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
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
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
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
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
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
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
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
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
Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machin...Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.展开更多
High-concentration single-atom doping remains a formidable challenge due to the propensity for single atoms to form clusters or aggregate at elevated concentrations.Herein,high-concentration (10.8 wt%) Zn singleatom-d...High-concentration single-atom doping remains a formidable challenge due to the propensity for single atoms to form clusters or aggregate at elevated concentrations.Herein,high-concentration (10.8 wt%) Zn singleatom-doped porous tubular g-C_(3)N_(4)(ZCN) was successfully obtained via a template-free,one-step calcination method,exhibiting excellent photocatalytic performance.The confinement of the pore walls suppresses the Zn atom'smigration and aggregation,enhancing the Zn single-atom stability.ZCN exhibited excellent photodegradation performance against tetracycline with outstanding stability.Moreover,ZCN displayed remarkable sterilization performance,achieving a 100%inactivation of Staphylococcus aureus within 90 min of visible-light exposure.Density functional theory calculations demonstrated that the Zn single-atom sites act as pivotal photocatalytic active sites,with the presence of Zn single atoms notably augmenting charge separation efficiency.This work provides a novel approach for managing photocatalytic efficiency through enlarging single-atom doping,offering an avenue for pollutant photodegradation and sterilization.展开更多
Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous Si...Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
In situ electron paramagnetic resonance(EPR)monitoring of the photocatalytic halogen atom transfer(XAT)reaction with organic amines has provided insights into the dynamic transformations of intermediates,including cat...In situ electron paramagnetic resonance(EPR)monitoring of the photocatalytic halogen atom transfer(XAT)reaction with organic amines has provided insights into the dynamic transformations of intermediates,including catalyst intermediate states,amine alkyl radicals,and the dehalogenation of halogenated hydrocarbons to form carbon-centered radicals.This approach facilitated the photocatalytic single-linear state oxygen-promoted halogen atom transfer quinoxalinone alkylation reaction.展开更多
Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on th...Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on the van der Waals potential based on quantum mechanics.Specifically,using the second-order perturbation theory in quantum mechanics,he derived a long-range attractive potential of the form−1/R6 between two widely separated atoms.Since individual atoms are non-polar,meaning their average dipole moments are zero,this interaction arises from fluctuations in the instantaneous electric dipole moments of the two atoms.展开更多
Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have re...Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.展开更多
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 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 (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 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.
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financial support from the National Key Research and Development Program of China(2018YFA0703400)the Fundamental Research Funds for the Provincial Universities of Zhejiang(GK239909299001021)+1 种基金the Ninth China Association for Science and Technology Youth Talent Lift Project Support Plan(KYZ015324002)the Changjiang Scholars Program of Chinese Ministry of Education。
文摘Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.
基金financially supported by the National Key Research and Development Program of China(No.2023YFF0612601)the Key Research and Development Program of Zhejiang Province(No.2023C02038)+2 种基金the Key Research and Development Program of Ningbo(No.2022Z178)China Construction Technology Research and Development Project(No.CSCEC-2021-Z-5)Zhejiang Provincial Natural Science Foundation of China(No.LQ23B010003)
文摘High-concentration single-atom doping remains a formidable challenge due to the propensity for single atoms to form clusters or aggregate at elevated concentrations.Herein,high-concentration (10.8 wt%) Zn singleatom-doped porous tubular g-C_(3)N_(4)(ZCN) was successfully obtained via a template-free,one-step calcination method,exhibiting excellent photocatalytic performance.The confinement of the pore walls suppresses the Zn atom'smigration and aggregation,enhancing the Zn single-atom stability.ZCN exhibited excellent photodegradation performance against tetracycline with outstanding stability.Moreover,ZCN displayed remarkable sterilization performance,achieving a 100%inactivation of Staphylococcus aureus within 90 min of visible-light exposure.Density functional theory calculations demonstrated that the Zn single-atom sites act as pivotal photocatalytic active sites,with the presence of Zn single atoms notably augmenting charge separation efficiency.This work provides a novel approach for managing photocatalytic efficiency through enlarging single-atom doping,offering an avenue for pollutant photodegradation and sterilization.
文摘Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
基金Project supported by the Domestic Visiting Fellows Program of Hangzhou Normal University(No.4095C5022521106)。
文摘In situ electron paramagnetic resonance(EPR)monitoring of the photocatalytic halogen atom transfer(XAT)reaction with organic amines has provided insights into the dynamic transformations of intermediates,including catalyst intermediate states,amine alkyl radicals,and the dehalogenation of halogenated hydrocarbons to form carbon-centered radicals.This approach facilitated the photocatalytic single-linear state oxygen-promoted halogen atom transfer quinoxalinone alkylation reaction.
文摘Translator’s Note:Shou Chin Wang(Wang Shoujing)was one of the few Chinese physicists who made significant contributions to the early development of quantum mechanics.One of his representative works is the study on the van der Waals potential based on quantum mechanics.Specifically,using the second-order perturbation theory in quantum mechanics,he derived a long-range attractive potential of the form−1/R6 between two widely separated atoms.Since individual atoms are non-polar,meaning their average dipole moments are zero,this interaction arises from fluctuations in the instantaneous electric dipole moments of the two atoms.
基金supported by the National Key R&D Program of China(2024YFB4106400)National Natural Science Foundation of China(22209200,52302331)。
文摘Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.
