{"title":"用柠檬酸辅助沉淀法制备具有宽温度窗口的 CeO2-CePO4 脱硝催化剂","authors":"Xiaoyu Liu, Xiao Liu, Chang Yang, Kangkang Wang, Hu Liu, Huidong Xie","doi":"10.1007/s10562-025-05017-5","DOIUrl":null,"url":null,"abstract":"<div><p>The catalytic activity window of conventional commercial V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> is too narrow, which is a main problem for selective catalytic reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub> (NH<sub>3</sub>-SCR) catalysts. Herein, a series of CeO<sub>2</sub>-CePO<sub>4</sub>-CA-<i>x</i> (<i>x</i> = 1–6) catalysts with wide temperature windows were prepared by a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7<sup>o</sup>C in which the NO conversion can exceed 80% when <i>x</i> is 4. Compared with the CeO<sub>2</sub>-CePO<sub>4</sub> catalyst prepared without adding citric acid, CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency. The prepared catalysts were characterized by N<sub>2</sub> adsorption-desorption, transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS), temperature-programmed reduction of H<sub>2</sub> (H<sub>2</sub>-TPR), and temperature-programmed desorption of NH<sub>3</sub> (NH<sub>3</sub>-TPD). Results showed that the CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 composites had more uniform mesoporous pore size and higher Ce<sup>3+</sup> and surface adsorbed oxygen content, higher H<sub>2</sub> consumption, and greater number of acidic sites than CeO<sub>2</sub>-CePO<sub>4</sub>. All of those are conducive to redox performance enhancement, thus improving the NH<sub>3</sub>-SCR reactivity and water and sulfur resistance of the catalyst. CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 with a wide temperature window as well as good SO<sub>2</sub> resistance shows good prospects in industrial applications.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div><div><p>Comparison of the NO conversions of the catalysts. We prepared a series of CeO<sub>2</sub>-CePO<sub>4</sub>-CA-<i>x</i> (<i>x</i> = 1–6) catalysts with wide temperature windows using a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7<sup>o</sup>C in which the NO conversion can exceed 80% when <i>x</i> is 4. Compared with the CeO<sub>2</sub>-CePO<sub>4</sub> catalyst prepared without adding citric acid, CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency</p></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 5","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Preparation of CeO2-CePO4 Denitration Catalyst with Wide Temperature Window by a Citric Acid-Assisted Precipitation Method\",\"authors\":\"Xiaoyu Liu, Xiao Liu, Chang Yang, Kangkang Wang, Hu Liu, Huidong Xie\",\"doi\":\"10.1007/s10562-025-05017-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The catalytic activity window of conventional commercial V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> is too narrow, which is a main problem for selective catalytic reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub> (NH<sub>3</sub>-SCR) catalysts. Herein, a series of CeO<sub>2</sub>-CePO<sub>4</sub>-CA-<i>x</i> (<i>x</i> = 1–6) catalysts with wide temperature windows were prepared by a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7<sup>o</sup>C in which the NO conversion can exceed 80% when <i>x</i> is 4. Compared with the CeO<sub>2</sub>-CePO<sub>4</sub> catalyst prepared without adding citric acid, CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency. The prepared catalysts were characterized by N<sub>2</sub> adsorption-desorption, transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS), temperature-programmed reduction of H<sub>2</sub> (H<sub>2</sub>-TPR), and temperature-programmed desorption of NH<sub>3</sub> (NH<sub>3</sub>-TPD). Results showed that the CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 composites had more uniform mesoporous pore size and higher Ce<sup>3+</sup> and surface adsorbed oxygen content, higher H<sub>2</sub> consumption, and greater number of acidic sites than CeO<sub>2</sub>-CePO<sub>4</sub>. All of those are conducive to redox performance enhancement, thus improving the NH<sub>3</sub>-SCR reactivity and water and sulfur resistance of the catalyst. CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 with a wide temperature window as well as good SO<sub>2</sub> resistance shows good prospects in industrial applications.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div><div><p>Comparison of the NO conversions of the catalysts. We prepared a series of CeO<sub>2</sub>-CePO<sub>4</sub>-CA-<i>x</i> (<i>x</i> = 1–6) catalysts with wide temperature windows using a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7<sup>o</sup>C in which the NO conversion can exceed 80% when <i>x</i> is 4. Compared with the CeO<sub>2</sub>-CePO<sub>4</sub> catalyst prepared without adding citric acid, CeO<sub>2</sub>-CePO<sub>4</sub>-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency</p></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 5\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-04-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-025-05017-5\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-025-05017-5","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
传统的商用V2O5-WO3/TiO2催化活性窗口过窄,是NH3 (NH3- scr)催化剂选择性催化还原NOx的主要问题。本文采用柠檬酸辅助沉淀法制备了一系列具有宽温度窗的CeO2-CePO4-CA-x (x = 1-6)催化剂。该系列具有212.9-579.7oC的最宽温度窗,当x = 4时,NO转化率可超过80%。与未添加柠檬酸制备的CeO2-CePO4催化剂相比,CeO2-CePO4- ca -4具有更好的耐水和耐硫性能,更低的SCR活化能和更高的周转频率。通过N2吸附-解吸、透射电镜(TEM)、x射线光电子能谱(XPS)、程序升温还原H2 (H2- tpr)和程序升温解吸NH3 (NH3- tpd)对催化剂进行了表征。结果表明,与CeO2-CePO4相比,CeO2-CePO4- ca -4复合材料具有更均匀的介孔孔径、更高的Ce3+和表面吸附氧含量、更高的H2消耗和更多的酸性位点。这些都有利于提高催化剂的氧化还原性能,从而提高催化剂的NH3-SCR反应活性和耐水、耐硫性能。CeO2-CePO4-CA-4具有较宽的温度窗和良好的抗SO2性能,具有良好的工业应用前景。图表摘要催化剂NO转化率的比较。采用柠檬酸辅助沉淀法制备了一系列具有宽温度窗的CeO2-CePO4-CA-x (x = 1-6)催化剂。该系列具有212.9-579.7oC的最宽温度窗,当x = 4时,NO转化率可超过80%。与未添加柠檬酸制备的CeO2-CePO4催化剂相比,CeO2-CePO4- ca -4具有更好的耐水和耐硫性能,更低的SCR活化能和更高的周转频率
Preparation of CeO2-CePO4 Denitration Catalyst with Wide Temperature Window by a Citric Acid-Assisted Precipitation Method
The catalytic activity window of conventional commercial V2O5-WO3/TiO2 is too narrow, which is a main problem for selective catalytic reduction of NOx by NH3 (NH3-SCR) catalysts. Herein, a series of CeO2-CePO4-CA-x (x = 1–6) catalysts with wide temperature windows were prepared by a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7oC in which the NO conversion can exceed 80% when x is 4. Compared with the CeO2-CePO4 catalyst prepared without adding citric acid, CeO2-CePO4-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency. The prepared catalysts were characterized by N2 adsorption-desorption, transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS), temperature-programmed reduction of H2 (H2-TPR), and temperature-programmed desorption of NH3 (NH3-TPD). Results showed that the CeO2-CePO4-CA-4 composites had more uniform mesoporous pore size and higher Ce3+ and surface adsorbed oxygen content, higher H2 consumption, and greater number of acidic sites than CeO2-CePO4. All of those are conducive to redox performance enhancement, thus improving the NH3-SCR reactivity and water and sulfur resistance of the catalyst. CeO2-CePO4-CA-4 with a wide temperature window as well as good SO2 resistance shows good prospects in industrial applications.
Graphical Abstract
Comparison of the NO conversions of the catalysts. We prepared a series of CeO2-CePO4-CA-x (x = 1–6) catalysts with wide temperature windows using a citric acid-assisted precipitation method. The series has the widest temperature window of 212.9-579.7oC in which the NO conversion can exceed 80% when x is 4. Compared with the CeO2-CePO4 catalyst prepared without adding citric acid, CeO2-CePO4-CA-4 exhibits better water and sulfur resistance, lower SCR activation energy, and greater turnover frequency
期刊介绍:
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.