Kevin Johnson, Juan Xu, Alyssa Yerkeson, Mingming Lu
{"title":"在温和的温度和大气压力下催化 2, 4, 4' 三氯联苯的加氢脱氯反应。","authors":"Kevin Johnson, Juan Xu, Alyssa Yerkeson, Mingming Lu","doi":"10.1080/10962247.2024.2353643","DOIUrl":null,"url":null,"abstract":"<p><p>Polychlorinated biphenyls (PCBs), including all 209 congeners, are designated as persistent organic pollutants (POPs) due to their high toxicity and bioaccumulation in human bodies and the ecosystem. The need for PCB remediation still remains long after their production ban. In this study, a catalytic hydro-dechlorination (HDC) method was employed to dechlorinate 2,4,4'-trichlorobiphenyl (PCB 28), a congener found ubiquitously in multiple environmental media. The HDC of PCB 28 was experimentally studied at mild temperatures viz. ~20, 50, and ~77°C and atmospheric pressure. Et<sub>3</sub>N (triethylamine) was added as a co-catalyst. The dechlorination rates increased with temperature as well as Et<sub>3</sub>N dosage, and the HDC pathway was hypothesized based on the product and intermediates observed. The less chlorinated intermediates suggested that the position of the chlorine strongly impacted HDC rates, and the preference of HDC at para positions can be orders of magnitudes higher than the ortho. The activation energy was estimated in the range of 12.4-13.9 kJ/mole, indicating a diffusion-controlled HDC system.<i>Implications:</i> The remediation need for polychlorinated biphenyls (PCBs) still remains long after their production ban around the world. The development of low-cost methods is highly desirable, especially for developing countries, in response to the Stockholm Convention. In this study, the dechorination of a ubiquitously present PCB congener was studied using a catalytic hydro-dechlorination (HDC) method in low temperatures up to ~77°C and was able to achieve near 100% dechlorination in 6 hr. Results indicated that the HDC process can be performed under mild temperatures and atmospheric conditions and can be a potential solution to real world PCB contamination issues.</p>","PeriodicalId":2,"journal":{"name":"ACS Applied Bio Materials","volume":null,"pages":null},"PeriodicalIF":4.6000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The catalytic hydro-dechlorination of 2, 4, 4' trichlorobiphenyl at mild temperatures and atmospheric pressure.\",\"authors\":\"Kevin Johnson, Juan Xu, Alyssa Yerkeson, Mingming Lu\",\"doi\":\"10.1080/10962247.2024.2353643\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Polychlorinated biphenyls (PCBs), including all 209 congeners, are designated as persistent organic pollutants (POPs) due to their high toxicity and bioaccumulation in human bodies and the ecosystem. The need for PCB remediation still remains long after their production ban. In this study, a catalytic hydro-dechlorination (HDC) method was employed to dechlorinate 2,4,4'-trichlorobiphenyl (PCB 28), a congener found ubiquitously in multiple environmental media. The HDC of PCB 28 was experimentally studied at mild temperatures viz. ~20, 50, and ~77°C and atmospheric pressure. Et<sub>3</sub>N (triethylamine) was added as a co-catalyst. The dechlorination rates increased with temperature as well as Et<sub>3</sub>N dosage, and the HDC pathway was hypothesized based on the product and intermediates observed. The less chlorinated intermediates suggested that the position of the chlorine strongly impacted HDC rates, and the preference of HDC at para positions can be orders of magnitudes higher than the ortho. The activation energy was estimated in the range of 12.4-13.9 kJ/mole, indicating a diffusion-controlled HDC system.<i>Implications:</i> The remediation need for polychlorinated biphenyls (PCBs) still remains long after their production ban around the world. The development of low-cost methods is highly desirable, especially for developing countries, in response to the Stockholm Convention. In this study, the dechorination of a ubiquitously present PCB congener was studied using a catalytic hydro-dechlorination (HDC) method in low temperatures up to ~77°C and was able to achieve near 100% dechlorination in 6 hr. Results indicated that the HDC process can be performed under mild temperatures and atmospheric conditions and can be a potential solution to real world PCB contamination issues.</p>\",\"PeriodicalId\":2,\"journal\":{\"name\":\"ACS Applied Bio Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Bio Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1080/10962247.2024.2353643\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/6/7 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, BIOMATERIALS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Bio Materials","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1080/10962247.2024.2353643","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/6/7 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"MATERIALS SCIENCE, BIOMATERIALS","Score":null,"Total":0}
The catalytic hydro-dechlorination of 2, 4, 4' trichlorobiphenyl at mild temperatures and atmospheric pressure.
Polychlorinated biphenyls (PCBs), including all 209 congeners, are designated as persistent organic pollutants (POPs) due to their high toxicity and bioaccumulation in human bodies and the ecosystem. The need for PCB remediation still remains long after their production ban. In this study, a catalytic hydro-dechlorination (HDC) method was employed to dechlorinate 2,4,4'-trichlorobiphenyl (PCB 28), a congener found ubiquitously in multiple environmental media. The HDC of PCB 28 was experimentally studied at mild temperatures viz. ~20, 50, and ~77°C and atmospheric pressure. Et3N (triethylamine) was added as a co-catalyst. The dechlorination rates increased with temperature as well as Et3N dosage, and the HDC pathway was hypothesized based on the product and intermediates observed. The less chlorinated intermediates suggested that the position of the chlorine strongly impacted HDC rates, and the preference of HDC at para positions can be orders of magnitudes higher than the ortho. The activation energy was estimated in the range of 12.4-13.9 kJ/mole, indicating a diffusion-controlled HDC system.Implications: The remediation need for polychlorinated biphenyls (PCBs) still remains long after their production ban around the world. The development of low-cost methods is highly desirable, especially for developing countries, in response to the Stockholm Convention. In this study, the dechorination of a ubiquitously present PCB congener was studied using a catalytic hydro-dechlorination (HDC) method in low temperatures up to ~77°C and was able to achieve near 100% dechlorination in 6 hr. Results indicated that the HDC process can be performed under mild temperatures and atmospheric conditions and can be a potential solution to real world PCB contamination issues.