Evolution of VOx on TiO2-ZSM-5 Composite Supports upon K Poisoning and Its Effects on Ultralow Temperature NH3–SCR

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Jiaying Li, Kaihao Fan, Yingying Jin, Yaping Yang, Changlong Zheng, Yang Gao, Letong Yang, Xuesong Liu, Xiaodong Wu
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Abstract

Compared with V2O5/TiO2, vanadia catalysts supported on TiO2-ZSM-5 composite support possess excellent resistance to potassium poisoning in the selective catalytic reduction of NO by NH3 (NH3–SCR). Appropriate addition of ZSM-5 (10 wt %) enhances the low-temperature activity of NH3–SCR with more than 80% NOx conversion at 175–450 °C, as the combination of TiO2 and ZSM-5 is conducive to the formation of more low-valent (polymeric) VOx preferentially deposited on TiO2. Compared with V2O5/TiO2, the composite support catalysts effectively shield V2O5 as the main active species from K poisoning by preferential ion-exchange of K+ with Brønsted acid sites (Si–O(H)–Al) of ZSM-5. According to physicochemical characterizations, the mechanism of catalyst deactivation is mainly attributed to excessive aggregation of VOx to form inactive crystalline V2O5 in addition to KVO3. In situ diffuse reflectance infrared Fourier transform spectroscopy indicates that the presence of K leads to the formation of inactive bidentate nitrates instead of active bridged nitrates. A novel vanadium-based catalyst with high alkali poisoning resistance for ultralow temperature (<200 °C) denitration was developed.

Abstract Image

K中毒时TiO2-ZSM-5复合载体上VOx的演化及其对超低温NH3-SCR的影响
与V2O5/TiO2相比,TiO2- zsm -5复合载体负载的钒催化剂在NH3选择性催化还原NO (NH3 - scr)中具有优异的抗钾中毒性能。适当添加ZSM-5 (10 wt %)可提高NH3-SCR的低温活性,在175 ~ 450℃时NOx转化率超过80%,因为TiO2与ZSM-5的结合有利于形成更多的低价(聚合)VOx优先沉积在TiO2上。与V2O5/TiO2相比,复合载体催化剂通过K+与ZSM-5的Brønsted酸位(Si-O (H) -Al)的优先离子交换,有效地屏蔽了V2O5作为主要活性物质的K中毒。根据理化表征,催化剂失活的机理主要是由于VOx过度聚集,形成除KVO3外无活性的V2O5晶体。原位漫反射红外傅立叶变换光谱表明,K的存在导致非活性双齿硝酸盐的形成,而不是活性桥式硝酸盐。研制了一种新型钒基超低温(200℃)脱硝催化剂,具有较高的抗碱中毒性能。
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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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