Hyper-Crosslinked Polymer-Derived Nitrogen-Doped Hierarchical Porous Carbon as Metal-Free Electrocatalysts for High-Efficiency Oxygen Reduction
Hyper-Crosslinked Polymer-Derived Nitrogen-Doped Hierarchical Porous Carbon as Metal-Free Electrocatalysts for High-Efficiency Oxygen Reduction
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DOI：
10.1021/acs.energyfuels.1c03087
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发表时间：
2021-11
期刊：
影响因子：
5.3
通讯作者：
Yue Yang;Zhuopei He;Shaolei Wang;Heng-guo Wang;G. Zhu
中科院分区：
文献类型：
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作者：
Yue Yang;Zhuopei He;Shaolei Wang;Heng-guo Wang;G. Zhu
由多孔有机聚合物，特别是低成本的超高交联聚合物制备的含氮多孔炭，为构建化学组成和孔结构可调的碳基无金属电催化剂提供了理想的平台。然而，由于大多数羟基磷灰石不含氮，直接热解法制备掺氮多孔碳具有一定的难度。本文采用简单的NH3活化法，制备了一种以六氯酚为前驱体的N掺杂层状多孔炭。影响催化剂催化性能的关键因素可以通过热解温度和基团进行规律性的调整，从而得到氮含量丰富、比表面积高(1865m2g-1)、缺陷丰富的催化剂(Py-NHCP-1000)。值得注意的是，具有出色电催化性能的Py-NHCP-1000的E1/2比商用铂/碳正移了27 mV，并且具有很好的耐用性和价格适中的氧还原反应性能。因此，本工作为从低成本、可扩展的六氯酚中设计和制备一种价格低廉、效率高的无金属电催化剂并将其推广到其他储能/转换材料中铺平了道路。
The development of N-doped porous carbon from porous organic polymers (POPs), especially low-cost hyper-crosslinked polymers (HCPs) provides an ideal platform for constructing carbon-based metal-free electrocatalysts with tunable chemical compositions and porous structures. However, most of the HCPs do not contain nitrogen, which makes it difficult to fabricate N-doped porous carbon by direct pyrolysis. Herein, a sort of N-doped hierarchically porous carbon using HCPs as a precursor is prepared by simple NH3activation. The key factors affecting the catalytic performance of the obtained carbon catalysts can be regularly tuned by the pyrolysis temperature and building blocks, which results in an optimal catalyst (Py-NHCP-1000) with abundant nitrogen content, a high surface area (1865 m2g–1), and rich defects. Remarkably, Py-NHCP-1000 with an outstanding electrocatalytic performance presents a positive shift of 27 mV forE1/2relative to commercial Pt/C, and well durable and affordable qualities for the oxygen reduction reaction. Therefore, this work paves an avenue for designing and preparing a kind of affordable and high-efficiency metal-free electrocatalyst from low-cost and scalable HCPs and extending it to other energy storage/conversion materials.