Facile H2O-Contributed O2 Activation Strategy over Mn-Based SCR Catalysts to Counteract SO2 Poisoning

被引:29
作者
An, Dongqi [1 ]
Ji, Jiawei [1 ]
Cheng, Qianni [1 ]
Zhao, Xin [1 ]
Cai, Yandi [1 ]
Tan, Wei [1 ]
Tong, Qing [1 ]
Ma, Kaili [2 ]
Zou, Weixin [1 ]
Sun, Jingfang [1 ]
Tang, Changjin [3 ]
Dong, Lin [1 ]
机构
[1] Nanjing Univ, China State Key Lab Pollut Control & Resource Reu, Sch Environm, Jiangsu Key Lab Vehicle Emiss Control,Ctr Modern, Nanjing 210093, Peoples R China
[2] Southeast Univ, Anal & Testing Ctr, Nanjing 211189, Peoples R China
[3] Nanjing Normal Univ, Jiangsu Prov Engn Res Ctr Environm Risk Prevent &, Sch Environm, Nanjing 210023, Peoples R China
基金
中国国家自然科学基金;
关键词
NH3-SCR; Mn-based catalysts; H2O promotion; SO2; resistance; O-2; activation; REDUCTION; MECHANISM; NH3; NO; GAMMA-MNO2; OXIDATION; OXIDE;
D O I
10.1021/acs.est.3c04314
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Mn-based catalysts preferred in low-temperature selective catalytic reduction (SCR) are susceptible to SO2 poisoning. The stubborn sulfates make insufficient O-2 activation and result in deficient reactive oxygen species (ROS) for activating reaction molecules. H2O has long been regarded as an accomplice to SO2, hastening catalyst deactivation. However, such a negative impression of the SCR reaction was reversed by our recent research. Here, we reported a H2O contribution over Mn-based SCR catalysts to counteract SO2 poisoning through accessible O(2)activation, in which O-2 was synergistically activated with H2O to generate ROS for less deactivation and more expected regeneration. The resulting ROS benefited from the energetically favorable route supported by water-induced E-a reduction and was actively involved in the NH3 activation and NO oxidation process. Besides, ROS maintained high stability over the SO2 + H2O-deactivated ?-MnO2 catalyst throughout the mild thermal treatment, achieving complete regeneration of its own NO disposal ability. This strategy was proven to be universally applicable to other Mn-based catalysts.
引用
收藏
页码:14737 / 14746
页数:10
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