Ultrafine Au nanoparticles confined in three-dimensional mesopores of MCM-48 for efficient and regenerable Hg0 removal sorbent in H2S and H2O containing natural gas

被引:35
作者
Wang, Juan [1 ]
Zhang, Mingzhu [1 ]
Li, Ge [2 ]
Zhou, Yifan [1 ]
Zhang, Yuhan [1 ]
Zhang, Wenrui [1 ]
Jiao, Tiantian [1 ]
Zhang, Yaqing [1 ]
Liang, Peng [1 ]
Zhang, Huawei [3 ]
机构
[1] Shandong Univ Sci & Technol, Coll Chem & Biol Engn, Qingdao 266590, Peoples R China
[2] Shandong Anal & Test Ctr, Jinan 250014, Peoples R China
[3] Qingdao Univ Technol, Sch Environm & Municipal Engn, Qingdao 266033, Peoples R China
基金
中国国家自然科学基金;
关键词
Natural gas; Hg-0; removal; Au nanoparticles; MCM-48; zeolite; H2S and H2O tolerance; ELEMENTAL MERCURY; ADSORPTION; CAPTURE; AG; RESISTANCE; CARBON; NANOCOMPOSITE; MECHANISM; ADSORBENT; SURFACE;
D O I
10.1016/j.fuel.2020.119479
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
The H2O and H2S in natural gas are frequently deemed to have inhibitory influences on Hg-0 removal performance of most noble metal based Hg-0 absorbents, it is extremely significant to develop an efficient and regenerable Hg-0 removal absorbent with excellent H2S and H2O tolerance. In the work, the Au/MCM-48 absorbent was controllable synthesized using a facile yet robust method for Hg-0 removal in H2S and H2O containing natural gas. The ultrafine Au nanoparticles with a diameter of 1.4 nm were embedded and uniformly dispersed in the three-dimensional channels of MCM-48. The absorbent of 1 wt% Au achieved a complete Hg-0 capture performance at 60,000 h(-1) and 30 degrees C by forming Au-Hg amalgam, and its Hg-0 adsorption capacity achieved to 7.23 mg.g(-1) at 5% breakthrough. The spent sample could be easily regenerated by thermal treatment without distinct degradation over 5 cycles. The introduction of H2S and H2O in gas flow had an inappreciable impact on Hg-0 removal performance over the Au/MCM-48 absorbent. The excellent Hg-0 adsorption efficiency, outstanding capture capacity and good regeneration performance of the absorbent due to the nano-confinement of MCM-48 channels, which prevents Au nanoparticles from growing and agglomerating. Excellent H2O tolerance is attributed to the good hydrophobicity of MCM-48 modified by trimethylchlorosilane, and the high H2S tolerance is due to the fact that the Au nanoparticles lack reactivity toward H2S. This work provides a promising method for the preparation of effective and regenerable absorbents for demercuration in H2S and H2O containing natural gas.
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页数:9
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