Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation  

作　　者：Qi Zhang Quanguo Jiang Xiang Yang Chi Zhang Jian Zhang Lu Yang Haiyan He Guobing Ying Huajie Huang 

机构地区：[1]College of Materials Science and Engineering,Hohai University,Nanjing 210098,Jiangsu,China [2]New Energy Technology Engineering Lab of Jiangsu Province,College of Science,Nanjing University of Posts&Telecommunications(NUPT),Nanjing 210023,Jiangsu,China [3]School of Materials Science and Engineering,Southeast University,Nanjing 211100,Jiangsu,China

出　　处：《Journal of Energy Chemistry》2024年第6期419-428,I0011,共11页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(11872171 and 22209037);the Project on Excellent Post-graduate Dissertation of Hohai University。

摘　　要：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 largely 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 Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient 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-toface"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 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~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.

关 键 词：Rhodium nanosheet Ti_(3)C_(2)T_(x)MXene HETEROINTERFACE ELECTROCATALYST Fuel cell 

分 类 号：TM911.4[电气工程—电力电子与电力传动] TQ426[化学工程]