Jinyan Xiao, Chi Zhang, Lei Yang, Shengwei Tang, Wenxiang Tang
{"title":"三维分层多孔 Co-Cu 纳米复合材料在低温高空间速度下催化消除挥发性有机化合物的非凡协同作用","authors":"Jinyan Xiao, Chi Zhang, Lei Yang, Shengwei Tang, Wenxiang Tang","doi":"10.1016/j.jes.2024.04.025","DOIUrl":null,"url":null,"abstract":"<div><p>It is still a challenge to develop hierarchically nanostructured catalysts with simple approaches to enhance the low-temperature catalytic activity. Herein, a set of mesoporous Co-Cu binary metal oxides with different morphologies were successfully prepared via a facile ammonium bicarbonate precipitation method without any templates or surfactants, which were further applied for catalytic removal of carcinogenic toluene. Among the catalysts with different ratios, the CoCu<sub>0.2</sub> composite oxide presented the best performance, where the temperature required for 90% conversion of toluene was only 237°C at the high weight hour space velocity (WHSV) of 240,000 mL/(g<sub>cat</sub>·hr). Meanwhile, compared to the related Co-Cu composite oxides prepared by using different precipitants (NaOH and H<sub>2</sub>C<sub>2</sub>O<sub>4</sub>), the NH<sub>4</sub>HCO<sub>3</sub>-derived CoCu<sub>0.2</sub> sample exhibited better catalytic efficiency in toluene oxidation, while the T<sub>90</sub> were 22 and 28°C lower than those samples prepared by NaOH and H<sub>2</sub>C<sub>2</sub>O<sub>4</sub> routes, respectively. Based on various characterizations, it could be deduced that the excellent performance was related to the small crystal size (6.7 nm), large specific surface area (77.0 m<sup>2</sup>/g), hollow hierarchical nanostructure with abundant high valence Co ions and adsorbed oxygen species. In situ DRIFTS further revealed that the possible reaction pathway for the toluene oxidation over CoCu<sub>0.2</sub> catalyst followed the route of absorbed toluene → benzyl alcohol → benzaldehyde → benzoic acid → carbonate → CO<sub>2</sub> and H<sub>2</sub>O. In addition, CoCu<sub>0.2</sub> sample could keep stable with long-time operation and occur little inactivation under humid condition (5 vol.% water), which revealed that the NH<sub>4</sub>HCO<sub>3</sub>-derived CoCu<sub>0.2</sub> nanocatalyst possessed great potential in industrial applications for VOCs abatement.</p></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2024-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Extraordinary synergy on 3D hierarchical porous Co-Cu nanocomposite for catalytic elimination of VOCs at low temperature and high space velocity\",\"authors\":\"Jinyan Xiao, Chi Zhang, Lei Yang, Shengwei Tang, Wenxiang Tang\",\"doi\":\"10.1016/j.jes.2024.04.025\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>It is still a challenge to develop hierarchically nanostructured catalysts with simple approaches to enhance the low-temperature catalytic activity. Herein, a set of mesoporous Co-Cu binary metal oxides with different morphologies were successfully prepared via a facile ammonium bicarbonate precipitation method without any templates or surfactants, which were further applied for catalytic removal of carcinogenic toluene. Among the catalysts with different ratios, the CoCu<sub>0.2</sub> composite oxide presented the best performance, where the temperature required for 90% conversion of toluene was only 237°C at the high weight hour space velocity (WHSV) of 240,000 mL/(g<sub>cat</sub>·hr). Meanwhile, compared to the related Co-Cu composite oxides prepared by using different precipitants (NaOH and H<sub>2</sub>C<sub>2</sub>O<sub>4</sub>), the NH<sub>4</sub>HCO<sub>3</sub>-derived CoCu<sub>0.2</sub> sample exhibited better catalytic efficiency in toluene oxidation, while the T<sub>90</sub> were 22 and 28°C lower than those samples prepared by NaOH and H<sub>2</sub>C<sub>2</sub>O<sub>4</sub> routes, respectively. Based on various characterizations, it could be deduced that the excellent performance was related to the small crystal size (6.7 nm), large specific surface area (77.0 m<sup>2</sup>/g), hollow hierarchical nanostructure with abundant high valence Co ions and adsorbed oxygen species. In situ DRIFTS further revealed that the possible reaction pathway for the toluene oxidation over CoCu<sub>0.2</sub> catalyst followed the route of absorbed toluene → benzyl alcohol → benzaldehyde → benzoic acid → carbonate → CO<sub>2</sub> and H<sub>2</sub>O. In addition, CoCu<sub>0.2</sub> sample could keep stable with long-time operation and occur little inactivation under humid condition (5 vol.% water), which revealed that the NH<sub>4</sub>HCO<sub>3</sub>-derived CoCu<sub>0.2</sub> nanocatalyst possessed great potential in industrial applications for VOCs abatement.</p></div>\",\"PeriodicalId\":15788,\"journal\":{\"name\":\"Journal of Environmental Sciences-china\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2024-04-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Sciences-china\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1001074224002067\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Sciences-china","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1001074224002067","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Extraordinary synergy on 3D hierarchical porous Co-Cu nanocomposite for catalytic elimination of VOCs at low temperature and high space velocity
It is still a challenge to develop hierarchically nanostructured catalysts with simple approaches to enhance the low-temperature catalytic activity. Herein, a set of mesoporous Co-Cu binary metal oxides with different morphologies were successfully prepared via a facile ammonium bicarbonate precipitation method without any templates or surfactants, which were further applied for catalytic removal of carcinogenic toluene. Among the catalysts with different ratios, the CoCu0.2 composite oxide presented the best performance, where the temperature required for 90% conversion of toluene was only 237°C at the high weight hour space velocity (WHSV) of 240,000 mL/(gcat·hr). Meanwhile, compared to the related Co-Cu composite oxides prepared by using different precipitants (NaOH and H2C2O4), the NH4HCO3-derived CoCu0.2 sample exhibited better catalytic efficiency in toluene oxidation, while the T90 were 22 and 28°C lower than those samples prepared by NaOH and H2C2O4 routes, respectively. Based on various characterizations, it could be deduced that the excellent performance was related to the small crystal size (6.7 nm), large specific surface area (77.0 m2/g), hollow hierarchical nanostructure with abundant high valence Co ions and adsorbed oxygen species. In situ DRIFTS further revealed that the possible reaction pathway for the toluene oxidation over CoCu0.2 catalyst followed the route of absorbed toluene → benzyl alcohol → benzaldehyde → benzoic acid → carbonate → CO2 and H2O. In addition, CoCu0.2 sample could keep stable with long-time operation and occur little inactivation under humid condition (5 vol.% water), which revealed that the NH4HCO3-derived CoCu0.2 nanocatalyst possessed great potential in industrial applications for VOCs abatement.
期刊介绍:
The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.