Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 12, Issue 4, Pages 1317-1325Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ee00162j
Keywords
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Funding
- National Natural Science Foundation of China (NSFC) [21520102002, 91622116, 21471014, 21701101]
- National Key Research and Development Project [2016YFF0204402, 2017YFA0206500]
- Fundamental Research Funds for the Central Universities
- Long-Term Subsidy Mechanism from the Ministry of Finance
- Long-Term Subsidy Mechanism from the Ministry of Education of China
- Shandong Scientific Research Awards Foundation for Outstanding Young Scientists [ZR2018JL010]
- Shandong Joint Fund of Outstanding Young Talents [ZR2017BB018]
- Loughborough University [H10841]
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Single-atom electrocatalysts (SAECs) have gained tremendous attention due to their unique active sites and strong metal-substrate interactions. However, the current synthesis of SAECs mostly relies on costly precursors and rigid synthetic conditions and often results in very low content of single-site metal atoms. Herein, we report an efficient synthesis method to prepare metal-nitrogen-carbon SAECs based on formamide condensation and carbonization, featuring a cost-effective general methodology for the mass production of SAECs with high loading of atomically dispersed metal sites. The products with metal inclusion were termed as formamide-converted metal-nitrogen-carbon (shortened as f-MNC) materials. Seven types of single-metallic f-MNC (Fe, Co, Ni, Mn, Zn, Mo and Ir), two bi-metallic (ZnFe and ZnCo) and one tri-metallic (ZnFeCo) SAECs were synthesized to demonstrate the generality of the methodology developed. Remarkably, these f-MNC SAECs can be coated onto various supports with an ultrathin layer as pyrolysis-free electrocatalysts, among which the carbon nanotube-supported f-FeNC and f-NiNC SAECs showed high performance for the O-2 reduction reaction (ORR) and the CO2 reduction reaction (CO2RR), respectively. Furthermore, the pyrolysis products of supported f-MNC can still render isolated metallic sites with excellent activity, as exemplified by the bi-metallic f-FeCoNC SAEC, which exhibited outstanding ORR performance in both alkaline and acid electrolytes by delivering approximate to 70 and approximate to 20 mV higher half-wave potentials than that of commercial 20 wt% Pt/C, respectively. This work offers a feasible approach to design and manufacture SAECs with tuneable atomic metal components and high density of single-site metal loading, and thus may accelerate the deployment of SAECs for various energy technology applications.
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