尿素热解制备氮掺杂Mo2C/AC及其催化还原NO2的性能提升机制Preparation of nitrogen-doped Mo2C/AC via urea pyrolysis and its performance enhancement mechanism in catalytic reduction of NO2
穆仕芳,王中兰,尚如静,张玉龙
摘要(Abstract):
针对传统NO_2检测用钼炉转化剂高温易失活及副反应干扰检测准确性的问题,文中采用浸渍-碳化法制备Mo_2C/AC,利用尿素在400~800℃区间的热解实现氮掺杂改性,制得Mo_2C/ACN-X系列催化剂。通过N_2物理吸附-脱附、拉曼光谱、X射线衍射、X射线光电子能谱对催化剂结构进行表征,深入探讨氮掺杂调控催化剂结构与其催化NO_2转化性能的提升机制。研究结果表明:氮掺杂后催化剂比表面积减小,Mo_2C/ACN-800平均孔径增大;尿素热解温度对催化剂体相钼物种及其表面价态分布具有调控作用。400℃与600℃热解条件下,MoO_2与Mo_2C共存,800℃热解时Mo_2C成为主导晶相。随热解温度升高,氮掺杂后催化剂表面Mo~(2+)含量上升,其中Mo_2C/ACN-800的Mo~(2+)含量显著增加;表面氮含量先升高后下降,吡啶氮占比上升。在60℃条件下,Mo_2C/ACN-800催化剂的NO_2转化率达97.5%,较未掺杂样品提高了9.7%。研究结论为开发高效NO_2低温转化剂开辟了新的材料设计思路,具有重要的理论与实际应用价值。
关键词(KeyWords): 尿素热解;氮掺杂;Mo_2C/AC;催化还原NO_2;低温转化
基金项目(Foundation): 河南省瓦斯地质与瓦斯治理重点实验室—省部共建国家重点实验室培育基地开放基金项目(WS2024B17)
作者(Author): 穆仕芳,王中兰,尚如静,张玉龙
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