Discovering Surface Structure and the Mechanism of Graphene Oxide-Triggered CeO2–WO3/TiO2 Catalysts for NO Abatement with NH3

催化作用 石墨烯 氧化物 材料科学 X射线光电子能谱 漫反射红外傅里叶变换 吸附 热脱附光谱法 X射线吸收精细结构 拉曼光谱 化学工程 解吸 纳米技术 无机化学 光催化 化学 光谱学 物理化学 冶金 生物化学 光学 量子力学 工程类 物理
作者
Yan Wang,Tong Shi,Qiyuan Fan,Yang Liu,Aiai Zhang,Zhaoqiang Li,Yanheng Hao,Lin Chen,Fenrong Liu,Xiaojun Gu,Shanghong Zeng
出处
期刊:ACS Catalysis 卷期号:12 (14): 8386-8403 被引量:28
标识
DOI:10.1021/acscatal.2c01364
摘要

Tricomponent cerium–tungsten–titanium catalysts have the potential for selective catalytic reduction of NO by NH3, while the accurate modulating of the surface structure and the understanding of the atomic-level mechanism remain extremely challenging. To resolve the conundrum, here, we investigate the modular ternary catalysts through advanced spectroscopic and computational studies. It reveals that the introduction of graphene oxide induces a high dispersion of W and Ce species, resulting in the generation of amorphous W–O–Ce- and Ce–O–Ti-bonding structures on the surface. More importantly, the high dispersion of CeO2 facilitates the formation of abundant oxygen vacancies, which are mobile active sites for adsorption and activation of NO and NH3. Temperature-programmed desorption of NO (NO-TPD) and temperature-programmed desorption of NH3 (NH3-TPD) validate the feasibility of adsorption of NO and NH3 at low temperatures. In situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy of the transient reaction indicates that both NO2 and monodentate nitrate are active intermediates, which can react with the adsorbed NH3 to generate N2 and H2O during catalysis. X-ray absorption fine structure (XAFS), in situ Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS) provide direct evidence for the presence of Ce, W, and Ti interactions. Theoretical simulations prove that the inherent interactions reliably accelerate the conversion efficiency of NOx to N2 by improving the electron transfer on the surface. Furthermore, the Langmuir–Hinshelwood mechanism is thermodynamically more feasible and predominant over the graphene oxide-triggered catalyst.
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