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使用氯掺杂质子化聚吡咯@MWCNTs 复合膜去除和回收气态元素汞。

Removal and Recovery of Gaseous Elemental Mercury Using a Cl-Doped Protonated Polypyrrole@MWCNTs Composite Membrane.

机构信息

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, PR China.

MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, PR China.

出版信息

Environ Sci Technol. 2022 Mar 15;56(6):3689-3698. doi: 10.1021/acs.est.1c07594. Epub 2022 Feb 28.

Abstract

Due to the restrictions on mercury mining, recovering the mercury from mercury-containing waste is attracting increasing attention. This study successfully achieved the removal and recovery of gaseous elemental mercury (Hg) by using membrane technology. A novel composite membrane of Cl-doped protonated polypyrrole-coated multiwall carbon nanotubes (Cl-PPy@MWCNTs) was fabricated in which MWCNTs acted as the framework to support the active component Cl-PPy. The morphology, structure, and composition of the prepared membranes were determined by field emission scanning electron microcopy, energy-dispersive spectroscopy, X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, etc. The composite membrane exhibited an excellent performance in Hg removal (97.3%) at a high space velocity of 200,000 h. The dynamical adsorption capacity of Hg was 3.87 mg/g when the Hg breakthrough reached 10%. The adsorbed Hg could be recovered/enriched via a leaching process using acidic NaCl solution; meanwhile, the membrane was regenerated. The recovered mercury was identified in the form of Hg, with a recovery efficiency of over 99%. Density functional theory calculations and mechanism analysis clarified that the electrons of Hg transported to the delocalized electron orbits of protonated PPy and then combined with Cl to form HgCl/HgCl. Finally, we first demonstrated that the analogous protonated conductive polymers (e.g., polyaniline) also possessed good Hg removal ability, implying that such species may offer more outstanding answers and attract attention in future.

摘要

由于对汞矿开采的限制,从含汞废物中回收汞越来越受到关注。本研究成功地利用膜技术实现了气态元素汞(Hg)的去除和回收。通过将 MWCNTs 作为支撑活性组分 Cl-PPy 的骨架,制备了一种新型的 Cl 掺杂质子化聚吡咯涂层多壁碳纳米管(Cl-PPy@MWCNTs)复合膜。采用场发射扫描电子显微镜、能量色散光谱仪、X 射线光电子能谱仪、傅里叶变换红外光谱仪等对制备的膜进行了形貌、结构和组成的测定。该复合膜在 200,000 h 的高气速下表现出优异的 Hg 去除性能(97.3%)。当 Hg 穿透达到 10%时,Hg 的动态吸附容量为 3.87 mg/g。吸附的 Hg 可以通过使用酸性 NaCl 溶液的浸出过程回收/富集,同时膜得到再生。回收的汞以 Hg 的形式存在,回收效率超过 99%。密度泛函理论计算和机理分析表明,Hg 的电子迁移到质子化 PPy 的离域电子轨道上,然后与 Cl 结合形成 HgCl/HgCl。最后,我们首次证明类似的质子化导电聚合物(如聚苯胺)也具有良好的 Hg 去除能力,这表明此类物质可能在未来提供更出色的答案并引起关注。

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