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Defect enriched N-doped carbon nanoflakes as robust carbocatalysts for H2S selective oxidation
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020-03-02 , DOI: 10.1039/d0ta00212g
Shiyan Li 1, 2, 3, 4, 5 , Qingqing Gu 1, 2, 3, 4, 5 , Ning Cao 5, 6, 7, 8 , Qian Jiang 1, 2, 3, 4, 5 , Chi Xu 1, 2, 3, 4, 5 , Chengfa Jiang 5, 6, 7, 8 , Congmei Chen 5, 9, 10 , Cuong Pham-Huu 11, 12, 13, 14, 15 , Yuefeng Liu 1, 2, 3, 4, 5
Affiliation  

Nanocarbons have emerged as low-cost, efficient and durable nonmetallic catalysts for H2S selective oxidation. However, the most efficient active sites for H2S activation remain elusive, which restricts further development of high-performance catalysts for industrial application. Herein, we report on the synthesis of N-doped carbon nanoflakes with tunable nitrogen dopants and abundant structural defects for H2S selective oxidation. These defect enriched N-doped carbon nanoflakes exhibited significantly enhanced catalytic performance (>740 gsulfur kgcat.−1 h−1), stability (>110 h) and decent tolerance to impurity gas (CO2) and steam toward continuous H2S selective oxidation. Combined advanced characterization, control experiments and theoretical simulation showed that the N species along with defects on N-doped carbon nanoflakes could enhance significantly the catalytic activity, and further confirmed that the pyridinic N was the most active species and the C atoms adjacent to N atoms exhibit strong interaction with HS. Our study provides predictive guidelines for the rational design of highly efficient and durable carbocatalysts for continuous catalytic oxidative desulfurization.

中文翻译:

缺陷富集的N掺杂碳纳米薄片可作为H2S选择性氧化的强力碳催化剂

纳米碳已经成为用于H 2 S选择性氧化的低成本,有效和耐用的非金属催化剂。然而,用于H 2 S活化的最有效的活性位点仍然难以捉摸,这限制了用于工业应用的高性能催化剂的进一步开发。在这里,我们报道了具有可调氮掺杂剂和H 2 S选择性氧化的丰富结构缺陷的N掺杂碳纳米片的合成。这些富含缺陷的氮掺杂碳纳米片表现出显着增强的催化性能(> 740 g千克kg cat。-1 h -1),稳定性(> 110 h)和对杂质气体(CO 2)的良好耐受性)并朝着连续H 2 S选择性氧化的方向蒸汽。结合先进的表征,控制实验和理论模拟表明,N物种以及N掺杂的碳纳米薄片上的缺陷可以显着增强催化活性,并进一步证实吡啶吡啶N是最活跃的物种,并且C原子与N原子相邻表现出强烈的相互作用与HS - 。我们的研究为合理设计高效,耐用的碳催化剂以进行连续催化氧化脱硫提供了预测指导。
更新日期:2020-03-02
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