Moderate Dealumination of Zeolites via Chelation to Facilitate Pt Anchoring and Toluene Removal.

Abstract

Zeolites are promising materials for volatile organic compound (VOC) adsorption and catalytic oxidation, where tuning their structure via defect engineering can enhance adsorption capacity and active metal dispersion. In this study, a concentration-sensitive chelation strategy using diethylenetriaminepentaacetic acid (DTPA) was developed to achieve moderate dealumination for Beta and Y zeolites. For Y zeolite, 0.1 M DTPA treatment increased the toluene adsorption capacity from 59 to 110 mg/g. After platinum (Pt) loading, both DTPA-modified Beta- and Y-based catalysts showed improved toluene oxidation efficiency compared to their unmodified counterparts. Remarkably, the Y-DTPA-0.01-Pt catalyst achieved 90% toluene conversion at 150 °C with CO₂ selectivity above 90%. DRIFTS and H₂-TPR results confirmed that moderate dealumination by DTPA generated silanol defects in zeolite Y that strongly anchored Pt²⁺ in a highly dispersed form and suppressed PtO formation. Severe dealumination using 0.1 M DTPA created larger defects that favored the aggregation of Pt⁰ clusters whilst causing significant loss in the micropores, thus reducing the Pt loading content and catalytic activity. This work demonstrates a simple and effective approach to optimize zeolite-based catalysts by controlling defect formation through controllable chelation, offering new insights into VOC abatement via tailored support design.