Qiuming Zhou , Shuaishuai Lyu , Hongwei Li , Congcong Niu , Rongjun Zhang , Chaopeng Hou , Binhang Yan , Sen Wang , Bo Peng , Run Xu , Mingfeng Li
{"title":"一种用于RWGS反应的高效Pt/TiO2-NaY-x催化剂:吸附剂NaY-x对CO2加氢转化的增强作用","authors":"Qiuming Zhou , Shuaishuai Lyu , Hongwei Li , Congcong Niu , Rongjun Zhang , Chaopeng Hou , Binhang Yan , Sen Wang , Bo Peng , Run Xu , Mingfeng Li","doi":"10.1016/j.ccst.2025.100452","DOIUrl":null,"url":null,"abstract":"<div><div>Selective removal of H<sub>2</sub>O <em>in-situ</em> from the reverse water gas shift (RWGS) reaction system is an effective approach to intensify the CO<sub>2</sub> conversion dictated by thermodynamics. Here, a composite material is prepared by combining a water adsorbent zeolite NaY-2 which modified by hydrothermal treatment at 500°C with Pt/TiO<sub>2</sub> catalyst. The synthesized Pt/TiO<sub>2</sub>-NaY-2 exhibits much higher activity and CO selectivity than conventional Pt/TiO<sub>2</sub>. It shows the highest CO<sub>2</sub> conversion of 42.3% and consistently exceeds the corresponding thermodynamic equilibrium conversion (28.6%) over 120 h on stream with 100% CO selectivity at 340°C. The persistent catalytic enhancement is mainly attributed to the well aligning between the desorption temperature of H<sub>2</sub>O on NaY-2 (270°C, 330°C) and the reaction temperature. The introduced NaY-2 demonstrates an electronic effect on Pt/TiO<sub>2</sub> during the reduction process and generates an electron-rich Pt species. The created Pt<sup>δ−</sup> sites on Pt/TiO<sub>2</sub>-NaY-2 possess higher intrinsic catalytic activity than Pt<sup>0</sup> sites on Pt/TiO<sub>2</sub>. The interaction also reduces Pt average particle size and thus weakens the adsorption of CO on Pt, which inhibits the methanation side reaction then improves the CO selectivity on Pt/TiO<sub>2</sub>-NaY-2. The RWGS reactions on the synthesized Pt-based catalysts proceed through intermediate decomposition mechanism exposed by <em>in-situ</em> IR spectroscopy. The findings of this work provide information of high interest to guide future research on RWGS reaction intensified process via <em>in-situ</em> removal of H<sub>2</sub>O.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100452"},"PeriodicalIF":0.0000,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A Highly Efficient Pt/TiO2-NaY-x Catalyst for RWGS reaction: Enhancement Effect of Adsorbent NaY-x on CO2 Hydrogenation Conversion\",\"authors\":\"Qiuming Zhou , Shuaishuai Lyu , Hongwei Li , Congcong Niu , Rongjun Zhang , Chaopeng Hou , Binhang Yan , Sen Wang , Bo Peng , Run Xu , Mingfeng Li\",\"doi\":\"10.1016/j.ccst.2025.100452\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Selective removal of H<sub>2</sub>O <em>in-situ</em> from the reverse water gas shift (RWGS) reaction system is an effective approach to intensify the CO<sub>2</sub> conversion dictated by thermodynamics. Here, a composite material is prepared by combining a water adsorbent zeolite NaY-2 which modified by hydrothermal treatment at 500°C with Pt/TiO<sub>2</sub> catalyst. The synthesized Pt/TiO<sub>2</sub>-NaY-2 exhibits much higher activity and CO selectivity than conventional Pt/TiO<sub>2</sub>. It shows the highest CO<sub>2</sub> conversion of 42.3% and consistently exceeds the corresponding thermodynamic equilibrium conversion (28.6%) over 120 h on stream with 100% CO selectivity at 340°C. The persistent catalytic enhancement is mainly attributed to the well aligning between the desorption temperature of H<sub>2</sub>O on NaY-2 (270°C, 330°C) and the reaction temperature. The introduced NaY-2 demonstrates an electronic effect on Pt/TiO<sub>2</sub> during the reduction process and generates an electron-rich Pt species. The created Pt<sup>δ−</sup> sites on Pt/TiO<sub>2</sub>-NaY-2 possess higher intrinsic catalytic activity than Pt<sup>0</sup> sites on Pt/TiO<sub>2</sub>. The interaction also reduces Pt average particle size and thus weakens the adsorption of CO on Pt, which inhibits the methanation side reaction then improves the CO selectivity on Pt/TiO<sub>2</sub>-NaY-2. The RWGS reactions on the synthesized Pt-based catalysts proceed through intermediate decomposition mechanism exposed by <em>in-situ</em> IR spectroscopy. The findings of this work provide information of high interest to guide future research on RWGS reaction intensified process via <em>in-situ</em> removal of H<sub>2</sub>O.</div></div>\",\"PeriodicalId\":9387,\"journal\":{\"name\":\"Carbon Capture Science & Technology\",\"volume\":\"16 \",\"pages\":\"Article 100452\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-06-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon Capture Science & Technology\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2772656825000910\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Capture Science & Technology","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772656825000910","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
A Highly Efficient Pt/TiO2-NaY-x Catalyst for RWGS reaction: Enhancement Effect of Adsorbent NaY-x on CO2 Hydrogenation Conversion
Selective removal of H2O in-situ from the reverse water gas shift (RWGS) reaction system is an effective approach to intensify the CO2 conversion dictated by thermodynamics. Here, a composite material is prepared by combining a water adsorbent zeolite NaY-2 which modified by hydrothermal treatment at 500°C with Pt/TiO2 catalyst. The synthesized Pt/TiO2-NaY-2 exhibits much higher activity and CO selectivity than conventional Pt/TiO2. It shows the highest CO2 conversion of 42.3% and consistently exceeds the corresponding thermodynamic equilibrium conversion (28.6%) over 120 h on stream with 100% CO selectivity at 340°C. The persistent catalytic enhancement is mainly attributed to the well aligning between the desorption temperature of H2O on NaY-2 (270°C, 330°C) and the reaction temperature. The introduced NaY-2 demonstrates an electronic effect on Pt/TiO2 during the reduction process and generates an electron-rich Pt species. The created Ptδ− sites on Pt/TiO2-NaY-2 possess higher intrinsic catalytic activity than Pt0 sites on Pt/TiO2. The interaction also reduces Pt average particle size and thus weakens the adsorption of CO on Pt, which inhibits the methanation side reaction then improves the CO selectivity on Pt/TiO2-NaY-2. The RWGS reactions on the synthesized Pt-based catalysts proceed through intermediate decomposition mechanism exposed by in-situ IR spectroscopy. The findings of this work provide information of high interest to guide future research on RWGS reaction intensified process via in-situ removal of H2O.