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DOI | 10.1039/c6ee03446b |
Active sites engineering leads to exceptional ORR and OER bifunctionality in P,N Co-doped graphene frameworks | |
Chai G.-L.; Qiu K.; Qiao M.; Titirici M.-M.; Shang C.; Guo Z. | |
发表日期 | 2017 |
ISSN | 17545692 |
起始页码 | 1186 |
结束页码 | 1195 |
卷号 | 10期号:5 |
英文摘要 | Bifunctional catalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) are highly desirable for rechargeable metal-air batteries and regenerative fuel cells. However, the commercial oxygen electrocatalysts (mainly noble metal based) can only exhibit either ORR or OER activity and also suffer from inherent cost and stability issues. It remains challenging to achieve efficient ORR and OER bifunctionality on a single catalyst. Metal-free structures offer relatively large scope for this bifunctionality to be engineered within one catalyst, together with improved cost-effectiveness and durability. Herein, by closely coupled computational design and experimental development, highly effective bifunctionality was achieved in a phosphorus and nitrogen co-doped graphene framework (PNGF)-with both ORR and OER activities reaching the theoretical limits of metal-free catalysts, superior to their noble metal counterparts in both (bi)functionality and durability. In particular, with the identification of active P-N sites for OER and N-doped sites for ORR, we successfully intensified these sites by one-pot synthesis to tailor the PNGF. The resulting catalyst achieved an ORR potential of 0.845 V vs. RHE at 3 mA cm-2 and an OER potential of 1.55 V vs. RHE at 10 mA cm-2. Its combined ORR and OER overpotential of 705 mV is much lower than those previously reported for metal-free bifunctional catalysts. © 2017 The Royal Society of Chemistry. |
英文关键词 | Durability; Electrocatalysts; Electrolytic reduction; Graphene; Metals; Oxygen; Precious metals; Regenerative fuel cells; Bi-functional catalysts; Computational design; Experimental development; Metal-air battery; Metal-free catalysts; Oxygen evolution reaction; Oxygen reduction reaction; Theoretical limits; Catalysts; bioengineering; carbon nanotube; catalyst; experimental design; experimental study; nitrogen; oxygen; phosphorus |
语种 | 英语 |
来源期刊 | Energy & Environmental Science
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/190545 |
作者单位 | Department of Chemistry, University College London, London, WC1H 0AJ, United Kingdom; State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China; Renewable Energy Group, College of Engineering, Mathematics and Physical Sciences, University of Exeter, Penryn Campus, TR10 9FE, United Kingdom; Materials Research Institute, School of Engineering and Materials Science, Queen Mary University of London, Mile End Road, London, E1 4NS, United Kingdom; Materials Research Institute, Queen Mary University of London, Mile End Road, London, E1 4NS, United Kingdom; School of Environmental Sciences, University of East Anglia, Norwich, NR4 7TJ, United Kingdom |
推荐引用方式 GB/T 7714 | Chai G.-L.,Qiu K.,Qiao M.,et al. Active sites engineering leads to exceptional ORR and OER bifunctionality in P,N Co-doped graphene frameworks[J],2017,10(5). |
APA | Chai G.-L.,Qiu K.,Qiao M.,Titirici M.-M.,Shang C.,&Guo Z..(2017).Active sites engineering leads to exceptional ORR and OER bifunctionality in P,N Co-doped graphene frameworks.Energy & Environmental Science,10(5). |
MLA | Chai G.-L.,et al."Active sites engineering leads to exceptional ORR and OER bifunctionality in P,N Co-doped graphene frameworks".Energy & Environmental Science 10.5(2017). |
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