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1.
《International Journal of Hydrogen Energy》2022,47(100):41956-41973
Due to stringent environmental regulations and the limited resources of fossil-based fuels, there is an urgent demand for clean and eco-friendly energy conversion devices. These criteria appear to be met by hydrogen proton exchange membrane fuel cells (PEMFCs). PEMFCs have attracted tremendous attention on account of their excellent performance with tunable operability and good portability. Nonetheless, their practical applications are hugely influenced by the scarcity and high cost of platinum (Pt) used as electrocatalysts at both cathode and anode. Pt is also susceptible to easy catalyst poisoning. Herein, this paper reviews the progress of the research regarding the development of electrocatalysts practically used in hydrogen PEMFCs, where the corner-stone reactions are cathodic oxygen reduction reaction (ORR) and anodic hydrogen oxidation reaction (HOR). To reduce the costs of PEMFCs, lessening or eliminating the use of Pt is of prime importance. For current and forthcoming laboratory/large-scale PEMFCs, there is much interest in developing substitute catalysts based on cheaper materials. As such are non-platinum (non-Pt), non-platinum group metals (non-PGMs), metal oxides, and non-metal electrocatalysts. Hence, high-performance, state-of-the-art, and novel structured electrocatalysts as replacements for Pt are needed. 相似文献
2.
《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
3.
《International Journal of Hydrogen Energy》2022,47(63):27023-27031
Hexagonal boron nitride (h-BN) as a layered inorganic nonmetallic material has been widely used. Hydrogen peroxide (H2O2) modification can trigger exfoliation and afford abundant B–OH active sites at edge of h-BN, which can enhance methane activation ability. Introducing tungsten oxide (WO3) to h-BN produces a similar effect, because doping WO3 into h-BN resulted in electron transfer to N, inducing fracture of B–N bond, resulting in N vacancy (triboron center), exposing more B sites and promoting the generation of B–OH. Significantly, the introduction of WO3 on the modified h-BN dramatically increased the concentration of B–OH compared with the unmodified h-BN, because H2O2 modification weakened B–N bond. By means of XRD, TEM, XPS,EPR, FT-IR, it is proved that the high concentration of B–OH active sites contributed to activating C–H bond, thus methane conversion and CO and H2 selectivity were significantly improved. 相似文献
4.
《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
5.
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
6.
《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
7.
《International Journal of Hydrogen Energy》2022,47(1):276-291
To the best of our knowledge, this is the first time to report the preparation of a dotted nanowire arrayed by 5 nm sized palladium and nickel composite nanoparticles (denoted as PdxNiy NPs) via a hydrothermal method using NU and PdO·H2O as the starting materials. The samples prepared at the mass ratio of NU to PdO·H2O 1:1, 1:2 and 2:1 were, respectively, nominated as catalyst c1, c2 and c3. The chemical compositions of all synthesized catalysts were mainly studied by using X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), revealing that metallic Ni was one main component of all prepared catalysts. Surprisingly, the main diffraction peaks appearing in the XRD patterns of all prepared catalysts were assigned to the metallic Ni rather than the metallic Pd. Very interestingly, as indicated by the TEM images, a large number of dotted nanowires arrayed by numerous equidistant 5 nm sized nanoparticles were distinctly exhibited in catalyst c1. More importantly, when being used as electrocatalysts for EOR, all prepared catalysts exhibited an evident electrocatalytic activity towards EOR. In the cyclic voltammetry (CV) test, the peak current density of the forward peak of EOR on catalyst c1 measured at 50 mV s?1 was as high as 56.1 mA cm?2, being almost 9 times higher than that of EOR on catalyst c3 (6.3 mA cm?2). Particularly, the polarized current density of EOR on catalyst c1 at 3600 s, as indicated by the chronoamperometry (CA) experiment, was still maintained to be around 1.47 mA cm?2, a value higher than the latest reported data of 1.3 mA cm?2 (measured on the pure Pd/C electrode). Presenting a novel method to prepare dotted nanowires arranged by 5 nm sized nanoparticles and showing the significant eletrocatalytic activities of the newly prepared dotted nanowires towards EOR were the major contributions of this preliminary work. 相似文献
8.
Hui Liu Yaohui Fu Jinhai Yuan Lei Yu Zhefei Wang Quan Liu Bo Wei Xuhong Wang 《Ceramics International》2021,47(12):16570-16578
To provide a basis for the high-temperature oxidation of ultra-high temperature ceramics (UHTCs), the oxidation behavior of Zr3[Al(Si)]4C6 and a novel Zr3[Al(Si)]4C6-ZrB2-SiC composite at 1500 °C were investigated for the first time. From the calculation results, the oxidation kinetics of the two specimens follow the oxidation dynamic parabolic law. Zr3[Al(Si)]4C6 exhibited a thinner oxide scale and lower oxidation rate than those of the composite under the same conditions. The oxide scale of Zr3[Al(Si)]4C6 exhibited a two-layer structure, while that of the composite exhibited a three-layer structure. Owing to the volatilization of B2O3 and the active oxidation of SiC, a porous oxide layer formed in the oxide scale of the composite, resulting in the degradation of its oxidation performance. Furthermore, the cracks and defects in the oxide scale of the composite indicate that the reliability of the oxide scale was poor. The results support the service temperature of the obtained ceramics. 相似文献
9.
This study deals with the anodisation of titanium grade 2 in 0.5-M sulphuric acid using a pulsed signal in a unipolar regime. The electrical parameters investigated are voltage, frequency and duty cycle. The use of duty cycles with a high percentage of anodic polarisation (90%), combined with high frequencies (1000 Hz) and the higher voltage tested (220 V), favoured the establishment of a plasma regime involving strong dielectric discharges, allowing the growth of thicker oxides but with rough architecture. The corrosion resistance of the formed film has been characterised by potentiodynamic tests in 0.5-M NaBr for localised corrosion resistance and by immersion tests in 10% v/v sulphuric acid solution for a uniform corrosion assessment. Current–time curves, visual observations and electron microscope analysis (scanning electron microscopy, energy-dispersive X-ray spectroscopy) were the tools selected to provide a correlation between technological parameters and oxide growth mechanism. For localised and uniform corrosion, anodisation at 220 V with a high level of anodic polarisation (90%) and frequency (1000 Hz) was verified to be particularly advantageous. 相似文献
10.
《International Journal of Hydrogen Energy》2022,47(4):2279-2292
A new catalyst for both water reduction and oxidation, based on an infinite chain, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n, is formed by the reaction of NiCl2, 1,3-propanediamine (tn) and K3 [Fe(CN)6]. {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can electro-catalyze hydrogen evolution from a neutral aqueous buffer (pH 7.0) with a turnover frequency (TOF) of 1561 mol of hydrogen per mole of catalyst per hour (H2/mol catalyst/h) at an overpotential (OP) of 837 mV {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n also can electro-catalyze O2 production from water with a TOF of ~45 mol O2 (mol cat)?1s?1 at an OP of 591 mV. Under blue light (λ = 469 nm), together with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H2A) as a sacrificial electron donor, {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n can photo-catalyze hydrogen generation from an aqueous buffer (pH 4.0) with a turnover number (TON) of 11,450 mol H2 per mole of catalyst (mol of H2 (mol of cat)?1) during 10 h irradiation. The average of apparent quantum yield (AQY) is as high as 40.96% during 10 h irradiation. Studies indicate that {[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n exists in two forms: a cyano-bridged chain ({[Ni(tn)2]3 [Fe(CN)4 (μ-CN)2]2}n) in solid, and a salt ([Ni(tn)2]3 [Fe(CN)6]2) in aqueous media; Catalytic reaction occurs on the nickel center of [Ni(tn)2]2+, and the introduction of [Fe(CN)6]3- can improve the catalytic efficiency of [Ni(tn)2]2+ for H2 or O2 generation. We hope these findings can afford a new method for the design of catalysts for both water reduction and oxidation. 相似文献