{"title":"原位气体调节铂的电子结构，促进 Pt/Fe3O4 上的 NH3-SCO 反应","authors":"Bo Wu, Yijia Wu, Jinglei Li, Xinyu Zheng, Limin Hu, Baiqiang Zhang","doi":"10.1016/j.seppur.2024.130514","DOIUrl":null,"url":null,"abstract":"The selective catalytic oxidation of ammonia (NH<sub>3</sub>-SCO) over Pt-based catalysts is a promising method for reducing NH<sub>3</sub> into N<sub>2</sub> and H<sub>2</sub>O. Iron oxide, a typical and cheap redox carrier, can potentially affect the electronic or geometric structure of Pt sites. What’s more, the properties of Pt sites could be easily modulated through <em>in-situ</em> gas modulation. In this study, the Pt-supported Fe<sub>3</sub>O<sub>4</sub> catalyst (PtFe) was subjected to modulation by reaction gases (21 % O<sub>2</sub> or 0.4 % NH<sub>3</sub>) at varying temperatures (250 °C and 500 °C). Among all samples, the PtFe reduced at 250 °C (PtFe-N250) displayed the most favourable NH<sub>3</sub>-SCO performance, with 93.3 % NH<sub>3</sub> oxidation and 65 % N<sub>2</sub> selectivity achieved at 225 °C. The mechanism of the NH<sub>3</sub>-SCO over PtFe-N250 was investigated through a series of <em>ex-situ</em> characterizations and <em>in-situ</em> DRIFTS. The favourable NH<sub>3</sub> oxidation performance observed over PtFe-N250 below 250 °C could be attributed to the high concentration of Pt<sup>0</sup> species and high content of strong acid sites. The <em>in-situ</em> DRIFTS indicated that the NH<sub>3</sub>-SCO over PtFe-N250 followed the internal selective catalytic reduction (<em>i</em>-SCR). This study offered a novel strategy for enhancing the NH<sub>3</sub>-SCO performance of PtFe using <em>in-situ</em> gas-modulating approachs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"75 1","pages":""},"PeriodicalIF":8.1000,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In-situ gas-modulating electron structure of Pt to boost NH3-SCO reactions over Pt/Fe3O4\",\"authors\":\"Bo Wu, Yijia Wu, Jinglei Li, Xinyu Zheng, Limin Hu, Baiqiang Zhang\",\"doi\":\"10.1016/j.seppur.2024.130514\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The selective catalytic oxidation of ammonia (NH<sub>3</sub>-SCO) over Pt-based catalysts is a promising method for reducing NH<sub>3</sub> into N<sub>2</sub> and H<sub>2</sub>O. Iron oxide, a typical and cheap redox carrier, can potentially affect the electronic or geometric structure of Pt sites. What’s more, the properties of Pt sites could be easily modulated through <em>in-situ</em> gas modulation. In this study, the Pt-supported Fe<sub>3</sub>O<sub>4</sub> catalyst (PtFe) was subjected to modulation by reaction gases (21 % O<sub>2</sub> or 0.4 % NH<sub>3</sub>) at varying temperatures (250 °C and 500 °C). Among all samples, the PtFe reduced at 250 °C (PtFe-N250) displayed the most favourable NH<sub>3</sub>-SCO performance, with 93.3 % NH<sub>3</sub> oxidation and 65 % N<sub>2</sub> selectivity achieved at 225 °C. The mechanism of the NH<sub>3</sub>-SCO over PtFe-N250 was investigated through a series of <em>ex-situ</em> characterizations and <em>in-situ</em> DRIFTS. The favourable NH<sub>3</sub> oxidation performance observed over PtFe-N250 below 250 °C could be attributed to the high concentration of Pt<sup>0</sup> species and high content of strong acid sites. The <em>in-situ</em> DRIFTS indicated that the NH<sub>3</sub>-SCO over PtFe-N250 followed the internal selective catalytic reduction (<em>i</em>-SCR). This study offered a novel strategy for enhancing the NH<sub>3</sub>-SCO performance of PtFe using <em>in-situ</em> gas-modulating approachs.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"75 1\",\"pages\":\"\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-11-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.seppur.2024.130514\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.seppur.2024.130514","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
In-situ gas-modulating electron structure of Pt to boost NH3-SCO reactions over Pt/Fe3O4
The selective catalytic oxidation of ammonia (NH3-SCO) over Pt-based catalysts is a promising method for reducing NH3 into N2 and H2O. Iron oxide, a typical and cheap redox carrier, can potentially affect the electronic or geometric structure of Pt sites. What’s more, the properties of Pt sites could be easily modulated through in-situ gas modulation. In this study, the Pt-supported Fe3O4 catalyst (PtFe) was subjected to modulation by reaction gases (21 % O2 or 0.4 % NH3) at varying temperatures (250 °C and 500 °C). Among all samples, the PtFe reduced at 250 °C (PtFe-N250) displayed the most favourable NH3-SCO performance, with 93.3 % NH3 oxidation and 65 % N2 selectivity achieved at 225 °C. The mechanism of the NH3-SCO over PtFe-N250 was investigated through a series of ex-situ characterizations and in-situ DRIFTS. The favourable NH3 oxidation performance observed over PtFe-N250 below 250 °C could be attributed to the high concentration of Pt0 species and high content of strong acid sites. The in-situ DRIFTS indicated that the NH3-SCO over PtFe-N250 followed the internal selective catalytic reduction (i-SCR). This study offered a novel strategy for enhancing the NH3-SCO performance of PtFe using in-situ gas-modulating approachs.
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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