Xiaoman Li , Chengyue Lai , Yaping Zhang , Sheng Wang , Shipeng Ding
{"title":"用于富氧条件下氮氧化物选择性催化还原和一氧化碳氧化的 V-Cu/TiO2 双功能催化剂","authors":"Xiaoman Li , Chengyue Lai , Yaping Zhang , Sheng Wang , Shipeng Ding","doi":"10.1016/j.mcat.2024.114574","DOIUrl":null,"url":null,"abstract":"<div><div>The simultaneous removal of CO and NO<sub>x</sub> in the sintering flue gas over a single catalyst is desirable but challenging. Herein, 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub> bifunctional catalysts that efficiently catalyzed CO and NO<sub>x</sub> at low temperatures were reported, with CO and NO<sub>x</sub> conversions of 100 % at 200–300 °C. The synergistic effect between copper and vanadium oxides enhanced the redox and CO adsorption capacities of 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub>, rendering it abundant acid sites and surface chemisorbed oxygen. The in situ DRIFTS experiments demonstrated that CO oxidation over the dual-active-sites 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub> catalyst follows the Mars-van Krevelen mechanism, while the E-R mechanism was the primary NH<sub>3</sub>-SCR pathway. Due to the presence of dual-active-sites (i.e., separated of the V active sites for the NH<sub>3</sub>-SCR reaction and the Cu active sites for CO oxidation), the competition adsorption of CO and NH<sub>3</sub> on the Cu sites was weakened, resulting in higher CO oxidation performance than the single-active-site catalysts. This work provided insights into the control of flue gas containing CO and NO<sub>x</sub> over a single catalyst.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114574"},"PeriodicalIF":3.9000,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Bifunctional catalysts V-Cu/TiO2 for selective catalytic reduction of NOx and CO oxidation under oxygen-rich conditions\",\"authors\":\"Xiaoman Li , Chengyue Lai , Yaping Zhang , Sheng Wang , Shipeng Ding\",\"doi\":\"10.1016/j.mcat.2024.114574\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The simultaneous removal of CO and NO<sub>x</sub> in the sintering flue gas over a single catalyst is desirable but challenging. Herein, 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub> bifunctional catalysts that efficiently catalyzed CO and NO<sub>x</sub> at low temperatures were reported, with CO and NO<sub>x</sub> conversions of 100 % at 200–300 °C. The synergistic effect between copper and vanadium oxides enhanced the redox and CO adsorption capacities of 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub>, rendering it abundant acid sites and surface chemisorbed oxygen. The in situ DRIFTS experiments demonstrated that CO oxidation over the dual-active-sites 2 %V<sub>2</sub>O<sub>5</sub>–5 %CuO/TiO<sub>2</sub> catalyst follows the Mars-van Krevelen mechanism, while the E-R mechanism was the primary NH<sub>3</sub>-SCR pathway. Due to the presence of dual-active-sites (i.e., separated of the V active sites for the NH<sub>3</sub>-SCR reaction and the Cu active sites for CO oxidation), the competition adsorption of CO and NH<sub>3</sub> on the Cu sites was weakened, resulting in higher CO oxidation performance than the single-active-site catalysts. This work provided insights into the control of flue gas containing CO and NO<sub>x</sub> over a single catalyst.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"569 \",\"pages\":\"Article 114574\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-09-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823124007569\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823124007569","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
在单一催化剂上同时去除烧结烟气中的一氧化碳和氮氧化物是一种理想但具有挑战性的方法。本文报告了 2 %V2O5-5 %CuO/TiO2 双功能催化剂,该催化剂可在低温下高效催化一氧化碳和氮氧化物,在 200-300 °C 温度下,一氧化碳和氮氧化物的转化率达到 100%。铜和钒氧化物之间的协同效应增强了 2 %V2O5-5 %CuO/TiO2 的氧化还原能力和 CO 吸附能力,使其具有丰富的酸性位点和表面化学吸附氧。原位 DRIFTS 实验表明,双活性位点 2 %V2O5-5 %CuO/TiO2 催化剂上的 CO 氧化遵循 Mars-van Krevelen 机制,而 E-R 机制则是主要的 NH3-SCR 途径。由于存在双活性位点(即用于 NH3-SCR 反应的 V 活性位点和用于 CO 氧化的 Cu 活性位点分离),CO 和 NH3 在 Cu 位点上的竞争吸附作用减弱,因此 CO 氧化性能高于单活性位点催化剂。这项工作为在单一催化剂上控制含有 CO 和 NOx 的烟气提供了启示。
Bifunctional catalysts V-Cu/TiO2 for selective catalytic reduction of NOx and CO oxidation under oxygen-rich conditions
The simultaneous removal of CO and NOx in the sintering flue gas over a single catalyst is desirable but challenging. Herein, 2 %V2O5–5 %CuO/TiO2 bifunctional catalysts that efficiently catalyzed CO and NOx at low temperatures were reported, with CO and NOx conversions of 100 % at 200–300 °C. The synergistic effect between copper and vanadium oxides enhanced the redox and CO adsorption capacities of 2 %V2O5–5 %CuO/TiO2, rendering it abundant acid sites and surface chemisorbed oxygen. The in situ DRIFTS experiments demonstrated that CO oxidation over the dual-active-sites 2 %V2O5–5 %CuO/TiO2 catalyst follows the Mars-van Krevelen mechanism, while the E-R mechanism was the primary NH3-SCR pathway. Due to the presence of dual-active-sites (i.e., separated of the V active sites for the NH3-SCR reaction and the Cu active sites for CO oxidation), the competition adsorption of CO and NH3 on the Cu sites was weakened, resulting in higher CO oxidation performance than the single-active-site catalysts. This work provided insights into the control of flue gas containing CO and NOx over a single catalyst.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods