Material composition and structural design are important factors influencing the electromagnetic wave(EMW)absorption performance of materials.To alleviate the impedance mismatch attributed to the high dielectric const...Material composition and structural design are important factors influencing the electromagnetic wave(EMW)absorption performance of materials.To alleviate the impedance mismatch attributed to the high dielectric constant of Ti_(3)C_(2)T_(x)MXene,we have successfully synthesized core‐shell structured SiO_(2)@MXene@MoS_(2)nanospheres.This architecture,comprising SiO_(2) as the core,MXene as the intermediate layer,and MoS_(2) as the outer shell,is achieved through an electrostatic self‐assembly method combined with a hydrothermal process.This complex core‐shell structure not only provides a variety of loss mechanisms that effectively dissipate electromagnetic energy but also prevents self‐aggregation of MXene and MoS_(2) nanosheets.Notably,the synergistic combination of SiO_(2) and MoS_(2) with highly conductive MXene enables the suitable dielectric constant of the composites,ensuring optimal impedance matching.Therefore,the core‐shell structured SiO_(2)@MXene@MoS_(2) nanospheres exhibit excellent EMW absorption performance,featuring a remarkable minimum reflection loss(RL_(min))of−52.11 dB(2.4 mm).It is noteworthy that these nanospheres achieve an ultra‐wide effective absorption bandwidth(EAB)of 6.72 GHz.This work provides a novel approach for designing and synthesizing high‐performance EMW absorbers characterized by“wide bandwidth and strong reflection loss.”展开更多
Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme hetero...Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.展开更多
Development of metal oxide semiconductors-based methane sensors with good response and low power consumption is one of the major challenges to realize the real-time monitoring of methane leakage.In this work,a self-as...Development of metal oxide semiconductors-based methane sensors with good response and low power consumption is one of the major challenges to realize the real-time monitoring of methane leakage.In this work,a self-assembled mulberry-like ZnO/SnO_(2)hierarchical structure is constructed by a two-step hydrothermal method.The resultant sensor works at room temperature with excellent response of~56.1%to 2000 ppm CH_(4)at 55%relative humidity.It is found that the strain induced at the ZnO/SnO_(2)interface greatly enhances the piezoelectric polarization on the ZnO surface and that the band bending results in the accumulation of chemically adsorbed O_(2)^(-)ions close to the interface,leading to significant improvement in the sensing performance of the methane gas sensor at room temperature.展开更多
The recent advancement in the design,synthesis,and fabrication of micro/nano structured LiNixCoyMnzO2 with one-,two-,and three-dimensional morphologies was reviewed.The major goal is to highlight LiNixCoyMnzO2 materia...The recent advancement in the design,synthesis,and fabrication of micro/nano structured LiNixCoyMnzO2 with one-,two-,and three-dimensional morphologies was reviewed.The major goal is to highlight LiNixCoyMnzO2 materials,which have been utilized in lithium ion batteries with enhanced energy and power density,high energy efficiency,superior rate capability and excellent cycling stability resulting from the doping,surface coating,nanocomposites and nano-architecturing.展开更多
Mo_(2)C is an excellent electrocatalyst for hydrogen evolution reaction(HER).However,Mo_(2)C is a poor electrocatalyst for oxygen evolution reaction(OER).Herein,two different elements,namely Co and Fe,are incorporated...Mo_(2)C is an excellent electrocatalyst for hydrogen evolution reaction(HER).However,Mo_(2)C is a poor electrocatalyst for oxygen evolution reaction(OER).Herein,two different elements,namely Co and Fe,are incorporated in Mo_(2)C that,therefore,has a finely tuned electronic structure,which is not achievable by incorporation of any one of the metals.Consequently,the resulting electrocatalyst Co_(0.8)Fe_(0.2)-Mo_(2)C-80 displayed excellent OER catalytic performance,which is evidenced by a low overpotential of 214.0(and 246.5)mV to attain a current density of 10(and 50)mA cm^(-2),an ultralow Tafel slope of 38.4 mV dec^(-1),and longterm stability in alkaline medium.Theoretical data demonstrates that Co_(0.8)Fe_(0.2)-Mo_(2)C-80 requires the lowest overpotential(1.00 V)for OER and Co centers to be the active sites.The ultrahigh catalytic performance of the electrocatalyst is attributed to the excellent intrinsic catalytic activity due to high Brunauer-Emmett-Teller specific surface area,large electrochemically active surface area,small Tafel slope,and low chargetransfer resistance.展开更多
As a promising anode material for magnesium ion rechargeable batteries,magnesium metavanadate(MgV_(2)O_(6))has attracted considerable research interest in recent years.A MgV_(2)O_(6)sample was synthesized via a facile...As a promising anode material for magnesium ion rechargeable batteries,magnesium metavanadate(MgV_(2)O_(6))has attracted considerable research interest in recent years.A MgV_(2)O_(6)sample was synthesized via a facile solid-state reaction by multistep-firing stoichiometric mixtures of MgO and V2O5 powder under an air atmosphere.The solid-state phase transition fromα-MgV_(2)O_(6)toβ-MgV_(2)O_(6)occurred at 841 K and the enthalpy change was 4.37±0.04 kJ/mol.The endothermic effect at 1014 K and the enthalpy change was 26.54±0.26 kJ/mol,which is related to the incongruent melting ofβ-MgV_(2)O_(6).In situ XRD was performed to investigate phase transition of the as-prepared MgV_(2)O_(6)at high temperatures.The cell parameters obtained by Rietveld refinement indicated that it crystallizes in a monoclinic system with the C2/m space group,and the lattice parameters of a=9.280 A°,b=3.501 A°,c=6.731 A°,β=111.76°.The solid-state phase transition fromα-MgV_(2)O_(6)toβ-MgV_(2)O_(6)was further studied by thermal kinetics,indicating that this process is controlled first by a fibril-like mechanism and then by a spherulitic-type mechanism with an increasing heating rate.Additionally,the enthalpy change of MgV_(2)O_(6)at high temperatures was measured utilizing the drop calorimetry,heat capacity was calculated and given as:Cp=208.3+0.03583T-4809000T^(−2)(298-923 K)(J mol^(−1)K^(−1)),the high-temperature heat capacity can be used to calculate Gibbs free energy of MgV_(2)O_(6)at high temperatures.展开更多
We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation O...We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation Observing System for Meteorology,Ionosphere,and Climate-2(COSMIC-2)satellite.Owing to the dense sampling of COSMIC-2,in addition to the strong peaks of gravity wave potential energy(GWPE)above the Andes and Tibetan Plateau,we found weak peaks above the Rocky,Atlas,Caucasus,and Tianshan Mountains.The land-sea contrast is responsible for the longitudinal variations of the GWPE in the lower and upper stratosphere.At 40°N/S,the peaks were mainly above the topographic regions during the winter.At 20°N/S,the peaks were a slight distance away from the topographic regions and might be the combined effect of nontopographic GWs and mountain waves.Near the Equator,the peaks were mainly above the regions with the lowest sea level altitude and may have resulted from convection.Our results indicate that even above the local regions with lower sea level altitudes compared with the Andes and Tibetan Plateau,the GWPE also exhibits fine structures in geographic distributions.We found that dissipation layers above the tropopause jet provide the body force to generate secondary waves in the upper stratosphere,especially during the winter months of each hemisphere and at latitudes of greater than 20°N/S.展开更多
The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction...The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.展开更多
The Schiff base, 2-{（2′-benzyl）iminoethyl}-5-methoxyphenol （C6H4CH2N=C（CH3）C6H3- （OMe-5）OH） 1, was synthesized and characterized by elemental analysis, IR and X-ray single-crystal diffraction. The compound cr...The Schiff base, 2-{（2′-benzyl）iminoethyl}-5-methoxyphenol （C6H4CH2N=C（CH3）C6H3- （OMe-5）OH） 1, was synthesized and characterized by elemental analysis, IR and X-ray single-crystal diffraction. The compound crystallizes in the orthorhombic system, space group Pbca with a = 8.9849（10）, b = 13.2699（15）, c = 22.975（2） A ,V= 2739.3（5） A^3, Mr= 255.31, Z= 8, F（000） = 1088, Dc = 1.238 g/cm^3, T= 293 K, μ = 0.082 mm^-1, λ = 0.71073 .A, the final R = 0.0596 and wR = 0.1575 for 1934 observed reflections with I 〉 2σ（I）. The complex was valued for its antimicrobial activity against bacterial strands using the agar diffusion method, and found to be active against the four test bacterial organisms.展开更多
The novel coordination polymer [Pr（BYBA）3（H2O）2]·[Pr（BYBA）3（H2O）] （BYBAH = 2-benzoylbenzoic acid） was yielded by hydrothermal synthesis, determined by single-crystal X-ray diffraction, and characterized...The novel coordination polymer [Pr（BYBA）3（H2O）2]·[Pr（BYBA）3（H2O）] （BYBAH = 2-benzoylbenzoic acid） was yielded by hydrothermal synthesis, determined by single-crystal X-ray diffraction, and characterized by FT-IR and UV-Vis spectra. The crystal crystallizes in the triclinic system, space group P1 with a = 9.112（3）, b = 14.644（5）, c = 27.076（11） A, α = 84.223（3）,β = 87.816（4）,γ = 88.902（4）°, V= 3592（2）A, C84H60O21Pr2, Mr = 1687.14, Z = 2, F（000） = 1700, Dc = 1.560 g/cm^3, μ=1.419mm^-1, the fmal R = 0.0485 and wR = 0.1258 for 13035 observed reflections with I 〉 2σ（Ⅰ）. The compound contains two different building milts, [Pr2（BYBA）6（H2O）4] and [Pr2（BYBA）6（H2O）2]. It is noticeable that [Pr2（BYBA）6（H2O）4] is an isolated binuclear building block, in which the Pr3＋ ion centers are both located in an eight-coordinated environment. However, in [Pr2（BYBA）6（H2O）2] the Pr^3＋ ion centers are located in a nine-coordinated envirormlent and connected by BYBA ligands to form 1D chains.展开更多
Several MoS2 catalysts of different structure, prepared by in situ decomposition of ammonium heptamolybdate （AHM） and molybdenum naphthenate （MoNaph）, and by MoS2 exfoliation （TDM）, were characterized by BET, X-...Several MoS2 catalysts of different structure, prepared by in situ decomposition of ammonium heptamolybdate （AHM） and molybdenum naphthenate （MoNaph）, and by MoS2 exfoliation （TDM）, were characterized by BET, X-ray diffraction （XRD）, Energy Dispersive X-ray （EDX） and transmission electron microscopy （TEM）. The analysis showed that MoS2 structure was dependant upon the preparation procedure. The activity of the catalysts was determined by measuring the hydrodeoxygenation （HDO） of phenol, 4-methylphenol and 4-methoxyphenol using a batch autoclave reactor operated at 2.8 MPa of hydrogen and temperatures ranging from 320-370℃. By comparing the conversion, the reactivity order of the catalysts was： AHM〉TDM-D〉MoNaph〉thermal〉MoS2 powder〉 TDM-W. Also, the effect of reaction temperature on the HDO conversion was explained in terms of equilibrium of reversible reaction kinetics. The main products of the HDO for phenolic compounds were identified by gas chromatography/mass spectrometry （GC/MS）. The results showed that the product distribution and the HDO selectivity were correlated with the reaction temperature. Two parallel reaction routes, direct hydrogenolysis and combined hydrogenation-hydrogenolysis, were confirmed by the analysis of the product distribution. High temperature favored hydrogenolysis over hydrogenation for HDO of phenol and 4-methoxyphenol, whereas for 4-methylphenol the reverse was true.展开更多
The title compound bi(2-nitrilethyl)aminoacetonitrile has been prepared by the addition reaction of aminoacetonitrile with acrylonitrile, and its crystal structure was determined by single-crystal X-ray diffraction. T...The title compound bi(2-nitrilethyl)aminoacetonitrile has been prepared by the addition reaction of aminoacetonitrile with acrylonitrile, and its crystal structure was determined by single-crystal X-ray diffraction. The compound (C8H10N4) crystallizes in monoclinic, space group P21/n with a = 7.646(12), b = 14.578(2), c = 8.341(1) ? ?= 100.38(1)? V = 914.5(14) 3, Mr = 162.20, Z = 4, F(000) = 344, Dc = 1.178 g/cm3, T = 293 K, = 0. 077 mm-1 and l = 0.71073 ? The structure was refined to R = 0.0574 and wR = 0.1331 for 1107 observed reflections with I > 2(I).展开更多
In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respective...In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respectively.The introduction of Cr^3+and Cr2O3/C,which were derived from the calcination of MIL-101,in the composite enhanced its visible light absorbing ability and lowered the recombination rate of the photogenerated electrons and holes.The large surface area of the Cr2O3/C@TiO2 composite provided numerous active sites for the photoreduction reaction.Consequently,the photocatalytic performance of the composite for the production of H2 was better than that of pure TiO2.Under the irradiation of a 300 W Xe arc lamp,the H2 production rate of the Cr2O3/C@TiO2 composite that was calcined at 500°C was 446μmol h−1 g−1,which was approximately four times higher than that of pristine TiO2 nanoparticles.Moreover,the composite exhibited the high H2 production rate of 25.5μmol h−1 g−1 under visible light irradiation(λ>420 nm).The high photocatalytic performance of Cr2O3/C@TiO2 could be attributed to its wide visible light photoresponse range and efficient separation of photogenerated electrons and holes.This paper offers some insights into the design of a novel efficient photocatalyst for water-splitting applications.展开更多
The 1,5-disubstituted thiocarbohydrazide ligands were prepared by the condensation of thiocarbohydrazide with salicylaldehyde and 5-methylsalicylaldehyde, respectively. The butyltin complexes,[(5-R-2-hydroxy)ArCH=NNH]...The 1,5-disubstituted thiocarbohydrazide ligands were prepared by the condensation of thiocarbohydrazide with salicylaldehyde and 5-methylsalicylaldehyde, respectively. The butyltin complexes,[(5-R-2-hydroxy)ArCH=NNH]2 CS(n-BuSnCl)2, R = H(T1);R = Me(T2), based on the1,5-disubstituted thiocarbohydrazide were obtained by microwave-assisted solvothermal reaction of n-butyltintrichloride precursor with the ligands in methanol environments, which have been structurally characterized by elemental analysis, IR and(1 H, 13 C) NMR spectra. The crystals belong to monoclinic system, space groups C2/c(T1) and Pc(T2), respectively. The Sn atom is six-coordinated with distorted octahedral geometry by O, N and S atoms from ligand, C atom of butyl and two Cl atoms. In the crystal, complex T1 forms three-dimensional supramolecular assembly mediated by noncovalent interactions such as C–H···Cl and π-stacking interactions.Similarly, T2 forms an interesting two-dimensional supramolecular structure by noncovalent interactions(e.g. C–H×××Cl and N–H×××Cl) of one-dimensional band-like chain. These ligands and its butyltin complexes have growth effect on the target plants, such as Portulaca oleracea L.,Amaranthus spinosus L., Cassia tora L., Brassica campestris L. ssp. chinensis var. utilis Tsen et Lee and Amaranthus tricolor L. The ligand L1 has a good inhibitory effect on the growth of Cassia tora L., and complex T2 has selective inhibition on the growth of Portulaca oleracea L. and Amaranthus tricolor L., which can be used as a candidate compound for Cassia tora L., Portulaca oleracea L.and Amaranthus tricolor L. herbicide.展开更多
基金Joint Fund of Research and Development Program of Henan Province,Grant/Award Number:222301420002National Natural Science Foundation of China,Grant/Award Number:U21A2064Scientific and Technological Innovation Talents in Colleges and Universities in Henan Province,Grant/Award Number:22HASTIT001。
文摘Material composition and structural design are important factors influencing the electromagnetic wave(EMW)absorption performance of materials.To alleviate the impedance mismatch attributed to the high dielectric constant of Ti_(3)C_(2)T_(x)MXene,we have successfully synthesized core‐shell structured SiO_(2)@MXene@MoS_(2)nanospheres.This architecture,comprising SiO_(2) as the core,MXene as the intermediate layer,and MoS_(2) as the outer shell,is achieved through an electrostatic self‐assembly method combined with a hydrothermal process.This complex core‐shell structure not only provides a variety of loss mechanisms that effectively dissipate electromagnetic energy but also prevents self‐aggregation of MXene and MoS_(2) nanosheets.Notably,the synergistic combination of SiO_(2) and MoS_(2) with highly conductive MXene enables the suitable dielectric constant of the composites,ensuring optimal impedance matching.Therefore,the core‐shell structured SiO_(2)@MXene@MoS_(2) nanospheres exhibit excellent EMW absorption performance,featuring a remarkable minimum reflection loss(RL_(min))of−52.11 dB(2.4 mm).It is noteworthy that these nanospheres achieve an ultra‐wide effective absorption bandwidth(EAB)of 6.72 GHz.This work provides a novel approach for designing and synthesizing high‐performance EMW absorbers characterized by“wide bandwidth and strong reflection loss.”
文摘Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.
基金financially supported by the National Natural Science Foundation of China(No.12174092,21902046,U21A20500)Overseas Expertise Introduction Center for Discipline Innovation(D18025)+1 种基金Hubei Provincial Department of Science and Technology(No.2019CFA079)Wuhan Science and Technology Bureau(2020010601012163)
文摘Development of metal oxide semiconductors-based methane sensors with good response and low power consumption is one of the major challenges to realize the real-time monitoring of methane leakage.In this work,a self-assembled mulberry-like ZnO/SnO_(2)hierarchical structure is constructed by a two-step hydrothermal method.The resultant sensor works at room temperature with excellent response of~56.1%to 2000 ppm CH_(4)at 55%relative humidity.It is found that the strain induced at the ZnO/SnO_(2)interface greatly enhances the piezoelectric polarization on the ZnO surface and that the band bending results in the accumulation of chemically adsorbed O_(2)^(-)ions close to the interface,leading to significant improvement in the sensing performance of the methane gas sensor at room temperature.
基金Projects(51134007,21003161,21250110060) supported by the National Natural Science Foundation of ChinaProject(11MX10) supported by Central South University Annual Mittal-Founded Innovation ProjectProject(2011ssxt086) supported by Fundamental Research Funds for the Central Universities,China
文摘The recent advancement in the design,synthesis,and fabrication of micro/nano structured LiNixCoyMnzO2 with one-,two-,and three-dimensional morphologies was reviewed.The major goal is to highlight LiNixCoyMnzO2 materials,which have been utilized in lithium ion batteries with enhanced energy and power density,high energy efficiency,superior rate capability and excellent cycling stability resulting from the doping,surface coating,nanocomposites and nano-architecturing.
基金financial support from the SERB-SURE under file number of SUR/2022/003129Jong Hyeok Park acknowledges the support of the National Research Foundation of Korea (NRF)funded by the Ministry of Science and ICT (RS-2023-00302697,RS-2023-00268523).
文摘Mo_(2)C is an excellent electrocatalyst for hydrogen evolution reaction(HER).However,Mo_(2)C is a poor electrocatalyst for oxygen evolution reaction(OER).Herein,two different elements,namely Co and Fe,are incorporated in Mo_(2)C that,therefore,has a finely tuned electronic structure,which is not achievable by incorporation of any one of the metals.Consequently,the resulting electrocatalyst Co_(0.8)Fe_(0.2)-Mo_(2)C-80 displayed excellent OER catalytic performance,which is evidenced by a low overpotential of 214.0(and 246.5)mV to attain a current density of 10(and 50)mA cm^(-2),an ultralow Tafel slope of 38.4 mV dec^(-1),and longterm stability in alkaline medium.Theoretical data demonstrates that Co_(0.8)Fe_(0.2)-Mo_(2)C-80 requires the lowest overpotential(1.00 V)for OER and Co centers to be the active sites.The ultrahigh catalytic performance of the electrocatalyst is attributed to the excellent intrinsic catalytic activity due to high Brunauer-Emmett-Teller specific surface area,large electrochemically active surface area,small Tafel slope,and low chargetransfer resistance.
基金supported by the National Key R&D Program of China(2018YFC1900500)the Graduate Scientific Research and Innovation Foundation of Chongqing,China(Grant No.CYB20002).
文摘As a promising anode material for magnesium ion rechargeable batteries,magnesium metavanadate(MgV_(2)O_(6))has attracted considerable research interest in recent years.A MgV_(2)O_(6)sample was synthesized via a facile solid-state reaction by multistep-firing stoichiometric mixtures of MgO and V2O5 powder under an air atmosphere.The solid-state phase transition fromα-MgV_(2)O_(6)toβ-MgV_(2)O_(6)occurred at 841 K and the enthalpy change was 4.37±0.04 kJ/mol.The endothermic effect at 1014 K and the enthalpy change was 26.54±0.26 kJ/mol,which is related to the incongruent melting ofβ-MgV_(2)O_(6).In situ XRD was performed to investigate phase transition of the as-prepared MgV_(2)O_(6)at high temperatures.The cell parameters obtained by Rietveld refinement indicated that it crystallizes in a monoclinic system with the C2/m space group,and the lattice parameters of a=9.280 A°,b=3.501 A°,c=6.731 A°,β=111.76°.The solid-state phase transition fromα-MgV_(2)O_(6)toβ-MgV_(2)O_(6)was further studied by thermal kinetics,indicating that this process is controlled first by a fibril-like mechanism and then by a spherulitic-type mechanism with an increasing heating rate.Additionally,the enthalpy change of MgV_(2)O_(6)at high temperatures was measured utilizing the drop calorimetry,heat capacity was calculated and given as:Cp=208.3+0.03583T-4809000T^(−2)(298-923 K)(J mol^(−1)K^(−1)),the high-temperature heat capacity can be used to calculate Gibbs free energy of MgV_(2)O_(6)at high temperatures.
基金the National Natural Science Foundation of China(Grant Nos.41831073,42174196,and 42374205)the Project of Stable Support for Youth Team in Basic Research Field,Chinese Academy of Sciences(CAS+4 种基金Grant No.YSBR-018)the Informatization Plan of CAS(Grant No.CAS-WX2021PY-0101)the Youth Cross Team Scientific Research project of the Chinese Academy of Sciences(Grant No.JCTD-2021-10)the Open Research Project of Large Research Infrastructures of CAS titled“Study on the Interaction Between Low-/Mid-Latitude Atmosphere and Ionosphere Based on the Chinese Meridian Project.”This work was also supported in part by the Specialized Research Fund and the Open Research Program of the State Key Laboratory of Space Weather.
文摘We derive the potential energy of gravity waves(GWs)in the upper troposphere and stratosphere at 45°S-45°N from December 2019 to November 2022 by using temperature profiles retrieved from the Constellation Observing System for Meteorology,Ionosphere,and Climate-2(COSMIC-2)satellite.Owing to the dense sampling of COSMIC-2,in addition to the strong peaks of gravity wave potential energy(GWPE)above the Andes and Tibetan Plateau,we found weak peaks above the Rocky,Atlas,Caucasus,and Tianshan Mountains.The land-sea contrast is responsible for the longitudinal variations of the GWPE in the lower and upper stratosphere.At 40°N/S,the peaks were mainly above the topographic regions during the winter.At 20°N/S,the peaks were a slight distance away from the topographic regions and might be the combined effect of nontopographic GWs and mountain waves.Near the Equator,the peaks were mainly above the regions with the lowest sea level altitude and may have resulted from convection.Our results indicate that even above the local regions with lower sea level altitudes compared with the Andes and Tibetan Plateau,the GWPE also exhibits fine structures in geographic distributions.We found that dissipation layers above the tropopause jet provide the body force to generate secondary waves in the upper stratosphere,especially during the winter months of each hemisphere and at latitudes of greater than 20°N/S.
基金supported by the National Key Research and Development Program of China(2021YFB4001301)the Science and Technology Commission of Shanghai Municipality(21DZ1208600)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2021ZD105)。
文摘The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.
基金This work was supported by the Key Laboratory of Marine Biotechnology of Jiangsu Province
文摘The Schiff base, 2-{（2′-benzyl）iminoethyl}-5-methoxyphenol （C6H4CH2N=C（CH3）C6H3- （OMe-5）OH） 1, was synthesized and characterized by elemental analysis, IR and X-ray single-crystal diffraction. The compound crystallizes in the orthorhombic system, space group Pbca with a = 8.9849（10）, b = 13.2699（15）, c = 22.975（2） A ,V= 2739.3（5） A^3, Mr= 255.31, Z= 8, F（000） = 1088, Dc = 1.238 g/cm^3, T= 293 K, μ = 0.082 mm^-1, λ = 0.71073 .A, the final R = 0.0596 and wR = 0.1575 for 1934 observed reflections with I 〉 2σ（I）. The complex was valued for its antimicrobial activity against bacterial strands using the agar diffusion method, and found to be active against the four test bacterial organisms.
基金the State Key Laboratory of Structural Chemistry and Foundation of Education Committee of Fujian Province (No. JB04049).
文摘The novel coordination polymer [Pr（BYBA）3（H2O）2]·[Pr（BYBA）3（H2O）] （BYBAH = 2-benzoylbenzoic acid） was yielded by hydrothermal synthesis, determined by single-crystal X-ray diffraction, and characterized by FT-IR and UV-Vis spectra. The crystal crystallizes in the triclinic system, space group P1 with a = 9.112（3）, b = 14.644（5）, c = 27.076（11） A, α = 84.223（3）,β = 87.816（4）,γ = 88.902（4）°, V= 3592（2）A, C84H60O21Pr2, Mr = 1687.14, Z = 2, F（000） = 1700, Dc = 1.560 g/cm^3, μ=1.419mm^-1, the fmal R = 0.0485 and wR = 0.1258 for 13035 observed reflections with I 〉 2σ（Ⅰ）. The compound contains two different building milts, [Pr2（BYBA）6（H2O）4] and [Pr2（BYBA）6（H2O）2]. It is noticeable that [Pr2（BYBA）6（H2O）4] is an isolated binuclear building block, in which the Pr3＋ ion centers are both located in an eight-coordinated environment. However, in [Pr2（BYBA）6（H2O）2] the Pr^3＋ ion centers are located in a nine-coordinated envirormlent and connected by BYBA ligands to form 1D chains.
文摘Several MoS2 catalysts of different structure, prepared by in situ decomposition of ammonium heptamolybdate （AHM） and molybdenum naphthenate （MoNaph）, and by MoS2 exfoliation （TDM）, were characterized by BET, X-ray diffraction （XRD）, Energy Dispersive X-ray （EDX） and transmission electron microscopy （TEM）. The analysis showed that MoS2 structure was dependant upon the preparation procedure. The activity of the catalysts was determined by measuring the hydrodeoxygenation （HDO） of phenol, 4-methylphenol and 4-methoxyphenol using a batch autoclave reactor operated at 2.8 MPa of hydrogen and temperatures ranging from 320-370℃. By comparing the conversion, the reactivity order of the catalysts was： AHM〉TDM-D〉MoNaph〉thermal〉MoS2 powder〉 TDM-W. Also, the effect of reaction temperature on the HDO conversion was explained in terms of equilibrium of reversible reaction kinetics. The main products of the HDO for phenolic compounds were identified by gas chromatography/mass spectrometry （GC/MS）. The results showed that the product distribution and the HDO selectivity were correlated with the reaction temperature. Two parallel reaction routes, direct hydrogenolysis and combined hydrogenation-hydrogenolysis, were confirmed by the analysis of the product distribution. High temperature favored hydrogenolysis over hydrogenation for HDO of phenol and 4-methoxyphenol, whereas for 4-methylphenol the reverse was true.
文摘The title compound bi(2-nitrilethyl)aminoacetonitrile has been prepared by the addition reaction of aminoacetonitrile with acrylonitrile, and its crystal structure was determined by single-crystal X-ray diffraction. The compound (C8H10N4) crystallizes in monoclinic, space group P21/n with a = 7.646(12), b = 14.578(2), c = 8.341(1) ? ?= 100.38(1)? V = 914.5(14) 3, Mr = 162.20, Z = 4, F(000) = 344, Dc = 1.178 g/cm3, T = 293 K, = 0. 077 mm-1 and l = 0.71073 ? The structure was refined to R = 0.0574 and wR = 0.1331 for 1107 observed reflections with I > 2(I).
文摘In this study,the Cr2O3/C@TiO2 composite was synthesized via the calcination of yolk–shell MIL-101@TiO2.The composite presented core–shell structure,where Cr-doped TiO2 and Cr2O3/C were the shell and core,respectively.The introduction of Cr^3+and Cr2O3/C,which were derived from the calcination of MIL-101,in the composite enhanced its visible light absorbing ability and lowered the recombination rate of the photogenerated electrons and holes.The large surface area of the Cr2O3/C@TiO2 composite provided numerous active sites for the photoreduction reaction.Consequently,the photocatalytic performance of the composite for the production of H2 was better than that of pure TiO2.Under the irradiation of a 300 W Xe arc lamp,the H2 production rate of the Cr2O3/C@TiO2 composite that was calcined at 500°C was 446μmol h−1 g−1,which was approximately four times higher than that of pristine TiO2 nanoparticles.Moreover,the composite exhibited the high H2 production rate of 25.5μmol h−1 g−1 under visible light irradiation(λ>420 nm).The high photocatalytic performance of Cr2O3/C@TiO2 could be attributed to its wide visible light photoresponse range and efficient separation of photogenerated electrons and holes.This paper offers some insights into the design of a novel efficient photocatalyst for water-splitting applications.
基金Supported by the Innovation Platform Open Foundation for Colleges and Universities of Hunan Province(No.16k011)
文摘The 1,5-disubstituted thiocarbohydrazide ligands were prepared by the condensation of thiocarbohydrazide with salicylaldehyde and 5-methylsalicylaldehyde, respectively. The butyltin complexes,[(5-R-2-hydroxy)ArCH=NNH]2 CS(n-BuSnCl)2, R = H(T1);R = Me(T2), based on the1,5-disubstituted thiocarbohydrazide were obtained by microwave-assisted solvothermal reaction of n-butyltintrichloride precursor with the ligands in methanol environments, which have been structurally characterized by elemental analysis, IR and(1 H, 13 C) NMR spectra. The crystals belong to monoclinic system, space groups C2/c(T1) and Pc(T2), respectively. The Sn atom is six-coordinated with distorted octahedral geometry by O, N and S atoms from ligand, C atom of butyl and two Cl atoms. In the crystal, complex T1 forms three-dimensional supramolecular assembly mediated by noncovalent interactions such as C–H···Cl and π-stacking interactions.Similarly, T2 forms an interesting two-dimensional supramolecular structure by noncovalent interactions(e.g. C–H×××Cl and N–H×××Cl) of one-dimensional band-like chain. These ligands and its butyltin complexes have growth effect on the target plants, such as Portulaca oleracea L.,Amaranthus spinosus L., Cassia tora L., Brassica campestris L. ssp. chinensis var. utilis Tsen et Lee and Amaranthus tricolor L. The ligand L1 has a good inhibitory effect on the growth of Cassia tora L., and complex T2 has selective inhibition on the growth of Portulaca oleracea L. and Amaranthus tricolor L., which can be used as a candidate compound for Cassia tora L., Portulaca oleracea L.and Amaranthus tricolor L. herbicide.
