Mass-Transfer Enhancement in the CO2 Oxidative Dehydrogenation of Propane over GaN Supported on Zeolite Nanosheets with a Short b-Axis and Hierarchical Pores

脱氢 丙烷 沸石 催化作用 传质 材料科学 化学工程 碳纤维 丙烯 焦炭 漫反射红外傅里叶变换 光化学 化学 光催化 有机化学 色谱法 复合材料 复合数 工程类
作者
Zhan‐Jun Zhu,Zhen‐Hong He,Yue Tian,Sen-Wang Wang,Yongchang Sun,Kuan Wang,Weitao Wang,Zhifang Zhang,Jiajie Liu,Zhao‐Tie Liu
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:14 (13): 10376-10391 被引量:8
标识
DOI:10.1021/acscatal.4c02599
摘要

The CO2 oxidative dehydrogenation of propane (CO2–ODHP) is a highly important reaction for not only producing large amounts of propylene but also consuming the CO2 resource. GaN/zeolite catalysts deliver preferable activity in the reaction. However, similar to Pt- and Cr-based catalysts, there are shortcomings such as poor stability and coke accumulation, especially when operated at temperatures higher than 550 °C. Generally, carbon deposition is one of the main reasons for catalyst deactivation. The limited mass transfer greatly aggravates the deposited carbon formation, since carbon precursors could not be removed in time. In the present work, we modified zeolites with a short b-axis and hierarchical pores, which could offer a shorter diffusion distance and pore-rich structure to enhance the mass transfer. Thanks to this enhancement, the catalyst offers an initial propane conversion of 68.0% with a yield of 39.4% to propylene, surpassing other reported GaN/zeolite catalysts to data. Importantly, the catalyst showed a low loss rate of activity and a low amount of deposited carbon, which was easily regenerated compared with those of other catalysts without a short b-axis or hierarchical pores. Density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirmed that the reaction involves a coupling reaction of direct dehydrogenation and CO2 reduction via reverse water–gas shift reaction, and CO2 participates in the reaction. The present work sheds light on designing an efficient catalyst for CO2–ODHP via a mass transfer-boosted strategy and, importantly, is expected to provide inspiration in constructing a zeolite with a short b-axis and hierarchical pores.
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