| Title: | Unraveling the Synergistic Reaction and the Deactivation Mechanism for the Catalytic Degradation of Double Components of Sulfur-Containing VOCs over ZSM-5-Based Materials |
| Author(s): | Tian R; Lu J; Xu Z; Zhang W; Liu J; Wang L; Xie Y; Zhao Y; Cao X; Luo Y; |
| Address: | "Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming650500, P. R. China. The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of Yunnan Province, Kunming650500, P. R. China. The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming650500, P. R. China. Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming650500, P. R. China" |
| ISSN/ISBN: | 1520-5851 (Electronic) 0013-936X (Linking) |
| Abstract: | "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 (CH(3)SH) and ethyl mercaptan (C(2)H(5)SH) 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 CH(3)CH(2)* and SH* groups are presented in decomposing C(2)H(5)SH, while the new species of CH(2)*, active H* and S*, instead of CH(3)* and SH*, are proved as the key elementary groups in decomposing CH(3)SH. The competitive recombining of SH* in C(2)H(5)SH with highly active H* in dimethyl sulfide (CH(3)SCH(3)), an intermediate in decomposing CH(3)SH, 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" |
| Keywords: | carbon and sulfur deposition competitive adsorption deactivation mechanism sulfur-containing VOCs synergistic catalytic decomposition; |
| Notes: | "PublisherTian, Rui Lu, Jichang Xu, Zhizhi Zhang, Wenjun Liu, Jiangping Wang, Langlang Xie, Yibing Zhao, Yutong Cao, Xiaohua Luo, Yongming eng 2022/10/06 Environ Sci Technol. 2022 Oct 4. doi: 10.1021/acs.est.2c04033" |
