{"title":"cu修饰Co3O4中表面晶格Co-O键及CuO与Co3O4界面相互作用对甲苯和丙酮催化完全氧化的影响","authors":"Yao Li, Xiaoyu Niu, Yujun Zhu","doi":"10.1016/j.seppur.2025.133316","DOIUrl":null,"url":null,"abstract":"Modifying the electronic structure of Co<sub>3</sub>O<sub>4</sub> and enhancing the rapid cycling ability between Co<sup>2+</sup> and Co<sup>3+</sup> are effective strategies to improve the catalytic oxidation of VOC by Co-based catalysts. The ionic radius of Cu is similar to that of Co, and the valence state of Cu is variable. Therefore, Cu<sub>a</sub>CoO<sub>x</sub> catalysts with varying Cu/Co molar ratios were synthesized through the hydrothermal method, followed by a comprehensive assessment of their oxidation performance for toluene and acetone degradation. Among them, Cu<sub>0.55</sub>CoO<sub>x</sub> can convert 90 % acetone and toluene at 169 and 217 °C (T<sub>90</sub>), respectively, but it shows quickly deactivation in the long-term activity stability test. Through controlled variation of the Cu/Co molar ratio, the amount of metal ions incorporated into Co<sub>3</sub>O<sub>4</sub> varies, which influences the electronic structure of the catalyst. Compared with Cu<sub>0.55</sub>CoO<sub>x</sub>, T<sub>90</sub> values over Cu<sub>0.18</sub>CoO<sub>x</sub> are177 and 222°C for the oxidation of acetone and toluene, respectively, but the activity can maintain stability in long time tests. These results show that the doping of Cu in Co<sub>3</sub>O<sub>4</sub> can cause lattice distortion, produce a Cu–O-Co bond, weaken the bond energy of the Co-O bond, thus increasing the mobility of lattice oxygen. When Cu is excessive, the appearance of CuO changes the structure of the catalyst and forms the CuO-Co<sub>3</sub>O<sub>4</sub> interface, which can also promote the generation of active oxygen at the interface. However, during the long-term test of toluene and acetone, the rate of active oxygen recycling is slow in the interface, resulting in poor stability.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"9 1","pages":""},"PeriodicalIF":8.1000,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of surface lattice Co-O bonds and interfacial interaction between CuO and Co3O4 in Cu-modified Co3O4 on catalytic complete oxidation of toluene and acetone\",\"authors\":\"Yao Li, Xiaoyu Niu, Yujun Zhu\",\"doi\":\"10.1016/j.seppur.2025.133316\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Modifying the electronic structure of Co<sub>3</sub>O<sub>4</sub> and enhancing the rapid cycling ability between Co<sup>2+</sup> and Co<sup>3+</sup> are effective strategies to improve the catalytic oxidation of VOC by Co-based catalysts. The ionic radius of Cu is similar to that of Co, and the valence state of Cu is variable. Therefore, Cu<sub>a</sub>CoO<sub>x</sub> catalysts with varying Cu/Co molar ratios were synthesized through the hydrothermal method, followed by a comprehensive assessment of their oxidation performance for toluene and acetone degradation. Among them, Cu<sub>0.55</sub>CoO<sub>x</sub> can convert 90 % acetone and toluene at 169 and 217 °C (T<sub>90</sub>), respectively, but it shows quickly deactivation in the long-term activity stability test. Through controlled variation of the Cu/Co molar ratio, the amount of metal ions incorporated into Co<sub>3</sub>O<sub>4</sub> varies, which influences the electronic structure of the catalyst. Compared with Cu<sub>0.55</sub>CoO<sub>x</sub>, T<sub>90</sub> values over Cu<sub>0.18</sub>CoO<sub>x</sub> are177 and 222°C for the oxidation of acetone and toluene, respectively, but the activity can maintain stability in long time tests. These results show that the doping of Cu in Co<sub>3</sub>O<sub>4</sub> can cause lattice distortion, produce a Cu–O-Co bond, weaken the bond energy of the Co-O bond, thus increasing the mobility of lattice oxygen. When Cu is excessive, the appearance of CuO changes the structure of the catalyst and forms the CuO-Co<sub>3</sub>O<sub>4</sub> interface, which can also promote the generation of active oxygen at the interface. However, during the long-term test of toluene and acetone, the rate of active oxygen recycling is slow in the interface, resulting in poor stability.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"9 1\",\"pages\":\"\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-05-03\",\"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.2025.133316\",\"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.2025.133316","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}
Effect of surface lattice Co-O bonds and interfacial interaction between CuO and Co3O4 in Cu-modified Co3O4 on catalytic complete oxidation of toluene and acetone
Modifying the electronic structure of Co3O4 and enhancing the rapid cycling ability between Co2+ and Co3+ are effective strategies to improve the catalytic oxidation of VOC by Co-based catalysts. The ionic radius of Cu is similar to that of Co, and the valence state of Cu is variable. Therefore, CuaCoOx catalysts with varying Cu/Co molar ratios were synthesized through the hydrothermal method, followed by a comprehensive assessment of their oxidation performance for toluene and acetone degradation. Among them, Cu0.55CoOx can convert 90 % acetone and toluene at 169 and 217 °C (T90), respectively, but it shows quickly deactivation in the long-term activity stability test. Through controlled variation of the Cu/Co molar ratio, the amount of metal ions incorporated into Co3O4 varies, which influences the electronic structure of the catalyst. Compared with Cu0.55CoOx, T90 values over Cu0.18CoOx are177 and 222°C for the oxidation of acetone and toluene, respectively, but the activity can maintain stability in long time tests. These results show that the doping of Cu in Co3O4 can cause lattice distortion, produce a Cu–O-Co bond, weaken the bond energy of the Co-O bond, thus increasing the mobility of lattice oxygen. When Cu is excessive, the appearance of CuO changes the structure of the catalyst and forms the CuO-Co3O4 interface, which can also promote the generation of active oxygen at the interface. However, during the long-term test of toluene and acetone, the rate of active oxygen recycling is slow in the interface, resulting in poor stability.
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.