Novel effects of copper precursors on the adsorption and desorption of elemental mercury over copper-based sulfides: Performance, mechanism, and kinetics

Novel effects of copper precursors on the adsorption and desorption of elemental mercury over copper-based sulfides: Performance, mechanism, and kinetics
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铜前驱体对铜基硫化物吸附和解吸元素汞的新影响:性能、机制和动力学

DOI:
10.1016/j.jtice.2022.104636
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发表时间:
2023-01
影响因子:
5.7
通讯作者:
Yang Shijian
Yang Shijian
中科院分区:
工程技术3区
文献类型:
--
作者:
Hou Jinbo;Wang Chang;Ma Yulei;Wang Jian;Mei Jian;Yang Shijian

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研究背景在O2和SO2存在下,Hg0在废CuSx/TiO2单键N [Cu(NO3)2作为Cu的前体]上的吸附量增加,而Hg0的解吸量减少,这可能与硫化前CuO硫酸化生成新的Cu前体(CuSO4)有关。方法:两种不同的Cu前体[即,研究了Cu(NO3)2和CuSO4]对CuSx/TiO2捕集Hg0的影响,比较了Hg0吸附和脱附动力学参数。重要发现:由于CuSO4具有较强的热稳定性,在煅烧后CuSO4基本上保持了其完整的结构,但Cu(NO3)2分解为CuO和Cu2O,因此在硫化过程中,与CuSx/TiO2单键N相比,CuSx/TiO2-S(CuSO4为前体)上既形成了更活泼的S22-,将物理吸附的Hg0氧化为HgS,又形成了更少的不稳定吸附位S0。同时,CuSx/TiO2-S上Hg0物理吸附的不饱和配位量明显大于CuSx/TiO2单键N上的不饱和配位量.因此,Hg0在CuSx/TiO2-S上的吸附量较大,但在CuSx/TiO2-S上的解吸量较小。因此,由CuSO4前体衍生的Cu基硫化物更适合于从冶炼烟气中捕集Hg °。
BackgroundMore Hg0adsorption onto the spent CuSx/TiO2single bondN [Cu(NO3)2as the Cu precursor] in the presence of O2and SO2and less Hg0desorption from it occurred simultaneously after the regeneration, which was likely related to the formation of new Cu precursor (CuSO4from the sulfation of CuO) before the sulfuration. Methods: The effects of two different Cu precursors [i.e., Cu(NO3)2and CuSO4] on the performance of CuSx/TiO2for Hg° capture were investigated by comparing the kinetic parameters of Hg0adsorption and desorption. Significant findings: CuSO4generally retained its intact structure after the calcination due to its strong heat stability, but Cu(NO3)2was decomposed into CuO and Cu2O; therefore, both more active S22−that oxidized the physically adsorbed Hg0to HgS and less S0that provided the unstable adsorption sites were formed on CuSx/TiO2-S (CuSO4as the precursor) during the sulfuration than CuSx/TiO2single bondN. Meanwhile, the amount of unsaturated coordination sites onto CuSx/TiO2-S for Hg0physical adsorption was significantly larger than that onto CuSx/TiO2single bondN. Therefore, not only did Hg0adsorb more onto CuSx/TiO2-S, but it also desorbed less from CuSx/TiO2-S. In consequence, Cu-based sulfides derived from the CuSO4precursor were more suitable for Hg° capture from smelting flue gas.
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