期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 54, 期 8, 页码 5249-5257出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.9b07524
关键词
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资金
- National Key R&D Program of China [2017YFC0806300]
- National Natural Science Foundation of China [21677096]
A novel, atomically dispersed carbon-based sorbent was synthesized by anchoring manganese atoms with N atoms for the capture of gaseous elemental Hg (Hg-0). Oxygen atoms were also introduced into the synthesis process to adjust the oxidizing ability of the Mn atoms. High-valence Mn (Mn4+) anchored by the O and N atoms (Mn-O/N-C) in the carbon-based materials provided more exposed active sites. The mercury removal efficiency of the composite exceeded 99%. The composite with a Mn loading of 0.9 wt % exhibited high affinity for Hg-0, and the capacity for He adsorption within 275 min at room temperature reached 16.95 mg.g(-1). The Mn utilization was similar to 56.61%, which is much larger than that of reported Mn-based oxide sorbents. The atomic-level distribution of Mn was well evidenced by aberration-corrected high-angle annular darkfield scanning transmission electron microscopy. Density functional theory calculations were conducted to evaluate the energy for adsorption of He on Mn-O/N-C. The results indicated that the amount of N and O atoms in the Mn coordination environment determined the Hg-0 adsorption energy, and the presence of five optimized Mn adsorption structures in Mn-O/N-C was confirmed by Hg temperature-programmed desorption analysis. These materials may be utilized for mercury removal from disposal sites with high concentrations of mercury, broken mercury-containing lamps, or mercurial thermometers. The strategy of atomic dispersion during synthesis of the materials and adjusting the oxidizing ability in the single-atom strategy may be helpful for the development of environmentally benign functional materials.
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