Cu/HZSM-5 Sorbent Treated by NH3 Plasma for Low-Temperature Simultaneous Adsorption-Oxidation of H2S and PH3

被引:45
作者
Feng, Jiayu [1 ]
Wang, Fei [1 ]
Wang, Chi [2 ]
Li, Kai [1 ]
Sun, Xin [1 ]
Ning, Ping [1 ,3 ]
机构
[1] Kunming Univ Sci & Technol, Fac Environm Sci & Engn, Kunming 650500, Yunnan, Peoples R China
[2] Kunming Univ Sci & Technol, Fac Chem Engn, Kunming 650500, Yunnan, Peoples R China
[3] Kunming Univ Sci & Technol, Natl Reg Engn Ctr Recovery Waste Gases Met & Chem, Kunming 650500, Yunnan, Peoples R China
关键词
plasma; H2S; PH3; adsorption-oxidation; HYDROGEN-SULFIDE; REACTIVE ADSORPTION; CATALYTIC-OXIDATION; NI/AL2O3; CATALYST; METAL-OXIDES; IRON-OXIDE; GAS; CONVERSION; PURIFICATION; PERFORMANCE;
D O I
10.1021/acsami.1c02584
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
In this study, an NH3 plasma-treated Cu/HZSM-5 sorbent was introduced to simultaneously remove H2S and PH3 in low-temperature and low-oxygen environments. The effects of the Cu loading amounts, modification methods, and plasma-treatment conditions on the adsorption-oxidation performance of the sorbents were investigated. From the performance test results, the sorbent treated by NH3 plasma with the specific energy input (SEI, electrical input energy to the unit volume of gas) value of 1 J.mL(-1) (Cu/HZSM-5-[S1]) was identified as having the highest breakthrough capacities of 108.9 mg S.g(-1) and 150.9 mg P.g(-1) among all of the materials tested. After three times of regeneration, the sorbent can still maintain the ideal performance. The results of Fourier transform infrared (FT-IR) spectroscopy and CO2 temperature-programmed desorption (CO2-TPD) indicated that the NH3 plasma treatment can introduce amino groups (functional groups) onto the sorbent surface, which greatly increases the number and strength of the basic sites on the sorbent surface. Results of N-2 adsorption/desorption isotherms and scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS) showed that the morphology of the sorbent changed after the plasma treatment, which exposed more active sites (copper species). In situ IR spectra showed that the amino groups are continuously consumed during the reaction process, indicating that these amino groups can help sorbents to capture gas molecules. Moreover, Xray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses indicated that CuO is the main active species and the consumption of CuO and accumulation of the reaction products on the surface and inner pores of the sorbent are the primary reasons for the deactivation of the sorbent.
引用
收藏
页码:24670 / 24681
页数:12
相关论文
共 59 条
[41]   Promotional effect of acidic oxide on catalytic activity and N2 selectivity over CeO2 for selective catalytic reduction of NOx by NH3 [J].
Song, Zhongxian ;
Liu, Pan ;
Fu, Yongmei ;
Liu, Hongpan ;
Huang, Zhenzhen ;
Kang, Haiyan ;
Mao, Yanli ;
Liu, Biao ;
Guo, Yifei .
APPLIED ORGANOMETALLIC CHEMISTRY, 2019, 33 (06)
[42]   SCR of NOx with NH3 over Cu/NaZSM-5 and Cu/HZSM-5 in the presence of decane [J].
Sultana, Asima ;
Nanba, Tetsuya ;
Haneda, Masaaki ;
Hamada, Hideaki .
CATALYSIS COMMUNICATIONS, 2009, 10 (14) :1859-1863
[43]   Low temperature catalytic oxidation of nitric oxide over the Mn-CoOx catalyst modified by nonthermal plasma [J].
Tang, Xiaolong ;
Gao, Fengyu ;
Xiang, Ying ;
Yi, Honghong ;
Zhao, Shunzheng .
CATALYSIS COMMUNICATIONS, 2015, 64 :12-17
[44]   MnOx Catalysts Modified By Nonthermal Plasma For NO Catalytic Oxidation [J].
Tang, Xiaolong ;
Li, Kai ;
Yi, Honghong ;
Ning, Ping ;
Xiang, Ying ;
Wang, Jiangen ;
Wang, Chi .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (18) :10017-10028
[45]   Catalytic decomposition of toxic phosphine gas on the developed nickel ferrite nanocrystals supported by Halloysite nanotubes [J].
Tang, Xuejiao ;
Xue, Jingjing ;
Xing, Cheng .
APPLIED SURFACE SCIENCE, 2020, 530
[46]   Catalytic activity of H-ZSM-5 and Cu-HZSM-5 zeolites of medium SiO2/Al2O3 ratio in conversion of n-hexane to aromatics [J].
Tursunov, Obid ;
Kustov, Leonid ;
Tilyabaev, Zaid .
JOURNAL OF PETROLEUM SCIENCE AND ENGINEERING, 2019, 180 :773-778
[47]   Plasma-Enhanced Catalytic Synthesis of Ammonia over a Ni/Al2O3 Catalyst at Near-Room Temperature: Insights into the Importance of the Catalyst Surface on the Reaction Mechanism [J].
Wang, Yaolin ;
Craven, Michael ;
Yu, Xiaotong ;
Ding, Jia ;
Bryant, Paul ;
Huang, Jun ;
Tu, Xin .
ACS CATALYSIS, 2019, 9 (12) :10780-10793
[48]   Preparation of Ce0.6-Cu60/Al40-[O] catalyst and role of CeO2/CuO in simultaneous removal of H2S and PH3 [J].
Wang, Yingwu ;
Lin, Qiang ;
Ning, Ping ;
Wang, Chi ;
Sun, Xin ;
Li, Kai .
JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS, 2018, 87 :44-53
[49]   Reaction behaviors of CH3CN catalytic combustion over CuCeOx-HZSM-5 composite catalysts: The mechanism of enhanced N2 selectivity [J].
Wang, Yuxing ;
Ying, Qingji ;
Zhang, Yaoyu ;
Liu, Yue ;
Wu, Zhongbiao .
APPLIED CATALYSIS A-GENERAL, 2020, 590
[50]   Catalyst Preparation with Plasmas: How Does It Work? [J].
Wang, Zhao ;
Zhang, Yao ;
Neyts, Erik C. ;
Cao, Xinxiang ;
Zhang, Xiaoshan ;
Jang, Ben W. -L. ;
Liu, Chang-jun .
ACS CATALYSIS, 2018, 8 (03) :2093-2110