Directly catalytic reduction of NO without NH3 by single atom iron catalyst: A DFT calculation
Directly catalytic reduction of NO without NH3 by single atom iron catalyst: A DFT calculation
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DOI：
10.1016/j.fuel.2019.01.125
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发表时间：
2019-05
期刊：
影响因子：
7.4
通讯作者：
Weijie Yang;Zhengyang Gao;Xiaoshuo Liu;Chuanzhi Ma;Xunlei Ding;W. Yan
中科院分区：
文献类型：
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作者：
Weijie Yang;Zhengyang Gao;Xiaoshuo Liu;Chuanzhi Ma;Xunlei Ding;W. Yan
一氧化氮（NO）是一种重要的大气污染物，其排放受到严格的控制。NH3选择性催化还原NO技术是一种成熟、高效的技术，但仍存在氨逃逸、二次细颗粒物生成、设备腐蚀等明显缺点。因此，提出了一种无氨注入的单空位石墨烯基单原子铁催化剂（Fe/MG）直接催化还原NO的方法。通过密度泛函理论计算研究了详细的反应机理。热力学和动力学分析表明，NO还原的主要反应机理为Langmuir-Hinshelwood机理，活化能为0.81 eV，低于焦边的活化能。NO的催化还原反应是放热的，并且是热力学上有利的。温度对NO的催化还原有促进作用。基于Fe/MG催化还原NO的热力学和动力学性能，提出Fe/MG是一种新型的无氨NO还原催化剂。该理论研究结果可为NO的脱除提供新的思路，并为后续的实验研究奠定一定的基础。
Nitric oxide (NO) has been recognized as a major air pollutant, and the emission of NO has been strictly regulated. The technology of selective catalytic reduction of NO with NH3injection is mature and efficient, but it still has some obvious drawbacks such as ammonia slipping, secondary fine particulates formation, and equipment corrosion. Therefore, a directly catalytic reduction of NO without ammonia injection by monovacancy graphene-based single atom iron catalyst (Fe/MG) was proposed. The detailed reaction mechanism was investigated through density functional theory calculation. Based on thermodynamic and kinetic analysis, we concluded that Langmuir-Hinshelwood is the dominant reaction mechanism for NO reduction, and the activation energy is 0.81 eV which is lower than char edges. The catalytic reduction reaction of NO is exothermic and thermodynamically favorable. The temperature can accelerate the catalytic reduction of NO. Based on the thermodynamic and kinetic performances of Fe/MG in NO reduction, Fe/MG is suggested to be a novel catalyst for NO reduction without NH3. This theoretical research results can provide a new insight for NO removal and lay some foundations for subsequent experimental research.