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In-situ synthesis of monodispersed CuxO heterostructure on porous carbon monolith for exceptional removal of gaseous Hg0

Journal 2019 · IF 14.229 · 发表于 2019 年 12 月 23 日
作者: Liyuan Zhang,Shu Yang,Yuekun Lai,Hui Liu,Yiang Fan,Cao Liu,Haiying Wang,Liyuan Chai
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摘要

Gaseous Hg 0 is one of the most deadly and hard-to-dispose pollutants. The oxidation of Hg 0 is a promising route, but the rational design and synthesis of highly efficient catalysts still remain grand challenges. Herein, CuO@Cu 2 O (or Cu x O) heterostructured nanoparticles uniformly monodispersing on porous carbon monolith were designed and successfully synthesized using oligo( m -phenylenediamine)-Cu 2+ complex as raw material. The Cu x O-carbon catalyst contains ∼28 wt% of Cu. Based on density functional theory calculation, the CuO@Cu 2 O junction interfaces can accelerate the Hg 0 oxidation by significantly reducing the energy barriers of reaction. Only 1 mg of the catalyst can catalyze the oxidation of more than 90 % of Hg 0 with [HCl] = 0.5 ppm, [O 2 ] = 6 vol%, T = 150 °C. The poisoning effect of either SO 2 or H 2 O on the catalysts is weak. Moreover, a long-term test confirmed that the Hg 0 oxidation rate can maintain more than 90 % even in the co-presence of SO 2 (5000 ppm) and H 2 O (10 vol%).