4.8 Article

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

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 6, Pages 3689-3698

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c07594

Keywords

elemental mercury removal; membrane method; polypyrrole; multiwall carbon nanotubes; flue gas

Funding

  1. Natural Science Foundation of China [52170108, 51978262, 52000067]
  2. Natural Science Foundation of Hebei [E2021502002, E2020502033]
  3. Hebei Key Laboratory of Mineral Resources and Ecological Environment Monitoring [HBMREEM202102]

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The study focused on removing and recovering gaseous elemental mercury (Hg-0) using a novel composite membrane technology, achieving high efficiency and excellent performance. Mercury was successfully recovered and the membrane regenerated via a leaching process. Mechanism analysis clarified the process of removing Hg-0 from the system.
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-0) 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(-1). The dynamical adsorption capacity of Hg-0 was 3.87 mg/g when the Hg-0 breakthrough reached 10%. The adsorbed Hg-0 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 Hg2+, with a recovery efficiency of over 99%. Density functional theory calculations and mechanism analysis clarified that the electrons of Hg-0 transported to the delocalized electron orbits of protonated PPy and then combined with Cl- to form Hg2Cl2/HgCl2. Finally, we first demonstrated that the analogous protonated conductive polymers (e.g., polyaniline) also possessed good Hg-0 removal ability, implying that such species may offer more outstanding answers and attract attention in future.

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