Zhu, JianbingXiao, MeilingSong, PingFu, JingJin, ZhaoMa, LiangGe, JunjieLiu, ChangpengChen, ZhongweiXing, Wei2018-06-292018-06-292018-07-01https://doi.org/10.1016/j.nanoen.2018.04.021http://hdl.handle.net/10012/13448The final publication is available at Elsevier via http://dx.doi.org/10.1016/j.nanoen.2018.04.021 © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/Metal-free electrocatalysts have eluded widespread adoption in polymer electrolyte membrane fuel cells due to their far inferior catalytic activity than most non-precious metal-N-C counterparts (M-Nx-C) for oxygen reduction reaction (ORR), despite their distinct advantages over the M-Nx-C catalysts, including lower cost and higher durability. Herein, we develop a rational bottom-up engineering strategy to improve the ORR performance of a metal-free catalyst by constructing a three-dimensional ultrathin N, P dual-doped carbon nanosheet. The resultant catalyst represents unprecedented ORR performance with an onset potential of 0.91 V, half-wave potential of 0.79 V. Impressively, a maximum power output at 579 mW cm−2 is generated in the fuel cell test, the best among reported metal-free catalysts and outperforms most of the M-Nx-C catalysts. The outstanding catalytic performance results from the highly active polarized carbon sites which are induced by selective graphitic nitrogen and phosphorous dual doping. Our findings provide new directions for the exploration of alternatives to Pt and bring a renew interests in the metal-free catalysts.enAttribution-NonCommercial-NoDerivatives 4.0 InternationalMetal-free catalystActive siteOxygen reduction reactionPolymer electrolyte membrane fuel cellArticle