首页 > 最新文献

Process Safety and Environmental Protection最新文献

英文 中文
Risk assessment and management strategy of geologic carbon storage in multi-well site 多井场地质碳封存的风险评估与管理策略
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-28 DOI: 10.1016/j.psep.2024.10.097
Tianlong Yu , Jingqi Gao , Hao Yang , Xiang Wu
Many oil and gas production areas may serve as potential geologic carbon storage(GCS) sites, but large-scale CO2 injection in these sites with multiple legacy wells poses a leakage risk. Therefore, it is crucial to analyze the well leakage risk of these GCS sites and develop effective risk management strategies to minimize CO2 and brine leakage. In this study, we hypothesized a GCS site based on the Jingbian area in the Ordos Basin, which has 177 legacy wells. We conducted a three-dimensional geological modeling of the site and simulated the injection and migration of CO2. Using the National Risk Assessment Partnership’s open-source Integrated Assessment toolkit, we outlined a workflow for assessing the risk of CO2 and brine leakage in multi-well site. Simulations of CO2 and brine leakage through 177 existing wells into the USDW or the atmosphere are used as an indicator of potential risk. Finally, we proposed risk management strategies based on well integrity, injection rate, and pollution range, verifying their effectiveness. The results of the 95th percentile (P95) model implementation showed that the leakage risk of GCS sites was low over 150 years, with a CO2 leakage of 15,996.4 tonnes(0.16 % of the 107 t injected). The risk-based strategy outperformed both distance-based strategy and hybrid strategy overall. Reducing injection rates alone proved ineffective as a risk management strategy. Only high-risk wells near the injection zone may cause pollution to USDW. Meanwhile, legacy wells have negligible impact on atmospheric pollution. The management strategy based on pollution range can be used as a supplement to the risk-based strategy in practical engineering.
许多油气生产区都可能成为潜在的地质碳封存(GCS)地点,但在这些拥有多口遗留井的地点大规模注入二氧化碳会带来泄漏风险。因此,分析这些地质碳封存地点的油井泄漏风险并制定有效的风险管理策略以最大限度地减少二氧化碳和盐水泄漏至关重要。在本研究中,我们以鄂尔多斯盆地靖边地区为基础,假设了一个拥有 177 口遗留井的全球碳捕集与封存区。我们对该地点进行了三维地质建模,并模拟了二氧化碳的注入和迁移。利用国家风险评估伙伴关系的开源综合评估工具包,我们概述了评估多井场二氧化碳和盐水泄漏风险的工作流程。模拟二氧化碳和盐水通过现有的 177 口井渗漏到美国水井或大气中,以此作为潜在风险的指标。最后,我们提出了基于油井完整性、注入率和污染范围的风险管理策略,并验证了其有效性。第 95 百分位数(P95)模型的实施结果表明,150 年内全球碳捕获和封存地点的泄漏风险较低,二氧化碳泄漏量为 15996.4 吨(占 107 吨注入量的 0.16%)。基于风险的战略总体上优于基于距离的战略和混合战略。事实证明,降低注入率本身并不是一种有效的风险管理策略。只有注入区附近的高风险井才可能对 USDW 造成污染。同时,遗留井对大气污染的影响微乎其微。在实际工程中,基于污染范围的管理策略可作为基于风险的策略的补充。
{"title":"Risk assessment and management strategy of geologic carbon storage in multi-well site","authors":"Tianlong Yu ,&nbsp;Jingqi Gao ,&nbsp;Hao Yang ,&nbsp;Xiang Wu","doi":"10.1016/j.psep.2024.10.097","DOIUrl":"10.1016/j.psep.2024.10.097","url":null,"abstract":"<div><div>Many oil and gas production areas may serve as potential geologic carbon storage(GCS) sites, but large-scale CO<sub>2</sub> injection in these sites with multiple legacy wells poses a leakage risk. Therefore, it is crucial to analyze the well leakage risk of these GCS sites and develop effective risk management strategies to minimize CO<sub>2</sub> and brine leakage. In this study, we hypothesized a GCS site based on the Jingbian area in the Ordos Basin, which has 177 legacy wells. We conducted a three-dimensional geological modeling of the site and simulated the injection and migration of CO<sub>2</sub>. Using the National Risk Assessment Partnership’s open-source Integrated Assessment toolkit, we outlined a workflow for assessing the risk of CO<sub>2</sub> and brine leakage in multi-well site. Simulations of CO<sub>2</sub> and brine leakage through 177 existing wells into the USDW or the atmosphere are used as an indicator of potential risk. Finally, we proposed risk management strategies based on well integrity, injection rate, and pollution range, verifying their effectiveness. The results of the 95th percentile (P95) model implementation showed that the leakage risk of GCS sites was low over 150 years, with a CO<sub>2</sub> leakage of 15,996.4 tonnes(0.16 % of the 10<sup>7</sup> t injected). The risk-based strategy outperformed both distance-based strategy and hybrid strategy overall. Reducing injection rates alone proved ineffective as a risk management strategy. Only high-risk wells near the injection zone may cause pollution to USDW. Meanwhile, legacy wells have negligible impact on atmospheric pollution. The management strategy based on pollution range can be used as a supplement to the risk-based strategy in practical engineering.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 822-836"},"PeriodicalIF":6.9,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient and easy-to-recover immobilized heterogeneous catalyst CuSF/ZIF-67 activates peroxymonosulfate to remove refractory antibiotics 高效且易于回收的固定化异相催化剂 CuSF/ZIF-67 活化过一硫酸盐以去除难溶性抗生素
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-28 DOI: 10.1016/j.psep.2024.10.098
Xueying Yang , Xiangdong Zhang , Jiaqi Wang , Jian Zhang , Haina Bai
Aiming at the challenge of catalyst recovery and reuse from aqueous solution, in this study, a novel immobilized heterogeneous catalyst, CuSF/ZIF-67, was innovatively designed and prepared, and PMS was activated by the synergistic effect of Cu, Co and low-valent sulfur species. The catalyst can degrade 98.01 % OTC (20 mg/L) within 20 minutes. Its high efficiency is mainly attributed to the promotion of Co2+ regeneration by low-valent sulfur species (S2-/S22-) and Cu+. In addition, the catalyst showed strong oxidation ability, and through the synergistic effect of free radicals (SO4•-, •OH, •O2-) and non-free radicals (1O2), it realized the efficient removal of various antibiotics and dyes. Additionally, after 10 cycles, its degradation efficiency only decreased by 5.12 %, which proved its good reusability. The intermediate was characterized in detail through LC-MS technology. The biological toxicity of the degradation intermediate was assessed both theoretically and experimentally, relying on the QSAR model and toxicology experiment. Ultimately, we designed and fabricated a catalytic reactor to validate the performance of the catalyst in the actual wastewater remediation process. The experimental results show that the solid catalyst shows great potential in practical application. This study not only offers a novel concept for the design of efficient and recyclable catalysts, but also furnishes robust technical support for the actual wastewater remediation.
针对催化剂从水溶液中回收和再利用的难题,本研究创新性地设计和制备了一种新型固定化异相催化剂 CuSF/ZIF-67,并通过 Cu、Co 和低价硫物种的协同作用激活了 PMS。该催化剂可在 20 分钟内降解 98.01% 的 OTC(20 mg/L)。催化剂的高效率主要归功于低价硫(S2-/S22-)和 Cu+ 对 Co2+ 再生的促进作用。此外,催化剂还具有很强的氧化能力,通过自由基(SO4--、-OH、-O2-)和非自由基(1O2)的协同作用,实现了对各种抗生素和染料的高效去除。此外,经过 10 次循环后,其降解效率仅下降了 5.12%,这证明了其良好的可再利用性。通过 LC-MS 技术对该中间体进行了详细表征。通过 QSAR 模型和毒理学实验,对降解中间体的生物毒性进行了理论和实验评估。最后,我们设计并制造了一个催化反应器,以验证催化剂在实际废水修复过程中的性能。实验结果表明,固体催化剂在实际应用中显示出巨大的潜力。这项研究不仅为高效、可回收催化剂的设计提供了新的理念,而且为实际废水修复提供了有力的技术支持。
{"title":"Efficient and easy-to-recover immobilized heterogeneous catalyst CuSF/ZIF-67 activates peroxymonosulfate to remove refractory antibiotics","authors":"Xueying Yang ,&nbsp;Xiangdong Zhang ,&nbsp;Jiaqi Wang ,&nbsp;Jian Zhang ,&nbsp;Haina Bai","doi":"10.1016/j.psep.2024.10.098","DOIUrl":"10.1016/j.psep.2024.10.098","url":null,"abstract":"<div><div>Aiming at the challenge of catalyst recovery and reuse from aqueous solution, in this study, a novel immobilized heterogeneous catalyst, CuSF/ZIF-67, was innovatively designed and prepared, and PMS was activated by the synergistic effect of Cu, Co and low-valent sulfur species. The catalyst can degrade 98.01 % OTC (20 mg/L) within 20 minutes. Its high efficiency is mainly attributed to the promotion of Co<sup>2+</sup> regeneration by low-valent sulfur species (S<sup>2-</sup>/S<sub>2</sub><sup>2-</sup>) and Cu<sup>+</sup>. In addition, the catalyst showed strong oxidation ability, and through the synergistic effect of free radicals (SO<sub>4</sub><sup>•-</sup>, •OH, •O<sub>2</sub><sup>-</sup>) and non-free radicals (<sup>1</sup>O<sub>2</sub>), it realized the efficient removal of various antibiotics and dyes. Additionally, after 10 cycles, its degradation efficiency only decreased by 5.12 %, which proved its good reusability. The intermediate was characterized in detail through LC-MS technology. The biological toxicity of the degradation intermediate was assessed both theoretically and experimentally, relying on the QSAR model and toxicology experiment. Ultimately, we designed and fabricated a catalytic reactor to validate the performance of the catalyst in the actual wastewater remediation process. The experimental results show that the solid catalyst shows great potential in practical application. This study not only offers a novel concept for the design of efficient and recyclable catalysts, but also furnishes robust technical support for the actual wastewater remediation.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 769-781"},"PeriodicalIF":6.9,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554910","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Plasma coupled with ultrasonic for degradation of organic pollutants in water: Revealing the generation of free radicals and the dominant degradation pathways 等离子体结合超声波降解水中的有机污染物:揭示自由基的产生和主要降解途径
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-28 DOI: 10.1016/j.psep.2024.10.095
He Guo, Shuang Yang, Jiaxin Wang, Wenxuan Jiang, Yawen Wang
This study explores the synergistic effects of dielectric barrier discharge (DBD) plasma coupled with ultrasound (US) in the degradation of organic pollutants in water. The optimal degradation conditions were determined to be 100 W ultrasonic power, 190 V DBD plasma voltage, and neutral pH. The combination of DBD plasma and US significantly enhances the generation of reactive species (·OH, ·O2-, and 1O2), leading to a 97.3 % degradation efficiency of methyl orange (MO), which is 17.3 % higher than DBD plasma alone. Electron spin resonance (ESR) identified ·OH, ·O2-, and 1O2 in DBD/US system, and radical scavengers were employed to elucidate their roles. The degradation process was assessed through changes in pH, conductivity, TOC and COD, with characterization and analysis via UV-Vis and LC-MS. By combining LC-MS with density functional theory (DFT) calculations, nine intermediates were identified and three degradation pathways dominated by free radicals were established. Additionally, the DBD/US system treated wastewater containing sulfamethoxazole (SMX), sulfadiazine (SDZ), tetracycline (TC), and ciprofloxacin (CIP), achieving degradation rates exceeding 80 %. These findings suggest that the DBD/US coupled system holds promising potential for treating organic pollutant wastewater.
本研究探讨了介质阻挡放电(DBD)等离子体与超声波(US)在降解水中有机污染物方面的协同效应。最佳降解条件确定为 100 W 超声波功率、190 V DBD 等离子体电压和中性 pH 值。DBD 等离子体与 US 的结合大大提高了活性物种(-OH、-O2- 和 1O2)的生成,使甲基橙(MO)的降解效率达到 97.3%,比单独使用 DBD 等离子体高出 17.3%。电子自旋共振(ESR)确定了 DBD/US 系统中的 -OH、-O2- 和 1O2,并使用自由基清除剂来阐明它们的作用。降解过程通过 pH 值、电导率、总有机碳和化学需氧量的变化进行评估,并通过紫外可见光和液相色谱-质谱进行表征和分析。通过将 LC-MS 与密度泛函理论(DFT)计算相结合,确定了九种中间产物,并建立了三种以自由基为主的降解途径。此外,DBD/US 系统还处理了含有磺胺甲噁唑(SMX)、磺胺嘧啶(SDZ)、四环素(TC)和环丙沙星(CIP)的废水,降解率超过 80%。这些研究结果表明,DBD/US 耦合系统具有处理有机污染物废水的巨大潜力。
{"title":"Plasma coupled with ultrasonic for degradation of organic pollutants in water: Revealing the generation of free radicals and the dominant degradation pathways","authors":"He Guo,&nbsp;Shuang Yang,&nbsp;Jiaxin Wang,&nbsp;Wenxuan Jiang,&nbsp;Yawen Wang","doi":"10.1016/j.psep.2024.10.095","DOIUrl":"10.1016/j.psep.2024.10.095","url":null,"abstract":"<div><div>This study explores the synergistic effects of dielectric barrier discharge (DBD) plasma coupled with ultrasound (US) in the degradation of organic pollutants in water. The optimal degradation conditions were determined to be 100 W ultrasonic power, 190 V DBD plasma voltage, and neutral pH. The combination of DBD plasma and US significantly enhances the generation of reactive species (·OH, ·O<sub>2</sub><sup>-</sup>, and <sup>1</sup>O<sub>2</sub>), leading to a 97.3 % degradation efficiency of methyl orange (MO), which is 17.3 % higher than DBD plasma alone. Electron spin resonance (ESR) identified ·OH, ·O<sub>2</sub><sup>-</sup>, and <sup>1</sup>O<sub>2</sub> in DBD/US system, and radical scavengers were employed to elucidate their roles. The degradation process was assessed through changes in pH, conductivity, TOC and COD, with characterization and analysis via UV-Vis and LC-MS. By combining LC-MS with density functional theory (DFT) calculations, nine intermediates were identified and three degradation pathways dominated by free radicals were established. Additionally, the DBD/US system treated wastewater containing sulfamethoxazole (SMX), sulfadiazine (SDZ), tetracycline (TC), and ciprofloxacin (CIP), achieving degradation rates exceeding 80 %. These findings suggest that the DBD/US coupled system holds promising potential for treating organic pollutant wastewater.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 793-802"},"PeriodicalIF":6.9,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554912","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hydroconversion of waste polyethylene plastics under mild conditions using mechanically mixed bifunctional catalysts: Impact of metal-acid balance and proximity 使用机械混合双官能催化剂在温和条件下加氢转化废聚乙烯塑料:金属酸平衡和邻近性的影响
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.089
Wenbo Zhang , Leilei Cheng , Weiqiang Zhu , Jing Gu , Shaonan Tian , Haoran Yuan , Yong Chen
The disposal of non-biodegradable waste polyolefin plastics poses a serious environmental threat, highlighting the need for cleaner and more efficient thermochemical recycling technologies. This study introduces a scalable mechanical method to synthesize a metal-acid bifunctional catalyst. The mechanical ball milling process not only exposes more acidic sites but also enhances metal-acid proximity without blocking the pores. By varying the metal-acid balance (MAB) through different mixing ratios, we achieved higher yields and selectivity for soluble products at the optimal MAB level. Under mild conditions (250°C) for 8 h, polyethylene (PE) is efficiently converted into liquid phase iso-paraffins with an isomer selectivity of up to 56 % in the diesel and aviation kerosene fractions (C11-C18). This research underscores the importance of the accessibility of acidic sites to long-chain macromolecules, metal-acid site distance, and their balance in the hydrocracking of PE. It provides valuable theoretical insights and catalytic strategies for converting waste PE plastics into high-value fuel fractions.
不可生物降解的聚烯烃废塑料的处理对环境构成了严重威胁,这凸显了对更清洁、更高效的热化学回收技术的需求。本研究介绍了一种可扩展的机械方法来合成金属-酸双功能催化剂。机械球磨过程不仅能暴露出更多的酸性位点,还能在不堵塞孔隙的情况下提高金属-酸的接近度。通过不同的混合比例改变金属-酸平衡(MAB),我们在最佳的 MAB 水平上获得了更高的产率和可溶性产物的选择性。在温和条件下(250°C)持续 8 小时,聚乙烯(PE)可高效转化为液相异链烷烃,在柴油和航空煤油馏分(C11-C18)中的异构体选择性高达 56%。这项研究强调了酸性位点对长链大分子的可及性、金属-酸性位点距离及其平衡在聚乙烯加氢裂化过程中的重要性。它为将废弃聚乙烯塑料转化为高价值燃料馏分提供了宝贵的理论见解和催化策略。
{"title":"Hydroconversion of waste polyethylene plastics under mild conditions using mechanically mixed bifunctional catalysts: Impact of metal-acid balance and proximity","authors":"Wenbo Zhang ,&nbsp;Leilei Cheng ,&nbsp;Weiqiang Zhu ,&nbsp;Jing Gu ,&nbsp;Shaonan Tian ,&nbsp;Haoran Yuan ,&nbsp;Yong Chen","doi":"10.1016/j.psep.2024.10.089","DOIUrl":"10.1016/j.psep.2024.10.089","url":null,"abstract":"<div><div>The disposal of non-biodegradable waste polyolefin plastics poses a serious environmental threat, highlighting the need for cleaner and more efficient thermochemical recycling technologies. This study introduces a scalable mechanical method to synthesize a metal-acid bifunctional catalyst. The mechanical ball milling process not only exposes more acidic sites but also enhances metal-acid proximity without blocking the pores. By varying the metal-acid balance (MAB) through different mixing ratios, we achieved higher yields and selectivity for soluble products at the optimal MAB level. Under mild conditions (250°C) for 8 h, polyethylene (PE) is efficiently converted into liquid phase iso-paraffins with an isomer selectivity of up to 56 % in the diesel and aviation kerosene fractions (C<sub>11</sub>-C<sub>18</sub>). This research underscores the importance of the accessibility of acidic sites to long-chain macromolecules, metal-acid site distance, and their balance in the hydrocracking of PE. It provides valuable theoretical insights and catalytic strategies for converting waste PE plastics into high-value fuel fractions.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 782-792"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554911","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Study on the migration and adsorption characteristics of barium ions in plastic concrete antifouling barriers 钡离子在塑料混凝土防污屏障中的迁移和吸附特性研究
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.102
Longjin Jiao , Jianguo Chen , Peng Ge , Haoqing Xu , Wenyang Zhang , Nan Zhang , Aizhao Zhou
The urgent need to address barium residue contamination sites is evident. Vertical antifouling barriers effectively prevent the outward spread of pollutants. However, the composition of barrier materials impacts the migration and adsorption behavior of contaminants. To explore the convection-dispersion-adsorption patterns of heavy metal barium in plastic concrete vertical antifouling barriers (comprising GS solidifying material, bentonite, and aggregate) at different mixing ratios, soil column tests and Batch tests were conducted. These tests determined the transport parameters of barium ions under varying bentonite content and water-cement ratios, comparing the retarding factors of barium ions in plastic concrete between the two experiments. The findings suggest that as the water-cement ratio and bentonite content increase, the effective diffusion coefficient and tortuosity factor of chloride ions in the samples also increase. The retarding factors decreases with a higher water-cement ratio but increases with greater bentonite content. Additionally, the retarding factors obtained from the Batch test exceeds that from the soil column test. These research outcomes contribute to optimizing the design of antifouling barriers, enhancing their effectiveness in managing barium residue contamination sites.
解决钡残留物污染场地问题的迫切性显而易见。垂直防污屏障可有效防止污染物向外扩散。然而,屏障材料的成分会影响污染物的迁移和吸附行为。为了探索重金属钡在不同混合比例的塑料混凝土垂直防污屏障(由 GS 固化材料、膨润土和骨料组成)中的对流-分散-吸附模式,我们进行了土柱试验和批量试验。这些试验测定了钡离子在不同膨润土含量和水灰比条件下的迁移参数,并比较了两次试验中钡离子在塑料混凝土中的阻滞因子。研究结果表明,随着水灰比和膨润土含量的增加,样品中氯离子的有效扩散系数和曲折系数也随之增加。水灰比越大,阻滞因子越小,但膨润土含量越高,阻滞因子越大。此外,批量试验获得的阻滞因子超过了土柱试验获得的阻滞因子。这些研究成果有助于优化防污屏障的设计,提高其在管理钡残留物污染场地方面的有效性。
{"title":"Study on the migration and adsorption characteristics of barium ions in plastic concrete antifouling barriers","authors":"Longjin Jiao ,&nbsp;Jianguo Chen ,&nbsp;Peng Ge ,&nbsp;Haoqing Xu ,&nbsp;Wenyang Zhang ,&nbsp;Nan Zhang ,&nbsp;Aizhao Zhou","doi":"10.1016/j.psep.2024.10.102","DOIUrl":"10.1016/j.psep.2024.10.102","url":null,"abstract":"<div><div>The urgent need to address barium residue contamination sites is evident. Vertical antifouling barriers effectively prevent the outward spread of pollutants. However, the composition of barrier materials impacts the migration and adsorption behavior of contaminants. To explore the convection-dispersion-adsorption patterns of heavy metal barium in plastic concrete vertical antifouling barriers (comprising GS solidifying material, bentonite, and aggregate) at different mixing ratios, soil column tests and Batch tests were conducted. These tests determined the transport parameters of barium ions under varying bentonite content and water-cement ratios, comparing the retarding factors of barium ions in plastic concrete between the two experiments. The findings suggest that as the water-cement ratio and bentonite content increase, the effective diffusion coefficient and tortuosity factor of chloride ions in the samples also increase. The retarding factors decreases with a higher water-cement ratio but increases with greater bentonite content. Additionally, the retarding factors obtained from the Batch test exceeds that from the soil column test. These research outcomes contribute to optimizing the design of antifouling barriers, enhancing their effectiveness in managing barium residue contamination sites.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 1085-1093"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Assessment of the polygeneration approach in wastewater treatment plants for enhanced energy efficiency and green hydrogen/ammonia production 评估污水处理厂的多联产方法,以提高能源效率和绿色氢气/氨气生产
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.077
Mohammad Alrbai , Sameer Al-Dahidi , Loiy Al-Ghussain , Bashar Shboul , Hassan Hayajneh , Ali Alahmer
Wastewater treatment plants (WWTPs) offer opportunities to optimize resource utilization and enhance energy efficiency. This study provides a comprehensive analysis of using the polygeneration approach in WWTPs to reduce grid energy dependence, optimize energy distribution, and utilize surplus energy for hydrogen (H2) and ammonia (NH3) production. Several models were employed, including photovoltaic (PV) cells, parabolic trough collectors (PTCs), steam methane reforming, and polymer electrolyte membranes, to assess the feasibility of this approach. Three scenarios were evaluated and compared: Scenario 1 (Baseline) represents the current situation, Scenario 2 maximizes the Net Present Value (NPV), and Scenario 3 minimizes NH3 production costs. Real data from As-Samra WWTP in Jordan was used to accurately assess the feasibility of each scenario. The results show that Scenario 2 offers the highest profitability and efficiency, with a NPV of 87.48 million USD and an annual NH3 production of 15,417 tons, reducing both grid dependency and biogas fuel consumption. Both Scenarios 2 and 3 demonstrate the ability to meet thermal demands efficiently while generating significant revenue from NH3 production. Scenario 3, in particular, achieves competitive H2 and NH3 production costs. Environmentally, Scenario 2 significantly reduces annual greenhouse gas emissions by 12.66 kilotons of CO2eq, with near-zero carbon intensity for thermal energy due to solar reliance. In conclusion, the polygeneration approach offers a promising pathway for WWTPs to achieve greater sustainability, economic gains, and reduced environmental impact, providing valuable insights for decision-makers.
污水处理厂(WWTPs)提供了优化资源利用和提高能源效率的机会。本研究全面分析了在污水处理厂使用多联产方法来减少对电网能源的依赖、优化能源分配以及利用剩余能源生产氢气(H2)和氨气(NH3)的情况。我们采用了多种模型,包括光伏电池、抛物槽式集热器、蒸汽甲烷转化和聚合物电解质膜,以评估这种方法的可行性。对三种方案进行了评估和比较:方案 1(基准)代表当前情况,方案 2 使净现值 (NPV) 最大化,方案 3 使 NH3 生产成本最小化。约旦 As-Samra 污水处理厂的真实数据被用来准确评估每种方案的可行性。结果表明,方案 2 具有最高的盈利能力和效率,净现值为 8748 万美元,年 NH3 产量为 15417 吨,既减少了对电网的依赖,又降低了沼气燃料消耗。方案 2 和方案 3 都证明了在高效满足热需求的同时,还能从 NH3 生产中获得可观收入的能力。尤其是方案 3,其 H2 和 NH3 生产成本均具有竞争力。在环境方面,方案 2 显著减少了每年 12.66 千吨二氧化碳当量的温室气体排放,由于依赖太阳能,热能的碳强度几乎为零。总之,多联产方法为污水处理厂实现更高的可持续性、经济收益和减少对环境的影响提供了一条可行的途径,为决策者提供了宝贵的见解。
{"title":"Assessment of the polygeneration approach in wastewater treatment plants for enhanced energy efficiency and green hydrogen/ammonia production","authors":"Mohammad Alrbai ,&nbsp;Sameer Al-Dahidi ,&nbsp;Loiy Al-Ghussain ,&nbsp;Bashar Shboul ,&nbsp;Hassan Hayajneh ,&nbsp;Ali Alahmer","doi":"10.1016/j.psep.2024.10.077","DOIUrl":"10.1016/j.psep.2024.10.077","url":null,"abstract":"<div><div>Wastewater treatment plants (WWTPs) offer opportunities to optimize resource utilization and enhance energy efficiency. This study provides a comprehensive analysis of using the polygeneration approach in WWTPs to reduce grid energy dependence, optimize energy distribution, and utilize surplus energy for hydrogen (H<sub>2</sub>) and ammonia (NH<sub>3</sub>) production. Several models were employed, including photovoltaic (PV) cells, parabolic trough collectors (PTCs), steam methane reforming, and polymer electrolyte membranes, to assess the feasibility of this approach. Three scenarios were evaluated and compared: Scenario 1 (Baseline) represents the current situation, Scenario 2 maximizes the Net Present Value (NPV), and Scenario 3 minimizes NH<sub>3</sub> production costs. Real data from As-Samra WWTP in Jordan was used to accurately assess the feasibility of each scenario. The results show that Scenario 2 offers the highest profitability and efficiency, with a NPV of 87.48 million USD and an annual NH<sub>3</sub> production of 15,417 tons, reducing both grid dependency and biogas fuel consumption. Both Scenarios 2 and 3 demonstrate the ability to meet thermal demands efficiently while generating significant revenue from NH<sub>3</sub> production. Scenario 3, in particular, achieves competitive H<sub>2</sub> and NH<sub>3</sub> production costs. Environmentally, Scenario 2 significantly reduces annual greenhouse gas emissions by 12.66 kilotons of CO<sub>2eq</sub>, with near-zero carbon intensity for thermal energy due to solar reliance. In conclusion, the polygeneration approach offers a promising pathway for WWTPs to achieve greater sustainability, economic gains, and reduced environmental impact, providing valuable insights for decision-makers.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 803-821"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanism of microwave-assisted coal desulfurization with urea peroxide 过氧化脲微波辅助煤炭脱硫的机理
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.086
Hai Yang , Jin Liu , Bo Zhang , Tao Cheng , Debing Zou , Xing Lv
To effectively remove organic sulfur from coal for higher resource efficiency, an innovative microwave-assisted urea peroxide for desulfurization system was designed. The experimental group with different microwave frequencies and the conventional pyrolysis control group were set up to prove the desulfurization effect of microwave in coordination with urea peroxide. The experimental results showed that under 1000 W microwave irradiation and the promotion of urea peroxide, the desulfurization efficiency can reach 67.29 %, with an increase of 38.32 % while the conventional pyrolysis is only 28.97 %. According to the Fourier transform infrared (FTIR) analysis, the effectiveness of microwave coordination with urea peroxide for desulfurization is explained from macroscopic point of view. Benzylidene thiol, dibenzyl sulfide, and dibenzyl disulfide were selected as model compounds for the quantum chemical calculation. The simulation results demonstrated that the changes in the pathway energy barriers for desulfurization align with the experimental material transformations, confirming the accuracy of the simulation. The sulfur-containing bonds of mercaptans will be destroyed to form hydrogen sulfide, and the undestroyed bonds will remain in the organic matter. After being oxidized, the sulfur-containing bond will break to form a water-soluble sulfonic acid free radical. The unoxidized sulfur bonds of thioethers will be destroyed to generate unstable phenyl free radicals and free sulfur radicals. To achieve stability, phenyl free radicals can pair to form diphenylethane or combine with other radicals (such as •H). In contrast, sulfur free radicals can only react with hydrogen radicals to form hydrogen sulfide. However, the limited availability of hydrogen radicals in the system restricts the desulfurization efficiency. After oxidation by urea peroxide, the thioethers will form sulfones. The sulfur-containing bonds will be fractured and directly generate phenyl and sulfur dioxide, which reduces the dependence on hydrogen free radicals. The three-dimensional desulfurization path of microwave collaboration with urea peroxide experiment was simulated and converted to the analytical bond breaking and formation mechanism. This study proved that microwave synergizes with urea peroxide can intensify the desulfurization process. It provides a high-efficiency method for the clean and green utilization of coal, which is conducive to supporting environmentally sustainable development.
为有效去除煤炭中的有机硫,提高资源利用效率,设计了一种创新的微波辅助过氧化脲脱硫系统。为了证明微波与过氧化脲协同作用的脱硫效果,实验组设置了不同微波频率的实验组和常规热解对照组。实验结果表明,在 1000 W 微波辐照和过氧化脲的促进下,脱硫效率可达 67.29 %,比常规热解提高了 38.32 %,而常规热解仅为 28.97 %。根据傅立叶变换红外(FTIR)分析,微波与过氧化脲配位的脱硫效果从宏观角度得到了解释。量子化学计算选择了亚苄基硫醇、二苄基硫醚和二苄基二硫醚作为模型化合物。模拟结果表明,脱硫路径能垒的变化与实验材料的转化一致,证实了模拟的准确性。硫醇的含硫键会被破坏形成硫化氢,未被破坏的键会留在有机物中。被氧化后,含硫键会断裂,形成水溶性磺酸自由基。硫醚中未氧化的硫键会被破坏,生成不稳定的苯基自由基和游离硫自由基。为了达到稳定性,苯基自由基可以配对形成二苯基乙烷或与其他自由基(如-H)结合。相反,硫自由基只能与氢自由基反应生成硫化氢。然而,系统中氢自由基的有限性限制了脱硫效率。过氧化脲氧化后,硫醚会形成砜。含硫键断裂后会直接生成苯基和二氧化硫,从而减少了对氢自由基的依赖。模拟了微波协同过氧化脲实验的三维脱硫路径,并将其转换为分析键的断裂和形成机理。该研究证明,微波与过氧化脲协同作用可强化脱硫过程。它为煤的清洁绿色利用提供了一种高效方法,有利于支持环境可持续发展。
{"title":"Mechanism of microwave-assisted coal desulfurization with urea peroxide","authors":"Hai Yang ,&nbsp;Jin Liu ,&nbsp;Bo Zhang ,&nbsp;Tao Cheng ,&nbsp;Debing Zou ,&nbsp;Xing Lv","doi":"10.1016/j.psep.2024.10.086","DOIUrl":"10.1016/j.psep.2024.10.086","url":null,"abstract":"<div><div>To effectively remove organic sulfur from coal for higher resource efficiency, an innovative microwave-assisted urea peroxide for desulfurization system was designed. The experimental group with different microwave frequencies and the conventional pyrolysis control group were set up to prove the desulfurization effect of microwave in coordination with urea peroxide. The experimental results showed that under 1000 W microwave irradiation and the promotion of urea peroxide, the desulfurization efficiency can reach 67.29 %, with an increase of 38.32 % while the conventional pyrolysis is only 28.97 %. According to the Fourier transform infrared (FTIR) analysis, the effectiveness of microwave coordination with urea peroxide for desulfurization is explained from macroscopic point of view. Benzylidene thiol, dibenzyl sulfide, and dibenzyl disulfide were selected as model compounds for the quantum chemical calculation. The simulation results demonstrated that the changes in the pathway energy barriers for desulfurization align with the experimental material transformations, confirming the accuracy of the simulation. The sulfur-containing bonds of mercaptans will be destroyed to form hydrogen sulfide, and the undestroyed bonds will remain in the organic matter. After being oxidized, the sulfur-containing bond will break to form a water-soluble sulfonic acid free radical. The unoxidized sulfur bonds of thioethers will be destroyed to generate unstable phenyl free radicals and free sulfur radicals. To achieve stability, phenyl free radicals can pair to form diphenylethane or combine with other radicals (such as •H). In contrast, sulfur free radicals can only react with hydrogen radicals to form hydrogen sulfide. However, the limited availability of hydrogen radicals in the system restricts the desulfurization efficiency. After oxidation by urea peroxide, the thioethers will form sulfones. The sulfur-containing bonds will be fractured and directly generate phenyl and sulfur dioxide, which reduces the dependence on hydrogen free radicals. The three-dimensional desulfurization path of microwave collaboration with urea peroxide experiment was simulated and converted to the analytical bond breaking and formation mechanism. This study proved that microwave synergizes with urea peroxide can intensify the desulfurization process. It provides a high-efficiency method for the clean and green utilization of coal, which is conducive to supporting environmentally sustainable development.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 1127-1137"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587407","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Insights into the relationship between Nitrilotri(methylphosphonic acid) (NTMP) adsorption and physicochemical properties of iron oxides 硝基三(甲基膦酸)(NTMP)吸附与铁氧化物理化性质之间关系的启示
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.103
Jun Wan , Runnian Gao , Xiaonan Feng
Non-reactive phosphorus (e.g., phosphonate) contributes to eutrophication, while little attention has been paid to its control. The iron-based materials are highly efficient in orthophosphate removal from water, while the correlation between their physicochemical properties and selective phosphonate (e.g. Nitrilotri(methylphosphonic acid) (NTMP)) adsorption is still unclear. In this study, Fe3O4 (magnetite), FeOOH (goethite) and Fe2O3 (hematite) with different crystal structures, particle sizes and surface area were synthesized for NTMP adsorption. The physicochemical properties of the three kinds of iron oxides were characterized. The batch experiments were applied to explore the NTMP adsorption and desorption performance. The maximum adsorption capacity of NTMP on Fe3O4, FeOOH and Fe2O3 were 4.14, 1.91 and 0.99 mg-P/g, respectively. Results implied the crystal structure and surface area of iron oxides determined the maximum NTMP adsorption capacity. The NTMP adsorption on the three iron oxides was spontaneous, endothermic and randomness increase. The iron oxides showed high selectivity towards NTMP adsorption in water containing anions, while the co-existing Ca2+ and Mg2+ remarkably increased the adsorption capacity. The successive adsorption-desorption cycles suggested a favorable reusability of the above iron oxides and a high NTMP desorption efficiency. The specific NTMP adsorption capacity followed the sequence of FeOOH > Fe2O3 > Fe3O4, and was highly dependent on surface OH proportion. The NTMP adsorption mechanism was mainly attributed to inner-sphere complexation. This study provides insights into the iron-based adsorbents design for selective phosphonate adsorption in the future.
非反应性磷(如膦酸盐)会导致水体富营养化,但对其控制却关注甚少。铁基材料能高效去除水中的正磷酸盐,但其理化性质与选择性膦酸盐(如氮基三(甲基膦酸)(NTMP))吸附之间的相关性仍不清楚。本研究合成了具有不同晶体结构、粒度和表面积的 Fe3O4(磁铁矿)、FeOOH(鹅铁矿)和 Fe2O3(赤铁矿),用于吸附 NTMP。对三种铁氧化物的物理化学性质进行了表征。采用批量实验探讨了 NTMP 的吸附和解吸性能。NTMP在Fe3O4、FeOOH和Fe2O3上的最大吸附容量分别为4.14、1.91和0.99 mg-P/g。结果表明,铁氧化物的晶体结构和表面积决定了 NTMP 的最大吸附容量。NTMP 在三种铁氧化物上的吸附是自发的、内热的和随机增加的。铁氧化物在含有阴离子的水中对 NTMP 的吸附具有很高的选择性,而同时存在的 Ca2+ 和 Mg2+ 则显著提高了吸附容量。连续的吸附-解吸循环表明,上述氧化铁具有良好的重复利用性和较高的 NTMP 解吸效率。特定的 NTMP 吸附能力遵循 FeOOH > Fe2O3 > Fe3O4 的顺序,并与表面 OH- 的比例高度相关。NTMP的吸附机理主要归因于内球络合。该研究为今后选择性吸附膦酸盐的铁基吸附剂设计提供了启示。
{"title":"Insights into the relationship between Nitrilotri(methylphosphonic acid) (NTMP) adsorption and physicochemical properties of iron oxides","authors":"Jun Wan ,&nbsp;Runnian Gao ,&nbsp;Xiaonan Feng","doi":"10.1016/j.psep.2024.10.103","DOIUrl":"10.1016/j.psep.2024.10.103","url":null,"abstract":"<div><div>Non-reactive phosphorus (e.g., phosphonate) contributes to eutrophication, while little attention has been paid to its control. The iron-based materials are highly efficient in orthophosphate removal from water, while the correlation between their physicochemical properties and selective phosphonate (e.g. Nitrilotri(methylphosphonic acid) (NTMP)) adsorption is still unclear. In this study, Fe<sub>3</sub>O<sub>4</sub> (magnetite), FeOOH (goethite) and Fe<sub>2</sub>O<sub>3</sub> (hematite) with different crystal structures, particle sizes and surface area were synthesized for NTMP adsorption. The physicochemical properties of the three kinds of iron oxides were characterized. The batch experiments were applied to explore the NTMP adsorption and desorption performance. The maximum adsorption capacity of NTMP on Fe<sub>3</sub>O<sub>4</sub>, FeOOH and Fe<sub>2</sub>O<sub>3</sub> were 4.14, 1.91 and 0.99 mg-P/g, respectively. Results implied the crystal structure and surface area of iron oxides determined the maximum NTMP adsorption capacity. The NTMP adsorption on the three iron oxides was spontaneous, endothermic and randomness increase. The iron oxides showed high selectivity towards NTMP adsorption in water containing anions, while the co-existing Ca<sup>2+</sup> and Mg<sup>2+</sup> remarkably increased the adsorption capacity. The successive adsorption-desorption cycles suggested a favorable reusability of the above iron oxides and a high NTMP desorption efficiency. The specific NTMP adsorption capacity followed the sequence of FeOOH &gt; Fe<sub>2</sub>O<sub>3</sub> &gt; Fe<sub>3</sub>O<sub>4</sub>, and was highly dependent on surface OH<sup>−</sup> proportion. The NTMP adsorption mechanism was mainly attributed to inner-sphere complexation. This study provides insights into the iron-based adsorbents design for selective phosphonate adsorption in the future.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 750-759"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554903","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Data-driven Bayesian risk assessment of factors influencing the severity of marine accidents in port areas 对影响港区海上事故严重性的因素进行数据驱动的贝叶斯风险评估
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-26 DOI: 10.1016/j.psep.2024.10.074
Mehmet Kaptan, Ozan Bayazit
The most prevalent types of ship accidents in port areas are allisions, collisions, and groundings. A comprehensive risk assessment is needed to prevent and mitigate these accidents and their consequences. This study evaluates the risk of such accidents in port areas by presenting a model that elucidates the relationship between risk-identifying factors (RIFs) and accident severity. In this context, the RIFs are determined by analyszing the reports of 528 accidents that occurred in port areas between 1995 and 2023. Subsequently, the model is created by analysing the data derived from these reports using the Tree Augmented Naive Bayes (TAN) algorithm, which is an approach of the data-driven Bayesian network method. The findings of the study indicate that accident type, wind, ship age, and vessel type are the most influential factors in predicting the severity of accidents in port areas. It is thought that the model will assist port authorities in identifying operational risks contributing to accidents and in formulating preventive regulations.
港区最常见的船舶事故类型是碰撞、相撞和搁浅。为了预防和减轻这些事故及其后果,需要进行全面的风险评估。本研究通过提出一个模型,阐明风险识别因素(RIFs)与事故严重性之间的关系,对港区此类事故的风险进行评估。在此背景下,通过分析 1995 年至 2023 年期间在港口地区发生的 528 起事故的报告,确定了风险识别因素。随后,利用数据驱动贝叶斯网络方法中的树状增强奈维贝叶斯(TAN)算法分析这些报告中的数据,创建模型。研究结果表明,事故类型、风力、船龄和船舶类型是预测港区事故严重程度的最有影响力的因素。据认为,该模型将有助于港口当局识别导致事故的操作风险,并制定预防性法规。
{"title":"Data-driven Bayesian risk assessment of factors influencing the severity of marine accidents in port areas","authors":"Mehmet Kaptan,&nbsp;Ozan Bayazit","doi":"10.1016/j.psep.2024.10.074","DOIUrl":"10.1016/j.psep.2024.10.074","url":null,"abstract":"<div><div>The most prevalent types of ship accidents in port areas are allisions, collisions, and groundings. A comprehensive risk assessment is needed to prevent and mitigate these accidents and their consequences. This study evaluates the risk of such accidents in port areas by presenting a model that elucidates the relationship between risk-identifying factors (RIFs) and accident severity. In this context, the RIFs are determined by analyszing the reports of 528 accidents that occurred in port areas between 1995 and 2023. Subsequently, the model is created by analysing the data derived from these reports using the Tree Augmented Naive Bayes (TAN) algorithm, which is an approach of the data-driven Bayesian network method. The findings of the study indicate that accident type, wind, ship age, and vessel type are the most influential factors in predicting the severity of accidents in port areas. It is thought that the model will assist port authorities in identifying operational risks contributing to accidents and in formulating preventive regulations.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 1094-1109"},"PeriodicalIF":6.9,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142587458","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electronic synergy between NiCo2O4 and adjacent carbon defects to enhance styrene cracking activity for styrene-saturated activated carbon regeneration 镍钴氧化物与相邻碳缺陷之间的电子协同作用可提高苯乙烯饱和活性炭再生中的苯乙烯裂解活性
IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-10-24 DOI: 10.1016/j.psep.2024.10.063
Zixiang Gao , Guoqiang Li , Jun Liu , Guojie Zhang , Yuqiong Zhao , Ying Wang
The design and construction of catalysts featuring abundant electron transfer and defect structures for the regeneration of styrene-saturated activated carbon (AC) pose a significant challenge. This paper presents successful preparation of a regenerated adsorbent with synergistic catalytic active sites of NiCo2O4 spinel and carbon defects using a simple impregnation method. Enhanced catalytic activity is attributed to the electronic synergy between NiCo2O4 and carbon defects in 2.5Ni-2.5Co-900, involving substantial electron transfers, abundant acidic sites, and strong reducibility. Reactive oxygen species and the robust oxygen transfer facilitate the deep oxidation of intermediates and carbon elimination. The optimized regenerated adsorbent achieved a styrene adsorption capacity of 446.4 mg/g with a recovery of 92.4 % of the fresh sample, which is 1.5 times higher than 5Ni-900 and about 1.8 times higher than the unmodified regenerated activated carbon sample, RAC-900. The mechanism of styrene cracking and the evolution of intermediates were investigated using thermogravimetric-infrared coupling, and the effects of catalytic temperature and active sites on styrene cracking, deep oxidation of intermediates, and elimination of carbon deposits were explored. Kinetic analysis demonstrated that the adsorption of styrene on regenerated samples entailed a multifaceted process integrating both physical and chemical adsorption. The significance of chemical adsorption became increasingly evident as the concentration of defective sites grew. Intra-pore diffusion is the main determining step of the adsorption process. After five cycles, the adsorption capacity of 2.5Ni-2.5Co-900 decreased to below 25 %, suggesting promising strategies to overcome challenges of regenerating styrene-saturated AC.
设计和构建具有丰富电子传递和缺陷结构的催化剂,用于苯乙烯饱和活性炭(AC)的再生,是一项重大挑战。本文采用简单的浸渍法成功制备了一种再生吸附剂,该吸附剂具有 NiCo2O4 尖晶石和碳缺陷的协同催化活性位点。催化活性的增强归因于 2.5Ni-2.5Co-900 中 NiCo2O4 与碳缺陷之间的电子协同作用,包括大量的电子转移、丰富的酸性位点和强还原性。活性氧物种和强大的氧传递促进了中间产物的深度氧化和碳消除。优化后的再生吸附剂对苯乙烯的吸附量达到 446.4 mg/g,对新鲜样品的回收率为 92.4%,是 5Ni-900 的 1.5 倍,是未改性再生活性炭样品 RAC-900 的约 1.8 倍。利用热重-红外耦合技术研究了苯乙烯裂解和中间产物演化的机理,并探讨了催化温度和活性位点对苯乙烯裂解、中间产物深度氧化和碳沉积消除的影响。动力学分析表明,再生样品对苯乙烯的吸附是一个集物理吸附和化学吸附于一体的多元过程。随着缺陷点浓度的增加,化学吸附的重要性日益明显。孔内扩散是吸附过程的主要决定步骤。经过五个循环后,2.5Ni-2.5Co-900 的吸附容量降至 25% 以下,这为克服再生苯乙烯饱和交流电的挑战提供了可行的策略。
{"title":"Electronic synergy between NiCo2O4 and adjacent carbon defects to enhance styrene cracking activity for styrene-saturated activated carbon regeneration","authors":"Zixiang Gao ,&nbsp;Guoqiang Li ,&nbsp;Jun Liu ,&nbsp;Guojie Zhang ,&nbsp;Yuqiong Zhao ,&nbsp;Ying Wang","doi":"10.1016/j.psep.2024.10.063","DOIUrl":"10.1016/j.psep.2024.10.063","url":null,"abstract":"<div><div>The design and construction of catalysts featuring abundant electron transfer and defect structures for the regeneration of styrene-saturated activated carbon (AC) pose a significant challenge. This paper presents successful preparation of a regenerated adsorbent with synergistic catalytic active sites of NiCo<sub>2</sub>O<sub>4</sub> spinel and carbon defects using a simple impregnation method. Enhanced catalytic activity is attributed to the electronic synergy between NiCo<sub>2</sub>O<sub>4</sub> and carbon defects in 2.5Ni-2.5Co-900, involving substantial electron transfers, abundant acidic sites, and strong reducibility. Reactive oxygen species and the robust oxygen transfer facilitate the deep oxidation of intermediates and carbon elimination. The optimized regenerated adsorbent achieved a styrene adsorption capacity of 446.4 mg/g with a recovery of 92.4 % of the fresh sample, which is 1.5 times higher than 5Ni-900 and about 1.8 times higher than the unmodified regenerated activated carbon sample, RAC-900. The mechanism of styrene cracking and the evolution of intermediates were investigated using thermogravimetric-infrared coupling, and the effects of catalytic temperature and active sites on styrene cracking, deep oxidation of intermediates, and elimination of carbon deposits were explored. Kinetic analysis demonstrated that the adsorption of styrene on regenerated samples entailed a multifaceted process integrating both physical and chemical adsorption. The significance of chemical adsorption became increasingly evident as the concentration of defective sites grew. Intra-pore diffusion is the main determining step of the adsorption process. After five cycles, the adsorption capacity of 2.5Ni-2.5Co-900 decreased to below 25 %, suggesting promising strategies to overcome challenges of regenerating styrene-saturated AC.</div></div>","PeriodicalId":20743,"journal":{"name":"Process Safety and Environmental Protection","volume":"192 ","pages":"Pages 719-737"},"PeriodicalIF":6.9,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142535088","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Process Safety and Environmental Protection
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1