Precision tuning of highly efficient Pt-based ternary alloys on nitrogen-doped multi-wall carbon nanotubes for methanol oxidation reaction

The electrochemical methanol oxidation is a crucial reaction in the conversion of renewable energy.To enable the widespread adoption of direct methanol fuel cells(DMFCs),it is essential to create and engineer catalysts that are both highly effective and robust for conducting the methanol oxidation reaction(MOR).In this work,trimetallic PtCoRu electrocatalysts on nitrogen-doped carbon and multi-wall carbon nanotubes(PtCoRu@NC/MWCNTs)were prepared through a two-pot synthetic strategy.The acceleration of CO oxidation to CO_(2) and the blocking of CO reduction on adjacent Pt active sites were attributed to the crucial role played by cobalt atoms in the as-prepared electrocatalysts.The precise control of Co atoms loading was achieved through precursor stoichiometry.Various physicochemical techniques were employed to analyze the morphology,element composition,and electronic state of the catalyst.Electrochemical investigations and theoretical calculations confirmed that the Pt_(1)Co_(3)Ru_(1)@NC/MWCNTs exhibit excellent electrocatalytic performance and durability for the process of MOR.The enhanced MOR activity can be attributed to the synergistic effect between the multiple elements resulting from precisely controlled Co loading content on surface of the electrocatalyst,which facilitates efficient charge transfer.This interaction between the multiple components also modifies the electronic structures of active sites,thereby promoting the conversion of intermediates and accelerating the MOR process.Thus,achieving precise control over Co loading in PtCoRu@NC/MWCNTs would enable the development of high-performance catalysts for DMFCs.

Hierarchically skeletal multi-layered Pt-Ni nanocrystals for highly efficient oxygen reduction and methanol oxidation reactions

Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.

Rational design ternary platinum based electrocatalysts for effective methanol oxidation reaction

Exploring effective, durable, and affordable electrocatalysts of methanol oxidation reaction(MOR) is of vital significance for the industrial application of direct methanol fuel cells. Herein, an efficient, general,and expandable method is developed to synthesis two-dimensional(2D) ternary Pt Bi M nanoplates(NPLs), in which various M(Co, Ni, Cu, Zn, Sn) is severed as the third component to the binary Pt Bi system. The MOR performance of Pt Bi M NPLs is entirely investigated, demonstrating that both the MOR activity and durability is enhanced with the introduction of the additional composition. Pt3Bi3Zn NPLs shows much higher MOR activity and stability than that of the Pt Bi counterparts, not to mention the current advanced Pt Ru/C and Pt/C catalysts. The prominent performances are attributed to the modulated electronic structure of the surface Pt in Pt Bi NPLs by the addition of Zn, resulting in a weakened affination between Pt and the adsorbed poisoning species(mainly CO) compared with Pt Bi NPLs, verified by density functional theory(DFT) calculations. In addition, the absorbed OH can be generated on the surface of Zn atom due to its favorable water activation properties, thus the CO removal on the adjacent Pt atoms is accelerated, further leading to a high activity and anti-poisoning performance of the resulting Pt_(3)Bi_(3)Zn catalyst. This work provides new insights and robust strategy for highly efficient MOR electrocatalyst with extraordinary anti-poisoning performance and stability.

Surface elemental distribution effect of Pt-Pb hexagonal nanoplates for electrocatalytic methanol oxidation reaction

Bimetallic Pt-based catalysts have been extensively investigated to enhance the performance of direct methanol fuel cells(DMFCs) because CO, a by-product, reduces the activity of the pure Pt catalysts. Herein, we synthesized Pt-Pb hexagonal nanoplates as a model catalyst for the methanol oxidation reaction(MOR) and further controlled the Pt and Pb distributions on the surface of the nanoplates through acetic acid(HAc) treatment. As a result, we obtained Pt-Pb nanoplates and HAc-treated Pt-Pb nanoplates with homogeneous and heterogeneous distributions of the Pt-Pb alloy surfaces, respectively. We showed that the MOR activity and stability of the Pt-Pb nanoplates improved compared to those of the HAc-treated Pt-Pb nanoplates, mainly due to the enhanced CO tolerance and the modified electronic structure of Pt under the influence of the oxophilic Pb.

Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction

Noble metal-based electrocatalysts present high activities for methanol oxidation reaction(MOR),but are limited by their high cost,low stability and poor resistance to carbon monoxide(CO) poisoning.The development of active and stable non-noble metal electrocatalysts for MOR is desired,but remains a challenge.Herein,we report a simple strategy to make copper nanocrystal/nitrogen-doped carbon(Cu/N-C)monoliths,which can serve as active and robust electrodes for MOR.Copper nanocrystals were electrochemically deposited onto a conductive polyaniline hydrogel and calcined to form Cu/N-C monolith,where the active copper nanocrystals are protected by nitrogen-doped carbon.Owing to their extremely high electrical conductivity(1.25 × 10^(5) S cm^(-1)) and mechanical robustness,these Cu/N-C monoliths can be directly used as electrodes for MOR,without using substrates or additives.The optimal Cu/N-C(FT)@500 monolith shows a high MOR activity of 189 mA cm^(-2) at 0.6 V vs.SCE in alkaline methanol solution,superior to most of reported Cu-based MOR catalysts.Cu/N-C(FT)@500 also presents a better stability than Pt/C catalyst in the long-term MOR test at high current densities.Upon carbon monoxide(CO) poisoning,Cu/N-C(FT)@500 retains 96% of its MOR activity,far exceeding the performance of Pt/C catalyst(61% retention).Owing to its facile synthesis,outstanding activity,high stability and mechanical robustness,Cu/N-C(FT)@500 monolith is promising as a low-cost,efficient and CO-resistant electrocatalyst for MOR.

A rational design of bimetallic PdAu nanoflowers as efficient catalysts for methanol oxidation reaction

Methanol fuel cells have been intensively developed as clean and high-efficiency energy conversion system due to their high efficiency and low emission of pollutants.Here,we developed a simple aqueous synthetic method to prepare bimetallic PdAu nanoflowers catalysts for methanol oxidation reaction(MOR)in alkaline environment.Their composition can be directly tuned by changing the ratio between Pd and Au precursors.Compared with commercial Pd/C catalyst,all of the PdAu nanoflowers catalysts show the enhanced catalytic activity and durability.In particular,the PdAu nanoflowers specific activity reached 0.72 mA/cm^(2),which is 14 times that of commercial Pd/C catalyst.The superior MOR activity could be attributed to the unique porous structure and the shift of the d-band center of Pd.

Greatly Enhanced Methanol Oxidation Reaction of CoPt Truncated Octahedral Nanoparticles by External Magnetic Fields

Tunable behavior in electrocatalysis by external multifields,such as magnetic field,thermal field,and electric field,is the most promising strategy to expand the theory,design,and synthesis of state-of-the-art catalysts and the cell in the near future.Here,a systematic investigation for the effect of external magnetic field and thermal field on methanol oxidation reactions(MOR)in magnetic nanoparticles is reported.For Co_(42)Pt_(58)truncated octahedral nanoparticles(TONPs),the catalytic performance in MOR is greatly increased to the maximum of 14.1%by applying a magnetic field up to 3000 Oe,and it shows a monotonical increase with increasing working temperature.The magnetic enhanced effect is closely related to the Co content of Co_(x)Pt_(100-x)TONPs.Furthermore,the enhancement effect under a magnetic field is more obvious for Co_(42)Pt_(58)TONPs annealed at 650℃.First-principle calculation points out that the magnetic fields can facilitate the dehydrogenation of both methanol and water by suppression of entropy of the electron spin and lowering of the activation barrier,where OH_(ad)intermediates on Co sites play a more important role.The application of magnetic fields together with thermal fields in MOR provides a new prospect to manipulate the performance of direct methanol fuel cells,which will accelerate their potential applications.

Recent development of Au arched Pt nanomaterials as promising electrocatalysts for methanol oxidation reaction

The recent development of Aurum(Au)introduced Platinum(Pt)based nanomaterials is of great significance to direct methanol fuel cell as electrocatalysts for anode reactions,due to its stability and anti-poisoning features.Therefore,the performance of PtAu based catalysts with different elements,atomic ratio,and morphology was studied in methanol solution to further improve its electrocatalytic activity.Furthermore,the effects of Au have aroused the researchers'attention in Pt-based nanocatalysts.In this review,we summarize the controllable synthesis,mechanism,and catalytic performance of Au introduced Pt-based electrocatalysts such as PtAu core-shell nanostructures,PtAu dendrite,PtAu nanowires,self-supporting Au@Pt NPs,and Au@Pt star-like nanocrystals for the methanol oxidation reaction.Finally,the challenges and research directions for the future development of PtAu based catalysts are provided.

Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-Functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation

Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.

Phosphorus-doping-tuned PtNi concave nanocubes with high-index facets for enhanced methanol oxidation reaction

Surface engineering has been found to be an efficient strategy to boost the catalytic performance of noble-metal-based nanocatalysts.In this work,a small amount of P was doped to the surface of PtNi concave cube(P-PtNi CNC).Interestingly,the P-PtNi CNC nanocatalyst shows an enhanced methanol oxidation reaction(MOR)performance with achieving 8.19 times of specific activity than that of comercial Pt/C.The electrochemical in situ Fourier transform infrared spectroscopy(FTIR)results reveal that the surface P doping promotes the adsorption energy of OH,enhancing the resistance against CO poisoning.Therefore,the intermediate adsorbed CO(COads)reacted with adsorbed OH(OHads)through the Langmuir–Hinshelwood(LH)mechanism to generate CO_(2)and release surface active sites for further adsorption.This work provides a promising strategy via the incorporation of non-metallic elements into the PtNi alloys bounded with high-index facets(HIFs)as efficient fuel cell catalysts.

Au nanowires with high aspect ratio and atomic shell of Pt-Ru alloy for enhanced methanol oxidation reaction

The methanol oxidation reaction(MOR)is the limiting half-reaction in direct methanol fuel cell(DMFC).Although Pt is the most active single-metal electrocatalyst for MOR,it is hampered by high cost and CO poisoning.Constructing a Pt or Ru monolayer on a second metal substrate by means of galvanic replacement of underpotentially deposited(UPD)Cu monolayer has been shown as an efficient catalyst design strategy for the electrocatalysis of MOR because of the presumed 100%utilization of atoms and resistance to CO poisoning.Herein,we prepared one-dimensional surface-alloyed electrocatalyst from predominantly(111)faceted Au nanowires with high aspect ratio as the substrate of under-potential deposition.The electrocatalyst comprises a core of the Au nanowire and a shell of catalytically active Pt coated by Ru.Coverage-dependent electro-catalytic activity and stability is demonstrated on the Pt/Ru submonolayers on Au wires for MOR.Among all these catalysts,Au@Pt_(ML)@Ru_(ML)exhibits the best electrocatalytic activity and poisoning tolerance to CO.This presents a viable method for the rational catalyst design for achieving high noble-metal utilization efficiency and high catalytic performance.

Autocatalytic reduction-assisted synthesis of segmented porous PtTe nanochains for enhancing methanol oxidation reaction

Morphology engineering has been developed as one of the most widely used strategies for improving the performance of electrocatalysts.However,the harsh reaction conditions and cumbersome reaction steps during the nanomaterials synthesis still limit their industrial applications.Herein,one-dimensional(1D)novel-segmented PtTe porous nanochains(PNCs)were successfully synthesized by the template methods assisted by Pt autocatalytic reduction.The PtTe PNCs consist of consecutive mesoporous architectures that provide a large electrochemical surface area(ECSA)and abundant active sites to enhance methanol oxidation reaction(MOR).Furthermore,1D nanostructure as a robust sustaining frame can maintain a high mass/charge transfer rate in a long-term durability test.After 2,000 cyclic voltammetry(CV)cycles,the ECSA value of PtTe PNCs remained as high as 44.47 m^(2)·gPt^(-1),which was much larger than that of commercial Pt/C(3.95 m^(2)·gPt^(-1)).The high catalytic activity and durability of PtTe PNCs are also supported by CO stripping test and density functional theory calculation.This autocatalytic reduction-assisted synthesis provides new insights for designing efficient low-dimensional nanocatalysts.

Ultrafine Pt nanoparticles supported on double-shelled C/TiO2 hollow spheres material as highly efficient methanol oxidation catalysts

Catalyst support is extremely important for future fuel cell devices.In this work,we developed doubleshelled C/TiO2(DSCT)hollow spheres as an excellent catalyst support via a template-directed method.The combination of hollow structure,TiO2 shell and carbon layer results in excellent electron conductivity,electrocatalytic activity,and chemical stability.These uniformed DSCT hollow spheres are used as catalyst support to synthesize Pt/DSCT hollow spheres electrocatalyst.The resulting Pt/DSCT hollow spheres exhibited high catalytic performance with a current density of 462 mA mg^-1 for methanol oxidation reaction,which is 2.52 times higher than that of the commercial Pt/C.Furthermore,the increased tolerance to carbonaceous poisoning with a higher If/Ibratio and a better long-term stability in acid media suggests that the DSCT hollow sphere is a promising C/TiO2-based catalyst support for direct methanol fuel cells applications.

Preparation of Surfactant-Free Pt and PtRu Nanoparticles with High Activity for Methanol Oxidation

A simple and green approach to synthesize highly active electro-catalysts for methanol oxi- dation reaction （MOR） without using any organic agents is described. Pt nanoparticles are directly deposited on the pre-cleaned and pre-oxidized multiwall carbon nanotubes （MWC- NTs） from Pt salt by using CO as the reductant. MOR activity has been characterized by both cyclic voltammetry and chronoamperometry, the current density and mass specific current at the peak potential （ca. 0.9 V vs. RHE） reaches 11.6 mA/cm^2 and 860 mA/mgpt, respectively. After electro-deposition of Ru onto the Pt/MWCNTs surface, the catalysts show steady state mass specific current of 20 and 80 mA/mgpt at 0.5 and 0.6 V, respectively.

Advanced heterostructure of Pd nanosheets@Pt nanoparticles boosts methanol electrooxidation

Heterostructures have emerged as elaborate structures to improve catalytic activity owing to their combined surface and distinct inverse interface.However,fabricating advanced nanocatalysts with facetdependent interface remains an unexploited and promising area.Herein,we render the controlled growth of Pt nanoparticles(NPs)on Pd nanosheets(NSs)by regulating the reduction kinetics of Pt^(2+)with solvents.Specifically,the fast reduction kinetic makes the Pt NPs uniformly deposited on the Pd NSs(U-Pd@Pt HS),while the slow reduction kinetic leads to the preferential growth of Pt NPs on the edge of the Pd NSs(E-Pd@Pt HS).Density functional theory calculations demonstrate that Pd(111)-Pt interface in U-Pd@Pt HS induces the electron-deficient status of Pd substrates,triggering the d-band center downshift and amplifying the Pd-Pt intermetallic interaction.The synergy between the electronic effect and interfacial effect facilitates the removal of poisonous intermediates on U-Pd@Pt HS.By virtue of the Pd NSs@Pt NPs interface,the heterostructure achieves exceptional methanol oxidation reaction activity as well as improved durability.This study innovatively proposes heterostructure engineering with facetdependent interfacial modulation,offering instructive guidelines for the rational design of versatile heterocatalysts.

Stable NiPt-Mo_(2)C active site pairs enable boosted water splitting and direct methanol fuel cell

Sluggish kinetics of methanol oxidation reaction(MOR)and alkaline hydrogen evolution reaction(HER)even on precious Pt catalyst impede the large-scale commercialization of direct methanol fuel cell(DMFC)and water electrolysis technologies.Since both of MOR and alkaline HER are related to water dissociation reaction(WDR),it is reasonable to invite secondary active sites toward WDR to pair with Pt for boosted MOR and alkaline HER activity on Pt.Mo_(2)C and Ni species are therefore employed to engineer NiPt-Mo_(2)C active site pairs,which can be encapsulated in carbon cages,via an in-situ self-confinement strategy.Mass activity of Pt in NiPt-Mo_(2)C@C toward HER is boosted to11.3 A mg_(pt)^(-1),33 times higher than that of Pt/C.Similarly,MOR catalytic activity of Pt in NiPt-Mo_(2)C@C is also improved by 10.5 times and the DMFC maximum power density is hence improved by 9-fold.By considering the great stability,NiPt-Mo_(2)C@C exhibits great practical application potential in DMFCs and water electrolysers.

Small-sized tungsten nitride anchoring into a 3D CNT- rGO framework as a superior bifunctional catalyst for the methanol oxidation and oxygen reduction reactions

The application of direct methanol fuel cells （DMFC） is hampered by high cost, low activity, and poor CO tolerance by the Pt catalyst. Herein, we designed a fancy 3D hybrid by anchoring tungsten nitride （WN） nanoparticles （NPs）, of about 3 nm in size, into a 3D carbon nanotube-reduced graphene oxide framework （CNT-rGO） using an assembly route. After depositing Pt, the contacted and strongly coupled Pt-WN NPs were formed, resulting in electron transfer from Pt to WN. The 3D Pt-WN/CNT-rGO hybrid can be used as a bifunctional electrocatalyst for both methanol oxidation reaction （MOR） and oxygen reduction reaction （ORR）. In MOR, the catalysts showed excellent CO tolerance and a high mass activity of 702.4 mA.mgpt-1, 2.44 and 3.81 times higher than those of Pt/CNT-rGO and Pt/C（JM） catalysts, respectively. The catalyst also exhibited a more positive onset potential （1.03 V）, higher mass activity （151.3 mA.mgpt-1）, and better cyclic stability and tolerance in MOR than ORR. The catalyst mainly exhibited a 4e-transfer mechanism with a low peroxide yield. The high activity was closely related to hybrid structure. That is, the 3D framework provided a favorable path for mass-transfer, the CNT-rGO support was favorable for charge transfer, and strongly coupled Pt-WN can enhance the catalytic activity and CO-tolerance of Pt. Pt-WN/CNT-rGO represents a new 3D catalytic platform that is promising as an electrocatalyst for DMFC because it can catalyze both ORR and MOR in an acidic medium with good stability and highly efficient Pt utilization.

Unraveling the role of NiSnPH@OOH/CC perovskite hydroxide for efficient electrocatalytic oxidation of methanol to formate

The sluggish kinetics of oxygen evolution reaction(OER)is the key tailback for hydrogen production from the water electrolysis.Masking OER with thermodynamically auspicious methanol oxidation reaction(MOR)can significantly boost the H_(2) and value-added products production.However,it is currently challenging to achieve a synergistic manipulation of product selectivity and performance for MOR electrocatalyst.Herein,we report NiSnPH@OOH/CC(CC=carbon cloth)perovskite hydroxide nanosphere as an efficient MOR electrocatalyst with high activity,stability,and selectivity towards methanol oxidation to formate.A surface amorphous layer of defect rich NiOOH was generated in operando by selective Sn leaching with stable perovskite hydroxide bulk structure,which mitigates the oxidative power and optimizes the local coordination environment of the active NiOOH sites.In situ Raman combined with electrochemical studies further confirm the key active species,NiOOH,generated in operando enhance the MOR and blocking the over oxidation of methanol to CO_(2).As a result,NiSnPH@OOH/CC effectively masks the OER and attains>99%selectivity with 100%Faradic efficiency for methanol-to-formate.The results of this study show the advances of NiSnPH@OOH/CC as an efficient electrocatalyst for MOR and also suggest its potential applications for various small organic molecules oxidation.

Crystal-phase-controlled PtSn intermetallic nanowires for efficient methanol oxidation

Developing highly efficient Pt-based methanol oxidation reaction(MOR)catalysts is pivotal for direct methanol fuel cells.Phase engineering of nanomaterials offers a promising strategy to improve their catalytic performance,yet achieving phase modulation in one-dimensional nanowires(NWs)remains a great challenge.Herein,we report a facile and one-pot synthesis approach for the crystal-phase-controlled Pt-Sn intermetallic nanowires(NWs),realizing the crystal-phases regulation of face-centered cubic Pt_(3)Sn intermetallic NWs(FCC-Pt_(3)Sn INTNWs)and hexagonal close-packed Pt Sn intermetallic NWs(HCP-PtSn INTNWs)by adjusting the amounts of Sn precursors.Notably,the FCC-Pt_(3)Sn INTNWs exhibit high mass and specific activities of 6.4 A mg_(Pt)^(-1)and 11.8 mA cm^(-2),respectively,surpassing its counterparts,the HCP-PtSn INTNWs and commercial Pt/C catalysts.After a 10,000 s durability test,the FCC-Pt_(3)Sn INTNWs still maintain a mass activity of 5.6 A mg_(Pt)^(-1),which is 24.3 times higher than that of commercial Pt/C catalyst.This dramatic enhancement of MOR performance is primarily attributed to the phasecontrolled structure and accelerated removal of CO intermediates(CO*).Theoretical calculations and CO stripping experiments demonstrate that the FCC-Pt_(3)Sn INTNWs lower the energy barrier for converting CO*into COOH*by reducing CO*binding and enhancing OH adsorption,thus significantly improving the MOR activity,CO tolerance,and stability.

Sonochemical Synthesis of Two Dimensional C3N4 Nanosheets Supported Palladium Composites and Their Electrocatalytic Activity for Oxygen Reduction and Methanol Oxidation Reaction

The preparation of highly active electrocatalysts with good durability and low cost for fuel cells is highly desir- able but still remains a significant challenge. Here we synthesized two dimensional （2D） C3N4 nanosheets supported palladium composites （C3N4/Pd） via a simple and convenient sonochemical approach. We have systematically stud- ied the electrocatalytic performance of as-prepared catalysts. We found that the prepared C3N4/Pd composites pos- sessed excellent catalytic activity and stability for oxygen reduction reaction （ORR） in alkaline media. Encourag- ingly, the C3N4/Pd catalysts exhibit the excellent electrocatalytic activity for methanol oxidation reaction （MOR） in alkaline media, even better than that of the commercial Pt/C catalyst, The excellent electrocatalytic performance of the 2D C3N4 nanosheets supported palladium composites catalysts results from their synergy effect between the ul- trathin substrate material with large surface area and excellent dispersion of palladium nanoparticles. This study demonstrates that sonochemical method opens up a new avenue for the preparation of electrocatalysts for fuel cells. We expect these materials are likely to find uses in a broad range of applications, for example, fuel cells, solar cells, batteries and other electrochemical analysis.