首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 78 毫秒
1.
To accelerate the commercialization of fuel cells, many efforts have been made to develope highly active and durable Pt-based catalyst for oxygen reduction reaction (ORR). Herein, PtCu porous nanowires (PNWs) with controllable composition are synthesized through an ultrasound-assisted galvanic replacement reaction. The porous structure, surface strain, and electronic property of PtCu PNWs are optimized by tuning composition, which can improve activity for ORR. Electrochemical tests reveal that the mass activity of Pt0.5Cu0.5 PNWs (Pt/Cu atomic ratio of 1:1) reaches 0.80 A mgPt?1, which is about 5 times higher than that of the commercial Pt/C catalyst. Notably, the improved activity of the porous nanowire catalyst is also confirmed in the single-cell test. In addition, the large contact area with the carrier and internal interconnection structure of Pt0.5Cu0.5 PNWs enables them to exhibit much better durability than the commercial Pt/C catalyst and Pt0.5Cu0.5 nanotubes in accelerated durability test.  相似文献   

2.
High cost and poor durability of Pt-based cathode catalysts for oxygen reduction reaction (ORR) severely hamper the popularization of proton exchange membrane fuel cells (PEMFCs). Tailoring carbon support is one of effective strategies for improving the performance of Pt-based catalysts. Herein, petroleum vacuum residue was used as carbon source, and nitrogen-doped porous carbon (N-PPC) was synthesized using a simple template-assisted and secondary calcination method. Small Pt nanoparticles (Pt NPs) with an average particles size of 1.8 nm were in-situ prepared and spread evenly on the N-PPC. Interestingly, the lattice compression (1.08%) of Pt NPs on the N-PPC (Pt/N-PPC) was clearly observed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), which was also verified by the shift of (111) crystal plane of Pt on N-PPC to higher angles. The X-ray photoelectron spectroscopy (XPS) results suggest that the N-PPC support had a strong effect on anchoring Pt NPs and endowing surface Pt NPs with lowered d band center. Thus, the Pt/N-PPC as a catalyst simultaneously boosted the ORR activity and durability. The specific activity (SA) and mass activity (MA) of the Pt/N-PPC at 0.9 V reached 0.83 mA cm−2 and 0.37 A mgPt−1, respectively, much higher than those of the commercial Pt/C (0.21 mA cm−2 and 0.11 A mgPt−1) in 0.1 M HClO4. The half-wave potential (E1/2) of Pt/N-PPC exhibited only a minimal negative shift of 7 mV after 30,000 accelerated durability tests (ADT) cycles. More importantly, an H2–O2 fuel cell with a Pt/N-PPC cathode achieved a power density of 866 mW cm−2, demonstrating that the prepared catalyst has a promising application potential in working environment of PEMFCs.  相似文献   

3.
Synthesis of Pt-based catalysts with high activity and durability for oxygen reduction reaction (ORR) remains a very challenging task in the field of fuel cells. Here, Co-doped Pt nanoparticles (NP) with surface-defect ZrO2 are supported on the multi-walled carbon nanotubes (MWCNTs) (denoted as Pt–Co + ZrO2/MWCNTs). The Pt–Co + ZrO2/MWCNTs displays an ORR mass activity of 0.98 A mgPt?1 at 0.9 V, which is 4.1-fold higher than that of the commercial Pt/C (0.238 A mgPt?1). Further durability test shows that the Pt–Co + ZrO2/MWCNTs remains nearly unchanged ORR mass activity after 50000 accelerated durability testings (ADTs). Based on the mass performance and surface performance, the fuel cell with Pt–Co + ZrO2/MWCNTs cathode has far better power performance than that with commercial Pt/C. Moreover, the fuel cell with Pt–Co + ZrO2/MWCNTs cathode undergo only a 6.1% maximum power loss after 50000 ADTs. However, that with commercial Pt/C cathode after 30000 ADTs has 39.6% maxinum power loss. More impressively, compared to the 220 mV loss of Pt/C after 30000 ADTs, the Pt–Co + ZrO2/MWCNTs cathode also displays only 20 mV loss at 0.8 A/cm2 after 50000 ADTs. The enhanced intrinsic activity of Pt–Co + ZrO2/MWCNTs may be attributed to the Co-doped Pt NPs and interface effect of Co-doped Pt NPs and surface defect-rich ZrO2.  相似文献   

4.
Developing active and durable electrocatalysts for oxygen reduction reaction (ORR) is of great significance in proton exchange membrane fuel cells (PEMFCs). Herein, we develop a facile strategy to synthesize PtCu nanoparticles with enhanced ORR performance through morphology tuning and transition-metal doping. Two distinct PtCu nanoparticles, namely nanooctahedrons (NOs) and nanospheres (NSs), are selectively synthesized in presence or absence of W(CO)6 via a facile one-pot method. Furthermore, by introducing a small amount of third transition metal, M-doped (M = Sc, Y, La, Gd, Fe) PtCu NOs are obtained. Electrocatalytic results suggest that the ORR performance of PtCu NOs is better than that of PtCu NSs due to the morphology advantages. And the ORR performance of PtCuM NOs is further promoted since the doping effect of transition metals compared to that of PtCu NOs. Particularly, PtCuSc NOs exhibit remarkable mass activity (1.652 mA μg−1Pt) and specific activity (2.093 mA cm−2), which are 9.9 and 7.2 times higher than that of commercial Pt/C catalysts at 0.8 V (vs. RHE). Moreover, after accelerated stability tests, the loss of mass activity for PtCuSc NOs is only 9.2%, which is much lower than that of PtCu NOs (16.5%) and commercial Pt/C (44.3%). This work provides a feasible idea to boost the ORR performances of Pt-based nanoparticles.  相似文献   

5.
Highly active and durable Pt-based catalysts for oxygen reduction reaction (ORR) are very important and necessary for the proton exchange membrane fuel cells (PEMFCs). In this paper, we report the preparation and performance study of ORR catalysts composed of core-shell Pt–Co alloy nanoparticles (NPs) on multi-walled carbon nanotubes (MWCNTs) anchored with ZrO2 NPs (denoted as Pt–Co–ZrO2/MWCNTs). Thanks to the unique three-phase structure, the mass activity of Pt–Co–ZrO2/MWCNTs for ORR at 0.9 V versus reversible hydrogen electrode (RHE) is1577 mA mgPt?1, which is ~6.6-fold higher than that of the commercial Pt/C (238 mA mgPt?1). After 50,000 cycles for durability test, the mass activity of Pt–Co–ZrO2/MWCNTs for ORR remained 88% of its initial value. In stark contrast, that of Pt/C kept only about 56.3% of its initial value. More importantly, its catalytic performance was fully observed/verified in a H2-air PEMFC single cell test. When the Pt loading of Pt–Co–ZrO2/MWCNTs loaded cathode was one fourth of that with commercial Pt/C as the cathode catalyst, comparable cell performance was achieved. More impressively, the MEA with Pt–Co–ZrO2/MWCNTs underwent only 24.5% degradation in maximum power density after 30,000 accelerated durability tests (ADTs). However, the MEA with Pt/C after 30,000 ADTs exhibited 39.6% performance loss in maximum power density. The enhanced mass activity and catalytic durability of Pt–Co–ZrO2/MWCNTs could be attributed to the core-shell Pt–Co alloy NPs with Pt-rich surface and the interface effect between Pt–Co alloy NPs and oxygen vacancy-rich ZrO2 NPs. In addition, this research also provided a solution to the durability issue of cathodes without sacrificing ORR mass activity, which would promote practical application of PEMFCs.  相似文献   

6.
Pt-based hollow nanocrystals have shown an astonishing performance toward oxygen reduction reaction (ORR) because of their open structures, high surface areas and large Pt atom utilization. However, the careful geometric control of hollow nanocrystals is still not easy. Here, a facile template-free method was reported for the synthesis of ultrathin-wall PtCu nanocages with small islands on the surface (U–PtCu NCs). Moreover, the wall thickness of nanocages and the density of islands were well-tuned by controlling the experiment conditions. In the end, the novel hollow structures with abundant defects as well as the synergistic interaction between Pt and Cu elements endowed U–PtCu NCs with enhanced ORR activity. Specifically, its mass activity was 0.36 A mg−1 and its specific activity was 0.71 mA cm−2, which were about 4.2 and 7.1 times higher than that of commercial Pt/C. In addition, the enhanced stability was proved by the accelerated durability test of 10 000 cycles.  相似文献   

7.
Designing oxygen reduction reaction (ORR) catalysts with high activity and long durability is significant for the development of proton exchange membrane fuel cells. Herein, the optimized platinum nanowires are used as templates for inducing growth of cobalt-containing metal-organic framework, deriving uniform nanofibers. After the calcination, the metal ions are transferred into the nitrogen-rich porous carbon, and wrapped by the carbon skeleton to form the PtCo bimetal incorporated nanofibers as high-performance ORR electrocatalyst. The Pt4Co@NC-900 catalyst yields high specific activity (1.37 mA cm−2) in comparison to Pt/C (0.38 mA cm−2). The mass activity (MA) of Pt4Co@NC-900 catalyst is approximately 3.8-fold higher than that of the commercial Pt/C under acidic conditions. After the accelerated durability tests, the Pt4Co@NC-900 catalyst presents only 16% loss in MA, while Pt/C catalyst retains 73.0% of the initial MA. The improved ORR performance can be ascribed to the synergistic interaction between Co and Pt.  相似文献   

8.
Pt-based catalysts are still most attractive and could be the major driving force for facile electrochemical reactions in direct methanol fuel cells (DMFCs). In this work, a Pt3Mn nanowire network structures (NWNs) catalyst was successfully synthesized by a soft template (CTAB) method. The morphology and elemental composition of the Pt3Mn NWNs were investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma-optical emission spectroscopy (ICP-OES). The electrocatalytic behavior of the synthesized Pt3Mn NWNs catalyst towards methanol oxidation reaction (MOR) was studied by cyclic voltammetry (CV) and chronoamperometry (CA). The results reveal that the Pt3Mn NWNs has superior MOR activity and durability compared to Pt NWNs and commercial Pt/C. The mass and specific activities of Pt3Mn NWNs are 0.843 A mg−1 and 1.8 mA cm−2 respectively, which are twice that of commercial Pt/C. Additionally, the results of CA test indicate that the Pt3Mn NWNs possesses better durability than Pt NWNs and commercial Pt/C catalysts in acidic media, which is expected to be a new alternative anode material in DMFCs.  相似文献   

9.
We report the use of nitrogen-doped three-dimensional carbon frameworks (N-MCF) to promote the catalytic performance of nano-sized Pt electrocatalyst for the catalysis of oxygen reduction reaction (ORR). The N-MCF, obtained by pyrolysis of zeolitic imidazolate framework, provides abundant edges, defects, and heteroatom-doped sites to anchor Pt nanoparticles, leading to strong Pt-support interaction and excellent particle dispersion within its three-dimensional mass transport channels. Electrochemical results show only 8 mV degradation in the half-wave potential after accelerated durability test for the N-MCF supported Pt catalysts. Meanwhile, the mass activity and specific activity of Pt/N-MFC could reach 246 mA mg−1Pt and 0.276 mA cm−2 at 0.90 VRHE, which is better than that of commercial Pt/C. Moreover, the high Pt utilization of Pt/N-MFC (186 mg Pt kW−1) could reach 1.9 times than that of fuel cell fabricated with commercial Pt/C cathode.  相似文献   

10.
High-performance platinum nanoparticle catalysts (Pt–NPCs) remain the most widespread applied electrocatalysts for oxygen reduction reaction (ORR). Here, cetyltrimethylammonium bromide (CTAB), a surface-controlling agent, is introduced to modulate the microstructure and size of Pt nanoparticles (NPs) via a microwave-assisted heating process. The Pt-NPC assisted by 5 wt% CTAB exhibits the highest mass activity (MA) of 0.072 A mgPt?1 and specific activity (SA) of 0.077 mA cm?2, higher than those of commercial Pt/C (0.023 A mgPt?1 and 0.035 mA cm?2). Transmission electron microscopy (TEM) results indicate that Pt NPs are uniformly dispersed onto carbon supports with an average size of 2.39 nm. When applied in membrane electrode assembly (MEA), it exhibits the highest power density of 1.142 W cm?2, which is about 1.24 times larger than that of commercial Pt/C.  相似文献   

11.
The objective of this study was to fabricate an efficient structural catalyst electrode of Pt/C consisting of double catalyst layers (DCL) with catalyst-ink spray and electrophoresis deposition (EPD) methods. The prepared Pt/C DCL electrode with Pt-dispersed and Pt-concentrated catalyst layers demonstrated better electrochemical properties than individual Pt/C single catalyst layer (SCL) electrodes. An S1E1 DCL electrode with Pt loading weight ratio of 1:1 between the Pt-dispersed and Pt-concentrated layers exhibited a higher electrochemical surface area (ECSA, 57.2 m2/gPt) and lower internal resistance (20 Ω) than an individual Pt-dispersed SCL electrode prepared with only the spray method (S1E0, 31.9 m2/gPt and 132 Ω) and an individual Pt-concentrated SCL electrode prepared with only the EPD method (S0E1, 34.1 m2/gPt and 120 Ω). The S1E1 DCL electrode exhibited 2.1 and 1.7 times higher mass activity for methanol oxidation reaction (MOR) than S1E0 and S0E1 SCL electrodes, respectively (1,230 mA/mgPt for S1E1 vs. 595 mA/mgPt for S1E0 and 715 mA/mgPt for S0E1). In addition, the S1E1 DCL electrode demonstrated high MOR durability after 1,000 sequential cycles while losing 30% activity. Meanwhile, S0E1 and S1E0 SCL electrodes rapidly lost 52% and 55% activity, respectively. These improved electrochemical performances of DCL electrode were owing to the advantages of separating Pt catalysts into two layers, which provides more Pt catalytic active sites to the electrolyte than those in SCL electrodes. Our observation may aid in minimizing the usage amount of Pt catalysts (~0.16 mgPt/cm2) compared to those in present commercial Pt/C composites (~0.3 mgPt/cm2) as well as maximize efficient Pt utilization. More importantly, with regard to proton exchange membrane fuel cell (PEMFC) activity as a crucial in-situ characterization of a catalyst, a membrane electrode assembly (MEA) containing S1E1 as the anode electrode could generate mass maximum power density of 3.84 W/mgPt, 3.6 times higher than the present commercial one (1.07 W/mgPt).  相似文献   

12.
This paper reports use of an ultrasonic spray for producing ultra-low Pt load membrane electrode assemblies (MEAs) with the catalyst coated membrane (CCM) fabrication technique. Anode Pt loading optimization and rough cathode Pt loading were investigated in the first stage of this research. Accurate cathode Pt coating with catalyst ink using the ultrasonic spray method was investigated in the second stage. It was found that 0.272 mgPt/cm2 showed the best observed performance for a 33 wt% Nafion CCM when it was ultrasonically spray coated with SGL 24BC, a Sigracet manufactured gas diffusion layer (GDL). Two different loadings (0.232 and 0.155 mgPt/cm2) exposed to 600 mA/cm2 showed cathode power mass densities of 1.69 and 2.36 W/mgPt, respectively. This paper presents impressive cathode mass power density and high fuel cell performance using air as the oxidant and operated at ambient pressure.  相似文献   

13.
To achieve the practical application of direct methanol fuel cells, it is highly important to develop effective electrocatalyst with high activity and favorable durability. Herein, we report the successful preparation of PtCu bimetallic nanoparticles supported on ceria/multi-walled carbon nanotubes composite (PtCu–CeO2/MWCNTs) via microwave-assisted polyol reduction procedure. The composition and morphology of as-obtained composite catalysts were characterized by X-ray diffraction, Raman, X-ray photoelectron spectra, scanning electron microscopy and transmission electron microscopy. The synergistic effects combining PtCu bimetallic effect and oxygen vacancy effect in ceria of such composite catalysts provide abundant active surface area and enhanced conductivity for the effective charge transport during the methanol oxidation reaction (MOR) process. As a results, the PtCu–CeO2/MWCNTs with optimized Pt proportion achieve greatly enhanced MOR activity with mass activity of 1.28 A mg−1Pt and specific activity of 2.03 mA cm−2, superior CO tolerance and reliable stability in contrast to that of commercial Pt/C catalysts.  相似文献   

14.
Nanostructures of PtNiCo alloy have been prepared using a simple solvothermal process followed by annealing at higher temperature and studied for electrochemical oxygen reduction reaction (ORR) kinetics. PtNiCo/C catalyst has demonstrated an interesting trend of enhancement in the ORR activity along with long-term durability. The specific activity of 2.47 mA cm?2 for PtNiCo-16h/C (PtNiCo/C prepared at reaction time of 16 h) is ~12 times higher than that of Pt/C (0.2 mA cm?2). Further, X-ray diffraction, transmission electron microscopy and X-ray photo electron spectroscopy studies have been carried out systematically to understand the phase formation, morphology along with surface defects and elemental analysis respectively. The durability of the catalyst was evaluated over 10,000 potential cycles using standard triangular potential scan in the lifetime regime. Interestingly, after 10k durability cycles, PtNiCo-16h/C electrocatalyst showed enhanced ORR activity (32% higher activity; Im@10k cycles = 0.716 A mgPt?1) and stability compared to commercial Pt/C signifying the retention of Ni and Co due to higher lattice contraction in PtNiCo alloy electrocatalyst.  相似文献   

15.
The commonly used Pt/C catalyst has low durability for oxygen reduction reaction (ORR). In this work, CNT-supported TiO2 nanoparticles, which synergistically combines the merits of TiO2 (high stability and strong interactions with the supported Pt nanoparticles) and CNT (high specific surface area and large electrical conductivity), are prepared by a sol-gel process coupled with an annealing process and used as the support for Pt nanoparticles, which are anchored around TiO2 nanoparticles by a photodeposition technique. The as-synthesized Pt/TiO2@CNT catalyst exhibits a mass activity 5.3 times as large as that of the commercial Pt/C catalyst (0.358 A mgPt−1 vs. 0.067 A mgPt−1 at 0.9 V) and an excellent stability (no activity loss after 10000 potential cycles) for ORR, which can be mainly attributed to the lower oxygen adsorption energy of Pt, resulting from the strong metal-support interaction induced by the deposition of Pt nanoparticles around the well-dispersed TiO2 nanoparticles on CNT.  相似文献   

16.
Platinum (Pt) is considered as the preferred metal catalyst for methanol oxidation reactions. However, the application prospects of Pt catalysts are limited due to the inherent scarcity and cost. Enabling a trace amount of Pt to exert satisfactory catalytic activity and durability has become a key issue in designing electrocatalysts. Here, Ru-doped PtSn alloy nanoplates (PtSn@Ru NP) with an average particle size of less than 5 nm were controllably synthesized by adjusting the Pt–Sn atomic ratio. Compared with Ru-doped PtSn alloy nanospheres (PtSn@Ru NS/C, 714.7 mA/mgPt), PtSn bimetallic nanoplates (PtSn NP/C, 880.2 mA/mgPt) and commercial Pt/C (299.6 mA/mgPt), the prepared PtSn@Ru NP/C (1105.1 mA/mgPt) exhibited an extraordinary methanol oxidation mass activity. Furthermore, the peak oxidation current retention of PtSn@Ru NP/C was as high as at 87.5% after 1000 accelerated durability tests. The significantly enhanced catalytic performance and durability were attributed to the synergistic effect of the alloy components and morphological advantages. This work has led us to think more deeply about the constitutive relationship between structure and performance.  相似文献   

17.
Factors as the Pt/C ratio of the catalyst, the binder content of the electrode and the catalyst deposition method were studied within the scope of ultra-low Pt loading electrodes for high temperature proton exchange membrane fuel cells (HT-PEMFCs). The Pt/C ratio of the catalyst allowed to tune the thickness of the catalytic layer and so to minimize the detrimental effect of the phosphoric acid flooding. A membrane electrode assembly (MEA) with 0.05 mgPtcm−2 at anode and 0.1 mgPtcm−2 at cathode (0.150 mgPtcm−2 in total) attained a peak power density of 346 mW cm−2. It was proven that including a binder in the catalytic layer of ultra-low Pt loading electrodes lowers its performance. Electrospraying-based MEAs with ultra-low Pt loaded electrodes (0.1 mgPtcm−2) rendered the best (peak power density of 400 mW cm−2) compared to conventional methods (spraying or ultrasonic spraying) but with the penalty of a low catalyst deposition rate.  相似文献   

18.
Developing platinum-based nanoparticles on carbon catalysts with high activity and stability for oxygen reduction reaction (ORR) is of great significance for the practical application of fuel cells. Herein, a synchronous strategy of preparing nano-sized PtCo supported on atomic Co and N co-doped carbon nanorods (PtCo/Co–N–C NR) was developed to replace the conventional method of impregnating Pt sources into ready-made carbon materials, in which metal-organic frameworks (MOFs) with Co and Zn ions of rhombic dodecahedron were first prepared using 2-methylimidazole as building block and then their morphology was transformed into porous nanorods via the reduction of Co ions to Co–B–O complex in the MOFs by NaBH4; subsequently, Pt was deposited on the Co–Zn MOF nanorods through the displacement reaction of PtCl62- and metallic Co and coordination between MOF and PtCl62-; after pyrolysis and acid-leaching process, highly dispersed PtCo/Co–N–C NR was obtained. Attributed to its unique characteristics of hierarchical pore structure, uniform PtCo alloy nanoparticles with the average size of 7.0 nm and strong supporting interaction effect, the catalyst exhibits high ORR activity and stability with the mass activity of 577.0 mA mg?1Pt and specific activity of 1.4 mA cm?2 at 0.9 V vs RHE in 0.1 M HClO4, which is about 3.6 times and 3.5 times high than that of commercial Pt/C catalyst respectively. This strategy would provide a flexible route to develop highly active and stable ORR electrocatalysts with various morphologies for optimizing the exposure of active sites.  相似文献   

19.
Developing the efficient and stable anode catalysts of direct methanol fuel cell has been a pivotal requirement for its extensive commercial application. Herein, we design the Fe-doped CoP nanotube heterostructure as the co-catalyst of Pt-based catalyst via combining a facile hydrothermal with phosphorization process, subsequently, the traditional NaBH4 reduction method is utilized to deposit Pt nanoparticles. As anticipated, Fe species have been successfully doped into CoP to generate the Fe-doped CoP nanotube heterostructure, and the involved characterizations identify that Pt–C/Fe2–CoP catalyst exhibits admirable mass activity (1237 mA·mg−1Pt) towards methanol oxidation reaction, which is approximately 2.04 and 3.66 times as high as the Pt–C/CoP (607 mA·mg−1Pt) and Pt–C–H (338 mA·mg−1Pt). After stability test, the decline ratio of mass activity for Pt–C/Fe2–CoP (83.43%) is markedly preferable to Pt–C/CoP (94.92%) and Pt–C–H (98.67%) catalysts. The enhanced catalytic activity and durability can be imputed to the formation of uniform Pt nanoparticles and co-catalysis effect of Fe-doped CoP nanotube heterostructure since the introduction of hetero-metal cations is able to effectively accelerate the charge transfer rate and adjust the electronic structure of material. Therefore, the fabrication of nanotube heterostructure and introduction of hetero-metal may provide a new direction to the development of other high-efficiency electrocatalysts.  相似文献   

20.
The catalysts for the electrooxidation of liquid fuel in the anodic electrode has severely limited the practical large-scale commercial application of fuel cells, and hence needs to be optimized. Herein, we report a facile one-pot method to successfully synthesize the sub-16 nm dendritic Pt–Cu nanocrystals (PtCu NCs) catalysts under the assistance of ultrasonic. In virtue of such dendritic structure, the alloy and electronic effects between Pt and Cu, such binary PtCu nanodendrites exhibited extremely high electrocatalytic performances towards ethylene glycol (EG) electrooxidation with the mass activity of 4259.2 mA mg?1, 4.5 times higher than that of the commercial Pt/C. Moreover, the Pt1Cu1 nanocatalysts can endure at least 500 cycles with less activity decay, demonstrating a new class of Pt-based electrocatalysts with enhanced performance for fuel cells and beyond.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号