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基于氮硫共掺杂石墨烯的碱性介质中先进氧还原反应催化剂

Advanced oxygen reduction reaction catalyst based on nitrogen and sulfur co-doped graphene in alkaline medium.

作者信息

Li Yongfeng, Li Meng, Jiang Liqing, Lin Lin, Cui Lili, He Xingquan

机构信息

Department of Chemistry and Chemical Engineering, Changchun University of Science and Technology, Changchun 130022, P. R. China.

出版信息

Phys Chem Chem Phys. 2014 Nov 14;16(42):23196-205. doi: 10.1039/c4cp02528h.

Abstract

A novel nitrogen and sulfur co-doped graphene (N-S-G) catalyst for oxygen reduction reaction (ORR) has been prepared by pyrolysing graphite oxide and poly[3-amino-5-mercapto-1,2,4-triazole] composite (PAMTa). The atomic percentage of nitrogen and sulfur for the prepared N-S-G can be adjusted by controlling the pyrolysis temperature. Furthermore, the catalyst pyrolysed at 1000 °C, denoted N-S-G 1000, exhibits the highest catalytic activity for ORR, which displays the highest content of graphitic-N and thiophene-S among all the pyrolysed samples. The electrocatalytic performance of N-S-G 1000 is significantly better than that of PAMTa and reduced graphite oxide composite. Remarkably, the N-S-G 1000 catalyst is comparable with Pt/C in terms of the onset and half-wave potentials, and displays larger kinetic limiting current density and better methanol tolerance and stability than Pt/C for ORR in an alkaline medium.

摘要

通过热解氧化石墨与聚[3-氨基-5-巯基-1,2,4-三唑]复合材料(PAMTa)制备了一种用于氧还原反应(ORR)的新型氮硫共掺杂石墨烯(N-S-G)催化剂。通过控制热解温度,可以调节所制备的N-S-G中氮和硫的原子百分比。此外,在1000℃热解的催化剂,记为N-S-G 1000,对ORR表现出最高的催化活性,在所有热解样品中其石墨氮和噻吩硫的含量最高。N-S-G 1000的电催化性能明显优于PAMTa和还原氧化石墨复合材料。值得注意的是,N-S-G 1000催化剂在起始电位和半波电位方面与Pt/C相当,并且在碱性介质中对ORR表现出比Pt/C更大的动力学极限电流密度、更好的甲醇耐受性和稳定性。

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