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1.
《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
2.
《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
3.
本文主要总结了新冠疫情期间作者的电磁场理论课程在线教学经验。对比分析了录播和直播的优缺点后,选择录播教学方式。基于超星网络教学平台,展示了录播网络教学的具体措施,包括网上答疑和学习效果检查以及在线批改作业等。给出了网络教学可以为线下教学继续使用的方法和手段,为疫情结束后的正常教学提供了新的网络教学补充措施。 相似文献
4.
《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
5.
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
6.
Tongling Xia Yue Qi Xilei Dai Jinyu Liu Can Xiao Ruoyu You Dayi Lai Junjie Liu Chun Chen 《Indoor air》2021,31(6):2020-2032
To evaluate the separate impacts on human health and establish effective control strategies, it is crucial to estimate the contribution of outdoor infiltration and indoor emission to indoor PM2.5 in buildings. This study used an algorithm to automatically estimate the long-term time-resolved indoor PM2.5 of outdoor and indoor origin in real apartments with natural ventilation. The inputs for the algorithm were only the time-resolved indoor/outdoor PM2.5 concentrations and occupants’ window actions, which were easily obtained from the low-cost sensors. This study first applied the algorithm in an apartment in Tianjin, China. The indoor/outdoor contribution to the gross indoor exposure and time-resolved infiltration factor were automatically estimated using the algorithm. The influence of outdoor PM2.5 data source and algorithm parameters on the estimated results was analyzed. The algorithm was then applied in four other apartments located in Chongqing, Shenyang, Xi'an, and Urumqi to further demonstrate its feasibility. The results provided indirect evidence, such as the plausible explanations for seasonal and spatial variation, to partially support the success of the algorithm used in real apartments. Through the analysis, this study also identified several further development directions to facilitate the practical applications of the algorithm, such as robust long-term outdoor PM2.5 monitoring using low-cost light-scattering sensors. 相似文献
7.
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
8.
Makoto Yamaguchi 《应用聚合物科学杂志》2021,138(14):50172
Perfluorosulfonic acid ionomer membranes have been widely used as proton conducting membranes in various electrochemical processes such as polymer electrolyte fuel cells and water electrolysis. While their thermal stability has been studied by thermogravimetry and analysis of low molecular weight products, their decomposition mechanism is little understood. In this study a newly developed methodology of thermal desorption and pyrolysis in combination with direct analysis in real time mass spectrometry is applied for Nafion membrane. An ambient ionization source and a high-resolution time-of-flight mass spectrometer enabled unambiguous assignment of gaseous products. Thermal decomposition is initiated by side chain detachment above 350°C, which leaves carbonyls on the main chain at the locations of the side chains. Perfluoroalkanes are released above 400°C by main chain scission and their further decomposition products dominate above 500 °C. DFT calculation of reaction energies and barrier heights of model compounds support proposed decomposition reactions. 相似文献
9.
Krzysztof M. Tokarz Wojciech Wesoowski Barbara Tokarz Wojciech Makowski Anna Wysocka Roman J. Jdrzejczyk Karolina Chrabaszcz Kamilla Malek Anna Kostecka-Gugaa 《International journal of molecular sciences》2021,22(2)
Grass pea (Lathyrus sativus) is a leguminous plant of outstanding tolerance to abiotic stress. The aim of the presented study was to describe the mechanism of grass pea (Lathyrus sativus L.) photosynthetic apparatus acclimatisation strategies to salinity stress. The seedlings were cultivated in a hydroponic system in media containing various concentrations of NaCl (0, 50, and 100 mM), imitating none, moderate, and severe salinity, respectively, for three weeks. In order to characterise the function and structure of the photosynthetic apparatus, Chl a fluorescence, gas exchange measurements, proteome analysis, and Fourier-transform infrared spectroscopy (FT-IR) analysis were done inter alia. Significant differences in the response of the leaf and stem photosynthetic apparatus to severe salt stress were observed. Leaves became the place of harmful ion (Na+) accumulation, and the efficiency of their carboxylation decreased sharply. In turn, in stems, the reconstruction of the photosynthetic apparatus (antenna and photosystem complexes) activated alternative electron transport pathways, leading to effective ATP synthesis, which is required for the efficient translocation of Na+ to leaves. These changes enabled efficient stem carboxylation and made them the main source of assimilates. The observed changes indicate the high plasticity of grass pea photosynthetic apparatus, providing an effective mechanism of tolerance to salinity stress. 相似文献
10.
《岩石力学与岩土工程学报(英文版)》2022,14(5):1421-1432
Prediction of mode I fracture toughness (KIC) of rock is of significant importance in rock engineering analyses. In this study, linear multiple regression (LMR) and gene expression programming (GEP) methods were used to provide a reliable relationship to determine mode I fracture toughness of rock. The presented model was developed based on 60 datasets taken from the previous literature. To predict fracture parameters, three mechanical parameters of rock mass including uniaxial compressive strength (UCS), Brazilian tensile strength (BTS), and elastic modulus (E) have been selected as the input parameters. A cluster of data was collected and divided into two random groups of training and testing datasets. Then, different statistical linear and artificial intelligence based nonlinear analyses were conducted on the training data to provide a reliable prediction model of KIC. These two predictive methods were then evaluated based on the testing data. To evaluate the efficiency of the proposed models for predicting the mode I fracture toughness of rock, various statistical indices including coefficient of determination (R2), root mean square error (RMSE), and mean absolute error (MAE) were utilized herein. In the case of testing datasets, the values of R2, RMSE, and MAE for the GEP model were 0.87, 0.188, and 0.156, respectively, while they were 0.74, 0.473, and 0.223, respectively, for the LMR model. The results indicated that the selected GEP model delivered superior performance with a higher R2 value and lower errors. 相似文献