Unraveling the contribution of acidic metal oxides modulating the CeO2/TiO2 catalyst acid sites for NH3-SCR activity and SO2 tolerance

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-07-30 Epub Date: 2025-01-27 DOI:10.1016/j.seppur.2025.131747
Zhian Gong , Jun Cao , Yingkang Hu , Yadi Yang , Jinhua Ye , Xiaojiang Yao
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Abstract

As a potential substitute for V2O5-WO3/TiO2 (V-W/Ti) catalyst, CeO2/TiO2 (Ce/Ti) catalyst still faces severe challenges regarding low-temperature denitrification performance and SO2 tolerance. To this end, we report an effective strategy to modulate Ce/Ti catalyst acid sites by different acidic metal oxides. The modification of Nb, Mo and W species can well weaken the L-acid sites and enhance the B-acid sites of Ce/Ti catalyst, which helps more NH3 adsorb to form the ionic NH4+ for activation at low temperatures. Moreover, the improvement of redox performance well weakens the adsorption of low reactive nitrates and facilitates the NO oxidation of NO2. The optimum sample (Ce-Nb/Ti) achieved 95 % NOx conversion within the active temperature window (225 − 425 °C) and admirable SO2-tolerant performance at 300 °C. The abundant surface acidity and strong interactions between metal ions not only suppress the adsorption of SO2 on the Ce-Nb/Ti but also decrease the thermal stability of ammonia bisulfate and alleviate sulfate deposition. Moreover, the in situ DRIFTS experiments demonstrated that introducing these acidic metal oxides on Ce/Ti catalyst did not change the reaction pathway, following the Langmuir-Hinshelwood and Eley-Rideal mechanisms.

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揭示酸性金属氧化物调节 CeO2/TiO2 催化剂酸性位点对 NH3-SCR 活性和二氧化硫耐受性的贡献
作为V2O5-WO3/TiO2 (V-W/Ti)催化剂的潜在替代品,CeO2/TiO2 (Ce/Ti)催化剂在低温脱硝性能和SO2耐受性方面仍面临严峻挑战。为此,我们报道了一种通过不同的酸性金属氧化物来调节Ce/Ti催化剂酸位的有效策略。Nb、Mo和W的改性能很好地削弱Ce/Ti催化剂的l酸位点,增强其b酸位点,有利于更多的NH3吸附形成离子NH4+进行低温活化。此外,氧化还原性能的提高很好地削弱了低活性硝酸盐的吸附,促进了NO对NO2的氧化。最佳样品(Ce-Nb/Ti)在有效温度窗口(225 − 425 °C)内实现了95% %的NOx转化率,并且在300 °C时具有令人满意的耐二氧化硫性能。丰富的表面酸度和金属离子之间的强相互作用不仅抑制了SO2在Ce-Nb/Ti上的吸附,而且降低了硫酸氢氨的热稳定性,减轻了硫酸盐沉积。此外,原位DRIFTS实验表明,在Ce/Ti催化剂上引入这些酸性金属氧化物不会改变反应途径,遵循Langmuir-Hinshelwood和ely - rideal机制。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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