{"title":"温度和剂量对煤基活性炭吸附多氯二苯并对二恶英和多氯二苯并呋喃的影响及机理研究","authors":"Peiyue Wang, Jianwen Lai, Xiaoqing Lin, Xiaodong Li, Shuaixi Xu","doi":"10.3390/recycling8060098","DOIUrl":null,"url":null,"abstract":"Using a trace polychlorinated-ρ-dibenzodioxins and dibenzofurans (PCDD/Fs) stabilizing generator, an experimental study related to the influence of temperature (150, 165, and 180 °C) and activated carbon (AC) dosage (0.10, 0.15, and 0.20 g) on the adsorption effect of gas-phase PCDD/Fs via coal-based AC was conducted. Increasing the AC dosage is the most efficient method to improve the PCDD/Fs adsorption efficiency from 65.8% (0.10 g) to 93.0% (0.20 g) at 150 °C in an exponential trend. Both the polychlorinated-ρ-dibenzodioxins (PCDD)/polychlorinated dibenzofurans (PCDF) ratio and the Cl-PCDD/Fs value showed positive correlations, with the AC dosage under the same temperature. Increasing adsorption temperature declined the adsorption capacity of AC, resulting in the exponentially decreased average I-TEQ value adsorbed per gram of AC, from 131.3 ng TEQ/Nm3 (150 °C) to 55.9 ng TEQ/Nm3 (180 °C). The coal-based AC used in this study preferred to adsorb lower chlorinated PCDD/Fs, tetrachlorianted dibenzo-p-dioxin and dibenzofurans (TCDD/Fs), and pentachlorianted dibenzo-p-dioxin and dibenzofurans (PeCDD/Fs) than highly chlorinated PCDD/Fs, heptachlorianted dibenzo-p-dioxin and dibenzofurans (HpCDD/Fs), hexachlorinated dibenzo-p-dioxin and dibenzofurans (HxCDD/Fs), and octachlorianted dibenzo-p-dioxin and dibenzofurans (OCDD/Fs), which was aggravated by the increasing temperature. The characterization of the surface properties of AC revealed that slight oxidation occurred on the AC surface during the adsorption process, introducing oxygen to the competitive adsorption. In addition, it was found in this study that an increased temperature led to a higher content of hydrophilic carboxyl and anhydride groups and weakened π-π interactions, which were also partly responsible for the negative impact of the increasing temperature on the AC adsorption capacity. The results of this study can contribute to the operation optimization for controlling PCDD/F emissions from municipal solid waste incineration (MSWI).","PeriodicalId":36729,"journal":{"name":"Recycling","volume":null,"pages":null},"PeriodicalIF":4.6000,"publicationDate":"2023-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A Study on the Influence and Mechanism of Temperature and Dosage on PCDD/Fs Adsorption via Coal-Based Activated Carbon\",\"authors\":\"Peiyue Wang, Jianwen Lai, Xiaoqing Lin, Xiaodong Li, Shuaixi Xu\",\"doi\":\"10.3390/recycling8060098\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Using a trace polychlorinated-ρ-dibenzodioxins and dibenzofurans (PCDD/Fs) stabilizing generator, an experimental study related to the influence of temperature (150, 165, and 180 °C) and activated carbon (AC) dosage (0.10, 0.15, and 0.20 g) on the adsorption effect of gas-phase PCDD/Fs via coal-based AC was conducted. Increasing the AC dosage is the most efficient method to improve the PCDD/Fs adsorption efficiency from 65.8% (0.10 g) to 93.0% (0.20 g) at 150 °C in an exponential trend. Both the polychlorinated-ρ-dibenzodioxins (PCDD)/polychlorinated dibenzofurans (PCDF) ratio and the Cl-PCDD/Fs value showed positive correlations, with the AC dosage under the same temperature. Increasing adsorption temperature declined the adsorption capacity of AC, resulting in the exponentially decreased average I-TEQ value adsorbed per gram of AC, from 131.3 ng TEQ/Nm3 (150 °C) to 55.9 ng TEQ/Nm3 (180 °C). The coal-based AC used in this study preferred to adsorb lower chlorinated PCDD/Fs, tetrachlorianted dibenzo-p-dioxin and dibenzofurans (TCDD/Fs), and pentachlorianted dibenzo-p-dioxin and dibenzofurans (PeCDD/Fs) than highly chlorinated PCDD/Fs, heptachlorianted dibenzo-p-dioxin and dibenzofurans (HpCDD/Fs), hexachlorinated dibenzo-p-dioxin and dibenzofurans (HxCDD/Fs), and octachlorianted dibenzo-p-dioxin and dibenzofurans (OCDD/Fs), which was aggravated by the increasing temperature. The characterization of the surface properties of AC revealed that slight oxidation occurred on the AC surface during the adsorption process, introducing oxygen to the competitive adsorption. In addition, it was found in this study that an increased temperature led to a higher content of hydrophilic carboxyl and anhydride groups and weakened π-π interactions, which were also partly responsible for the negative impact of the increasing temperature on the AC adsorption capacity. The results of this study can contribute to the operation optimization for controlling PCDD/F emissions from municipal solid waste incineration (MSWI).\",\"PeriodicalId\":36729,\"journal\":{\"name\":\"Recycling\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2023-12-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Recycling\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.3390/recycling8060098\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Recycling","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.3390/recycling8060098","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY","Score":null,"Total":0}
引用次数: 0
摘要
利用痕量多氯-ρ-二苯并二噁英和二苯并呋喃(PCDD/Fs)稳定发生器,就温度(150、165 和 180 °C)和活性炭(AC)用量(0.10、0.15 和 0.20 克)对煤基 AC 吸附气相多氯-ρ-二苯并二噁英和二苯并呋喃(PCDD/Fs)效果的影响进行了实验研究。在 150 °C条件下,增加活性炭用量是提高多氯二苯并对二恶英和多氯二苯并呋喃吸附效率的最有效方法,吸附效率从 65.8%(0.10 克)提高到 93.0%(0.20 克),且呈指数增长趋势。在相同温度下,多氯-ρ-二苯并二恶英(PCDD)/多氯二苯并呋喃(PCDF)比值和 Cl-PCDD/Fs 值均与 AC 的用量呈正相关。吸附温度升高会降低 AC 的吸附容量,导致每克 AC 平均吸附的 I-TEQ 值呈指数下降,从 131.3 ng TEQ/Nm3 (150 °C) 降至 55.9 ng TEQ/Nm3 (180 °C) 。与高度氯化的多氯二苯并对二恶英和多氯二苯并呋喃(PCDD/Fs)相比,本研究中使用的煤基 AC 更倾向于吸附氯化程度较低的多氯二苯并对二恶英和多氯二苯并呋喃(PCDD/Fs)、四氯二苯并对二恶英和二苯并呋喃(TCDD/Fs)以及五氯二苯并对二恶英和二苯并呋喃(PeCDD/Fs)、和六氯二苯并对二恶英和二苯并呋喃(HxCDD/Fs)以及八氯二苯并对二恶英和二苯并呋喃(OCDD/Fs)相比,温度升高会加剧这种情况。对 AC 表面特性的表征表明,在吸附过程中,AC 表面发生了轻微氧化,在竞争性吸附中引入了氧气。此外,本研究还发现,温度升高导致亲水性羧基和酸酐基团含量增加,π-π 相互作用减弱,这也是温度升高对 AC 吸附能力产生负面影响的部分原因。本研究的结果有助于优化城市固体废物焚烧(MSWI)的操作,以控制多氯二苯并对二恶英和多氯二苯并呋喃的排放。
A Study on the Influence and Mechanism of Temperature and Dosage on PCDD/Fs Adsorption via Coal-Based Activated Carbon
Using a trace polychlorinated-ρ-dibenzodioxins and dibenzofurans (PCDD/Fs) stabilizing generator, an experimental study related to the influence of temperature (150, 165, and 180 °C) and activated carbon (AC) dosage (0.10, 0.15, and 0.20 g) on the adsorption effect of gas-phase PCDD/Fs via coal-based AC was conducted. Increasing the AC dosage is the most efficient method to improve the PCDD/Fs adsorption efficiency from 65.8% (0.10 g) to 93.0% (0.20 g) at 150 °C in an exponential trend. Both the polychlorinated-ρ-dibenzodioxins (PCDD)/polychlorinated dibenzofurans (PCDF) ratio and the Cl-PCDD/Fs value showed positive correlations, with the AC dosage under the same temperature. Increasing adsorption temperature declined the adsorption capacity of AC, resulting in the exponentially decreased average I-TEQ value adsorbed per gram of AC, from 131.3 ng TEQ/Nm3 (150 °C) to 55.9 ng TEQ/Nm3 (180 °C). The coal-based AC used in this study preferred to adsorb lower chlorinated PCDD/Fs, tetrachlorianted dibenzo-p-dioxin and dibenzofurans (TCDD/Fs), and pentachlorianted dibenzo-p-dioxin and dibenzofurans (PeCDD/Fs) than highly chlorinated PCDD/Fs, heptachlorianted dibenzo-p-dioxin and dibenzofurans (HpCDD/Fs), hexachlorinated dibenzo-p-dioxin and dibenzofurans (HxCDD/Fs), and octachlorianted dibenzo-p-dioxin and dibenzofurans (OCDD/Fs), which was aggravated by the increasing temperature. The characterization of the surface properties of AC revealed that slight oxidation occurred on the AC surface during the adsorption process, introducing oxygen to the competitive adsorption. In addition, it was found in this study that an increased temperature led to a higher content of hydrophilic carboxyl and anhydride groups and weakened π-π interactions, which were also partly responsible for the negative impact of the increasing temperature on the AC adsorption capacity. The results of this study can contribute to the operation optimization for controlling PCDD/F emissions from municipal solid waste incineration (MSWI).