期刊
DALTON TRANSACTIONS
卷 48, 期 16, 页码 5285-5291出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9dt00395a
关键词
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资金
- National Natural Science Foundation of China [21671019, 21871026, 21771020]
- 973 Program [2014CB932103]
The Keggin-type mono-transition-metal-substituted [PW11M(H2O)O-39](5-) (PW11M, M = Ni, Co, Cu) were intercalated into Zn2Cr-based layered double hydroxide (Zn2Cr-LDH) by an exfoliation-reassembly method and the synthesized Zn2Cr-LDH-PW11M composites were thoroughly characterized by Fourier transform infrared (FT-IR) spectroscopy, powder X-ray diffraction (PXRD), solid state P-31 nuclear magnetic resonance (P-31 NMR) spectroscopy, thermogravimetric analysis (TGA), inductively coupled plasma atomic emission spectroscopy (ICP-AES), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The three composites can be used as heterogeneous catalysts to promote the oxidative decontamination of the sulfur mustard simulant 2-chloroethyl ethyl sulfide (CEES). Interestingly, a cooperative effect between the PW11M cluster and Zn2Cr-LDH is evidenced by the fact that the composites have a higher catalytic performance than either of the individual constituents alone. The catalytic activity of Zn2Cr-LDH-PW11M is significantly influenced by the substituted transition metals, showing the order: Zn2Cr-LDH-PW11Ni > Zn2Cr-LDH-PW11Co > Zn2Cr-LDH-PW11Cu. Under ambient conditions, the Zn2Cr-LDH-PW11Ni composite can convert 98% of CEES in 3 h using nearly stoichiometric 3% aqueous H2O2 with the selectivity of 94% for the nontoxic product 2-chloroethyl ethyl sulfoxide (CEESO). Moreover, the decontaminating material, Zn2Cr-LDH-PW11Ni, is stable to leaching and can be readily reused for up to ten cycles without obvious loss of its activity.
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