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71.
《International Journal of Hydrogen Energy》2021,46(56):28397-28405
Water electrolysis powered by renewable electricity will likely be critical to a future hydrogen economy. However, the typical use of strongly acidic or alkaline electrolytes necessitates the use of expensive materials, while bubbles add to capital and operational costs, due to blocking of the electrode surface and the necessary use of pumps and gas-liquid separators. Here ‘bubble-free’ oxygen evolution at mild pH is carried out using an electrocatalyst that mimics photosystem II (PSII). The bubble-free electrode includes a gas-extracting Gore-Tex® membrane. Edge-functionalised graphene (EFG) is included to mimic the metal-binding local protein environment, and the tyrosine residue, in the oxygen evolving complex (OEC) of PSII, while MnOx and Ca2+ are incorporated to mimic the Mn4CaO5 cluster. Interaction between EFG, MnOx, and Ca2+ results in a significant, 130 mV fall in the overpotential required to drive electrocatalytic oxygen evolution at 10 mA cm−2, compared to the electrode without these biomimetic components. 相似文献
72.
Using a comprehensive set of drop weight impact test data (h50) newly compiled from literature for 308 materials, a recent approach to predict impact sensitivities of nitro compounds is generalized to most explosive substances of interest. Compared to previous ones, this procedure is more thoroughly validated and exhibits a good predictive value. Furthermore, it yields new insight into the physical mechanisms involved, explaining for instance the unexpected desensitization of some oxygen-deficient triazoles upon nitration. 相似文献
73.
74.
The main aim of this work is dual computer analysis of probabilistic coefficients for the homogenized tensor of the polymer filled with the rubber particles having randomized Poisson ratios of both constituents. The major issue is to verify an influence of a randomness in rubber Poisson ratio close to the compressibility limit on the uncertainty of the effective tensor probabilistic characteristics. Probabilistic analysis presented here is carried out using mainly the stochastic perturbation technique provided by the common application of the traditional FEM commercial code ABAQUS and the symbolic computations package MAPLE. This FEM-based technique employs polynomial response function of the optimum order recovered from the weighted least squares method and following a set of deterministic solutions obtained for various values of the randomized input parameter. Optimization procedure is released entirely into a symbolic environment, where maximization of the correlation factor together with minimization of the fitting variance and approximation error are applied. Homogenization technique consists in equating of deformation energies for the real composite and the artificial one characterized by the effective elasticity tensor with uncertainty. 相似文献
75.
《International Journal of Hydrogen Energy》2021,46(64):32480-32489
Based on that hydrogen energy is widely used in fuel cells, we focus our interests on the design and research of new complexes that catalyze the reaction in both directions, such as hydrogen evolution reactions (HERs) and hydrogen oxidation reactions (HORs). A highly efficient catalyst for both hydrogen evolution and oxidation, based on a nickel(II) complex, [Ni-en-P2](ClO4)2, has been designed and provided by the reaction of Ni(ClO4)2 with N,N′-bis[o-(diphenylphosphino)benzylidene]ethylenediamine (en-P2) in our group. Its structure has been determined by X-ray diffraction. [Ni-en-P2](ClO4)2 can electro-catalyze hydrogen evolution both from acetic acid and a neutral buffer (pH 7.0) with a turnover frequency (TOF) of 204 and 1327 mol of hydrogen per mole of catalyst per hour (H2/mol catalyst/h) under an overpotential (OP) of 914.6 mV and 836.6 mV, respectively. [Ni-en-P2](ClO4)2 also can electro-catalyze hydrogen oxidation with a TOF of 111.7 s−1 under an OP of 330 mV. The results can be attributed to that [NiII-en-P2](ClO4)2 has three good reversible redox waves at 1.01 (NiIII/II), −0.79 (NiII/I) and −1.38 V (NiI/0) versus Fc+/0, respectively. We hope these findings can afford a new method for the design of electrocatalysts for both H2 evolution and H2 oxidation. 相似文献
76.
《International Journal of Hydrogen Energy》2020,45(3):1640-1648
Facile yet efficient synthesis of high-performance nanocatalysts for hydrogen evolution from ammonia-borane (AB) hydrolysis is paramount. Here, we reported a novel hybrid nanocatalyst comprised of Rh nanoclusters (1.56 nm in diameters) anchored on nitrogen (N)-doped carbon nanotubes with embedded Ni nanoparticles (Ni@NCNTs), which was fabricated through adsorption of Rh ions on Ni@NCNTs. The achieved hybrid of Rh/Ni@NCNTs displayed excellent catalytic property (Turnover frequency: 959 min−1) toward AB hydrolysis, higher than many prior developed Rh-based catalysts. Note that this hybrid could be reused for at least nine runs with complete AB conversion to hydrogen. Rh nanoclusters with small size exhibiting high atom utilization and the synergetic effect between Ni and Rh are responsible for the excellent catalytic property of Rh/Ni@NCNTs toward AB hydrolysis. This work highlights the importance of utilization of magnetically recyclable Ni@NCNTs as support and synergetic component for efficient hydrolysis of AB. 相似文献
77.
This paper investigates the N-policy M/M/1 queueing system with working vacation and server breakdowns. As soon as the system becomes empty, the server begins a working vacation. The server works at a lower service rate rather than completely stopping service during a vacation period. The server may break down with different breakdown rates during the idle, working vacation, and normal busy periods. It is assumed that service times, vacation times, and repair times are all exponentially distributed. We analyze this queueing model as a quasi-birth–death process. Furthermore, the equilibrium condition of the system is derived for the steady state. Using the matrix-geometric method, we find the matrix-form expressions for the stationary probability distribution of the number of customers in the system and system performance measures. The expected cost function per unit time is constructed to determine the optimal values of the system decision variables, including the threshold N and mean service rates. We employ the particle swarm optimization algorithm to solve the optimization problem. Finally, numerical results are provided, and an application example is given to demonstrate the applicability of the queueing model. 相似文献
78.
Timothy Zurrer Kenneth Wong Jonathan Horlyck Emma C. Lovell Joshua Wright Nicholas M. Bedford Zhaojun Han Kang Liang Jason Scott Rose Amal 《Advanced functional materials》2021,31(9):2007624
The vast chemical and structural tunability of metal–organic frameworks (MOFs) are beginning to be harnessed as functional supports for catalytic nanoparticles spanning a range of applications. However, a lack of straightforward methods for producing nanoparticle-encapsulated MOFs as efficient heterogeneous catalysts limits their usage. Herein, a mixed-metal MOF, NiMg-MOF-74, is utilized as a template to disperse small Ni nanoclusters throughout the parent MOF. By exploiting the difference in Ni O and Mg O coordination bond strength, Ni2+ is selectively reduced to form highly dispersed Ni nanoclusters constrained by the parent MOF pore diameter, while Mg2+ remains coordinated in the framework. By varying the ratio of Ni to Mg in the parent MOF, accessible surface area and crystallinity can be tuned upon thermal treatment, influencing CO2 adsorption capacity and hydrogenation selectivity. The resulting Ni nanoclusters prove to be an active catalyst for CO2 methanation and are examined using extended X-ray absorption fine structure and X-ray photoelectron spectroscopy. By preserving a segment of the Mg2+-containing MOF framework, the composite system retains a portion of its CO2 adsorption capacity while continuing to deliver catalytic activity. The approach is thus critical for designing materials that can bridge the gap between carbon capture and CO2 utilization. 相似文献
79.
《International Journal of Hydrogen Energy》2020,45(29):14964-14971
Sr3Fe2O7-δ (SFO) with two-layer Ruddlesden-Popper (R–P) structure has recently been proved to be a promising material for the single phase cathode in proton conducting solid oxide fuel cells (P–SOFCs). To investigate the hydration reactions and proton conducting mechanisms of SFO and cobalt doped SFO (SFCO), both bulk and surface properties were calculated. We conclude that R–P structures have advantages in P–SOFCs. The unique Sr–O–M layer can facilitate the hydration process. Although in Sr–O–F and Sr–O–N layers, it is difficult for the formation and migration of oxygen vacancies, protons are most stable. Furthermore, cobalt doping can not only improve the electronic conductivity but also enhance surface properties of SFCO. The easily exposed Co–Fe–O surface can also facilitate the hydration reactions on the surface. Our work could give an informative insight into the relationships among the doped elements, the R–P structures, the hydration process and the proton conducting properties. 相似文献
80.
Xianghui Wang Pengda Zhao Jianwei Chen Huizhong Zhao Kai He 《Ceramics International》2018,44(11):12162-12168
Al–Cr slag is the solid waste generated by the smelting of Cr metal. It presents a range of environmental hazards. This study addressed the corrosion resistance of Al–Cr slag containing chromium–corundum refractories to slags with different basicity. Herein, we provide suggestions for the use of Cr–corundum of different basicity in kilns. Al–Cr slag, brown fused Al2O3, and chrome green were used as the raw materials, with pure calcium aluminate cement being used as a binder. The brick samples, prepared using different blends of chrome green and corundum, were fired at 1600?°C, and subsequently subjected to a slag corrosion test. After corrosion by slag of different basicity, the phase composition and microstructure of the sample were analyzed by X-ray diffraction, energy dispersive spectrometer and scanning electron microscopy. There were two major findings. First, Cr–corundum brick made from Al–Cr slag has a better slag corrosion resistance than that made from Cr2O3 and brown fused Al2O3. Second, Cr–corundum brick made from Al–Cr slag has superior corrosion resistance to slag with a CaO:SiO2 ratio of 2:1. 相似文献