Pt nanoparticles supported by sulfur and phosphorus co-doped graphene as highly active catalyst for acidic methanol electrooxidation

• Published in: Electrochimica acta 2018-09, Vol.285, p.202-213
• Main Authors: An, Meichen, Du, Lei, Du, Chunyu, Sun, Yongrong, Wang, Yajing, Yin, Geping, Gao, Yunzhi
• Format: Article
• Language: English
• Subjects: Catalysis; Catalyst support; Catalysts; Chemical synthesis; Electrocatalysts; Fuel cells; Functional groups; Graphene; Metals; Methanol; Methanol oxidation reaction; Nanoparticles; Oxidation; Phosphorus; Platinum; Sulfur; Sulfur/phosphorus co-doping
• ISSN: 0013-4686; 1873-3859
• DOI: 10.1016/j.electacta.2018.07.237

Heteroatoms doped graphene is a promising support to improve the methanol oxidation reaction (MOR) activity of its supported Pt-based catalysts due to their strong interactions. This work reports the synthesis of sulfur (S) and phosphorus (P) co-doped graphene (SPG) as a support of Pt nanoparticles by a thermally annealing procedure. The employment of additional S remarkably enhances the doping content of P from 1.9% of P doped graphene (PG) to 4.6%, leading to higher defect sites for uniformly dispersing Pt nanoparticles and enhanced interactions with Pt. Compared with Pt/PG and Pt/C catalysts, the Pt/SPG catalyst exhibits over 1.2 and 1.4 times higher electrochemical surface area, 1.6 and 3.6 times higher MOR activity, respectively, and desirable stability toward the MOR. It is revealed that the Pt/SPG catalyst has a strong CO-tolerance due to the more generated oxygen-containing functional groups and the enhanced oxidation of adsorbed CO. This work provides an ideal candidate of developing heteroatoms co-doped graphene based electrocatalysts towards MOR in fuel cells. [Display omitted] •S and P atoms are successfully incorporated into graphene matrix (SPG).•Introduction of S remarkably promotes the doping content of P (from 1.9% to 4.6%).•Pt/SPG catalyst presents excellent methanol oxidation activity and stability.•More metallic Pt and oxygen-containing species enhance CO-tolerance of Pt/SPG.