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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(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
3.
《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
4.
《Ceramics International》2022,48(6):8297-8305
Pure and Sn/Fe co-doped (0.2 at.% Sn and 0.6 at.% Fe, 0.6 at.% Sn and 0.2 at.% Fe, 1.0 at.% Sn and 1.0 at.% Fe) TiO2 nanoparticles were synthesized via a sol-gel method and subsequently calcined at different temperatures. Furthermore, the particles were analyzed by TG-DSC, XRD, TEM, HRTEM, EDS, SAED and UV–Vis for investigating the influences of dopant and calcination temperature on the thermal effect, composition, morphology, energy band gap (Eg) and the degradation efficiency of methyl orange (MO) under various light irradiations respectively. Results indicated that Sn/Fe co-doping inhibited the crystallization transformation from anatase to rutile phase of TiO2 and decreased the Eg. The increased calcination temperature and Sn/Fe co-doped effect brought about the abnormal grain growth of TiO2 nanoparticles. 0.6 at.% Sn/0.2 at.% Fe and 1.0 at.% Sn/1.0 at.% Fe co-doped TiO2 nanoparticles presented better photocatalytic performance than pure and 0.2 at.% Sn/0.6 at.% Fe co-doped TiO2 nanoparticles under visible light irradiation mainly due to the decreased Eg. On the contrary, 0.2 at.% Sn and 0.6 at.% Fe co-doped TiO2 nanoparticles calcined at 650 °C showed the most excellent photocatalytic performance under UV light irradiation, which was about twice as large as that of pure TiO2 possibly due to the formed hybrid structure of anatase and rutile phase as well as the h+-mediated decomposition pathway. 相似文献
5.
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
6.
Qian Wu Xiangmei Liu Bo Li Lei Tan Yong Han Zhaoyang Li Yanqin Liang Zhenduo Cui Shengli Zhu Shuilin Wu Yufeng Zheng 《材料科学技术学报》2021,67(8):70-79
Pathogens pose a serious challenge to environmental sanitation and a threat to public health.The frequent use of chemicals for sterilization in recent years has not only caused secondary damage to the environment but also increased pathogen resistance to drugs,which further threatens public health.To address this issue,the use of non-chemical antibacterial means has become a new trend for environmental disinfection.In this study,we developed red phosphorus nanoparticles(RPNPs),a safe and degradable photosensitive material with good photocatalytic and photothermal properties.The red phosphorus nanoparticles were prepared using a template method and ultrasonication.Under the irradiation of simulated sunlight for 20 min,the RPNPs exhibited an efficiency of 99.98%in killing Staphylococcus aureus due to their excellent photocatalytic and photothermal abilities.Transmission electron microscopy and ultraviolet–visible spectroscopy revealed that the RPNPs exhibited degradability within eight weeks.Both the RPNPs and their degradation products were nontoxic to fibroblast cells.Therefore,such RPNPs are expected to be used as a new type of low-cost,efficient,degradable,biocompatible,and eco-friendly photosensitive material for environmental disinfection. 相似文献
7.
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
8.
《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
9.
In this work, we designed a magnetically-separable Fe3O4-rGO-ZnO ternary catalyst, ZnO anchored on the surface of reduced graphene oxide (rGO)-wrapped Fe3O4 magnetic nanoparticles, where rGO, as an effective interlayer, can enhance the synergistic effect between ZnO and Fe3O4. The effects of three operational parameters, namely irradiation time, hydrogen peroxide dosage, and the catalyst dosage, on the photo-Fenton degradation of methylene blue and methyl orange were investigated. The results showed that the Fe3O4-rGO-ZnO had great potential for the destruction of organic compounds from wastewater using the Fenton chemical oxidation method at neutral pH. Repeatability of the photocatalytic activity after 5 cycles showed only a tiny drop in the catalytic efficiency. 相似文献
10.
《Ceramics International》2020,46(12):19942-19951
1D TiO2 nanotube arrays (TNTs), as versatile nanostructures, have attracted a considerable amount of scientific attention, particularly in photocatalytic applications. In the present study, UV radiation-assisted anodization method with various irradiation times (30–120 min) was employed as a preferable approach to fabricating TNTs with remarkable optical property and photocatalytic activity. The results revealed that in situ irradiation not only improved the surface area (from 30.10 to 48.5 m2), but also increased the roughness factor (from 77.27 to 124.73). Furthermore, UV radiation had a significant impact on optical property and by altering elemental composition, led to a red shift in absorption edge (from 3.2 to 1.4eV). Meanwhile, voltammetric experiments showed that 120 min UV radiation during anodization was able to substantially cause a surge of the photocurrent density and the photoconversion efficiency of TNTs from 0.15 to 0.55 mA cm−2 and from 13% to 40%, respectively. As a consequence of the improvement in optical property and photochemical features, anodic TNTs fabricated under 120 min UV radiation could increase the photocatalytic degradation of 2,4-DCP from 75% to 100%. Moreover, the kinetics study showed that all photocatalytic reactions followed zero-order kinetics which rate constant over the synthesized TNTs under 120 min UV radiation was about 5.1 times greater than that of conventionally fabricated TNTs. Likewise, the pathway of photocatalytic degradation and the proportion of reactive species in this process were assessed by scavenging tests. The results confirmed that holes (h+) play the main role that 53% of photocatalytic degradation occurred via both direct and indirect reactions with h+ species. The rest of the degradation pathways were also allocated to e− and •O2− species by accounting for 37% and 10%, respectively. 相似文献