Structural/surface characterization of transition metal element-doped H-ZSM-5 adsorbent for CH3SH removal: identification of active adsorption sites and deactivation mechanism

被引:4
作者
Xie, Yuxuan [1 ]
Peng, Xiao [1 ,4 ]
Song, Xin [1 ,3 ]
Ning, Ping [1 ,3 ]
Sun, Xin [1 ]
Ma, Yixing [1 ,3 ]
Wang, Chi [2 ]
Li, Kai [1 ,3 ]
机构
[1] Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Peoples R China
[2] Kunming Univ Sci & Technol, Fac Chem Engn, Kunming 650500, Peoples R China
[3] Kunming Univ Sci & Technol, Natl Reg Engn Ctr Recovery Waste Gases Met & Chem, Kunming 650500, Peoples R China
[4] Zhaotong Coll, Fac Chem & Chem Engn, Zhaotong 657000, Peoples R China
基金
中国国家自然科学基金;
关键词
CH3SH; Low temperature adsorption; Active acid sites; Cu-modified adsorbent; Sulfur deposition; METHYL MERCAPTAN; CATALYTIC PERFORMANCE; RARE-EARTH; HZSM-5; ZEOLITE; NANOPARTICLES; COPPER; DESULFURIZATION; DECOMPOSITION; DESILICATION; HYDROLYSIS;
D O I
10.1007/s11356-024-32518-4
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
CH3SH is a potential hazard to both chemical production and human health, so controlling its emissions is an urgent priority. In this work, a series of transition metal-loaded H-ZSM-5 adsorbents (Si/Al = 25) (Cu, Fe, Co, Ni, Mn, and Zn) were synthesized through the wet impregnation method and tested for CH3SH physicochemical adsorption at 60( degrees)C. It was shown that the Cu-modified H-ZSM-5 adsorbent was much more active for CH3SH removal due to its abundant strong acid sites than other transition metal-modified H-ZSM-5 adsorbents. The detailed physicochemical properties of various modified H-ZSM-5 adsorbents were characterized by SEM, XRD, N2 physisorption, XPS, H-2-TPR, and NH3-TPD. The effects of metal loading mass ratio, calcination temperature, and acid or alkali modification on the performance of the adsorbent were also investigated, and finally 20% Cu/ZSM-5 was found to have the best adsorption capacity after calcined at 350 degrees C. Additionally, the Cu/ZSM-5 adsorbent modified by sodium bicarbonate could expose more active components, which improved the adsorbent's stability. However, the consumption and reduction of the active component Cu2+ and the accumulation of sulfate during the adsorption process are the main reasons for the deactivation of the adsorbent. In addition, the simultaneous purging of N-2 + O(2 )can effectively restore the adsorption capacity of the deactivated adsorbent and can be used as a potential strategy to regenerate the adsorbent.
引用
收藏
页码:24398 / 24411
页数:14
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