Le Yu , Lei Wang , Zhaoyi Xu , Shourong Zheng , Tao Long
{"title":"调整RhNi/CeO2催化剂的性能以提高氯酸盐还原效率","authors":"Le Yu , Lei Wang , Zhaoyi Xu , Shourong Zheng , Tao Long","doi":"10.1016/j.jece.2025.119301","DOIUrl":null,"url":null,"abstract":"<div><div>Chlorate (ClO<sub>3</sub><sup>-</sup>) are commonly identified oxyanions pollutant in the water environment, and catalytic hydrogenation reduction of oxyanions has emerged as a promising water treatment strategy. Supported Rh catalysts have been widely applied in the liquid phase catalytic hydrogenation due to their high activation capacity for H<sub>2</sub>, while exploring highly active and stable catalysts for different pollutants remains a great challenge. The transition metal Ni was introduced into the Rh-based catalyst Rh/CeO<sub>2</sub> by the impregnation method to obtain the bimetallic catalyst RhNi<sub>10</sub>/CeO<sub>2</sub>, which was used in the catalytic hydrogenation reduction of ClO<sub>3</sub><sup>-</sup>. In-situ DRIFTS identifies the highly dispersed Rh nanoparticles in the catalyst, and the strong metal-support interaction between the supported bimetallic Rh-Ni and CeO<sub>2</sub> supports is determined by XPS characterization. RhNi<sub>10</sub>/CeO<sub>2</sub> exhibits an initial activity approximately 27 times higher than that of Rh/CeO<sub>2</sub>. Furthermore, theoretical calculations corroborate the experimental observation that when chlorate is adsorbed on the Rh surface, the energy released increases with the introduction of Ni. We reveal the enhanced reactivity of the RhNi<sub>10</sub>/CeO<sub>2</sub> through changing ClO<sub>3</sub><sup>-</sup> concentration, which renders adsorption on catalyst surface pathway sequencely more favorable. In addition, the reusability of the catalyst was tested by adding chloride ions (Cl<sup>-</sup>) and catalyst recycling. Results revealed that RhNi<sub>10</sub>/CeO<sub>2</sub> maintained 100 % removal efficiency despite slight inhibition by Cl<sup>-</sup> (12 times the ClO<sub>3</sub><sup>-</sup> concentration of 0.4 mM). After 5 cycles, the activity loss remained below 9 % with 100 % removal efficiency. The bimetallic synergy leads to increased resistance to chloride ion interference, providing high catalytic stability.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"13 6","pages":"Article 119301"},"PeriodicalIF":7.2000,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tailoring the properties of RhNi/CeO2 catalysts for improved chlorate reduction efficiency\",\"authors\":\"Le Yu , Lei Wang , Zhaoyi Xu , Shourong Zheng , Tao Long\",\"doi\":\"10.1016/j.jece.2025.119301\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Chlorate (ClO<sub>3</sub><sup>-</sup>) are commonly identified oxyanions pollutant in the water environment, and catalytic hydrogenation reduction of oxyanions has emerged as a promising water treatment strategy. Supported Rh catalysts have been widely applied in the liquid phase catalytic hydrogenation due to their high activation capacity for H<sub>2</sub>, while exploring highly active and stable catalysts for different pollutants remains a great challenge. The transition metal Ni was introduced into the Rh-based catalyst Rh/CeO<sub>2</sub> by the impregnation method to obtain the bimetallic catalyst RhNi<sub>10</sub>/CeO<sub>2</sub>, which was used in the catalytic hydrogenation reduction of ClO<sub>3</sub><sup>-</sup>. In-situ DRIFTS identifies the highly dispersed Rh nanoparticles in the catalyst, and the strong metal-support interaction between the supported bimetallic Rh-Ni and CeO<sub>2</sub> supports is determined by XPS characterization. RhNi<sub>10</sub>/CeO<sub>2</sub> exhibits an initial activity approximately 27 times higher than that of Rh/CeO<sub>2</sub>. Furthermore, theoretical calculations corroborate the experimental observation that when chlorate is adsorbed on the Rh surface, the energy released increases with the introduction of Ni. We reveal the enhanced reactivity of the RhNi<sub>10</sub>/CeO<sub>2</sub> through changing ClO<sub>3</sub><sup>-</sup> concentration, which renders adsorption on catalyst surface pathway sequencely more favorable. In addition, the reusability of the catalyst was tested by adding chloride ions (Cl<sup>-</sup>) and catalyst recycling. Results revealed that RhNi<sub>10</sub>/CeO<sub>2</sub> maintained 100 % removal efficiency despite slight inhibition by Cl<sup>-</sup> (12 times the ClO<sub>3</sub><sup>-</sup> concentration of 0.4 mM). After 5 cycles, the activity loss remained below 9 % with 100 % removal efficiency. The bimetallic synergy leads to increased resistance to chloride ion interference, providing high catalytic stability.</div></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":\"13 6\",\"pages\":\"Article 119301\"},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2025-09-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343725039971\",\"RegionNum\":2,\"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":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343725039971","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Tailoring the properties of RhNi/CeO2 catalysts for improved chlorate reduction efficiency
Chlorate (ClO3-) are commonly identified oxyanions pollutant in the water environment, and catalytic hydrogenation reduction of oxyanions has emerged as a promising water treatment strategy. Supported Rh catalysts have been widely applied in the liquid phase catalytic hydrogenation due to their high activation capacity for H2, while exploring highly active and stable catalysts for different pollutants remains a great challenge. The transition metal Ni was introduced into the Rh-based catalyst Rh/CeO2 by the impregnation method to obtain the bimetallic catalyst RhNi10/CeO2, which was used in the catalytic hydrogenation reduction of ClO3-. In-situ DRIFTS identifies the highly dispersed Rh nanoparticles in the catalyst, and the strong metal-support interaction between the supported bimetallic Rh-Ni and CeO2 supports is determined by XPS characterization. RhNi10/CeO2 exhibits an initial activity approximately 27 times higher than that of Rh/CeO2. Furthermore, theoretical calculations corroborate the experimental observation that when chlorate is adsorbed on the Rh surface, the energy released increases with the introduction of Ni. We reveal the enhanced reactivity of the RhNi10/CeO2 through changing ClO3- concentration, which renders adsorption on catalyst surface pathway sequencely more favorable. In addition, the reusability of the catalyst was tested by adding chloride ions (Cl-) and catalyst recycling. Results revealed that RhNi10/CeO2 maintained 100 % removal efficiency despite slight inhibition by Cl- (12 times the ClO3- concentration of 0.4 mM). After 5 cycles, the activity loss remained below 9 % with 100 % removal efficiency. The bimetallic synergy leads to increased resistance to chloride ion interference, providing high catalytic stability.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.