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1.
The performance of high temperature polymer electrolyte fuel cell (HT-PEMFC) using platinum supported over tin oxide and Vulcan carbon (Pt/SnOx/C) as cathode catalyst was evaluated at 160-200 °C and compared with Pt/C. This paper reports first time the Pt/SnOx/C preparation, fuel cell performance, and durability test up to 200 h. Pt/SnOx/C of varying SnO compositions were characterized using XRD, SEM, TEM, EDX and EIS. The face-centered cubic structure of nanosized Pt becomes evident from XRD data. TEM and EDX measurements established that the average size of the Pt nanoparticles were ∼6 nm. Low ionic resistances were derived from EIS, which ranged from 0.5 to 5 Ω-cm2 for cathode and 0.05 to 0.1 Ω-cm2 for phosphoric acid, doped PBI membrane. The addition of the SnOx to Pt/C significantly promoted the catalytic activity for the oxygen reduction reaction (ORR). The 7 wt.% SnO in Pt/SnO2/C catalyst showed the highest electro-oxidation activity for ORR. High temperature PEMFC measurements performed at 180 °C under dry gases (H2 and O2) showed 0.58 V at a current density of 200 mA cm−2, while only 0.40 V was obtained in the case of Pt/C catalyst. When the catalyst contained higher concentrations of tin oxide, the performance decreased as a result of mass transport limitations within the electrode. Durability tests showed that Pt/SnOx/C catalysts prepared in this work were stable under fuel cell working conditions, during 200 h at 180 °C demonstrate as potential cathode catalyst for HT-PEMFCs.  相似文献   

2.
New nanostructured carbons have been developed through pyrolysis of organic aerogels, based on supercritical drying of cellulose acetate gels. These cellulose acetate-based carbon aerogels (CA) are activated by CO2 at 800 °C and impregnated by PtCl62−; the platinum salt is then chemically or electrochemically reduced. The resulting platinized carbon aerogels (Pt/CA) are characterized with transmission electron microscopy (TEM) and electrochemistry. The active area of platinum is estimated from hydrogen adsorption/desorption or CO-stripping voltammetry: it is possible to deposit platinum nanoparticles onto the cellulose acetate-based carbon aerogel surface in significant proportions. The oxygen reduction reaction (ORR) kinetic parameters of the Pt/CA materials, determined from quasi-steady-state voltammetry, are comparable with that of Pt/Vulcan XC72R. These cellulose acetate-based carbon aerogels are thus promising electrocatalyst support for PEM application.  相似文献   

3.
The electrochemical activity towards hydrogen oxidation reaction (HOR) of a high performance carbon-supported Pt-Ru electrocatalyst (HP 20 wt.% 1:1 Pt-Ru alloy on Vulcan XC-72 carbon black) has been studied using the thin-film rotating disk electrode (RDE) technique. The physical properties of the Pt-Ru nanoparticles in the electrocatalyst were previously determined by transmission electron microscopy (TEM), high resolution TEM, fast Fourier transform (FFT), electron diffraction and X-ray diffraction (XRD). The corresponding compositional and size-shape analyses indicated that nanoparticles generally presented a 3D cubo-octahedral morphology with about 26 at.% Ru in the lattice positions of the face-centred cubic structure of Pt. The kinetics for HOR was studied in a hydrogen-saturated 0.5 M H2SO4 solution using thin-film electrodes prepared by depositing an ink of the electrocatalyst with different Nafion contents in a one-step process on a glassy carbon electrode. A maximum electrochemically active surface area (ECSA) of 119 m2 g Pt−1 was found for an optimum Nafion composition of the film of about 35 wt.%. The kinetic current density in the absence of mass transfer effects was 21 mA cm−2. A Tafel slope of 26 mV dec−1, independent of the rotation rate and Nafion content, was always obtained, evidencing that HOR behaves reversibly. The exchange current density referred to the ECSA of the Pt-Ru nanoparticles was 0.17 mA cm−2, a similar value to that previously found for analogous inks containing pure Pt nanoparticles.  相似文献   

4.
Multi-walled carbon nanotubes (MWCNTs) were used as catalyst support for depositing platinum nanoparticles by a wet chemistry route. MWCNTs were initially surface modified by citric acid to introduce functional groups which act as anchors for metallic clusters. A two-phase (water-toluene) method was used to transfer PtCl62− from aqueous to organic phase and the subsequent sodium formate solution reduction step yielded Pt nanoparticles on MWCNTs. High-resolution TEM images showed that the platinum particles in the size range of 1-3 nm are homogeneously distributed on the surface of MWCNTs. The Pt/MWCNTs nanocatalyst was evaluated in the proton exchange membrane (PEM) single cell using H2/O2 at 80 °C with Nafion-212 electrolyte. The single PEM fuel cell exhibited a peak power density of about 1100 mW cm−2 with a total catalyst loading of 0.6 mg Pt cm−2 (anode: 0.2 mg Pt cm−2 and cathode: 0.4 mg Pt cm−2). The durability of Pt/MWCNTs nanocatalyst was evaluated for 100 h at 80 °C at ambient pressure and the performance (current density at 0.4 V) remained stable throughout. The electrochemically active surface area (64 m2 g−1) as estimated by cyclic voltammetry (CV) was also similar before and after the durability test.  相似文献   

5.
The preparation of a Pt–Co/C electrocatalyst for the oxygen reduction reaction in PEM fuel cells was achieved via a combined process of impregnation and seeding. The effects of initial pH of the precursor solution and Pt loading were all found to have a significant effect on both the electrocatalyst morphology and the cell performance when tested in a single PEM fuel cell. The optimum condition found for preparing the Pt–Co/C electrocatalyst was from an initial precursor solution pH of 2 at the metal loading of 23.6–30.3% (w/w). The Pt–Co/C electrocatalysts, formed under these optimal conditions, tested in a single PEM fuel cell with the carbon sub-layer, gave a cell performance of 772 mA/cm2 or 460 mW/cm2 at 0.6 V in a H2/O2 system. An electron pathway of oxygen reduction on the prepared Pt–Co/C electrocatalyst was also determined using a rotating disk electrode.  相似文献   

6.
Different Pt-based electrocatalysts supported on carbon nanofibers and carbon black (Vulcan XC-72R) have been prepared using a polymer-mediated synthesis. The electrocatalysts have been characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and cyclic voltammetry. The effect of carbon nanofibers treatment with HNO3 solution on Pt particle size and electroactive area has been analyzed. Highly dispersed Pt with homogeneous particle size and an electroactive area around of 100 m2 g−1 is obtained in raw carbon nanofibers. The oxidizing treatment of the carbon nanofibers produces agglomeration of the platinum nanoparticles and an electroactive area of 53 m2 g−1. Durability studies indicate a decrease of 14% in the electroactive area after 90 h at 1.2 V in 0.5 M H2SO4 for platinum supported on raw carbon nanofibers and Vulcan XC-72R. The electrocatalyst supported on oxidized carbon nanofibers are stable under similar conditions.  相似文献   

7.
The graphene supported Pt nanoparticles are prepared by ethylene glycol reduction method. The obtained Pt/graphene (Pt/G) nanocomposites are characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). TEM images show that the spherical Pt nanoparticles with sizes of 3.1 nm disperse uniformly on the surface of the graphene, which is consistent with the XRD date of 2.97 nm. The Pt/G nanocomposites show electrochemically active surface area (ECSA) of 62.7 m2/g. It has been found by electrochemical measurements (i.e., cyclic voltammetry, chronoamperometry) that the Pt/G nanocomposites exhibit good electrocatalytic activity and stability toward borohydride oxidation. Besides, the Pt/G nanocomposites are used as anode electrocatalyst in a direct borohydride fuel cell at 298 K, and the maximum power density is 42 mW/cm2, which is apparently higher than Vulcan XC-72R supported Pt (Pt/C) nanoparticles (34 mW/cm2).  相似文献   

8.
Nano-sized Pt–Pd/C and Pt–Co/C electrocatalysts have been synthesized and characterized by an alcohol-reduction process using ethylene glycol as the solvent and Vulcan XC-72R as the supporting material. While the Pt–Pd/C electrodes were compared with Pt/C (20 wt.% E-TEK) in terms of electrocatalytic activity towards oxidation of H2, CO and H2–CO mixtures, the Pt–Co/C electrodes were evaluated towards oxygen reduction reaction (ORR) and compared with Pt/C (20 wt.% E-TEK) and Pt–Co/C (20 wt.% E-TEK) and Pt/C (46 wt.% TKK) in a single cell. In addition, the Pt–Pd/C and Pt–Co/C electrocatalyst samples were characterized by XRD, XPS, TEM and electroanalytical methods. The TEM images of the carbon supported platinum alloy electrocatalysts show homogenous catalyst distribution with a particle size of about 3–4 nm. It was found that while the Pt–Pd/C electrocatalyst has superior CO tolerance compared to commercial catalyst, Pt–Co/C synthesized by polyol method has shown better activity and stability up to 60 °C compared to commercial catalysts. Single cell tests using the alloy catalysts coated on Nafion-212 membranes with H2 and O2 gases showed that the fuel cell performance in the activation and the ohmic regions are almost similar comparing conventional electrodes to Pt–Pd anode electrodes. However, conventional electrodes give a better performance in the ohmic region comparing to Pt–Co cathode. It is worth mentioning that these catalysts are less expensive compared to the commercial catalysts if only the platinum contents were considered.  相似文献   

9.
Multi-walled carbon nanotubes (MWCNTs) based micro-porous layer on the carbon paper substrates was prepared by in situ growth in a chemical vapor deposition setup. Platinum nanoparticles were deposited on in situ grown MWCNTs/carbon paper by a wet chemistry route at <100 °C. The in situ MWCNTs/carbon paper was initially surface modified by silane derivative to incorporate sulfonic acid–silicate intermediate groups which act as anchors for metal ions. Platinum nanoparticles deposition on the in situ MWCNTs/carbon paper was carried out by reducing platinum (II) acetylacetonate precursor using glacial acetic acid. High resolution TEM images showed that the platinum particles are homogeneously distributed on the outer surface of MWCNTs with a size range of 1–2 nm. The Pt/MWCNTs/carbon paper electrode with a loading of 0.3 and 0.5 mg Pt cm−2 was evaluated in proton exchange membrane single cell fuel cell using H2/O2. The single cells exhibited a peak power density of 600 and 800 mW cm−2 with catalyst loadings of 0.3 and 0.5 mg Pt cm−2, respectively with H2/O2 at 80 °C, using Nafion-212 electrolyte. In order to understand the intrinsically higher fuel cell performance, the electrochemically active surface area was estimated by the cyclic voltammetry of the Pt/MWCNTs/carbon paper.  相似文献   

10.
Enhancement in durability of electrocatalyst is still one of the most important issues in polymer electrolyte fuel cells (PEFCs). Here, we report a structurally coated electrocatalyst supported on carbon nanotubes (CNT), in which platinum (Pt) nanoparticles are coated by nitrogen doped carbon (NC) layers. CNT/NC/Pt/NC shows comparable electrochemical surface area (ECSA) and oxygen reduction reaction (ORR) activity to the non-coated electrocatalyst (CNT/NC/Pt), indicating that NC layer on Pt nanoparticles almost negligibly affects the activities of electrocatalyst; while, CNT/NC/Pt/NC exhibits a higher Pt stability due to the unique structure, in which the Pt nanoparticles are stabilized by the NC layers and Pt aggregation is decelerated proved by TEM measurement. Maximum power density of CNT/NC/Pt/NC reached 604 mW cm?2 with Pt loading of 0.1 mgPt cm?2, which only decreases by 7% compared to CNT/NC/Pt (650 mW cm?2). The electrochemical analysis and fuel cell test illustrate that NC layer on Pt nanoparticles enhances the durability without serious deterioration of fuel cell performance.  相似文献   

11.
Carbon supported Pt-Cu bimetallic nanoparticles are prepared by a modified NaBH4 reduction method in aqueous solution and used as the anode electrocatalyst of direct borohydride-hydrogen peroxide fuel cell (DBHFC). The physical and electrochemical properties of the as-prepared electrocatalysts are investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD), cyclic voltammetry (CV), chronoamperometry (CA), chronopotentiometry (CP) and fuel cell test. The results show that the carbon supported Pt-Cu bimetallic catalysts have much higher catalytic activity for the direct oxidation of BH4 than the carbon supported pure nanosized Pt catalyst, especially the Pt50Cu50/C catalyst presents the highest catalytic activity among all as-prepared catalysts, and the DBHFC using Pt50Cu50/C as anode electrocatalyst and Pt/C as cathode electrocatalyst shows as high as 71.6 mW cm−2 power density at a discharge current density of 54.7 mA cm−2 at 25 °C.  相似文献   

12.
We report a durable electrocatalyst support, highly graphitized mesoporous carbon (GMPC), for oxygen reduction in polymer electrolyte membrane (PEM) fuel cells. GMPC is prepared through graphitizing the self-assembled soft-template mesoporous carbon (MPC) under high temperature. Heat-treatment at 2800 °C greatly improves the degree of graphitization while most of the mesoporous structures and the specific surface area of MPC are retained. GMPC is then noncovalently functionalized with poly(diallyldimethylammonium chloride) (PDDA) and loaded with Pt nanoparticles by reducing Pt precursor (H2PtCl6) in ethylene glycol. Pt nanoparticles of ∼3.0 nm in diameter are uniformly dispersed on GMPC. Compared to Pt supported on Vulcan XC-72 carbon black (Pt/XC-72), Pt/GMPC exhibits a higher mass activity towards oxygen reduction reaction (ORR) and the mass activity retention (in percentage) is improved by a factor of ∼2 after 44 h accelerated degradation test under the potential step (1.4-0.85 V) electrochemical stressing condition which focuses on support corrosion. The enhanced activity and durability of Pt/GMPC are attributed to the graphitic structure of GMPC which is more resistant to corrosion. These findings demonstrate that GMPC is a promising oxygen reduction electrocatalyst support for PEM fuel cells. The approach reported in this work provides a facile, eco-friendly promising strategy for synthesizing stable metal nanoparticles on hydrophobic support materials.  相似文献   

13.
New nanostructured carbons have been prepared from pyrolysis of recently developed highly porous cellulose, aerocellulose (AC). Aerocellulose is an ultra-light and highly porous pure cellulose material prepared from cellulose gels followed by drying in carbon dioxide supercritical conditions. The carbonized aerocellulose (CAC) materials were obtained after pyrolysis of the aerocellulose under nitrogen flow at 830 °C, and subsequently doped by platinum nanoparticles. The platinum insertion process consisted of (i) thermal activation at various temperatures in CO2 atmosphere, (ii) impregnation by PtCl62− and (iii) platinum salt chemical reduction. The aerocellulose materials and their carbonized counterparts were investigated by scanning and transmission electron microscopy (SEM and TEM), mercury porosimetry and thermogravimetric analysis. The morphology of the platinum particles deposited on the carbonized aerocellulose materials (Pt/CAC) was investigated by transmission electron microscopy (TEM) and X-ray diffraction (XRD): the Pt particles are of 4–5 nm size, mainly agglomerated, as a result of the complex surface chemistry of the CAC. Their electrocatalytic activity was investigated by quasi-steady-state voltammetry in the rotating disk electrode (RDE) setup, regarding the oxygen reduction reaction (ORR). The Pt/CAC materials exhibit ORR specific activities comparable with those of commercial Pt/Vulcan XC72R. Their mass activity is lower, as a result of the ca. 10 times smaller specific area of platinum as compared with the commercial electrocatalyst. We nevertheless believe that provided an appropriate pyrolysis temperature is chosen, such green carbonized aerocellulose could be a promising electrocatalyst support for PEM application.  相似文献   

14.
Suspensions of Pt/C catalyst nanoparticles in Nafion®-alcohol solutions have been electrosprayed over carbon paper to prepare cathodes for proton exchange membrane fuel cells (PEMFC). Catalyst layers with platinum loading ranging from 0.1 mgPt cm−2 down to 0.0125 mgPt cm−2 and different Nafion® contents were obtained by this method. Morphological studies of the catalyst layers by SEM inspection showed fractal structures with a high dispersion of catalyst. Fuel cell performance of membrane-electrode assemblies (MEAs) made from these cathodes revealed a strong dependence on the Nafion® concentration in the electrosprayed suspension. In the platinum loading range 0.1-0.025 mgPt cm−2 and optimal Nafion® content, a linear relation between fuel cell power density and platinum loading has been found, such that a reduction of platinum content by a factor 4 only reduces the performance by roughly a factor 2. However for the lowest platinum loading investigated, 0.0125 mgPt cm−2, a sharp drop in performance was noticed.  相似文献   

15.
Increasing the efficiency of electrocatalyst is the key demand for the polymer electrolyte membrane fuel cells (PEMFC). To address the activity and performance challenges of commercial electrocatalyst, Pt/C, we introduce a new hybrid catalyst support for Pt nanoparticles. In this regard, combining or mixing specific type of carbon-based supports is a feasible strategy to increase catalyst utilization and performance. In the current study, Pt nanoparticles (NPs) were decorated on a new hybrid network, comprising of carbon nanofiber (CNF) and carbon black (CB), by means of a facile and efficient microwave (MW) assisted reduction method. All synthesized electrocatalysts were characterized to elucidate chemical and morphological structures. Then, the hybrid electrocatalysts were utilized as hydrogen oxidation reaction (HOR) and oxygen reduction reaction (ORR) electrocatalysts and their electrocatalytic activities were investigated by using cyclic voltammetry (CV) and linear sweep voltammetry (LSV), respectively. We found that the hybridization of CNF with CB substantially improved not only the electrocatalytic activity but also the fuel cell performance, which can be attributed to a consecutive conductive network, in which CB acts as a spacer, and synergistic effects between the CNF and CB. The hybrid electrocatalyst (Pt/CNF-CB with 50:50 wt%) showed a superior activity toward HOR and ORR while also offering exceptional fuel cell performance. That hybrid possessed the highest electrochemically active surface area (ECSA) compared with Pt/CNF and Pt/CB. In addition, the mass activity (at 0.80 V vs RHE) of the Pt/CNF-CB (50:50 wt%) is about 3.3 and 3.5 times higher than that of Pt/CNF and Pt/CB, respectively. Furthermore, that hybrid electrocatalyst exhibited enhanced fuel cell performance with 907 mW.cm−1 maximum power density. This work demonstrated that the CNF-CB supported Pt nanoparticles as electrocatalysts are extremely promising for fuel cell reactions.  相似文献   

16.
We fabricate polybenzimidazole (PBI) wrapped carbon nanotubes (MWCNTs) as support material for platinum-based fuel cell electrocatalyst. With the aid of microwave-assisted polyol reduction, we obtain very fine platinum (Pt) nanoparticles on PBI/MWCNT support while reducing the amount of Pt waste during synthesis. Cyclic voltammetry (CV) concludes that Pt-PBI/MWCNT has 43.0 m2 g−1 of electrochemically active surface area (ECSA) to catalyze hydrogen oxidation. Furthermore, after the 1000th cycle, Pt-PBI/MWCNT preserves almost 80% of its maximum ECSA, meaning that Pt-PBI/MWCNT is much more durable than the Pt/MWCNT and commercial Pt/C. High-temperature proton exchange membrane fuel cell (HT-PEMFC) performance tests are conducted under H2/Air conditions at the temperatures ranging from 150 °C to 180 °C. Nevertheless, tests conclude that the maximum power density values of the Pt-PBI/MWCNT are found inferior to the Pt/C at all temperatures (e.g., 47 vs. 62 mW cm−2 at 180 °C), suggesting that some balance between durability and performance has to be taken into consideration.  相似文献   

17.
Platinum electrocatalysts deposited on multi-walled carbon nanotubes (CNT) with high loading were prepared using a microwave-assisted polyol reduction method and employed for direct methanol fuel cells (DMFC). A zwitterionic surfactant was used as a stabilizing agent for the formation of Pt nanoparticles. A uniform and narrow size distribution of highly dispersed Pt nanoparticles could be achieved by adjusting the weight ratio of surfactant to Pt precursor allowing for Pt loadings of up to 60 wt%. The heating time and the temperature for the ethylene glycol (EG) oxidation were found to be the key factors for depositing Pt nanoparticles homogeneously on carbon nanotubes. The smallest average particle diameter of 1.8 nm was obtained through microwave heating to 140 °C in 50 s. The structure, amount and morphology of the electrocatalysts were characterized with XRD, TGA, and TEM, respectively. Single cell DMFC measurements were performed in a membrane-electrode assembly (MEA) with 5 cm2 active area and very low catalyst loading (0.25 mg cm−2 of noble metal on both anode and cathode). The DMFC performance of the surfactant stabilized cathode catalyst obtained by the new method described here revealed that the power density was three times higher than for a commercial catalyst used for comparison and two times higher than for an unstabilized CNT supported catalyst.  相似文献   

18.
In this study, the effects of the addition of multi-wall carbon nanotubes (MWCNTs) into a microporous layer (MPL) containing Vulcan XC72R on the oxygen reduction reaction (ORR) were studied. We tested various percentages of MWCNTs and Vulcan XC72R in the MPLs of gas-diffusion electrodes (GDEs) with various Pt loadings in the catalyst layer. The performance of the ORR in the electrodes was studied with linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS), and chronoamperometry. The structures of the MPLs were investigated by using scanning electron microscopy (SEM), mercury porosimetry (MP), and gas permeability. In addition, the optimum polytetrafluoroethylene (PTFE) content of the MPL was determined. Our results indicate that the performances of the GDEs are optimal under the following conditions: (a) 60 wt% MWCNTs and 40 wt% Vulcan XC72R with a Pt loading of 0.115 mg/cm2; (b) 80 wt% MWCNTs and 20 wt% Vulcan XC72R with a Pt loading of 0.5 mg/cm2; and (c) 40 wt% MWCNTs and 60 wt% Vulcan XC72R with a Pt loading of 1 mg/cm2.  相似文献   

19.
The carbon supported Pt hollow nanospheres were prepared by employing cobalt nanoparticles as sacrificial templates at room temperature in aqueous solution and used as the anode electrocatalyst for direct borohydride-hydrogen peroxide fuel cell (DBHFC). The physical and electrochemical properties of the as-prepared electrocatalysts were investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD), cyclic voltammetry (CV), chronoamperometry (CA), chronopotentiometry (CP) and fuel cell test. The results showed that the carbon supported Pt nanospheres were coreless and composed of discrete Pt nanoparticles with the crystallite size of about 2.8 nm. Besides, it has been found that the carbon supported Pt hollow nanospheres exhibited an enhanced electrocatalytic performance for BH4 oxidation compared with the carbon supported solid Pt nanoparticles, and the DBHFC using the carbon supported Pt hollow nanospheres as electrocatalyst showed as high as 54.53 mW cm−2 power density at a discharge current density of 44.9 mA cm−2.  相似文献   

20.
In this study, new electrocatalysts for PEM fuel cells, based on Pt nanoparticles supported on hybrid carbon support networks comprising reduced graphene oxide (rGO) and carbon black (CB) at varying ratios, were designed and prepared by means of a rapid and efficient microwave-assisted synthesis method. Resultant catalysts were characterized ex-situ for their structure, morphology, electrocatalytic activity. In addition, membrane-electrode assemblies (MEAs) fabricated using resultant electrocatalysts and evaluated in-situ for their fuel cell performance and impedance characteristics. TEM studies showed that Pt nanoparticles were homogeneously decorated on rGO and rGO-CB hybrids while they had bigger size and partially agglomerated distribution on CB. The electrocatalyst, supported on GO-CB hybrid containing 75% GO (HE75), possessed very encouraging results in terms of Pt particle size and dispersion, catalytic activity towards HOR and ORR, and fuel cell performance. The maximum power density of 1090 mW cm?2 was achieved with MEA (Pt loading of 0.4 mg cm?2) based on electrocatalyst, HE75. Therefore, the resultant hybrid demonstrated higher Pt utilization with enhanced FC performance output. Our results, revealing excellent attributes of hybrid supported electrocatalysts, can be ascribed to the role of CB preventing rGO sheets from restacking, effectively modifying the array of graphene and providing more available active catalyst sites in the electrocatalyst material.  相似文献   

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