{"title":"添加剂改性对 Fe/g-C3N4 催化 CO 加氢反应产物分布的影响","authors":"Bing Li, Xinhua Gao, Kangzhou Wang, Yaqin Xing, Caihu Li, Qingxiang Ma, Tian-sheng Zhao, Jianli Zhang","doi":"10.1007/s11144-024-02676-0","DOIUrl":null,"url":null,"abstract":"<p>The melamine thermal shrinkage method was used to prepare carbon nitride (g-C<sub>3</sub>N<sub>4</sub>). Fe/g-C<sub>3</sub>N<sub>4</sub> was obtained by impregnation, and Na, K, and Zn additives were added as modifiers. The CO hydrogenation performances of the catalysts were studied before and after modification. The effect of additive modification on the textural properties of the Fe/g-C<sub>3</sub>N<sub>4</sub> catalyst and product distribution of CO hydrogenation was investigated by combining several characterization techniques such as N<sub>2</sub> physical adsorption and desorption, XRD, SEM, TEM, FT-IR, TG, CO<sub>2</sub>-TPD, Raman, XPS, and contact angle (CA) experiments. The textural characteristics and performance of the catalyst were markedly affected by the additive modifications. Na and K modifications weakened the strong interactions between Fe and g-C<sub>3</sub>N<sub>4</sub> and improved the activity of the catalyst; additionally, hydrophilicity was enhanced. The Zn modified catalyst Fe/g-C<sub>3</sub>N<sub>4</sub>-Zn exhibited a weaker water gas shift reaction activity, and a lower CO<sub>2</sub> selectivity was obtained for CO hydrogenation. In the CO hydrogenation reaction, the Na-modified and K-modified catalysts, which exhibit enhanced surface alkalinity, inhibited secondary olefin hydrogenation and displayed high olefin selectivity and lower CH<sub>4</sub> selectivity. Fe/g-C<sub>3</sub>N<sub>4</sub>-Na exhibited the highest olefin selectivity, with C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup> up to 47.5%, and an O/P value of 5.1.</p><h3 data-test=\"abstract-sub-heading\">Graphical abstract</h3>\n","PeriodicalId":750,"journal":{"name":"Reaction Kinetics, Mechanisms and Catalysis","volume":null,"pages":null},"PeriodicalIF":1.7000,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of additive modification on the product distribution in CO hydrogenation catalyzed by Fe/g-C3N4\",\"authors\":\"Bing Li, Xinhua Gao, Kangzhou Wang, Yaqin Xing, Caihu Li, Qingxiang Ma, Tian-sheng Zhao, Jianli Zhang\",\"doi\":\"10.1007/s11144-024-02676-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The melamine thermal shrinkage method was used to prepare carbon nitride (g-C<sub>3</sub>N<sub>4</sub>). Fe/g-C<sub>3</sub>N<sub>4</sub> was obtained by impregnation, and Na, K, and Zn additives were added as modifiers. The CO hydrogenation performances of the catalysts were studied before and after modification. The effect of additive modification on the textural properties of the Fe/g-C<sub>3</sub>N<sub>4</sub> catalyst and product distribution of CO hydrogenation was investigated by combining several characterization techniques such as N<sub>2</sub> physical adsorption and desorption, XRD, SEM, TEM, FT-IR, TG, CO<sub>2</sub>-TPD, Raman, XPS, and contact angle (CA) experiments. The textural characteristics and performance of the catalyst were markedly affected by the additive modifications. Na and K modifications weakened the strong interactions between Fe and g-C<sub>3</sub>N<sub>4</sub> and improved the activity of the catalyst; additionally, hydrophilicity was enhanced. The Zn modified catalyst Fe/g-C<sub>3</sub>N<sub>4</sub>-Zn exhibited a weaker water gas shift reaction activity, and a lower CO<sub>2</sub> selectivity was obtained for CO hydrogenation. In the CO hydrogenation reaction, the Na-modified and K-modified catalysts, which exhibit enhanced surface alkalinity, inhibited secondary olefin hydrogenation and displayed high olefin selectivity and lower CH<sub>4</sub> selectivity. Fe/g-C<sub>3</sub>N<sub>4</sub>-Na exhibited the highest olefin selectivity, with C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup> up to 47.5%, and an O/P value of 5.1.</p><h3 data-test=\\\"abstract-sub-heading\\\">Graphical abstract</h3>\\n\",\"PeriodicalId\":750,\"journal\":{\"name\":\"Reaction Kinetics, Mechanisms and Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":1.7000,\"publicationDate\":\"2024-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Reaction Kinetics, Mechanisms and Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1007/s11144-024-02676-0\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Reaction Kinetics, Mechanisms and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1007/s11144-024-02676-0","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
采用三聚氰胺热收缩法制备氮化碳（g-C3N4）。通过浸渍法获得 Fe/g-C3N4，并加入 Na、K 和 Zn 添加剂作为改性剂。研究了改性前后催化剂的 CO 加氢性能。结合 N2 物理吸附和解吸、XRD、SEM、TEM、FT-IR、TG、CO2-TPD、拉曼、XPS 和接触角（CA）实验等多种表征技术，研究了添加剂改性对 Fe/g-C3N4 催化剂质构特性和 CO 加氢产物分布的影响。添加剂改性对催化剂的质构特征和性能有明显影响。Na 和 K 改性削弱了铁和 g-C3N4 之间的强相互作用，提高了催化剂的活性；此外，亲水性也得到了增强。Zn 改性催化剂 Fe/g-C3N4-Zn 的水气变换反应活性较弱，在 CO 加氢反应中获得的 CO2 选择性较低。在 CO 加氢反应中，表面碱性增强的 Na 改性和 K 改性催化剂抑制了仲烯烃的加氢反应，并显示出较高的烯烃选择性和较低的 CH4 选择性。Fe/g-C3N4-Na 的烯烃选择性最高，C2=-C4=高达 47.5%，O/P 值为 5.1。
Effect of additive modification on the product distribution in CO hydrogenation catalyzed by Fe/g-C3N4
The melamine thermal shrinkage method was used to prepare carbon nitride (g-C3N4). Fe/g-C3N4 was obtained by impregnation, and Na, K, and Zn additives were added as modifiers. The CO hydrogenation performances of the catalysts were studied before and after modification. The effect of additive modification on the textural properties of the Fe/g-C3N4 catalyst and product distribution of CO hydrogenation was investigated by combining several characterization techniques such as N2 physical adsorption and desorption, XRD, SEM, TEM, FT-IR, TG, CO2-TPD, Raman, XPS, and contact angle (CA) experiments. The textural characteristics and performance of the catalyst were markedly affected by the additive modifications. Na and K modifications weakened the strong interactions between Fe and g-C3N4 and improved the activity of the catalyst; additionally, hydrophilicity was enhanced. The Zn modified catalyst Fe/g-C3N4-Zn exhibited a weaker water gas shift reaction activity, and a lower CO2 selectivity was obtained for CO hydrogenation. In the CO hydrogenation reaction, the Na-modified and K-modified catalysts, which exhibit enhanced surface alkalinity, inhibited secondary olefin hydrogenation and displayed high olefin selectivity and lower CH4 selectivity. Fe/g-C3N4-Na exhibited the highest olefin selectivity, with C2=–C4= up to 47.5%, and an O/P value of 5.1.
期刊介绍：
Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields:
-kinetics of homogeneous reactions in gas, liquid and solid phase;
-Homogeneous catalysis;
-Heterogeneous catalysis;
-Adsorption in heterogeneous catalysis;
-Transport processes related to reaction kinetics and catalysis;
-Preparation and study of catalysts;
-Reactors and apparatus.
Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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