Heteroatom-doped carbon materials are intensively studied in supercapacitors and fuel cells, because of their great potential for sustainably bearing on the energy crisis and environmental pollution. Although enormous efforts are put in material perfection with a hierarchically porous microstructure, the simultaneous optimization of both porous structures and surface functionalities is hard to achieve due to inevitable concurrent dopant leaching effect and structural collapse under required high pyrolysis temperature. In this study, an in situ dehalogenation polymerization and activation protocol is introduced to synthesize nitrogen- and sulfur-codoped carbon materials (NS-PCMs) with hierarchical pore distribution and abundant surface doping, which endows them with good conductivity, abundant accessible active sites, and efficient mass transport. As a result, the as-prepared carbon materials (NS-a-PCM-1000) show an excellent mass specific capacitance of 461.5 F g-1 at a current density of 0.1 A g-1 , long cycle life (>23 k, 10 A g-1 ), and high device energy and power density (17.3 Wh kg-1 , 250 W kg-1 ). Significantly, NS-a-PCM-1000 also exhibits one of the highest oxygen reduction reaction activities (onset potential of 1.0 V vs reversible hydrogen electrode) in alkaline media among all reported metal-free catalysts.

中文翻译：

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定制多层多孔的氮，硫掺杂碳，以用于高性能超级电容器和减氧。

掺杂杂原子的碳材料在超级电容器和燃料电池中得到了广泛的研究，因为它们具有可持续承受能源危机和环境污染的巨大潜力。尽管在具有分层多孔微结构的材料完善方面投入了巨大的努力，但是由于不可避免的同时的掺杂物浸出效应和在所需的高热解温度下结构崩溃，很难同时实现多孔结构和表面功能的同时优化。在这项研究中，引入了原位脱卤聚合和活化方案以合成具有分级孔隙分布和丰富表面掺杂的氮和硫共掺杂碳材料（NS-PCM），这赋予它们良好的导电性，丰富的可利用活性位点，高效的大众运输。结果，所制备的碳材料（NS-a-PCM-1000）在电流密度为0.1 A g-1时表现出优异的质量比电容461.5 F g-1，循环寿命长（> 23 k， 10 A g-1），高器件能量和功率密度（17.3 Wh kg-1，250 W kg-1）。值得注意的是，在所有已报道的无金属催化剂中，NS-a-PCM-1000在碱性介质中还表现出最高的氧还原反应活性之一（相对于可逆氢电极的起始电位为1.0 V）。