The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for ...The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.展开更多
Developing a simple scalable method to fabricate electrodes with high capacity and wide voltage range is desired for the real use of electrochemical supercapacitors.Herein,we synthesized amorphous NiCo-LDH nanosheets ...Developing a simple scalable method to fabricate electrodes with high capacity and wide voltage range is desired for the real use of electrochemical supercapacitors.Herein,we synthesized amorphous NiCo-LDH nanosheets vertically aligned on activated carbon cloth substrate,which was in situ transformed from Co-metal-organic framework materials nano-columns by a simple ion exchange process at room temperature.Due to the amorphous and vertically aligned ultrathin structure of NiCo-LDH,the NiCo-LDH/activated carbon cloth composites present high areal capacities of 3770 and 1480 mF cm^(-2)as cathode and anode at 2 mA cm^(-2),and 79.5%and 80%capacity have been preserved at 50 mA cm^(-2).In the meantime,they all showed excellent cycling performance with negligible change after>10000 cycles.By fabricating them into an asymmetric supercapacitor,the device achieves high energy densities(5.61 mWh cm^(-2)and 0.352 mW cm^(-3)).This work provides an innovative strategy for simplifying the design of supercapacitors as well as providing a new understanding of improving the rate capabilities/cycling stability of NiCo-LDH materials.展开更多
The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to C...The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.展开更多
Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis...Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis and modification of CNNs to improve their photocatalytic properties,and many exciting progresses have been gained.In order to elucidate the fundamentals of CNNs based catalysts and provide the insights into rational design of photocatalysis system,we describe recent progress made in CNNs preparation strategies and their applications in this review.Firstly,the physicochemical properties of CNNs are briefly introduced.Secondly,the synthesis approaches of CNNs are reviewed,including top-down stripping strategies(thermal,gas,liquid,and composite stripping)and bottom-up precursor molecules design strategies(solvothermal,template,and supramolecular self-assembly method).Subsequently,the modification strategies based on CNNs in recent years are discussed,including crystal structure design,doping,surface functionalization,constructing 2D heterojunction,and anchoring single-atom.Then the multifunctional applications of g-C_(3)N_(4) nanosheet based materials in photocatalysis including H_(2) evolution,O_(2) evolution,overall water splitting,H_(2)O_(2) production,CO_(2) reduction,N_(2) fixation,pollutant removal,organic synthesis,and sensing are highlighted.Finally,the opportunities and challenges for the development of high-performance CNNs photocatalytic systems are also prospected.展开更多
Liquid-phase exfoliation was employed to synthesize Sr_(2)Nb_(3)O_(10) perovskite nanosheets with thicknesses down to 1.76 nm.Transmission electron microscopy(TEM),atomic force microscope(AFM),X-ray photoelectron spec...Liquid-phase exfoliation was employed to synthesize Sr_(2)Nb_(3)O_(10) perovskite nanosheets with thicknesses down to 1.76 nm.Transmission electron microscopy(TEM),atomic force microscope(AFM),X-ray photoelectron spectrometer(XPS),and other characterization techniques were used to evaluate the atomic structure and chemical composition of the exfoliated nanosheets.A UV photodetector based on individual Sr_(2)Nb_(3)O_(10) nanosheets was prepared to demonstrate the application of an ultraviolet(UV) photodetector.The UV photodetector exhibited outstanding photocurrent and responsivity with a responsivity of 3×10^(5) A·W^(-1) at 5 V bias under 280 nm illumination,a photocurrent of 60 nA,and an on/off ratio of 3×10^(2).展开更多
The unique structural features of hard carbon(HC)make it a promising anode candidate for sodium-ion batteries(SIB).However,traditional methods of preparing HC require special equipment,long reaction times,and large en...The unique structural features of hard carbon(HC)make it a promising anode candidate for sodium-ion batteries(SIB).However,traditional methods of preparing HC require special equipment,long reaction times,and large energy consumption,resulting in low throughputs and efficiency.In our contribution,a novel synthesis method is proposed,involving the formation of HC nanosheets(NS-CNs)within minutes by creating an anoxic environment through flame combustion and further introducing sulfur and nitrogen sources to achieve heteroatom doping.The effect of heterogeneous element doping on the microstructure of HC is quantitatively analyzed by high-resolution transmission electron microscopy and image processing technology.Combined with density functional theory calculation,it is verified that the functionalized HC exhibits stronger Na^(+)adsorption ability,electron gain ability,and Na^(+) migration ability.As a result,NS-CNs as SIB anodes provide an ultrahigh reversible capacity of 542.7mAh g^(-1) at 0.1Ag^(-1),and excellent rate performance with a reversible capacity of 236.4mAh g^(-1) at 2Ag^(-1) after 1200 cycles.Furthermore,full cell assembled with NS-CNs as the can present 230mAh g^(-1) at 0.5Ag^(-1) after 150 cycles.Finally,in/ex situ techniques confirm that the excellent sodium storage properties of NS-CNs are due to the construction of abundant active sites based on the novel synthesis method for realizing the reversible adsorption of Na^(+).This work provides a novel strategy to develop novel carbons and gives deep insights for the further investigation of facile preparation methods to develop high-performance carbon anodes for alkali-ion batteries.展开更多
It has been demonstrated that almost all polymer-clay nanocomposites show higher temperature stability than that of pure polymer, which is attributed to the active exfoliated clay nanosheet firmly adsorbed onto the po...It has been demonstrated that almost all polymer-clay nanocomposites show higher temperature stability than that of pure polymer, which is attributed to the active exfoliated clay nanosheet firmly adsorbed onto the polymer chains, due to polerization and nucleation effect, the clay nanosheets could protect the polymer chains from destroying. To prove such mechanism, the water-soluble polymer nanocomposites(AAA/SLS-MMT) were synthesized by the in-situ polymerization of 2-acrylamide-2-methyl-propane sulfonic acid, acrylamide, 4-acryloylmorpholine, and organically modified montmorillonite. The techniques of nuclear magnetic resonance, atomic force microscopy and scanning electron microscopy etc., clearly characterized the successful synthesized of sample's structure, the exfoliated MMT nanosheet adsorbed polymer chain's scale, and well-dispersed morphology, espectively. The adsorption model, X-ray photoelectron spectroscopy presented the existence of strong adsorption, while molecular simulation calculations first concluded that the strong adsorption energy was-13032.06 kcal/mol. Thermo-gravimetric-analysis proved the temperature of maximum thermal degradation of powder sample(AAA/1.0 wt% SLS-MMT) was over 298℃. After ageing at 180℃ for 4 h, the apparent viscosity of 5 g/L AAA/1.0 wt% SLS-MMT aqueous solution was 326.7 mPa,s, while that of pure polymer(AAA) was only 8.3 mPa,s. This optimized sample has the smallest FLAPIvalue at all test temperatures from 180 to 220℃ in both fresh and salt water based drilling fluid. All the evidences of high temperature resistance indicate that the strong adsorption can enhance the thickness of hydrated shell and adsorption of clay particles in drilling fluid at high temperature. Such mechanism supplied the better way to design high-temperature resistant fluid loss additives for deep and ultra-deep oil and gas formation engineering.展开更多
As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the ...As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp^(3)-C/sp^(2)-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.展开更多
The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic tw...The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic two-dimensional material,possesses remarkable properties.However,its inherently wide bandgap significantly limits their potential for visible-light-responsive catalysis,and conventional chemical methods struggle to overcome this limitation.In this study,we employed high-energy ionizing radiation to precisely regulate defect formation in BNNS at ambient temperature and pressure.The results showed that gamma-ray radiation markedly enhanced the efficiency of photocatalytic hydrogen production of the irradiated BNNS with increasing absorbed dose.The maximum hydrogen production rate of the samples reached 1033.7μmol/(g·h),which represents an increase of almost two orders of magnitude compared to commercial BNNS.The structural characterization also confirmed that the introduction of three-boron-center defects results in forming intermediate energy levels and improving the charge carrier separation efficiency of BNNS.This transformation converts BNNS from a wide bandgap semiconductor to a visible-light-responsive catalyst.This work not only provides a novel approach for the application of BNNS in visible-light photocatalysis,but also demonstrates the unique role of radiation technology in quantitatively regulating defects and improving catalytic activity.展开更多
The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces c...The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.展开更多
Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheet...Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.展开更多
Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)...Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.展开更多
Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely li...Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.展开更多
As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,...As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,and straightforward surface functionalization.Therefore,they may replace Pt-based catalysts in oxygen reduction reaction(ORR)applications.Herein,a simple method is developed to design hierarchical nano-frame structures assembled via 2D NiO and N-doped graphene(NG)nanosheets.This procedure can yield nanostructures that satisfy the criteria correlated with improved electrocatalytic performance,such as large surface area,numerous undercoordinated atoms,and high defect densities.Further,porous NG nanosheet architectures,featuring NiO nanosheets densely coordinated with accessible holey Fe_(2)O_(3) moieties,can enhance mesoporosity and balance hydrophilicity.Such improvements can facilitate charge transport and expose formerly inaccessible reaction sites,maximizing active site density utilization.Density functional theory(DFT)calculations reveal favored O_(2) adsorption and dissociation on Fe_(2)O_(3) hybrid structures when supported by 2D NiO and NG nanomaterials,given 2D materials donated charge to Fe_(2)O_(3) active sites.Our systematic studies reveal that synergistic contributions are responsible for enriching the catalytic activity of Fe_(2)O_(3)@NiO/NG in alkaline media-encompassing internal voids and pores,unique hierarchical support structures,and concentrated N-dopant and bimetallic atomic interactions.Ultimately,this work expands the toolbox for designing and synthesizing highly efficient 2D/2D shelled functional nanomaterials with transition metals,endeavoring to benefit energy conversion and related ORR applications.展开更多
Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance...Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).展开更多
Porous graphitic carbon nitride(pg-C3N4) nanosheets have been prepared through a one-step ammonia thermopolymerization method.The effects of synthetic temperature on the structural,optical and photocatalytic propert...Porous graphitic carbon nitride(pg-C3N4) nanosheets have been prepared through a one-step ammonia thermopolymerization method.The effects of synthetic temperature on the structural,optical and photocatalytic properties of the samples have been investigated.Characterization results show that the heptazine-based conjugate heterocyclic structure was formed over 500℃,which is attributed to the inhibitory effect of ammonia from the decomposition of NH4SCN.Precise nanosheet morphology and an increased pore distribution with an enlarged surface area are observed for the samples obtained under high temperatures.Optical analysis results show that the bandgap of the samples widens and photoluminescene intensity is gradually quenched as the treating temperature is increased.The results demonstrate that a higher polymerization temperature improves the nanolayer structure,porosity and migration rate of the photo-induced carriers of the samples.The pg-C3N4 nanosheets prepared at 600℃ presents the highest photocatalytic activity for hydrogen evolution from water under visible-light irradiation.This study demonstrates a novel strategy for the synthesis and optimization of polymer semiconductor nanosheets with gratifying photocatalytic performance.展开更多
Petal-like ZnO nanosheets were synthesized with zinc nitrate hexahydrate and sodium hydroxide as starting materials in ammonia and ethanol mixture solution. RuO2 modified ZnO nanosheets were also prepared by a calcina...Petal-like ZnO nanosheets were synthesized with zinc nitrate hexahydrate and sodium hydroxide as starting materials in ammonia and ethanol mixture solution. RuO2 modified ZnO nanosheets were also prepared by a calcination route. The as-prepared products were characterized by X-ray powder diffraction and field emission scanning electron microscopy, and its specific BET surface area was calculated by nitrogen adsorption method. The sensitivity, response and recovery speed were examined. The results show that RuO2 modified petal-like ZnO based sensor exhibits a high sensitivity, a low detection limit, fast response and recovery properties to ethanol and acetone. The sensitivities of the RuO2 modified petal-like ZnO based sensor to 100×10^-6 ethanol and acetone at 360 °C are 33 and 67, respectively. The response and recovery times of the sensor are 4 s and 9 s to 10×10^-6 ethanol, and are 3 s and 10 s to 10×10^-6 acetone, respectively.展开更多
Vanadium (III) phosphate monoclinic VPO4·H2O was synthesized hydrothermally. The ε-VOPO4 nanosheets, formed by the oxidative de-intercalation of protons from monoclinic VPO4·H2O, can reversibly react wit...Vanadium (III) phosphate monoclinic VPO4·H2O was synthesized hydrothermally. The ε-VOPO4 nanosheets, formed by the oxidative de-intercalation of protons from monoclinic VPO4·H2O, can reversibly react with more than 1 mol lithium atoms in two steps. Crystal XRD analysis revealed that the structure of the ε-VOPO4 nanosheets is monoclinic with lattice parameters of α=7.2588(4) A, b=6.8633(2) A and c=7.2667(4) A. The results show that the ε-VOPO4 nanosheets have a thickness of 200 nm and uniform crystallinity. Electrochemical characterization of the ε-VOPO4 monoclinic nanosheets reveals that they have good electrochemical properties at high current density, and deliver high initial capacity of 230.3 mA· h/g at a current density of 0.09 mA/cm2. Following the first charge cycle, reversible electrochemical lithium extraction/insertion at current density of 0.6 mA/cm2 affords a capacity retention rate of 73.6% (2.0?4.3 V window) that is stable for at least 1000 cycles.展开更多
The mechanical and tribological properties of hot-pressed copper-based composites containing different amounts of graphene nanosheets(GNSs) are compared with those of copper-graphite(Gr) composites fabricated by t...The mechanical and tribological properties of hot-pressed copper-based composites containing different amounts of graphene nanosheets(GNSs) are compared with those of copper-graphite(Gr) composites fabricated by the same method.The results show that the Cu-GNSs composites exhibit higher relative density,microhardness and bending strength compared with Cu-Gr composites with the same volume fraction of GNSs and Gr.Moreover,the friction coefficients and wear rates reduce significantly by the addition of GNSs,whereas the limited impact on reducing friction and wear is found on graphite.The abrasive and delamination wear are the dominant wear mechanisms of the composites.It is believed that the superior mechanical and tribological performances of Cu-GNSs composites are attributed to the unique strengthening effect as well as the higher lubricating efficiency of graphene nanosheets compared with those of graphite,which demonstrates that GNS is an ideal filler for copper matrix composites,acting as not only an impactful lubricant but also a favorable reinforcement.展开更多
Two-dimensional (2D) layered vanadium disulfide (VS2) is a promising anode material for lithium ion batteries (LIBs) due to the high theoretical capacity.However,it remains a challenge to synthesize monodispersed ultr...Two-dimensional (2D) layered vanadium disulfide (VS2) is a promising anode material for lithium ion batteries (LIBs) due to the high theoretical capacity.However,it remains a challenge to synthesize monodispersed ultrathin VS2 nanosheets to realize the full potential.Herein,a novel solvothermal method has been developed to prepare the monodispersed bowl-shaped NH3-inserted VS2 nanosheets (VS2).The formation of such a unique structure is caused by the blocked growth of (001) or (002) crystal planes in combination with a ripening process driven by the thermodynamics.The annealing treatment in Ar/H2creates porous monodispersed VS2(H-VS2),which is subsequently integrated with graphene oxide to form porous monodispersed H-VS2/rGO composite coupled with a reduction process.As an anode material for LIBs,H-VS2/rGO delivers superior rate performance and longer cycle stability:a high average capacity of 868/525 mAh g^-1 at a current density of 1/10 A g^-1;a reversible capacity of 1177/889 mAh g^-1 after 150/500 cycles at 0.2/1 A g^-1.Such excellent electrochemical performance may be attributed to the increased active sites available for lithium storage,the alleviated volume variations and the shortened Li-ion diffusion induced from the porous structure with large specific surface area,as well as the protective effect from graphene nanosheets.展开更多
基金supported by the National Natural Science Foundation of China(22108238,21878259)the Zhejiang Provincial Natural Science Foundation of China(LR18B060001)+5 种基金Anhui Provincial Natural Science Founda-tion(1908085QB68)the Natural Science Foundation of the Anhui Higher Education Institutions of China(KJ2020A0275)Major Science and Technology Project of Anhui Province(201903a05020055)Foundation of Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology(ZJKL-ACEMT-1802)China Postdoctoral Science Foundation(2019M662060,2020T130580)Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology(BM2012110).
文摘The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.
基金the funding from Natural Science Foundation of China(No.52003163)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515010670)+1 种基金Science and Technology Innovation Commission of Shenzhen(Nos.KQTD20170810105439418 and 20200812112006001)NTUT-SZU Joint Research Program(Nos.2022005 and 2022015)
文摘Developing a simple scalable method to fabricate electrodes with high capacity and wide voltage range is desired for the real use of electrochemical supercapacitors.Herein,we synthesized amorphous NiCo-LDH nanosheets vertically aligned on activated carbon cloth substrate,which was in situ transformed from Co-metal-organic framework materials nano-columns by a simple ion exchange process at room temperature.Due to the amorphous and vertically aligned ultrathin structure of NiCo-LDH,the NiCo-LDH/activated carbon cloth composites present high areal capacities of 3770 and 1480 mF cm^(-2)as cathode and anode at 2 mA cm^(-2),and 79.5%and 80%capacity have been preserved at 50 mA cm^(-2).In the meantime,they all showed excellent cycling performance with negligible change after>10000 cycles.By fabricating them into an asymmetric supercapacitor,the device achieves high energy densities(5.61 mWh cm^(-2)and 0.352 mW cm^(-3)).This work provides an innovative strategy for simplifying the design of supercapacitors as well as providing a new understanding of improving the rate capabilities/cycling stability of NiCo-LDH materials.
基金Natural Science Foundation of Shandong Province,Grant/Award Number:ZR2022MB106national training program of innovation and entrepreneurship for undergraduates,Grant/Award Number:202210424099National Natural Science Foundation of China,Grant/Award Numbers:21601067,21701057,21905147。
文摘The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.
基金supported by the National Natural Science Foundation of China(22172195)Central South University Graduate Students Independent Exploration and Innovation Project(2023ZZTS0736 and 2023ZZTS0760).
文摘Graphitic carbon nitride nanosheets(CNNs)become the most promising member in the carbon nitride family benefitted from their two-dimensional structural features.Recently,great endeavors have been made in the synthesis and modification of CNNs to improve their photocatalytic properties,and many exciting progresses have been gained.In order to elucidate the fundamentals of CNNs based catalysts and provide the insights into rational design of photocatalysis system,we describe recent progress made in CNNs preparation strategies and their applications in this review.Firstly,the physicochemical properties of CNNs are briefly introduced.Secondly,the synthesis approaches of CNNs are reviewed,including top-down stripping strategies(thermal,gas,liquid,and composite stripping)and bottom-up precursor molecules design strategies(solvothermal,template,and supramolecular self-assembly method).Subsequently,the modification strategies based on CNNs in recent years are discussed,including crystal structure design,doping,surface functionalization,constructing 2D heterojunction,and anchoring single-atom.Then the multifunctional applications of g-C_(3)N_(4) nanosheet based materials in photocatalysis including H_(2) evolution,O_(2) evolution,overall water splitting,H_(2)O_(2) production,CO_(2) reduction,N_(2) fixation,pollutant removal,organic synthesis,and sensing are highlighted.Finally,the opportunities and challenges for the development of high-performance CNNs photocatalytic systems are also prospected.
基金Funded by the National Natural Science Foundation of China(Nos.51872214 and 52172124)the Fundamental Research Funds for the Central Universities(WUT:2021Ⅲ019JC and 2018Ⅲ041GX)。
文摘Liquid-phase exfoliation was employed to synthesize Sr_(2)Nb_(3)O_(10) perovskite nanosheets with thicknesses down to 1.76 nm.Transmission electron microscopy(TEM),atomic force microscope(AFM),X-ray photoelectron spectrometer(XPS),and other characterization techniques were used to evaluate the atomic structure and chemical composition of the exfoliated nanosheets.A UV photodetector based on individual Sr_(2)Nb_(3)O_(10) nanosheets was prepared to demonstrate the application of an ultraviolet(UV) photodetector.The UV photodetector exhibited outstanding photocurrent and responsivity with a responsivity of 3×10^(5) A·W^(-1) at 5 V bias under 280 nm illumination,a photocurrent of 60 nA,and an on/off ratio of 3×10^(2).
基金supported by the National Natural Science Foundation of China (Grant Nos.51872236,52072307)MOE SUTD Kickstarter Innitiative (SKI 2021_02_16).
文摘The unique structural features of hard carbon(HC)make it a promising anode candidate for sodium-ion batteries(SIB).However,traditional methods of preparing HC require special equipment,long reaction times,and large energy consumption,resulting in low throughputs and efficiency.In our contribution,a novel synthesis method is proposed,involving the formation of HC nanosheets(NS-CNs)within minutes by creating an anoxic environment through flame combustion and further introducing sulfur and nitrogen sources to achieve heteroatom doping.The effect of heterogeneous element doping on the microstructure of HC is quantitatively analyzed by high-resolution transmission electron microscopy and image processing technology.Combined with density functional theory calculation,it is verified that the functionalized HC exhibits stronger Na^(+)adsorption ability,electron gain ability,and Na^(+) migration ability.As a result,NS-CNs as SIB anodes provide an ultrahigh reversible capacity of 542.7mAh g^(-1) at 0.1Ag^(-1),and excellent rate performance with a reversible capacity of 236.4mAh g^(-1) at 2Ag^(-1) after 1200 cycles.Furthermore,full cell assembled with NS-CNs as the can present 230mAh g^(-1) at 0.5Ag^(-1) after 150 cycles.Finally,in/ex situ techniques confirm that the excellent sodium storage properties of NS-CNs are due to the construction of abundant active sites based on the novel synthesis method for realizing the reversible adsorption of Na^(+).This work provides a novel strategy to develop novel carbons and gives deep insights for the further investigation of facile preparation methods to develop high-performance carbon anodes for alkali-ion batteries.
基金financially supported by the National Major Project (No. 2017ZX05009-003,50)National Natural Science Foundation of China (No. 51974339+2 种基金51674270)Foreign Expert Project of the Belt and Road Innovation Talents Exchange (DL2022122001)the Research Institute of Petroleum Exploration Development of China National Petroleum Cooperation (HX20201095)。
文摘It has been demonstrated that almost all polymer-clay nanocomposites show higher temperature stability than that of pure polymer, which is attributed to the active exfoliated clay nanosheet firmly adsorbed onto the polymer chains, due to polerization and nucleation effect, the clay nanosheets could protect the polymer chains from destroying. To prove such mechanism, the water-soluble polymer nanocomposites(AAA/SLS-MMT) were synthesized by the in-situ polymerization of 2-acrylamide-2-methyl-propane sulfonic acid, acrylamide, 4-acryloylmorpholine, and organically modified montmorillonite. The techniques of nuclear magnetic resonance, atomic force microscopy and scanning electron microscopy etc., clearly characterized the successful synthesized of sample's structure, the exfoliated MMT nanosheet adsorbed polymer chain's scale, and well-dispersed morphology, espectively. The adsorption model, X-ray photoelectron spectroscopy presented the existence of strong adsorption, while molecular simulation calculations first concluded that the strong adsorption energy was-13032.06 kcal/mol. Thermo-gravimetric-analysis proved the temperature of maximum thermal degradation of powder sample(AAA/1.0 wt% SLS-MMT) was over 298℃. After ageing at 180℃ for 4 h, the apparent viscosity of 5 g/L AAA/1.0 wt% SLS-MMT aqueous solution was 326.7 mPa,s, while that of pure polymer(AAA) was only 8.3 mPa,s. This optimized sample has the smallest FLAPIvalue at all test temperatures from 180 to 220℃ in both fresh and salt water based drilling fluid. All the evidences of high temperature resistance indicate that the strong adsorption can enhance the thickness of hydrated shell and adsorption of clay particles in drilling fluid at high temperature. Such mechanism supplied the better way to design high-temperature resistant fluid loss additives for deep and ultra-deep oil and gas formation engineering.
文摘As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp^(3)-C/sp^(2)-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.
文摘The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic two-dimensional material,possesses remarkable properties.However,its inherently wide bandgap significantly limits their potential for visible-light-responsive catalysis,and conventional chemical methods struggle to overcome this limitation.In this study,we employed high-energy ionizing radiation to precisely regulate defect formation in BNNS at ambient temperature and pressure.The results showed that gamma-ray radiation markedly enhanced the efficiency of photocatalytic hydrogen production of the irradiated BNNS with increasing absorbed dose.The maximum hydrogen production rate of the samples reached 1033.7μmol/(g·h),which represents an increase of almost two orders of magnitude compared to commercial BNNS.The structural characterization also confirmed that the introduction of three-boron-center defects results in forming intermediate energy levels and improving the charge carrier separation efficiency of BNNS.This transformation converts BNNS from a wide bandgap semiconductor to a visible-light-responsive catalyst.This work not only provides a novel approach for the application of BNNS in visible-light photocatalysis,but also demonstrates the unique role of radiation technology in quantitatively regulating defects and improving catalytic activity.
基金partial support from the Jiujiang Research Institute at Xiamen University.
文摘The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
基金supported by the Research Funds of Institute of Zhejiang University-Quzhou(IZQ2023RCZX032)the Natural Science Foundation of Guangdong Province(2022A1515010185)+1 种基金the Fundamental Research Funds for the Central Universities(FRF-TP-20-005A3)partially supported by the Special Funds for Postdoctoral Research at Tsinghua University(100415017)。
文摘Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.
基金supported by the National Natural Science Foundation of China(21571038,22035004)the Education Department of Guizhou Province(2021312)+2 种基金the Foundation of Guizhou Province(2019-5666)the National Key R&D Program of China(2017YFA0700101)the State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University,202009)。
文摘Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.
基金supported by the National Natural Science Foundation of China(11872171 and 22209037)the Project on Excellent Post-graduate Dissertation of Hohai University。
文摘Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.
基金supported by the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(MSIT)(RS2023-00235596)and ERC Center(2022R1A5A1033719)。
文摘As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,and straightforward surface functionalization.Therefore,they may replace Pt-based catalysts in oxygen reduction reaction(ORR)applications.Herein,a simple method is developed to design hierarchical nano-frame structures assembled via 2D NiO and N-doped graphene(NG)nanosheets.This procedure can yield nanostructures that satisfy the criteria correlated with improved electrocatalytic performance,such as large surface area,numerous undercoordinated atoms,and high defect densities.Further,porous NG nanosheet architectures,featuring NiO nanosheets densely coordinated with accessible holey Fe_(2)O_(3) moieties,can enhance mesoporosity and balance hydrophilicity.Such improvements can facilitate charge transport and expose formerly inaccessible reaction sites,maximizing active site density utilization.Density functional theory(DFT)calculations reveal favored O_(2) adsorption and dissociation on Fe_(2)O_(3) hybrid structures when supported by 2D NiO and NG nanomaterials,given 2D materials donated charge to Fe_(2)O_(3) active sites.Our systematic studies reveal that synergistic contributions are responsible for enriching the catalytic activity of Fe_(2)O_(3)@NiO/NG in alkaline media-encompassing internal voids and pores,unique hierarchical support structures,and concentrated N-dopant and bimetallic atomic interactions.Ultimately,this work expands the toolbox for designing and synthesizing highly efficient 2D/2D shelled functional nanomaterials with transition metals,endeavoring to benefit energy conversion and related ORR applications.
基金the National Science Fund for Distinguished Young Scholars(Grant No.52125103)the National Natural Science Foundation of China(Grant Nos.52301232,52071041,12074048,and 12147102)China Postdoctoral Science Foundation(Grant No.2022M720552).
文摘Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).
基金supported by the National Natural Science Foundation of China(21503096)the Natural Science Foundation of Jiangsu Province(BK20140507)~~
文摘Porous graphitic carbon nitride(pg-C3N4) nanosheets have been prepared through a one-step ammonia thermopolymerization method.The effects of synthetic temperature on the structural,optical and photocatalytic properties of the samples have been investigated.Characterization results show that the heptazine-based conjugate heterocyclic structure was formed over 500℃,which is attributed to the inhibitory effect of ammonia from the decomposition of NH4SCN.Precise nanosheet morphology and an increased pore distribution with an enlarged surface area are observed for the samples obtained under high temperatures.Optical analysis results show that the bandgap of the samples widens and photoluminescene intensity is gradually quenched as the treating temperature is increased.The results demonstrate that a higher polymerization temperature improves the nanolayer structure,porosity and migration rate of the photo-induced carriers of the samples.The pg-C3N4 nanosheets prepared at 600℃ presents the highest photocatalytic activity for hydrogen evolution from water under visible-light irradiation.This study demonstrates a novel strategy for the synthesis and optimization of polymer semiconductor nanosheets with gratifying photocatalytic performance.
基金Projects(61079010)supported by the National Natural Science Foundation of China and the Civil Aviation Administration of ChinaProject(3122013P001)supported by the Significant Pre-research Funds of Civil Aviation University of ChinaProject(2014)supported by the Science and Technology Innovation Guide Funds of Civil Aviation Administration of China
文摘Petal-like ZnO nanosheets were synthesized with zinc nitrate hexahydrate and sodium hydroxide as starting materials in ammonia and ethanol mixture solution. RuO2 modified ZnO nanosheets were also prepared by a calcination route. The as-prepared products were characterized by X-ray powder diffraction and field emission scanning electron microscopy, and its specific BET surface area was calculated by nitrogen adsorption method. The sensitivity, response and recovery speed were examined. The results show that RuO2 modified petal-like ZnO based sensor exhibits a high sensitivity, a low detection limit, fast response and recovery properties to ethanol and acetone. The sensitivities of the RuO2 modified petal-like ZnO based sensor to 100×10^-6 ethanol and acetone at 360 °C are 33 and 67, respectively. The response and recovery times of the sensor are 4 s and 9 s to 10×10^-6 ethanol, and are 3 s and 10 s to 10×10^-6 acetone, respectively.
基金Projects(51172065,51404097,51504083,U1404613)supported by the National Natural Science Foundation of ChinaProject(16A150009)supported by the Key Scientific Research Project for Higher Education of Henan Province,China+2 种基金Project(16A150009)supported by the Natural Science Foundation of Henan Province(General Program)ChinaProject(166115)supported by the Postdoctoral Science Foundation of Henan Province,China
文摘Vanadium (III) phosphate monoclinic VPO4·H2O was synthesized hydrothermally. The ε-VOPO4 nanosheets, formed by the oxidative de-intercalation of protons from monoclinic VPO4·H2O, can reversibly react with more than 1 mol lithium atoms in two steps. Crystal XRD analysis revealed that the structure of the ε-VOPO4 nanosheets is monoclinic with lattice parameters of α=7.2588(4) A, b=6.8633(2) A and c=7.2667(4) A. The results show that the ε-VOPO4 nanosheets have a thickness of 200 nm and uniform crystallinity. Electrochemical characterization of the ε-VOPO4 monoclinic nanosheets reveals that they have good electrochemical properties at high current density, and deliver high initial capacity of 230.3 mA· h/g at a current density of 0.09 mA/cm2. Following the first charge cycle, reversible electrochemical lithium extraction/insertion at current density of 0.6 mA/cm2 affords a capacity retention rate of 73.6% (2.0?4.3 V window) that is stable for at least 1000 cycles.
文摘The mechanical and tribological properties of hot-pressed copper-based composites containing different amounts of graphene nanosheets(GNSs) are compared with those of copper-graphite(Gr) composites fabricated by the same method.The results show that the Cu-GNSs composites exhibit higher relative density,microhardness and bending strength compared with Cu-Gr composites with the same volume fraction of GNSs and Gr.Moreover,the friction coefficients and wear rates reduce significantly by the addition of GNSs,whereas the limited impact on reducing friction and wear is found on graphite.The abrasive and delamination wear are the dominant wear mechanisms of the composites.It is believed that the superior mechanical and tribological performances of Cu-GNSs composites are attributed to the unique strengthening effect as well as the higher lubricating efficiency of graphene nanosheets compared with those of graphite,which demonstrates that GNS is an ideal filler for copper matrix composites,acting as not only an impactful lubricant but also a favorable reinforcement.
基金the Natural Science Foundation of Hunan Province(Grant no.2017JJ1008)the Key Research and Development Program of Hunan Province of China under Grant 2018GK2031。
文摘Two-dimensional (2D) layered vanadium disulfide (VS2) is a promising anode material for lithium ion batteries (LIBs) due to the high theoretical capacity.However,it remains a challenge to synthesize monodispersed ultrathin VS2 nanosheets to realize the full potential.Herein,a novel solvothermal method has been developed to prepare the monodispersed bowl-shaped NH3-inserted VS2 nanosheets (VS2).The formation of such a unique structure is caused by the blocked growth of (001) or (002) crystal planes in combination with a ripening process driven by the thermodynamics.The annealing treatment in Ar/H2creates porous monodispersed VS2(H-VS2),which is subsequently integrated with graphene oxide to form porous monodispersed H-VS2/rGO composite coupled with a reduction process.As an anode material for LIBs,H-VS2/rGO delivers superior rate performance and longer cycle stability:a high average capacity of 868/525 mAh g^-1 at a current density of 1/10 A g^-1;a reversible capacity of 1177/889 mAh g^-1 after 150/500 cycles at 0.2/1 A g^-1.Such excellent electrochemical performance may be attributed to the increased active sites available for lithium storage,the alleviated volume variations and the shortened Li-ion diffusion induced from the porous structure with large specific surface area,as well as the protective effect from graphene nanosheets.