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
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
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
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
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
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
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
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
Harvesting the immense and renewable osmotic energy with reverse electrodialysis(RED)technology shows great promise in dealing with the ever-growing energy crisis.One key challenge is to improve the output power densi...Harvesting the immense and renewable osmotic energy with reverse electrodialysis(RED)technology shows great promise in dealing with the ever-growing energy crisis.One key challenge is to improve the output power density with improved trade-off between membrane permeability and selectivity.Herein,polyelectrolyte hydrogels(channel width,2.2 nm)with inherent high ion conductivity have been demonstrated to enable excellent selective ion transfer when confined in cylindrical anodized aluminum pore with lateral size even up to the submillimeter scale(radius,0.1 mm).The membrane permeability of the anti-swelling hydrogel can also be further increased with cellulose nanofibers.With real seawater and river water,the output power density of a three-chamber cell on behalf of repeat unit of RED system can reach up to 8.99 W m^(-2)(per unit total membrane area),much better than state-of-the-art membranes.This work provides a new strategy for the preparation of polyelectrolyte hydrogel-based ion-selective membranes,owning broad application prospects in the fields of osmotic energy collection,electrodialysis,flow battery and so on.展开更多
For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable sur...For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.展开更多
The prelithiated SiO_(x)anode showcases markedly improved Li-storage capabilities compared to its unlithiated counterparts,yet it faces hurdles such as slurry gassing,electrolyte deterioration,and capacity fade attrib...The prelithiated SiO_(x)anode showcases markedly improved Li-storage capabilities compared to its unlithiated counterparts,yet it faces hurdles such as slurry gassing,electrolyte deterioration,and capacity fade attributed to residual alkali and an unstable electrolyte/anode interface.To tackle these challenges,we propose a strategic utilization of residual alkali by creating an in-situ γ-LiAlO_(2)functional layer on the prelithiated SiO_(x)@C anode material.This is accomplished by incorporating a minor amount of Al_(2)O_(3)into the SiO_(x)@C/LiH precursor mixture before the solid-phase prelithiation process.The resulting modified prelithiated SiO_(x)@C anode with in-situ formed electrolyte-isolatingγ-LiAlO_(2)layer exhibits no discernible slurry gas generation within 7 days and substantially mitigates side reactions with the electrolyte,thereby boosting the initial coulombic efficiency and cycling stability of the SiO_(x)@C anode.In half-cell evaluations,the prelithiated SiO_(x)@C anode demonstrates a high Li-storage capacity of 1323 mAh g^(-1)and an impressive initial coulombic efficiency of 91.09%.When assessed in a 3.2 Ah 18,650 cylindrical battery,the prelithiated SiO_(x)@C anode showcases exceptional cyclability,retaining 81% of its capacity after 1000 cycles,underscoring its potential for practical applications.This study introduces a scalable and cost-effective prelithiation technique that propels the development and practical deployment of Si-based anodes by resolving persistent scientific challenges with the use of inexpensive additives.展开更多
The Li-CO_(2)battery has been highly rated as an intriguing technique for balancing the carbon cycle for years,but it is still significantly challenged by the obstacles such as limited reversibility,sluggish kinetics,...The Li-CO_(2)battery has been highly rated as an intriguing technique for balancing the carbon cycle for years,but it is still significantly challenged by the obstacles such as limited reversibility,sluggish kinetics,and poor energy efficiency.Hence,the design and development of advance catalysts that can enhance the kinetics and reversibility of the CO_(2)electrochemical cycling reactions are considered the imperative tasks.Transition metal-based catalysts are widely considered appealing owing to their unfilled dorbitals,rich and adjustable valences,as well as processibility.In this review,the working mechanism and the key issues of the CO_(2)electrochemical cycling reaction are discussed first.Then the strategies for composition and structure design of different type of transition metal-based catalysts are highlighted,including their benefits,limitations,and the ways to implement these strategies.Finally,based on the pioneering research,the perspectives on the challenges and key points for the future development of cathode catalyst are proposed.展开更多
Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated gra...Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated graphene(EEG)nanosheets were easily made as one composited electrode material for boosting the charge storage performances of supercapacitors.Coupled with the fluent electron and ion transport from two-dimensional EEG nanosheets,the uniformly anchoredδ-MnO_(2) nanoflake arrays present high reversible capacity,superior cycling stability,and unique rate capability.As expected,the MnO_(2)/EEG-10 electrode delivers high specific capacitance of 190 F·g^(−1) at 0.2 A·g^(−1),and holds 97.3%of its initial capacitance after 10000 cycles at 5 A·g^(−1).Furthermore,an asymmetrical supercapacitor using MnO_(2)/EEG-10 as the positive electrode achieves an energy density of 17.7 W·h·kg^(−1) at a power density of 922.7 W·kg^(−1) with 82.9%capacity retention upon 10000 cycles at 5 A·g^(−1).This work highlights the facile fabrication of high-performance MnO_(2)/graphene composites with excellent structure stability using graphene nanosheets as the conductive matrix.展开更多
Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve t...Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve the migration of a highly efficient hydrogen species to Pt sites over Pt/Co@NC,which is obtained through a facile calcination and electrodeposition method.It exhibits an outstanding geometric activity(η_(10)=31 m V),which surpasses the commercial 20 wt%Pt/C(η_(10)=37 mV).Moreover,the mass activity of Pt/Co@NC is 5.6 A mg_(Pt)^(-1) at-50 mV vs.RHE,which is 2.23 times higher than that of 20 wt%Pt/C.Experimental and theoretical results indicate that the work function of the outer carbon layer,which is changed by the introduction of the inner cobalt core,plays a crucial role in reversing the direction of electron migration between the carbon layer and Pt.The negatively charged Pt^(δ-)can spontaneously attract positively charged protons via the electrostatic interaction effect,thereby achieving the directional migration of hydrogen species.This work presents a strategy for designing advanced alkaline HER electrocatalysts by the electrostatic effect.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically re...Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.展开更多
Hollow NiCoSe_(x)(H-NiCoSe_(x)) nanospheres encapsulated with carbon shell were prepared via one-step easy solvothermal method followed by the carbon coating process.H-NiCoSe_(x)@C has large interior void with the uni...Hollow NiCoSe_(x)(H-NiCoSe_(x)) nanospheres encapsulated with carbon shell were prepared via one-step easy solvothermal method followed by the carbon coating process.H-NiCoSe_(x)@C has large interior void with the uniform dimension around 350 nm and the thickness of carbon shell around 20-30 nm.Coupling with the large interior void as well as robust protective carbon shell,H-NiCoSe_(x)@C can retain the reversible capacity of 805.6 mAh·g^(-1) after 100 cycles at 200 mA·g^(-1).In particular,H-NiCoSe_(x)@C delivers large reversible capacity of 1532.2 mAh·g^(-1) upon cycling for 1000 loops at 1000 mA·g^(-1)with the capacity retention as high as 128.2% upon long period of activation.Even at the high rate of 3000 mA·g^(-1),its specific capacity still retains up to 659.3 mAh·g^(-1).The superior lithium storage performances for H-NiCoSe_(x)@C profit from its robust hollow core-shell structure as well as enhanced electrical conductivity and ion transport.展开更多
Powered by the solar light as energy source,gas-phase photothermal carbon dioxide(CO_(2)) catalysis has recently sprung up as a promising route to convert CO_(2) molecules into value-added chemicals,feedstocks,and fue...Powered by the solar light as energy source,gas-phase photothermal carbon dioxide(CO_(2)) catalysis has recently sprung up as a promising route to convert CO_(2) molecules into value-added chemicals,feedstocks,and fuels,profiting from the great potential to be well integrated into the existing petrochemical production system.展开更多
Sn3O4, a common two-dimensional semiconductor photocatalyst, can absorb visible light.However, owing to its rapid recombination of photogenerated electron-hole pairs, its absorption is not sufficient for practical app...Sn3O4, a common two-dimensional semiconductor photocatalyst, can absorb visible light.However, owing to its rapid recombination of photogenerated electron-hole pairs, its absorption is not sufficient for practical application.In this work, a Sn nanoparticle/Sn3O4-x nanosheet heterostructure was prepared by in situ reduction of Sn3O4 under a H2 atmosphere.The Schottky junctions formed between Sn and Sn3O4-x can enhance the photogenerated carrier separation ability.During the hydrogenation process, a portion of the oxygen in the semiconductor can be extracted by hydrogen to form water, resulting in an increase in oxygen vacancies in the semiconductor.The heterostructure showed the ability to remove Rhodamine B.Cell cytocompatibility experiments proved that Sn/Sn3O4-x can significantly enhance cell compatibility and reduce harm to organisms.This work provides a new method for the fabrication of a Schottky junction composite photocatalyst rich in oxygen vacancies with enhanced photocatalytic performance.展开更多
The carbon cycle is important for maintaining a stable climate and carbon balance on Earth. Renewable-electricitydriven upcycling of carbon dioxide (CO_(2)) into value-added multi-carbon molecules is a potentially sus...The carbon cycle is important for maintaining a stable climate and carbon balance on Earth. Renewable-electricitydriven upcycling of carbon dioxide (CO_(2)) into value-added multi-carbon molecules is a potentially sustainable way to alleviate greenhouse gas emission and enable production of various chemicals and fuels.展开更多
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 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 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 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supported by The Project of“20 Items of University”of Jinan(Grant No.202228078)Innovative Research Team in Higher Educational Institutions of Shandong Province(Grant No.2023KJ107)+2 种基金Taishan Scholars Program of Shandong Province(tsqn201812085)National Natural Science Foundation of China(Grant No.51903102,Grant No.52376063,Grant No.52302256)China Postdoctoral Science Foundation(Grant No.2023MD744223).
文摘Harvesting the immense and renewable osmotic energy with reverse electrodialysis(RED)technology shows great promise in dealing with the ever-growing energy crisis.One key challenge is to improve the output power density with improved trade-off between membrane permeability and selectivity.Herein,polyelectrolyte hydrogels(channel width,2.2 nm)with inherent high ion conductivity have been demonstrated to enable excellent selective ion transfer when confined in cylindrical anodized aluminum pore with lateral size even up to the submillimeter scale(radius,0.1 mm).The membrane permeability of the anti-swelling hydrogel can also be further increased with cellulose nanofibers.With real seawater and river water,the output power density of a three-chamber cell on behalf of repeat unit of RED system can reach up to 8.99 W m^(-2)(per unit total membrane area),much better than state-of-the-art membranes.This work provides a new strategy for the preparation of polyelectrolyte hydrogel-based ion-selective membranes,owning broad application prospects in the fields of osmotic energy collection,electrodialysis,flow battery and so on.
基金supported by National Natural Science Foundation of China(No.52202366)Taishan Scholar Project of Shandong Province(tstp20240515,tsqn202312217)+1 种基金Natural Science Foundation of Shandong Province(China,No.2025HWYQ-050,ZR2021QE011,ZR2022QH072,ZR2021QE284)the King Abdullah University of Science and Technology,the Center of Excellence for Renewable Energy and Storage Technologies.
文摘For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.
基金supported by the National Natural Science Foundation of China(52234001,52201254)the Science and Technology Planning Project of Hunan Province(2018TP1017)+3 种基金the Science,Technoloy and Innovation Project of Changsha Research Institute of Mining and Metallurgy(22-C5CL001)the Young Student Fundamental Research Project of Hunan Natural Science Foundation(2024JJ10036)the Introducing Major Universities and Research Institutions to Jointly Build Innovative Carrier Project of Jining City(2023DYDS022)the Scientific Research Foundation for New Talents in University of Jinan(XRC2406)。
文摘The prelithiated SiO_(x)anode showcases markedly improved Li-storage capabilities compared to its unlithiated counterparts,yet it faces hurdles such as slurry gassing,electrolyte deterioration,and capacity fade attributed to residual alkali and an unstable electrolyte/anode interface.To tackle these challenges,we propose a strategic utilization of residual alkali by creating an in-situ γ-LiAlO_(2)functional layer on the prelithiated SiO_(x)@C anode material.This is accomplished by incorporating a minor amount of Al_(2)O_(3)into the SiO_(x)@C/LiH precursor mixture before the solid-phase prelithiation process.The resulting modified prelithiated SiO_(x)@C anode with in-situ formed electrolyte-isolatingγ-LiAlO_(2)layer exhibits no discernible slurry gas generation within 7 days and substantially mitigates side reactions with the electrolyte,thereby boosting the initial coulombic efficiency and cycling stability of the SiO_(x)@C anode.In half-cell evaluations,the prelithiated SiO_(x)@C anode demonstrates a high Li-storage capacity of 1323 mAh g^(-1)and an impressive initial coulombic efficiency of 91.09%.When assessed in a 3.2 Ah 18,650 cylindrical battery,the prelithiated SiO_(x)@C anode showcases exceptional cyclability,retaining 81% of its capacity after 1000 cycles,underscoring its potential for practical applications.This study introduces a scalable and cost-effective prelithiation technique that propels the development and practical deployment of Si-based anodes by resolving persistent scientific challenges with the use of inexpensive additives.
基金financially supported by the National Natural Science Foundation of China(52201254,52234001,52074177)the National Key Research and Development Program(2022YFC3900905)+3 种基金the Natural Science Foundation of Shandong Province(ZR2020QE012,ZR2020MB090,ZR2023ME155,ZR2023ME085)the Scientific Research Foundation for New Talents in University of Jinan(XRC2406)the project of “20 Items of University”of Jinan(202228046)the Introducing Major Universities and Research Institutions to Jointly Build Innovative Carrier Project of Jining City(2023DYDS022)。
文摘The Li-CO_(2)battery has been highly rated as an intriguing technique for balancing the carbon cycle for years,but it is still significantly challenged by the obstacles such as limited reversibility,sluggish kinetics,and poor energy efficiency.Hence,the design and development of advance catalysts that can enhance the kinetics and reversibility of the CO_(2)electrochemical cycling reactions are considered the imperative tasks.Transition metal-based catalysts are widely considered appealing owing to their unfilled dorbitals,rich and adjustable valences,as well as processibility.In this review,the working mechanism and the key issues of the CO_(2)electrochemical cycling reaction are discussed first.Then the strategies for composition and structure design of different type of transition metal-based catalysts are highlighted,including their benefits,limitations,and the ways to implement these strategies.Finally,based on the pioneering research,the perspectives on the challenges and key points for the future development of cathode catalyst are proposed.
基金supported by Natural Science Foundation of Shandong Province(ZR2023ME155 and ZR2023ME085)the project of“20 Items of University”of Jinan(202228046)the Taishan Scholar Project of Shandong Province(tsqn202306226 and tsqn202211171).
文摘Supercapacitors represent one specific class of energy storage devices that bridge the gap between traditional capacitors and batteries.In current work,δ-MnO_(2) nanoflakes arrayed on electrochemically exfoliated graphene(EEG)nanosheets were easily made as one composited electrode material for boosting the charge storage performances of supercapacitors.Coupled with the fluent electron and ion transport from two-dimensional EEG nanosheets,the uniformly anchoredδ-MnO_(2) nanoflake arrays present high reversible capacity,superior cycling stability,and unique rate capability.As expected,the MnO_(2)/EEG-10 electrode delivers high specific capacitance of 190 F·g^(−1) at 0.2 A·g^(−1),and holds 97.3%of its initial capacitance after 10000 cycles at 5 A·g^(−1).Furthermore,an asymmetrical supercapacitor using MnO_(2)/EEG-10 as the positive electrode achieves an energy density of 17.7 W·h·kg^(−1) at a power density of 922.7 W·kg^(−1) with 82.9%capacity retention upon 10000 cycles at 5 A·g^(−1).This work highlights the facile fabrication of high-performance MnO_(2)/graphene composites with excellent structure stability using graphene nanosheets as the conductive matrix.
基金financially supported by the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB610003)the Natural Science Foundation of Jiangsu Province(BK20240339)+2 种基金the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(No.2023KJ104)the National Natural Science Foundation of China(No.52202092)the Natural Science Foundation of Shandong Province(No.ZR2022QE076)。
文摘Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve the migration of a highly efficient hydrogen species to Pt sites over Pt/Co@NC,which is obtained through a facile calcination and electrodeposition method.It exhibits an outstanding geometric activity(η_(10)=31 m V),which surpasses the commercial 20 wt%Pt/C(η_(10)=37 mV).Moreover,the mass activity of Pt/Co@NC is 5.6 A mg_(Pt)^(-1) at-50 mV vs.RHE,which is 2.23 times higher than that of 20 wt%Pt/C.Experimental and theoretical results indicate that the work function of the outer carbon layer,which is changed by the introduction of the inner cobalt core,plays a crucial role in reversing the direction of electron migration between the carbon layer and Pt.The negatively charged Pt^(δ-)can spontaneously attract positively charged protons via the electrostatic interaction effect,thereby achieving the directional migration of hydrogen species.This work presents a strategy for designing advanced alkaline HER electrocatalysts by the electrostatic effect.
基金supported by the National Natural Science Foundation of China (22071172)the Ministry of Science and Technology of China (2016YFB0401100,2017YFA0204503,and 2018YFA0703200)Shandong Provincial Natural Science Foundation (No. ZR2019BB025)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.
基金financially supported by the National Natural Science Foundation of China(No.51772133)the Natural Science Foundation of Shandong Province(No.ZR2017JL022)+1 种基金the Project of“20 Items of University”of Jinan(No.2018GXRC001)the Case-by-Case Project for Top Outstanding Talents of Jinan。
文摘Hollow NiCoSe_(x)(H-NiCoSe_(x)) nanospheres encapsulated with carbon shell were prepared via one-step easy solvothermal method followed by the carbon coating process.H-NiCoSe_(x)@C has large interior void with the uniform dimension around 350 nm and the thickness of carbon shell around 20-30 nm.Coupling with the large interior void as well as robust protective carbon shell,H-NiCoSe_(x)@C can retain the reversible capacity of 805.6 mAh·g^(-1) after 100 cycles at 200 mA·g^(-1).In particular,H-NiCoSe_(x)@C delivers large reversible capacity of 1532.2 mAh·g^(-1) upon cycling for 1000 loops at 1000 mA·g^(-1)with the capacity retention as high as 128.2% upon long period of activation.Even at the high rate of 3000 mA·g^(-1),its specific capacity still retains up to 659.3 mAh·g^(-1).The superior lithium storage performances for H-NiCoSe_(x)@C profit from its robust hollow core-shell structure as well as enhanced electrical conductivity and ion transport.
文摘Powered by the solar light as energy source,gas-phase photothermal carbon dioxide(CO_(2)) catalysis has recently sprung up as a promising route to convert CO_(2) molecules into value-added chemicals,feedstocks,and fuels,profiting from the great potential to be well integrated into the existing petrochemical production system.
基金financially supported by the National Natural Science Foundation of China (Nos.51802115 and 51732007)the Natural Science Foundation of Shandong Province, China (No.ZR2019YQ21)。
文摘Sn3O4, a common two-dimensional semiconductor photocatalyst, can absorb visible light.However, owing to its rapid recombination of photogenerated electron-hole pairs, its absorption is not sufficient for practical application.In this work, a Sn nanoparticle/Sn3O4-x nanosheet heterostructure was prepared by in situ reduction of Sn3O4 under a H2 atmosphere.The Schottky junctions formed between Sn and Sn3O4-x can enhance the photogenerated carrier separation ability.During the hydrogenation process, a portion of the oxygen in the semiconductor can be extracted by hydrogen to form water, resulting in an increase in oxygen vacancies in the semiconductor.The heterostructure showed the ability to remove Rhodamine B.Cell cytocompatibility experiments proved that Sn/Sn3O4-x can significantly enhance cell compatibility and reduce harm to organisms.This work provides a new method for the fabrication of a Schottky junction composite photocatalyst rich in oxygen vacancies with enhanced photocatalytic performance.
基金financially supported by the National Natural Science Foundation of China (Nos.50835002 and 51105102)。
文摘The carbon cycle is important for maintaining a stable climate and carbon balance on Earth. Renewable-electricitydriven upcycling of carbon dioxide (CO_(2)) into value-added multi-carbon molecules is a potentially sustainable way to alleviate greenhouse gas emission and enable production of various chemicals and fuels.
