ChemRxiv
These are preliminary reports that have not been peer-reviewed. They should not be regarded as conclusive, guide clinical practice/health-related behavior, or be reported in news media as established information. For more information, please see our FAQs.
1/1
0/0

Tunable Carbon Surface from Mono- to Multi-Metallic Single Atoms

preprint
submitted on 07.05.2020 and posted on 08.05.2020 by Weihong Lai, Heng Wang, Quan jiang, Zichao Yan, Hanwen Liu, Yaojie Lei, Lingfei Zhao, Wang Zhang, Lei Wang, Hirofumi Yoshikawa, Daiju Matsumura, Yunxiao Wang, Qiao sun, Jiazhao Wang, Huakun Liu, Shulei Chou, Shixue Dou

Herein, we develop a non-selective charge compensation strategy to prepare multi-single-atom doped carbon (MSAC) in which a sodium p-toluenesulfonate (PTS-Na) doped polypyrrole (S-PPy) polymer is designed to anchor discretionary mixtures of multiple metal cations, including iron (Fe3+), cobalt (Co3+), ruthenium (Ru3+), palladium (Pd2+), indium (In3+), iridium (Ir2+), and platinum (Pt2+) . As illustrated in Figure 1, the carbon surface can be tuned with different level of compositional complexities, including unary Pt1@NC, binary (MSAC-2, (PtFe)1@NC), ternary (MSAC-3, (PtFeIr)1@NC), quaternary (MSAC-4, (PtFeIrRu)1@NC), quinary (MSAC-5, (PtFeIrRuCo)1@NC), senary (MSAC-6, (PtFeIrRuCoPd)1@NC), and septenary (MSAC-7, (PtFeIrRuCoPdIn)1@NC) samples. The structural evolution of carbon surface dictates the activities of both ORR and HER. The senary MSAC-6 achieves the ORR mass activity of 18.1 A·mgmetal-1 at 0.9 V (Vs reversible hydrogen electrode (RHE)) over 30K cycles, which is 164 times higher than that of commercial Pt/C. The quaternary MSAC-4 presented a comparable HER catalytic capability with that of Pt/C. These results indicate that the highly complexed carbon surface can enhance its ability over general electrochemical catalytic reactions. The mechanisms regarding of the ORR and HER activities of the alternated carbon surface are also theoretically and experimentally investigated in this work, showing that the synergistic effects amongst the co-doped atoms can activate or inactivate certain single-atom sites.

History

Email Address of Submitting Author

wl478@uowmail.edu.au

Institution

University of Wollongong

Country

Australia

ORCID For Submitting Author

0000-0002-8685-9662

Declaration of Conflict of Interest

No conflict interest

Exports

Logo branding

Exports