Homogeneous physical mixtures containing a commercial Cu/ZnO/Al2O3 catalyst and a solid–acid catalyst were used to examine the acidity effects on dimethyl ether hydrolysis and their subsequent effects on dimethyl ether steam reforming (DME-SR). The acid catalysts used were zeolites Y [Si/Al = 2.5 and 15: denoted Y(Si/Al)], ZSM-5 [Si/Al = 15, 25, 40, and 140: denoted Z(Si/Al)] and other conventional catalyst supports (ZrO2, and γ-Al2O3). The homogeneous physical mixtures contained equal amounts, by volume, of the solid–acid catalyst and the commercial Cu/ZnO/Al2O3 catalyst (BASF K3-110, denoted as K3). The steam reforming of dimethyl ether was carried out in an isothermal packed-bed reactor at ambient pressure.
The most promising physical mixtures for the low-temperature production of hydrogen from DME contained ZSM-5 as the solid–acid catalyst, with hydrogen yields exceeding 90% (T = 275 °C, S/C = 1.5, τ = 1.0 s and P = 0.78 atm) and hydrogen selectivities exceeding 94%, comparable to those observed for methanol steam reforming (MeOH-SR) over BASF K3-110, with values equaling 95% and 99%, respectively (T = 225 °C, S/C = 1.0, τ = 1.0 s and P = 0.78 atm). Large production rates of hydrogen were directly related to the type of acid catalyst used. The hydrogen production activity trend as a function of physical mixture was
A key component of a hydrogen fuel cell is a catalyst to dissociate dihydrogen to hydrogen atoms. In the present study, the adsorption of hydrogen on Pt/C fuel cell catalysts has been investigated by inelastic neutron scattering spectroscopy.
Monitoring a clean Pt(50%)/C catalyst with low energy neutron spectroscopy, after exposure to dihydrogen at 20 K, as it was heated to room temperature, showed three distinct temperature regimes: (i) a decrease in intensity from 10 to 60 K, (ii) a rise to a maximum between 60 and 120 K and then (iii) a slow fall-off towards room temperature. We assign the three regions as: (i) desorption of physisorbed dihydrogen, (ii) dissociation of dihydrogen to give an adsorbed layer and (iii) damping of the response by an increasing Debye–Waller factor.
The vibrational INS spectra of a series of Pt/C catalysts prepared under varying conditions were similar indicating that the same types of site are common to all the catalysts, although the relative proportions of each site are sample dependent. Features at 520, 950 and part of the intensity at 1300 cm−1 are assigned to hydrogen on (1 1 1) faces, in good agreement with single crystal data. The mode at 640 cm−1 is assigned as the doubly degenerate asymmetric stretch of Pt(1 0 0) faces with the symmetric stretch near 550 cm−1.
We assign the bending mode of the on-top site to the feature at 470 cm−1. The Pt–H stretch mode was observed at 2079 cm−1. This is a significant result: this is the first time that hydrogen on the on-top sites has been observed on nanosized platinum particles supported on high surface area carbon black. The width of the INS peak is surprisingly large and may give additional information on the type and relative proportions of the crystallographic faces present on the catalyst particles. 相似文献
A novel concept for integrating fuel cells with desalination systems is proposed and investigated in this work. Two unique case studies are discussed — the first involving a hybrid system with a reverse osmosis (RO) unit and the second — integrating with a thermal desalination process such as multi-stage flash (MSF). The underlying motivation for this system integration is that the exhaust gas from a hybrid power plant (fuel cell/turbine system) contains considerable amount of thermal energy, which may be utilized for desalination units. This exhaust heat can be suitably used for preheating the feed in desalination processes such as reverse osmosis which not only increases the potable water production, but also decreases the relative energy consumption by approximately 8% when there is an increase of just 8°C rise in temperature. Additionally, an attractive hybrid system application which combines power generation at 70%+ system efficiency with efficient waste heat utilization is thermal desalination. In this work, it is shown that the system efficiency can be raised appreciably when a high-temperature fuel cell co-generates DC power in-situ with waste heat suitable for MSF. Results indicate that such hybrid system could show a 5.6% increase in global efficiency. Such combined hybrid systems have overall system efficiencies (second-law base) exceeding those of either fuel-cell power plants or traditional desalination plants. 相似文献
A Pt-deposited carbon nanotube (CNT) shows higher performance than a commercial Pt-deposited carbon black (CB) with reducing 60% Pt load per electrode area in polymer electrolyte fuel cells (PEFCs) below 500 mA/cm2. K2PtCl4 and H2PtCl6·6(H2O) are used for the Pt deposition onto multi-walled CNTs (MWCNTs), which are produced by the catalytic decomposition of hydrocarbons. The electric power densities produced using the Pt/CNT electrodes are greater than that of the Pt/CB by a factor of two to four on the basis of the Pt load per power. CNTs are thus found to be a good support of Pt particles for PEFC electrodes. TEM images show 2–4-nm Pt nanoparticles dispersed on the CNT surfaces. These high performances are considered to be due to the efficient formation of the triple-phase boundaries of gas–electrode–electrolyte. The mechanisms of Pt deposition are discussed for these Pt-deposited CNTs. 相似文献
Platinum-based catalysts, for the electro-oxidation of methanol, have been made by thermal decomposition of chloride precursors onto titanium mesh. The catalysed electrodes were successfully operated in acidic methanol electrolytes. Electrochemical characterisation has been carried out using cyclic voltammetry, electrochemical impedance spectroscopy and galvanostatic polarisations. A complete analysis of the electrochemical results showed that the preliminary performance of the catalysed titanium mesh was comparable to that achieved with carbon-supported PtRu catalysts. The catalysts formed on titanium mesh by thermal decomposition also exhibited dimensional stability. Catalysed titanium mesh therefore appears to be a promising alternative to carbon-supported catalysts for certain fuel cell applications. 相似文献
Carbon-supported Pt-based ternary alloy electrocatalysts were prepared by incipient wetness method in order to elucidate the origin of the enhanced activity of oxygen reduction reaction in PEMFC. To measure the catalytic activity and stability of the cathode alloy catalysts (electrodes containing Pt loading of 0.3 mg/cm2, 20 wt.% Pt/C, E-TEK), the I-V polarization curves were obtained. All alloy catalysts showed higher performances than Pt/C. It can be concluded that as platinum formed alloys with transition metals, the electronic state of Pt and the nearest neighbor Pt-Pt distance changes, which significantly influence the electrocatalytic activity for oxygen reduction.Long-term stability test was performed with the Pt6Co1Cr1/C alloy catalyst for 500 h. According to XPS analysis, the lower oxide component with Pt6Co1Cr1/C electrocatalyst provides a large portion of platinum in metallic species in the electrocatalyst and it seems to be mainly responsible for its enhanced activity towards oxygen reduction. 相似文献