A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liqu...A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liquid-phase carbonization of isotropic pitch to the emergence of carbon microbeads in the matrix and finally their growth to form a 100%anisotropic bulk meso-phase,but rather a reverse transformation.The effects of C_(60) loading and reaction temperature on the morphological transformation of mesophase were investigated by polarizing optical and scanning electron microscopies.The physical changes in the NMP induced by C_(60) were characterized by thermogravimetric analysis,Fourier transform infrared spectroscopy,X-ray diffractometry and Raman spectroscopy.The results show that the coalesced NMP can be converted to a spherical type at 300-320℃ with the addition of 5%C_(60),and the size of the mesophase microbeads increases with increasing temperature.Furthermore,a model is established to ex-plain the unique induction effect of C_(60) in the transformation process.This work makes the morphological transformation of MP con-trollable,and provides a new idea for the understanding and research of mesophase pitch.展开更多
Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries(LSBs).Phase transformation of MoSe_(2) from the 2H phase ...Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries(LSBs).Phase transformation of MoSe_(2) from the 2H phase to the 1T phase has been proven to be a significant method to improve the catalytic activity.However,precisely controllable phase engineering of MoSe_(2) has rarely been reported.Herein,by in situ Li ions intercalation in MoSe_(2),a precisely controllable phase evolution from 2H-MoSe_(2) to 1T-MoSe_(2) was realized.More importantly,the definite functional relationship between cut-off voltage and phase structure was first identified for phase engineering through in situ observation and modulation methods.The sulfur host(CNFs/1T-MoSe_(2))presents high charge density,strong polysulfides adsorption,and catalytic kinetics.Moreover,Li-S cells based on it display capacity retention of 875.3mAh g^(-1) after 500 cycles at 1 C and an areal capacity of 8.71mAh cm^(-2) even at a high sulfur loading of 8.47mg cm^(-2).Furthermore,the flexible pouch cell exhibiting decent performance will endow a promising potential in the wearable energy storage field.This study proposes an effective strategy to precisely control the phase structure of MoSe_(2),which may provide the reference to fabricate the highly efficient electrocatalysts for LSBs and other energy systems.展开更多
MXenes are under the spotlight due to their versatile physicochemical characteristics. Since their discovery in 2011, significant advancements have been achieved in their synthesis and application sectors. However, th...MXenes are under the spotlight due to their versatile physicochemical characteristics. Since their discovery in 2011, significant advancements have been achieved in their synthesis and application sectors. However, the spontaneous oxidation of MXenes, which is critical to its processing and product lifespan, has gotten less attention due to its chemical complexity and poorly understood oxidation mechanism. This perspective focuses on the oxidation stability of MXenes and addresses the most recent advancements in understanding and the possible countermeasures to limit the spontaneous oxidation of MXenes. A section is dedicated to the presently accessible methods for monitoring oxidation, with a discussion on the debatable oxidation mechanism and coherently operating factors that contribute to the complexity of MXenes oxidation. The current potential solutions for mitigating MXenes oxidation and the existing challenges are also discussed with prospects to prolong MXene's shelf-life storage and expand their application scope.展开更多
The addition of 2,5-pyridinedicarboxylic acid(2,5-PDCA)to the Mg-Al LDH coating,which was prepared by one-step hydrothermal synthesis,had extremely enhanced the corrosion protection of AZ31 Mg alloy,although the 2,5-P...The addition of 2,5-pyridinedicarboxylic acid(2,5-PDCA)to the Mg-Al LDH coating,which was prepared by one-step hydrothermal synthesis,had extremely enhanced the corrosion protection of AZ31 Mg alloy,although the 2,5-PDCA could not be intercalated into the interlayer spacing.The corrosion current density of 0.05 mol L^(−1)2,5-PDCA LDH containing LDH coating is 3.18 nA cm^(−2),reduced by two orders of magnitude compared to the LDH coating without inhibitor,and the corrosion inhibition efficiency of the coating is 98.05%.The coating formed on the surface of AZ31 was peeled off from the substrate by using a mechanical method and SEM observation of the cross-section showed that the coating consisted of three different layers.The innermost layer is a thick layer that consists of Mg(OH)_(2)and the intermediate layer is LDH,which is vertical to the substrate and the outmost layer is a thin but very dense deposit layer of LDH agglomerates with complexes of 2,5-PDCA and Mg.This kind of sediment/LDH/Mg(OH)_(2)three-layer composite structure was accountable for the increase in the corrosion resistance of AZ31 Mg alloy.展开更多
Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic wat...Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic water oxidation.Herein,lotus root-like RuIr alloys with native micro-strain were constructed by an epitaxial growth of Ru-richened hcp-(0001)branches on Ir-richened fcc-(111)seeds using a polyol thermal synthesis strategy.The resultant Ru_(60)Ir_(40) alloy shows an OER overpotential of 197 mV at 10 mA cm^(-2) and a Tafel slope of 46.59 mV dec^(-1),showing no obvious activity decay for 80 h continuous chronopotentiometry test in 0.5 M H_(2)SO_(4).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy and density functional theory(DFT)calculations show that that the remarkably improved activity of the lotus root-like alloy can be attributed to the(0001)facet-triggered strain,which can efficiently optimize the electronic band structure of the active metal and the weakening of the chemisorption of oxygen-containing substances to boost OER electrocatalysis.Therefore,this work provides a new strategy to designing a class of advanced electrocatalysts with high strain using diverse nanostructures as building materials for carbon-free clean energy conversion systems.展开更多
MXenes,a new family of two-dimensional(2D)materials with excellent electronic conductivity and hydrophilicity,have shown distinctive advantages as a highly conductive matrix material for lithium-ion battery anodes.Her...MXenes,a new family of two-dimensional(2D)materials with excellent electronic conductivity and hydrophilicity,have shown distinctive advantages as a highly conductive matrix material for lithium-ion battery anodes.Herein,a facile electrostatic self-assembly of SnO2 quantum dots(QDs)on Ti3C2Tx MXene sheets is proposed.The as-prepared SnO2/MXene hybrids have a unique 0D-2D structure,in which the 0D SnO2 QDs(~4.7 nm)are uniformly distributed over 2D Ti3C2Tx MXene sheets with controllable loading amount.The SnO2 QDs serve as a high capacity provider and the“spacer”to prevent the MXene sheets from restacking;the highly conductive Ti3C2Tx MXene can not only provide efficient pathways for fast transport of electrons and Li ions,but also buffer the volume change of SnO2 during lithiation/delithiation by confining SnO2 QDs between the MXene nanosheets.Therefore,the 0D-2D SnO2 QDs/MXene hybrids deliver superior lithium storage properties with high capacity(887.4 mAh g?1 at 50 mA g?1),stable cycle performance(659.8 mAh g?1 at 100 mA g?1 after 100 cycles with a capacity retention of 91%)and excellent rate performance(364 mAh g?1 at 3 A g?1),making it a promising anode material for lithium-ion batteries.展开更多
Sodium-ion batteries(SIBs)have attracted significant attentions as promising alternatives to lithium-ion batteries for large-scale energy storage applications.Here carbon materials are considered as the most competiti...Sodium-ion batteries(SIBs)have attracted significant attentions as promising alternatives to lithium-ion batteries for large-scale energy storage applications.Here carbon materials are considered as the most competitive anodes for SIBs based on their low-cost,abundant availability and excellent structural stability.Pitch,with high carbon content and low cost,is an ideal raw precursor to prepare carbon materials for large-scale applications.Nevertheless,the microstructures of pitch-based carbon are highly ordered with smaller interlayer distances,which are unfavorable for Na ion storage.Many efforts have been made to improve the sodium storage performance of pitch-based carbon materials.This review summarizes the recent progress about the application of pitch-based carbons for SIBs anodes in the context of carbon’s morphology and structure regulation strategies,including morphology adjustment,heteroatoms doping,fabricating heterostructures,and the increase of the degree of disorder.Besides,the advantages,present challenges,and possible solutions to current issues in pitch-based carbon anode are discussed,with the highlight of future research directions.This review will provide a deep insight into the development of low-cost and high-performance pitch-based carbon anode for SIBs.展开更多
The growing energy concern all over the world has recognized hydrogen energy as the most promising renewable energy sources.Recently,electrocatalytic hydrogen evolution reaction(HER)by water splitting has been extensi...The growing energy concern all over the world has recognized hydrogen energy as the most promising renewable energy sources.Recently,electrocatalytic hydrogen evolution reaction(HER)by water splitting has been extensively studied with a focus on developing efficient electrocatalysts that can afford HER at overpotential with minimum power consumption.The two-dimensional transition metal carbides and nitride,also known as MXenes,are becoming the rising star in developing efficient electrocatalysts for HER,owing to their integrated chemical and electronic properties,e.g.,metallic conductivity,variety of redox-active transition metals,high hydrophilicity,and tunable surface functionalities.In this review,the recent progress about the fundamental understanding and materials engineering of MXenes-based electrocatalysts is summarized in concern with two aspects:i)the regulation of the intrinsic properties of MXenes,which include the composition,surface functionality,and defects;and ii)MXenes-based composites for HER process.In the end,we summarize the present challenges concerning the efficiency of MXenes-based HER electrocatalysts and propose the directions of future research efforts.展开更多
ZnS has great potentials as an anode for lithium storage because of its high theoretical capacity and resource abundance;however,the large volume expansion accompanied with structural collapse and low conductivity of ...ZnS has great potentials as an anode for lithium storage because of its high theoretical capacity and resource abundance;however,the large volume expansion accompanied with structural collapse and low conductivity of ZnS cause severe capacity fading and inferior rate capability during lithium storage. Herein,0D-2 D ZnS nanodots/Ti_(3)C_(2)T_x MXene hybrids are prepared by anchoring ZnS nanodots on Ti_(3)C_(2)T_(x) MXene nanosheets through coordination modulation between MXene and MOF precursor(ZIF-8) followed with sulfidation. The MXene substratecoupled with the ZnS nanodots can synergistically accommodate volume variation of ZnS over charge–discharge to realize stable cyclability. As revealed by XPS characterizations and DFT calculations,the strong interfacial interaction between ZnS nanodots and MXene nanosheets can boost fast electron/lithium-ion transfer to achieve excellent electrochemical activity and kinetics for lithium storage. Thereby,the as-prepared ZnS nanodots/MXene hybrid exhibits a high capacity of 726.8 mAh g^(-1) at 30 mA g^(-1),superior cyclic stability(462.8 mAh g^(-1) after 1000 cycles at 0.5 A g^(-1)),and excellent rate performance. The present results provide new insights into the understanding of the lithium storage mechanism of ZnS and the revealing of the e ects of interfacial interaction on lithium storage performance enhancement.展开更多
MXene nanosheets have been used for preparing highly flexible integrated electrodes due to their two-dimensional(2D)morphology,flexibility,high conductivity,and abundant functional groups.However,restacking of 2D nano...MXene nanosheets have been used for preparing highly flexible integrated electrodes due to their two-dimensional(2D)morphology,flexibility,high conductivity,and abundant functional groups.However,restacking of 2D nanosheets inhibits the ion transport in MXene electrodes,limiting their thickness,rate performance,and energy storage capacity.Here,we employed a natural sedimentation method instead of the conventional vacuum-assisted filtration to prepare flexible Ti3C2TxMXene films with enlarged interlayer spacing,which facilitates the access of the lithium ions to the interlayers and thus leads to a greatly enhanced electrochemical performance.The naturally sedimented flexible film shows a double lithium storage capacity compared to the conventional vacuum-filtered MXene film,along with improved rate performance and excellent cycle stability.展开更多
The effect of particle size on the density and resistivity of ITO green bodies and targets was systematically investigated.The experimental results show that the relative density of ITO green bodies decreases with the...The effect of particle size on the density and resistivity of ITO green bodies and targets was systematically investigated.The experimental results show that the relative density of ITO green bodies decreases with the increase of ITO particle size.When the particle size is 10.7 nm,the relative density of ITO green bodies rises to the maximum value of 56.6%.The resistivity declines exponentially with the increase of particle size,which satisfies the exponential equation of R=exp(-41.823 × d).When the particle size is 41.6 nm,the resistivity reaches the minimum value of 0.8 Ω·cm.The relative density of ITO target decreases with the increase of particle size.Fine particles can increase the driving force of densification in initial stage.Electron mobility,caused by grain boundary scattering,will increase due to the increase of particle size or the decrease of grain boundary potential.When the particle size is 10.7 nm,the target with compact grain stacking and low porosity shows a maximum relative density of 99.25%,and the resistivity reaches the minimum value of 0.34×10^-3 Ω·cm.展开更多
2D MXene nanosheets with metallic conductivity and high pseudo-capacitance are promising electrode materials for supercapacitors.Especially,MXene films can be directly used as electrodes for flexible supercapacitors.H...2D MXene nanosheets with metallic conductivity and high pseudo-capacitance are promising electrode materials for supercapacitors.Especially,MXene films can be directly used as electrodes for flexible supercapacitors.However,they suffer from sluggish ion transport due to self-restacking,causing limited electrochemical performance.Herein,a flexible 3D porous MXene film is fabricated by incorporating graphene oxide(GO) into MXene film followed by self-propagating reduction.The self-propagating process is facile and effective,which can be accomplished in 1.25 s and result in 3D porous framework by releasing substantial gas instantaneously.As the 3D porous structure provides massive ion-accessible active sites and promotes fast ion transport,the MXene-rGO films exhibit superior capacitance and rate performance.With the rGO content of 20%,the MXene-rGO-20 film delivers a high capacitance of 329.9 F g^(-1) at 5 mV s^(-1) in 3 M H2 SO4 electrolyte and remains 260.1 F g^(-1) at 1,000 mV s^(-1) as well as good flexibility.Furthermore,the initial capacitance is retained above 90% after 40,000 cycles at 100 A g^(-1),revealing good cycle stability.This work not only provides a high-performance flexible electrode for supercapacitors,but also proposes an efficient and time-saving strategy for constructing 3D structure from 2D materials.展开更多
Li metal,possessing advantages of high theoretical specific capacity and low electrochemical potential,is regarded as the most promising anode material for next-generation batteries.However,despite decades of intensiv...Li metal,possessing advantages of high theoretical specific capacity and low electrochemical potential,is regarded as the most promising anode material for next-generation batteries.However,despite decades of intensive research,its practical application is still hindered by safety hazard and low Coulombic efficiency,which is primarily caused by dendritic Li deposition.To address this issue,restraining dendrite growth at the nucleation stage is deemed as the most effective method.By utilizing the difference of electronegativity between boron atoms and carbon atoms,carbon atoms around boron atoms in boron-doped graphene(BG)turn into lithiophilic sites,which can enhance the adsorption capacity to Li^(+)at the nucleation stage.Consequently,an ultralow overpotential of 10 mV at a current density of 0.5 mA/cm^(2) and a high average Coulombic efficiency of 98.54%over more than 140 cycles with an areal capacity of 2 mAh/cm^(2) at a current density of 1 m A/cm^(2) were achieved.BG-Li|LiFePO_(4) full cells delivered a long lifespan of480 cycles at 0.5 C and excellent rate capability.This work provides a novel method for rational design of dendrite-free Li metal batteries by regulating nucleation process.展开更多
The influences of chromium-free chemical conversion treatment and anodizing treatment on bonding strength of AZ31 magnesium alloy were studied by lap-shear test, SEM and electrochemical methods. Both chemical conversi...The influences of chromium-free chemical conversion treatment and anodizing treatment on bonding strength of AZ31 magnesium alloy were studied by lap-shear test, SEM and electrochemical methods. Both chemical conversion treatment and anodizing can increase the bonding strength. The anodizing treatment gives higher bonding strength and better corrosion resistance than chemical conversion treatment. The increase of bonding strength by the treatmetlts may be attributed to the uneven surface structures with micro-pores, resulting in increased bonding areas and the embedding effect.展开更多
This work proposed a simple and efficient approach for synthesis of durable and efficient non-precious metal oxygen reduction reaction(ORR) electro-catalysts in MFCs. The rod-like carbon nanotubes(CNTs)were formed...This work proposed a simple and efficient approach for synthesis of durable and efficient non-precious metal oxygen reduction reaction(ORR) electro-catalysts in MFCs. The rod-like carbon nanotubes(CNTs)were formed on the Fe–N/SLG sheets after a carbonization process. The maximum power density of1210 ± 23 m W·mobtained with Fe–N/SLG catalyst in an MFC was 10.7% higher than that of Pt/C catalyst(1080 ± 20 mW ·m) under the same condition. The results of RDE test show that the ORR electron transfer number of Fe–N/SLG was 3.91 ± 0.02, which suggested that ORR catalysis proceeds through a four-electron pathway. The whole time of the synthesis of electro-catalysts is about 10 h, making the research take a solid step in the MFC expansion due to its low-cost, high efficiency and favorable electrochemical performance. Besides, we compared the electrochemical properties of catalysts using SLG, high conductivity graphene(HCG, a kind of multilayer graphene) and high activity graphene(HAG, a kind of GO) under the same conditions, providing a solution for optimal selection of cathode catalyst in MFCs.The morphology, crystalline structure, elemental composition and ORR activity of these three kinds of Fe–N/C catalysts were characterized. Their ORR activities were compared with commercial Pt/C catalyst.It demonstrates that this kind of Fe–N/SLG can be a type of promising highly efficient catalyst and could enhance ORR performance of MFCs.展开更多
The adsorbing effect of calcined layered double hydroxide (CLDH) for chloride ions in simulated concrete pore (SCP) solutions was investigated with the potentiodynamic polarization method, impedance measurement, i...The adsorbing effect of calcined layered double hydroxide (CLDH) for chloride ions in simulated concrete pore (SCP) solutions was investigated with the potentiodynamic polarization method, impedance measurement, ion selective electrode analysis and XRD. CLDH could effectively adsorb Cl^- and increase pH value in SCP solutions containing NaCl. The chloride to hydroxyl ions ratio ([C1^-]/[OH^-]) of the solution greatly decreased by CLDH treatment. In CLDH treated SCP solution with CI-, the pitting potential of carbon steel notably increased, and the surface impedance was much higher, indicating strengthened passivation. The process of CLDH adsorbing chloride ions from SCP solutions was accompanied with the reconstruction of the layered structure.展开更多
The correlation between the microhardness and microstructure features of anodic films on 2024 aluminum alloy formed in the mixed sulfuric acid/oxalic acid electrolyte was studied using micro-hardness tester and scanni...The correlation between the microhardness and microstructure features of anodic films on 2024 aluminum alloy formed in the mixed sulfuric acid/oxalic acid electrolyte was studied using micro-hardness tester and scanning electron microscope (SEIVI). The results show that the microhardness of the anodic film is influenced by the mierostructure of the anodic film such as the film porosity, and the order and continuity of the hexagon columnar ceils. The film microhardness increases as the porosity of the anodic film decreases and the order and continuity of the film ceils increase. With the same current density, as the anodic film thickens with anodizing time, the film microhardness increases because the film porosity decreases and the order and continuity of the cells are also improved. Under the condition of the same anodizing time, as the current density increases, the film microhardness decreases due to the higher film porosity and the poorer order and continuity of the film ceils. The film porosity increases because the increased current density can accelerate the oxidation reaction, strengthen the filed-assisted dissolution and the heating effect in the anodic film, resulting in decreased film order and continuity.展开更多
Monodispersed Bi-Tenano arrays are achieved via template-free bipotentiostatic deposition. The diameter and length of individual nanorod is ~80 nm and ~250 nm respectively. The electrodeposition process is demonstrate...Monodispersed Bi-Tenano arrays are achieved via template-free bipotentiostatic deposition. The diameter and length of individual nanorod is ~80 nm and ~250 nm respectively. The electrodeposition process is demonstrated to follow a two-step mechanism: an instantaneous reductive potential is applied to form dispersive nuclei, then a reverse oxidative potential strips partial Bi atoms to prevent further cross-growth. Repeatedly, the nano arrays film is obtained eventually. The thermoelectric properties of the obtained Bi-Tenano arrays such as electrical resistance, carrier density, Seebeck coefficient and power factor are measured to be 2.438 × 10-4?Ω·m, 4.251 × 1020 cm-3, -25.892 μV·K-1, 2.750 × 10-6 W·m-1·K2, respectively.展开更多
Two kinds of simulated concrete pore solutions(SPSs) were treated with different amounts of synthetic calcium silicate hydrate(C-S-H). The variation of the [Cl^-]/[OH^-] ratio in SPS was measured and the corrosion...Two kinds of simulated concrete pore solutions(SPSs) were treated with different amounts of synthetic calcium silicate hydrate(C-S-H). The variation of the [Cl^-]/[OH^-] ratio in SPS was measured and the corrosion susceptibility of carbon steel in the SPS was investigated with potentiodynamic polarization, EIS and weight lose tests. The experimental results showed that for the SPS at p H 12.5, as the amount of C-S-H increases, the [Cl^-]/[OH^-] ratio increases thereby causing an increase in the corrosion susceptibility of the steel. While for the SPS at p H 9.7, with increasing C-S-H amount, the drop amplitudes of both [Cl^-]/[OH^-] ratio and steel corrosion rate first decrease and then increase, and a 3% C-S-H addition shows the best inhibition effect. XPS results demonstrate that after C-S-H treating in p H 12.5 SPS the [Fe^(3+)]/[Fe^(2+)] ratio in the film on steel surface is reduced while in p H 9.7 SPS the [Fe^(3+)]/[Fe^(2+)] ratio is increased. The different effects of the C-S-H amount on the two SPSs and the steel corrosion behavior result from the influences of C-S-H on the SPS p H, which is related to the composition of the SPS.展开更多
Design and development of advanced electrocatalysts with high performance and low Pt consumption are crucial for reducing the kinetic energy barrier of the cathode oxygen reduction reaction(ORR)and improving the effic...Design and development of advanced electrocatalysts with high performance and low Pt consumption are crucial for reducing the kinetic energy barrier of the cathode oxygen reduction reaction(ORR)and improving the efficiency of proton exchange membrane fuel cells(PEMFC).In this study,we demonstrate a Pb-modulated PtCo system for efficient ORR,in which the inclusion of Pb in ternary alloys induces dislocation defects due to the significant difference in atomic radius.Dislocation-PtCoPb was confirmed to exhibit significantly higher ORR activity and stability in acidic ORR.In practical PEMFC applications,it outperforms the corresponding commercial Pt/C with a mass activity of 0.58 A·mgPt^(-1),making it a promising alternative to state-of-the-art Pt-based catalysts.The combination of experimental results and density functional theory(DFT)calculations offers valuable atomic-level insights into the dislocation structures.Pb with a larger atomic radius is located in the lattice stretching region below the dislocation slip plane,forming a structure similar to a Cottrell atmosphere,which reduces the dislocation energy and puts the system in a lower energy state.The Cottrell atmosphere pins the dislocation structure and stabilizes the ternary alloy.By adjusting the amount of added Pb,a moderate level of dislocation density induces a tuned strain effect,thereby enhancing the electrocatalytic mechanism by optimizing the electronic structure of the alloy surface and the adsorption and desorption of oxygen species.This work provides valuable insights into the design and development of lattice dislocation defect structures to trigger strain effects for improving ORR performance.展开更多
文摘A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liquid-phase carbonization of isotropic pitch to the emergence of carbon microbeads in the matrix and finally their growth to form a 100%anisotropic bulk meso-phase,but rather a reverse transformation.The effects of C_(60) loading and reaction temperature on the morphological transformation of mesophase were investigated by polarizing optical and scanning electron microscopies.The physical changes in the NMP induced by C_(60) were characterized by thermogravimetric analysis,Fourier transform infrared spectroscopy,X-ray diffractometry and Raman spectroscopy.The results show that the coalesced NMP can be converted to a spherical type at 300-320℃ with the addition of 5%C_(60),and the size of the mesophase microbeads increases with increasing temperature.Furthermore,a model is established to ex-plain the unique induction effect of C_(60) in the transformation process.This work makes the morphological transformation of MP con-trollable,and provides a new idea for the understanding and research of mesophase pitch.
基金National Natural Science Foundation of China,Grant/Award Numbers:U2004172,51972287 and 51502269the Foundation for University Key Teachers of Henan Province,Grant/Award Number:2020GGJS009Natural Science Foundation of Henan Province,Grant/Award Number:202300410368。
文摘Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries(LSBs).Phase transformation of MoSe_(2) from the 2H phase to the 1T phase has been proven to be a significant method to improve the catalytic activity.However,precisely controllable phase engineering of MoSe_(2) has rarely been reported.Herein,by in situ Li ions intercalation in MoSe_(2),a precisely controllable phase evolution from 2H-MoSe_(2) to 1T-MoSe_(2) was realized.More importantly,the definite functional relationship between cut-off voltage and phase structure was first identified for phase engineering through in situ observation and modulation methods.The sulfur host(CNFs/1T-MoSe_(2))presents high charge density,strong polysulfides adsorption,and catalytic kinetics.Moreover,Li-S cells based on it display capacity retention of 875.3mAh g^(-1) after 500 cycles at 1 C and an areal capacity of 8.71mAh cm^(-2) even at a high sulfur loading of 8.47mg cm^(-2).Furthermore,the flexible pouch cell exhibiting decent performance will endow a promising potential in the wearable energy storage field.This study proposes an effective strategy to precisely control the phase structure of MoSe_(2),which may provide the reference to fabricate the highly efficient electrocatalysts for LSBs and other energy systems.
基金financial support by the National Natural Science Foundation of China (Grant No. U2004212 and 51802012)。
文摘MXenes are under the spotlight due to their versatile physicochemical characteristics. Since their discovery in 2011, significant advancements have been achieved in their synthesis and application sectors. However, the spontaneous oxidation of MXenes, which is critical to its processing and product lifespan, has gotten less attention due to its chemical complexity and poorly understood oxidation mechanism. This perspective focuses on the oxidation stability of MXenes and addresses the most recent advancements in understanding and the possible countermeasures to limit the spontaneous oxidation of MXenes. A section is dedicated to the presently accessible methods for monitoring oxidation, with a discussion on the debatable oxidation mechanism and coherently operating factors that contribute to the complexity of MXenes oxidation. The current potential solutions for mitigating MXenes oxidation and the existing challenges are also discussed with prospects to prolong MXene's shelf-life storage and expand their application scope.
文摘The addition of 2,5-pyridinedicarboxylic acid(2,5-PDCA)to the Mg-Al LDH coating,which was prepared by one-step hydrothermal synthesis,had extremely enhanced the corrosion protection of AZ31 Mg alloy,although the 2,5-PDCA could not be intercalated into the interlayer spacing.The corrosion current density of 0.05 mol L^(−1)2,5-PDCA LDH containing LDH coating is 3.18 nA cm^(−2),reduced by two orders of magnitude compared to the LDH coating without inhibitor,and the corrosion inhibition efficiency of the coating is 98.05%.The coating formed on the surface of AZ31 was peeled off from the substrate by using a mechanical method and SEM observation of the cross-section showed that the coating consisted of three different layers.The innermost layer is a thick layer that consists of Mg(OH)_(2)and the intermediate layer is LDH,which is vertical to the substrate and the outmost layer is a thin but very dense deposit layer of LDH agglomerates with complexes of 2,5-PDCA and Mg.This kind of sediment/LDH/Mg(OH)_(2)three-layer composite structure was accountable for the increase in the corrosion resistance of AZ31 Mg alloy.
基金supported by the National Natural Science Funds of China(Grant number 22278016)Science and technology planning project of Yunnan Precious Metals Laboratory(Grant number YPML-2023050204)。
文摘Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic water oxidation.Herein,lotus root-like RuIr alloys with native micro-strain were constructed by an epitaxial growth of Ru-richened hcp-(0001)branches on Ir-richened fcc-(111)seeds using a polyol thermal synthesis strategy.The resultant Ru_(60)Ir_(40) alloy shows an OER overpotential of 197 mV at 10 mA cm^(-2) and a Tafel slope of 46.59 mV dec^(-1),showing no obvious activity decay for 80 h continuous chronopotentiometry test in 0.5 M H_(2)SO_(4).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy and density functional theory(DFT)calculations show that that the remarkably improved activity of the lotus root-like alloy can be attributed to the(0001)facet-triggered strain,which can efficiently optimize the electronic band structure of the active metal and the weakening of the chemisorption of oxygen-containing substances to boost OER electrocatalysis.Therefore,this work provides a new strategy to designing a class of advanced electrocatalysts with high strain using diverse nanostructures as building materials for carbon-free clean energy conversion systems.
基金supported by the National Key Research and Development Program of China“New Energy Project for Electric Vehicle”(2016YFB0100204)the National Natural Science Foundation of China(Nos.51772030,21805011,51572011,51802012)+2 种基金the Joint Funds of the National Natural Science Foundation of China(U1564206)Beijing Key Research and Development Plan(Z181100004518001)China Postdoctoral Science Foundation(Nos.2017M620637,2018M643697,2019T120930).
文摘MXenes,a new family of two-dimensional(2D)materials with excellent electronic conductivity and hydrophilicity,have shown distinctive advantages as a highly conductive matrix material for lithium-ion battery anodes.Herein,a facile electrostatic self-assembly of SnO2 quantum dots(QDs)on Ti3C2Tx MXene sheets is proposed.The as-prepared SnO2/MXene hybrids have a unique 0D-2D structure,in which the 0D SnO2 QDs(~4.7 nm)are uniformly distributed over 2D Ti3C2Tx MXene sheets with controllable loading amount.The SnO2 QDs serve as a high capacity provider and the“spacer”to prevent the MXene sheets from restacking;the highly conductive Ti3C2Tx MXene can not only provide efficient pathways for fast transport of electrons and Li ions,but also buffer the volume change of SnO2 during lithiation/delithiation by confining SnO2 QDs between the MXene nanosheets.Therefore,the 0D-2D SnO2 QDs/MXene hybrids deliver superior lithium storage properties with high capacity(887.4 mAh g?1 at 50 mA g?1),stable cycle performance(659.8 mAh g?1 at 100 mA g?1 after 100 cycles with a capacity retention of 91%)and excellent rate performance(364 mAh g?1 at 3 A g?1),making it a promising anode material for lithium-ion batteries.
基金financially supported by the Beijing Municipal Science and Technology Commission(Grant No.Z181100004718007)the National Key R&D Program of China(Grant No.2017YFB0102204)。
文摘Sodium-ion batteries(SIBs)have attracted significant attentions as promising alternatives to lithium-ion batteries for large-scale energy storage applications.Here carbon materials are considered as the most competitive anodes for SIBs based on their low-cost,abundant availability and excellent structural stability.Pitch,with high carbon content and low cost,is an ideal raw precursor to prepare carbon materials for large-scale applications.Nevertheless,the microstructures of pitch-based carbon are highly ordered with smaller interlayer distances,which are unfavorable for Na ion storage.Many efforts have been made to improve the sodium storage performance of pitch-based carbon materials.This review summarizes the recent progress about the application of pitch-based carbons for SIBs anodes in the context of carbon’s morphology and structure regulation strategies,including morphology adjustment,heteroatoms doping,fabricating heterostructures,and the increase of the degree of disorder.Besides,the advantages,present challenges,and possible solutions to current issues in pitch-based carbon anode are discussed,with the highlight of future research directions.This review will provide a deep insight into the development of low-cost and high-performance pitch-based carbon anode for SIBs.
基金financially supported by the National Natural Science Foundation of China(NSFC,51572011)the Fundamental Research Funds for the Central Universities(buctrc201819)。
文摘The growing energy concern all over the world has recognized hydrogen energy as the most promising renewable energy sources.Recently,electrocatalytic hydrogen evolution reaction(HER)by water splitting has been extensively studied with a focus on developing efficient electrocatalysts that can afford HER at overpotential with minimum power consumption.The two-dimensional transition metal carbides and nitride,also known as MXenes,are becoming the rising star in developing efficient electrocatalysts for HER,owing to their integrated chemical and electronic properties,e.g.,metallic conductivity,variety of redox-active transition metals,high hydrophilicity,and tunable surface functionalities.In this review,the recent progress about the fundamental understanding and materials engineering of MXenes-based electrocatalysts is summarized in concern with two aspects:i)the regulation of the intrinsic properties of MXenes,which include the composition,surface functionality,and defects;and ii)MXenes-based composites for HER process.In the end,we summarize the present challenges concerning the efficiency of MXenes-based HER electrocatalysts and propose the directions of future research efforts.
基金supported by the National Natural Science Foundation of China (21805011,51902251,52072021,and U2004212)the State Key Laboratory of Organic-Inorganic Composites (oic-202101010)+1 种基金the Natural Science Foundation of Shaanxi Provincial Department of Education (20JK0753)the Provincial Joint Fund of Shaanxi (2021JLM-28)。
文摘ZnS has great potentials as an anode for lithium storage because of its high theoretical capacity and resource abundance;however,the large volume expansion accompanied with structural collapse and low conductivity of ZnS cause severe capacity fading and inferior rate capability during lithium storage. Herein,0D-2 D ZnS nanodots/Ti_(3)C_(2)T_x MXene hybrids are prepared by anchoring ZnS nanodots on Ti_(3)C_(2)T_(x) MXene nanosheets through coordination modulation between MXene and MOF precursor(ZIF-8) followed with sulfidation. The MXene substratecoupled with the ZnS nanodots can synergistically accommodate volume variation of ZnS over charge–discharge to realize stable cyclability. As revealed by XPS characterizations and DFT calculations,the strong interfacial interaction between ZnS nanodots and MXene nanosheets can boost fast electron/lithium-ion transfer to achieve excellent electrochemical activity and kinetics for lithium storage. Thereby,the as-prepared ZnS nanodots/MXene hybrid exhibits a high capacity of 726.8 mAh g^(-1) at 30 mA g^(-1),superior cyclic stability(462.8 mAh g^(-1) after 1000 cycles at 0.5 A g^(-1)),and excellent rate performance. The present results provide new insights into the understanding of the lithium storage mechanism of ZnS and the revealing of the e ects of interfacial interaction on lithium storage performance enhancement.
基金financially supported by the National Key Research and Development Program of China(2017YFB0102204)the National Natural Science Foundation of China(NSFC,51572011).
文摘MXene nanosheets have been used for preparing highly flexible integrated electrodes due to their two-dimensional(2D)morphology,flexibility,high conductivity,and abundant functional groups.However,restacking of 2D nanosheets inhibits the ion transport in MXene electrodes,limiting their thickness,rate performance,and energy storage capacity.Here,we employed a natural sedimentation method instead of the conventional vacuum-assisted filtration to prepare flexible Ti3C2TxMXene films with enlarged interlayer spacing,which facilitates the access of the lithium ions to the interlayers and thus leads to a greatly enhanced electrochemical performance.The naturally sedimented flexible film shows a double lithium storage capacity compared to the conventional vacuum-filtered MXene film,along with improved rate performance and excellent cycle stability.
基金Funded by the Beijing Municipal Natural Science Foundation (No. 2192041)。
文摘The effect of particle size on the density and resistivity of ITO green bodies and targets was systematically investigated.The experimental results show that the relative density of ITO green bodies decreases with the increase of ITO particle size.When the particle size is 10.7 nm,the relative density of ITO green bodies rises to the maximum value of 56.6%.The resistivity declines exponentially with the increase of particle size,which satisfies the exponential equation of R=exp(-41.823 × d).When the particle size is 41.6 nm,the resistivity reaches the minimum value of 0.8 Ω·cm.The relative density of ITO target decreases with the increase of particle size.Fine particles can increase the driving force of densification in initial stage.Electron mobility,caused by grain boundary scattering,will increase due to the increase of particle size or the decrease of grain boundary potential.When the particle size is 10.7 nm,the target with compact grain stacking and low porosity shows a maximum relative density of 99.25%,and the resistivity reaches the minimum value of 0.34×10^-3 Ω·cm.
基金financially supported by the National Natural Science Foundation of China (NSFC, 51572011 and 51802012)the National Key Research and Development Program of China (2017YFB0102204)the Fundamental Research Funds for the Central Universities (buctrc201813 and buctrc201819)。
文摘2D MXene nanosheets with metallic conductivity and high pseudo-capacitance are promising electrode materials for supercapacitors.Especially,MXene films can be directly used as electrodes for flexible supercapacitors.However,they suffer from sluggish ion transport due to self-restacking,causing limited electrochemical performance.Herein,a flexible 3D porous MXene film is fabricated by incorporating graphene oxide(GO) into MXene film followed by self-propagating reduction.The self-propagating process is facile and effective,which can be accomplished in 1.25 s and result in 3D porous framework by releasing substantial gas instantaneously.As the 3D porous structure provides massive ion-accessible active sites and promotes fast ion transport,the MXene-rGO films exhibit superior capacitance and rate performance.With the rGO content of 20%,the MXene-rGO-20 film delivers a high capacitance of 329.9 F g^(-1) at 5 mV s^(-1) in 3 M H2 SO4 electrolyte and remains 260.1 F g^(-1) at 1,000 mV s^(-1) as well as good flexibility.Furthermore,the initial capacitance is retained above 90% after 40,000 cycles at 100 A g^(-1),revealing good cycle stability.This work not only provides a high-performance flexible electrode for supercapacitors,but also proposes an efficient and time-saving strategy for constructing 3D structure from 2D materials.
基金supported by the National Key R&D Program of China(Grant No.2018YFA0306900)the National Natural Science Foundation of China(Nos.51872012)the Fundamental Research Funds for the Central Universities and the 111 Project(B17002)。
文摘Li metal,possessing advantages of high theoretical specific capacity and low electrochemical potential,is regarded as the most promising anode material for next-generation batteries.However,despite decades of intensive research,its practical application is still hindered by safety hazard and low Coulombic efficiency,which is primarily caused by dendritic Li deposition.To address this issue,restraining dendrite growth at the nucleation stage is deemed as the most effective method.By utilizing the difference of electronegativity between boron atoms and carbon atoms,carbon atoms around boron atoms in boron-doped graphene(BG)turn into lithiophilic sites,which can enhance the adsorption capacity to Li^(+)at the nucleation stage.Consequently,an ultralow overpotential of 10 mV at a current density of 0.5 mA/cm^(2) and a high average Coulombic efficiency of 98.54%over more than 140 cycles with an areal capacity of 2 mAh/cm^(2) at a current density of 1 m A/cm^(2) were achieved.BG-Li|LiFePO_(4) full cells delivered a long lifespan of480 cycles at 0.5 C and excellent rate capability.This work provides a novel method for rational design of dendrite-free Li metal batteries by regulating nucleation process.
基金Funded by the Key Project of Science and Technology of Ministry of Education of China(No.108129)
文摘The influences of chromium-free chemical conversion treatment and anodizing treatment on bonding strength of AZ31 magnesium alloy were studied by lap-shear test, SEM and electrochemical methods. Both chemical conversion treatment and anodizing can increase the bonding strength. The anodizing treatment gives higher bonding strength and better corrosion resistance than chemical conversion treatment. The increase of bonding strength by the treatmetlts may be attributed to the uneven surface structures with micro-pores, resulting in increased bonding areas and the embedding effect.
文摘This work proposed a simple and efficient approach for synthesis of durable and efficient non-precious metal oxygen reduction reaction(ORR) electro-catalysts in MFCs. The rod-like carbon nanotubes(CNTs)were formed on the Fe–N/SLG sheets after a carbonization process. The maximum power density of1210 ± 23 m W·mobtained with Fe–N/SLG catalyst in an MFC was 10.7% higher than that of Pt/C catalyst(1080 ± 20 mW ·m) under the same condition. The results of RDE test show that the ORR electron transfer number of Fe–N/SLG was 3.91 ± 0.02, which suggested that ORR catalysis proceeds through a four-electron pathway. The whole time of the synthesis of electro-catalysts is about 10 h, making the research take a solid step in the MFC expansion due to its low-cost, high efficiency and favorable electrochemical performance. Besides, we compared the electrochemical properties of catalysts using SLG, high conductivity graphene(HCG, a kind of multilayer graphene) and high activity graphene(HAG, a kind of GO) under the same conditions, providing a solution for optimal selection of cathode catalyst in MFCs.The morphology, crystalline structure, elemental composition and ORR activity of these three kinds of Fe–N/C catalysts were characterized. Their ORR activities were compared with commercial Pt/C catalyst.It demonstrates that this kind of Fe–N/SLG can be a type of promising highly efficient catalyst and could enhance ORR performance of MFCs.
基金Funded by the National Natural Science Foundation of China(51171014 and 51210001)the Fundamental Research Funds for the Central Universities(No.ZZ1116)
文摘The adsorbing effect of calcined layered double hydroxide (CLDH) for chloride ions in simulated concrete pore (SCP) solutions was investigated with the potentiodynamic polarization method, impedance measurement, ion selective electrode analysis and XRD. CLDH could effectively adsorb Cl^- and increase pH value in SCP solutions containing NaCl. The chloride to hydroxyl ions ratio ([C1^-]/[OH^-]) of the solution greatly decreased by CLDH treatment. In CLDH treated SCP solution with CI-, the pitting potential of carbon steel notably increased, and the surface impedance was much higher, indicating strengthened passivation. The process of CLDH adsorbing chloride ions from SCP solutions was accompanied with the reconstruction of the layered structure.
基金Funded by the National Natural Science Foundation of China(No.51210001)
文摘The correlation between the microhardness and microstructure features of anodic films on 2024 aluminum alloy formed in the mixed sulfuric acid/oxalic acid electrolyte was studied using micro-hardness tester and scanning electron microscope (SEIVI). The results show that the microhardness of the anodic film is influenced by the mierostructure of the anodic film such as the film porosity, and the order and continuity of the hexagon columnar ceils. The film microhardness increases as the porosity of the anodic film decreases and the order and continuity of the film ceils increase. With the same current density, as the anodic film thickens with anodizing time, the film microhardness increases because the film porosity decreases and the order and continuity of the cells are also improved. Under the condition of the same anodizing time, as the current density increases, the film microhardness decreases due to the higher film porosity and the poorer order and continuity of the film ceils. The film porosity increases because the increased current density can accelerate the oxidation reaction, strengthen the filed-assisted dissolution and the heating effect in the anodic film, resulting in decreased film order and continuity.
文摘Monodispersed Bi-Tenano arrays are achieved via template-free bipotentiostatic deposition. The diameter and length of individual nanorod is ~80 nm and ~250 nm respectively. The electrodeposition process is demonstrated to follow a two-step mechanism: an instantaneous reductive potential is applied to form dispersive nuclei, then a reverse oxidative potential strips partial Bi atoms to prevent further cross-growth. Repeatedly, the nano arrays film is obtained eventually. The thermoelectric properties of the obtained Bi-Tenano arrays such as electrical resistance, carrier density, Seebeck coefficient and power factor are measured to be 2.438 × 10-4?Ω·m, 4.251 × 1020 cm-3, -25.892 μV·K-1, 2.750 × 10-6 W·m-1·K2, respectively.
基金Funded by the National Natural Science Foundation of China(Nos.51171014 and 51210001)
文摘Two kinds of simulated concrete pore solutions(SPSs) were treated with different amounts of synthetic calcium silicate hydrate(C-S-H). The variation of the [Cl^-]/[OH^-] ratio in SPS was measured and the corrosion susceptibility of carbon steel in the SPS was investigated with potentiodynamic polarization, EIS and weight lose tests. The experimental results showed that for the SPS at p H 12.5, as the amount of C-S-H increases, the [Cl^-]/[OH^-] ratio increases thereby causing an increase in the corrosion susceptibility of the steel. While for the SPS at p H 9.7, with increasing C-S-H amount, the drop amplitudes of both [Cl^-]/[OH^-] ratio and steel corrosion rate first decrease and then increase, and a 3% C-S-H addition shows the best inhibition effect. XPS results demonstrate that after C-S-H treating in p H 12.5 SPS the [Fe^(3+)]/[Fe^(2+)] ratio in the film on steel surface is reduced while in p H 9.7 SPS the [Fe^(3+)]/[Fe^(2+)] ratio is increased. The different effects of the C-S-H amount on the two SPSs and the steel corrosion behavior result from the influences of C-S-H on the SPS p H, which is related to the composition of the SPS.
基金support of the National Natural Science Funds of China(No.22278016).
文摘Design and development of advanced electrocatalysts with high performance and low Pt consumption are crucial for reducing the kinetic energy barrier of the cathode oxygen reduction reaction(ORR)and improving the efficiency of proton exchange membrane fuel cells(PEMFC).In this study,we demonstrate a Pb-modulated PtCo system for efficient ORR,in which the inclusion of Pb in ternary alloys induces dislocation defects due to the significant difference in atomic radius.Dislocation-PtCoPb was confirmed to exhibit significantly higher ORR activity and stability in acidic ORR.In practical PEMFC applications,it outperforms the corresponding commercial Pt/C with a mass activity of 0.58 A·mgPt^(-1),making it a promising alternative to state-of-the-art Pt-based catalysts.The combination of experimental results and density functional theory(DFT)calculations offers valuable atomic-level insights into the dislocation structures.Pb with a larger atomic radius is located in the lattice stretching region below the dislocation slip plane,forming a structure similar to a Cottrell atmosphere,which reduces the dislocation energy and puts the system in a lower energy state.The Cottrell atmosphere pins the dislocation structure and stabilizes the ternary alloy.By adjusting the amount of added Pb,a moderate level of dislocation density induces a tuned strain effect,thereby enhancing the electrocatalytic mechanism by optimizing the electronic structure of the alloy surface and the adsorption and desorption of oxygen species.This work provides valuable insights into the design and development of lattice dislocation defect structures to trigger strain effects for improving ORR performance.