Effect of Pr/Zr atomic ratio on the activity of catalytic oxidation denitration of PrxZr1−xO2−δ

Q3 Energy 燃料化学学报 Pub Date : 2023-07-01 DOI:10.1016/S1872-5813(23)60341-X
GONG You-jing, HE Ren-guang, ZHAO Guang-lei, JIA Li-juan, GAO Ji-yun, WANG Fang, DUAN Kai-jiao, LIU Tian-cheng
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Abstract

The PrxZr1–xO2–δ catalyst with different atom ratio of Pr/Zr was prepared by the sol-gel to catalytic oxidation denitration. Results showed that the efficiency of catalytic oxidation denitration increased initially and decreased afterward with the ratio of Pr atom increased. And the optimum denitration activity could achieve 94.62% at 250 °C when the atom ratio of Pr/Zr was 5:5. The catalysts were characterized by SEM, N2 adsorption-desorption, XRD, XPS, H2-TPR, and FT-IR. The results illustrated that the catalyst (Pr0.5Zr0.5O2–δ) with the best activity has a “layered” morphology, many pores on the surface, and it has a large specific surface area and pore volume of 77.74 m2/g and 0.66 cm3/g, respectively. Furthermore, the crystalline phase transforms from c-ZrO2 to Pr2Zr2O7 with the increasing of Pr atom. XPS and H2-TPR results showed that the surface chemosorption oxygen and surface Pr4+ oxides increased, and the rising of Pr atom ratio was beneficial to produce oxygen vacancy (Vӧ) site which advantageous to improve the efficiency of catalytic oxidation denitration. FT-IR characterization results indicated that Pr0.5Zr0.5O2–δ solid solution had better NO selectivity, which was conducive to the catalytic oxidation of NO. The anti-SO2 and H2O toxicity experiments showed that Pr/Zr atomic ratio at 5:5 had better anti-toxicity than other ratios. In addition, using IC to analysis absorption products, the result showed that NO2 and NO3 were the main products in the absorption solution.

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Pr/Zr原子比对PrxZr1−xO2−δ催化氧化脱硝活性的影响
摘要采用溶胶-凝胶法制备了不同Pr/Zr原子比的PrxZr1-xO2 -δ催化剂,用于催化氧化脱硝。结果表明,随着Pr原子比的增大,催化氧化脱硝效率先升高后降低。在250℃条件下,Pr/Zr原子比为5:5时,脱硝活性达到94.62%。采用SEM、N2吸附-脱附、XRD、XPS、H2-TPR和FT-IR对催化剂进行了表征。结果表明,活性最好的催化剂(Pr0.5Zr0.5O2 -δ)具有“层状”形态,表面气孔较多,比表面积大,孔体积分别为77.74 m2/g和0.66 cm3/g。随着Pr原子数的增加,晶相由c-ZrO2转变为Pr2Zr2O7。XPS和H2-TPR结果表明,表面化学吸附氧和表面Pr4+氧化物增加,Pr原子比的升高有利于氧空位(vz)的产生,有利于提高催化氧化脱硝效率。FT-IR表征结果表明,Pr0.5Zr0.5O2 -δ固溶体对NO有较好的选择性,有利于NO的催化氧化。抗so2和H2O毒性实验表明,Pr/Zr原子比为5:5时的抗毒性较好。此外,利用集成电路对吸收产物进行了分析,结果表明,吸收溶液中的主要产物为no2 -和no3 -。
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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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