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21.
《International Journal of Hydrogen Energy》2022,47(94):39864-39874
The reaction of H2 and O2 to water are studied over a Ag–Pd/TiO2 anatase catalyst, under dark and photo-irradiation conditions in the gas and liquid phases. The catalyst consisted of metal particles of mean size of ca.1 nm dispersed over 10–15 nm TiO2 particles. Kinetic parameters including order of reaction (n), rate constant (k), and activation energy (Ea), were evaluated. Ea for the thermal reaction was found to be 49-47 kJ mol?1. The oxidation reaction rate constant was found to be ca. 3 times higher in the presence of photons when compared to dark reaction at room temperature. The overall quantum yield of the reaction in the slurry phase was found to be 0.09. Considering the number of metal particles on TiO2, the photon yield per metal particle was found to be 0.16. A possible explanation of the changes in kinetics with respect to experimental conditions is given. 相似文献
22.
《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
23.
《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
24.
《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
25.
摘 要:为了提高码索引调制(code index modulation,CIM)系统的传输效率,提出了一种具有更低复杂度的单输入单输出(single input single output,SISO)的广义正交码索引调制(generalized orthogonal code index modulation,GQCIM)系统。CIM 系统使用扩频码和星座符号传输信息,但只能激活两个扩频码索引和一个调制符号。而 GQCIM 系统以一种新颖的方式克服了只激活一个调制符号的限制,同时充分利用了调制符号的正交性,增加扩频码索引以传输更多的额外信息位,提高了系统的传输效率。此外,分析了GQCIM系统的理论性能,推导了误码率性能的上界。通过蒙特卡罗仿真验证了GQCIM系统的性能,对比发现GQCIM系统的理论和仿真性能一致。而且在相同的传输效率下,结果显示GQCIM系统的性能优于同样具有正交性的调制系统,如广义码索引调制(generalized code index modulation,GCIM)系统、CIM系统、码索引调制-正交空间调制(code index modulation aided quadrature spatial modulation,CIM-QSM)系统、码索引调制-正交空间调制(code index modulation aided spatial modulation,CIM-SM)系统、脉冲索引调制(pulse index modulation,PIM)系统。 相似文献
26.
《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
27.
Yuchi Wan Hongjiang Zhou Muyun Zheng Zheng-Hong Huang Feiyu Kang Jia Li Ruitao Lv 《Advanced functional materials》2021,31(30):2100300
Electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy for ammonia (NH3) production under ambient conditions. However, it is severely impeded by the challenging activation of the NN bond and the competing hydrogen evolution reaction (HER), which makes it crucial to design electrocatalysts rationally for efficient NRR. Herein, the rational design of bismuth (Bi) nanoparticles with different oxidation states embedded in carbon nanosheets (Bi@C) as efficient NRR electrocatalysts is reported. The NRR performance of Bi@C improves with the increase of Bi0/Bi3+ atomic ratios, indicating that the oxidation state of Bi plays a significant role in electrochemical ammonia synthesis. As a result, the Bi@C nanosheets annealed at 900 ° C with the optimal oxidation state of Bi demonstrate the best NRR performance with a high NH3 yield rate and remarkable Faradaic efficiency of 15.10 ± 0.43% at − 0.4 V versus RHE. Density functional theory calculations reveal that the effective modulation of the oxidation state of Bi can tune the p-filling of active Bi sites and strengthen adsorption of *NNH, which boost the potential-determining step and facilitate the electrocatalytic NRR under ambient conditions. This work may offer valuable insights into the rational material design by modulating oxidation states for efficient electrocatalysis. 相似文献
28.
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
29.
Marc Neumann Patrick Gehre Rapuruchukwu Ifeyinwa Nwokoye Hans Jelitto Gerold A. Schneider Christos G. Aneziris 《Ceramics International》2021,47(13):18656-18661
Main objective of the presented research is the life time prediction of self-supporting flame-sprayed Al2O3- and Al2O3 -ZrO2 -TiO2-materials under constant load. The characteristic life time and its scatter were derived from stable crack growth tests and Weibull-statistics including the four-point-bending and ball-on-three-balls method. The potential life time was estimated in order to assess room-temperature handling and long term storage of self-supporting flame-sprayed alumina components. In terms of flexural strength, energy release, and subcritical crack growth parameters, distinct differences between both materials were shown. In turn, the characteristic life times only barely deviated from each other. From that the conclusion was drawn that life time performance under constant load application is governed by the characteristic flame-spray microstructure. However, advantages in the flame-spray processing of Al2O3 - ZrO2 -TiO2 are still given, attributed to its lower melting temperature. 相似文献
30.
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