Catalytic ozonation for low-temperature NOX (x = 1, 2) removal with OH radicals over Cu doped Ce0.90Co0.10O2 − δ catalysts and mechanism analysis
Catalytic ozonation for low-temperature NOX (x = 1, 2) removal with OH radicals over Cu doped Ce0.90Co0.10O2 − δ catalysts and mechanism analysis
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DOI：
10.1016/j.fuproc.2017.07.033
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发表时间：
2017-12
影响因子：
7.5
通讯作者：
Lina Guo;Q. Zhong;Jie Ding;Zhiyong Deng;Wenkai Zhao
中科院分区：
文献类型：
--
作者：
Lina Guo;Q. Zhong;Jie Ding;Zhiyong Deng;Wenkai Zhao
采用碱性水热法合成了一系列Ce0.90Co0.10O2-δ和Ce0.90-xCuxCo0.10O2-δ（x = 0.03、0.07和0.10）催化剂，用作低温臭氧氧化催化剂去除NOX（x = 1，2）。本课题组研制了一种新型催化剂-管道分离式臭氧催化氧化脱氮装置。Ce0.83Cu0.07Co0.10O2 − δ表现出最高的催化活性（120 °C时去除率为91.5%），而Ce0.80Cu0.10Co0.10O2 − δ表现出最低的催化活性（120 °C时去除率为74.1%）。在尾溶液中仅检测到NO3−。催化性能与相应的dotOH自由基浓度呈正相关。自由基dotOH自由基可以从催化剂表面“转移”到管道，通过其自身的再生反应延长活化时间。在本方法中，自由基dotOH的浓度是由表面-OH的活化作用决定的，而不是表面-OH的密度. Ce0.83Cu0.07Co0.10O2 − δ中含有大量高活性的桥连-OH，而Ce0.80Cu0.10Co0.10O2 − δ中不存在桥连-OH。因此，Ce0.83Cu0.07Co0.10O2 − δ比Ce0.80Cu0.10Co0.10O2 − δ显示出更高的促进自由基dotOH形成的活性。
A series of Ce0.90Co0.10O2 − δand Ce0.90 − xCuxCo0.10O2 − δ(x = 0.03, 0.07 and 0.10) catalysts synthesized by an alkaline hydrothermal method were utilized as ozonation catalysts for the NOX(x = 1, 2) removal at low temperatures. A novel catalyst-duct separation apparatus for denitrification by catalytic ozonation was developed by our group. Ce0.83Cu0.07Co0.10O2 − δexhibits the highest catalytic activity (91.5% removal at 120 °C), whereas Ce0.80Cu0.10Co0.10O2 − δpresents the lowest (74.1% removal at 120 °C). Only NO3−is detected in the tail solutions. The catalytic performance presents a positive relationship with the corresponding radical dotOH concentration. radical dotOH radical can be “transferred” from catalyst surface to the duct, prolonging activation time through its own reproduction reaction. The surface –OH activation, not the surface –OH density determines the radical dotOH concentration in the present method. Ce0.83Cu0.07Co0.10O2 − δcontains a large number of high-activation bridging –OH, whereas the bridging –OH is absent in Ce0.80Cu0.10Co0.10O2 − δ. Therefore, Ce0.83Cu0.07Co0.10O2 − δshows much higher activation for promoting the formation of radical dotOH than Ce0.80Cu0.10Co0.10O2 − δ.