化学
催化作用
硫黄
吸附
漫反射红外傅里叶变换
硫化物
分解
无机化学
反应机理
光化学
ZSM-5型
化学工程
有机化学
沸石
光催化
工程类
作者
Rui Tian,Jichang Lu,Zhipeng Xu,Wenjun Zhang,Jiangping Liu,Langlang Wang,Yibing Xie,Ye Zhao,Xiaohua Cao,Yongming Luo
标识
DOI:10.1021/acs.est.2c04033
摘要
The competitive adsorption behavior, the synergistic catalytic reaction, and deactivation mechanisms under double components of sulfur-containing volatile organic compounds (VOCs) are a bridge to solve their actual pollution problems. However, they are still unknown. Herein, simultaneous catalytic decomposition of methyl mercaptan (CH3SH) and ethyl mercaptan (C2H5SH) is investigated over lanthanum (La)-modified ZSM-5, and kinetic and thermodynamic results confirm a great difference in the adsorption property and catalytic transformation behavior. Meanwhile, the new synergistic reaction and deactivation mechanisms are revealed at the molecular level by combining with in situ diffuse reflectance infrared spectroscopy (in situ DRIFTS) and density functional theory (DFT) calculations. The CH3CH2* and SH* groups are presented in decomposing C2H5SH, while the new species of CH2*, active H* and S*, instead of CH3* and SH*, are proved as the key elementary groups in decomposing CH3SH. The competitive recombining of SH* in C2H5SH with highly active H* in dimethyl sulfide (CH3SCH3), an intermediate in decomposing CH3SH, would aggravate the deposition of carbon and sulfur. La/ZSM-5 exhibits potential environmental application due to the excellent stability of 200 h and water resistance. This work gives an understanding of the adsorption, catalysis, reaction, and deactivation mechanisms for decomposing double components of sulfur-containing VOCs.
科研通智能强力驱动
Strongly Powered by AbleSci AI