Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy infl...Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy influence the competitiveness of economies,while the level of energy consumption impacts the standard of living for individuals.This paper aims to examine environmental challenges and steps for a sustainable transition towards a hydrogen economy,focusing on its potential as an alternative to fossil fuels and the importance of developing the hydrogen paradigm.The research methodology is based on a combination of qualitative and quantitative methods,including an analysis of global and regional trends in the energy transition,the impact of various forms of hydrogen production(green,blue,gray hydrogen)on greenhouse gas emissions,and a comparison of existing policies and strategies in different countries transitioning to a sustainable hydrogen economy.Research results show that green hydrogen,produced via electrolysis using renewable energy sources,holds the greatest potential for reducing greenhouse gas emissions,while gray and blue hydrogen can serve as transitional options.The development of the hydrogen paradigm,rooted in innovative technologies,renewable energy sources,and international cooperation,is crucial for decarbonization and the creation of a sustainable global economy,despite challenges such as high costs and the need for global coordination.The hydrogen paradigm is becoming a cornerstone of these efforts,laying the foundation for a long-term,sustainable global economy.Currently,over 180 hydrogen transport projects,60 distribution projects,80 storage projects,30 terminal and port projects,and more than 220 hydrogen production projects are under development worldwide.The global momentum of the hydrogen transition helps mitigate climate change and build a sustainable future.展开更多
Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using iso...Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source.The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of(S)-rivastigmine.Building on this success,we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal,nickel.展开更多
Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_...Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(5)(PPh_(3))}(2)(R=2-cyanobenzyl),were synthesized and characterized by infrared spectroscopy,UV-Vis spectroscopy,single-crystal diffraction,powder X-ray diffraction,etc.Their performances as photocatalysts for H_(2)production through water splitting were evaluated.The results showed that 316.8μmol of H_(2)was produced on compound 1 after 3 h of illumination,with a catalytic efficiency of 25.1μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 36.8.The replacement of carbonyl with PPh3 could significantly improve the catalytic performance of the complex,and 705.0μmol of H_(2)was produced on 2 after 3 h of illumination,with a catalytic efficiency of 37.9μmol·mg^(-1)·h^(-1)and a TON of 81.8.CCDC:2515700,1;2515702,1′;2515701,2.展开更多
0 INTRODUCTION Throughout human history,three major energy transitions have occurred:from burning wood in primitive times to using coal in 18th Century,then to oil and gas in 20th Century,and to the renewable energy r...0 INTRODUCTION Throughout human history,three major energy transitions have occurred:from burning wood in primitive times to using coal in 18th Century,then to oil and gas in 20th Century,and to the renewable energy revolution in the 21st Century(Zou et al.,2023).The three transitions have three characteristics in common:shifted from nonrenewable to renewable energy,from“resource-centric”to a“technology-centric”,and from“high-carbon fossil”to“net-zero”.展开更多
Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we repor...Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.展开更多
This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal th...This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal the diffusion behavior of hydrogen atoms at grain boundaries and their consequential impact on the hydrogen embrittlement sensitivity of iron alloys.The findings indicate that as the hydrogen concentration increases,both the yield strength and ultimate tensile strength of Fe-H alloys exhibit a declining trend.Moreover,the capture of hydrogen atoms at the grain boundaries significantly influences the fracture toughness of the material and promotes the formation and propagation of cracks.This study provides a novel theoretical basis for understanding and predicting the hydrogen embrittlement behavior of iron-based materials in hydrogen-rich environments,offering valuable insights for the design and development of Fe alloys with enhanced resistance to hydrogen embrittlement.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
This letter reports a gravitational redshift measurement experiment using a satellite-based compact passive hydrogen maser(PHM)in a lunar distant retrograde orbit(DRO).In March 2024,the Chinese Academy of Sciences lau...This letter reports a gravitational redshift measurement experiment using a satellite-based compact passive hydrogen maser(PHM)in a lunar distant retrograde orbit(DRO).In March 2024,the Chinese Academy of Sciences launched the DRO-A/B twin satellites,which entered a DRO in July 2024.This orbit has a geocentric distance of approximately 300,000–450,000 kilometers and a 2:1 resonance ratio.Employing microwave dual one-way ranging(DOWR),satellite-ground time-frequency comparisons were successfully achieved in April 2025 using the PHM aboard the DRO-A satellite.This study validated the in-orbit performance of the compact PHM and supported tests of the Einstein Equivalence Principle.The gravitational redshift measurement result is(8.74±4.17)×10^(−3).As the world’s first fundamental physics experiment to deploy PHMs in a lunar DRO,this study provides significant new engineering approaches for testing gravitational theories in cislunar space.展开更多
The inherent oxygen sensitivity of hydrogenases has limited their biomedical use.We report a hybrid peptide-nanocluster hydrogel that establishes a self-sustained anaerobic microenvironment,enabling hydrogenase-cataly...The inherent oxygen sensitivity of hydrogenases has limited their biomedical use.We report a hybrid peptide-nanocluster hydrogel that establishes a self-sustained anaerobic microenvironment,enabling hydrogenase-catalyzed hydrogen therapy under aerobic conditions.The Fmoc-KYF peptide network traps O_(2) in hydrophobic pockets,while photoexcited silver nanoclusters rapidly scavenge residual oxygen,ensuring stable hydrogen evolution.In vitro,the generated hydrogen mitigates oxidative stress and inflammation.In diabetic mice,the light-activated system accelerates wound closure,promotes angiogenesis,and drives macrophage polarization toward a reparative phenotype.This study introduces a bioengineering strategy that integrates material design,enzyme catalysis,and photodynamics to overcome oxygen limitation and advance hydrogenase-based therapeutic applications.展开更多
Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion applications.The workhorse ...Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion applications.The workhorse of warm dense matter theory is thermal density functional theory(DFT),which,however,suffers from two limitations:(i)its accuracy can depend on the utilized exchange-correlation functional,which has to be approximated,and(ii)it is generally limited to single-electron properties such as the density distribution.Here,we present a new ansatz combining time-dependent DFT results for the dynamic structure factor S_(ee)(q,ω)with static DFT results for the density response.This allows us to estimate the electron-electron static structure factor S_(ee)(q)of warm dense hydrogen with high accuracy over a broad range of densities and temperatures.In addition to its value for the study of warm dense matter,our work opens up new avenues for the future study of electronic correlations exclusively within the framework of DFT for a host of applications.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 sp^(3)-hybridized σ electrons 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
Micropillar compression tests were used to investigate the influence of hydrogen on the deformation behavior and hydrogen embrittlement(HE)of nitrogen-alloyed austenitic stainless steel QN_(2)109.Results indicate that...Micropillar compression tests were used to investigate the influence of hydrogen on the deformation behavior and hydrogen embrittlement(HE)of nitrogen-alloyed austenitic stainless steel QN_(2)109.Results indicate that the hydrogen increases the dislocation density,reduces the yield stress,and accelerates the formation and intersection of slip bands,with hydrogen-induced cracks initiating at slip band intersections.X-ray diffraction confirms the absence of martensitic transformation,ruling out the role of martensitic transformation in HE.The micropillar compression technique is highly sensitive for characterizing hydrogen-material interactions,owing to the material’s low hydrogen diffusivity and the small size of its hydrogen-affected zone.These findings align with the hydrogen-enhanced localized plasticity mechanism.展开更多
Hydrogen,as a zero-carbon secondary energy carrier,provides a unified pathway for low-carbon energy transformation.In electro–hydrogen coupling systems(EHCSs),surplus renewable power is stored via water electrolysis ...Hydrogen,as a zero-carbon secondary energy carrier,provides a unified pathway for low-carbon energy transformation.In electro–hydrogen coupling systems(EHCSs),surplus renewable power is stored via water electrolysis and later reconverted to electricity using fuel cells or gas turbines,enhancing the system’s flexibility and reliability in support of deep decarbonization.This study constructs an electricity–hydrogen energy-recycling model based on a coupling relationship considering the bidirectional conversion between electricity and hydrogen.A multistage carbon-emission-reduction indicator constraint is also established.Additionally,the green-certificate and carbon trading markets are introduced to optimize equipment investment and operation costs while achieving carbon-emission reduction.A case study reveals that the proposed EHCS planning model effectively allocates carbon emissions across different system stages,while mitigating economic repercussions,thus ensuring closer alignment with China’s emission-reduction policies.Incorporating diverse market mechanisms significantly enhances the system’s economy and decision-making flexibility,particularly in addressing future challenges in the energy market.展开更多
The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(...The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(2)storage.However,the performance limitations of dehydrogenation catalysts have hindered the rapid development of LOHC technology.In this study,we successfully developed boron-modified Pt/ZrO_(2)catalysts,which exhibit exceptional catalytic performance in cyclohexane dehydrogenation.The optimal boron content is determined to be 0.5 wt.%,with the Pt/0.5B–ZrO_(2)catalyst achieving high turnover frequency(TOF)of 10,627.3 mol_(H_(2))·mol_(Pt)^(−1)·h^(−1)and benzene selectivity of 99%at 295°C.The catalyst also demonstrates H_(2)evolution rate of 908 mmol·g_(Pt)^(−1)·min^(−1)and low deactivation rate of 0.0043 h^(−1).Remarkably,the catalyst displays outstanding stability and regeneration performance,maintaining its activity without significant loss during a 60-h dehydrogenation reaction and retaining a cyclohexane conversion of 77.2%after 10 consecutive cycles.Comprehensive characterization techniques,including XPS,CO-FTIR,NH_(3)-TPD,H_(2)-TPD,Benzene-TPD,and Py-IR,reveals that boron modification reduces the electron density of Pt,generating abundant electron-deficient Pt atoms.These electron-deficient Pt atoms enhance H_(2)adsorption and accelerate benzene desorption,effectively preventing coke formation from deep benzene dehydrogenation,which is responsible for the high catalytic performance of the Pt/0.5B–ZrO_(2)catalyst.These findings offer a valuable strategy for optimizing dehydrogenation catalysts in LOHC technologies,addressing a critical bottleneck in the development of this essential energy storage solution.展开更多
In the sentence beginning'and more irreversible hydrogentrapping sites….'in this article,the value'0.38×10^(25) cm^(-3)'should have read'0.68×10^(20) cm^(-3)'.These corrections do no...In the sentence beginning'and more irreversible hydrogentrapping sites….'in this article,the value'0.38×10^(25) cm^(-3)'should have read'0.68×10^(20) cm^(-3)'.These corrections do not alter the primary conclusion that the irreversible hydrogen trap density in 42CrNiMoV steel is nearly twice that of 40CrNiMo steel.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
The preparation and application of supported gold and copper catalysts are fundamentally and practically very important.Herein,we confirm that the Au-Cu promoted In_(2)O_(3) catalyst demonstrates a significant electro...The preparation and application of supported gold and copper catalysts are fundamentally and practically very important.Herein,we confirm that the Au-Cu promoted In_(2)O_(3) catalyst demonstrates a significant electronic metal-support interaction(EMSI),which plays a critical role in CO_(2) hydrogenation to methanol and leads to significantly improved activity,compared to the mono-metallic Au and Cu promoted In_(2)O_(3)catalysts.This interaction arises from electron transfer between the oxygen deficient In_(2)O_(3) support and the bimetallic clusters,rendering both Au and Cu clusters positively charged.The presence of Cu^(3+)stabilizes and optimizes the content of oxygen vacancies,leading to a more pronounced positive charge on Au clusters(Au^(3+)).The ability to activate H_(2) is thus enhanced.CO adsorption on Au-Cu/In_(2)O_(3) is also stronger than Au/In_(2)O_(3).This results in higher methanol selectivity of Au-Cu/In_(2)O_(3),with which CO hydrogenation pathway is taken for CO_(2) hydrogenation to methanol.The enhanced H_(2) activation and stronger CO adsorption over Au-Cu/In_(2)O_(3) are key factors in boosting the activity for methanol formation from CO_(2)hvdrogenation.展开更多
Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prep...Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.展开更多
As one of the most promising new energy sources,hydrogen energy is expected to usher in a full-fledged“hydrogen economy”in the 21st century.Compared with traditional high-pressure gaseous and cryogenic liquid hydrog...As one of the most promising new energy sources,hydrogen energy is expected to usher in a full-fledged“hydrogen economy”in the 21st century.Compared with traditional high-pressure gaseous and cryogenic liquid hydrogen storage methods,solid-state chemical hydrogen storage shows significant advantages in safety,high efficiency,and cost-effectiveness.Magnesium-based lightweight hydrogen storage materials have attracted widespread attention due to their high gravimetric hydrogen storage density(7.6%)and favorable reversibility.However,their sluggish reaction kinetics and stringent operating conditions(with H2 release temperatures exceeding 350°C and H2 absorption pressures above 4 MPa)pose major challenges for practical applications.Domestic and international researchers have conducted in-depth studies to address these issues,achieving substantial progress in the modification of magnesium-based hydrogen storage alloys.This paper systematically elaborates on major modification techniques such as alloying,nanostructuring,and catalytic material doping,providing a comprehensive analysis of the strengths and limitations of each approach.Furthermore,it offers prospects for the future development of magnesium-based hydrogen storage materials by integrating current theoretical and experimental research findings.展开更多
Cyclohexene is an important raw material in the production of nylon.Selective hydrogenation of benzene is a key method for preparing cyclohexene.However,the Ru catalysts used in current industrial processes still face...Cyclohexene is an important raw material in the production of nylon.Selective hydrogenation of benzene is a key method for preparing cyclohexene.However,the Ru catalysts used in current industrial processes still face challenges,including high metal usage,high process costs,and low cyclohexene yield.This study utilizes existing literature data combined with machine learning methods to analyze the factors influencing benzene conversion,cyclohexene selectivity,and yield in the benzene hydrogenation to cyclohexene reaction.It constructs predictive models based on XGBoost and Random Forest algorithms.After analysis,it was found that reaction time,Ru content,and space velocity are key factors influencing cyclohexene yield,selectivity,and benzene conversion.Shapley Additive Explanations(SHAP)analysis and feature importance analysis further revealed the contribution of each variable to the reaction outcomes.Additionally,we randomly generated one million variable combinations using the Dirichlet distribution to attempt to predict high-yield catalyst formulations.This paper provides new insights into the application of machine learning in heterogeneous catalysis and offers some reference for further research.展开更多
文摘Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy influence the competitiveness of economies,while the level of energy consumption impacts the standard of living for individuals.This paper aims to examine environmental challenges and steps for a sustainable transition towards a hydrogen economy,focusing on its potential as an alternative to fossil fuels and the importance of developing the hydrogen paradigm.The research methodology is based on a combination of qualitative and quantitative methods,including an analysis of global and regional trends in the energy transition,the impact of various forms of hydrogen production(green,blue,gray hydrogen)on greenhouse gas emissions,and a comparison of existing policies and strategies in different countries transitioning to a sustainable hydrogen economy.Research results show that green hydrogen,produced via electrolysis using renewable energy sources,holds the greatest potential for reducing greenhouse gas emissions,while gray and blue hydrogen can serve as transitional options.The development of the hydrogen paradigm,rooted in innovative technologies,renewable energy sources,and international cooperation,is crucial for decarbonization and the creation of a sustainable global economy,despite challenges such as high costs and the need for global coordination.The hydrogen paradigm is becoming a cornerstone of these efforts,laying the foundation for a long-term,sustainable global economy.Currently,over 180 hydrogen transport projects,60 distribution projects,80 storage projects,30 terminal and port projects,and more than 220 hydrogen production projects are under development worldwide.The global momentum of the hydrogen transition helps mitigate climate change and build a sustainable future.
基金supported by the National Natural Science Foundation of China(Nos.22271007,W2431014)Peking University Shenzhen Graduate School+2 种基金State Key Laboratory of Chemical OncogenomicsShenzhen Key Laboratory of Chemical GenomicsShenzhen Bay Laboratory.
文摘Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source.The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of(S)-rivastigmine.Building on this success,we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal,nickel.
文摘Two[FeFe]-hydrogenase compounds with 2-cyanobenzyl groups,{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(6)}(1 or 1′,which are the crystalline states from petroleum ether and dichloromethane solution,respectively)and{Fe_(2)[(SCH_(2)CH_(3))(SR)](CO)_(5)(PPh_(3))}(2)(R=2-cyanobenzyl),were synthesized and characterized by infrared spectroscopy,UV-Vis spectroscopy,single-crystal diffraction,powder X-ray diffraction,etc.Their performances as photocatalysts for H_(2)production through water splitting were evaluated.The results showed that 316.8μmol of H_(2)was produced on compound 1 after 3 h of illumination,with a catalytic efficiency of 25.1μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 36.8.The replacement of carbonyl with PPh3 could significantly improve the catalytic performance of the complex,and 705.0μmol of H_(2)was produced on 2 after 3 h of illumination,with a catalytic efficiency of 37.9μmol·mg^(-1)·h^(-1)and a TON of 81.8.CCDC:2515700,1;2515702,1′;2515701,2.
基金supported by the National Natural Science Foundation of China“Quantitative characterization of lacustrine shale oil mobility based on nano-scale oil-rock interactions”(No.42172180)Science and Technology Research Project for the China National Petroleum Corporation“Source-reservoir characteristics and sweet spot evaluation for terrestrial shale oil in China”(No.2021DJ1802)。
文摘0 INTRODUCTION Throughout human history,three major energy transitions have occurred:from burning wood in primitive times to using coal in 18th Century,then to oil and gas in 20th Century,and to the renewable energy revolution in the 21st Century(Zou et al.,2023).The three transitions have three characteristics in common:shifted from nonrenewable to renewable energy,from“resource-centric”to a“technology-centric”,and from“high-carbon fossil”to“net-zero”.
基金financially supported by the“National Natural Science Foundation of China”(No.22279082)the“Natural Science Foundation of Sichuan”(2025YFHZ0056)。
文摘Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.
基金supported by the National Science Fund for Distinguished Young Scholars(No.52425404).
文摘This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal the diffusion behavior of hydrogen atoms at grain boundaries and their consequential impact on the hydrogen embrittlement sensitivity of iron alloys.The findings indicate that as the hydrogen concentration increases,both the yield strength and ultimate tensile strength of Fe-H alloys exhibit a declining trend.Moreover,the capture of hydrogen atoms at the grain boundaries significantly influences the fracture toughness of the material and promotes the formation and propagation of cracks.This study provides a novel theoretical basis for understanding and predicting the hydrogen embrittlement behavior of iron-based materials in hydrogen-rich environments,offering valuable insights for the design and development of Fe alloys with enhanced resistance to hydrogen embrittlement.
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This letter reports a gravitational redshift measurement experiment using a satellite-based compact passive hydrogen maser(PHM)in a lunar distant retrograde orbit(DRO).In March 2024,the Chinese Academy of Sciences launched the DRO-A/B twin satellites,which entered a DRO in July 2024.This orbit has a geocentric distance of approximately 300,000–450,000 kilometers and a 2:1 resonance ratio.Employing microwave dual one-way ranging(DOWR),satellite-ground time-frequency comparisons were successfully achieved in April 2025 using the PHM aboard the DRO-A satellite.This study validated the in-orbit performance of the compact PHM and supported tests of the Einstein Equivalence Principle.The gravitational redshift measurement result is(8.74±4.17)×10^(−3).As the world’s first fundamental physics experiment to deploy PHMs in a lunar DRO,this study provides significant new engineering approaches for testing gravitational theories in cislunar space.
基金partially supported by the Center for Advanced Systems Understanding (CASUS), financed by Germany’s Federal Ministry of Education and Research and the Saxon State Government out of the State Budget approved by the Saxon State Parliamentthe European Union’s Just Transition Fund (JTF) within the project Röntgenlaser Optimierung der Laserfusion (ROLF), Contract No. 5086999001, co-financed by the Saxon State Government out of the State Budget approved by the Saxon State Parliament+3 种基金the European Research Council (ERC) under the European Union’s Horizon 2022 Research and Innovation Programme (Grant Agreement No. 101076233, “PREXTREME”)Computations were performed on a Bull Cluster at the Center for Information Services and High-Performance Computing (ZIH) at Technische Universität Dresden and at the Norddeutscher Verbund für Hoch- und Höchstleistungsrechnen (HLRN) under Grant No. mvp00024support by the National Natural Science Foundation of China under Grant No. 12274171support by the Advanced Materials–National Science and Technology Major Project (Grant No. 2024ZD0606900)
文摘Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion applications.The workhorse of warm dense matter theory is thermal density functional theory(DFT),which,however,suffers from two limitations:(i)its accuracy can depend on the utilized exchange-correlation functional,which has to be approximated,and(ii)it is generally limited to single-electron properties such as the density distribution.Here,we present a new ansatz combining time-dependent DFT results for the dynamic structure factor S_(ee)(q,ω)with static DFT results for the density response.This allows us to estimate the electron-electron static structure factor S_(ee)(q)of warm dense hydrogen with high accuracy over a broad range of densities and temperatures.In addition to its value for the study of warm dense matter,our work opens up new avenues for the future study of electronic correlations exclusively within the framework of DFT for a host of applications.
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 sp^(3)-hybridized σ electrons 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support from the National Natural Science Foundation of China(Grant No.U24A20105 and 52071209)the Major Scientific and Technological Innovation Project of CITIC Group(Grant No.2022ZXKYA06100,with Hongzhou Lu as the principal grant recipient)the Program of Shanghai Academic and Technology Research Leader(Grant No.18XD1402200).
文摘Micropillar compression tests were used to investigate the influence of hydrogen on the deformation behavior and hydrogen embrittlement(HE)of nitrogen-alloyed austenitic stainless steel QN_(2)109.Results indicate that the hydrogen increases the dislocation density,reduces the yield stress,and accelerates the formation and intersection of slip bands,with hydrogen-induced cracks initiating at slip band intersections.X-ray diffraction confirms the absence of martensitic transformation,ruling out the role of martensitic transformation in HE.The micropillar compression technique is highly sensitive for characterizing hydrogen-material interactions,owing to the material’s low hydrogen diffusivity and the small size of its hydrogen-affected zone.These findings align with the hydrogen-enhanced localized plasticity mechanism.
基金supported by State Grid Jiangsu Electric Power Co.,Ltd.Technology Project(Research on Planning and Operation Technology of Electric–Hydrogen Coupling System Driven by the Electric–Carbon–Green Certificate Market):J2024005.
文摘Hydrogen,as a zero-carbon secondary energy carrier,provides a unified pathway for low-carbon energy transformation.In electro–hydrogen coupling systems(EHCSs),surplus renewable power is stored via water electrolysis and later reconverted to electricity using fuel cells or gas turbines,enhancing the system’s flexibility and reliability in support of deep decarbonization.This study constructs an electricity–hydrogen energy-recycling model based on a coupling relationship considering the bidirectional conversion between electricity and hydrogen.A multistage carbon-emission-reduction indicator constraint is also established.Additionally,the green-certificate and carbon trading markets are introduced to optimize equipment investment and operation costs while achieving carbon-emission reduction.A case study reveals that the proposed EHCS planning model effectively allocates carbon emissions across different system stages,while mitigating economic repercussions,thus ensuring closer alignment with China’s emission-reduction policies.Incorporating diverse market mechanisms significantly enhances the system’s economy and decision-making flexibility,particularly in addressing future challenges in the energy market.
基金supported by National Natural Science Foundation of China(22478076,U25B6005)National Key R&D Program of China(2021YFA1500302)+1 种基金Industrial Joint Fund of Qingyuan Innovation Laboratory(00422001)111 Project(D17005).
文摘The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(2)storage.However,the performance limitations of dehydrogenation catalysts have hindered the rapid development of LOHC technology.In this study,we successfully developed boron-modified Pt/ZrO_(2)catalysts,which exhibit exceptional catalytic performance in cyclohexane dehydrogenation.The optimal boron content is determined to be 0.5 wt.%,with the Pt/0.5B–ZrO_(2)catalyst achieving high turnover frequency(TOF)of 10,627.3 mol_(H_(2))·mol_(Pt)^(−1)·h^(−1)and benzene selectivity of 99%at 295°C.The catalyst also demonstrates H_(2)evolution rate of 908 mmol·g_(Pt)^(−1)·min^(−1)and low deactivation rate of 0.0043 h^(−1).Remarkably,the catalyst displays outstanding stability and regeneration performance,maintaining its activity without significant loss during a 60-h dehydrogenation reaction and retaining a cyclohexane conversion of 77.2%after 10 consecutive cycles.Comprehensive characterization techniques,including XPS,CO-FTIR,NH_(3)-TPD,H_(2)-TPD,Benzene-TPD,and Py-IR,reveals that boron modification reduces the electron density of Pt,generating abundant electron-deficient Pt atoms.These electron-deficient Pt atoms enhance H_(2)adsorption and accelerate benzene desorption,effectively preventing coke formation from deep benzene dehydrogenation,which is responsible for the high catalytic performance of the Pt/0.5B–ZrO_(2)catalyst.These findings offer a valuable strategy for optimizing dehydrogenation catalysts in LOHC technologies,addressing a critical bottleneck in the development of this essential energy storage solution.
文摘In the sentence beginning'and more irreversible hydrogentrapping sites….'in this article,the value'0.38×10^(25) cm^(-3)'should have read'0.68×10^(20) cm^(-3)'.These corrections do not alter the primary conclusion that the irreversible hydrogen trap density in 42CrNiMoV steel is nearly twice that of 40CrNiMo steel.
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 National Natural Science Foundation of China(22138009)the Fundamental Research Funds for the Central Universities of China。
文摘The preparation and application of supported gold and copper catalysts are fundamentally and practically very important.Herein,we confirm that the Au-Cu promoted In_(2)O_(3) catalyst demonstrates a significant electronic metal-support interaction(EMSI),which plays a critical role in CO_(2) hydrogenation to methanol and leads to significantly improved activity,compared to the mono-metallic Au and Cu promoted In_(2)O_(3)catalysts.This interaction arises from electron transfer between the oxygen deficient In_(2)O_(3) support and the bimetallic clusters,rendering both Au and Cu clusters positively charged.The presence of Cu^(3+)stabilizes and optimizes the content of oxygen vacancies,leading to a more pronounced positive charge on Au clusters(Au^(3+)).The ability to activate H_(2) is thus enhanced.CO adsorption on Au-Cu/In_(2)O_(3) is also stronger than Au/In_(2)O_(3).This results in higher methanol selectivity of Au-Cu/In_(2)O_(3),with which CO hydrogenation pathway is taken for CO_(2) hydrogenation to methanol.The enhanced H_(2) activation and stronger CO adsorption over Au-Cu/In_(2)O_(3) are key factors in boosting the activity for methanol formation from CO_(2)hvdrogenation.
基金Supported by National Key R&D Program of China(2022YFA1503400)。
文摘Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.
基金Supported by Design and Performance Study of High-flux Metal Hydride Reactor Based on the Bionic Optimization(2078262)the‘Four-Chain’Integration Project at the Qinchuangyuan Chief Platform(S2025-YF-ZDXM)。
文摘As one of the most promising new energy sources,hydrogen energy is expected to usher in a full-fledged“hydrogen economy”in the 21st century.Compared with traditional high-pressure gaseous and cryogenic liquid hydrogen storage methods,solid-state chemical hydrogen storage shows significant advantages in safety,high efficiency,and cost-effectiveness.Magnesium-based lightweight hydrogen storage materials have attracted widespread attention due to their high gravimetric hydrogen storage density(7.6%)and favorable reversibility.However,their sluggish reaction kinetics and stringent operating conditions(with H2 release temperatures exceeding 350°C and H2 absorption pressures above 4 MPa)pose major challenges for practical applications.Domestic and international researchers have conducted in-depth studies to address these issues,achieving substantial progress in the modification of magnesium-based hydrogen storage alloys.This paper systematically elaborates on major modification techniques such as alloying,nanostructuring,and catalytic material doping,providing a comprehensive analysis of the strengths and limitations of each approach.Furthermore,it offers prospects for the future development of magnesium-based hydrogen storage materials by integrating current theoretical and experimental research findings.
基金Supported by CAS Basic and Interdisciplinary Frontier Scientific Research Pilot Project(XDB1190300,XDB1190302)Youth Innovation Promotion Association CAS(Y2021056)+1 种基金Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2022007)The special fund for Science and Technology Innovation Teams of Shanxi Province(202304051001007)。
文摘Cyclohexene is an important raw material in the production of nylon.Selective hydrogenation of benzene is a key method for preparing cyclohexene.However,the Ru catalysts used in current industrial processes still face challenges,including high metal usage,high process costs,and low cyclohexene yield.This study utilizes existing literature data combined with machine learning methods to analyze the factors influencing benzene conversion,cyclohexene selectivity,and yield in the benzene hydrogenation to cyclohexene reaction.It constructs predictive models based on XGBoost and Random Forest algorithms.After analysis,it was found that reaction time,Ru content,and space velocity are key factors influencing cyclohexene yield,selectivity,and benzene conversion.Shapley Additive Explanations(SHAP)analysis and feature importance analysis further revealed the contribution of each variable to the reaction outcomes.Additionally,we randomly generated one million variable combinations using the Dirichlet distribution to attempt to predict high-yield catalyst formulations.This paper provides new insights into the application of machine learning in heterogeneous catalysis and offers some reference for further research.
