Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.展开更多
Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation o...Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation of charges,resulting in poor photocatalytic activity.In the present study,we successfully synthesize SrTaO_(2)N photocatalyst with low density of defect states,uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping.Some important parameters,such as the size of unit cell,the content of nitrogen,and microstructure,prove the successful doping of Mg.The defect-related carrier recombination has been significantly reduced by Mg doping,which effectively promotes the charge separation.Moreover,Mg doping induces a change of the band edge,which makes proton reduction have a stronger driving force.After modifying with the core/shell-structured Pt/Cr_(2)O_(3)cocatalyst,the H_(2)evolution activity of the optimized SrTaO_(2)N:Mg is 10 times that of the undoped SrTaO_(2)N,with an impressive apparent quantum yield of 1.51%at 420 nm.By coupling with Au-FeCoO_(x)modified BiVO_(4)as an O_(2)-evolution photocatalyst and[Fe(CN)_(6)]_(3)−/[Fe(CN)_(6)]_(4)−as the redox couple,a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36%at 420 nm.This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.展开更多
TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microsc...TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray electron spectroscopy,and fluorescence spectroscopy.At room temperature,with a relative humidity of 50.0%,the total gas flow rate of 1.0 L·min-1,the space velocity of 1.05×10^(4) h^(-1),and toluene volume concentration of 25.0µL·L^(-1),two 6 W vacuum ultraviolet lamps were used as light sources to catalyze,degrade,and mineralize toluene.The results show that the prepared catalyst is in the shape of nano-ribbons.The loading of Co_(3)O_(4) inhibits the recombina-tion of photogenerated electrons and holes and can effectively improve the catalytic performance.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%Co_(3)O_(4) has the best catalytic effect.When N2 was used as a carrier gas,the degradation rate of tol-uene was only 34.7%.The toluene degradation is mainly due to the photolysis of vacuum ultraviolet light.When air was used as a carrier gas,O_(3) was produced.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%and vacuum ultraviolet synergistical-ly promote toluene degradation.The highest degradation rate of toluene was 91.7%and the mineralization rate was 74.6%.The degradation rate of toluene was 2.6 times that of nitrogen as a carrier gas.展开更多
Based on the Hirota bilinear method,this study derived N-soliton solutions,breather solutions,lump solutions and interaction solutions for the(2+1)-dimensional extended Boiti-Leon-Manna-Pempinelli equation.The dynamic...Based on the Hirota bilinear method,this study derived N-soliton solutions,breather solutions,lump solutions and interaction solutions for the(2+1)-dimensional extended Boiti-Leon-Manna-Pempinelli equation.The dynamical characteristics of these solutions were displayed through graphical,particularly revealing fusion and ssion phenomena in the interaction of lump and the one-stripe soliton.展开更多
MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-d...MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-duction performance of MoS_(2)/CuS prepared with different molar ratios of Mo to Cu precursors(n_(Mo)∶n_(Cu))as cathodic catalysts was investigated in the two-chamber microbial electrolytic cell(MEC).X-ray diffraction(XRD),X-ray pho-toelectron spectroscopy(XPS),scanning electron microscopy(SEM),transmission electron microscope(TEM),linear scanning voltammetry(LSV),electrochemical impedance analysis(EIS),and cyclic voltammetry(CV)were used to characterize the synthesized catalysts for testing and analyzing the hydrogen-producing performance.The results showed that the hydrogen evolution performance of MoS_(2)/CuS-20%(nMo∶nCu=5∶1)was better than that of platinum(Pt)mesh,and the hydrogen production rate of MoS_(2)/CuS-20%as a cathode in MEC was(0.2031±0.0237)m^(3)_(H_(2))·m^(-3)·d^(-1) for 72 h at an applied voltage of 0.8 V,which was slightly higher than that of Pt mesh of(0.1886±0.0134)m^(3)_(H_(2))·m^(-3)·d^(-1).The addition of a certain amount of CuS not only regulates the electron transfer ability of MoS_(2) but also increases the density of active sites.展开更多
目的观察黄连解毒汤联合低热量饮食对新诊断肥胖2型糖尿病患者血糖及胰岛素分泌影响。方法选取医院2021年1月—10月新诊断肥胖2型糖尿病患者196例为研究对象,依据随机数字表法均分为对照组和观察组各98例,对照组采用利拉鲁肽皮下注射用...目的观察黄连解毒汤联合低热量饮食对新诊断肥胖2型糖尿病患者血糖及胰岛素分泌影响。方法选取医院2021年1月—10月新诊断肥胖2型糖尿病患者196例为研究对象,依据随机数字表法均分为对照组和观察组各98例,对照组采用利拉鲁肽皮下注射用药联合低热量饮食干预,观察组在对照组的基础上增加黄连解毒汤治疗。比较两组患者的肥胖指标,血糖水平,胰岛素分泌功能,不良反应发生情况。结果治疗前两组患者的一般资料、肥胖指标,血糖水平、胰岛素分泌情况差异均无统计学意义(P>0.05),具有临床可比性。治疗后两组体质量、体质指数、体脂率显著下降,观察组降低更为明显,与对照组比较组间差异有统计学意义(P<0.05)。治疗后两组患者的空腹血糖(fasting plasma glucose,FPG)、餐后2 h血糖(2 hours postprandial blood glucose,2 h PG)、糖化血红蛋白(glycosylated hemoglobin,HbAlc)均显著降低,且观察组FPG及2 h PG显著低于对照组(P<0.05),但两组HbAlc水平差异无统计学意义(P>0.05)。治疗后两组空腹胰岛素(fasting insulin,FINS)、胰岛素抵抗指数(homeostasis model assessment insulinresistance,HOMA-IR)降低,胰岛素分泌指数(homeostasis model assessmentβ,HOMA-β)升高,观察组变化更为明显,与对照组比较组间差异有统计学意义(P<0.05)。观察组、对照组的不良反应发生率分别为9.2%(9/98)、6.1%(6/98),组间差异无统计学意义(P>0.05),不良反应均较轻微、可自行缓解。结论黄连解毒汤联合低热量饮食治疗新诊断肥胖2型糖尿病患者具有肯定的临床效果,能够改善患者的肥胖情况、有效控制血糖水平、改善胰岛素分泌功能,可以作为安全有效的治疗方案。展开更多
The photochemical reaction process of anthraquinone-2-sodium sulfonate (AQS) in the mixture of water (H2O) and N-butylpyridinium tetrafluoroborate ([BPy] [BF4]) was studied using the laser flash photolysis techn...The photochemical reaction process of anthraquinone-2-sodium sulfonate (AQS) in the mixture of water (H2O) and N-butylpyridinium tetrafluoroborate ([BPy] [BF4]) was studied using the laser flash photolysis technique. Experimental results show that the excited triplet of AQS (3AQS*) could react rapidly with H2O and the transient absorption spectra greatly changed by increasing the volume fraction of the ionic liquid (VIL) in [BPy][BF4]/H2O mixtures. The absorbance at 510 nm increased gradually with increasing VIL when 0〈VIL〈0.1. By contrast, the absorbance decreased gradually when VIL〉0.1. Otherwise, the absorbance of the band near 380 nm steadily increased. The apparent kinetic parameters of transient species B and ^3AQS* are obtained approximately. 3AQS* abstracting hydrogen from [BPy]+ was also explored. It was deduced that the 350-420 nm band was the superposition of the peaks of 3AQS* and AQSH'. The two reactions of 3AQS* with [BPy][BF4] and H2O are a pair of competitive reactions. We also concluded that the entire reaction processes slow down in the case of high [BPy] [BF4] concentrations.展开更多
Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide elect...Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide electrolysis cell(SOEC).Herein,highly dispersed nickel species with low loading(1.0 wt%)were trapped within the La_(0.8)Sr_(0.2)FeO_(3)–δ‐Ce_(0.8)Sm_(0.2)O_(2)–δvia a facial mechanical milling ap‐proach,which demonstrated excellent CO_(2) electrolysis performance.The highly dispersed nickel species can significantly alter the electronic structures of the LSF‐SDC without affecting its porous network and facilitate oxygen vacancy formation,thus greatly promote the CO_(2) electrolysis perfor‐mance.The highest current density of 1.53 A·cm^(-2) could be achieved when operated under 800℃ at 1.6 V,which is about 91%higher than the LSF‐SDC counterpart.展开更多
In this paper, we prove the existence in H+^2, an incomplete metric subspace of H^2×H^2×H^2, of global solutions to the system for a one-dimensional non-monotone fluid in bounded domainΩ=(0,1). The resul...In this paper, we prove the existence in H+^2, an incomplete metric subspace of H^2×H^2×H^2, of global solutions to the system for a one-dimensional non-monotone fluid in bounded domainΩ=(0,1). The results in this paper have improved those previously related results.展开更多
In this work,we explore the suitability of several density functionals with the generalized gradient approximation(GGA)and beyond for describing the dissociative chemisorption of methane on the reconstructed Pt(110)-(...In this work,we explore the suitability of several density functionals with the generalized gradient approximation(GGA)and beyond for describing the dissociative chemisorption of methane on the reconstructed Pt(110)-(2×1)surface.The bulk and surface structures of the metal,methane adsorption energy,and dissociation barrier are used to assess the functionals.A van der Waals corrected GGA functional(optPBE-vdW)and a metaGGA functional with van der Waals correction(MS PBEl-rVV10)are selected for ab initio molecular dynamics calculations of the sticking probability.Our results suggest that the use of these two functionals may lead to a better agreement with existing experimental results,thus serving as a good starting point for future development of reliable machine-learned potential energy surfaces for the dissociation of methane on the Pt(110)-(2×1)surface.展开更多
Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and storage.However,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge...Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and storage.However,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers,resulting in slow reaction kinetics and limited CO_(2)conversion.Here,we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS process.The novel material achieved an unprecedented CO production rate of 381 mL g^(-1)min^(-1)with 99%CO_(2)conversion at 850℃,outperforming state-of-the-art materials.In situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO_(2)splitting.Preferential oxidation of the FeNi alloy at the interface(as opposed to forming an FeO_(x)passivation shell encapsulating bare metallic iron)and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO_(2)to CO.Facile regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas(H_(2)/CO=2,syngas yield>96%).Overall,the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production,with a theoretical solar-to-fuel efficiency of up to 58%,in the absence of any heat integration.展开更多
Loading of cocatalysts can effectively inhibit the recombination of photogenerated carriers in photocatalysts and greatly improve the photocatalytic hydrogen production rate. Cocatalysts can be deposited at the outlet...Loading of cocatalysts can effectively inhibit the recombination of photogenerated carriers in photocatalysts and greatly improve the photocatalytic hydrogen production rate. Cocatalysts can be deposited at the outlet points of electrons using a photochemical method, which is beneficial for the following photocatalytic hydrogen production reaction. H2PO2^– has been used in the photochemical reduction of transition metals because of its special properties. However, the particles formed in the presence of H2PO2^– are very large and highly crystalline, which may inhibit the activity of photocatalysts. In this study, we designed a new method for synthesizing photocatalysts by photodeposition using some other phosphates, aiming to prepare controllable weakly crystalline and small-size cocatalysts to improve the hydrogen production activity. The cocatalyst prepared using H2PO3^– as an inorganic sacrificial agent has an amorphous structure and an average size of about 10 nm. The optimal photocatalytic hydrogen production rate of the obtained Ni(OH)2/g-C3N4(4.36 wt%) is 13707.86 μmol·g^-1·h^-1, which is even higher than the activity of Pt-4.36 wt%/g-C3N4(11210.93 μmol·g^-1·h^-1). Mechanistic studies show that loading of Ni(OH)2 can efficiently accelerate the separation and transfer efficiency of photogenerated charge carriers.展开更多
The lg c-pH diagram of the CaCl2-Ca(OH)2-H2O system and its two subsystems at 298.15 K are constructed according to the theory of thermodynamic equilibrium. The interaction characteristics between the solubility of ...The lg c-pH diagram of the CaCl2-Ca(OH)2-H2O system and its two subsystems at 298.15 K are constructed according to the theory of thermodynamic equilibrium. The interaction characteristics between the solubility of CaCl2 and Ca(OH)e can be found out from the diagrams. CaCl26H2O (s), Ca(OH)2(s) and solution coexist when the pH value of solution is about 10.8. CaC12 with the minimum solubility of 1 682.4 g/L is in equilibrium with solution when the pH value is lower than 9.4, and Ca(OH)2 with the minimum solubility of 2.749 g/L is in equilibrium with solution at the pH value over 12.1, which provides a theoretical basis for the treatment and reuse of calcium chloride mother liquor for collocating lime cream which is the precipitant in the process of synthesizing magnesium hydroxide.展开更多
H_(2)S is one of the most important characteristic decomposition components of SF_(6)insulated gas,and the detection of trace H_(2)S is significant for early fault diagnosis of gas insulated electrical equipment.A 157...H_(2)S is one of the most important characteristic decomposition components of SF_(6)insulated gas,and the detection of trace H_(2)S is significant for early fault diagnosis of gas insulated electrical equipment.A 1578 nm wavelength distributed feedback diode laser(DFB-DL)based cavity ring-down spectroscopy(CRDS)experimental platform is developed to monitor the concentrations of H_(2)S in SF_(6)and SF_(6)/N_(2)mixture carrier gas.The detection sensitivity is higher than 1×10^(-6).The absorption cross section parameterσis vital for calculating the concentration.With repeated experiments using standard gas samples,parameterσof H_(2)S in pure SF_(6)and SF_(6)/N_(2)mixture carrier with different mixing ratios is calibrated.Compared with the simulatedσvalues,the influence of carrier gas on the broadening of spectral profile is discussed.The variation of absorption cross sectionσwith different carrier gas mixing ratios is studied as well,so that the calculation of the concentration in the carrier gas of any mixing ratio is possible.Thus,the application of CRDS in trace component detection of gas insulated electrical equipment is promising.展开更多
The photodissociation dynamics of 2-bromobutane has been investigated at 264.77 and 264.86 nm by ion-velocity map imaging technique coupled with resonance-enhanced multi- photon ionization. The speed and angular distr...The photodissociation dynamics of 2-bromobutane has been investigated at 264.77 and 264.86 nm by ion-velocity map imaging technique coupled with resonance-enhanced multi- photon ionization. The speed and angular distributions have been derived from the velocity map images of Br and Br^*. The speed distributions of Br and Br^* atoms in the photodis- sociation of 2-bromobutane at -265 nm can be fitted using only one Gaussian function indicating that bromine fragments were produced via direct dissociation of C-Br bond. The contributions of the excited 3^Q0, 3Q1, and 1^Q1 states to the products (Br and Br^*) were discussed. It is found that the nonadiabatic 1^Q1←3^Q0 transition plays an important role for Br photofragment in the dissociation of 2-C4HgBr at -265 nm. Relative quantum yield of 0.621 for Br(2P3/2) at -265 nm in the photodissociation of 2-bromobutane is derived. By comparing the photodissociation of 2-C4H9Br at -265 nm and that that at-234 nm, the anisotropy parameter β(Br) and β(Br^*), and relative quantum yield Ф(Br) decrease with increasing wavelength, the probability of curve crossing between 3 ^Q0 and 1^Q1 decreases with increasing laser wavelength.展开更多
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.
文摘Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation of charges,resulting in poor photocatalytic activity.In the present study,we successfully synthesize SrTaO_(2)N photocatalyst with low density of defect states,uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping.Some important parameters,such as the size of unit cell,the content of nitrogen,and microstructure,prove the successful doping of Mg.The defect-related carrier recombination has been significantly reduced by Mg doping,which effectively promotes the charge separation.Moreover,Mg doping induces a change of the band edge,which makes proton reduction have a stronger driving force.After modifying with the core/shell-structured Pt/Cr_(2)O_(3)cocatalyst,the H_(2)evolution activity of the optimized SrTaO_(2)N:Mg is 10 times that of the undoped SrTaO_(2)N,with an impressive apparent quantum yield of 1.51%at 420 nm.By coupling with Au-FeCoO_(x)modified BiVO_(4)as an O_(2)-evolution photocatalyst and[Fe(CN)_(6)]_(3)−/[Fe(CN)_(6)]_(4)−as the redox couple,a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36%at 420 nm.This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy.
文摘TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray electron spectroscopy,and fluorescence spectroscopy.At room temperature,with a relative humidity of 50.0%,the total gas flow rate of 1.0 L·min-1,the space velocity of 1.05×10^(4) h^(-1),and toluene volume concentration of 25.0µL·L^(-1),two 6 W vacuum ultraviolet lamps were used as light sources to catalyze,degrade,and mineralize toluene.The results show that the prepared catalyst is in the shape of nano-ribbons.The loading of Co_(3)O_(4) inhibits the recombina-tion of photogenerated electrons and holes and can effectively improve the catalytic performance.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%Co_(3)O_(4) has the best catalytic effect.When N2 was used as a carrier gas,the degradation rate of tol-uene was only 34.7%.The toluene degradation is mainly due to the photolysis of vacuum ultraviolet light.When air was used as a carrier gas,O_(3) was produced.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%and vacuum ultraviolet synergistical-ly promote toluene degradation.The highest degradation rate of toluene was 91.7%and the mineralization rate was 74.6%.The degradation rate of toluene was 2.6 times that of nitrogen as a carrier gas.
基金Supported by the National Natural Science Foundation of China(12275172)。
文摘Based on the Hirota bilinear method,this study derived N-soliton solutions,breather solutions,lump solutions and interaction solutions for the(2+1)-dimensional extended Boiti-Leon-Manna-Pempinelli equation.The dynamical characteristics of these solutions were displayed through graphical,particularly revealing fusion and ssion phenomena in the interaction of lump and the one-stripe soliton.
文摘MoS_(2)/CuS composite catalysts were successfully synthesized using a one-step hydrothermal method with sodium molybdate dihydrate,thiourea,oxalic acid,and copper nitrate trihydrate as raw materials.The hydrogen pro-duction performance of MoS_(2)/CuS prepared with different molar ratios of Mo to Cu precursors(n_(Mo)∶n_(Cu))as cathodic catalysts was investigated in the two-chamber microbial electrolytic cell(MEC).X-ray diffraction(XRD),X-ray pho-toelectron spectroscopy(XPS),scanning electron microscopy(SEM),transmission electron microscope(TEM),linear scanning voltammetry(LSV),electrochemical impedance analysis(EIS),and cyclic voltammetry(CV)were used to characterize the synthesized catalysts for testing and analyzing the hydrogen-producing performance.The results showed that the hydrogen evolution performance of MoS_(2)/CuS-20%(nMo∶nCu=5∶1)was better than that of platinum(Pt)mesh,and the hydrogen production rate of MoS_(2)/CuS-20%as a cathode in MEC was(0.2031±0.0237)m^(3)_(H_(2))·m^(-3)·d^(-1) for 72 h at an applied voltage of 0.8 V,which was slightly higher than that of Pt mesh of(0.1886±0.0134)m^(3)_(H_(2))·m^(-3)·d^(-1).The addition of a certain amount of CuS not only regulates the electron transfer ability of MoS_(2) but also increases the density of active sites.
文摘目的观察黄连解毒汤联合低热量饮食对新诊断肥胖2型糖尿病患者血糖及胰岛素分泌影响。方法选取医院2021年1月—10月新诊断肥胖2型糖尿病患者196例为研究对象,依据随机数字表法均分为对照组和观察组各98例,对照组采用利拉鲁肽皮下注射用药联合低热量饮食干预,观察组在对照组的基础上增加黄连解毒汤治疗。比较两组患者的肥胖指标,血糖水平,胰岛素分泌功能,不良反应发生情况。结果治疗前两组患者的一般资料、肥胖指标,血糖水平、胰岛素分泌情况差异均无统计学意义(P>0.05),具有临床可比性。治疗后两组体质量、体质指数、体脂率显著下降,观察组降低更为明显,与对照组比较组间差异有统计学意义(P<0.05)。治疗后两组患者的空腹血糖(fasting plasma glucose,FPG)、餐后2 h血糖(2 hours postprandial blood glucose,2 h PG)、糖化血红蛋白(glycosylated hemoglobin,HbAlc)均显著降低,且观察组FPG及2 h PG显著低于对照组(P<0.05),但两组HbAlc水平差异无统计学意义(P>0.05)。治疗后两组空腹胰岛素(fasting insulin,FINS)、胰岛素抵抗指数(homeostasis model assessment insulinresistance,HOMA-IR)降低,胰岛素分泌指数(homeostasis model assessmentβ,HOMA-β)升高,观察组变化更为明显,与对照组比较组间差异有统计学意义(P<0.05)。观察组、对照组的不良反应发生率分别为9.2%(9/98)、6.1%(6/98),组间差异无统计学意义(P>0.05),不良反应均较轻微、可自行缓解。结论黄连解毒汤联合低热量饮食治疗新诊断肥胖2型糖尿病患者具有肯定的临床效果,能够改善患者的肥胖情况、有效控制血糖水平、改善胰岛素分泌功能,可以作为安全有效的治疗方案。
基金This work was supported by the National Natural Science Foundation of China (No.21173002) and the Anhui Provincial Natural Science Foundation, China (No.1308085MB20).
文摘The photochemical reaction process of anthraquinone-2-sodium sulfonate (AQS) in the mixture of water (H2O) and N-butylpyridinium tetrafluoroborate ([BPy] [BF4]) was studied using the laser flash photolysis technique. Experimental results show that the excited triplet of AQS (3AQS*) could react rapidly with H2O and the transient absorption spectra greatly changed by increasing the volume fraction of the ionic liquid (VIL) in [BPy][BF4]/H2O mixtures. The absorbance at 510 nm increased gradually with increasing VIL when 0〈VIL〈0.1. By contrast, the absorbance decreased gradually when VIL〉0.1. Otherwise, the absorbance of the band near 380 nm steadily increased. The apparent kinetic parameters of transient species B and ^3AQS* are obtained approximately. 3AQS* abstracting hydrogen from [BPy]+ was also explored. It was deduced that the 350-420 nm band was the superposition of the peaks of 3AQS* and AQSH'. The two reactions of 3AQS* with [BPy][BF4] and H2O are a pair of competitive reactions. We also concluded that the entire reaction processes slow down in the case of high [BPy] [BF4] concentrations.
文摘Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide electrolysis cell(SOEC).Herein,highly dispersed nickel species with low loading(1.0 wt%)were trapped within the La_(0.8)Sr_(0.2)FeO_(3)–δ‐Ce_(0.8)Sm_(0.2)O_(2)–δvia a facial mechanical milling ap‐proach,which demonstrated excellent CO_(2) electrolysis performance.The highly dispersed nickel species can significantly alter the electronic structures of the LSF‐SDC without affecting its porous network and facilitate oxygen vacancy formation,thus greatly promote the CO_(2) electrolysis perfor‐mance.The highest current density of 1.53 A·cm^(-2) could be achieved when operated under 800℃ at 1.6 V,which is about 91%higher than the LSF‐SDC counterpart.
文摘In this paper, we prove the existence in H+^2, an incomplete metric subspace of H^2×H^2×H^2, of global solutions to the system for a one-dimensional non-monotone fluid in bounded domainΩ=(0,1). The results in this paper have improved those previously related results.
基金financial support from the National Natural Science Foundation of China(No.21973013 and No.21673040)the National Natural Science Foundation of Fujian Province,China(No.2020J02025)+3 种基金the“Chuying Program”for the Top Young Talents of Fujian Provincesupported financially through a NWO/CW TOP grant(No.715.017.001)by a grant of supercomputer time from NWO Exacte en Natuurwetenschappen(NWO-ENW,No.2019.015)the National Science Foundation(No.CHE1951328)。
文摘In this work,we explore the suitability of several density functionals with the generalized gradient approximation(GGA)and beyond for describing the dissociative chemisorption of methane on the reconstructed Pt(110)-(2×1)surface.The bulk and surface structures of the metal,methane adsorption energy,and dissociation barrier are used to assess the functionals.A van der Waals corrected GGA functional(optPBE-vdW)and a metaGGA functional with van der Waals correction(MS PBEl-rVV10)are selected for ab initio molecular dynamics calculations of the sticking probability.Our results suggest that the use of these two functionals may lead to a better agreement with existing experimental results,thus serving as a good starting point for future development of reliable machine-learned potential energy surfaces for the dissociation of methane on the Pt(110)-(2×1)surface.
文摘Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and storage.However,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers,resulting in slow reaction kinetics and limited CO_(2)conversion.Here,we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS process.The novel material achieved an unprecedented CO production rate of 381 mL g^(-1)min^(-1)with 99%CO_(2)conversion at 850℃,outperforming state-of-the-art materials.In situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO_(2)splitting.Preferential oxidation of the FeNi alloy at the interface(as opposed to forming an FeO_(x)passivation shell encapsulating bare metallic iron)and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO_(2)to CO.Facile regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas(H_(2)/CO=2,syngas yield>96%).Overall,the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production,with a theoretical solar-to-fuel efficiency of up to 58%,in the absence of any heat integration.
文摘Loading of cocatalysts can effectively inhibit the recombination of photogenerated carriers in photocatalysts and greatly improve the photocatalytic hydrogen production rate. Cocatalysts can be deposited at the outlet points of electrons using a photochemical method, which is beneficial for the following photocatalytic hydrogen production reaction. H2PO2^– has been used in the photochemical reduction of transition metals because of its special properties. However, the particles formed in the presence of H2PO2^– are very large and highly crystalline, which may inhibit the activity of photocatalysts. In this study, we designed a new method for synthesizing photocatalysts by photodeposition using some other phosphates, aiming to prepare controllable weakly crystalline and small-size cocatalysts to improve the hydrogen production activity. The cocatalyst prepared using H2PO3^– as an inorganic sacrificial agent has an amorphous structure and an average size of about 10 nm. The optimal photocatalytic hydrogen production rate of the obtained Ni(OH)2/g-C3N4(4.36 wt%) is 13707.86 μmol·g^-1·h^-1, which is even higher than the activity of Pt-4.36 wt%/g-C3N4(11210.93 μmol·g^-1·h^-1). Mechanistic studies show that loading of Ni(OH)2 can efficiently accelerate the separation and transfer efficiency of photogenerated charge carriers.
基金Project(2008BAB35B04) supported by National High Technology Research and Development Program of ChinaProject(2010QZZD003) supported by Advanced Research Program of Central South University,China
文摘The lg c-pH diagram of the CaCl2-Ca(OH)2-H2O system and its two subsystems at 298.15 K are constructed according to the theory of thermodynamic equilibrium. The interaction characteristics between the solubility of CaCl2 and Ca(OH)e can be found out from the diagrams. CaCl26H2O (s), Ca(OH)2(s) and solution coexist when the pH value of solution is about 10.8. CaC12 with the minimum solubility of 1 682.4 g/L is in equilibrium with solution when the pH value is lower than 9.4, and Ca(OH)2 with the minimum solubility of 2.749 g/L is in equilibrium with solution at the pH value over 12.1, which provides a theoretical basis for the treatment and reuse of calcium chloride mother liquor for collocating lime cream which is the precipitant in the process of synthesizing magnesium hydroxide.
基金supported in part by the National Key R&D Program of China(No.2021YFF0603100)in part by the Leading Innovation and Entrepreneurship Team in Zhejiang Province(No.2019R01014)
文摘H_(2)S is one of the most important characteristic decomposition components of SF_(6)insulated gas,and the detection of trace H_(2)S is significant for early fault diagnosis of gas insulated electrical equipment.A 1578 nm wavelength distributed feedback diode laser(DFB-DL)based cavity ring-down spectroscopy(CRDS)experimental platform is developed to monitor the concentrations of H_(2)S in SF_(6)and SF_(6)/N_(2)mixture carrier gas.The detection sensitivity is higher than 1×10^(-6).The absorption cross section parameterσis vital for calculating the concentration.With repeated experiments using standard gas samples,parameterσof H_(2)S in pure SF_(6)and SF_(6)/N_(2)mixture carrier with different mixing ratios is calibrated.Compared with the simulatedσvalues,the influence of carrier gas on the broadening of spectral profile is discussed.The variation of absorption cross sectionσwith different carrier gas mixing ratios is studied as well,so that the calculation of the concentration in the carrier gas of any mixing ratio is possible.Thus,the application of CRDS in trace component detection of gas insulated electrical equipment is promising.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (No.21073177 and No.20873133), the Ministry of Science and Technology of China (No.2007CB815203 and No.2010CB923302), the Chinese Academy of Sciences (No.KJCX2-YW- N24 and No.KJCX2-EW-W09), the Fundamental Research Funds for the Central Universities of China (No.WK2340000012), and the USTC-NSRL Joint Funds (No.KY2340000021).
文摘The photodissociation dynamics of 2-bromobutane has been investigated at 264.77 and 264.86 nm by ion-velocity map imaging technique coupled with resonance-enhanced multi- photon ionization. The speed and angular distributions have been derived from the velocity map images of Br and Br^*. The speed distributions of Br and Br^* atoms in the photodis- sociation of 2-bromobutane at -265 nm can be fitted using only one Gaussian function indicating that bromine fragments were produced via direct dissociation of C-Br bond. The contributions of the excited 3^Q0, 3Q1, and 1^Q1 states to the products (Br and Br^*) were discussed. It is found that the nonadiabatic 1^Q1←3^Q0 transition plays an important role for Br photofragment in the dissociation of 2-C4HgBr at -265 nm. Relative quantum yield of 0.621 for Br(2P3/2) at -265 nm in the photodissociation of 2-bromobutane is derived. By comparing the photodissociation of 2-C4H9Br at -265 nm and that that at-234 nm, the anisotropy parameter β(Br) and β(Br^*), and relative quantum yield Ф(Br) decrease with increasing wavelength, the probability of curve crossing between 3 ^Q0 and 1^Q1 decreases with increasing laser wavelength.