首页|Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation
Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation
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Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix lar-gely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti3C2Tx MXene nanolamellas(Rh NS/MXene)via a conve-nient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-to-face"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m2 gRh-1,a high mass activity of 1056.9 mA mgRh-1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.
College of Materials Science and Engineering Hohai University,Nanjing 210098,Jiangsu,China
New Energy Technology Engineering Lab of Jiangsu Province,College of Science,Nanjing University of Posts & Telecommunications(NUPT),Nanjing 210023,Jiangsu,China
School of Materials Science and Engineering,Southeast University,Nanjing 211100,Jiangsu,China
National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaProject on Excellent Postgraduate Dissertation of Hohai University