Catalytic oxidation of 2-chlorophenol in confined channels of ZSM-48

Kuen Song Lin; H. Paul Wang

doi:10.1021/jp0043874

Catalytic oxidation of 2-chlorophenol in confined channels of ZSM-48

Kuen Song Lin, H. Paul Wang

Department of Environmental Engineering

Research output: Contribution to journal › Article › peer-review

23 Citations (Scopus)

Abstract

Experimentally, the formation of undesired heavy polycyclic aromatic hydrocarbons (PAHs) and chlorinated phenol byproducts in the supercritical water oxidation (SCWO) of 2-chlorophenol (2CP) catalyzed by CuO/ZSM-48 at 673 K was significantly reduced. The reduction was attributed to the byproduct shape selectivity of the confined ZSM-48 channels. Speciation of active copper species in ZSM-48 was studied by X-ray absorption near edge structural (XANES) and extended X-ray absorption fine structural (EXAFS) spectroscopies, which suggested the existence of (Cu₃O₂)_n (n_max = 150, cross section of about 1.9 Å) clusters in the channels of ZSM-48 (5.3-5.8 Å). The diffusion coefficients of the copper-oxide cluster (determined by low-temperature electron paramagnetic resonance (EPR) spectroscopy) were greater than that of the tight-fit 2CP in the channels of ZSM-48 by at least three orders. Since the catalytic SCWO of 2CP was extremely fast, we consider the possibility that copper-oxide clusters were relatively mobile if compared with the 2CP in the confined channels of ZSM-48.

Original language	English
Pages (from-to)	4956-4960
Number of pages	5
Journal	Journal of Physical Chemistry B
Volume	105
Issue number	21
DOIs	https://doi.org/10.1021/jp0043874
Publication status	Published - 2002 May 31

All Science Journal Classification (ASJC) codes

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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title = "Catalytic oxidation of 2-chlorophenol in confined channels of ZSM-48",

abstract = "Experimentally, the formation of undesired heavy polycyclic aromatic hydrocarbons (PAHs) and chlorinated phenol byproducts in the supercritical water oxidation (SCWO) of 2-chlorophenol (2CP) catalyzed by CuO/ZSM-48 at 673 K was significantly reduced. The reduction was attributed to the byproduct shape selectivity of the confined ZSM-48 channels. Speciation of active copper species in ZSM-48 was studied by X-ray absorption near edge structural (XANES) and extended X-ray absorption fine structural (EXAFS) spectroscopies, which suggested the existence of (Cu3O2)n (nmax = 150, cross section of about 1.9 {\AA}) clusters in the channels of ZSM-48 (5.3-5.8 {\AA}). The diffusion coefficients of the copper-oxide cluster (determined by low-temperature electron paramagnetic resonance (EPR) spectroscopy) were greater than that of the tight-fit 2CP in the channels of ZSM-48 by at least three orders. Since the catalytic SCWO of 2CP was extremely fast, we consider the possibility that copper-oxide clusters were relatively mobile if compared with the 2CP in the confined channels of ZSM-48.",

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T1 - Catalytic oxidation of 2-chlorophenol in confined channels of ZSM-48

AU - Lin, Kuen Song

AU - Wang, H. Paul

PY - 2002/5/31

Y1 - 2002/5/31

N2 - Experimentally, the formation of undesired heavy polycyclic aromatic hydrocarbons (PAHs) and chlorinated phenol byproducts in the supercritical water oxidation (SCWO) of 2-chlorophenol (2CP) catalyzed by CuO/ZSM-48 at 673 K was significantly reduced. The reduction was attributed to the byproduct shape selectivity of the confined ZSM-48 channels. Speciation of active copper species in ZSM-48 was studied by X-ray absorption near edge structural (XANES) and extended X-ray absorption fine structural (EXAFS) spectroscopies, which suggested the existence of (Cu3O2)n (nmax = 150, cross section of about 1.9 Å) clusters in the channels of ZSM-48 (5.3-5.8 Å). The diffusion coefficients of the copper-oxide cluster (determined by low-temperature electron paramagnetic resonance (EPR) spectroscopy) were greater than that of the tight-fit 2CP in the channels of ZSM-48 by at least three orders. Since the catalytic SCWO of 2CP was extremely fast, we consider the possibility that copper-oxide clusters were relatively mobile if compared with the 2CP in the confined channels of ZSM-48.

AB - Experimentally, the formation of undesired heavy polycyclic aromatic hydrocarbons (PAHs) and chlorinated phenol byproducts in the supercritical water oxidation (SCWO) of 2-chlorophenol (2CP) catalyzed by CuO/ZSM-48 at 673 K was significantly reduced. The reduction was attributed to the byproduct shape selectivity of the confined ZSM-48 channels. Speciation of active copper species in ZSM-48 was studied by X-ray absorption near edge structural (XANES) and extended X-ray absorption fine structural (EXAFS) spectroscopies, which suggested the existence of (Cu3O2)n (nmax = 150, cross section of about 1.9 Å) clusters in the channels of ZSM-48 (5.3-5.8 Å). The diffusion coefficients of the copper-oxide cluster (determined by low-temperature electron paramagnetic resonance (EPR) spectroscopy) were greater than that of the tight-fit 2CP in the channels of ZSM-48 by at least three orders. Since the catalytic SCWO of 2CP was extremely fast, we consider the possibility that copper-oxide clusters were relatively mobile if compared with the 2CP in the confined channels of ZSM-48.

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Catalytic oxidation of 2-chlorophenol in confined channels of ZSM-48

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