The direct methanol fuel cell is an emerging energy conversion device for which Pt is considered as the state-of-the-art anode catalyst. Herein, we show that the activity and stability of Pt for methanol oxidation can be significantly enhanced using Mo-doped CeO2 (Ce1−xMoxO2−δ) solid solutions as co-catalysts. X-ray photoelectron spectroscopy (XPS) reveals a strong electronic interaction between Ce1−xMoxO2−δ and Pt in Pt/Ce1−xMoxO2−δ–C catalysts. Among all Pt/Ce1−xMoxO2−δ–C catalysts, the catalyst with a Ce/Mo atomic ratio of 7/3 (Pt/Ce0.7Mo0.3O2−δ–C) exhibits the highest activity, up to 1888.4 mA mgPt−1, which is one of the best results reported so far. A direct methanol fuel cell incorporating the Pt/Ce0.7Mo0.3O2−δ–C as the anode catalyst exhibits a maximum power density of 69.4 mW cm−2, which is 1.8 times that of an analogous fuel cell using the commercial Pt/C-JM as the anode catalyst.

•A graphene film on Al is prepared by taking advantage of Al ions dissociated from Al substrate.•Dissociated Al ions act as crosslinkers of graphene oxides, as evidenced by FTIR and XPS.•The graphene coated aluminum shows good corrosion resistance and maintains high conductivity.•A corrosion current of <1 × 10−6 A/cm2 and interfacial contact resistance of <5 mΩ cm2 achieved.•The corrosion current and interfacial contact resistance meets the DOE 2020 targets of bipolar plates.We report in this paper a novel method to form protective graphene film on aluminum substrate, which is particularly applicable to bipolar plates in proton exchange membrane (PEM) fuel cells. By simply immersing an aluminum sheet in an aqueous solution of graphene oxide (GO), a layer of cross-linked GO gel forms on the aluminum sheet, taking advantage of dissociated aluminum ions as a cross-linker. Then the cross-linked GO is converted to graphene at 400 °C in hydrogen atmosphere. The chemistry of the self-assembled GO layer and its conversion to graphene film is revealed by FTIR and XPS. Under simulated fuel cell environment the graphene coated aluminum sheet shows a corrosion current density of <1 × 10−6 A/cm2, which is around four orders of magnitude lower than a bare aluminum sheet. Meanwhile, the graphene film on aluminum results in a much lower and more stable interfacial contact resistance (ICR) of <5 mΩ cm2. These enable the graphene coated aluminum sheet to meet the U.S. DOE targets of 2020 for bipolar plates in terms of both the corrosion and electrical resistance. Thus the proposed method is very promising for protecting aluminum bipolar plates in PEM fuel cells.Download high-res image (271KB)Download full-size image

•3D-NG@SiO2-2-900 is prepared by pyrolyzing POPD, with silica colloid as templates.•The number of graphene layers and the pore diameter of 3D-NG@SiO2 are controllable.•3D-NG@SiO2-2-900 has super ORR catalytic performance and durability in 0.1 M KOH.•High porosity, many planar nitrogen and mass transmission channel benefit the ORR.Three-dimensional nitrogen-doped graphene (3D-NG@SiO2) is prepared by pyrolyzing poly (o-phenylenediamine) (POPD) with high nitrogen content. POPD is prepared via an in situ chemical oxidation polymerization of o-phenylenediamine (OPD) in acetic acid with silica colloid as templates. The optimum parameter is OPD:SiO2 = 1:2, pyrolysis @ 900 °C. SEM and TEM images show the wrinkled and porous graphene structures. Raman spectra indicate that 3D-NG@SiO2 consists of 4–6 layers graphene. N2 adsorption–desorption isotherms reveal that the pore size distributions mainly centralize at 5–10 nm. XRD illustrates the amorphous structure. XPS analysis shows that the nitrogen content is 3.6% and nitrogen mainly exists in the form of pyridinic nitrogen and pyrrolic nitrogen. The oxygen reduction reaction (ORR) performance investigated using a rotating disk electrode shows that the initial potential of 3D-NG@SiO2 is 0.08 V (vs. Hg/HgO). The electron transfer number is 3.92 @ −0.3 V (vs. Hg/HgO), indicating that 3D-NG@SiO2 mainly occurs via a four-electron process. The oxygen reduction current density decreases by 21% after 60 h in the chronoamperometry test. The CVs manifests a current density loss of 0.16 mA cm−2 after scanning for 5000 cycles. The high activity and durability indicate the promising potential of 3D-NG@SiO2 as ORR catalysts.Download high-res image (353KB)Download full-size image

In this work, a simple and facile aqueous solution method was developed for the synthesis of uniform porous Pt–Cu nanocrystals (NCs) supported on 1-aminopyrene functionalized graphene nanoplates (p-Pt–Cu/AP-GNPs), without any high boiling point organic solvents, surfactants, stabilizers and templates. The as-prepared p-Pt–Cu/AP-GNP catalysts exhibit superior electrocatalytic activities and stabilities for methanol oxidation under alkaline conditions compared to Pt/AP-GNPs and Pt/C-JM, and the electrocatalytic performance varies with the relative content of Pt and Cu with the p-Pt1Cu1/AP-GNP catalyst topping all p-Pt–Cu/AP-GNP catalysts studied. This strategy may open a new route to design and prepare superior electrocatalysts for fuel cells.

In the search for alternatives to conventional Pt electrocatalysts, we synthesized a series of graphene nanoplate (GNP)-supported Pt3Cu1 nanocrystals (NCs), possessing almost the same composition but different morphologies to probe their electrochemical properties as a function of morphology for the ethanol oxidation reaction. The morphology of the Pt3Cu1 catalysts could be systematically evolved from dendritic (D-Pt3Cu1/GNPs) to wire-like (W-Pt3Cu1/GNPs) and spherical (Pt3Cu1/GNPs) by only varying pH of the reaction solution. The as-prepared Pt3Cu1 catalysts were subsequently characterized using a suite of techniques including transmission electron microscopy (TEM), selected area electron diffraction (SAED), X-ray diffraction (XRD), inductively coupled plasma mass spectrometry (ICP-MS) and X-ray photoelectron spectroscopy (XPS) to verify not only their morphologies and chemical compositions but also the incorporation of Cu into the Pt lattice, as well as physical structure and integrity. Gratifyingly, the three Pt3Cu1 catalysts exhibited superior electrocatalytic properties for the ethanol oxidation compared to the monometallic Pt/GNPs and Pt/C-JM (Johnson Matthey), with the activities, durabilities and anti-poisonous abilities following the order Pt3Cu1/GNPs < W-Pt3Cu1/GNPs < D-Pt3Cu1/GNPs.

•A post treatment affords the SPEEK membrane with gradient crosslinking structure.•Benzhydrol and sulfonic acid combine to form the crosslinks, evidenced by NMR, FTIR.•Such structure restrains the membrane from over swelling, enhances tensile strength.•The membrane shows high conductivity and low activation energy, comparable to Nafion.•H2/O2 fuel cell with the post treated membrane shows good performance at 80 °C.Polymer electrolyte membranes in fuel cells should be high in both ionic conductivity and mechanical strength. However, the two are often exclusive to each other. To solve this conundrum, a novel strategy is proposed in this paper, with extensively researched sulfonated poly (ether ether ketone) (SPEEK) membrane as a paradigm. A SPEEK membrane of high sulfonation degree is simply post-treated with NaBH4 and H2SO4 solution at ambient temperature for a certain time to afford the membrane with a gradient crosslinking structure. Measurements via 1H NMR, ATR-FTIR and SEM-EDS are conducted to verify such structural changes. The gradient crosslinks make practically no damage to proton conductance, but effectively restrain the membrane from over swelling and greatly enhance its tensile strength. A H2–O2 fuel cell with the gradiently crosslinked SPEEK membrane shows a maximal power density of 533 mW cm−2 at 80 °C, whereas the fuel cell with the pristine SPEEK membrane cannot be operated beyond 30 °C.

In this paper, we present a simple and facile strategy to prepare highly uniform Pd–Pt alloy nanoparticles (NPs) with different Pt/Pd molar ratios on 1-pyrenecarboxylic acid (PCA) decorated graphite nanoplatelets (GNPs). The binary composition of these Pd–Pt/GNPs catalysts is controlled by simply adjusting the molar ratio of the Pd and Pt precursors. The obtained catalysts were characterized by ultraviolet-visible light (UV-vis) spectroscopy, Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma optical emission spectrometry (ICP-OES). The HRTEM measurements show that all of the metallic NPs exhibit well-defined crystalline structures. Both cyclic voltammetry (CV) and chronoamperometry (CA) demonstrate that the Pd1Pt3/GNPs catalyst has the highest catalytic activity towards methanol oxidation reaction (MOR) among the Pd–Pt/GNPs with different compositions studied. Moreover, the Pd1Pt3/GNPs catalyst markedly outperforms Pt/GNPs and the commercial Pt/C-JM catalyst in terms of both MOR activity and stability. The present method represents a simple and general approach to synthesizing bimetallic Pt-M electrocatalysts on an alternative carbon support, which is expected to find applications in fuel cells.

A series of high loading Pt nanoparticles (NPs) with a small particle size uniformly dispersed on graphite nanoplatelets (GNPs) have been synthesized in the presence of an imidazolium-based ionic liquid (Pt/I-IL (x)/GNPs). I-IL, an amphoteric ion used as an additive agent to stabilize Pt NPs, can also prevent the aggregation of the GNPs. The results obtained from X-ray diffraction, transmission electron microscopy and electrochemical testing showed that the I-IL assisted synthesis method resulted in size reduction of Pt NPs, an improvement of Pt dispersion on GNPs, and the identification of the relationships between the mean size of Pt NPs and the volume of I-IL. Among all as-prepared Pt/GNP catalysts with or without I-IL assisted, the sample with 10 microliters of I-IL assisted (Pt/I-IL (10)/GNPs) exhibits the highest electrocatalytic activity and the best stability toward the methanol oxidation reaction. Moreover, the Pt/I-IL (10)/GNP catalyst markedly outperforms the commercial Pt/C from Johnson Matthey in terms of both methanol oxidation activity and stability, revealed by cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy.

A novel electrocatalyst of heteroatom-doped carbon (HDC) has been developed via facile pyrolysis of hen egg yolk without incorporating external heteroatoms. This HDC showed a high electrocatalytic activity towards oxygen reduction/evolution reactions in alkaline media, which indicates that it might be a very promising alternative to costly Pt-based electrocatalysts.

With the aim to improve the conductivity of proton exchange membranes (PEMs), an external AC electric field is applied to a sulfonated poly (ether ether ketone) (SPEEK)-titanium (IV) oxide (TiO2) hybrid casting solution during solvent evaporation. Present technique gives a potentially useful method to fabricate PEMs with oriented proton channels, and resulting in increased conductivity by 75% in the trans-plane direction versus normal methods. In addition, reciprocation of TiO2 under the AC electric field prevents the nanoparticles from aggregating and improves mechanical strength of the PEMs. Factors affect the proton channels' alignment degree such as the applied field magnitude and frequency are also investigated.Graphical abstractTiO2 particles line up under an electrical field with sulfonate groups attached.Highlights► A inorganic–organic hybrid PEM with uniformly distributed TiO2 particles is obtained. ► An external electric field leads to orientation of proton channels in the PEM. ► Such orientation results in TiO2/SPEEK hybrid membranes of improved conductivity. ► Mechanical strength of the electric field treated PEM has also been improved.

A Nafion membrane with enhanced performance has been prepared by using a novel casting solution containing low-polarity nonsolvent tetrachloroethylene (TCE). TCE induces self-organization of the ionomer and turns the originally transparent Nafion in dimethylformamide (DMF) solution into opaque. The Nafion membrane cast from such opaque solution remains mechanically robust and shows a proton conductivity of 0.07 S cm−1 at room temperature, and 0.21 S cm−1 at 80 °C under saturated humidity, which is an increase of 62% and 103% respectively over the membrane without TCE involvement. Besides, water content and water permeability of the new membrane become higher. The enhanced membrane performance is attributed to larger clusters of sulfonate groups in Nafion, which is revealed by small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM).Graphical abstractHighlights► Nonsolvent tetrachloroethylene leads to self-organization of ionomer in casting solution. ► Such casting solution results in Nafion membranes with greatly improved proton conductivity. ► Higher water content and water permeability of the membrane were also observed. ► The membranes were mechanically robust despite of polymer aggregation in casting solution. ► Larger clusters of sulfonate groups in the membranes were detected via SAXS and TEM.

•Non-solvent CCl4 leads to phase separation of the casting solution of Nafion.•Electric field treatment to the solution leads to improved proton conductivity.•Proton channels of the PEM are oriented in the trans-plane direction.•The PEMs are mechanically robust despite of phase separation in casting solution.•It is suggested that the non-solvent induced phase separation is a deciding factor.A novel solution casting method of membrane preparation is explored to improve the conductivity of proton exchange membranes (PEMs). A high voltage alternative electric field is applied to a heterogeneous Nafion solution while evaporating the solvents, leaving aligned proton channels in the solidified membrane, and SAXS and WAXS have been given as direct evidences. Therefore, the trans-plane conductivity of the PEM is increased. A Non-solvent of low polarity carbon tetrachloride (CCl4) causes phase separation in the casting solution, which facilitates the Nafion ionomer to respond to the applied electric field. Despite the severe phase separation in the casting solution, the resultant electro-casting membrane shows a higher mechanical strength than that of the normal recast Nafion membrane.

•Highly uniform Pt nanoparticles were deposited on graphite nanoplatelets.•Graphitic structure of the support was preserved to improve the catalyst durability.•The catalyst has a high ORR activity and CO tolerance.•The impact of decorating agent on the Pt deposition was investigated.Graphite nanoplatelets (GNPs), which consist of layers of graphene, are an ideal electrocatalyst support due to their high electrical and thermal conductivity, excellent chemical stability, and easy availability. However, GNPs are somewhat chemically inert, which makes the even deposition of catalytic metal nanoparticles on their surface difficult. In this paper, we present a facile method to prepare highly uniform Pt nanoparticles on GNPs, which are decorated with 1-pyrenecarboxylic acid (PCA). When the hydrophobic pyrene group of the PCA is adsorbed on the surface of GNPs via π–π interaction, its carboxylic group can serve as an anchor for the Pt deposition. This decoration facilitates a narrow size profile, which is centered at approximately 2–3 nm, and an even spatial distribution on the GNPs surface for the Pt nanoparticles. The resultant Pt/GNPs catalyst exhibits a noticeably higher durability and electrochemical activity than the commonly used Pt/C catalyst and is therefore a promising cathodic catalyst for proton exchange membrane fuel cells.

A lattice model of catalyst layer in proton exchange membrane fuel cells (PEMFCs), consisting of randomly distributed catalyst phase (C phase) and mixed ionomer-pore phase (IP phase), was established by means of Monte Carlo method. Transport and electrochemical reactions in the model catalyst layer were calculated. The newly proposed C-IP model was compared with previously established pore-solid two phase model. The variation of oxygen level and reaction rate along the thickness of catalyst layer with cell current was discussed. The effect of ionomer distribution across catalyst layer was studied by comparing profiles of oxygen level, reaction rate and overpotential, as well as corresponding polarization curves.Highlights► We propose a novel two phase lattice model of catalyst layer in PEMFC. ► The model features a catalyst phase and a mixed ionomer and pores phase. ► Transport and electrochemical reaction in the lattice are simulated. ► The model enables more accurate results than pore-solid two phase model. ► Profiles of oxygen level and reaction rate across catalyst layer vary with cell current.

A lattice model of the nanoscaled catalyst layer structure in proton exchange membrane fuel cells (PEMFC) was established by Monte Carlo method. The model takes into account all the four components in a typical PEMFC catalyst layer: platinum (Pt), carbon, ionomer and pore. The elemental voxels in the lattice were set fine enough so that each average sized Pt particulate in Pt/C catalyst can be represented. Catalyst utilization in the modeled catalyst layer was calculated by counting up the number of facets of Pt voxels where “three phase contact” are met. The effects of some factors, including porosity, ionomer content, Pt/C particle size and Pt weight percentage in the Pt/C catalyst, on catalyst utilization were investigated and discussed.

Sulfonated poly(ether ether ketone) (SPEEK) was blended with poly(ether sulfone) (PES) to make solid polymer electrolyte (SPE) membranes for hydrogen production via water electrolysis. The blend membranes were characterized in terms of proton conductivity and the swelling degree in water. Membrane electrode assemblies (MEA), with Ir anode and Pt cathode at the two side of the blended membrane, were prepared by a decal method. The effect of hot pressing conditions in fabricating the MEA and the influence of ionomers in the catalyst layers were investigated. The MEA, with an effective area of 4 cm2, were tested using a single cell water electrolysis test stand. An electrolytic current of 1655 mA/cm2 were obtained at 2 V and 80 °C with the SPEEK based MEA and under suitable fabrication conditions. The experimental results suggest that SPEEK/PES blend membrane could be an alternative to costly perfluorosulfonate membranes in SPE water electrolysis for hydrogen production.

A steady-state numerical model for multi-ion parallel-plate electrode (PPE) system is developed to investigate the concentration and electric distribution in the process of salt water electrolysis under forced convection. The finite-element method is used to solve this multi-ion transport model coupled with ionic diffusion, convection and ionic migration. The flow field and the electrode current's effect on the concentration distribution are investigated. The comparison between the diffusion-transported current and the migration-transported current demonstrates that the current is almost fully transported by the ionic migration, with the result that the diffusion-transported current can be neglected and the control equation of potential is simplified. For comparison, a hypothetical model with uncoupled situation of concentration and electric field is taken into consideration. The variation of electric field strength near the cathode can reach 25% of the value of the uncoupled model in the condition of u0 = 0.01 m/s. Compared with this, the variation of ionic electro-conductivity shows a reverse tendency.

The performance of the polymer electrolyte membrane fuel cell (PEMFC) is greatly controlled by the structure of the catalyst layer. Low catalyst utilization is still a significant obstacle to the commercialization of the PEMFC. In order to get a fundamental understanding of the electrode structure and to find the limiting factor in the low catalyst utilization, it is necessary to develop the mechanical model on the effect of catalyst layer structure on the catalyst utilization and the performance of the PEMFC. In this work, the structure of the catalyst layer is studied based on the lattice model with the Monte Carlo simulation. The model can predict the effects of some catalyst layer components, such as Pt/C catalyst, electrolyte and gas pores, on the utilization of the catalyst and the cell performance. The simulation result shows that the aggregation of conduction grains can greatly affect the degree of catalyst utilization. The better the dispersion of the conduction grains, the larger the total effective area of the catalyst is. To achieve higher utilization, catalyst layer components must be distributed by means of engineered design, which can prevent aggregation.

A new kind of inorganic–organic composite membranes based on sulfonated polyethersulfone Cardo (SPES-C) with embedded phosphotungstic acid (PWA) was prepared. The composite membranes were characterized by using FT-IR, XRD, TGA and SEM techniques. FT-IR and XRD measurements confirmed the presence of PWA particles into the polymer matrix. FT-IR spectra indicated the existence of a specific interaction between PWA particles and SPES-C polymer. TGA results showed that the composite membranes were thermally stable up to approximately about 200 °C. SEM micrographs verified that nano-scale PWA particles were homogeneously distributed into the polymer matrix. By incorporation PWA into SPES-C polymer the proton conductivity of the composite membranes was enhanced. It was 4.5 × 10−2 S cm−1 at 90 °C and 6.7 × 10−2 S cm−1 at 110 °C, while the conductivity of Nafion® 115 membrane was 4.1 × 10−2 S cm−1 and 4.7 × 10−2 S cm−1 at 90 °C and 110 °C, respectively.

A novel anion exchange membrane, quaternized polyethersulfone Cardo, was prepared. Polyethersulfone Cardo was chloromethylated with the complex solution of chloromethylether and chloride zinc. Subsequent reaction with trimethylamine and ion exchange with sodium hydroxide yields alkaline anion exchange membrane. The quaternized polyethersulfone Cardo (QPES-C) membrane may be suitable for use in low temperature direct methanol alkaline fuel cells. Ionic conductivity and methanol permeability of such membrane as a function of temperature were investigated. Ionic conductivity of QPES-C membrane in 1 M NaOH solution was 4.1 × 10−2 S/cm at room temperature and 9.2 × 10−2 S/cm at 70 °C. Methanol permeability of QPES-C membrane was from 5.72 × 10−8 to 1.23 × 10−7 cm2/s over the temperature range 25–70 °C.

Sulfonated poly(ether ether ketone) (SPEEK) membranes with various degrees of sulfonation (DS) were prepared. Their proton conductivity and methanol permeability as a function of temperature were investigated. It was found that the proton conductivity of SPEEK membranes exceeded 10−2 S/cm above 80 °C, which is close to that of Nafion® 115 membrane under the same condition. The methanol permeability of SPEEK membranes was about an order of magnitude lower than that of Nafion® 115 membrane. The direct methanol fuel cell (DMFC) performance of the SPEEK membranes was better than that of Nafion® 115 membrane at 80 °C.

•Layered double hydroxides delaminated via nature-inspired temperature shock method.•The temperature shock consists of freezing in liquid N2 and melting in hot water.•The method involves no conventionally employed organic solvents and sonication.•Monolayered nanosheets with large lateral size obtained, evidenced by XRD, dynamic light scattering and AFM.Inspired by the natural frost weathering of rocks and minerals, layered double hydroxides (LDHs) were delaminated by a facile temperature shock method, without the usual involvement of organic solvents and sonication. The temperature shock was carried out with cycles of freezing the LDH solution in liquid nitrogen and subsequent melting the frozen solution in a 80 °C water bath. Around 67% LDHs were delaminated into nanosheets after 16 such cycles. Moreover, the LDH monolayers thus obtained retain their lateral size at least three times better than that prepared in formamide under sonication. The present work provides a green and general approach to obtain high quality LDH nanosheets, which are finding application across a wide spectrum of areas.

In this work, a simple and facile aqueous solution method was developed for the synthesis of uniform porous Pt–Cu nanocrystals (NCs) supported on 1-aminopyrene functionalized graphene nanoplates (p-Pt–Cu/AP-GNPs), without any high boiling point organic solvents, surfactants, stabilizers and templates. The as-prepared p-Pt–Cu/AP-GNP catalysts exhibit superior electrocatalytic activities and stabilities for methanol oxidation under alkaline conditions compared to Pt/AP-GNPs and Pt/C-JM, and the electrocatalytic performance varies with the relative content of Pt and Cu with the p-Pt1Cu1/AP-GNP catalyst topping all p-Pt–Cu/AP-GNP catalysts studied. This strategy may open a new route to design and prepare superior electrocatalysts for fuel cells.

The direct methanol fuel cell is an emerging energy conversion device for which Pt is considered as the state-of-the-art anode catalyst. Herein, we show that the activity and stability of Pt for methanol oxidation can be significantly enhanced using Mo-doped CeO2 (Ce1−xMoxO2−δ) solid solutions as co-catalysts. X-ray photoelectron spectroscopy (XPS) reveals a strong electronic interaction between Ce1−xMoxO2−δ and Pt in Pt/Ce1−xMoxO2−δ–C catalysts. Among all Pt/Ce1−xMoxO2−δ–C catalysts, the catalyst with a Ce/Mo atomic ratio of 7/3 (Pt/Ce0.7Mo0.3O2−δ–C) exhibits the highest activity, up to 1888.4 mA mgPt−1, which is one of the best results reported so far. A direct methanol fuel cell incorporating the Pt/Ce0.7Mo0.3O2−δ–C as the anode catalyst exhibits a maximum power density of 69.4 mW cm−2, which is 1.8 times that of an analogous fuel cell using the commercial Pt/C-JM as the anode catalyst.

In this paper, we present a simple and facile strategy to prepare highly uniform Pd–Pt alloy nanoparticles (NPs) with different Pt/Pd molar ratios on 1-pyrenecarboxylic acid (PCA) decorated graphite nanoplatelets (GNPs). The binary composition of these Pd–Pt/GNPs catalysts is controlled by simply adjusting the molar ratio of the Pd and Pt precursors. The obtained catalysts were characterized by ultraviolet-visible light (UV-vis) spectroscopy, Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma optical emission spectrometry (ICP-OES). The HRTEM measurements show that all of the metallic NPs exhibit well-defined crystalline structures. Both cyclic voltammetry (CV) and chronoamperometry (CA) demonstrate that the Pd1Pt3/GNPs catalyst has the highest catalytic activity towards methanol oxidation reaction (MOR) among the Pd–Pt/GNPs with different compositions studied. Moreover, the Pd1Pt3/GNPs catalyst markedly outperforms Pt/GNPs and the commercial Pt/C-JM catalyst in terms of both MOR activity and stability. The present method represents a simple and general approach to synthesizing bimetallic Pt-M electrocatalysts on an alternative carbon support, which is expected to find applications in fuel cells.