GONG You-jing, HE Ren-guang, ZHAO Guang-lei, JIA Li-juan, GAO Ji-yun, WANG Fang, DUAN Kai-jiao, LIU Tian-cheng
{"title":"Pr/Zr原子比对PrxZr1−xO2−δ催化氧化脱硝活性的影响","authors":"GONG You-jing, HE Ren-guang, ZHAO Guang-lei, JIA Li-juan, GAO Ji-yun, WANG Fang, DUAN Kai-jiao, LIU Tian-cheng","doi":"10.1016/S1872-5813(23)60341-X","DOIUrl":null,"url":null,"abstract":"<div><h3>Abstract</h3><p>The Pr<sub><em>x</em></sub>Zr<sub>1–<em>x</em></sub>O<sub>2–<em>δ</em></sub> 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, N<sub>2</sub> adsorption-desorption, XRD, XPS, H<sub>2</sub>-TPR, and FT-IR. The results illustrated that the catalyst (Pr<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2–<em>δ</em></sub>) 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 m<sup>2</sup>/g and 0.66 cm<sup>3</sup>/g, respectively. Furthermore, the crystalline phase transforms from <em>c</em>-ZrO<sub>2</sub> to Pr<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> with the increasing of Pr atom. XPS and H<sub>2</sub>-TPR results showed that the surface chemosorption oxygen and surface Pr<sup>4+</sup> 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 Pr<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2–<em>δ</em></sub> solid solution had better NO selectivity, which was conducive to the catalytic oxidation of NO. The anti-SO<sub>2</sub> and H<sub>2</sub>O 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\n<span><math><msubsup><mrow><mtext>NO</mtext></mrow><mrow><mtext>2</mtext></mrow><mrow><mo>–</mo></mrow></msubsup></math></span> and\n<span><math><msubsup><mrow><mtext>NO</mtext></mrow><mrow><mtext>3</mtext></mrow><mrow><mo>–</mo></mrow></msubsup></math></span> were the main products in the absorption solution.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2023-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of Pr/Zr atomic ratio on the activity of catalytic oxidation denitration of PrxZr1−xO2−δ\",\"authors\":\"GONG You-jing, HE Ren-guang, ZHAO Guang-lei, JIA Li-juan, GAO Ji-yun, WANG Fang, DUAN Kai-jiao, LIU Tian-cheng\",\"doi\":\"10.1016/S1872-5813(23)60341-X\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><h3>Abstract</h3><p>The Pr<sub><em>x</em></sub>Zr<sub>1–<em>x</em></sub>O<sub>2–<em>δ</em></sub> 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, N<sub>2</sub> adsorption-desorption, XRD, XPS, H<sub>2</sub>-TPR, and FT-IR. The results illustrated that the catalyst (Pr<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2–<em>δ</em></sub>) 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 m<sup>2</sup>/g and 0.66 cm<sup>3</sup>/g, respectively. Furthermore, the crystalline phase transforms from <em>c</em>-ZrO<sub>2</sub> to Pr<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> with the increasing of Pr atom. XPS and H<sub>2</sub>-TPR results showed that the surface chemosorption oxygen and surface Pr<sup>4+</sup> 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 Pr<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2–<em>δ</em></sub> solid solution had better NO selectivity, which was conducive to the catalytic oxidation of NO. The anti-SO<sub>2</sub> and H<sub>2</sub>O 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\\n<span><math><msubsup><mrow><mtext>NO</mtext></mrow><mrow><mtext>2</mtext></mrow><mrow><mo>–</mo></mrow></msubsup></math></span> and\\n<span><math><msubsup><mrow><mtext>NO</mtext></mrow><mrow><mtext>3</mtext></mrow><mrow><mo>–</mo></mrow></msubsup></math></span> were the main products in the absorption solution.</p></div>\",\"PeriodicalId\":15956,\"journal\":{\"name\":\"燃料化学学报\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"燃料化学学报\",\"FirstCategoryId\":\"1087\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S187258132360341X\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"燃料化学学报","FirstCategoryId":"1087","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S187258132360341X","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
Effect of Pr/Zr atomic ratio on the activity of catalytic oxidation denitration of PrxZr1−xO2−δ
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
and
were the main products in the absorption solution.
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.