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Carbon skeleton doped with Co, N, S and P as efficient electrocatalyst for oxygen evolution reaction

掺杂钴、 氮、 硫、 磷的碳骨架作为电化学析氧反应的高效催化剂

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Abstract

A new strategy for the preparation of highly efficient catalyst used in oxygen evolution reaction (OER) in alkaline media was developed. A Co-containing carbonitride polymer network (CoCN) was selected as a structural-directing template and a hypercross-linked polymer containing S and P, which formed on CoCN skeleton in situ, was used as a cover. After calcination at 450°C for 2 h, an interconnected nanostructure was obtained and showed excellent activity and high stability for electrochemical water splitting. Trace amount of Co and other heteroatoms including N, S, P and the formed Co–N and Co–O species are essential for the impressive catalysis performance. The calcination temperature of 450°C is optimal to the catalysis performance. These results suggest that Co in addition to heteroatom-doped (S, P) carbonitride could be used as a supplement and/or an alternative to noble metal oxides for water splitting.

摘要

本文提出了一种制备碱性介质中电化学析氧反应高效催化剂的新方法. 该方法选用一种含钴的碳-氮聚合物网络作为结构模板, 外面包裹一层原位制备的、 含硫和磷的超支化交联聚合物. 450°C煅烧2 h后, 获得可用于电化学析氧反应的、 内部交联、 微观呈现层状结构的催化剂. 该催化剂在1.0 mol L-1的氢氧化钾水溶液中表现出很好的电化学催化活性和高稳定性. 电子衍射图谱(EDS)和X-射线光电子能谱(XPS)研究表明该催化剂含有痕量钴及其他杂原子, 包括氮、 硫、 磷, 且证实了能够大幅提高催化活性的Co-N和Co-O活性物质的存在. 将钴替换为铜和镍之后, 催化剂的催化活性大大降低, 表明当前方法对钴基催化剂的制备最为有效. 煅烧过程中所选用的温度对催化剂的催化活性亦有显著影响, 450°C为最优温度. 这些结果表明, 含钴的、 杂原子(硫、 磷)掺杂的碳氮化物有望成为一类新的电解水催化剂, 以取代贵金属氧化物, 或作为其有益的补充.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (21603243, 21402215 and 61474124), the Natural Science Foundation of Gansu Province (1606RJZA112) and the Natural science research project of Education Department of Shaanxi Province (17JK0093).

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Authors and Affiliations

  1. State Key Laboratory of Solid Lubrication & Laboratory of Clean Energy Chemistry and Materials, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou, 730000, China

    Jiamei Cao  (曹佳梅), Yongqiang Feng  (冯永强), Baoyong Liu  (刘宝勇) & Hongguang Li  (李洪光)

  2. School of Materials Science and Engineering, Shaanxi University of Science & Technology, Xi’an, 710021, China

    Jiamei Cao  (曹佳梅) & Baoyong Liu  (刘宝勇)

  3. University of Chinese Academy of Sciences, Beijing, 100049, China

    Yongqiang Feng  (冯永强)

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  1. Jiamei Cao  (曹佳梅)
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  3. Baoyong Liu  (刘宝勇)
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  4. Hongguang Li  (李洪光)
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Correspondence to Yongqiang Feng  (冯永强) or Hongguang Li  (李洪光).

Additional information

Jiamei Cao obtained her BSc degree from the Department of Northwest Normal University in 2014, and her MSc degree from Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, under the supervision of Prof. Hongguang Li, in July 2017. Her research interest is focused on microporous polymeric materials and functional fullerenes for applications in clean energy.

Yongqiang Feng obtained his BSc degree from Sichuan University in 2010 and PhD degree from the Institute of Chemistry, Chinese Academy of Sciences in 2015. After that, he joined Prof. Hongguang Li’s group in Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences as an assistant professor. Now, he is an associate professor in Shannxi University of Science & Technology. His current interest is focused on the design of carbon-based nanomaterials for applications in optoelectronic devices.

Baoyong Liu obtained his BSc degree from Shandong University in 2003. And he received his Master’s degree in chemical engineering from China University of Petroleum (East China) in 2008. He is currently a PhD candidate at Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences under the supervision of Prof. Hongguang Li. His research interest includes carbon nanomaterials and tribology.

Hongguang Li obtained his BSc degree and PhD degree from Shandong University in 2003 and 2008, respectively. After three-year postdoc research, he joined the Laboratory of Clean Energy Chemistry and Materials, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences as a professor. His current interest focuses on the design of novel π-conjugated molecules and engineering carbon nanomaterials for the applications in optoelectronic devices.

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Cao, J., Feng, Y., Liu, B. et al. Carbon skeleton doped with Co, N, S and P as efficient electrocatalyst for oxygen evolution reaction. Sci. China Mater. 61, 686–696 (2018). https://doi.org/10.1007/s40843-017-9149-y

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