4.7 Article

Charge distribution modulation and morphology controlling of copper selenide for an enhanced elemental mercury adsorption activity in flue gas

期刊

CHEMICAL ENGINEERING JOURNAL
卷 442, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136145

关键词

Elemental mercury; Selenide; Charge distribution; Coal combustion; Flue gas

资金

  1. National Natural Science Foun-dation of China [51906260]
  2. Science and Technology Innovation Program of Hunan Province [2021JJ30851]
  3. Natural Science Foundation of Hunan Province, China [CX20210098]
  4. Postgraduate Scientific Research Innovation Project of Hunan Province [2022-K09, 2022-K52]
  5. Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering [2021YFG0117]
  6. Key Research and Development Program of Sichuan Province

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This study developed a charge distribution modulation strategy to improve the adsorption capacity and adsorption rate of metal selenide ligands for elemental mercury (Hg0) remediation. The modulated copper selenide (Cu2Se) ligand exhibited environmentally stable immobilization of Hg0 as mercury selenide (HgSe) and showed higher adsorption capacity and faster adsorption rate compared to regular Cu2Se. Additionally, the modulation technique allowed for the construction of thinner and larger nanosheets, providing more active sites for binding Hg0. This newly designed method has significant implications for real-world applications.
The abatement of elemental mercury (Hg0) emissions from industrial flue gases remains an enormous challenge. Metal selenides have been demonstrated to be promising Hg0 remediators, and the electron-transfer ability of selenide ligands is one of the key factors that determining the uptake capacity and adsorption rate of Hg0. Herein, a charge distribution modulation strategy was developed to generate desired selenide ligands. The selenide ligands on a tutorial sample, copper selenide (Cu2Se), was artificially modulated to -1 valances (Se1-) via electrostatic adsorption of positively charged head groups of cetyltrimethylammonium bromide (CTAB). Unlike other selenide ligand such as Se2-, the Se1- directly acted as an electron acceptor for Hg0 and realize one-step immobilization of Hg0 as environmentally stable mercury selenide (HgSe). Besides, CTAB was beneficial to construct nanosheets with thinner and larger plates, hence facilitated a sufficient exposure of active sites for binding Hg0. Profiting from the above advantages, the Hg0 adsorption capacity of CTAB modulated Cu2Se (Cu2Se-CTAB) was up to 80.2 mg center dot g- 1, about two times higher than that of bare Cu2Se. Meanwhile, the average Hg0 adsorption rate of Cu2Se-CTAB before achieving saturation was 9.99 mg center dot g- 1 center dot h- 1, much faster comparing with 6.90 mg center dot g- 1 center dot h- 1 for regular Cu2Se. The Cu2Se-CTAB showed superior Hg0 adsorption performance at 40-80 degrees C and excellent resistance to flue gas interference, which are crucial for real-world applications. This newly designed method not only provides an excellent Hg0 remediator but also offers a tutorial example for a rational modulation of metal selenides for diverse environmental remediations.

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