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11.
《International Journal of Hydrogen Energy》2022,47(6):3550-3555
Electrocatalytic nitrogen reduction reaction (ENRR) offers a carbon-neutral process to fix nitrogen into ammonia, but its feasibility depends on the development of highly efficient electrocatalysts. Herein, we report that Fe ion grafted on MoO3 nanorods synthesized by an impregnation technique can efficiently enhance the electron harvesting ability and the selectivity of H+ during the NRR process in neutral electrolyte. In 0.1 M Na2SO4 solution, the electrocatalyst exhibited a remarkable NRR activity with an NH3 yield of 9.66 μg h?1 mg?1cat and a Faradaic efficiency (FE) of 13.1%, far outperforming the ungrafted MnO3. Density functional theory calculations revealed that the Fe sites are major activation centers along the alternating pathway. 相似文献
12.
寒区河道凌汛灾害河势“弯道效应”的量化评估十分重要。基于分形理论提出河道横断面-纵剖面-平面多维度河势分形维数计算方法及其物理机制,并探讨黄河内蒙古段不同维度河势演变分形特征及其与凌汛灾害的关联关系。结果表明,黄河内蒙古段不同维度河势均具有多尺度自相似分形特征,且具有多年记忆周期的长程相关性;冰坝(严重性冰塞)发生频次与河道主槽弯曲分形维数呈正相关指数型函数关系,与河相系数、深泓点高程和河段平均底坡分形维数负相关,与水深-面积分形维数正相关,总体表明冰坝灾害更易发生于主槽偏移摆动大、蜿蜒曲折、河湾发育程度高的宽浅型弯曲河道,研究成果可为凌汛期冰塞冰坝灾害易发河段诊断及预测提供重要理论依据。 相似文献
13.
用块状渣土置换软弱地基和回填低洼谷地等是处置工程渣土的有效途径。为了分析饱和块状混合回填土地基的固结性状,运用混合物理论建立了其一维固结模型。首先,假定块状土固相和充填土固相之间满足等应变条件,获得了饱和块状混合回填土中各相应变与块状土孔隙变形和充填土孔隙变形的关系式。其次,在小应变条件下,根据自由能势函数方程建立了饱和块状混合回填土的一维线弹性本构方程,再结合达西定律和应力平衡方程获得了一维固结控制方程。再次,利用分离变量法得到一维固结解析解,通过退化本文模型与已有模型进行对比,验证了本文模型的正确性。最后,基于所得解析解,分析了充填土孔隙渗透系数、块状土孔隙渗透系数以及流体交换参数等因素对饱和块状混合回填土地基固结性状的影响。分析结果表明:充填土孔隙渗透系数对饱和块状混合回填土地基整体固结性状起主导作用;在固结初期,块状土超孔压会有一定程度的上升,且3个参数具有相似的作用机理。 相似文献
14.
《International Journal of Hydrogen Energy》2022,47(99):41783-41794
To satisfy arising energy needs and to handle the forthcoming worldwide climate transformation, the major research attention has been drawn to environmentally friendly, renewable and abundant energy resources. Hydrogen plays an ideal and significant role is such resources, due to its non-carbon based energy and production through clean energy. In this work, we have explored catalytic activity of a newly predicted haeckelite boron nitride quantum dot (haeck-BNQD), constructed from the infinite BN sheet, for its utilization in hydrogen production. Density functional theory calculations are employed to investigate geometry optimization, electronic and adsorption mechanism of haeck-BNQD using Gaussian16 package, employing the hybrid B3LYP and wB97XD functionals, along with 6–31G(d,p) basis set. A number of physical quantities such as HOMO/LUMO energies, density of states, hydrogen atom adsorption energies, Mulliken populations, Gibbs free energy, work functions, overpotentials, etc., have been computed and analysed in the context of the catalytic performance of haeck-BNQD for the hydrogen-evolution reaction (HER). Based on our calculations, we predict that the best catalytic performance will be obtained for H adsorption on top of the squares or the octagons of haeck-BNQD. We hope that our prediction of most active catalytic sites on haeck-BNQD for HER will be put to test in future experiments. 相似文献
15.
《International Journal of Hydrogen Energy》2022,47(5):3022-3032
In the present work, the bonding length, electronic structure, stability, and dehydrogenation properties of the Perovskite-type ZrNiH3 hydride, under different uniaxial/biaxial strains are investigated through ab-initio calculations based on the plane-wave pseudo-potential (PW-PP) approach. The findings reveal that the uniaxial/biaxial compressive and tensile strains are responsible for the structural deformation of the ZrNiH3 crystal structure, and its lattice deformation becomes more significant with decreasing or increasing the strain magnitude. Due to the strain energy contribution, the uniaxial/biaxial strain not only lowers the stability of ZrNiH3 but also decreases considerably the dehydrogenation enthalpy and decomposition temperature. Precisely, the formation enthalpy and decomposition temperature are reduced from ?67.73 kJ/mol.H2 and 521 K for non-strained ZrNiH3 up to ?33.73 kJ/mol.H2 and 259.5 K under maximal biaxial compression strain of ε = ?6%, and to ?50.99 kJ/mol.H2 and 392.23 K for the maximal biaxial tensile strain of ε = +6%. The same phenomenon has been also observed for the uniaxial strain, where the formation enthalpy and decomposition temperature are both decreased to ?39.36 kJ/mol.H2 and 302.78 K for a maximal uniaxial compressive strain of ε = - 12%, and to ?51.86 kJ/mol.H2 and 399 K under the maximal uniaxial tensile strain of ε = +12%. Moreover, the densities of states analysis suggests that the strain-induced variation in the dehydrogenation and structural properties of ZrNiH3 are strongly related to the Fermi level value of total densities of states. These ab-initio calculations demonstrate insightful novel approach into the development of Zr-based intermetallic hydrides for hydrogen storage practical applications. 相似文献
16.
《Ceramics International》2022,48(22):32827-32836
To investigate the crystal structure, electrical properties, and magnetic properties of Ca–Sn co-doped Y3-xCaxFe5-xSnxO12 (x = 0.00–0.25 in steps of 0.05), solid-state reaction experiments, first principles calculations, and complex crystal bonding theoretical calculations were performed. The relative permittivity (εr) is strongly correlated with the average bond ionicity when Ca2+ is added. Furthermore, appropriate Sn4+ substitution significantly lowers the dielectric loss (tanδε) associated with the lattice energy. The right amount of Ca–Sn co-doping can change the saturation magnetization (4πMS) and improve the microscopic morphology of YIG, lowering the ferromagnetic resonance linewidth (ΔH) of YIG. The optimized microwave dielectric and magnetic properties are as follows: εr = 14.7, tanδε = 4.15 × 10?4, 4πMS = 1680 G, and ΔH = 53 Oe for Y2.8Ca0.2Fe4.8Sn0.2O12 sintered for 6 h at 1425 °C. Based on this material, a simple 3D model of a strip-line circulator with an insertion loss of less than 0.3 dB at each port and isolation greater than 20 dB in the 10–12 GHz range was developed, indicating the potential of the material for microwave high-frequency components such as circulators. 相似文献
17.
Crystallographic characteristics and microwave dielectric properties of Ni-modified MgTa2O6 ceramics
Liang Shi Xueying Wang Rui Peng Gang Wang Cheng Liu Xiaolei Shi Dainan Zhang Huaiwu Zhang 《Ceramics International》2021,47(16):22514-22521
Ni2+ modified MgTa2O6 ceramics with a trirutile phase and space group P42/mnm were obtained. The correlations between crystallographic characteristics and microwave dielectric performance of MgTa2O6 ceramics were systematically studied based on the chemistry bond theory (PVL theory) for the first time. The results indicate that the introduction of Ni2+ causes a change in polarizability and the Mg–O bond ionicity, which contributes to the variation of dielectric constant. Moreover, the lattice energy, and packing fraction, full width at half maximum of the Raman peak of Ta–O bond, as the quantitative characterization of crystallographic parameters, regulate the dielectric loss of MgTa2O6 ceramics in GHz frequency band. In addition, the study of sintering behavior shows that the densification and micromorphology are the crucial factors affecting the microwave dielectric performance. Typically, Ni2+ doping on the A-site of MgTa2O6 can effectively promote the Q × f values to 173,000 GHz (at 7.43 GHz), which ensures its applicability in 5G communication technology. 相似文献
18.
目的 在传统器物的创新设计中,最重要的环节是了解消费者对所使用产品的不同感受与意向并转换为具体的设计要素.研究消费者心理的感性因素与传统器物设计元素之间的联系,确定设计要素,从而对产品进行创新设计,为提升传统器物附加值作出贡献.方法 以中国传统器物茶宠为例,首先对8位相关的茶宠专家进行访谈,通过魅力工学中的评价构造法整理并提取魅力因子,设计出问卷调查表;然后以访谈内容为依据,使用问卷调查法得到大众对茶宠的魅力评价,共回收84份有效问卷;最后应用数量化一类分析茶宠魅力因子影响权重.结果 得到了数量化一类统计表,选取了其中影响因素较大的魅力因子作为茶宠设计前的风格定调考量.结论 通过茶宠的研究案例证明了该理论的可行性,为未来传统器物的设计提供了更多元且新颖的设计依据. 相似文献
19.
Jinming Wang Meng Yang Guodong Zou Di Liu Qiuming Peng 《Advanced functional materials》2021,31(21):2101180
Lithium (Li) metal, as an appealing candidate for the next-generation of high-energy-density batteries, is plagued by its safety issue mainly caused by uncontrolled dendrite growth and infinite volume expansion. Developing new materials that can improve the performance of Li-metal anode is one of the urgent tasks. Herein, a new MXene derivative containing pure rutile TiO2 and N-doped carbon prepared by heat-treating MXene under a mixing gas, exhibiting high chemical activity in molten Li, is reported. The lithiation MXene derivative with a hybrid of LiTiO2-Li3N-C and Li offers outstanding electrochemical properties. The symmetrical cell assembling lithiation MXene derivative hybrid anode exhibits an ultra-long cycle lifespan of 2000 h with an overpotential of ≈30 mV at 1 mA cm−2, which overwhelms Li-based anodes reported so far. Additionally, long-term operations of 34, 350, and 500 h at 10 mA cm−2 can be achieved in symmetrical cells at temperatures of −10, 25, and 50 °C, respectively. Both experimental tests and density functional theory calculations confirm that the LiTiO2-Li3N-C skeleton serves as a promising host for Li infusion by alleviating volume variation. Simultaneously, the superlithiophilic interphase of Li3N guides Li deposition along the LiTiO2-Li3N-C skeleton to avoid dendrite growth. 相似文献
20.
Yunqi Li Jing Li Yang-Gang Wang Xiran Chen Mingtao Liu Zhong Zheng Xihong Peng 《International Journal of Hydrogen Energy》2021,46(24):13273-13282
In this work, density functional theory (DFT) calculations were used to investigate the mechanism of carbon corrosion on nitrogen-doped carbon support. Free energy diagrams were generated based on three proposed reaction pathways to evaluate corrosion mechanisms. The most energetically preferred mechanism on nitrogen-doped carbon was determined. The results show that the step of water dissociation to form #OH was the rate-determining step for gra-G-1N (graphene doped with graphitic N) and pyrr-G-1N (graphene doped with pyrrolic N). As for graphene doped with pyridinic N, the step of C#OC#O formation was critical. It was found that the control of nitrogen concentration was necessary for precisely designing optimized carbon materials. Abundance of nitrogen moieties aggravated the carbon corrosion. When the high potential was applied, specific types of graphitic N and pyridinic N were found to be favorable carbon modifications to improve carbon corrosion resistance. Moreover, the solvent effect was also investigated. The results provide theoretical insights and design guidelines to improve corrosion resistance in carbon support through material modification by inhibiting the adsorption of surface oxides (OH, O, and OOH). 相似文献