CaO-Promoted Lattice Oxygen Activation and Antichlorine Poisoning over Mullite for Catalytic Chlorobenzene Combustion
CaO-Promoted Lattice Oxygen Activation and Antichlorine Poisoning over Mullite for Catalytic Chlorobenzene Combustion
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DOI：
10.1021/acscatal.3c01871
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发表时间：
2023-07
期刊：
影响因子：
12.9
通讯作者：
Yi Liu;Fanyu Wang;Fei Xie;Jiamin Zheng;Jintong Lan;Furong Guo;Yifei Sun;Lizhi Zhang;
中科院分区：
文献类型：
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作者：
Yi Liu;Fanyu Wang;Fei Xie;Jiamin Zheng;Jintong Lan;Furong Guo;Yifei Sun;Lizhi Zhang;
利用催化燃烧技术降解含氯挥发性有机化合物(Cl-VOCs)存在有毒副产物生成和催化剂氯中毒的悖论。针对氯苯在SmMn2O5催化剂上催化燃烧性能较差的问题，提出了CaO助燃策略。CaO协同作用的SmMn2O5的T90比未改性和惰性SiO_2复合的SmMn2O5分别降低了142℃和125℃。综合表征结果证实了CaO的协同作用导致了CaO向SmMn2O5的电子转移，从而减少了Mn和O原子之间的轨道重叠，从而激活了晶格氧(Olatt)。活化的Olattenable可使氯苯在275℃的较低温度下完全燃烧，在此温度下不会产生有毒副产品。此外，脱氯中心从SmMn2O5到CaO的转换避免了SmMn2O5上活性中心的氯中毒，从而使CaO协同作用的SmMn2O5具有显著的稳定性。
The degradation of chlorine-containing volatile organic compounds (Cl–VOCs) utilizing catalytic combustion technology is subject to the paradox of toxic byproduct formation and catalyst chlorine poisoning. Herein, a CaO-assisted strategy is proposed to resolve the awkward stuff for improving the catalytic combustion performance of chlorobenzene on SmMn2O5. The CaO-collaborated SmMn2O5exhibits a significant decrease inT90by 142 and 125 °C compared with unmodified and inert SiO2-composited SmMn2O5, respectively. The integrated characterization results confirm that CaO collaboration causes electron transfer from CaO to SmMn2O5, resulting in a reduction of the orbital overlap between Mn and O atoms to activate lattice oxygen (Olatt). The activated Olattenables chlorobenzene to combust completely at a lower temperature of 275 °C at which toxic byproducts are not generated. Furthermore, the switching of the dechlorination site from SmMn2O5to CaO avoids chlorine poisoning of active sites on SmMn2O5and thus endows CaO-collaborated SmMn2O5with prominent stability.