Elucidating the role of confinement and shielding effect over zeolite enveloped Ru catalysts for propane low temperature degradation

Jinxiong Tao; Qiuli Zhang; Yonghua Zhao; Hunan Chen; Wenming Liu; Yuzhao He; Yuni Yin; Tianyao He; Jian Chen; Xufang Wang; Daishe Wu; Honggen Peng

doi:10.1016/j.chemosphere.2022.134884

Elucidating the role of confinement and shielding effect over zeolite enveloped Ru catalysts for propane low temperature degradation

Chemosphere. 2022 Sep:302:134884. doi: 10.1016/j.chemosphere.2022.134884. Epub 2022 May 9.

Authors

Jinxiong Tao¹, Qiuli Zhang¹, Yonghua Zhao², Hunan Chen², Wenming Liu¹, Yuzhao He³, Yuni Yin³, Tianyao He², Jian Chen⁴, Xufang Wang⁴, Daishe Wu², Honggen Peng⁵

Affiliations

¹ Key Laboratory of Jiangxi Province for Environment and Energy Catalysis, College of Chemistry, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China.
² Key Laboratory of Poyang Lake Environment and Resource Utilization, Ministry of Education, School of Resources Environmental and Chemical Engineering, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China.
³ Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, 510006, China.
⁴ Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua, 321004, China.
⁵ Key Laboratory of Jiangxi Province for Environment and Energy Catalysis, College of Chemistry, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China; Key Laboratory of Poyang Lake Environment and Resource Utilization, Ministry of Education, School of Resources Environmental and Chemical Engineering, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi, 330031, China. Electronic address: penghonggen@ncu.edu.cn.

PMID: 35551937
DOI: 10.1016/j.chemosphere.2022.134884

Abstract

Volatile organic compounds (VOCs) are the main precursor for ozone formation and hazardous to human health. Light alkane as one of the typical VOCs is difficult to degrade to CO₂ and H₂O by catalytic degradation method due to its strong C-H bond. Herein, a series of ultrafine Ru nanoclusters (<0.95 nm) enveloped in silicalite-1 (S-1) zeolite catalysts were designed and prepared by a simple one-pot method and applied for catalytic degradation of propane. The results demonstrate that the enveloped Ru₁@S-1 catalyst has excellent propane degradation performance. Its T₉₅ is as low as 294 °C with moisture, and the turnover frequency (TOF) value is up to 5.07 × 10^-3 s^-1, evidently higher than that of the comparison supported catalyst (Ru₁/S-1). Importantly, Ru₁@S-1 exhibits superior thermal stability, water resistance and recyclability, which should be attributed to the confinement and shielding effect of the S-1 shell. The in-situ DRIFTS result reveals that the propane degradation over Ru₁@S-1 follows the Mars-van-Krevelen (MvK) mechanism, where the hydroxy from the framework of zeolite can provide the active oxygen species. Our work provides a new candidate and guideline for an efficient and stable catalyst for the low-temperature degradation of the light alkane VOCs.

Keywords: Propane degradation; Sinter and water resistance; Ultrafine Ru nanoclusters; Volatile organic compounds; Zeolite enveloped catalysts.

MeSH terms

Alkanes
Catalysis
Humans
Propane
Temperature
Volatile Organic Compounds* / chemistry
Zeolites* / chemistry

Substances

Alkanes
Volatile Organic Compounds
Zeolites
Propane