sequestration into the core.However,these models do not account for the modulating effects of major light elements such as oxygen and silicon in the core during Earth’s primordial differentiation.In this study,we use first-principles molecular dynamics simulations,augmented by machine learning techniques,to quantify hydrogen chemical potentials in quaternary Fe-O-Si-H systems under early core-mantle boundary conditions(135 GPa,5000 K).Our results demonstrate that the presence of 5.2 wt%oxygen and 4.8 wt%silicon reduces the siderophile affinity of hydrogen by 35%,decreasing its alloy-silicate partition coefficient from 18.2(in the case of Fe-H)to 11.8(in the case of Fe-O-Si-H).These findings suggest that previous estimates of the core hydrogen content derived from binary system models require downward revision.Our study underscores the critical role of multicomponent interactions in core formation models and provides first-principles-derived constraints to reconcile Earth’s present-day hydrogen reservoirs with its accretionary history.
基金supported by National Natural Science Foundation of China(NSFC,22338006,92356301,9235630033 and 22375062)Shanghai Municipal Science and Technology Major Project(21JC1401700)+4 种基金Shanghai Pilot Program for Basic Research(22TQ1400100-10)Fundamental Research Funds for the Central UniversitiesShanghai Pujiang Program(22PJ1402400)“Chenguang Program”supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(22CGA32)the Young Elite Scientists Sponsorship Program by CAST(2023QNRC001).
文摘Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a binary nanophotocatalyst fabricated by blending two polymers,PS-PEG5(PS)and PBT-PEG5(PBT),with matched absorption and emission spectra,enabling a Forster resonance energy transfer(FRET)process for enhanced photocatalysis.These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation(FNP)technique with precious kinetic control over binary nanoparticle formation.The resulting nanoparticles exhibit an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g^(-1) h^(-1),2.5 times higher than that single component nanoparticles.Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles,which prolongs the excited-state lifetime and extends the namely“effective exciton diffusion length”.Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.
基金supported by the National Key R&D Program of China(No.2022YFB3504700)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA0400304)the Research Fund of Key Laboratory of Rare Earths,Chinese Academy of Sciences(No.E32PF00116).
文摘Hydrogen energy has gained widespread recognition for its environmentally friendly nature,high energy density and abundant resources,making it a promising energy carrier for a sustainable and clean energy society.However,safe and efficient hydrogen storage remains a significant challenge due to its inherent leakiness and flammability.To overcome these challenges,alloys featuring body-centered cubic(BCC)structures have emerged as compelling candidates for hydrogen storage,owing to their exceptional capacity to achieve high-density hydrogen storage up to 3.8 wt%at ambient temperatures.Nonetheless,their practical application faces limited dehydriding capacity,complex activation processes,high costs and poor cyclic stability.Various modification strategies have been explored to overcome these limitations,including lattice regulation,element substitution,rare earth doping and heat treatment.This progress report presents an overview of the previous advancements to enhance five crucial aspects(high-V,medium-V,low-V,V-free and high-entropy alloys)in composition design and hydrogen storage properties within BCC-structured alloys.Subsequently,an in-depth analysis is conducted to examine the relationship between crystal structures and hydrogen storage properties specific to BCC-structured alloys,covering aspects such as composition,crystal structure,hydrogen storage capacity,enthalpy and entropy.Furthermore,this review explores current challenges in this field and outlines directions for future research.These insights provide valuable guidance for the design of innovative and cost-effective hydrogen storage alloys.
基金National Key R&D Program of China,Grant/Award Number:2021YFA1500900Basic and Applied Basic Research Foundation of Guangdong Province-Regional Joint Fund Project,Grant/Award Number:2021B1515120024+9 种基金Science Funds of the Education Office of Jiangxi Province,Grant/Award Number:GJJ2201324Science Funds of Jiangxi Province,Grant/Award Numbers:20242BAB25168,20224BAB213018Doctoral Research Start-up Funds of JXSTNU,Grant/Award Number:2022BSQD05China Postdoctoral Science Foundation,Grant/Award Number:2023M741121National Natural Science Foundation of China,Grant/Award Number:22172047Provincial Natural Science Foundation of Hunan,Grant/Award Number:2021JJ30089Shenzhen Science and Technology Program,Grant/Award Number:JCYJ20210324122209025Changsha Municipal Natural Science Foundation,Grant/Award Number:kq2107008Hunan Province of Huxiang Talent project,Grant/Award Number:2023rc3118Natural Science Foundation of Hunan Province,Grant/Award Number:2022JJ10006.
文摘Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.
基金financial support by the National Natural Science Foundation of China(No.52102241)Doctor of Suzhou University Scientific Research Foundation(Nos.2022BSK019,2020BS015)+2 种基金the Primary Research and Development Program of Anhui Province(No.201904a05020087)the Natural Science Research Project in Universities of Anhui Province in China(Nos.2022AH051386,KJ2021A1114)the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking Qilu University of Technology。
文摘Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
文摘CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.
基金financial support by Sichuan Science and Technology,China(No.2023YFG0070).
文摘Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it is necessary for the quality of hydrogen to adhere to the standards set by ISO 14687:2019,which sets maximum limits for 14 impurities in hydrogen,aiming to prevent any degradation of fuel cell performance.Ammonia(NH_(3))is a prominent pollutant in fuel cells,and accurate measurements of its concentration are crucial for hydrogen fuel cell quantity.In this study,a novel detection platform was developed for determining NH_(3)in real hydrogen samples.The online analysis platform integrates a self-developed online dilution module with a Fourier transform infrared spectrometer(ODM-FTIR).The ODM-FTIR can be operated fully automatically with remote operation.Under the optimum conditions,this method achieved a wide linear range between(50∼1000)nmol/mol.The limit of detection(LOD)was as low as 2 nmol/mol with a relative standard deviation(RSD,n=7)of 3.6%at a content of 50 nmol/mol.To ensure that the quality of the hydrogen products meets the requirement of proton exchange membrane fuel cell vehicles(PEMFCV),the developed ODM-FTIR system was applied to monitor the NH_(3)content in Chengdu Hydrogen Energy Co.,Ltd.for 21 days during Chengdu 2021 FISU World University Games.The proposed method retains several unique advantages,including a low detection limit,excellent repeatability,high accuracy,high speed,good stability,and calibration flexibility.It is an effective analytical method for accurately quantifying NH_(3)in hydrogen,especially suitable for online analysis.It also provides a new idea for the analysis of other impurity components in hydrogen.
