Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr...Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.展开更多
Sustainable production of hydrogen is a hopeful requirement of a strategic future economy and development.Water splitting driven by electricity is a favorable pathway for renewable hydrogen production.This critical re...Sustainable production of hydrogen is a hopeful requirement of a strategic future economy and development.Water splitting driven by electricity is a favorable pathway for renewable hydrogen production.This critical review highlighted recent efforts toward the development of the nanoscale synthesis of nonprecious metal's graphene-supported electrocatalysts and their electrocatalytic features for remarkable hydrogen evolution reaction(HER).Different essential nonprecious metal's graphene-supported electrocatalysts,including metal carbides,sulfides,phosphides,selenides,oxides,and nitrides are reviewed.In the exploration,attention is given to the strategies of activity enhancement,the synthetic approach,and the composition/structure electrocatalytic-performance relationship of these HER electrocatalysts.We are hopeful that this review confers a new momentum to the rational design of remarkable performance nonprecious metal's graphenesupported electrocatalysts and comprehensive guide for researchers to utilize the subject catalysts in regular water splitting.展开更多
Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni...Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni/MoO_(2) nano-needle with three-phase heterojunction(Ni/MoO_(2)@CN)for accelerating the WS under industrial alkaline condition.Density functional theory calculations reveal that the electrons are redistributed at the three-phase heterojunction interface,which optimizes the adsorption energy of H-and O-containing intermediates to obtain the best ΔG_(H*) for hydrogen evolution reaction(HER)and decrease the ΔG value of ratedetermining step for oxygen evolution reaction(OER),thus enhancing the HER/OER catalytic activity.Electrochemical results confirm that Ni/MoO_(2)@CN exhibits good activity for HER(ƞ_(-10)=33 mV,ƞ_(-1000)=267 mV)and OER(ƞ_(10)=250 mV,ƞ_(1000)=420 mV).It shows a low potential of 1.86 V at 1000 mA cm^(−2) for WS in 6.0 M KOH solution at 60℃ and can steadily operate for 330 h.This good HER/OER performance can be attributed to the three-phase heterojunction with high intrinsic activity and the self-supporting nano-needle with more active sites,faster mass diffusion,and bubbles release.This work provides a unique idea for designing high efficiency catalytic materials for WS.展开更多
Sulfuric acid leaching of high iron-bearing zinc calcine was investigated to assess the effects of sulfuric acid concentration, liquid-to-solid ratio, leaching time, leaching temperature, and the stirring speed on the...Sulfuric acid leaching of high iron-bearing zinc calcine was investigated to assess the effects of sulfuric acid concentration, liquid-to-solid ratio, leaching time, leaching temperature, and the stirring speed on the leaching rates of zinc and iron. The results showed that the sulfuric acid concentration, liquid-to-solid ratio, leaching time, and leaching temperature strongly influenced the leaching of zinc and iron, whereas stirring speed had little influence. Zinc was mainly leached and the leaching rate of iron was low when the sulfuric acid concentration was less than 100 g/L. At sulfuric acid concentrations higher than 100 g/L, the leaching rate of iron increased quickly with increasing sulfuric acid concentration. This behavior is attributed to iron-bearing minerals such as zinc ferrite in zinc calcine dissolving at high temperatures and high sulfuric acid concentrations but not at low temperatures and low sulfuric acid concentrations.展开更多
Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure ...Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure of catalyst layers with efficient mass transportation channels plays a vital role.Herein,PEMFCs with order-structured cathodic electrodes were fabricated by depositing Pt nanoparticles by Ebeam onto vertically aligned carbon nanotubes(VACNTs)growth on Al foil via plasma-enhanced chemical vapor deposition.Results demonstrate that the proportion of hydrophilic Pt-deposited region along VACNTs and residual hydrophobic region of VANCTs without Pt strongly influences the cell performance,in particular at high current densities.When Pt nanoparticles deposit on the top depth of around 600 nm on VACNTs with a length of 4.6μm,the cell shows the highest performance,compared with others with various lengths of VACNTs.It delivers a maximum power output of 1.61 W cm^(-2)(H_(2)/O_(2),150 k Pa)and 0.79 W cm^(-2)(H_(2)/Air,150 k Pa)at Pt loading of 50μg cm^(-2),exceeding most of previously reported PEMFCs with Pt loading of<100μg cm^(-2).Even though the Pt loading is down to 30μg cm^(-2)(1.36 W cm^(-2)),the performance is also better than 100μg cm^(-2)(1.24 W cm^(-2))of commercial Pt/C,and presents better stability.This excellent performance is critical attributed to the ordered hydrophobic region providing sufficient mass passages to facilitate the fast water drainage at high current densities.This work gives a new understanding for oxygen reduction reaction occurred in VACNTs-based ordered electrodes,demonstrating the most possibility to achieve a substantial reduction in Pt loading<100μg cm^(-2) without sacrificing in performance.展开更多
In order to found new dielectrics ceramics in tungsten bronze structure, unfilled tungsten bronze(TB) ceramics with nominal formula Ba4PrFe(0.5)Nb(9.5)O(30) were prepared by the solid state reaction method. Th...In order to found new dielectrics ceramics in tungsten bronze structure, unfilled tungsten bronze(TB) ceramics with nominal formula Ba4PrFe(0.5)Nb(9.5)O(30) were prepared by the solid state reaction method. The microstructure and dielectric properties were studied using powder X-ray diffraction, field emission scanning electron microscope, and variable temperature dielectric test system. The results show that the ceramics have a single phase and belong to the space group of P4bm with the cell of a = b = 12.4839(3) ?, c = 3.9409(5) ?, V = 614.192(2) ?3. The frequency dependent dielectrics properties show that the ceramics have a Debye-like relaxation at room temperature, while the temperature dependent dielectrics properties indicate that the ceramics are a relaxor and the relaxation is due to the nanopolars and oxygen vacancies. The ceramics have a potential application in electronic ceramics as temperature-stable multilayer ceramic capacitors.展开更多
In this paper, the preparation of graphene oxide was achieved by Hummers method and the surface modification was achieved by poly(hexaneditiol), which was a synthetic thermotropic liquid crystalline polymer. The c-PHD...In this paper, the preparation of graphene oxide was achieved by Hummers method and the surface modification was achieved by poly(hexaneditiol), which was a synthetic thermotropic liquid crystalline polymer. The c-PHDT/GO/PF composites were prepared by blending, rolling and compression molding techniques. Then, the as-prepared samples were characterized by FTIR, Raman, XRD, TGA and POM to obtain information on their structures and properties. After that, the effects of c-PHDT/GO content on the mechanical properties, friction performance and dynamic mechanical performance of c-PHDT/GO/PF composites were studied by Mechanical and Dynamic Mechanical Analysis (DMA) methods. Also, Scanning Electron Microscope (SEM) was used for the characterization of wear and fracture surface morphology. The results revealed that the reinforcing effect of c-PHDT/GO was significant as a considerable enhancement on the mechanical performance of c-PHDT/GO/PF composite as compared to pure phenol-formaldehyde composites was observed: the impact strength, bending modulus and bending strength increased from 1.63 kJ/m2, 8.61 GPa and 41.55 MPa to 2.31 kJ/m2, 10.16 GPa and 54.40 MPa respectively at the c-PHDT/GO content = 0.75%. Moreover, the initial storage modulus increased by 28.4%, while the wear mass loss decreased by 17.8%. More importantly, the reinforcement by c-PHDT/GO was further enhanced as compared to GO/PF and p-PHDT/GO/PF composites, the impact strength of c-PHDT/GO/PF composite increased by 27.6% and 11.1%, the bending strength increased by 11.8% and 7.6%, the initial storage modulus increased by 16.2% and 4.2% and the mass loss due to wear decreased by 12.7% and 8.8%, respectively. Based on these results, we can conclude that the surface modification of GO by poly(hexanedithiol), which includes synergistic effect by c-PHDT and GO, improves the interfacial adhesion between GO and the resin matrix, thus reinforcing the composites.展开更多
The global practical implementation of proton exchange membrane fuel cells(PEMFCs)heavily relies on the advancement of highly effective platinum(Pt)-based electrocatalysts for the oxygen reduction reaction(ORR).To ach...The global practical implementation of proton exchange membrane fuel cells(PEMFCs)heavily relies on the advancement of highly effective platinum(Pt)-based electrocatalysts for the oxygen reduction reaction(ORR).To achieve high ORR performance,electrocatalysts with highly accessible reactive surfaces are needed to promote the uncovering of active positions for easy mass transportation.In this critical review,we introduce different approaches for the emerging development of effective ORR electrocatalysts,which offer high activity and durability.The strategies,including morphological engineering,geometric configuration modification via supporting materials,alloys regulation,core-shell,and confinement engineering of single atom electrocatalysts(SAEs),are discussed in line with the goals and requirements of ORR performance enhancement.We review the ongoing development of Pt electrocatalysts based on the syntheses,nanoarchitecture,electrochemical performances,and stability.We eventually explore the obstacles and research directions on further developing more effective electrocatalysts.展开更多
Multimetallic Pt-based alloys with excavated structures have attracted great interest owing to their compositional and morphological tunability, high specific surface areas, and impressive electro-catalytic activities...Multimetallic Pt-based alloys with excavated structures have attracted great interest owing to their compositional and morphological tunability, high specific surface areas, and impressive electro-catalytic activities. Herein, we report the first facile one-pot synthesis of trimetallic Pt-Ni-Cu highly excavated rhombic dodecahedrons (ERDs) with a yield approaching 100%. More importantly, these highly uniform nanocrystals have three-dimensionally accessible excavated surfaces, where abundant stepped atoms are observed. Benefiting from the highly excavated rhombic dodecahedral structures, electronic and synergistic effects within the trimetallic allo3~ and abundant stepped atoms, the as-prepared trimetallic Pt-Ni-Cu ERDs exhibit an enhanced electro-catalytic performance for the electro-oxidation of methanol compared to commercial Pt/C and bimetallic Pt-Cu ERDs and Pt-Ni-Cu solid rhombic dodecahedrons solid rhombic dodecahedrons (SRDs).展开更多
Electrochemical water splitting is regarded as the most auspicious technology for renewable sources,transport,and storage of hydrogen energy.Currently,noble Pt metal and noble-metal oxides(IrO_(2)and RuO_(2))are recog...Electrochemical water splitting is regarded as the most auspicious technology for renewable sources,transport,and storage of hydrogen energy.Currently,noble Pt metal and noble-metal oxides(IrO_(2)and RuO_(2))are recognized as state-of-the-art electrocatalysts for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively.Searching for earth-abundant electrocatalysts for the HER and OER with remarkable performance and high stability to replace precious metals plays a significant role in the commercial application of electrochemical water splitting.In this review,recent advancements in nanostructured transition metal electrocatalysts are assessed through the selected examples of nitrides,carbides,phosphides,sulfides,borides,layered double hydroxides,and oxides.Recent breakthroughs in nanostructured transition metal electrocatalysts are discussed in terms of their mechanisms,controllable production,structural design,and innovative strategies for boosting their performance.For instance,most nanostructured transition metal electrocatalysts for overall water splitting(OWS)only function well in neutral and alkaline solutions.Finally,current research challenges and future perspectives for increasing the performance of nanostructured transition metals for OWS are proposed.展开更多
Layered double hydroxides(LDHs) as a class of anionic clays have extensive applications due to their unique structures. Nowadays, the emphasis is laid on the development of LDH coatings for corrosion resistance and ...Layered double hydroxides(LDHs) as a class of anionic clays have extensive applications due to their unique structures. Nowadays, the emphasis is laid on the development of LDH coatings for corrosion resistance and medical applications. Thus, this review highlights synthetic methods of LDH coatings and LDH-based composite coatings on magnesium alloys. Special attention is focused on self-healing,biocompatible and self-cleaning LDH-based composite coatings on magnesium alloys.展开更多
Graphene/polyaniline nanotube (GPNT) composite was synthesized using Vitamin C as both the template of polyaniline nanotube via in situ polymerization of aniline and the reducing agent of graphene oxide. The pure po...Graphene/polyaniline nanotube (GPNT) composite was synthesized using Vitamin C as both the template of polyaniline nanotube via in situ polymerization of aniline and the reducing agent of graphene oxide. The pure polyaniline (PANI), graphene/PANI composite (GP) (using hydrazine monohydrate instead of VC) and GO/PANI composite were also prepared. IR spectroscopy and morphologies of the as-prepared samples were characterized. And the electrochemical performances were conducted on a three-electrode cell. IR spectroscopy demonstrated the in- teraction between graphene and PANI nanotube in GPNT, which is beneficial to enhance the electrochemical performance of the composite electrode. Surface morphology showed PANI nanotube with outer diameter of 140 nm in GPNT. GPNT composites exhibited better electrochemical performances than GP composite and pure PANI. The electrochemical performances showed that the specific capacitance of GPNT was 561 F/g which is more than that of either GP or PANI, it is not only due to the graphene which can provide good electrical conductivity and high specific surface area, but also associated with a good redox activity of ordered PANI nanotubes. The as-prepared GPNT composites with higher conductivity, lower resistance and better cycle life in our laboratory are promising electrode materials for high-performance electrical energy storage devices.展开更多
Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(...Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(XRD)and scanning electron microscopy(SEM),respectively.The main crystalline phase is monoclinic Nd(Mg_(1/2)Sn_(1/2))O_(3) with a double perovskite structure(P21/n space group)for the NMS system proved by XRD.The sample at x=0.01 has the best crystallinity and evenly distributed crystal grains observed by SEM.The optimum performances(ε_(r)=19.87,Q×f=41840 GHz,f=12.05 GHz)are obtained at x=0.01.Lattice vibrational modes of the Raman spectra were assigned and illustrated,in detail.The dielectric properties obtained by fitting infrared reflectance spectra with the help of four-parameter semi-quantum model are consistent with the calculated values by microscopic polarization and damping coefficients.The reverse translational vibration of the NdeMgO_(6),the F_(5u)^((5)) mode,provides the greatest contribution to the dielectric response.The relationships between crystal structures and dielectric properties were mainly established using lattice vibrational modes as a media.展开更多
Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeW...Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeWO_(4)-WO_(3) heterostructure catalyst growing on nickel foam (FeWO_(4)-WO_(3)/NF) by a combination of hydrothermal and calcination method. It shows good catalytic activity with ultralow potentials for OER (ζ_(10) = 1.43 V, ζ_(1.000) = 1.56 V) and HzOR (ζ_(10) = −0.034 V, ζ_(1.000) = 0.164 V). Moreover, there is little performance degradation after being tested for _(10)0 h at 1,000 (OER) and _(10)0 (HzOR) mA·cm−2, indicating good stability. The superior performance could be attributed to the wolframite structure and heterostructure: The former provides a high electrical conductivity to ensure the electronic transfer capability, and the later induces interfacial electron redistribution to enhance the intrinsic activity and stability. The work offers a brand-new way to prepare good performance catalysts for OER and HzOR, especially at large current density.展开更多
Fe-Ni-Cr-based super-high-strength maraging stainless steels were generally realized by multiple-element alloying under a given heat treatment processing. A series of alloy compositions were designed with a uniform cl...Fe-Ni-Cr-based super-high-strength maraging stainless steels were generally realized by multiple-element alloying under a given heat treatment processing. A series of alloy compositions were designed with a uniform cluster formula of [Ni16Fe192](Cr32(Ni16-x-y-z-m-n MoxTiyNbzAlmVn)) (at.%) that was developed out of a unique alloy design tool, a cluster- plus-glue-atom model. Alloy rods with a diameter of 6 mm were prepared by copper-mold suction-cast processing under the argon atmosphere. These alloy samples were solid-solutioned at 1273 K for 1 h, followed by water-quenching, and then aged at 783 K for 3 h. The effect of the valence electron concentration, characterized with the number of valence electrons per unit cluster (VE/uc) formula of 16 atoms, on microhardness of these designed maraging stainless steels at both solid- solutioned and aged states was investigated. The relationship between alloy compositions and microhardness in maraging stainless steels was firstly established by the random forest (RF, a kind of machine learning methods) based on the experimental results. It was found that not only the microhardness of any given composition alloy within the frame of cluster formula, but also the alloy composition with a maximum microhardness for any given VE/uc, could be predicted in good agreement with the guidance of the relationship by RF. The contributions of minor-alloying elements to the microhardness of the aged alloys were also discussed.展开更多
Mo-V-Nb tri-component oxide catalysts were prepared and firstly used for the selective oxidation of Cα-OH lignin compounds.The catalytic performance of the composite oxides was obviously enhanced due to the synergist...Mo-V-Nb tri-component oxide catalysts were prepared and firstly used for the selective oxidation of Cα-OH lignin compounds.The catalytic performance of the composite oxides was obviously enhanced due to the synergistic effects of Mo and V elements.Mo5-xVxO14 phase with a variable Mo/V ratio provided suitable active sites for the oxidative dehydrogenation(ODH)of Cα-OH lignin model compound.The optimized Mo-V-Nb molar composition was confirmed as Mo0.61V0.31Nb0.08Ox/TiO2,which exhibited the prominent catalytic activity with the turnover frequency of 1.04×10-3 mmol·g(cat)-1·s-1.Even at room temperature,the catalysts showed highly-efficient ODH reaction activities.The active phase for selective oxidation reaction and the inhibiting effect ofα-MoO3 phase were also discussed in the study.展开更多
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University.
文摘Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.
文摘Sustainable production of hydrogen is a hopeful requirement of a strategic future economy and development.Water splitting driven by electricity is a favorable pathway for renewable hydrogen production.This critical review highlighted recent efforts toward the development of the nanoscale synthesis of nonprecious metal's graphene-supported electrocatalysts and their electrocatalytic features for remarkable hydrogen evolution reaction(HER).Different essential nonprecious metal's graphene-supported electrocatalysts,including metal carbides,sulfides,phosphides,selenides,oxides,and nitrides are reviewed.In the exploration,attention is given to the strategies of activity enhancement,the synthetic approach,and the composition/structure electrocatalytic-performance relationship of these HER electrocatalysts.We are hopeful that this review confers a new momentum to the rational design of remarkable performance nonprecious metal's graphenesupported electrocatalysts and comprehensive guide for researchers to utilize the subject catalysts in regular water splitting.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Hundred Talents Program of Guangxi Universities,the Excellent Scholars and Innovation Team of Guangxi Universities+1 种基金the Innovation Project of Guangxi Graduate Education(YCBZ2021011)the High-performance Computing Platform of Guangxi University.
文摘Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni/MoO_(2) nano-needle with three-phase heterojunction(Ni/MoO_(2)@CN)for accelerating the WS under industrial alkaline condition.Density functional theory calculations reveal that the electrons are redistributed at the three-phase heterojunction interface,which optimizes the adsorption energy of H-and O-containing intermediates to obtain the best ΔG_(H*) for hydrogen evolution reaction(HER)and decrease the ΔG value of ratedetermining step for oxygen evolution reaction(OER),thus enhancing the HER/OER catalytic activity.Electrochemical results confirm that Ni/MoO_(2)@CN exhibits good activity for HER(ƞ_(-10)=33 mV,ƞ_(-1000)=267 mV)and OER(ƞ_(10)=250 mV,ƞ_(1000)=420 mV).It shows a low potential of 1.86 V at 1000 mA cm^(−2) for WS in 6.0 M KOH solution at 60℃ and can steadily operate for 330 h.This good HER/OER performance can be attributed to the three-phase heterojunction with high intrinsic activity and the self-supporting nano-needle with more active sites,faster mass diffusion,and bubbles release.This work provides a unique idea for designing high efficiency catalytic materials for WS.
基金financially supported by the National Natural Science Foundation of China (Nos. 51774099 and 51364003)the Ministry-Province Jointly Constructed Cultivation Base for State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials,Guangxi Zhuang Autonomous Region, China (GXKFJ16-01)
文摘Sulfuric acid leaching of high iron-bearing zinc calcine was investigated to assess the effects of sulfuric acid concentration, liquid-to-solid ratio, leaching time, leaching temperature, and the stirring speed on the leaching rates of zinc and iron. The results showed that the sulfuric acid concentration, liquid-to-solid ratio, leaching time, and leaching temperature strongly influenced the leaching of zinc and iron, whereas stirring speed had little influence. Zinc was mainly leached and the leaching rate of iron was low when the sulfuric acid concentration was less than 100 g/L. At sulfuric acid concentrations higher than 100 g/L, the leaching rate of iron increased quickly with increasing sulfuric acid concentration. This behavior is attributed to iron-bearing minerals such as zinc ferrite in zinc calcine dissolving at high temperatures and high sulfuric acid concentrations but not at low temperatures and low sulfuric acid concentrations.
基金finically supported by the National Natural Science Foundation of China(22075055)the Guangxi Science and Technology Project(AB16380030)the Innovation Project of Guangxi Graduate Education(YCSW2020052)。
文摘Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure of catalyst layers with efficient mass transportation channels plays a vital role.Herein,PEMFCs with order-structured cathodic electrodes were fabricated by depositing Pt nanoparticles by Ebeam onto vertically aligned carbon nanotubes(VACNTs)growth on Al foil via plasma-enhanced chemical vapor deposition.Results demonstrate that the proportion of hydrophilic Pt-deposited region along VACNTs and residual hydrophobic region of VANCTs without Pt strongly influences the cell performance,in particular at high current densities.When Pt nanoparticles deposit on the top depth of around 600 nm on VACNTs with a length of 4.6μm,the cell shows the highest performance,compared with others with various lengths of VACNTs.It delivers a maximum power output of 1.61 W cm^(-2)(H_(2)/O_(2),150 k Pa)and 0.79 W cm^(-2)(H_(2)/Air,150 k Pa)at Pt loading of 50μg cm^(-2),exceeding most of previously reported PEMFCs with Pt loading of<100μg cm^(-2).Even though the Pt loading is down to 30μg cm^(-2)(1.36 W cm^(-2)),the performance is also better than 100μg cm^(-2)(1.24 W cm^(-2))of commercial Pt/C,and presents better stability.This excellent performance is critical attributed to the ordered hydrophobic region providing sufficient mass passages to facilitate the fast water drainage at high current densities.This work gives a new understanding for oxygen reduction reaction occurred in VACNTs-based ordered electrodes,demonstrating the most possibility to achieve a substantial reduction in Pt loading<100μg cm^(-2) without sacrificing in performance.
基金Funded by the National Natural Science Foundation of China(11564009)the Natural Science Foundation of Guangxi Province(2013GXNSFBA019230 and 2014GXNSFAA118350)the Open Founding of Guangxi Ministry-Province Jointly-Constructed Cultivation Base for State Key Laboratory of Processing for Nonferrous Metal and Featured Materials(13KF-17 and 15KF-12)
文摘In order to found new dielectrics ceramics in tungsten bronze structure, unfilled tungsten bronze(TB) ceramics with nominal formula Ba4PrFe(0.5)Nb(9.5)O(30) were prepared by the solid state reaction method. The microstructure and dielectric properties were studied using powder X-ray diffraction, field emission scanning electron microscope, and variable temperature dielectric test system. The results show that the ceramics have a single phase and belong to the space group of P4bm with the cell of a = b = 12.4839(3) ?, c = 3.9409(5) ?, V = 614.192(2) ?3. The frequency dependent dielectrics properties show that the ceramics have a Debye-like relaxation at room temperature, while the temperature dependent dielectrics properties indicate that the ceramics are a relaxor and the relaxation is due to the nanopolars and oxygen vacancies. The ceramics have a potential application in electronic ceramics as temperature-stable multilayer ceramic capacitors.
文摘In this paper, the preparation of graphene oxide was achieved by Hummers method and the surface modification was achieved by poly(hexaneditiol), which was a synthetic thermotropic liquid crystalline polymer. The c-PHDT/GO/PF composites were prepared by blending, rolling and compression molding techniques. Then, the as-prepared samples were characterized by FTIR, Raman, XRD, TGA and POM to obtain information on their structures and properties. After that, the effects of c-PHDT/GO content on the mechanical properties, friction performance and dynamic mechanical performance of c-PHDT/GO/PF composites were studied by Mechanical and Dynamic Mechanical Analysis (DMA) methods. Also, Scanning Electron Microscope (SEM) was used for the characterization of wear and fracture surface morphology. The results revealed that the reinforcing effect of c-PHDT/GO was significant as a considerable enhancement on the mechanical performance of c-PHDT/GO/PF composite as compared to pure phenol-formaldehyde composites was observed: the impact strength, bending modulus and bending strength increased from 1.63 kJ/m2, 8.61 GPa and 41.55 MPa to 2.31 kJ/m2, 10.16 GPa and 54.40 MPa respectively at the c-PHDT/GO content = 0.75%. Moreover, the initial storage modulus increased by 28.4%, while the wear mass loss decreased by 17.8%. More importantly, the reinforcement by c-PHDT/GO was further enhanced as compared to GO/PF and p-PHDT/GO/PF composites, the impact strength of c-PHDT/GO/PF composite increased by 27.6% and 11.1%, the bending strength increased by 11.8% and 7.6%, the initial storage modulus increased by 16.2% and 4.2% and the mass loss due to wear decreased by 12.7% and 8.8%, respectively. Based on these results, we can conclude that the surface modification of GO by poly(hexanedithiol), which includes synergistic effect by c-PHDT and GO, improves the interfacial adhesion between GO and the resin matrix, thus reinforcing the composites.
基金A.A.,G.H.,S.H.,A.L.,and X.Y.J.thank the financial support from Kempe Foundation(SMK21-0011,SMK21-0020)A.L.acknowledges Swedish Research Council(2019-03865)European Union’s Horizon Europe research and innovation program under grant agreement No.101086667.X.Y.J.thanks the financial support from Horizon-EIC and Pathfinder challenges,Grant Number:101070976.
文摘The global practical implementation of proton exchange membrane fuel cells(PEMFCs)heavily relies on the advancement of highly effective platinum(Pt)-based electrocatalysts for the oxygen reduction reaction(ORR).To achieve high ORR performance,electrocatalysts with highly accessible reactive surfaces are needed to promote the uncovering of active positions for easy mass transportation.In this critical review,we introduce different approaches for the emerging development of effective ORR electrocatalysts,which offer high activity and durability.The strategies,including morphological engineering,geometric configuration modification via supporting materials,alloys regulation,core-shell,and confinement engineering of single atom electrocatalysts(SAEs),are discussed in line with the goals and requirements of ORR performance enhancement.We review the ongoing development of Pt electrocatalysts based on the syntheses,nanoarchitecture,electrochemical performances,and stability.We eventually explore the obstacles and research directions on further developing more effective electrocatalysts.
文摘Multimetallic Pt-based alloys with excavated structures have attracted great interest owing to their compositional and morphological tunability, high specific surface areas, and impressive electro-catalytic activities. Herein, we report the first facile one-pot synthesis of trimetallic Pt-Ni-Cu highly excavated rhombic dodecahedrons (ERDs) with a yield approaching 100%. More importantly, these highly uniform nanocrystals have three-dimensionally accessible excavated surfaces, where abundant stepped atoms are observed. Benefiting from the highly excavated rhombic dodecahedral structures, electronic and synergistic effects within the trimetallic allo3~ and abundant stepped atoms, the as-prepared trimetallic Pt-Ni-Cu ERDs exhibit an enhanced electro-catalytic performance for the electro-oxidation of methanol compared to commercial Pt/C and bimetallic Pt-Cu ERDs and Pt-Ni-Cu solid rhombic dodecahedrons solid rhombic dodecahedrons (SRDs).
基金the Guangxi Science and Technology Project(AA17204083,AB16380030)the link project of the National Natural Science Foundation of China and Fujian Province(U1705252)the Natural Science Foundation of Guangdong Province(2015A030312007).
文摘Electrochemical water splitting is regarded as the most auspicious technology for renewable sources,transport,and storage of hydrogen energy.Currently,noble Pt metal and noble-metal oxides(IrO_(2)and RuO_(2))are recognized as state-of-the-art electrocatalysts for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively.Searching for earth-abundant electrocatalysts for the HER and OER with remarkable performance and high stability to replace precious metals plays a significant role in the commercial application of electrochemical water splitting.In this review,recent advancements in nanostructured transition metal electrocatalysts are assessed through the selected examples of nitrides,carbides,phosphides,sulfides,borides,layered double hydroxides,and oxides.Recent breakthroughs in nanostructured transition metal electrocatalysts are discussed in terms of their mechanisms,controllable production,structural design,and innovative strategies for boosting their performance.For instance,most nanostructured transition metal electrocatalysts for overall water splitting(OWS)only function well in neutral and alkaline solutions.Finally,current research challenges and future perspectives for increasing the performance of nanostructured transition metals for OWS are proposed.
基金supported by the National Natural Science Foundation of China (Grant Nos. 51601108, 51571134)the Natural Science Foundation of Shandong Province (Grant No. 2016ZRB01A62)the SDUST Research Fund (No. 2014TDJH104) and the Ministry-province jointly-constructed cultivation base for state key laboratory of Processing for non-ferrous metal and featured materials, "Guangxi Zhuang Autonomous Region"
文摘Layered double hydroxides(LDHs) as a class of anionic clays have extensive applications due to their unique structures. Nowadays, the emphasis is laid on the development of LDH coatings for corrosion resistance and medical applications. Thus, this review highlights synthetic methods of LDH coatings and LDH-based composite coatings on magnesium alloys. Special attention is focused on self-healing,biocompatible and self-cleaning LDH-based composite coatings on magnesium alloys.
基金Acknowledgement The authors acknowledge financial support of National Natural Science Foundation of China (No. 51363005), Scientific Foundation of Colleges and Universities of Guangxi Province (No. 2013YB115), Innovation Project of Guangxi Graduate Education (No. YCSZ2013076), and Guangxi Funds for Specially-appointed Expert.
文摘Graphene/polyaniline nanotube (GPNT) composite was synthesized using Vitamin C as both the template of polyaniline nanotube via in situ polymerization of aniline and the reducing agent of graphene oxide. The pure polyaniline (PANI), graphene/PANI composite (GP) (using hydrazine monohydrate instead of VC) and GO/PANI composite were also prepared. IR spectroscopy and morphologies of the as-prepared samples were characterized. And the electrochemical performances were conducted on a three-electrode cell. IR spectroscopy demonstrated the in- teraction between graphene and PANI nanotube in GPNT, which is beneficial to enhance the electrochemical performance of the composite electrode. Surface morphology showed PANI nanotube with outer diameter of 140 nm in GPNT. GPNT composites exhibited better electrochemical performances than GP composite and pure PANI. The electrochemical performances showed that the specific capacitance of GPNT was 561 F/g which is more than that of either GP or PANI, it is not only due to the graphene which can provide good electrical conductivity and high specific surface area, but also associated with a good redox activity of ordered PANI nanotubes. The as-prepared GPNT composites with higher conductivity, lower resistance and better cycle life in our laboratory are promising electrode materials for high-performance electrical energy storage devices.
基金supported by National Natural Science Foundation of China(Grant 11874240)Guangxi Information Materials Key Laboratory Open Research Fund(171007-K)+3 种基金State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(No.KF201811)the Opening Project of Key Laboratory of Inorganic Functional Materials and Devices,Chinese Academy of Sciences(Grant No.KLIFMD201803)the Natural Science Foundation of Shandong Province,China(No.ZR2016EMM21)Scientific Research Foundation of Shandong University of Science and Technology for Recruited Talents(No.2016RCJJ002).
文摘Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(XRD)and scanning electron microscopy(SEM),respectively.The main crystalline phase is monoclinic Nd(Mg_(1/2)Sn_(1/2))O_(3) with a double perovskite structure(P21/n space group)for the NMS system proved by XRD.The sample at x=0.01 has the best crystallinity and evenly distributed crystal grains observed by SEM.The optimum performances(ε_(r)=19.87,Q×f=41840 GHz,f=12.05 GHz)are obtained at x=0.01.Lattice vibrational modes of the Raman spectra were assigned and illustrated,in detail.The dielectric properties obtained by fitting infrared reflectance spectra with the help of four-parameter semi-quantum model are consistent with the calculated values by microscopic polarization and damping coefficients.The reverse translational vibration of the NdeMgO_(6),the F_(5u)^((5)) mode,provides the greatest contribution to the dielectric response.The relationships between crystal structures and dielectric properties were mainly established using lattice vibrational modes as a media.
基金This work is supported by the National Natural Science Foundation of China(No.21872040)the Hundred Talents Program of Guangxi Universities,the Excellent Scholars and Innovation Team of Guangxi Universities,Guangxi Major Projects of Science and Technology(No.GXMPSTAA17202032),Guangxi Ba-Gui Scholars Program.
文摘Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeWO_(4)-WO_(3) heterostructure catalyst growing on nickel foam (FeWO_(4)-WO_(3)/NF) by a combination of hydrothermal and calcination method. It shows good catalytic activity with ultralow potentials for OER (ζ_(10) = 1.43 V, ζ_(1.000) = 1.56 V) and HzOR (ζ_(10) = −0.034 V, ζ_(1.000) = 0.164 V). Moreover, there is little performance degradation after being tested for _(10)0 h at 1,000 (OER) and _(10)0 (HzOR) mA·cm−2, indicating good stability. The superior performance could be attributed to the wolframite structure and heterostructure: The former provides a high electrical conductivity to ensure the electronic transfer capability, and the later induces interfacial electron redistribution to enhance the intrinsic activity and stability. The work offers a brand-new way to prepare good performance catalysts for OER and HzOR, especially at large current density.
文摘Fe-Ni-Cr-based super-high-strength maraging stainless steels were generally realized by multiple-element alloying under a given heat treatment processing. A series of alloy compositions were designed with a uniform cluster formula of [Ni16Fe192](Cr32(Ni16-x-y-z-m-n MoxTiyNbzAlmVn)) (at.%) that was developed out of a unique alloy design tool, a cluster- plus-glue-atom model. Alloy rods with a diameter of 6 mm were prepared by copper-mold suction-cast processing under the argon atmosphere. These alloy samples were solid-solutioned at 1273 K for 1 h, followed by water-quenching, and then aged at 783 K for 3 h. The effect of the valence electron concentration, characterized with the number of valence electrons per unit cluster (VE/uc) formula of 16 atoms, on microhardness of these designed maraging stainless steels at both solid- solutioned and aged states was investigated. The relationship between alloy compositions and microhardness in maraging stainless steels was firstly established by the random forest (RF, a kind of machine learning methods) based on the experimental results. It was found that not only the microhardness of any given composition alloy within the frame of cluster formula, but also the alloy composition with a maximum microhardness for any given VE/uc, could be predicted in good agreement with the guidance of the relationship by RF. The contributions of minor-alloying elements to the microhardness of the aged alloys were also discussed.
基金This work was supported by the National Natural Science Foundation of China(Grant No.21676285)the Shandong University of Science and Technology Research Fund(Grant No.2014TDJH104)+1 种基金the Qingdao Indigenous Innovation Program(Grant No.15-9-1-76-jch)the Scientific Research Foundation of Shandong University of Science and Technology for Recruited Talents(Grant No.2017RCJJ015).
文摘Mo-V-Nb tri-component oxide catalysts were prepared and firstly used for the selective oxidation of Cα-OH lignin compounds.The catalytic performance of the composite oxides was obviously enhanced due to the synergistic effects of Mo and V elements.Mo5-xVxO14 phase with a variable Mo/V ratio provided suitable active sites for the oxidative dehydrogenation(ODH)of Cα-OH lignin model compound.The optimized Mo-V-Nb molar composition was confirmed as Mo0.61V0.31Nb0.08Ox/TiO2,which exhibited the prominent catalytic activity with the turnover frequency of 1.04×10-3 mmol·g(cat)-1·s-1.Even at room temperature,the catalysts showed highly-efficient ODH reaction activities.The active phase for selective oxidation reaction and the inhibiting effect ofα-MoO3 phase were also discussed in the study.