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
Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a chall...Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.展开更多
Atmospheric escape plays a critical role in shaping the long-term climate evolution of Mars.Among the various escape mechanisms,energetic neutral atoms(ENAs)generated through charge exchange between solar wind ions an...Atmospheric escape plays a critical role in shaping the long-term climate evolution of Mars.Among the various escape mechanisms,energetic neutral atoms(ENAs)generated through charge exchange between solar wind ions and exospheric neutrals serve as an important diagnostic for ion-neutral interactions and upper atmospheric loss.This study presents direct observations of hydrogen ENAs(H-ENAs)on the dayside of Mars by using the Mars Ion and Neutral Particle Analyzer(MINPA)onboard China’s Tianwen-1 orbiter.By analyzing H-ENA data during a coronal mass ejection and a stream interaction region from December 29,2021,to January 1,2022,and comparing these data with MAVEN/SWIA(Mars Atmosphere and Volatile EvolutioN/Solar Wind Ion Analyzer)solar wind measurements,we examine the temporal evolution of H-ENA flux and the associated sputtered escape of atmospheric constituents.The observed H-ENA velocity is consistent with upstream solar wind ions,and the H-ENA-to-ion intensity ratio is used to infer variations in exospheric density,revealing a delayed response to enhanced solar wind activity.Penetrating H-ENA intensities reach up to 5.3×10^(6)s^(−1) cm^(−2),with energy fluxes on the order of(0.5-8.1)×10^(−3) mW/m^(2).The estimated oxygen sputtered escape rate driven by penetrating H-ENAs ranges from 5.5×10^(23)s^(−1) to 5.2×10^(24)s^(−1),comparable to or exceeding previous estimates based on penetrating ions.The findings highlight the need for low-altitude H-ENA observations to better quantify their atmospheric interactions and refine our understanding of nonthermal escape processes at Mars.展开更多
Conversion between different types of entangled states is an interesting problem in quantum mechanics.But research on the conversion between the Greenberger-Horne-Zeilinger(GHZ)state and Knill-Laflamme-Milburn(KLM)sta...Conversion between different types of entangled states is an interesting problem in quantum mechanics.But research on the conversion between the Greenberger-Horne-Zeilinger(GHZ)state and Knill-Laflamme-Milburn(KLM)state in an atomic system has not been reported.In this paper,we propose a scheme to realize the interconversion(one-step)between the GHZ state and KLM state with Rydberg atoms.By utilizing Rydberg-mediated interactions,we simplify the system.By combining a Lie-transform-based pulse design,the evolution path is built up to realize interconversion of the GHZ state and KLM state.The numerical simulation result shows that the present scheme is robust against decoherence and operational imperfection.展开更多
The introduction of metal single atoms(SAs)and nanoparticles(NPs)are effective approaches to mod-ify electronic configuration of semiconductors,whereas recognizing the synergistic effects of metal SAs and NPs are stil...The introduction of metal single atoms(SAs)and nanoparticles(NPs)are effective approaches to mod-ify electronic configuration of semiconductors,whereas recognizing the synergistic effects of metal SAs and NPs are still challenging in photocatalytic water purification.Herein,a general strategy is achieved by subsequentially anchoring Fe SAs and Fe NPs in graphitic carbon nitride.The modification of Fe SAs and Fe NPs improves the energy band structure and constructs a gradient charge polarization,directly expanding the optical absorption range and facilitating the efficient separation and transfer of charge car-riers.With the assistance of the gradient charge polarization,pollutants are readily oxidated by h+,which strengthens the continuous reduction of O2 on Fe NPs for pollutant oxidation in water.This work rein-forces the synergistic effect of SAs and NPs on electronic configuration modulation at the atomic level,which exhibits great potential for the construction of an efficient and sustainable water purification sys-tem.展开更多
The photocatalytic oxidation of methane to methanol using molecule oxygen directly is an attractive catalytic reaction,but designing catalysts to avoid over-oxidation remains a significant challenge.Herein,Cu single-a...The photocatalytic oxidation of methane to methanol using molecule oxygen directly is an attractive catalytic reaction,but designing catalysts to avoid over-oxidation remains a significant challenge.Herein,Cu single-atom anchored on the defective carbon nitride structure(Cu SA/Def-CN)is designed for selective photocatalytic oxidation of methane into methanol using O_(2) under mild conditions.The Cu SA/Def-CN catalyst exhibits a high methanol selectivity of 92.8%under optimized conditions.Mechanistic studies reveal a synergistic effect between Def-CN and Cu SA,where Def-CN is responsible for the in-situ generation of hydrogen peroxide,which is subsequently decomposed by the Cu SA sites to produce·OH radicals that play a key role in the rate-determining step of methane activation to form methanol.Additionally,the presence of Cu SA not only enhances the electron-hole separation efficiency and improves the transfer of the photo-generated charges,but also increases the number of active sites for methane adsorption and activation.These insights provide valuable guidance for designing efficient catalysts for the highly selective photocatalytic oxidation of methane to methanol.展开更多
We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loa...We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loading a green MOT of ^(171)Yb atoms, the phase shift is obtained with a two-color Mach–Zehnder interferometer by means of ±45 MHz detuning with respect to the ^(1)S_(0)–^(1)P_(1) transition. We measured a phase shift of about 100 mrad corresponding to an atom count of around 5 × 10^(5). This demonstrates that it is possible to obtain the number of atoms without direct destructive measurement compared with the absorption imaging method. This scheme could be an important approach towards a high-precision lattice clock for clock operation through suppression of the impact of the Dick effect.展开更多
We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equatio...We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.展开更多
Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duct...Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duction to H_(2)O_(2),it is a challenge for polymeric photocatalysts to achieve efficient photocatalytic H_(2)O_(2) production.Herein,Ag single atoms and nitrogen defects decorated carbon nitride(Ag@MCT)are con-structed through self-assembly and pyrolysis methods.The optimized photocatalyst displays exceptional performance in pure water,with an H_(2)O_(2) production rate of as high as 528.4μmol g^(-1) h^(-1) and an apparent quantum yield for H_(2)O_(2)production of 4.5%at 420 nm.Experimental and theoretical results reveal that the Ag atomic sites act as electron mediators that promote the capture and transfer of photo-generated charge carriers,while nitrogen defects as electron collectors and reaction sites to enhance the adsorption and activation of O_(2),accelerating reduction kinetics from O_(2) to H_(2)O_(2).This work presents a re-liable strategy to design excellent photocatalysts by rationally modulating electronic structures and active sites for accelerating photo-generated charge carriers transfer and surface reaction kinetics.展开更多
The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportio...The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst design.Herein,a Ni2+-loaded porous poly(ionic liquids)(PIL)precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing temperature.The catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO_(2)into CO.Operando Ni K-edge X-ray absorption near-edge structure(XANES)spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and NPs.The charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active sites.In the electroreduction of CO_(2),the coexistence of Ni SAs and NPs strengthened the CO_(2)activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO_(2)→*COOH step,and therefore promoted the catalysis efficiency.展开更多
The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding p...The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(Fe_(SA)-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h^(+),and the H_(2)O_(2)generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.展开更多
Platinum-based(Pt)catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide(CO)poisoning.Overcoming this poisoning deactivation of Pt-based catalysts while enhancing...Platinum-based(Pt)catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide(CO)poisoning.Overcoming this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity,selectivity,and durability remains a major challenge.Herein,we propose a strategy to enhance the CO tolerance of Pt clusters(Pt_n)by introducing neighboring functionalized vip single atoms(such as Fe,Co,Ni,Cu,Sb,and Bi).Among them,antimony(Sb)single atoms(SAs)exhibit significant performance enhancement,achieving 99%CO selectivity and 33.6%CO_(2)conversion at 450℃,Experimental results and density functional theory(DFT)calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters,leading to optimal 5d electron redistribution in Pt clusters compared to other functionalized vip single atoms.The redistribution of 5d electrons weaken both theσdonation andπbackdonation interactions,resulting in a weakened bond strength with CO and enhancing catalyst activity and selectivity.In situ environmental transmission electron microscopy(ETEM)further demonstrates the exception thermal stability of the catalyst,even under H_(2)at 700℃.Notably,the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts,including Co/CeO_(2),Ni/CeO_(2),Pt/Al_(2)O_(3),and Pt/CeO_(2)-C.This finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts,making their broader applications in various industrial catalysts.展开更多
Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow...Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow-loading of Ru single atoms(0.42 wt%)into Mn_(2)O_(3)matrix(0.4%Ru-Mn_(2)O_(3))greatly boosts its catalytic activity for the aerobic oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA).The FDCA productivity over the 0.4%Ru-Mn_(2)O_(3)(5.4 mmol_(FDCA)g_(cat)h^(-1))is 4.9 times higher than the Mn_(2)O_(3).Especially,this FDCAproductivity is also significantly higher than that of existing Ru and Mn-based catalysts.Experimental and theoretical investigations discovered that the Ru single atom facilitated the formation of oxygen vacancy(O_(v))in the catalyst,which synergistically weakened the Mn-O bond and promoted the activation of O_L.The co-presence of Ru single atoms and O_(v)also promote the adsorption and activation of both O_(2)and HMF.Consequently,the dehydrogenation reaction energy barrier of the rate-determining step was reduced via both the O_L and chemisorbed O_(2)dehydrogenation pathways,thus boosting the catalytic oxidation reactions.展开更多
The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challen...The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challenging.Herein,N-doped carbon(N-C)anchored atomically dispersed Ni-N_(3)site with proximity defects(Ni-N_(3)D)induced by Te atoms doping is reported.Benefitting from the inductive effect of proximity defect,the Ni-N_(3)D/Te-N-C catalyst performs excellent ORR and HER performance in alkaline and acid condition.Both in situ characterization and theoretical calculation reveal that the existence of proximity defect effect is conducive to lower rate-determining-step energy barrier of ORR and HER,thus accelerating the multielectron reaction kinetics.This work paves a novel strategy for constructing highactivity bifunctional SACs by defect engineering for development of sustainable energy.展开更多
The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the ...The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.展开更多
Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolu...Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.展开更多
This study presents an achievement of laser cooling of alkaline-earth atoms in the Chinese Space Station’s strontium(Sr)atomic space optical clock.The system’s core components,physical unit,optical unit,and electric...This study presents an achievement of laser cooling of alkaline-earth atoms in the Chinese Space Station’s strontium(Sr)atomic space optical clock.The system’s core components,physical unit,optical unit,and electrical unit,have a total volume of 306 L and a total mass of 163.8 kg.These compact and robust units can overcome mechanical vibrations and temperature fluctuations during space launch.The laser sources of the optical unit are composed of diode lasers,and the injection locking of slave lasers is automatically performed by a program.In the experiment,a blue magneto-optical trap of cold atoms was achieved,with the atom numbers estimated to be approximately(1.50±0.13)×10^(6) for 87Sr and(8.00±0.56)×10^(6) for 88Sr.This work establishes a foundation for atomic confinement and high-precision interrogation in space-based optical clocks and expands the frontiers of cold atom physics in microgravity.展开更多
Solar-driven water splitting has emerged as a promising route for sustainable hydrogen generation,however,developing broad-spectrum responsive photocatalysts remains a challenge for achieving efficient solar-to-hydrog...Solar-driven water splitting has emerged as a promising route for sustainable hydrogen generation,however,developing broad-spectrum responsive photocatalysts remains a challenge for achieving efficient solar-to-hydrogen conversion.Here,we demonstrate a g-C_(3)N_(4)-based(UCN)catalyst with dispersed Ag single atoms(Ag SAs)and Ag nanoparticles(Ag NPs)for synergistically broad-spectrum photocatalytic hydrogen evolution.Experimental and theoretical results reveal that both Ag SAs and Ag NPs serve as active sites,with the Schottky junction between Ag NPs and g-C_(3)N_(4)effectively promoting charge separation,while Ag NPs induce localized surface plasmon resonance,extending the light response range from visible to near-infrared regions.The optimized catalyst Ag-UCN-3 exhibits a hydrogen evolution rate as high as 22.11 mmol/g/h and an apparent quantum efficiency(AQE)of 10.16%under 420 nm light illumination.Notably,it still had a high hydrogen evolution rate of 633.57μmol/g/h under 700 nm irradiation.This work unveils dual active sites engineering strategy that couples Ag SAs and Ag NPs with plasma and hot electrons,offering a new strategy for designing high-performance solar-driven energy systems.展开更多
Plastics are ubiquitous in human life and pose certain hazards to the environment and human body.The increasing amount of CO_(2)in the atmosphere will lead to the greenhouse effect.Therefore,it is urgent to treat micr...Plastics are ubiquitous in human life and pose certain hazards to the environment and human body.The increasing amount of CO_(2)in the atmosphere will lead to the greenhouse effect.Therefore,it is urgent to treat microplastic waste and CO_(2)by using environmentally friendly and efficient technologies.In this work,we developed an efficient photoelectrocatalytic system composed of Ni single atoms(Ni SAs)supported by P,N-doped amorphous NiFe_(2)O_(4)(Ni SAs/A-P-N-NFO)as anode and Ag nanoparticles(Ag NPs)supported by CuO/Cu_(2)O nanocubes(Ag NPs@CuO/Cu_(2)O NCs)as cathode for microplastic oxidation and CO_(2)reduction.The Ni SAs/A-P-N-NFO was synthesized by calcination-H_(2)reduction method,and it achieved a Faraday efficiency of 93%for the oxidation reaction of poly(ethylene terephthalate)(PET)solution under AM 1.5 G light.As a photocathode,the synthesized Ag NPs@CuO/Cu_(2)O NCs was utilized to reduce CO_(2)to ethylene and CO at 1.5 V vs.RHE with selectivity of 42%and 55%,respectively.This work shows that the photoelectrocatalysis,as an environmentally friendly technology,is a feasible strategy for reducing the environmental and biological hazards of light plastics,as well as for efficient CO_(2)reduction.展开更多
Hydrogen storage plays a pivotal role in the hydrogen industry,yet its current status presents a bottle-neck.Diverse strategies have emerged in recent years to address this challenge.MgH_(2) has stood out as a promisi...Hydrogen storage plays a pivotal role in the hydrogen industry,yet its current status presents a bottle-neck.Diverse strategies have emerged in recent years to address this challenge.MgH_(2) has stood out as a promising solid-state hydrogen storage material due to its impressive gravimetric and volumetric hydrogen density,but its practical application is hampered by elevated thermal stability and sluggish kinetics.In this study,we introduce a solution by synthesizing Pd metallene through a one-pot solvothermal method,revealing a distinctive highly curved lamellar structure with a thickness of around 1.6 nm.Incorporating this Pd metallene into MgH_(2) results in a composite system wherein the starting dehydrogenation temperature is significantly lowered to 439 K and complete dehydrogenation occurs at 583 K,releasing 6.14 wt.%hydrogen.The activation energy of dehydrogenation for MgH_(2) was reduced from 170.4 kJ mol^(-1) to 79.85 kJ mol^(-1) after Pd metallene decoration.The enthalpy of dehydrogenation of the MgH_(2)-10 wt.%Pd sample was calculated to be 73 kJ mol^(-1) H_(2)^(-1) and decreased by 4.4 kJ mol^(-1) H_(2)^(-1) from that of dehydrogenation of pure MgH_(2)(77.4 kJ mol^(-1) H_(2)-1).Theoretical calculations show that the average formation energy and average adsorption energy of hydrogen vacancies can be significantly reduced in the presence of both Pd clusters and Pd single atoms on the surface of MgH_(2)/Mg,respectively.It suggests that the synergistic effect of in situ formed Pd single atoms and clusters significantly improves the hydrogenation and dehydrogenation kinetics.The identified active sites in this study hold potential as references for forthcoming multi-sized active site catalysts,underscoring a significant advancement toward resolving hydrogen storage limitations.展开更多
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(Nos.52070103 and 22102102)Zhejiang Provincial Natural Science Foundation of China(Nos.LY21E090004 and LQ22B050004)+1 种基金Ningbo Public Welfare Science and Technology Program(No.2021S025)Ningbo Youth Leading Talent Project(No.2024QL038).
文摘Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.
基金supported by the National Natural Science Foundation of China (Grant Nos. 42188101, 42274211, 41974170, 42374184, 42122032, and 41974196)the Chinese Academy of Sciences (Grant Nos. QYZDJSSW-JSC028, XDA15052500, XDA17010301, and XDB41000000)+3 种基金the CNSA (Grant No. D050103)the Specialized Research Fund for State Key Laboratories of Chinathe Specialized Research Fund for Laboratory of Geospace Environment of the University of Science and Technology of Chinasupported by the International Space Science Institute (ISSI) in Bern and Beijing through the ISSI/ISSI-BJ International Team Project titled “Understanding the Mars Space Environment Through Multi-Spacecraft Measurements” (ISSI Team Project No. 23-582 and ISSI-BJ Team Project No. 58)
文摘Atmospheric escape plays a critical role in shaping the long-term climate evolution of Mars.Among the various escape mechanisms,energetic neutral atoms(ENAs)generated through charge exchange between solar wind ions and exospheric neutrals serve as an important diagnostic for ion-neutral interactions and upper atmospheric loss.This study presents direct observations of hydrogen ENAs(H-ENAs)on the dayside of Mars by using the Mars Ion and Neutral Particle Analyzer(MINPA)onboard China’s Tianwen-1 orbiter.By analyzing H-ENA data during a coronal mass ejection and a stream interaction region from December 29,2021,to January 1,2022,and comparing these data with MAVEN/SWIA(Mars Atmosphere and Volatile EvolutioN/Solar Wind Ion Analyzer)solar wind measurements,we examine the temporal evolution of H-ENA flux and the associated sputtered escape of atmospheric constituents.The observed H-ENA velocity is consistent with upstream solar wind ions,and the H-ENA-to-ion intensity ratio is used to infer variations in exospheric density,revealing a delayed response to enhanced solar wind activity.Penetrating H-ENA intensities reach up to 5.3×10^(6)s^(−1) cm^(−2),with energy fluxes on the order of(0.5-8.1)×10^(−3) mW/m^(2).The estimated oxygen sputtered escape rate driven by penetrating H-ENAs ranges from 5.5×10^(23)s^(−1) to 5.2×10^(24)s^(−1),comparable to or exceeding previous estimates based on penetrating ions.The findings highlight the need for low-altitude H-ENA observations to better quantify their atmospheric interactions and refine our understanding of nonthermal escape processes at Mars.
基金supported by the Department of Education of Liaoning Province(Grant Nos.LJKZ1015,LJ2020005,LJKZZ20220120)the Natural Science Foundation of Liaoning Province(Grant Nos.2020-BS-234,2021-MS-317,2022-MS-372)the Program of Liaoning Bai Qian Wan Talents Program(Grant No.2021921096)。
文摘Conversion between different types of entangled states is an interesting problem in quantum mechanics.But research on the conversion between the Greenberger-Horne-Zeilinger(GHZ)state and Knill-Laflamme-Milburn(KLM)state in an atomic system has not been reported.In this paper,we propose a scheme to realize the interconversion(one-step)between the GHZ state and KLM state with Rydberg atoms.By utilizing Rydberg-mediated interactions,we simplify the system.By combining a Lie-transform-based pulse design,the evolution path is built up to realize interconversion of the GHZ state and KLM state.The numerical simulation result shows that the present scheme is robust against decoherence and operational imperfection.
基金the National Natural Science Foundation of China(Nos.52100032 and 52350005)the Basic and Applied Basic Research Project of Guangzhou(Nos.2024A04J3679, 2024A03J0088)+2 种基金the Introduced Innovative Research and Development Team Project under the“The Pearl River Talent Recruitment Program”of Guangdong Province(No.2019ZT08L387)the Special Basic Research Fund for Central Public Research Institutes of China(No.PMzx703-202204-152)the Research Fund Program of Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology(No.2023B1212060016).
文摘The introduction of metal single atoms(SAs)and nanoparticles(NPs)are effective approaches to mod-ify electronic configuration of semiconductors,whereas recognizing the synergistic effects of metal SAs and NPs are still challenging in photocatalytic water purification.Herein,a general strategy is achieved by subsequentially anchoring Fe SAs and Fe NPs in graphitic carbon nitride.The modification of Fe SAs and Fe NPs improves the energy band structure and constructs a gradient charge polarization,directly expanding the optical absorption range and facilitating the efficient separation and transfer of charge car-riers.With the assistance of the gradient charge polarization,pollutants are readily oxidated by h+,which strengthens the continuous reduction of O2 on Fe NPs for pollutant oxidation in water.This work rein-forces the synergistic effect of SAs and NPs on electronic configuration modulation at the atomic level,which exhibits great potential for the construction of an efficient and sustainable water purification sys-tem.
文摘The photocatalytic oxidation of methane to methanol using molecule oxygen directly is an attractive catalytic reaction,but designing catalysts to avoid over-oxidation remains a significant challenge.Herein,Cu single-atom anchored on the defective carbon nitride structure(Cu SA/Def-CN)is designed for selective photocatalytic oxidation of methane into methanol using O_(2) under mild conditions.The Cu SA/Def-CN catalyst exhibits a high methanol selectivity of 92.8%under optimized conditions.Mechanistic studies reveal a synergistic effect between Def-CN and Cu SA,where Def-CN is responsible for the in-situ generation of hydrogen peroxide,which is subsequently decomposed by the Cu SA sites to produce·OH radicals that play a key role in the rate-determining step of methane activation to form methanol.Additionally,the presence of Cu SA not only enhances the electron-hole separation efficiency and improves the transfer of the photo-generated charges,but also increases the number of active sites for methane adsorption and activation.These insights provide valuable guidance for designing efficient catalysts for the highly selective photocatalytic oxidation of methane to methanol.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. U20A2075,11803072,and 12374467)the Innovation Program for Quantum Science and Technology (Grant No. 2021ZD0300902)the Hubei Provincial Science and Technology Major Project (Grant No. ZDZX2022000004)。
文摘We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loading a green MOT of ^(171)Yb atoms, the phase shift is obtained with a two-color Mach–Zehnder interferometer by means of ±45 MHz detuning with respect to the ^(1)S_(0)–^(1)P_(1) transition. We measured a phase shift of about 100 mrad corresponding to an atom count of around 5 × 10^(5). This demonstrates that it is possible to obtain the number of atoms without direct destructive measurement compared with the absorption imaging method. This scheme could be an important approach towards a high-precision lattice clock for clock operation through suppression of the impact of the Dick effect.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174115 and 91836103)。
文摘We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(No.52488201)the National Natural Science Foundation of China(No.52276213)+1 种基金the Key Research and Development Program of Shaanxi Province(No.2024GX-YBXM-459)the Fundamental Research Funds for the Central Universities.
文摘Photosynthesis of hydrogen peroxide(H_(2)O_(2))from H_(2)O and O_(2)is considered to be a promising approach.However,limited to the rapid recombination of photo-generated carriers and sluggish kinetics of O_(2)re-duction to H_(2)O_(2),it is a challenge for polymeric photocatalysts to achieve efficient photocatalytic H_(2)O_(2) production.Herein,Ag single atoms and nitrogen defects decorated carbon nitride(Ag@MCT)are con-structed through self-assembly and pyrolysis methods.The optimized photocatalyst displays exceptional performance in pure water,with an H_(2)O_(2) production rate of as high as 528.4μmol g^(-1) h^(-1) and an apparent quantum yield for H_(2)O_(2)production of 4.5%at 420 nm.Experimental and theoretical results reveal that the Ag atomic sites act as electron mediators that promote the capture and transfer of photo-generated charge carriers,while nitrogen defects as electron collectors and reaction sites to enhance the adsorption and activation of O_(2),accelerating reduction kinetics from O_(2) to H_(2)O_(2).This work presents a re-liable strategy to design excellent photocatalysts by rationally modulating electronic structures and active sites for accelerating photo-generated charge carriers transfer and surface reaction kinetics.
基金National Natural Science Foundation of China(grants 22072065,22178162,and 22222806)Distinguished Youth Foundation of Jiangsu Province(grant BK20220053)Six talent peaks project in Jiangsu Province(grant JNHB-035)。
文摘The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst design.Herein,a Ni2+-loaded porous poly(ionic liquids)(PIL)precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing temperature.The catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO_(2)into CO.Operando Ni K-edge X-ray absorption near-edge structure(XANES)spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and NPs.The charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active sites.In the electroreduction of CO_(2),the coexistence of Ni SAs and NPs strengthened the CO_(2)activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO_(2)→*COOH step,and therefore promoted the catalysis efficiency.
基金financially supported by the National Natural Science Foundation of China(Nos.52100032 and 52350005)the Basic and Applied Basic Research Project of Guangzhou(Nos.2024A04J3679 and 2024A03J0088)+2 种基金the Introduced Innovative Research and Development Team Project under the“The Pearl River Talent Recruitment Program”of Guangdong Province(No.2019ZT08L387)the Opening Project of Shanxi Province Key Laboratory of Chemical Process Intensification,North University of China(No.2023-HOCE10)the National College Students’Innovation and Entrepreneurship Training Program(No.202211078135)
文摘The introduction of metal single atoms(SAs)into semiconductors can effectively optimize their electronic configuration and enhance their photocatalytic properties.Therefore,it is crucial to clarify the corresponding principles and photocatalytic mechanisms for efficient and sustainable photocatalytic water remediation systems.Herein,a promising Fe single-atom photocatalyst(Fe_(SA)-CN)is obtained by anchoring Fe SAs in graphitic carbon nitride using a simple calcination strategy.Characterization and experimental results indicate that the modification of Fe SAs not only introduces a doping energy level,but also changes the valence band position,which expands the light absorption range,enhances the reduction ability of photogenerated electrons,and improves the separation and transfer of photogenerated charge carriers.Subsequently,contaminants adsorbed on the FeSA-CN surface trigger their oxidation removal by h^(+),and the H_(2)O_(2)generated via two-electron direct reductions is converted in situ into OH by self-Fenton reaction for the synergistic contaminant degradation.In summary,FeSA-CN offers a promising pathway for single-atom photocatalysts in water remediation because of outstanding contamination removal efficiency,adaptability,and stability.
基金financially supported by the Shanghai RisingStar Program(No.23QA1403700)the National Natural Science Foundation of China(NSFC,Grant No.U2230102)+1 种基金the sponsored by National Key Research and Development Program of China(No.2021YFB3502200)the Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University.
文摘Platinum-based(Pt)catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide(CO)poisoning.Overcoming this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity,selectivity,and durability remains a major challenge.Herein,we propose a strategy to enhance the CO tolerance of Pt clusters(Pt_n)by introducing neighboring functionalized vip single atoms(such as Fe,Co,Ni,Cu,Sb,and Bi).Among them,antimony(Sb)single atoms(SAs)exhibit significant performance enhancement,achieving 99%CO selectivity and 33.6%CO_(2)conversion at 450℃,Experimental results and density functional theory(DFT)calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters,leading to optimal 5d electron redistribution in Pt clusters compared to other functionalized vip single atoms.The redistribution of 5d electrons weaken both theσdonation andπbackdonation interactions,resulting in a weakened bond strength with CO and enhancing catalyst activity and selectivity.In situ environmental transmission electron microscopy(ETEM)further demonstrates the exception thermal stability of the catalyst,even under H_(2)at 700℃.Notably,the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts,including Co/CeO_(2),Ni/CeO_(2),Pt/Al_(2)O_(3),and Pt/CeO_(2)-C.This finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts,making their broader applications in various industrial catalysts.
基金financially supported by National Natural Science Foundation of China(22208137 and 22068022)Yunnan Fundamental Research Projects(202101BE070001-033,202401AT070825,202201BE070001007 and 202301AV070005)。
文摘Concurrent activation of lattice oxygen(O_L)and molecular oxygen(O_(2))is crucial for the efficient catalytic oxidation of biomass-derived molecules over metal oxides.Herein,we report that the introduction of ultralow-loading of Ru single atoms(0.42 wt%)into Mn_(2)O_(3)matrix(0.4%Ru-Mn_(2)O_(3))greatly boosts its catalytic activity for the aerobic oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA).The FDCA productivity over the 0.4%Ru-Mn_(2)O_(3)(5.4 mmol_(FDCA)g_(cat)h^(-1))is 4.9 times higher than the Mn_(2)O_(3).Especially,this FDCAproductivity is also significantly higher than that of existing Ru and Mn-based catalysts.Experimental and theoretical investigations discovered that the Ru single atom facilitated the formation of oxygen vacancy(O_(v))in the catalyst,which synergistically weakened the Mn-O bond and promoted the activation of O_L.The co-presence of Ru single atoms and O_(v)also promote the adsorption and activation of both O_(2)and HMF.Consequently,the dehydrogenation reaction energy barrier of the rate-determining step was reduced via both the O_L and chemisorbed O_(2)dehydrogenation pathways,thus boosting the catalytic oxidation reactions.
基金financially supported by the National Natural Science Foundation of China(22478432,22108306,22178388)Taishan Scholars Program of Shandong Province(tsqn201909065)+2 种基金Shandong Provincial Natural Science Foundation(ZR2024JQ004)Innovation Fund Project for Graduate Student of China University of Petroleum(East China)the Fundamental Research Funds for the Central Universities(No.25CX04020A)。
文摘The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challenging.Herein,N-doped carbon(N-C)anchored atomically dispersed Ni-N_(3)site with proximity defects(Ni-N_(3)D)induced by Te atoms doping is reported.Benefitting from the inductive effect of proximity defect,the Ni-N_(3)D/Te-N-C catalyst performs excellent ORR and HER performance in alkaline and acid condition.Both in situ characterization and theoretical calculation reveal that the existence of proximity defect effect is conducive to lower rate-determining-step energy barrier of ORR and HER,thus accelerating the multielectron reaction kinetics.This work paves a novel strategy for constructing highactivity bifunctional SACs by defect engineering for development of sustainable energy.
文摘The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.
基金support from the European Union Horizon 2020 program(project HERMES,nr.952184)the Ministry of Education,Youth and Sports of the Czech Republic for supporting CEMNAT(LM2023037)+1 种基金Czech-NanoLab(LM2023051)infrastructures for providing ALD,SEM,EDX,XPS,TEM,and XRDCzech Science Foundation(project 23-08019X,EXPRO).
文摘Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB35010202)the National Natural Science Foundation of China(Grants No.62275268)。
文摘This study presents an achievement of laser cooling of alkaline-earth atoms in the Chinese Space Station’s strontium(Sr)atomic space optical clock.The system’s core components,physical unit,optical unit,and electrical unit,have a total volume of 306 L and a total mass of 163.8 kg.These compact and robust units can overcome mechanical vibrations and temperature fluctuations during space launch.The laser sources of the optical unit are composed of diode lasers,and the injection locking of slave lasers is automatically performed by a program.In the experiment,a blue magneto-optical trap of cold atoms was achieved,with the atom numbers estimated to be approximately(1.50±0.13)×10^(6) for 87Sr and(8.00±0.56)×10^(6) for 88Sr.This work establishes a foundation for atomic confinement and high-precision interrogation in space-based optical clocks and expands the frontiers of cold atom physics in microgravity.
文摘Solar-driven water splitting has emerged as a promising route for sustainable hydrogen generation,however,developing broad-spectrum responsive photocatalysts remains a challenge for achieving efficient solar-to-hydrogen conversion.Here,we demonstrate a g-C_(3)N_(4)-based(UCN)catalyst with dispersed Ag single atoms(Ag SAs)and Ag nanoparticles(Ag NPs)for synergistically broad-spectrum photocatalytic hydrogen evolution.Experimental and theoretical results reveal that both Ag SAs and Ag NPs serve as active sites,with the Schottky junction between Ag NPs and g-C_(3)N_(4)effectively promoting charge separation,while Ag NPs induce localized surface plasmon resonance,extending the light response range from visible to near-infrared regions.The optimized catalyst Ag-UCN-3 exhibits a hydrogen evolution rate as high as 22.11 mmol/g/h and an apparent quantum efficiency(AQE)of 10.16%under 420 nm light illumination.Notably,it still had a high hydrogen evolution rate of 633.57μmol/g/h under 700 nm irradiation.This work unveils dual active sites engineering strategy that couples Ag SAs and Ag NPs with plasma and hot electrons,offering a new strategy for designing high-performance solar-driven energy systems.
文摘Plastics are ubiquitous in human life and pose certain hazards to the environment and human body.The increasing amount of CO_(2)in the atmosphere will lead to the greenhouse effect.Therefore,it is urgent to treat microplastic waste and CO_(2)by using environmentally friendly and efficient technologies.In this work,we developed an efficient photoelectrocatalytic system composed of Ni single atoms(Ni SAs)supported by P,N-doped amorphous NiFe_(2)O_(4)(Ni SAs/A-P-N-NFO)as anode and Ag nanoparticles(Ag NPs)supported by CuO/Cu_(2)O nanocubes(Ag NPs@CuO/Cu_(2)O NCs)as cathode for microplastic oxidation and CO_(2)reduction.The Ni SAs/A-P-N-NFO was synthesized by calcination-H_(2)reduction method,and it achieved a Faraday efficiency of 93%for the oxidation reaction of poly(ethylene terephthalate)(PET)solution under AM 1.5 G light.As a photocathode,the synthesized Ag NPs@CuO/Cu_(2)O NCs was utilized to reduce CO_(2)to ethylene and CO at 1.5 V vs.RHE with selectivity of 42%and 55%,respectively.This work shows that the photoelectrocatalysis,as an environmentally friendly technology,is a feasible strategy for reducing the environmental and biological hazards of light plastics,as well as for efficient CO_(2)reduction.
基金the National Key R&D Program of China(No.2023YFB4005402)the National Natural Science Foundation of China(Nos.NSFC-NSAF U2330111,52071177)the Natural Science Foundation of Jiangsu province,China(No.BK20221473).
文摘Hydrogen storage plays a pivotal role in the hydrogen industry,yet its current status presents a bottle-neck.Diverse strategies have emerged in recent years to address this challenge.MgH_(2) has stood out as a promising solid-state hydrogen storage material due to its impressive gravimetric and volumetric hydrogen density,but its practical application is hampered by elevated thermal stability and sluggish kinetics.In this study,we introduce a solution by synthesizing Pd metallene through a one-pot solvothermal method,revealing a distinctive highly curved lamellar structure with a thickness of around 1.6 nm.Incorporating this Pd metallene into MgH_(2) results in a composite system wherein the starting dehydrogenation temperature is significantly lowered to 439 K and complete dehydrogenation occurs at 583 K,releasing 6.14 wt.%hydrogen.The activation energy of dehydrogenation for MgH_(2) was reduced from 170.4 kJ mol^(-1) to 79.85 kJ mol^(-1) after Pd metallene decoration.The enthalpy of dehydrogenation of the MgH_(2)-10 wt.%Pd sample was calculated to be 73 kJ mol^(-1) H_(2)^(-1) and decreased by 4.4 kJ mol^(-1) H_(2)^(-1) from that of dehydrogenation of pure MgH_(2)(77.4 kJ mol^(-1) H_(2)-1).Theoretical calculations show that the average formation energy and average adsorption energy of hydrogen vacancies can be significantly reduced in the presence of both Pd clusters and Pd single atoms on the surface of MgH_(2)/Mg,respectively.It suggests that the synergistic effect of in situ formed Pd single atoms and clusters significantly improves the hydrogenation and dehydrogenation kinetics.The identified active sites in this study hold potential as references for forthcoming multi-sized active site catalysts,underscoring a significant advancement toward resolving hydrogen storage limitations.
