期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 10, 期 11, 页码 6086-6095出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta06897k
关键词
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资金
- National Natural Science Foundation of China [21902078, 21875112]
- Natural Science Foundation of Jiangsu Higher Education Institutions of China [19KJB150033]
- Natural Science Foundation of Jiangsu Province [BK20171473]
- National and Local Joint Engineering Research Centre of Biomedical Functional Materials
- Priority Academic Program Development of Jiangsu Higher Education Institutions
This study successfully integrates single atom sites with small-sized noble metals to break out their incompatibility in synthesis and to improve their thermostability, offering a versatile approach to develop single atom-based bifunctional catalysts for energy devices.
Developing effective bifunctional catalysts for the oxygen reduction and evolution reaction (ORR/OER) is essential for accelerating the cathode efficiency of Zn-air batteries. Herein, atomically dispersed Ni single atoms are supported by sub-10 nm Pd nanocrystals embedded in N-doped carbon frameworks (Ni SAs-Pd@NC), in an effort to achieve superior bifunctional activity in both the ORR and OER. The key synthetic point depends on the protection mechanism of 1-naphthylamine, which could provide a carbon source for Ni SAs and restrict the Pd size under sub-10 nm during 600 degrees C pyrolysis, simultaneously. The synergistic effect of sub-10 nm Pd with superior ORR activity and Ni-N-4 SAs with favourable OER activity leads to bifunctional catalytic performance, meanwhile the rod-like carbon frameworks with ultrathin, porous and N-doped features contribute to accelerated electron transfer and structural robustness. As a proof-of-concept application, Ni SAs-Pd@NC demonstrates ultrahigh ORR activity with a positive half-wave potential of 0.84 V and a low OER overpotential of 380 mV at 10 mA cm(-2), in an alkaline medium. For a rechargeable Zn-air battery, the Ni SAs-Pd@NC cathode delivers a low charge-discharge voltage gap of 0.87 V, a high energy density of 884.6 W h kg(Zn)(-1), a high power density of 134.2 mW cm(-2) and remarkable long-term cyclability for operation over 700 cycles, outperforming commercial Pt/C + RuO2 benchmarks. This work successfully integrates single atom sites with small-sized noble metals to break out their incompatibility in synthesis and to improve their thermostability, which offers a versatile approach to develop single atom-based bifunctional catalysts for energy devices.
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