Promotional effect of sulfur trioxide (SO3) on elemental mercury removal over Cu/ZSM-5 catalyst

Promotional effect of sulfur trioxide (SO3) on elemental mercury removal over Cu/ZSM-5 catalyst
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三氧化硫(SO3)对Cu/ZSM-5催化剂去除元素汞的促进作用

DOI:
10.1016/j.apsusc.2020.145604
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发表时间:
2020-05
影响因子:
6.7
通讯作者:
Pan Wei-Ping
Pan Wei-Ping
中科院分区:
材料科学1区
文献类型:
--
作者:
Zhang Huicong;Wang Tao;Liu Jun;Zhang Yongsheng;Wang Jiawei;Sun Baomin;Pan Wei-Ping

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采用Cu/ZSM-5分子筛研究了SO 3对脱汞的影响。SO2的加入降低了Hg 0的去除率,但在200 °C下引入21 ppm的SO 3后,Hg 0的去除率从82%提高到95%。在400 °C时,SO2对脱汞的抑制作用减弱,SO 3对脱汞的促进作用显著增强。HgSO 4是SO 3存在下催化剂上形成的主要汞物种。原位红外光谱结果表明,在SOx(SO2和SO 3)存在下,催化剂表面产生了大量的硫相关峰。当反应气氛中SO2和SO 3共存时,SO2吸附峰减弱。这是由于SO 3抑制了SO2的吸附。Hg 0引入后,SO 3的吸附峰最明显,随后逐渐消耗。同时,催化剂表面出现了硫酸根峰。这表明SO 3优先吸附在催化剂上形成Hg 0氧化为HgSO 4的活性位。与200 °C相比,400 ° C时SO 3在催化剂上的吸附得到了促进,这直接促进了Hg 0的脱除。
The Cu/ZSM-5 was used to study the effects of SO3on mercury removal. The addition of SO2decreased the Hg0removal efficiency but the efficiency increased from 82% to 95% after 21 ppm SO3was introduced at 200 °C. The inhibition effect of SO2on mercury removal was weakened at 400 °C and the promotion effect of SO3on mercury removal was enhanced significantly. HgSO4was the main mercury species formed on the catalyst in the presence of SO3. Thein-situFTIR results showed a large number of S-related peaks were generated on the surface of the catalyst with SOx(SO2and SO3). The peak of adsorbed SO2weakened when SO2and SO3coexisted in the reaction atmosphere. This is due to the SO3inhibiting the adsorption of SO2. The peak of adsorbed SO3was the most obvious and was then gradually consumed after Hg0introduced. Meanwhile, the peak of sulphate appeared on the surface of the catalyst. This indicated SO3preferentially adsorbed on the catalyst to form active sites for oxidizing Hg0to HgSO4. The adsorption of SO3on the catalyst was promoted at 400 °C, compared with 200 °C, which directly contributed to the enhancement of Hg0removal.
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