Due to the technical fault,a wrong version of the paper was uploaded.The content of the article was not affected,but the layout of the article was affected.The original article has been corrected.
SnO_(2)films exhibit significant potential as cost-effective and high electron mobility substitutes for In_(2)O_(3)films.In this study,Li is incorporated into the interstitial site of the SnO_(2)lattice resulting in a...SnO_(2)films exhibit significant potential as cost-effective and high electron mobility substitutes for In_(2)O_(3)films.In this study,Li is incorporated into the interstitial site of the SnO_(2)lattice resulting in an exceptionally low resistivity of 2.028×10^(-3)Ω·cm along with a high carrier concentration of 1.398×10^(20)cm^(-3)and carrier mobility of 22.02 cm^(2)/V·s.展开更多
Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion ...Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion to higher-value forms(referred to as“up-carbonization”here),these abundant feedstocks provide viable opportunities for energy-rich fuels and sustainable platform chemicals production.However,many of the current methods for such up-carbonization still lack sufficient energy,cost,and material efficiency,which affect their economics and carbon-emissions footprint.With external electricity precisely delivered,discharge plasmas enable many stubborn reactions to occur under mild conditions,by creating locally intensified and highly reactive environments.This technology emerges as a novel,versatile technology platform for integrated or stand-alone conversion of carbon-rich resources.The plasma-based processes are compatible for integration with increasingly abundant and cost-effective renewable electricity,making the whole conversion carbon-neutral and further paving the plasma-electrified upcarbonization to be performance-,environment-,and economics-viable.Despite the chief interest in this emerging area,no review article brings together the state-of-the-art results from diverse disciplines and underlies basic mechanisms and chemistry underpinned.As such,this review aims to fill this gap and provide basic guidelines for future research and transformation,by providing an overview of the application of plasma techniques for carbon-rich resource conversion,with particular focus on the perspective of discharge plasmas,the fundamentals of why plasmas are particularly suited for upcarbonization,and featured examples of plasma-enabled resource valorization.With parallels drawn and specificity highlighted,we also discuss the technique shortcomings,current challenges,and research needs for future work.展开更多
Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their po...Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their potential in promoting CO_(2)reduction reaction(CO_(2)RR),however,their low phase stability has limited their application perspective.Herein,we present a reduced graphene oxide(rGO)wrapped CsPbI_3 perovskite nanocrystal(NC)CO_(2)RR catalyst(CsPbI_3/rGO),demonstrating enhanced stability in the aqueous electrolyte.The CsPbI_3/rGO catalyst exhibited>92%Faradaic efficiency toward formate production at a CO_(2)RR current density of~12.7 mA cm^(-2).Comprehensive characterizations revealed the superior performance of the CsPbI_3/rGO catalyst originated from the synergistic effects between the CsPbI_3 NCs and rGO,i.e.,rGO stabilized theα-CsPbI_3 phase and tuned the charge distribution,thus lowered the energy barrier for the protonation process and the formation of~*HCOO intermediate,which resulted in high CO_(2)RR selectivity toward formate.This work shows a promising strategy to rationally design robust metal halide perovskites for achieving efficient CO_(2)RR toward valuable fuels.展开更多
The artificial nitrogen(N_(2)) reduction reaction(NRR) via electrocatalysis is a newly developed methodology to produce ammonia(NH3) at ambient conditions,but faces the challenges in N_(2)activation and poor reaction ...The artificial nitrogen(N_(2)) reduction reaction(NRR) via electrocatalysis is a newly developed methodology to produce ammonia(NH3) at ambient conditions,but faces the challenges in N_(2)activation and poor reaction selectivity.Herein,Nb-based MXenes are developed to remarkably enhance the NRR activity through the engineering of the stretched 3D structure and oxygen vacancies(VO).The theoretical studies indicate that N_(2)could be initially adsorbed on VOwith an end-on configuration,and the potential determining step might be the first hydrogenation step.The catalysts achieve an NH3production rate of 29.1 μg h^(-1)mg_(cat)^(-1)and excellent Faradic efficiency of 11.5%,surpassing other Nbbased catalysts.The selectivity of NRR is assigned to the unique structure of the catalysts,including(1) the layered graphitic structure for fast electron transfer and active site distribution,(2) the reactive VOfor N_(2)adsorption and activation,and(3) the expanded interlayer space for mass transfer.展开更多
Nickel selenide(NiSe)has been a promising positive electrode for hybrid supercapacitors due to its multiple oxidation states,tunability,and high specific capacity.However,sluggish ion transfers and particle agglomerat...Nickel selenide(NiSe)has been a promising positive electrode for hybrid supercapacitors due to its multiple oxidation states,tunability,and high specific capacity.However,sluggish ion transfers and particle agglomeration hamper its electrochemical performance.In the present study,we have grown NiSe nanoparticles on two-dimensional(2D)graphitic carbon nitride(g-C_(3)N_(4))nanosheets to realize three-dimensional(3D)architecture.The 2D support,high nitrogen content,and features of g-C_(3)N_(4)enhanced the specific capacity of the NiSe/g-C_(3)N_(4)nanocomposite material.The resulting nanocomposite shows a specific capacity of 320 mA h g^(-1)at a current density of 1 A g^(-1),which is considerably higher than pristine NiSe.Later,the hybrid supercapacitor(HSC)device was fabricated using NiSe/g-C_(3)N_(4)composite as positive and activated carbon(AC)as negative electrodes.The cell delivered an energy density of 52.5 Wh kg^(-1)at a power density of 1488 W kg^(-1)with excellent cyclic stability of 84.9%over 8000 cycles.The electrochemical performance enhancement corresponds to a 3D structure,high electrochemical active sites,and improved charge transportation at the electrode/electrolyte interface.Thus,the present work offers an easy approach and architectural design for high-performance HSC.展开更多
Combining with the advantages of two-dimensional(2D)nanomaterials,MXenes have shown great potential in next generation rechargeable batteries.Similar with other 2D materials,MXenes generally suffer severe self-agglome...Combining with the advantages of two-dimensional(2D)nanomaterials,MXenes have shown great potential in next generation rechargeable batteries.Similar with other 2D materials,MXenes generally suffer severe self-agglomeration,low capacity,and unsatisfied durability,particularly for larger sodium/potassium ions,compromising their practical values.In this work,a novel ternary heterostructure self-assembled from transition metal selenides(MSe,M=Cu,Ni,and Co),MXene nanosheets and N-rich carbonaceous nanoribbons(CNRibs)with ultrafast ion transport properties is designed for sluggish sodium-ion(SIB)and potassium-ion(PIB)batteries.Benefiting from the diverse chemical characteristics,the positively charged MSe anchored onto the electronegative hydroxy(-OH)functionalized MXene surfaces through electrostatic adsorption,while the fungal-derived CNRibs bonded with the other side of MXene through amino bridging and hydrogen bonds.This unique MXene-based heterostructure prevents the restacking of 2D materials,increases the intrinsic conductivity,and most importantly,provides ultrafast interfacial ion transport pathways and extra surficial and interfacial storage sites,and thus,boosts the high-rate storage performances in SIB and PIB applications.Both the quantitatively kinetic analysis and the density functional theory(DFT)calculations revealed that the interfacial ion transport is several orders higher than that of the pristine MXenes,which delivered much enhanced Na+(536.3 mAh g^(−1)@0.1 A g^(−1))and K^(+)(305.6 mAh g^(−1)@1.0 A g^(−1))storage capabilities and excel-lent long-term cycling stability.Therefore,this work provides new insights into 2D materials engineering and low-cost,but kinetically sluggish post-Li batteries.展开更多
The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,...The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.展开更多
The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material.In particular,nanocrystals(NCs)of inorganic perovskites have demonstrated excellen...The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material.In particular,nanocrystals(NCs)of inorganic perovskites have demonstrated excellent performance for light-emitting and display applications.However,the presence of surface defects on the NCs negatively impacts their performance in devices.Herein,we report a compatible facial post-treatment of CsPbI_(3) nanocrystals using guanidinium iodide(GuI).It is found that the GuI treatment effectively passivated the halide vacancy defects on the surface of the NCs while offering effective surface protection and exciton confinement thanks to the beneficial contribution of iodide and guanidinium cation.As a consequence,the film of treated CsPbI_(3) nanocrystals exhibited significantly enhanced luminescence and charge transport properties,leading to high-performance light-emitting diode with maximum external quantum efficiency of 13.8%with high brightness(peak luminance of 7039 cd m^(−2) and a peak current density of 10.8 cd A^(−1)).The EQE is over threefold higher than performance of untreated device(EQE:3.8%).The operational half-lifetime of the treated devices also was significantly improved with T50 of 20 min(at current density of 25 mA cm^(−2)),outperforming the untreated devices(T50~6 min).展开更多
Oxygen vacancies(Vo)in electrocatalysts are closely correlated with the hydrogen evo-lution reaction(HER)activity.The role of vacancy defects and the effect of their concentration,how-ever,yet remains unclear.Herein,B...Oxygen vacancies(Vo)in electrocatalysts are closely correlated with the hydrogen evo-lution reaction(HER)activity.The role of vacancy defects and the effect of their concentration,how-ever,yet remains unclear.Herein,Bi2O3,an unfavorable electrocata-lyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy(ΔGH*),is utilized as a perfect model to explore the func-tion of Vo on HER performance.Through a facile plasma irradia-tion strategy,Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER process.Unexpectedly,while the generated oxygen vacancies contribute to the enhanced HER performance,higher Vo concentrations beyond a saturation value result in a significant drop in HER activity.By tunning the Vo concentration in the Bi_(2)O_(3)nanosheets via adjusting the treatment time,the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52×10^(24)cm^(−3)demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm^(−2),a Tafel slope of 80 mV dec−1,and an exchange current density of 316 mA cm−2 in an alkaline solution,which approaches the top-tier activity among Bi-based HER electrocatalysts.Density-functional theory calculations confirm the preferred adsorption of H*onto Bi2O3 as a function of oxygen chemical potential(ΔμO)and oxygen partial potential(PO2)and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER activity.This study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.展开更多
Two-dimensional/two-dimensional(2D/2D)heterostructures consisting of two or more 2D building blocks possess intriguing electronic features at the nanosized interfacial regions,endowing the possibility for effectively ...Two-dimensional/two-dimensional(2D/2D)heterostructures consisting of two or more 2D building blocks possess intriguing electronic features at the nanosized interfacial regions,endowing the possibility for effectively modulating the confinement,and transport of charge carriers,excitons,photons,phonons,etc.to bring about a wide range of extraordinary physical,chemical,thermal,and/or mechanical properties.By rational design and synthesis of 2D/2D heterostructures,electrochemical properties for advanced batteries and electrocatalysis can be well regulated to meet some practical requirements.In this review,a summary on the commonly employed synthetic strategies for 2D/2D heterostructures is first given,followed by a comprehensive review on recent progress for their applications in batteries and various electrocatalysis reactions.Finally,a critical outlook on the current challenges and promising solutions is presented,which is expected to offer some insightful ideas on the design principles of advanced 2D-based nanomaterials to address the current challenges in sustainable energy storages and green fuel generations.展开更多
The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale...The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale implementation of renewable energy devices.Integration of bifunctional electrocatalysts on both anode and cathode electrodes remains a significant challenge.Herein,we report on a novel and facile strategy to construct the ordered and aligned MoS_(2)nanosheet-encapsulated metal–organic frameworks(MOFs)derived hollow CoS polyhedron,in-situ grown on a nickel foam(NF).The starfish-like MoS_(2)/CoS/NF heterojunctions were formed due to the ordered growth of the material caused by NF substrate.The optimized 2-MoS_(2)/CoS/NF heterojunction exhibits robust bifunctional electrocatalytic activity with a low overpotential of 67 and 207 m V toward the HER and OER at 10 mA cm^(-2),and the long-term stability,which exceeds most of the reported bifunctional electrocatalysts.Such high electrocatalytic performance arises due to the synergistic effect between the MoS_(2)and CoS phases across the interface,the abundant active sites,as well as the hierarchical pore framework,which collectively enhance the mass and electron transfer during the reactions.The work provides a promising approach to fabricating bifunctional catalysts with custom-designed heterojunctions and remarkable performance for applications in electrochemical energy devices and related areas.展开更多
Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismu...Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismuth oxides and subcarbonate encounter stability issues. This work is designated to exemplify that the operando synthesis can be an effective means to enhance the stability of electrocatalysts under operando CO_(2)RR conditions. A synthetic approach is developed to electrochemically convert Bi^(O)Cl into Cl-containing subcarbonate(Bi_(2)O_(2)(CO_(3))_(x)Cl_(y)) under operando CO_(2)RR conditions. The systematic operando spectroscopic studies depict that BiOCl is converted to Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) via a cathodic potential-promoted anion-exchange process. The operando synthesizedBi_(2)O_(2)(CO_(3))_(x)Cl_(y) can tolerate-1.0 V versus RHE, while for the wet-chemistry synthesized pure Bi_(2)O_(2)CO_(3),the formation of metallic Bio occurs at-0.6 V versus RHE. At-0.8 V versus RHE, Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) can readily attain a FEHCOO-of 97.9%,much higher than that of the pure Bi_(2)O_(2)CO_(3)(81.3%). DFT calculations indicate that differing from the pure Bi_(2)O_(2)CO_(3)-catalyzed CO_(2)RR, where formate is formed via a *OCHO intermediate step that requires a high energy input energy of 2.69 eV to proceed, the formation of H COO-over Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) has proceeded via a *COOH intermediate step that only requires low energy input of 2.56 eV.展开更多
A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance o...A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance of the nitrate or nitrite solution.At the inflection points of the pure nitrate solution,the derivative absorbance is zero and independent of the nitrate’s concentration,and thus the nitrite’s concentration in a mixed nitrate and nitrite solution can be obtained by using the Beer’s law at these points.The nitrate’s concentration can also be achieved from the inflection points of nitrite in the same manner.The relation between the tested substance’s(nitrate or nitrite)concentration and the second-or the third-order absorbances is obtained at these inflection points.Test measurements for mixed aqueous solutions of nitrate and nitrite with or without hydrogen peroxide confirm the reliability of this technique.We applied this technique to quantify the nitrate and nitrite generated in air plasma treated aqueous solutions.The results indicate that both nitrate and nitrite concentrations increase with the plasma treatment time,and the nitrite species is found to be generated prior to the nitrate species in the air plasma treated aqueous solution.Moreover,the production rate of total nitrogen species is independent of the solutions’p H value.These results are relevant to diverse applications of plasma activated solutions in materials processing,biotechnology,medicine and other fields.展开更多
With the rapid development of mobile Internet and intelligent devices,flexible electronic technology has attracted wide attention driven by the huge demand of the market.As one type of flexible electronic devices,flex...With the rapid development of mobile Internet and intelligent devices,flexible electronic technology has attracted wide attention driven by the huge demand of the market.As one type of flexible electronic devices,flexible sensors have attracted great interest because of their promising prospects in artificial intelligence,medical health,and environmental protection.In recent years,flexible sensors with high sensitivity,selectivity,good deformability,reliable stability,and portability are urgently needed to meet the developments of artificial skin,human-computer interaction,point of care diagnostics and wearable electronic devices.展开更多
Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air ...Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.展开更多
Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nont...Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.展开更多
Magnesium diboride(MgB_(2))magnets have the potential to be the next-generation liquid-helium-free magnet for magnetic resonance imaging(MRI)application due to their relatively high superconducting transition temperat...Magnesium diboride(MgB_(2))magnets have the potential to be the next-generation liquid-helium-free magnet for magnetic resonance imaging(MRI)application due to their relatively high superconducting transition temperature,high current density and low raw material cost compared with current commercial niobium-titanium(Nb-Ti)magnets.A typical superconducting magnet includes several coils.To produce an ultra-stable magnetic field for imaging in MRI,a superconducting electromagnet operating in a persistent mode is crucial.Superconducting coils of the electromagnet in MRI are short-circuited to operate in the persistent mode by connecting coils with superconducting joints.Per-sistent joints have been demonstrated for in-situ and ex-situ wires of both mono-and multi-filamentary structures,made predominantly by PIT techniques similar to those used in wire production.To realise further engagement of MgB_(2)in MRI applications,enhancing the performance of MgB_(2)superconducting joints is essential.This literature review summarises research and development on MgB_(2)superconducting joining technology.展开更多
In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail ov...In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail over ADT and bond to CA due to its stronger triple H-bonding affiliation,forming hollow microtubes assembled by oriented CAM crystalline arrays,as guided by the directionality of peripheral hydrogen bonds.Furthermore,competitive interaction between hydrogen bonding and ionic/covalent bonding is demonstrated by mixing Ag+ions with the CA-ADT fibers,where sulfur atoms are abstracted from ADT molecules to produce Ag_(2)S ligaments.The in situ-formed Ag_(2)S serves as a binding glue to generate CA-ADT/Ag_(2)S composites with significantly enhanced mechanical strength compared to the pristine CA-ADT fiber pellet.展开更多
Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a...Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.展开更多
文摘Due to the technical fault,a wrong version of the paper was uploaded.The content of the article was not affected,but the layout of the article was affected.The original article has been corrected.
基金supported by the Key-Area Research and Development Program of Guangdong Province(Grant No.2021B0101260001)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2019A1515110411)partly the INTPART Program at the Research Council of Norway(Grant No.322382)。
文摘SnO_(2)films exhibit significant potential as cost-effective and high electron mobility substitutes for In_(2)O_(3)films.In this study,Li is incorporated into the interstitial site of the SnO_(2)lattice resulting in an exceptionally low resistivity of 2.028×10^(-3)Ω·cm along with a high carrier concentration of 1.398×10^(20)cm^(-3)and carrier mobility of 22.02 cm^(2)/V·s.
基金support from the National Key R&D Program of China(2020YFD0900900)Science and Technology Planning Project of Zhoushan of China(2022C41001)Zhejiang Ocean University(11135091221)。
文摘Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion to higher-value forms(referred to as“up-carbonization”here),these abundant feedstocks provide viable opportunities for energy-rich fuels and sustainable platform chemicals production.However,many of the current methods for such up-carbonization still lack sufficient energy,cost,and material efficiency,which affect their economics and carbon-emissions footprint.With external electricity precisely delivered,discharge plasmas enable many stubborn reactions to occur under mild conditions,by creating locally intensified and highly reactive environments.This technology emerges as a novel,versatile technology platform for integrated or stand-alone conversion of carbon-rich resources.The plasma-based processes are compatible for integration with increasingly abundant and cost-effective renewable electricity,making the whole conversion carbon-neutral and further paving the plasma-electrified upcarbonization to be performance-,environment-,and economics-viable.Despite the chief interest in this emerging area,no review article brings together the state-of-the-art results from diverse disciplines and underlies basic mechanisms and chemistry underpinned.As such,this review aims to fill this gap and provide basic guidelines for future research and transformation,by providing an overview of the application of plasma techniques for carbon-rich resource conversion,with particular focus on the perspective of discharge plasmas,the fundamentals of why plasmas are particularly suited for upcarbonization,and featured examples of plasma-enabled resource valorization.With parallels drawn and specificity highlighted,we also discuss the technique shortcomings,current challenges,and research needs for future work.
基金financial support by Australian Research Council(ARC)supported by the generous funding from Science and Engineering faculty,QUT。
文摘Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their potential in promoting CO_(2)reduction reaction(CO_(2)RR),however,their low phase stability has limited their application perspective.Herein,we present a reduced graphene oxide(rGO)wrapped CsPbI_3 perovskite nanocrystal(NC)CO_(2)RR catalyst(CsPbI_3/rGO),demonstrating enhanced stability in the aqueous electrolyte.The CsPbI_3/rGO catalyst exhibited>92%Faradaic efficiency toward formate production at a CO_(2)RR current density of~12.7 mA cm^(-2).Comprehensive characterizations revealed the superior performance of the CsPbI_3/rGO catalyst originated from the synergistic effects between the CsPbI_3 NCs and rGO,i.e.,rGO stabilized theα-CsPbI_3 phase and tuned the charge distribution,thus lowered the energy barrier for the protonation process and the formation of~*HCOO intermediate,which resulted in high CO_(2)RR selectivity toward formate.This work shows a promising strategy to rationally design robust metal halide perovskites for achieving efficient CO_(2)RR toward valuable fuels.
基金financially supported by China Postdoctoral Science Foundation (2019M652305)Qingdao Postdoctoral Application Research Project。
文摘The artificial nitrogen(N_(2)) reduction reaction(NRR) via electrocatalysis is a newly developed methodology to produce ammonia(NH3) at ambient conditions,but faces the challenges in N_(2)activation and poor reaction selectivity.Herein,Nb-based MXenes are developed to remarkably enhance the NRR activity through the engineering of the stretched 3D structure and oxygen vacancies(VO).The theoretical studies indicate that N_(2)could be initially adsorbed on VOwith an end-on configuration,and the potential determining step might be the first hydrogenation step.The catalysts achieve an NH3production rate of 29.1 μg h^(-1)mg_(cat)^(-1)and excellent Faradic efficiency of 11.5%,surpassing other Nbbased catalysts.The selectivity of NRR is assigned to the unique structure of the catalysts,including(1) the layered graphitic structure for fast electron transfer and active site distribution,(2) the reactive VOfor N_(2)adsorption and activation,and(3) the expanded interlayer space for mass transfer.
基金the financial support from UGC NET-JRF(517906)support from UGC NFOBC(202021-201610071195)+1 种基金funding from SERB(EEQ/2022/001076)DST-SERB for startup research grant(SRG/2021/001791)。
文摘Nickel selenide(NiSe)has been a promising positive electrode for hybrid supercapacitors due to its multiple oxidation states,tunability,and high specific capacity.However,sluggish ion transfers and particle agglomeration hamper its electrochemical performance.In the present study,we have grown NiSe nanoparticles on two-dimensional(2D)graphitic carbon nitride(g-C_(3)N_(4))nanosheets to realize three-dimensional(3D)architecture.The 2D support,high nitrogen content,and features of g-C_(3)N_(4)enhanced the specific capacity of the NiSe/g-C_(3)N_(4)nanocomposite material.The resulting nanocomposite shows a specific capacity of 320 mA h g^(-1)at a current density of 1 A g^(-1),which is considerably higher than pristine NiSe.Later,the hybrid supercapacitor(HSC)device was fabricated using NiSe/g-C_(3)N_(4)composite as positive and activated carbon(AC)as negative electrodes.The cell delivered an energy density of 52.5 Wh kg^(-1)at a power density of 1488 W kg^(-1)with excellent cyclic stability of 84.9%over 8000 cycles.The electrochemical performance enhancement corresponds to a 3D structure,high electrochemical active sites,and improved charge transportation at the electrode/electrolyte interface.Thus,the present work offers an easy approach and architectural design for high-performance HSC.
基金the National Natural Science Foundation of China(Grant No.21571080)Ziqi thanks the financial support from Australian Research Council through an ARC Future Fellowship(FT180100387)+1 种基金an ARC Discovery Project(DP200103568)Specially,Junming wants to thank his parents and fiancée for their unconditional love and support in his career as a graduate student.
文摘Combining with the advantages of two-dimensional(2D)nanomaterials,MXenes have shown great potential in next generation rechargeable batteries.Similar with other 2D materials,MXenes generally suffer severe self-agglomeration,low capacity,and unsatisfied durability,particularly for larger sodium/potassium ions,compromising their practical values.In this work,a novel ternary heterostructure self-assembled from transition metal selenides(MSe,M=Cu,Ni,and Co),MXene nanosheets and N-rich carbonaceous nanoribbons(CNRibs)with ultrafast ion transport properties is designed for sluggish sodium-ion(SIB)and potassium-ion(PIB)batteries.Benefiting from the diverse chemical characteristics,the positively charged MSe anchored onto the electronegative hydroxy(-OH)functionalized MXene surfaces through electrostatic adsorption,while the fungal-derived CNRibs bonded with the other side of MXene through amino bridging and hydrogen bonds.This unique MXene-based heterostructure prevents the restacking of 2D materials,increases the intrinsic conductivity,and most importantly,provides ultrafast interfacial ion transport pathways and extra surficial and interfacial storage sites,and thus,boosts the high-rate storage performances in SIB and PIB applications.Both the quantitatively kinetic analysis and the density functional theory(DFT)calculations revealed that the interfacial ion transport is several orders higher than that of the pristine MXenes,which delivered much enhanced Na+(536.3 mAh g^(−1)@0.1 A g^(−1))and K^(+)(305.6 mAh g^(−1)@1.0 A g^(−1))storage capabilities and excel-lent long-term cycling stability.Therefore,this work provides new insights into 2D materials engineering and low-cost,but kinetically sluggish post-Li batteries.
基金financially supported by the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005)the support of the Australian Research Council (Grant No. FT160100207)the ontinued support from the Queensland University of Technology (QUT) through the centre for Materials Science。
文摘The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.
基金supported by Australian Research Council Discovery Project(DP190102252).
文摘The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material.In particular,nanocrystals(NCs)of inorganic perovskites have demonstrated excellent performance for light-emitting and display applications.However,the presence of surface defects on the NCs negatively impacts their performance in devices.Herein,we report a compatible facial post-treatment of CsPbI_(3) nanocrystals using guanidinium iodide(GuI).It is found that the GuI treatment effectively passivated the halide vacancy defects on the surface of the NCs while offering effective surface protection and exciton confinement thanks to the beneficial contribution of iodide and guanidinium cation.As a consequence,the film of treated CsPbI_(3) nanocrystals exhibited significantly enhanced luminescence and charge transport properties,leading to high-performance light-emitting diode with maximum external quantum efficiency of 13.8%with high brightness(peak luminance of 7039 cd m^(−2) and a peak current density of 10.8 cd A^(−1)).The EQE is over threefold higher than performance of untreated device(EQE:3.8%).The operational half-lifetime of the treated devices also was significantly improved with T50 of 20 min(at current density of 25 mA cm^(−2)),outperforming the untreated devices(T50~6 min).
基金This work was financially supported by the Australian Research Council(ARC)through Future Fellowship grants(FT180100387 and FT160100281)Discovery Projects(DP200103568,DP210100472,and DP200102546)+1 种基金WL thanks the support of the Science and Technology Commission of Shanghai Municipality(19520713200)Open access funding provided by Shanghai Jiao Tong University
文摘Oxygen vacancies(Vo)in electrocatalysts are closely correlated with the hydrogen evo-lution reaction(HER)activity.The role of vacancy defects and the effect of their concentration,how-ever,yet remains unclear.Herein,Bi2O3,an unfavorable electrocata-lyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy(ΔGH*),is utilized as a perfect model to explore the func-tion of Vo on HER performance.Through a facile plasma irradia-tion strategy,Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER process.Unexpectedly,while the generated oxygen vacancies contribute to the enhanced HER performance,higher Vo concentrations beyond a saturation value result in a significant drop in HER activity.By tunning the Vo concentration in the Bi_(2)O_(3)nanosheets via adjusting the treatment time,the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52×10^(24)cm^(−3)demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm^(−2),a Tafel slope of 80 mV dec−1,and an exchange current density of 316 mA cm−2 in an alkaline solution,which approaches the top-tier activity among Bi-based HER electrocatalysts.Density-functional theory calculations confirm the preferred adsorption of H*onto Bi2O3 as a function of oxygen chemical potential(ΔμO)and oxygen partial potential(PO2)and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER activity.This study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.
基金supported by Australian Research Council (ARC) through an ARC Discovery Project (DP200103568)two ARC Future Fel owship projects (FT180100387 and FT160100281)+1 种基金the financial support by a QUT 2020 ECR Scheme Grant (No. 2020001179)the project mentorship provided by Prof. Godwin Ayoko
文摘Two-dimensional/two-dimensional(2D/2D)heterostructures consisting of two or more 2D building blocks possess intriguing electronic features at the nanosized interfacial regions,endowing the possibility for effectively modulating the confinement,and transport of charge carriers,excitons,photons,phonons,etc.to bring about a wide range of extraordinary physical,chemical,thermal,and/or mechanical properties.By rational design and synthesis of 2D/2D heterostructures,electrochemical properties for advanced batteries and electrocatalysis can be well regulated to meet some practical requirements.In this review,a summary on the commonly employed synthetic strategies for 2D/2D heterostructures is first given,followed by a comprehensive review on recent progress for their applications in batteries and various electrocatalysis reactions.Finally,a critical outlook on the current challenges and promising solutions is presented,which is expected to offer some insightful ideas on the design principles of advanced 2D-based nanomaterials to address the current challenges in sustainable energy storages and green fuel generations.
基金the financial support from the National Natural Science Foundation of China(22005273,21825106 and 21671175)the Natural Science Foundation of Henan Province(222300420258)+3 种基金the Scientific and Technological Research Project in Henan Province(222102240065 and 212102210647)the Key scientific research projects of colleges and universities in Henan Province(No.22A530006)the Natural Science Foundation of Jiangsu Province(BK20220598)the Program for Science&Technology Innovative Research Team in University of Henan Province(20IRTSTHN007)。
文摘The utilization of non-noble metal catalysts with robust and highly efficient electrocatalytic activity for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)are extremely important for the large-scale implementation of renewable energy devices.Integration of bifunctional electrocatalysts on both anode and cathode electrodes remains a significant challenge.Herein,we report on a novel and facile strategy to construct the ordered and aligned MoS_(2)nanosheet-encapsulated metal–organic frameworks(MOFs)derived hollow CoS polyhedron,in-situ grown on a nickel foam(NF).The starfish-like MoS_(2)/CoS/NF heterojunctions were formed due to the ordered growth of the material caused by NF substrate.The optimized 2-MoS_(2)/CoS/NF heterojunction exhibits robust bifunctional electrocatalytic activity with a low overpotential of 67 and 207 m V toward the HER and OER at 10 mA cm^(-2),and the long-term stability,which exceeds most of the reported bifunctional electrocatalysts.Such high electrocatalytic performance arises due to the synergistic effect between the MoS_(2)and CoS phases across the interface,the abundant active sites,as well as the hierarchical pore framework,which collectively enhance the mass and electron transfer during the reactions.The work provides a promising approach to fabricating bifunctional catalysts with custom-designed heterojunctions and remarkable performance for applications in electrochemical energy devices and related areas.
基金financially supported by Australian Research Council Discovery Project(DP200100965)。
文摘Bismuth-based materials(e.g., metallic, oxides and subcarbonate) are emerged as promising electrocatalysts for converting CO_(2) to formate. However, Bio-based electrocatalysts possess high overpotentials, while bismuth oxides and subcarbonate encounter stability issues. This work is designated to exemplify that the operando synthesis can be an effective means to enhance the stability of electrocatalysts under operando CO_(2)RR conditions. A synthetic approach is developed to electrochemically convert Bi^(O)Cl into Cl-containing subcarbonate(Bi_(2)O_(2)(CO_(3))_(x)Cl_(y)) under operando CO_(2)RR conditions. The systematic operando spectroscopic studies depict that BiOCl is converted to Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) via a cathodic potential-promoted anion-exchange process. The operando synthesizedBi_(2)O_(2)(CO_(3))_(x)Cl_(y) can tolerate-1.0 V versus RHE, while for the wet-chemistry synthesized pure Bi_(2)O_(2)CO_(3),the formation of metallic Bio occurs at-0.6 V versus RHE. At-0.8 V versus RHE, Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) can readily attain a FEHCOO-of 97.9%,much higher than that of the pure Bi_(2)O_(2)CO_(3)(81.3%). DFT calculations indicate that differing from the pure Bi_(2)O_(2)CO_(3)-catalyzed CO_(2)RR, where formate is formed via a *OCHO intermediate step that requires a high energy input energy of 2.69 eV to proceed, the formation of H COO-over Bi_(2)O_(2)(CO_(3))_(x)Cl_(y) has proceeded via a *COOH intermediate step that only requires low energy input of 2.56 eV.
基金National Natural Science Foundation of China(No.52077185)the Basic Research Program of Science and Technology of Shenzhen,China(No.JCYJ20190809162617137)for partial financial support。
文摘A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance of the nitrate or nitrite solution.At the inflection points of the pure nitrate solution,the derivative absorbance is zero and independent of the nitrate’s concentration,and thus the nitrite’s concentration in a mixed nitrate and nitrite solution can be obtained by using the Beer’s law at these points.The nitrate’s concentration can also be achieved from the inflection points of nitrite in the same manner.The relation between the tested substance’s(nitrate or nitrite)concentration and the second-or the third-order absorbances is obtained at these inflection points.Test measurements for mixed aqueous solutions of nitrate and nitrite with or without hydrogen peroxide confirm the reliability of this technique.We applied this technique to quantify the nitrate and nitrite generated in air plasma treated aqueous solutions.The results indicate that both nitrate and nitrite concentrations increase with the plasma treatment time,and the nitrite species is found to be generated prior to the nitrate species in the air plasma treated aqueous solution.Moreover,the production rate of total nitrogen species is independent of the solutions’p H value.These results are relevant to diverse applications of plasma activated solutions in materials processing,biotechnology,medicine and other fields.
文摘With the rapid development of mobile Internet and intelligent devices,flexible electronic technology has attracted wide attention driven by the huge demand of the market.As one type of flexible electronic devices,flexible sensors have attracted great interest because of their promising prospects in artificial intelligence,medical health,and environmental protection.In recent years,flexible sensors with high sensitivity,selectivity,good deformability,reliable stability,and portability are urgently needed to meet the developments of artificial skin,human-computer interaction,point of care diagnostics and wearable electronic devices.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51772162)the Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technologythe Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)。
文摘Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.
基金partially supported by the Australian Research Council(ARC)the National Science Fund for Distinguished Young Scholars(grant number 51925703)。
文摘Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.
基金thankful for the support from the Australian Research Council(ARC)Linkage Project(LP200200689).
文摘Magnesium diboride(MgB_(2))magnets have the potential to be the next-generation liquid-helium-free magnet for magnetic resonance imaging(MRI)application due to their relatively high superconducting transition temperature,high current density and low raw material cost compared with current commercial niobium-titanium(Nb-Ti)magnets.A typical superconducting magnet includes several coils.To produce an ultra-stable magnetic field for imaging in MRI,a superconducting electromagnet operating in a persistent mode is crucial.Superconducting coils of the electromagnet in MRI are short-circuited to operate in the persistent mode by connecting coils with superconducting joints.Per-sistent joints have been demonstrated for in-situ and ex-situ wires of both mono-and multi-filamentary structures,made predominantly by PIT techniques similar to those used in wire production.To realise further engagement of MgB_(2)in MRI applications,enhancing the performance of MgB_(2)superconducting joints is essential.This literature review summarises research and development on MgB_(2)superconducting joining technology.
基金the financial support by the Australian Research Council.
文摘In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail over ADT and bond to CA due to its stronger triple H-bonding affiliation,forming hollow microtubes assembled by oriented CAM crystalline arrays,as guided by the directionality of peripheral hydrogen bonds.Furthermore,competitive interaction between hydrogen bonding and ionic/covalent bonding is demonstrated by mixing Ag+ions with the CA-ADT fibers,where sulfur atoms are abstracted from ADT molecules to produce Ag_(2)S ligaments.The in situ-formed Ag_(2)S serves as a binding glue to generate CA-ADT/Ag_(2)S composites with significantly enhanced mechanical strength compared to the pristine CA-ADT fiber pellet.
基金the support from the National Natural Science Foundation of China(21878271,51702284,21878270,and 21961160742)the Zhejiang Provincial Natural Science Foundation of China(LR19B060002)+8 种基金the Fundamental Research Funds for the Central Universitiesthe Startup Foundation for Hundred-Talent Program of Zhejiang Universitythe Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01006)Key Laboratory of Marine Materials and Related Technologies,CASZhejiang Key Laboratory of Marine Materials and Protective Technologies(2020K10)the support of the NSFC 21501138the Natural Science Foundation of Hubei Province(2019CFB556)Science Research Foundation of Wuhan Institute of Technology(K2019039)the Australian Research Council(ARC)and QUT Centre for Materials Science for partial support.
文摘Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.
