Nitrogen-Rich Mesoporous Carbons: Highly Efficient, Regenerable Metal-Free Catalysts for Low-Temperature Oxidation of H2S

详细信息    查看全文

• 作者：Fugen Sun ; Jun Liu ; Huichao Chen ; Zixiao Zhang ; Wenming Qiao ; Donghui Long ; Licheng Ling
• 刊名：ACS Catalysis
• 出版年：2013
• 出版时间：May 3, 2013
• 年：2013
• 卷：3
• 期：5
• 页码：862-870
• 全文大小：672K
• 年卷期：v.3,no.5(May 3, 2013)
• ISSN：2155-5435

文摘

We demonstrate that it is possible to transform traditional mesoporous carbons into a superior metal-free catalyst for low-temperature H₂S removal via doping a high concentration of nitrogen atoms into the carbon. The nitrogen doping level is important for the activity of mesoporous carbons as a metal-free catalyst. Although carbons doped with only an intermediate amount of nitrogen (e.g., 4.3 wt %), show little aptitude for the catalytic oxidation of H₂S when nitrogen doping reaches a certain high level (e.g., 8.5 wt %), the nitrogen-rich mesoporous carbons (NMC) exhibit high catalytic activity and selectivity toward H₂S oxidation at low temperature. Further study suggests that the pyridinic nitrogen atoms are responsible for the catalytic activity in H₂S oxidation. Owing to the metal-free nature of the NMC catalyst, it can be easily regenerated by CS₂ scrubbing, and the product sulfur can be recovered. Our desulfurization results suggest that such metal-free carbons could, indeed, overcome the limitations of the conventional H₂S catalysts and provide suitable, sustainable, and inexpensive solutions for technological development in H₂S removal.

Keywords:

Mesoporous carbon; nitrogen doping; metal-free catalysis; catalytic oxidation; H₂S removal