Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer e...Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.展开更多
Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient ...Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.展开更多
Surface acoustic wave(SAW)resonators offer distinct advantages for coupling to semiconductor qubits,including low loss,high stability,and compatibility with magnetic fields.However,the integration of SAW resonators wi...Surface acoustic wave(SAW)resonators offer distinct advantages for coupling to semiconductor qubits,including low loss,high stability,and compatibility with magnetic fields.However,the integration of SAW resonators with double quantum dots(DQDs)that host charge and spin qubits remains largely unexplored.In this work,we propose a flip-chip architecture that enables three-dimensional integration of a semiconductor DQD with a SAW resonator.Taking experimental feasibility into account,we estimate the coupling strength between a DQD and a SAW resonator.The results suggest that the strong coupling regime can be reached in our design.This study provides theoretical insight and practical guidance for experimental exploration of phonon–electron coupling in hybrid SAW-DQD quantum systems.展开更多
Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demons...Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.展开更多
Silicone rubber(SR)exhibits superior breathability and high-temperature resistance.However,SR is prone to degradation under extreme heat or combustion,limiting its effectiveness in mitigating secondary hazards.In this...Silicone rubber(SR)exhibits superior breathability and high-temperature resistance.However,SR is prone to degradation under extreme heat or combustion,limiting its effectiveness in mitigating secondary hazards.In this study,phosphate glass powder was used to calcinate zinc borate,lanthanum oxide,and cerium oxide.Methylphenyl polysiloxane was then grafted onto the surface of the glass powder,resulting in the modified pow-ders designated as Methylphenyl polysiloxane-grafted zinc borate-modified phosphate glass powder(GF-ZnBM),Methylphenyl polysiloxane-grafted lanthanum oxide-modified phosphate glass powder(GF-LaM),and Methylphenyl polysiloxane-grafted cerium oxide-modified phosphate glass powder(GF-CeM).The modified powders were sub-sequently incorporated into silicone rubber composites to enhance the ceramicization capability of silicone rubber at high temperatures.Specifically,GF-CeM and GF-LaM significantly increased the limiting oxygen index(LOI)to 33%and reduced the tendency for combustion propagation.Additionally,GF-CeM notably contributed to enhancing ceramicization strength.The presence of cerium oxide helps in the melting of the glass powder and enhances its adhesion to the silicone rubber matrix.SR/ZnB-GF exhibited the lowest activation energy among the tested composites,along with the best protective capability.The inclusion of modified glass powder has a minor impact on the rheological properties,indicating that the composite retains its ability to flow and deform under stress.This confirms that the material remains flexible under normal conditions and forms a ceramic structure when heated,thereby exhibiting self-supporting properties.This study provides a practical methodology for the targeted modification of glass powders,thereby further enhancing the fire safety of silicone-based composites.展开更多
In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-dept...In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry.Typically,the isotropy of a specific facet provides a perfect support for studying heteroatom doping.Herein,this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals.The presence of iron not only modifies the electronic structure of lithium tantalate,improving its light absorption capacity,but also functions as an active site for the nitrogen adsorption and activation.The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95μg cm^(−2)h^(−1),which is three times higher than that of undoped lithium tantalate.The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating.This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.展开更多
Under submerged conditions, compared with traditional self-excited oscillating pulsed waterjets(SOPWs), annular fluid-enhanced self-excited oscillating pulsed waterjets(AFESOPWs) exhibit a higher surge pressure throug...Under submerged conditions, compared with traditional self-excited oscillating pulsed waterjets(SOPWs), annular fluid-enhanced self-excited oscillating pulsed waterjets(AFESOPWs) exhibit a higher surge pressure through self-priming. However, their pressure frequency and cavitation characteristics remain unclear, resulting in an inability to fully utilize resonance and cavitation erosion to break coal and rock. In this study, high-frequency pressure testing, high-speed photography, and large eddy simulation(LES) are used to investigate the distribution of the pressure frequency band, evolution law of the cavitation cloud, and its regulation mechanism of a continuous waterjet, SOPW, and AFESOPW. The results indicated that the excitation of the plunger pump, shearing layer vortex, and bubble collapse corresponded to the three high-amplitude frequency bands of the waterjet pressure. AFESOPWs have an additional self-priming frequency that can produce a larger amplitude under a synergistic effect with the second high-amplitude frequency band. A better cavitation effect was produced after self-priming the annulus fluid, and the shedding frequency of the cavitation clouds of the three types of waterjets was linearly related to the cavitation number. The peak pressure of the waterjet and cavitation erosion effect can be improved by modulating the waterjet pressure oscillation frequency and cavitation shedding frequency.展开更多
The laser-assisted manufacturing technology has significant advantages in meeting various demands such as complex structures,functional integration,customized devices,and cost-effectiveness,which makes it a highly att...The laser-assisted manufacturing technology has significant advantages in meeting various demands such as complex structures,functional integration,customized devices,and cost-effectiveness,which makes it a highly attractive option for fabricating sensors.In this review,the latest advancements and strategies in intelligent sensor development through laser processing were surveyed and outlined following the interaction of laser and materials.Laser-assisted manufacturing technologies have been extensively applied in materials science and device processing.Firstly,laser technology can be utilized in a wide range of materials,encompassing carbon-based materials,metals,and metallic oxides.In the field of device scale processing,laser manufacturing is widely used in micro/nano structures,planar device construction,and stereoscopic electronic devices such as cutting,engraving,and lithography.Additionally,laser technology provides robust support for sensor applications,covering fields such as pressure sensing,temperature sensing,gas sensing,and biosensors.Furthermore,laser considerably serves in real application areas such as multifunctional sensing systems,actuators,and robots.The widespread application of laser manufacturing technology in sensor platform fabrication offers effective solutions for realizing the miniaturization,multifunctionality,and integration of sensors.展开更多
Infrared radiation(IR)ceramics have been recognized as energy-saving materials for high-temperature industry due to excellent IR performance.However,for conventional IR ceramics,low emissivity in partial band and emis...Infrared radiation(IR)ceramics have been recognized as energy-saving materials for high-temperature industry due to excellent IR performance.However,for conventional IR ceramics,low emissivity in partial band and emissivity degradation during high-temperature service restricted the practical application.Herein,we integrated broad-band high emissivity and slow degradation rate in novel high-entropy perovskite ceramics:La(Al_(0.2)Co_(0.2)Fe_(0.2)Ni_(0.2)Cr_(0.2))O_(3−δ)(HE-1) and La(Al_(0.2)Co_(0.2)Fe_(0.2)Ni_(0.2)Mn_(0.2))O_(3−δ)(HE-2).Specifically,the high-energy ceramic HE-1&HE-2 displayed high emissivity of 0.94/0.90 and 0.90/0.95 in the broad-band of near/mid-infrared(0.76–14µm).This excellent IR performance can be attributed to impurity energy level absorption,free carrier absorption,and lattice vibration absorption.During high-temperature service,these high-entropy ceramics have much slower emissivity degradation rate than conventional IR ceramic,because of hysteresis diffusion effect.Additionally,energy-saving ratios of 17.70%and 10.77%were realized by heating water with porous burner containing HE-1 and HE-2 coating respectively,due to enhanced heat radiation in systems.Thus,these high-entropy IR ceramics have significant application potential for long-term energy-saving in high-temperature industry.展开更多
Rational design of porous metal oxide films that serve as not only the scaffolds for light absorbers but also the transfer layer of photo generated charges is essential for fabricating highly efficient photoanodes for...Rational design of porous metal oxide films that serve as not only the scaffolds for light absorbers but also the transfer layer of photo generated charges is essential for fabricating highly efficient photoanodes for photoelectrochemical(PEC)hydrogen generation.In this work,w report a facile one-step pyrolysis method which can convert Zn-based MOF to porous ZnO(m-ZnO)with rough surface and abundant oxygen vacancies(O_(v)).When incorporating core-shell quantum dots(QDs)as the light absorbers,the obtained photoanodes(m-ZnO@QDs)achieved outstanding PEC performance for hydrogen generation,exhibiting 1.6 times and 5.8 times higher saturated photocurrent density(J_(sc))than thos of conventional TiO_(2)@QDs and ZnO@QDs photoanodes,respectively.Comprehensive optical and electrochemical measurements reveal tha the rough surface of m-ZnO can significantly improve the light-harvesting capacity of corresponding photoanodes through surface-enhanced light scattering.Moreover,the O_(v)in m-ZnO facilitate the interfacial transfer of photogenerated electrons.Our findings indicate that the MOF are valuable precursors for the preparation of porous films,offering a promising route to develop high-performance QDs-based PEC devices.展开更多
Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapi...Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapid,contactless,and environmentally benign operation,has emerged as a promising approach for precise liquid control.However,conventional magnetic strategies typically govern droplet movement on open surfaces,facing limitations such as restricted liquid volumes,uncertain flow paths,and inevitable evaporation,thereby constraining their broader practical applications.Recently,a variety of magneticdriven strategies have been developed to dynamically regulate liquids within enclosed spaces,especially through physicochemical mechanisms.These approaches provide efficient control over liquid behavior by leveraging magnetically induced chemical changes,structural deformations,and dragging motions,opening new opportunities for flexible and versatile fluid management.This review explores the design and mechanisms of magneto-responsive confined interfaces for the manipulation of nonmagnetic liquids,highlighting key advancements and potential applications including liquid valves,liquid mixing,liquid flow regulation,and liquid pumping.Finally,the existing challenges and future prospects in this field are presented.展开更多
Developing efficient electrocatalysts for the nitrate reduction reaction(NIRR)to ammonia is vital for environmental remediation and sustainable ammonia synthesis.Metal-oxide-based single-atom catalysts(SACs)offer atom...Developing efficient electrocatalysts for the nitrate reduction reaction(NIRR)to ammonia is vital for environmental remediation and sustainable ammonia synthesis.Metal-oxide-based single-atom catalysts(SACs)offer atomic-scale efficiency,yet unclear anchoring strategies for single metal sites hinder their rational design.This study systematically explored the effects of surface-loading and latticedoping strategies on anchoring transition,rare-earth,and main-group metal atoms onto Co_(3)O_(4)via the synergy of machine learning and density functional theory calculations.Through a comprehensive assessment of stability,catalytic activity,and electronic structures,it is discovered that lattice-doping enhances SACs stability by firmly anchoring metal atoms on Co sites,while surface-loading significantly boosts catalytic activity for the NIRR.Calculations predicted that Al,Ir,Rh,and Mo sites anchored through the surface-loading strategy exhibited exceptional NIRR activity(the limiting potential for Al site can reaches-0.25 V versus the reversible hydrogen electrode),far surpassing many other configurations.To further decipher the underlying mechanisms,the machine learning algorithms,especially the treebased pipeline optimization tool model,revealed that SACs activity is highly correlated with the local environment of the active center,particularly its electronic and structural characteristics.This work establishes a new design paradigm for SACs,providing both theoretical guidelines for anchoring strategy selection and a predictive framework for efficient NIRR electrocatalysts.展开更多
Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composit...Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composite was evaluated using the degradation of rhodamine B(RhB)and tetracycline hydrochloride(TCH)under visible light.The results demonstrated that Ti_(3)C_(2)/BOC composite had higher photocatalytic activity than pure BOC.The optimum incorporation amount of Ti_(3)C_(2) was 2 wt%.The photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC at 10 min to 20 mg/L RhB was 97.6%,which was much higher than that of BOC(75.3%).Similarly,the photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC to 10 mg/L TCH at 30 min was 80.4%,which was higher than BOC(68.1%).In addition,the prepared 2 wt%-Ti_(3)C_(2)/BOC composite also maintained good stability even after four cycles.Electrochemical impedance spectroscopy(EIS),transient photocurrent response(IT)and ultraviolet-visible diffuse reflectance spectroscopy(UV-vis)confirmed that the photoelectrochemical properties of 2 wt%-Ti_(3)C_(2)/BOC composite were significantly improved.On the basis of analyzing the action mechanism of photocatalyst,it was pointed out that·O_(2)^(-)and h~+were the main active substances in the photodegradation of RhB and TCH by 2 wt%-Ti_(3)C_(2)/BOC.展开更多
Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to th...Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.展开更多
Electrocatalytic conversion of carbon dioxide(CO_(2))into formate offers a sustainable pathway to mitigate environmental degradation and the energy crisis.Tin(Sn)-based materials are promising electrocatalysts for CO_...Electrocatalytic conversion of carbon dioxide(CO_(2))into formate offers a sustainable pathway to mitigate environmental degradation and the energy crisis.Tin(Sn)-based materials are promising electrocatalysts for CO_(2)reduction to formate;however,their efficiency is limited by weak CO_(2)adsorption and activation,as well as sluggish reaction kinetics.In this work,we designed an intercrossing nanoporous Cu_(6)Sn_(5)/Sn intermetallic heterojunction via a scalable alloying-etching protocol.The resulting Cu_(6)Sn_(5)/Sn catalyst with abundant interfacial sites exhibited enhanced formate selectivity(60.79%)at−0.93 V versus the reversible hydrogen electrode(RHE),together with a high partial current density of 12.56 mA/cm^(2)and stable operation for 16 h.The modulated electronic structure of Cu_(6)Sn_(5)coupled with the robust interfacial interaction between Sn and Cu_(6)Sn_(5)synergistically promoted CO_(2)adsorption and activation,thereby improving CO_(2)reduction reaction(CO_(2)RR)performance.Electrochemical measurements and in situ infrared spectroscopy confirmed that the dual-phase interfaces facilitate H_(2)O decomposition and the generation of abundant*H intermediates,which in turn accelerate the protonation of CO_(2)to formate.This work highlights a scalable strategy for constructing intermetallic heterojunction catalysts that combine facile synthesis,reproducibility,and superior catalytic activity for CO_(2)RR.展开更多
Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a signific...Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a significant challenge.Herein,we report a vacancy occupation-triggered phase transition strategy to fabricate a core-shell 1T phase nanorod structure,which is composed of S-vacancies decorated MoS_(2)as the core,and N,P co-doped carbons as the shell(1T-MoS_(2)@NPC).The co-insertion of N and P dopants into MoS_(2)can occupy partial S-vacancies,triggering a phase transformation from the semiconducting 2H phase to the conducting 1T phase with a reduced energy barrier.Profiting from the strong coupling effect between N,P dopants and S-vacancies,the as-made 1T-MoS_(2)@NPC exhibits excellent electrocatalytic activity for both HER(η_(10)=148 m V)and OER(η_(10)=232 mV)in alkaline solution.Meanwhile,a low cell voltage of 1.62 V is needed to drive a current density of 10mA cm^(-2)in 1.0 M KOH electrolyte.The theoretical calculation results reveal that the S-vacancies decorated C atoms in the meta-position relative to N,P atoms represent the most active HER and OER sites,which synergistically upshift the d band center and balance the rate-determining step,thus ensuring the simultaneous optimization of adsorption free energy and electronic structure.This vacancy-occupation-derived phase transformation strategy caused by non-metallic doping may provide valuable guidance for enhancing the performance of alkaline water electrolysis.展开更多
Metal halide perovskites have rapidly emerged as outstanding semiconductors for laser applications.Surface plasmon resonances of metals offer a platform for improving the perovskite lasing properties of metal halide p...Metal halide perovskites have rapidly emerged as outstanding semiconductors for laser applications.Surface plasmon resonances of metals offer a platform for improving the perovskite lasing properties of metal halide perovskites by accelerating radiative recombination.However,the constraint on degrees of freedom of perovskite-metal interactions in two dimensions keeps us from getting a full picture of plasmon-involved carrier dynamics and reaching the optimum perovskite lasing performance.Here we report a strategy of synthesizing quantitative coassemblies of perovskite and metal nanocrystals for studying the effect of surface plasmons on carrier dynamics in depth and exploring plasmon-enhanced perovskite lasing performance.Within the coassembly,each metal nanocrystal supports localized surface plasmon resonances capable of accelerating radiative recombination of all adjacent perovskite nanocrystals in three dimensions.The quantitative coassemblies disclose the evolution of radiative and nonradiative recombination processes in perovskite nanocrystals with the plasmon modes,identifying an optimal metal nanocrystal content for fulfilling the highest radiative efficiency in perovskite nanocrystals.By virtue of accelerated radiative recombination,the coassemblies of perovskite and metal nanocrystals allowed for the construction of microlaser arrays with enhanced performance including low thresholds and ultrafast outputs.This work fundamentally advances the perovskite-metal systems for plasmonically enhancing perovskite optoelectronic performance.展开更多
The development of high-performance lithium-ion batteries(LIBs)hinges on searching for advanced anode materials with large specific capacities as well as high cycling stability.However,traditional graphite anodes have...The development of high-performance lithium-ion batteries(LIBs)hinges on searching for advanced anode materials with large specific capacities as well as high cycling stability.However,traditional graphite anodes have not met the demand for higher energy storage owing to the deficiency of low lithium storage capacity.In the current work,we focus on designing one composite anode material with multiscale porous(MP)structure and phosphorus(P)doping.The coupling effects of three-dimensional(3D)interconnected skeleton,hollow pore channels,and P doping can facilitate the electrolyte diffusion and the mass transfer,as well as accommodate the volume changes during lithiation/delithiation processes.As expected,the as-prepared MP-SiGeSnSbPAl composite exhibits superior lithium storage performance,achieving a specific capacity of 827.9 mAh/g after 150 cycles at 200 mA/g and maintaining the high capacity of 456.7 mAh/g after 400 cycles at 1 A/g.Contrastively,the corresponding surplus capacities are only 590.3 and 225.7 mAh/g for the non-doped counterparts,respectively.In particular,MP-SiGeSnSbPAl displays much more stable cycling performances under the measurement of high areal mass loading of~3 mg/cm^(2)and the full-cell tests with the lithium iron phosphate as the cathode.This work witnesses one scalable protocol for preparing multinary Si-based composite in terms of facile operation and high lithium storage performances.展开更多
Alkaline electrolytic hydrogen production has emerged as one of the most practical methods for industrial-scale hydrogen production.However,the initial hydrolysis dissociation in alkaline media impedes the hydrogen ev...Alkaline electrolytic hydrogen production has emerged as one of the most practical methods for industrial-scale hydrogen production.However,the initial hydrolysis dissociation in alkaline media impedes the hydrogen evolution reaction(HER)kinetics of commercial catalysts.To overcome this limitation,this study focuses on the development of a highly efficient electrocatalyst for alkaline HER.Ni-based intermetallic compounds exhibit remarkable catalytic activity for HER,with the NiMo alloy being among the most active catalysts in alkaline environments.Here,we designed and fabricated self-supported multiscale porous NiZn/NiMo intermetallic compounds on a metal foam substrate using a versatile dealloying method.The resulting electrode exhibits excellent HER activity,achieving an overpotential of just 204 mV at 1000 mA/cm^(2),and dem-onstrates robust long-term catalytic stability,maintaining performance at 100 mA/cm^(2) for 400 h in an alkaline electrolyte.Thesefindings underscore the potential of nanosized intermetallic compounds fabricated via a dealloying approach to deliver exceptional catalytic performance for alkaline water electrolysis.展开更多
In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.H...In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.However,these immobilization strategies inevitably compromise the interfacial mass diffusion and cause activity decline relative to the suspended catalyst.Here,we propose a binder-free surface immobilization strategy for fabrication of high-activity photocatalytic membrane.Through a simple dimethylformamide(DMF)treatment,the nanofibers of polyvinylidene fluoride membrane were softened and stretched,creating enlarged micropores to efficiently capture the photocatalyst.Subsequently,the nanofibers underwent shrinking during DMF evaporation,thus firmly strapping the photocatalyst microparticles on the membrane surface.This surface self-bounded photocatalytic membrane,with firmly bounded yet highly exposed photocatalyst,exhibited 4.2-fold higher efficiency in hydrogen peroxide(H_(2)O_(2))photosynthesis than the matrix-embedded control,due to improved O_(2)accessibility and H_(2)O_(2)diffusion.It even outperformed the suspension photocatalytic system attributed to alleviated H_(2)O_(2)decomposition at the hydrophobic surface.When adopted for UV-based water treatment,the photocatalytic system exhibited tenfold faster micropollutants photodegradation than the catalyst-free control and demonstrated superior robustness for treating contaminated tap water,lake water and secondary wastewater effluent.This immobilization strategy can also be extended to the fabrication of other photocatalytic membranes with diverse catalyst types and membrane substrate.Overall,our work opens a facile avenue for fabrication of high-performance photocatalytic membranes,which may benefit advanced oxidation water purification application and beyond.展开更多
基金supported by the National Natural Science Foundation of China(No.22278156)the Guangdong Special Support Program Project(No.2021JC060580)+1 种基金the Young Elite Scientists Sponsorship Program by CAST-Doctoral Student Special Plan,the China Scholarship Council Program(No.202406150148)the Natural Science Foundation of Guangdong Province(No.2023A1515011186).
文摘Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.
基金the financial support from the Shandong Province colleges and universities youth innovation technology plan innovation team project(2022KJ285)the Natural Science Foundation of Shandong Province(ZR2022QE076)+1 种基金the National Natural Science Foundation of China(52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(2023KJ104).
文摘Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.
基金supported by the National Natural Science Foundation of China(Grant Nos.12274401,12274397,12034018)the National Key Research and Development Program of China(Grant No.2022YFA1405900)the Natural Science Foundation of Jiangsu Province(Grant No.BK20240123)。
文摘Surface acoustic wave(SAW)resonators offer distinct advantages for coupling to semiconductor qubits,including low loss,high stability,and compatibility with magnetic fields.However,the integration of SAW resonators with double quantum dots(DQDs)that host charge and spin qubits remains largely unexplored.In this work,we propose a flip-chip architecture that enables three-dimensional integration of a semiconductor DQD with a SAW resonator.Taking experimental feasibility into account,we estimate the coupling strength between a DQD and a SAW resonator.The results suggest that the strong coupling regime can be reached in our design.This study provides theoretical insight and practical guidance for experimental exploration of phonon–electron coupling in hybrid SAW-DQD quantum systems.
基金financially supported by the Natural Science Foundation of Shandong Province (No.ZR2022QE076)the National Natural Science Foundation of China (No.52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China (No.2023KJ104)。
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.
基金supported by National Natural Science Foundation of China(51991352 and 51874266).
文摘Silicone rubber(SR)exhibits superior breathability and high-temperature resistance.However,SR is prone to degradation under extreme heat or combustion,limiting its effectiveness in mitigating secondary hazards.In this study,phosphate glass powder was used to calcinate zinc borate,lanthanum oxide,and cerium oxide.Methylphenyl polysiloxane was then grafted onto the surface of the glass powder,resulting in the modified pow-ders designated as Methylphenyl polysiloxane-grafted zinc borate-modified phosphate glass powder(GF-ZnBM),Methylphenyl polysiloxane-grafted lanthanum oxide-modified phosphate glass powder(GF-LaM),and Methylphenyl polysiloxane-grafted cerium oxide-modified phosphate glass powder(GF-CeM).The modified powders were sub-sequently incorporated into silicone rubber composites to enhance the ceramicization capability of silicone rubber at high temperatures.Specifically,GF-CeM and GF-LaM significantly increased the limiting oxygen index(LOI)to 33%and reduced the tendency for combustion propagation.Additionally,GF-CeM notably contributed to enhancing ceramicization strength.The presence of cerium oxide helps in the melting of the glass powder and enhances its adhesion to the silicone rubber matrix.SR/ZnB-GF exhibited the lowest activation energy among the tested composites,along with the best protective capability.The inclusion of modified glass powder has a minor impact on the rheological properties,indicating that the composite retains its ability to flow and deform under stress.This confirms that the material remains flexible under normal conditions and forms a ceramic structure when heated,thereby exhibiting self-supporting properties.This study provides a practical methodology for the targeted modification of glass powders,thereby further enhancing the fire safety of silicone-based composites.
基金supported by Natural Science Foundation of Shandong Province(Nos.ZR2022YQ42,ZR2021JQ15,ZR2021QE011,ZR2021ZD20,2022GJJLJRC-01)Innovative Team Project of Jinan(No.2021GXRC019)the National Natural Science Foundation of China(Nos.52022037,52202366).
文摘In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry.Typically,the isotropy of a specific facet provides a perfect support for studying heteroatom doping.Herein,this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals.The presence of iron not only modifies the electronic structure of lithium tantalate,improving its light absorption capacity,but also functions as an active site for the nitrogen adsorption and activation.The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95μg cm^(−2)h^(−1),which is three times higher than that of undoped lithium tantalate.The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating.This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.
基金supported by the program for National Natural Science Foundation of China (Nos. 52174173, 52274188, and 52104190)the Joint Funds of the National Natural Science Foundation of China (No. U24A2091)+1 种基金The Natural Science Foundation of Henan Polytechnic University (No. B2021-2)Double FirstClass Initiative of Safety and Energy Engineering (Henan Polytechnic University) (Nos. AQ20240703 and AQ20230304)。
文摘Under submerged conditions, compared with traditional self-excited oscillating pulsed waterjets(SOPWs), annular fluid-enhanced self-excited oscillating pulsed waterjets(AFESOPWs) exhibit a higher surge pressure through self-priming. However, their pressure frequency and cavitation characteristics remain unclear, resulting in an inability to fully utilize resonance and cavitation erosion to break coal and rock. In this study, high-frequency pressure testing, high-speed photography, and large eddy simulation(LES) are used to investigate the distribution of the pressure frequency band, evolution law of the cavitation cloud, and its regulation mechanism of a continuous waterjet, SOPW, and AFESOPW. The results indicated that the excitation of the plunger pump, shearing layer vortex, and bubble collapse corresponded to the three high-amplitude frequency bands of the waterjet pressure. AFESOPWs have an additional self-priming frequency that can produce a larger amplitude under a synergistic effect with the second high-amplitude frequency band. A better cavitation effect was produced after self-priming the annulus fluid, and the shedding frequency of the cavitation clouds of the three types of waterjets was linearly related to the cavitation number. The peak pressure of the waterjet and cavitation erosion effect can be improved by modulating the waterjet pressure oscillation frequency and cavitation shedding frequency.
基金supported by National Key Research and Development Program of China(2023YFB3210400)the National Natural Science Foundation of China(52472097 and 52102171)+2 种基金Natural Science Foundation of Shandong Province(ZR2021JQ15,ZR2023LLZ008 and ZR2022YQ42)Taishan Scholar Project of Shandong Province(tstp20240515)Innovative Team Project of Jinan(2021GXRC019).
文摘The laser-assisted manufacturing technology has significant advantages in meeting various demands such as complex structures,functional integration,customized devices,and cost-effectiveness,which makes it a highly attractive option for fabricating sensors.In this review,the latest advancements and strategies in intelligent sensor development through laser processing were surveyed and outlined following the interaction of laser and materials.Laser-assisted manufacturing technologies have been extensively applied in materials science and device processing.Firstly,laser technology can be utilized in a wide range of materials,encompassing carbon-based materials,metals,and metallic oxides.In the field of device scale processing,laser manufacturing is widely used in micro/nano structures,planar device construction,and stereoscopic electronic devices such as cutting,engraving,and lithography.Additionally,laser technology provides robust support for sensor applications,covering fields such as pressure sensing,temperature sensing,gas sensing,and biosensors.Furthermore,laser considerably serves in real application areas such as multifunctional sensing systems,actuators,and robots.The widespread application of laser manufacturing technology in sensor platform fabrication offers effective solutions for realizing the miniaturization,multifunctionality,and integration of sensors.
基金financially supported by the National Natural Science Foundation of China(Nos.52372029,U22A20127,52304356,and 92263205)the Key R&D Plan Project in Hubei Province(No.2023BCB100).
文摘Infrared radiation(IR)ceramics have been recognized as energy-saving materials for high-temperature industry due to excellent IR performance.However,for conventional IR ceramics,low emissivity in partial band and emissivity degradation during high-temperature service restricted the practical application.Herein,we integrated broad-band high emissivity and slow degradation rate in novel high-entropy perovskite ceramics:La(Al_(0.2)Co_(0.2)Fe_(0.2)Ni_(0.2)Cr_(0.2))O_(3−δ)(HE-1) and La(Al_(0.2)Co_(0.2)Fe_(0.2)Ni_(0.2)Mn_(0.2))O_(3−δ)(HE-2).Specifically,the high-energy ceramic HE-1&HE-2 displayed high emissivity of 0.94/0.90 and 0.90/0.95 in the broad-band of near/mid-infrared(0.76–14µm).This excellent IR performance can be attributed to impurity energy level absorption,free carrier absorption,and lattice vibration absorption.During high-temperature service,these high-entropy ceramics have much slower emissivity degradation rate than conventional IR ceramic,because of hysteresis diffusion effect.Additionally,energy-saving ratios of 17.70%and 10.77%were realized by heating water with porous burner containing HE-1 and HE-2 coating respectively,due to enhanced heat radiation in systems.Thus,these high-entropy IR ceramics have significant application potential for long-term energy-saving in high-temperature industry.
基金supported by the National Natural Science Foundation of China(Grant No.12275190,12105201)Jiangsu Funding Program for Excellent Postdoctoral Talent(Grant No.2024ZB723)。
文摘Rational design of porous metal oxide films that serve as not only the scaffolds for light absorbers but also the transfer layer of photo generated charges is essential for fabricating highly efficient photoanodes for photoelectrochemical(PEC)hydrogen generation.In this work,w report a facile one-step pyrolysis method which can convert Zn-based MOF to porous ZnO(m-ZnO)with rough surface and abundant oxygen vacancies(O_(v)).When incorporating core-shell quantum dots(QDs)as the light absorbers,the obtained photoanodes(m-ZnO@QDs)achieved outstanding PEC performance for hydrogen generation,exhibiting 1.6 times and 5.8 times higher saturated photocurrent density(J_(sc))than thos of conventional TiO_(2)@QDs and ZnO@QDs photoanodes,respectively.Comprehensive optical and electrochemical measurements reveal tha the rough surface of m-ZnO can significantly improve the light-harvesting capacity of corresponding photoanodes through surface-enhanced light scattering.Moreover,the O_(v)in m-ZnO facilitate the interfacial transfer of photogenerated electrons.Our findings indicate that the MOF are valuable precursors for the preparation of porous films,offering a promising route to develop high-performance QDs-based PEC devices.
基金supported by the National Natural Science Foundation of China(Nos.52025132,U24A20205,52303373,21621091,22021001,and 22121001)the China Postdoctoral Science Foundation(No.2024M763174)+2 种基金the 111 Project(Nos.B17027,B16029)the Natural Science Foundation of Fujian Province of China(No.2022J02059)the New Cornerstone Science Foundation through the Xplorer Prize。
文摘Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapid,contactless,and environmentally benign operation,has emerged as a promising approach for precise liquid control.However,conventional magnetic strategies typically govern droplet movement on open surfaces,facing limitations such as restricted liquid volumes,uncertain flow paths,and inevitable evaporation,thereby constraining their broader practical applications.Recently,a variety of magneticdriven strategies have been developed to dynamically regulate liquids within enclosed spaces,especially through physicochemical mechanisms.These approaches provide efficient control over liquid behavior by leveraging magnetically induced chemical changes,structural deformations,and dragging motions,opening new opportunities for flexible and versatile fluid management.This review explores the design and mechanisms of magneto-responsive confined interfaces for the manipulation of nonmagnetic liquids,highlighting key advancements and potential applications including liquid valves,liquid mixing,liquid flow regulation,and liquid pumping.Finally,the existing challenges and future prospects in this field are presented.
基金the Shandong Province Colleges and Universities Youth Innovation Technology Plan Innovation Team Project(2022KJ285)the National Natural Science Foundation of China(52202092)the Major Subject Project of the University of Jinan。
文摘Developing efficient electrocatalysts for the nitrate reduction reaction(NIRR)to ammonia is vital for environmental remediation and sustainable ammonia synthesis.Metal-oxide-based single-atom catalysts(SACs)offer atomic-scale efficiency,yet unclear anchoring strategies for single metal sites hinder their rational design.This study systematically explored the effects of surface-loading and latticedoping strategies on anchoring transition,rare-earth,and main-group metal atoms onto Co_(3)O_(4)via the synergy of machine learning and density functional theory calculations.Through a comprehensive assessment of stability,catalytic activity,and electronic structures,it is discovered that lattice-doping enhances SACs stability by firmly anchoring metal atoms on Co sites,while surface-loading significantly boosts catalytic activity for the NIRR.Calculations predicted that Al,Ir,Rh,and Mo sites anchored through the surface-loading strategy exhibited exceptional NIRR activity(the limiting potential for Al site can reaches-0.25 V versus the reversible hydrogen electrode),far surpassing many other configurations.To further decipher the underlying mechanisms,the machine learning algorithms,especially the treebased pipeline optimization tool model,revealed that SACs activity is highly correlated with the local environment of the active center,particularly its electronic and structural characteristics.This work establishes a new design paradigm for SACs,providing both theoretical guidelines for anchoring strategy selection and a predictive framework for efficient NIRR electrocatalysts.
基金Funded by the National Natural Science Foundation of China(Nos.52102110 and 42272355)the China Postdoctoral Science Foundation(No.2023M732724)。
文摘Ti_(3)C_(2)/BiOCl composite was successfully synthesized by combining BiOCl(BOC)with an exposed(110)crystal plane and Ti_(3)C_(2) using a simple hydrothermal process.The photocatalytic performance of produced composite was evaluated using the degradation of rhodamine B(RhB)and tetracycline hydrochloride(TCH)under visible light.The results demonstrated that Ti_(3)C_(2)/BOC composite had higher photocatalytic activity than pure BOC.The optimum incorporation amount of Ti_(3)C_(2) was 2 wt%.The photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC at 10 min to 20 mg/L RhB was 97.6%,which was much higher than that of BOC(75.3%).Similarly,the photodegradation rate of 2 wt%-Ti_(3)C_(2)/BOC to 10 mg/L TCH at 30 min was 80.4%,which was higher than BOC(68.1%).In addition,the prepared 2 wt%-Ti_(3)C_(2)/BOC composite also maintained good stability even after four cycles.Electrochemical impedance spectroscopy(EIS),transient photocurrent response(IT)and ultraviolet-visible diffuse reflectance spectroscopy(UV-vis)confirmed that the photoelectrochemical properties of 2 wt%-Ti_(3)C_(2)/BOC composite were significantly improved.On the basis of analyzing the action mechanism of photocatalyst,it was pointed out that·O_(2)^(-)and h~+were the main active substances in the photodegradation of RhB and TCH by 2 wt%-Ti_(3)C_(2)/BOC.
基金supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization(NEDO),the JST Fusion Oriented Research for disruptive Science and Technology Program(JPMJFR213D)JSPS KAKENHI(JP24K17774)Domen for his guidance during their PhD studies at the University of Tokyo,as well as for his ongoing support,encouragement,and mentorship.
文摘Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral society.In this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic research.We highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen Group.His team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer method.Furthermore,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization techniques.Together with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and sunlight.His work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic systems.Through this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel production.By building on his contributions,we anticipate a significant impact on addressing major global energy challenges.
基金supported by Natural Science Foundation of Shandong Province(No.ZR2023ME155)the project of“20 Items of University”of Jinan(No.202228046)the Tais-han Scholar Project of Shandong Province(Nos.tsqn202306226 and tsqn202211171).
文摘Electrocatalytic conversion of carbon dioxide(CO_(2))into formate offers a sustainable pathway to mitigate environmental degradation and the energy crisis.Tin(Sn)-based materials are promising electrocatalysts for CO_(2)reduction to formate;however,their efficiency is limited by weak CO_(2)adsorption and activation,as well as sluggish reaction kinetics.In this work,we designed an intercrossing nanoporous Cu_(6)Sn_(5)/Sn intermetallic heterojunction via a scalable alloying-etching protocol.The resulting Cu_(6)Sn_(5)/Sn catalyst with abundant interfacial sites exhibited enhanced formate selectivity(60.79%)at−0.93 V versus the reversible hydrogen electrode(RHE),together with a high partial current density of 12.56 mA/cm^(2)and stable operation for 16 h.The modulated electronic structure of Cu_(6)Sn_(5)coupled with the robust interfacial interaction between Sn and Cu_(6)Sn_(5)synergistically promoted CO_(2)adsorption and activation,thereby improving CO_(2)reduction reaction(CO_(2)RR)performance.Electrochemical measurements and in situ infrared spectroscopy confirmed that the dual-phase interfaces facilitate H_(2)O decomposition and the generation of abundant*H intermediates,which in turn accelerate the protonation of CO_(2)to formate.This work highlights a scalable strategy for constructing intermetallic heterojunction catalysts that combine facile synthesis,reproducibility,and superior catalytic activity for CO_(2)RR.
基金supported by the National Natural Science Foundation of China(Grant No.22275210)the Natural Science Foundation of Shandong Province(Grant No.ZR2024QB025,ZR2023ME155)the Taishan Scholar Project of Shandong Province(tsqn202306226)。
文摘Optimizing the energy barrier of 2H-to-1T phase transformation plays a crucial role in modulating the intrinsic electronic structure of MoS_(2)to achieve satisfactory water-splitting performance,but remains a significant challenge.Herein,we report a vacancy occupation-triggered phase transition strategy to fabricate a core-shell 1T phase nanorod structure,which is composed of S-vacancies decorated MoS_(2)as the core,and N,P co-doped carbons as the shell(1T-MoS_(2)@NPC).The co-insertion of N and P dopants into MoS_(2)can occupy partial S-vacancies,triggering a phase transformation from the semiconducting 2H phase to the conducting 1T phase with a reduced energy barrier.Profiting from the strong coupling effect between N,P dopants and S-vacancies,the as-made 1T-MoS_(2)@NPC exhibits excellent electrocatalytic activity for both HER(η_(10)=148 m V)and OER(η_(10)=232 mV)in alkaline solution.Meanwhile,a low cell voltage of 1.62 V is needed to drive a current density of 10mA cm^(-2)in 1.0 M KOH electrolyte.The theoretical calculation results reveal that the S-vacancies decorated C atoms in the meta-position relative to N,P atoms represent the most active HER and OER sites,which synergistically upshift the d band center and balance the rate-determining step,thus ensuring the simultaneous optimization of adsorption free energy and electronic structure.This vacancy-occupation-derived phase transformation strategy caused by non-metallic doping may provide valuable guidance for enhancing the performance of alkaline water electrolysis.
基金supported by the National Natural Science Foundation of China(Nos.52272186,22090023 and 22375207)Beijing Institute of Technology Research Fund Program for Young Scholars(No.XSQD-6120220081)
文摘Metal halide perovskites have rapidly emerged as outstanding semiconductors for laser applications.Surface plasmon resonances of metals offer a platform for improving the perovskite lasing properties of metal halide perovskites by accelerating radiative recombination.However,the constraint on degrees of freedom of perovskite-metal interactions in two dimensions keeps us from getting a full picture of plasmon-involved carrier dynamics and reaching the optimum perovskite lasing performance.Here we report a strategy of synthesizing quantitative coassemblies of perovskite and metal nanocrystals for studying the effect of surface plasmons on carrier dynamics in depth and exploring plasmon-enhanced perovskite lasing performance.Within the coassembly,each metal nanocrystal supports localized surface plasmon resonances capable of accelerating radiative recombination of all adjacent perovskite nanocrystals in three dimensions.The quantitative coassemblies disclose the evolution of radiative and nonradiative recombination processes in perovskite nanocrystals with the plasmon modes,identifying an optimal metal nanocrystal content for fulfilling the highest radiative efficiency in perovskite nanocrystals.By virtue of accelerated radiative recombination,the coassemblies of perovskite and metal nanocrystals allowed for the construction of microlaser arrays with enhanced performance including low thresholds and ultrafast outputs.This work fundamentally advances the perovskite-metal systems for plasmonically enhancing perovskite optoelectronic performance.
基金supported by National Science Foundation of Shandong Province(Nos.ZR2023ME155 and ZR2023ME085)the Taishan Scholar Project of Shandong Province(Nos.tsqn202306226 and tsqn202211171).
文摘The development of high-performance lithium-ion batteries(LIBs)hinges on searching for advanced anode materials with large specific capacities as well as high cycling stability.However,traditional graphite anodes have not met the demand for higher energy storage owing to the deficiency of low lithium storage capacity.In the current work,we focus on designing one composite anode material with multiscale porous(MP)structure and phosphorus(P)doping.The coupling effects of three-dimensional(3D)interconnected skeleton,hollow pore channels,and P doping can facilitate the electrolyte diffusion and the mass transfer,as well as accommodate the volume changes during lithiation/delithiation processes.As expected,the as-prepared MP-SiGeSnSbPAl composite exhibits superior lithium storage performance,achieving a specific capacity of 827.9 mAh/g after 150 cycles at 200 mA/g and maintaining the high capacity of 456.7 mAh/g after 400 cycles at 1 A/g.Contrastively,the corresponding surplus capacities are only 590.3 and 225.7 mAh/g for the non-doped counterparts,respectively.In particular,MP-SiGeSnSbPAl displays much more stable cycling performances under the measurement of high areal mass loading of~3 mg/cm^(2)and the full-cell tests with the lithium iron phosphate as the cathode.This work witnesses one scalable protocol for preparing multinary Si-based composite in terms of facile operation and high lithium storage performances.
基金Taishan Scholar Project of Shandong Province(No.tsqn202306226)Natural Science Foundation of Shandong Prov-ince(No.ZR2023ME155)+1 种基金The project of“20 Items of University”of Jinan(No.202228046)Luzhou Municipal Science and Technol-ogy Plan Project(Nos.2024JYJ016 and 2024JYJ018).
文摘Alkaline electrolytic hydrogen production has emerged as one of the most practical methods for industrial-scale hydrogen production.However,the initial hydrolysis dissociation in alkaline media impedes the hydrogen evolution reaction(HER)kinetics of commercial catalysts.To overcome this limitation,this study focuses on the development of a highly efficient electrocatalyst for alkaline HER.Ni-based intermetallic compounds exhibit remarkable catalytic activity for HER,with the NiMo alloy being among the most active catalysts in alkaline environments.Here,we designed and fabricated self-supported multiscale porous NiZn/NiMo intermetallic compounds on a metal foam substrate using a versatile dealloying method.The resulting electrode exhibits excellent HER activity,achieving an overpotential of just 204 mV at 1000 mA/cm^(2),and dem-onstrates robust long-term catalytic stability,maintaining performance at 100 mA/cm^(2) for 400 h in an alkaline electrolyte.Thesefindings underscore the potential of nanosized intermetallic compounds fabricated via a dealloying approach to deliver exceptional catalytic performance for alkaline water electrolysis.
基金supported by the National Key R&D Program of China(2024YFA1211004)the National Natural Science Foundation of China(52300069,52192681,U21A20160)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20230276)Science and Technology Program of Suzhou,China(SWY20222003,2022SS19).
文摘In photocatalytic water treatment processes,the particulate photocatalysts are typically immobilized on membrane,through either chemical/physical loading onto the surface or directly embedding in the membrane matrix.However,these immobilization strategies inevitably compromise the interfacial mass diffusion and cause activity decline relative to the suspended catalyst.Here,we propose a binder-free surface immobilization strategy for fabrication of high-activity photocatalytic membrane.Through a simple dimethylformamide(DMF)treatment,the nanofibers of polyvinylidene fluoride membrane were softened and stretched,creating enlarged micropores to efficiently capture the photocatalyst.Subsequently,the nanofibers underwent shrinking during DMF evaporation,thus firmly strapping the photocatalyst microparticles on the membrane surface.This surface self-bounded photocatalytic membrane,with firmly bounded yet highly exposed photocatalyst,exhibited 4.2-fold higher efficiency in hydrogen peroxide(H_(2)O_(2))photosynthesis than the matrix-embedded control,due to improved O_(2)accessibility and H_(2)O_(2)diffusion.It even outperformed the suspension photocatalytic system attributed to alleviated H_(2)O_(2)decomposition at the hydrophobic surface.When adopted for UV-based water treatment,the photocatalytic system exhibited tenfold faster micropollutants photodegradation than the catalyst-free control and demonstrated superior robustness for treating contaminated tap water,lake water and secondary wastewater effluent.This immobilization strategy can also be extended to the fabrication of other photocatalytic membranes with diverse catalyst types and membrane substrate.Overall,our work opens a facile avenue for fabrication of high-performance photocatalytic membranes,which may benefit advanced oxidation water purification application and beyond.
