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过渡金属元素掺杂 H-ZSM-5 吸附剂去除 CHSH 的结构/表面特性:活性吸附位的鉴定和失活动力学。

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

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, 650500, People's Republic of China.

Faculty of Chemistry and Chemical Engineering, Zhaotong College, Zhaotong, 657000, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2024 Apr;31(16):24398-24411. doi: 10.1007/s11356-024-32518-4. Epub 2024 Mar 5.

Abstract

CHSH 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 CHSH physicochemical adsorption at 60 °C. It was shown that the Cu-modified H-ZSM-5 adsorbent was much more active for CHSH 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, N physisorption, XPS, H-TPR, and NH-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 °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 Cu 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 + O can effectively restore the adsorption capacity of the deactivated adsorbent and can be used as a potential strategy to regenerate the adsorbent.

摘要

CHSH 对化学生产和人类健康都是潜在的危害,因此控制其排放是当务之急。在这项工作中,通过湿浸渍法合成了一系列负载过渡金属的 H-ZSM-5 吸附剂(Si/Al=25)(Cu、Fe、Co、Ni、Mn 和 Zn),并在 60°C 下测试了它们对 CHSH 的物理化学吸附性能。结果表明,由于 Cu 改性的 H-ZSM-5 吸附剂具有丰富的强酸位,因此比其他过渡金属改性的 H-ZSM-5 吸附剂对 CHSH 的去除更具活性。通过 SEM、XRD、N 物理吸附、XPS、H-TPR 和 NH-TPD 对各种改性 H-ZSM-5 吸附剂的详细物理化学性质进行了表征。还研究了金属负载质量比、煅烧温度以及酸或碱改性对吸附剂性能的影响,最终发现 350°C 煅烧的 20%Cu/ZSM-5 具有最佳的吸附容量。此外,用碳酸氢钠改性的 Cu/ZSM-5 吸附剂可以暴露更多的活性成分,从而提高了吸附剂的稳定性。然而,在吸附过程中活性成分 Cu 的消耗和还原以及硫酸盐的积累是吸附剂失活的主要原因。此外,同时吹扫 N+O 可以有效地恢复失活吸附剂的吸附能力,这可以作为一种潜在的吸附剂再生策略。

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