Nitrogen-doped porous carbons (NPCs) have been regarded as an efficient metal-free catalyst for HS oxidation. However, critical factors affecting their desulfurization ability are still unclear, making it difficult to accurately adjust their desulfurization performance to meet industrial requirements. Herein, a novel 3D-interconnected NPC with hierarchical pore structure was synthesized by one-step “leavening” strategy using rice husk and (NH)CO as a carbon source and foaming agent, respectively, for HS oxidation at room temperature. Pyrolysis temperature is the major factor for physicochemical properties of NPCs, and breakthrough sulfur capacity of the optimal NPC reaches up to 1036.68 mg/g, which can remain stable during three desulfurization-regeneration cycles. Comparative experiment shows that HS capacity of NPC is 1.8 and 4.0 times those of PC and NC, respectively, revealing the excellent desulfurization performance of NPC. The structure-effect relationships between HS and NPC reveal that both textural and chemical properties of NPC, especially specific surface area, structural defect, and pyrrolic N, play dominant roles in HS removal. It is very necessary to balance the relationship between textural performances and pyrrolic N to synthesize optimal NPC catalyst. This work provides a valuable reference for rational design of high-efficiency carbon-based catalysts for persistent desulfurization at room temperature.

中文翻译：

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具有分级孔结构的3D互连氮掺杂多孔碳作为室温H2S氧化的高效催化剂


氮掺杂多孔碳（NPC）被认为是一种有效的 H2S 氧化无金属催化剂。然而，影响其脱硫能力的关键因素仍不清楚，导致其脱硫性能难以准确调节以满足工业要求。在此，利用稻壳和(NH)CO分别作为碳源和发泡剂，通过一步“发酵”策略合成了一种具有分级孔结构的新型3D互联NPC，在室温下进行H2S氧化。热解温度是影响NPC理化性质的主要因素，最佳NPC的突破硫容达到1036.68 mg/g，在3次脱硫-再生循环中保持稳定。对比实验表明，NPC的脱硫能力分别是PC和NC的1.8和4.0倍，揭示了NPC优异的脱硫性能。 HS 和 NPC 之间的结构效应关系表明，NPC 的结构和化学性质，特别是比表面积、结构缺陷和吡咯氮，在 HS 去除中起主导作用。平衡结构性能与吡咯N之间的关系以合成最佳的NPC催化剂是非常必要的。该工作为合理设计高效碳基常温持久脱硫催化剂提供了有价值的参考。