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H2O-Enabled Reversible SO2 Resistance on Separately Dual-Functional Pd–W Sites for Low-Temperature Hydrocarbon Oxidation
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DOI：10.1021/acs.est.6c03881.png)
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Abstract
En 中文
Sulfur dioxide (SO2) poisoning remains a critical challenge for noble-metal catalysts in hydrocarbon oxidation, particularly under industrial humid conditions. H2O is commonly regarded as a detrimental component in SO2-containing exhaust streams where sulfur-water synergistic deactivation prevails. Here we prove that, when combined with rational active-site design, H2O molecules can instead promote SO2-resistance in hydrocarbon oxidation catalysis. A Pd/W–Al2O3 catalyst with spatially separated Pd and W sites exhibits superior low-temperature methyl ethyl ketone (MEK) oxidation activity and unprecedented resistance to SO2 poisoning under both dry and humid conditions. In the absence of water, SO2 is selectively immobilized as SO32– species on W sites, preventing competitive adsorption on Pd and preserving MEK oxidation pathways. Under humid conditions, however, SO2 can be transformed into HSO3– species that interact directly with Pd-bound ketone intermediates. Spectroscopic and theoretical investigations reveal that HSO3– functions as a dynamic proton shuttle, enabling a proton-bridge-assisted C–C bond cleavage pathway that facilitates intermediate conversion and drives reversible recovery from SO2 poisoning. This work demonstrates how H2O molecules fundamentally reshape SO2-catalyst interactions and highlights a general strategy for converting SO2 poisons into reaction promoters through spatially separated dual-functional active sites.
Keywords:
Adsorption
Catalysts
Group 16 compounds
Oxidation
Oxides
MEK oxidation
separately dual-functional sites
reversible SO2 resistance
humidity
surface mechanism
Journal
E
IF:
11.3
Papers:
1.9K
Citations:
1
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Cited Papers