Carbon-neutral application of renewable biogas to valuable chemical raw materials has received much attention in sustainable areas, while sulfur poisoning remains a big problem in biogas dry reforming process. In this work, sulfur deactivation and regeneration performance of a Ni/SiO₂ catalyst in model biogas dry reforming and related mechanisms were studied. The effects of H₂S content (50 and 100 ppm) and reaction temperature (700–800 °C) on biogas dry reforming were investigated. Three regeneration methods (H₂S feeding cessation, temperature-programmed calcination (TPC), and O₂ activation) were applied. The results showed that the presence of H₂S caused server deactivation in catalytic activity, and higher H₂S content led to faster deactivation. The deactivation was not reversed simply by stopping H₂S feeding and TPC, but O₂ activation could totally recover deactivated catalysts. The formation of Ni₇S₆, detected for the first time in biogas conditioning catalytic processes, confirmed by X-ray diffraction and X-ray photoelectron spectroscopy, led to sulfur poisoning, as well as catalyst sintering and carbon deposition. This work revealed that sulfur poisoning and regeneration mechanism is the formation and elimination of Ni₇S₆, and concluded that oxygen activation was the most effective method for reviving the catalytic activity, preventing sintering, and reducing carbon deposition. These findings will contribute to the industrial application of syngas production from biogas dry reforming.

中文翻译：

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Ni / SiO ₂催化剂上模型沼气的干重整：硫中毒和再生的总体性能及其机理

在可持续发展领域，可再生沼气以碳中和方式应用到有价值的化学原料上已引起了广泛关注，而硫中毒仍然是沼气干法重整过程中的一大问题。在这项工作中，研究了在模型沼气干重整中Ni / SiO ₂催化剂的硫失活和再生性能及其相关机理。研究了H ₂ S含量（50和100 ppm）和反应温度（700–800°C）对沼气干重整的影响。应用了三种再生方法（停止H ₂ S进料，程序升温煅烧（TPC）和O ₂活化）。结果表明，H ₂的存在S导致服务器催化活性失活，较高的H ₂ S含量导致失活速度更快。不能仅通过停止H ₂ S进料和TPC来使失活逆转，但是O ₂活化可以完全回收失活的催化剂。在沼气调节催化过程中首次检测到的Ni ₇ S ₆的形成，通过X射线衍射和X射线光电子能谱证实，导致了硫中毒以及催化剂的烧结和碳沉积。这项工作表明，硫中毒和再生机理是Ni ₇ S ₆的形成和消除。并得出结论，氧气活化是恢复催化活性，防止烧结和减少碳沉积的最有效方法。这些发现将有助于沼气干重整生产合成气的工业应用。