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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >Sulfur-doping achieves efficient oxygen reduction in pyrolyzed zeolitic imidazolate frameworks
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Sulfur-doping achieves efficient oxygen reduction in pyrolyzed zeolitic imidazolate frameworks

机译：硫掺杂在热解沸石咪唑酸盐骨架中实现高效氧还原

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摘要

We report the first synthesis of sulfurated porous carbon materials with well-defined morphologies and uniform N/S distributions via pyrolysis of zeolitic imidazolate frameworks loaded with sulfur-containing molecules. The optimized sulfurated catalyst demonstrates excellent electrocatalytic activity for the oxygen reduction reaction (ORR) in both acid and alkaline media. The sulfurization process under optimized conditions can lower the ORR over-potential by ca. 170 mV at 3 mA cm(-2), giving a non-precious metal catalyst with an onset ORR potential of 0.90 V (vs. RHE, similarly hereinafter)/half-wave potential of 0.78 V in 0.1 M HClO4 and an onset ORR potential of 0.98 V/half-wave potential of 0.88 V in 0.1 M KOH. Furthermore, the S-doped porous carbon materials perform better in the long-term durability test than the non-S-doped samples and standard commercially available Pt/C. We also discuss different sulfuration methods for the ZIF system, morphologies of pyrolyzed samples, and catalytically active sites.
机译：我们报道了通过热解装有含硫分子的沸石咪唑酸盐骨架，首次合成了具有明确形态和均匀 N/S 分布的硫化多孔碳材料。优化后的硫化催化剂在酸性和碱性介质中均表现出优异的氧还原反应（ORR）电催化活性。优化条件下的硫化过程可以在3 mA cm（-2）下将ORR过电位降低约170 mV，从而得到非贵金属催化剂，在0.1 M HClO4中起始ORR电位为0.90 V（与RHE相比）/半波电位为0.78 V，在0.1 M KOH中起始ORR电位为0.98 V/半波电位为0.88 V。此外，S掺杂多孔碳材料在长期耐久性测试中优于非S掺杂样品和标准市售Pt/C。我们还讨论了ZIF系统的不同硫化方法、热解样品的形态和催化活性位点。

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