In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics...In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics(BM),we have theoretically explored the two-electron correlation characteristics while generating high-order harmonics in xenon atoms subjected to intense laser fields.We initially employed Bohmian trajectories to reproduce the dynamics of the electrons and subsequently utilized time-frequency analysis spectra to ascertain the emission time windows for high-order harmonics.Within these time windows,we classified the nuclear region Bohmian trajectories and observed that intense high-order harmonics are solely generated when paired Bohmian particles(BPs)concurrently appear in the nuclear region and reside there for a duration within a re-collision time window.Furthermore,our analysis of characteristic trajectories producing high-order harmonics led us to propose a two-electron re-collision model to elucidate this phenomenon.The study demonstrates that intense high-order harmonics are only generated when both electrons are in the ground state within the re-collision time window.This work discusses the implications of correlation effects between two electrons and offers valuable insights for studying correlation in multi-electron high-order harmonic generation.展开更多
The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basi...The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basis set.Contrary to the localized behavior observed in the ground and the doubly excited 2p^(23)Pe states,for this state our results identify that while the behavior of the inner electron increasingly resembles that of a hydrogen-like atomic system,the outer electron in the excited state exhibits diffused hydrogen-like character and becomes perpendicular to the inner electron as nuclear charge Z approaches Z_(c).This study provides insights into the electronic structure and stability of the two-electron system in the vicinity of the critical nuclear charge.展开更多
Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within ...Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within the framework of Ritz variational method.The wavefunction is expanded in explicitly correlated Hylleraas type basis set.The screened Coulomb potential is consideredas mimic the WCP environment.The atomic systems tend towards gradual instability and the number of excited metastable bound states reduces with increasing plasma strength.The wavelengths corresponding to 2 pnf(1,3F^e)→2 pnf(1,3Do)(n=4–6;n′=3–6)transitions occurring between doubly excited states of plasma embedded two-electron ions are also reported.展开更多
The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and doubl...The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and double ionization process are calculated by the BM theory and their results are in good agreement with those calculated by numerically solving the time-dependent Schrodinger equation. The analyses of the types, trajectories, and forces of Bohmian particles(BPs)undergoing the single and double ionizations indicate that the re-collision process accounts for a considerable proportion in the singly ionized cases. Furthermore, the analysis of the work done by the external force acting on the BPs shows that the quantum force plays an important role in the re-collision process. This work is helpful in understanding the ionization of two-electron atom in an intense laser field.展开更多
Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screen...Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screening parameters for each system considered and provide an insight into their physical structure. The energy eigenvalues have been exactly calculated for atoms with nuclear charge Z in the range 1 ≤ Z ≤ 12, clarifying the relation between the screening parameteter and Z.展开更多
Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturiza...Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.展开更多
Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,...A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.展开更多
The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin cat...The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin catalyst(Ir@KM)is realized on a potassium-manganese oxide(K_(0.25)MnO_(x)(KM))using an ion-exchange method.The Ir-skin over the prepared Ir@KM has a low Ir-Ir atomic distance,endowing an energetically favorable oxide path mechanism to allow a low theoretical overpotential of 0.13 V.Ir@KM offers a low overpotential of~280 mV at a current density of 10 mA cm^(-2)and provides a high mass activity of up to 18,500 A at a cell voltage of 1.8 V in PEM,which is 17.6 times higher than that of IrO_(2),demonstrating a significant advantage in reducing the cost of the membrane electrode.The presented Ir-skin concept represents a promising strategy to fabricate low-Ir catalyst with high activity and durability for practical applications of PEM.展开更多
The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulat...The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.展开更多
Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibite...Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.展开更多
Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g...Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.展开更多
Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity...Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.展开更多
The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric charac...The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric character and features of internal motion of the ~1S^e heliumstates having different K--numbers have been shown, the mechanism for energy transfer andthe details of radial-radial correlation have been inspected. The motion of the inner electroniccloud as a whole is found to be strongly correlated with the motion of the outer electron.展开更多
By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electri...By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electric field. For a certain infinite set of discrete oscillator frequencies, we obtain the analytical solutions. The ground state polarization of the atom is then calculated. The same result is also obtained through linear response theory.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the compl...The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.展开更多
Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.Thi...Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.This paper presents a high-fidelity numerical study of liquidatomization and spray combustion under high-pressure conditions,emphasizing the effects of pres-sure oscillations on the flow evolution and combustion dynamics.The theoretical framework isbased on the three-dimensional conservation equations for multiphase flows and turbulent combus-tion.The numerical solution is achieved using a coupling method of volume-of-fluid and Lagran-gian particle tracking.The Zhuang-Kadota-Sutton(ZKS)high-pressure evaporation model andthe eddy breakup-Arrhenius combustion model are employed.Simulations are conducted for amodel combustion chamber with impinging-jet injectors using liquid oxygen and kerosene as pro-pellants.Both conditions with and without inlet and outlet pressure oscillations are considered.Thefindings reveal that pressure oscillations amplify flow fluctuations and can be characterized usingkey physical parameters such as droplet evaporation,chemical reaction,and chamber pressure.The spectral analysis uncovers the axial variations of the dominant and secondary frequenciesand their amplitudes in terms of the characteristic physical quantities.This research helps establisha methodology for exploring the coupling effect of liquid atomization and spray combustion.It alsoprovides practical insights into their responses to pressure oscillations during the occurrence ofcombustion instability.This information can be used to enhance the design and operation ofliquid-fueled propulsion engines.展开更多
Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(...Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(3) with irregular,rod-like,and flower-like morphologies are used for catalytic CO_(2) hydrogenation to methanol.Results indicate that the flower-like Ru/In_(2)O_(3)(Ru/In_(2)O_(3)-F)exhibits higher catalytic performance than Ru/In_(2)O_(3) with other morphologies,achieving a 12.9%CO_(2) conversion,74.02%methanol selectivity,and 671.36 mg_(MeOH) h^(−1) g_(cat)^(−1) methanol spatiotemporal yield.Furthermore,Ru/In_(2)O_(3)-F maintains its catalytic stability over 200 h at 5 MPa and 290℃.The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In_(2)O_(3).The strong interaction between atomically dispersed Ru and In_(2)O_(3)-F enhances the structural stability of Ru,inhibiting the agglomeration of the catalyst during the reaction process.Furthermore,density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes,facilitating the catalytic activation of H_(2) into H intermediates.It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO_(2) reduction.These findings provide a theoretical basis for the development of high-performance catalysts for CO_(2) hydrogenation.展开更多
基金Project supported by the Natural Science Foundation(General Project)of Jilin Province,China(Grant No.20230101283JC)。
文摘In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics(BM),we have theoretically explored the two-electron correlation characteristics while generating high-order harmonics in xenon atoms subjected to intense laser fields.We initially employed Bohmian trajectories to reproduce the dynamics of the electrons and subsequently utilized time-frequency analysis spectra to ascertain the emission time windows for high-order harmonics.Within these time windows,we classified the nuclear region Bohmian trajectories and observed that intense high-order harmonics are solely generated when paired Bohmian particles(BPs)concurrently appear in the nuclear region and reside there for a duration within a re-collision time window.Furthermore,our analysis of characteristic trajectories producing high-order harmonics led us to propose a two-electron re-collision model to elucidate this phenomenon.The study demonstrates that intense high-order harmonics are only generated when both electrons are in the ground state within the re-collision time window.This work discusses the implications of correlation effects between two electrons and offers valuable insights for studying correlation in multi-electron high-order harmonic generation.
基金supported by the National Natural Science Foundation of China(Grant Nos.12074295,12304271,and 12104420).
文摘The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basis set.Contrary to the localized behavior observed in the ground and the doubly excited 2p^(23)Pe states,for this state our results identify that while the behavior of the inner electron increasingly resembles that of a hydrogen-like atomic system,the outer electron in the excited state exhibits diffused hydrogen-like character and becomes perpendicular to the inner electron as nuclear charge Z approaches Z_(c).This study provides insights into the electronic structure and stability of the two-electron system in the vicinity of the critical nuclear charge.
基金Supported under Grant No. EMR/2017/000737 from DST-SERB, Govt. of India, Grant No. 23(Sanc.)/ST/P/S&T/16G-35/2017 from DHESTB, Govt. of West Bengal, Indiaby the DHESTB,Govt.of West Bengal,India under Grant No.249(Sanc.)/ST/P/S&T/16G-26/2017
文摘Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within the framework of Ritz variational method.The wavefunction is expanded in explicitly correlated Hylleraas type basis set.The screened Coulomb potential is consideredas mimic the WCP environment.The atomic systems tend towards gradual instability and the number of excited metastable bound states reduces with increasing plasma strength.The wavelengths corresponding to 2 pnf(1,3F^e)→2 pnf(1,3Do)(n=4–6;n′=3–6)transitions occurring between doubly excited states of plasma embedded two-electron ions are also reported.
基金Project supported by the Jilin Provincial Science and Technology Development Plan Program for Excellent Youth Talents,China(Grant No.20180520174JH)the National Natural Science Foundation of China(Grant Nos.11704145,11904050,11774129,11747007,11534004,and 12074145).
文摘The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and double ionization process are calculated by the BM theory and their results are in good agreement with those calculated by numerically solving the time-dependent Schrodinger equation. The analyses of the types, trajectories, and forces of Bohmian particles(BPs)undergoing the single and double ionizations indicate that the re-collision process accounts for a considerable proportion in the singly ionized cases. Furthermore, the analysis of the work done by the external force acting on the BPs shows that the quantum force plays an important role in the re-collision process. This work is helpful in understanding the ionization of two-electron atom in an intense laser field.
文摘Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screening parameters for each system considered and provide an insight into their physical structure. The energy eigenvalues have been exactly calculated for atoms with nuclear charge Z in the range 1 ≤ Z ≤ 12, clarifying the relation between the screening parameteter and Z.
基金supported by the Beijing Natural Science Foundation(Grant No.3252013)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0300402)+1 种基金the National Natural Science Foundation of China(Grant No.61673041)Key Area Research and Development Program of Guangdong Province(Grant No.2021B0101410005)。
文摘Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.
基金supported by the National Key R&D Program of China(2021YFA1502802)the National Natural Science Foundation of China(U21B2092,22202213,22402210,22502215,22502214,22572200,and 22579171)+4 种基金the International Partnership Program of Chinese Academy of Sciences(172GJHZ2022028MI)the Shenyang Bureau of Science and Technology(24-213-3-25)the Natural Science Foundation of Liaoning Province(2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119The XAS experiments were conducted in Beijing Synchrotron Radiation Facility(BSRF)and Shanghai Synchrotron Radiation Facility(SSRF).
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
基金supported by the National Natural Science Foundation of China (22472031,U24A20567,22032002)the 111 Project。
文摘A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2023GXJS165)the National Natural Science Foundation of China(52164028,22109035,52274297)+2 种基金the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,MRUKF2021029)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20084,21170)the Specific Research Fund of the Innovation Platform for Academicians of Hainan Province。
文摘The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin catalyst(Ir@KM)is realized on a potassium-manganese oxide(K_(0.25)MnO_(x)(KM))using an ion-exchange method.The Ir-skin over the prepared Ir@KM has a low Ir-Ir atomic distance,endowing an energetically favorable oxide path mechanism to allow a low theoretical overpotential of 0.13 V.Ir@KM offers a low overpotential of~280 mV at a current density of 10 mA cm^(-2)and provides a high mass activity of up to 18,500 A at a cell voltage of 1.8 V in PEM,which is 17.6 times higher than that of IrO_(2),demonstrating a significant advantage in reducing the cost of the membrane electrode.The presented Ir-skin concept represents a promising strategy to fabricate low-Ir catalyst with high activity and durability for practical applications of PEM.
基金supported by the National Natural Science Foundation of China(52402166)the Science and Technology Development Fund+2 种基金Macao SAR(0065/2023/AFJ,0116/2022/A3)the Australian Research Council(DE220100154)the Natural Science Foundation of Guangdong Province(2025A1515011120)。
文摘The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.
基金supported by the National Natural Science Foundation of China(Nos.22406081,22276086,22306086)the Natural Science Foundation of Jiangxi Province(No.20232BAB213029),all of which are greatly acknowledged by the authors.
文摘Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.
基金supported by Natural Science Foundation of China(Nos.U23B20165 and 52170085)National Key R&D Program International Cooperation Project(No.2023YFE0108100)+1 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
基金supported by the National Natural Science Foundation of China(Nos.22179093 and 21905202)。
文摘Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.
基金Project supported by the National Natural Science Foundation of China.
文摘The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric character and features of internal motion of the ~1S^e heliumstates having different K--numbers have been shown, the mechanism for energy transfer andthe details of radial-radial correlation have been inspected. The motion of the inner electroniccloud as a whole is found to be strongly correlated with the motion of the outer electron.
基金Supported by the National Natural Science Foundation of China under Grant No.10805029ZheJiang NSF under Grant No.R6090717the K.C.Wong Magna Foundation of Ningbo University
文摘By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electric field. For a certain infinite set of discrete oscillator frequencies, we obtain the analytical solutions. The ground state polarization of the atom is then calculated. The same result is also obtained through linear response theory.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金supported by the Pre-research fund(No.412130024).
文摘The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.
基金supported by the National Natural Science Foundation of China(Nos.U23B6009 and 12272050)。
文摘Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.This paper presents a high-fidelity numerical study of liquidatomization and spray combustion under high-pressure conditions,emphasizing the effects of pres-sure oscillations on the flow evolution and combustion dynamics.The theoretical framework isbased on the three-dimensional conservation equations for multiphase flows and turbulent combus-tion.The numerical solution is achieved using a coupling method of volume-of-fluid and Lagran-gian particle tracking.The Zhuang-Kadota-Sutton(ZKS)high-pressure evaporation model andthe eddy breakup-Arrhenius combustion model are employed.Simulations are conducted for amodel combustion chamber with impinging-jet injectors using liquid oxygen and kerosene as pro-pellants.Both conditions with and without inlet and outlet pressure oscillations are considered.Thefindings reveal that pressure oscillations amplify flow fluctuations and can be characterized usingkey physical parameters such as droplet evaporation,chemical reaction,and chamber pressure.The spectral analysis uncovers the axial variations of the dominant and secondary frequenciesand their amplitudes in terms of the characteristic physical quantities.This research helps establisha methodology for exploring the coupling effect of liquid atomization and spray combustion.It alsoprovides practical insights into their responses to pressure oscillations during the occurrence ofcombustion instability.This information can be used to enhance the design and operation ofliquid-fueled propulsion engines.
基金financially supported by the Key Laboratory of Carbon-based Energy Molecular Chemical Utilization Technology in Guizhou Province(No.2023008)Guizhou Provincial Science and Technology Projects(No.ZKZD2023004)+1 种基金One Hundred Person Project of Guizhou Province(No.GCC 2023013)Scientific and Technological Innovation Talents Team Project of Guizhou Province(No.CXTD2023029).
文摘Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(3) with irregular,rod-like,and flower-like morphologies are used for catalytic CO_(2) hydrogenation to methanol.Results indicate that the flower-like Ru/In_(2)O_(3)(Ru/In_(2)O_(3)-F)exhibits higher catalytic performance than Ru/In_(2)O_(3) with other morphologies,achieving a 12.9%CO_(2) conversion,74.02%methanol selectivity,and 671.36 mg_(MeOH) h^(−1) g_(cat)^(−1) methanol spatiotemporal yield.Furthermore,Ru/In_(2)O_(3)-F maintains its catalytic stability over 200 h at 5 MPa and 290℃.The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In_(2)O_(3).The strong interaction between atomically dispersed Ru and In_(2)O_(3)-F enhances the structural stability of Ru,inhibiting the agglomeration of the catalyst during the reaction process.Furthermore,density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes,facilitating the catalytic activation of H_(2) into H intermediates.It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO_(2) reduction.These findings provide a theoretical basis for the development of high-performance catalysts for CO_(2) hydrogenation.
