Pub Date : 2024-11-15DOI: 10.1016/j.seppur.2024.130544
Rui Ding, Jingjing Liu, Qingguo Meng, Teng Wang, Xiaomei Zhang
Due to the strong carcinogenicity, non-degradability and bioaccumulation of Cr (VI), exploring ingenious strategies and renewable materials to simultaneously detect and remove Cr (VI) from industrial wastewater, to reduce its damage to ecosystems, is of great importance. Covalent organic frameworks are considered as excellent adsorbents, but most of them are neutral and rigid materials. Herein, a cationic and flexible COF (Imi-TPP-COF-Br-AR) was fabricated for the first time by integrating porphyrin and charged imidazole into a framework, followed by reduction. Such elaborate design endowed Imi-TPP-COF-Br-AR with excellent light-driven oxidase-like activity, dense ion sites, and stable photoelectric properties. Imi-TPP-COF-Br-AR could purify Cr (VI) polluted water to drinking levels with outstanding adsorption performance (Qmax = 373.14 mg/g), also exhibited broader detection range (0.5–220 μM) and lower limit of detection (LOD, 41 nM) for Cr (VI). Mechanism studies and density functional theory (DFT) calculations disclosed that the electrostatic interaction between cationic material and the negatively charged Cr (VI) anions, and the extended π-conjugated structure cooperatively promoted the remarkable performance of Imi-TPP-COF-Br-AR for Cr (VI). This work provides a novel strategy for the structural and functional design of cationic and flexible COFs materials, especially those can realize dual functions only within one material.
{"title":"Dual-functional flexible cationic porphyrin-based covalent organic frameworks for selective adsorption and sensitive detection of Cr (VI)","authors":"Rui Ding, Jingjing Liu, Qingguo Meng, Teng Wang, Xiaomei Zhang","doi":"10.1016/j.seppur.2024.130544","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130544","url":null,"abstract":"Due to the strong carcinogenicity, non-degradability and bioaccumulation of Cr (VI), exploring ingenious strategies and renewable materials to simultaneously detect and remove Cr (VI) from industrial wastewater, to reduce its damage to ecosystems, is of great importance. Covalent organic frameworks are considered as excellent adsorbents, but most of them are neutral and rigid materials. Herein, a cationic and flexible COF (Imi-TPP-COF-Br-AR) was fabricated for the first time by integrating porphyrin and charged imidazole into a framework, followed by reduction. Such elaborate design endowed Imi-TPP-COF-Br-AR with excellent light-driven oxidase-like activity, dense ion sites, and stable photoelectric properties. Imi-TPP-COF-Br-AR could purify Cr (VI) polluted water to drinking levels with outstanding adsorption performance (Q<sub>max</sub> = 373.14 mg/g), also exhibited broader detection range (0.5–220 μM) and lower limit of detection (LOD, 41 nM) for Cr (VI). Mechanism studies and density functional theory (DFT) calculations disclosed that the electrostatic interaction between cationic material and the negatively charged Cr (VI) anions, and the extended π-conjugated structure cooperatively promoted the remarkable performance of Imi-TPP-COF-Br-AR for Cr (VI). This work provides a novel strategy for the structural and functional design of cationic and flexible COFs materials, especially those can realize dual functions only within one material.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637894","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-15DOI: 10.1016/j.seppur.2024.130541
Shishun Wang , Shuang Gai , Kui Cheng , Zhuqing Liu , Markus Antonietti , Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO4•-, and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
{"title":"Artificial humic acid mediated Fe(II) regeneration to restart Fe(III)/PMS for the degradation of atrazine","authors":"Shishun Wang , Shuang Gai , Kui Cheng , Zhuqing Liu , Markus Antonietti , Fan Yang","doi":"10.1016/j.seppur.2024.130541","DOIUrl":"10.1016/j.seppur.2024.130541","url":null,"abstract":"<div><div>The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO<sub>4</sub><sup>•-</sup>, and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"359 ","pages":"Article 130541"},"PeriodicalIF":8.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-15DOI: 10.1016/j.seppur.2024.130554
Jingwei Cai , Bingzhi Yi , Jian Liu , Jiahui Li , Yangjiadi Han , Ziwen Deng , Xiangjun Hu , Mingyang Chen , Junbo Gong
Large amounts of Mo, Co and Al are contained in spent hydrodesulfurization (HDS) catalysts, and recovering these valuable metals from spent catalysts achieves sustainable utilization of resources and promotes environmental protection. However, the leaching efficiency of valuable metal often experiences a sharp decline during scale-up. In this study, leaching experiments and fluid dynamics were used to jointly investigate the major factors and regulation mechanisms affecting leaching efficiency during the scale-up process. Optimization of flow field conditions is guided by Computational Fluid Dynamics (CFD) simulation. including different paddle types, agitation speed and particle size. After controlling flow field assisted with CFD simulation, about 20% of the sulfuric acid solution was saved and 99.7% of Mo, 98.2% of Co and 83.7% of Al were successfully recovered. Additionally, the leaching mechanisms of these metals in H2SO4 were systematically studied. The findings indicated that the leaching kinetics of Co, Mo and Al are governed by diffusion-controlled model, consistent with the shrinking core model. Correlation coefficients and activation energy analyses further demonstrated that the leaching process is diffusion-controlled, highlighting the importance of flow field mixing in scaling up the acid-mediated recovery of Mo, Co and Al from spent HDS catalysts. The fluid dynamic and leaching mechanism study provides valuable insights for large-scale recovery of valuable metals.
{"title":"Enhancing Co, Mo and Al leaching from spent HDS catalysts during scale-up process based on fluid dynamic and leaching mechanism","authors":"Jingwei Cai , Bingzhi Yi , Jian Liu , Jiahui Li , Yangjiadi Han , Ziwen Deng , Xiangjun Hu , Mingyang Chen , Junbo Gong","doi":"10.1016/j.seppur.2024.130554","DOIUrl":"10.1016/j.seppur.2024.130554","url":null,"abstract":"<div><div>Large amounts of Mo, Co and Al are contained in spent hydrodesulfurization (HDS) catalysts, and recovering these valuable metals from spent catalysts achieves sustainable utilization of resources and promotes environmental protection. However, the leaching efficiency of valuable metal often experiences a sharp decline during scale-up. In this study, leaching experiments and fluid dynamics were used to jointly investigate the major factors and regulation mechanisms affecting leaching efficiency during the scale-up process. Optimization of flow field conditions is guided by Computational Fluid Dynamics (CFD) simulation. including different paddle types, agitation speed and particle size. After controlling flow field assisted with CFD simulation, about 20% of the sulfuric acid solution was saved and 99.7% of Mo, 98.2% of Co and 83.7% of Al were successfully recovered. Additionally, the leaching mechanisms of these metals in H<sub>2</sub>SO<sub>4</sub> were systematically studied. The findings indicated that the leaching kinetics of Co, Mo and Al are governed by diffusion-controlled model, consistent with the shrinking core model. Correlation coefficients and activation energy analyses further demonstrated that the leaching process is diffusion-controlled, highlighting the importance of flow field mixing in scaling up the acid-mediated recovery of Mo, Co and Al from spent HDS catalysts. The fluid dynamic and leaching mechanism study provides valuable insights for large-scale recovery of valuable metals.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"359 ","pages":"Article 130554"},"PeriodicalIF":8.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The selective catalytic oxidation of ammonia (NH3-SCO) over Pt-based catalysts is a promising method for reducing NH3 into N2 and H2O. Iron oxide, a typical and cheap redox carrier, can potentially affect the electronic or geometric structure of Pt sites. What’s more, the properties of Pt sites could be easily modulated through in-situ gas modulation. In this study, the Pt-supported Fe3O4 catalyst (PtFe) was subjected to modulation by reaction gases (21 % O2 or 0.4 % NH3) at varying temperatures (250 °C and 500 °C). Among all samples, the PtFe reduced at 250 °C (PtFe-N250) displayed the most favourable NH3-SCO performance, with 93.3 % NH3 oxidation and 65 % N2 selectivity achieved at 225 °C. The mechanism of the NH3-SCO over PtFe-N250 was investigated through a series of ex-situ characterizations and in-situ DRIFTS. The favourable NH3 oxidation performance observed over PtFe-N250 below 250 °C could be attributed to the high concentration of Pt0 species and high content of strong acid sites. The in-situ DRIFTS indicated that the NH3-SCO over PtFe-N250 followed the internal selective catalytic reduction (i-SCR). This study offered a novel strategy for enhancing the NH3-SCO performance of PtFe using in-situ gas-modulating approachs.
{"title":"In-situ gas-modulating electron structure of Pt to boost NH3-SCO reactions over Pt/Fe3O4","authors":"Bo Wu, Yijia Wu, Jinglei Li, Xinyu Zheng, Limin Hu, Baiqiang Zhang","doi":"10.1016/j.seppur.2024.130514","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130514","url":null,"abstract":"The selective catalytic oxidation of ammonia (NH<sub>3</sub>-SCO) over Pt-based catalysts is a promising method for reducing NH<sub>3</sub> into N<sub>2</sub> and H<sub>2</sub>O. Iron oxide, a typical and cheap redox carrier, can potentially affect the electronic or geometric structure of Pt sites. What’s more, the properties of Pt sites could be easily modulated through <em>in-situ</em> gas modulation. In this study, the Pt-supported Fe<sub>3</sub>O<sub>4</sub> catalyst (PtFe) was subjected to modulation by reaction gases (21 % O<sub>2</sub> or 0.4 % NH<sub>3</sub>) at varying temperatures (250 °C and 500 °C). Among all samples, the PtFe reduced at 250 °C (PtFe-N250) displayed the most favourable NH<sub>3</sub>-SCO performance, with 93.3 % NH<sub>3</sub> oxidation and 65 % N<sub>2</sub> selectivity achieved at 225 °C. The mechanism of the NH<sub>3</sub>-SCO over PtFe-N250 was investigated through a series of <em>ex-situ</em> characterizations and <em>in-situ</em> DRIFTS. The favourable NH<sub>3</sub> oxidation performance observed over PtFe-N250 below 250 °C could be attributed to the high concentration of Pt<sup>0</sup> species and high content of strong acid sites. The <em>in-situ</em> DRIFTS indicated that the NH<sub>3</sub>-SCO over PtFe-N250 followed the internal selective catalytic reduction (<em>i</em>-SCR). This study offered a novel strategy for enhancing the NH<sub>3</sub>-SCO performance of PtFe using <em>in-situ</em> gas-modulating approachs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"75 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637522","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-15DOI: 10.1016/j.seppur.2024.130559
Yue Zhang, Rui Han, Shujun Zhou, Xijun Wang, Jun Zhao, Yikun Zhang, Lili Wang, Xiaoyan Sun, Li Xia, Shuguang Xiang
Deep eutectic solvents (DESs) have shown great potential in capturing carbon dioxide (CO2) and are expected to help alleviate the pressing issue of global warming. This study utilizes experimental approaches and molecular dynamics(MD) simulation to research the process of CO2 capture with amine-based DESs. The DESs, composed of methyltriphenylphosphonium bromide (MTPPB) and methyldiethanolamine (MDEA) as the hydrogen bond acceptor (HBA) and donor (HBD), respectively, were evaluated for their physical properties and CO2 absorption capacity. Additionally, the impact of different water contents and temperatures on CO2 absorption was investigated. Results demonstrated that HBD quantity negatively correlates with viscosity while positively correlating with CO2 solubility. The water content of the DESs ranged from 10 wt% to 50 wt%, leading to a progressive reduction in viscosity, while the CO2 absorption capacity initially decreased and then increased. The DES with a molar ratio of 1:16 had the lowest viscosity of 10.5 mPa.s and the greatest CO2 absorption of 0.1004 g CO2/g DES at 50 wt% water content and 303.15 K, causing significant savings in solvent costs. MD simulations were utilized to explore the microscopic interactions among HBA, HBD, CO2, and water, revealing that the addition of 50 wt% water does not affect the structure of the DES. The experimental and computational studies presented in this study illustrate that the introduction of a specific quantity of water to DESs and selecting suitable temperatures can enhance CO2 capture efficiency, providing theoretical support for industrial application of CO2 capture.
深共晶溶剂（DES）在捕获二氧化碳（CO2）方面显示出巨大潜力，有望帮助缓解全球变暖这一紧迫问题。本研究利用实验方法和分子动力学（MD）模拟研究了胺基 DESs 的二氧化碳捕集过程。研究评估了分别以甲基三苯基溴化磷（MTPPB）和甲基二乙醇胺（MDEA）作为氢键受体（HBA）和供体（HBD）的DES的物理性质和二氧化碳吸收能力。此外，还研究了不同含水量和温度对二氧化碳吸收的影响。结果表明，HBD 数量与粘度呈负相关，而与二氧化碳溶解度呈正相关。DES 的含水量从 10 wt% 到 50 wt%，导致粘度逐渐降低，而二氧化碳吸收能力则先降低后升高。摩尔比为 1:16 的 DES 粘度最低，为 10.5 mPa.s，在含水量为 50 wt%、温度为 303.15 K 的条件下，二氧化碳吸收量最大，为 0.1004 g CO2/g DES，从而大大节省了溶剂成本。利用 MD 模拟探索了 HBA、HBD、CO2 和水之间的微观相互作用，结果表明添加 50 wt% 的水不会影响 DES 的结构。本研究中的实验和计算研究表明，在 DES 中引入特定数量的水并选择合适的温度可以提高二氧化碳捕获效率，为二氧化碳捕获的工业应用提供了理论支持。
{"title":"Amine-based deep eutectic solvents for CO2 capture: Experiments and molecular thermodynamics","authors":"Yue Zhang, Rui Han, Shujun Zhou, Xijun Wang, Jun Zhao, Yikun Zhang, Lili Wang, Xiaoyan Sun, Li Xia, Shuguang Xiang","doi":"10.1016/j.seppur.2024.130559","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130559","url":null,"abstract":"Deep eutectic solvents (DESs) have shown great potential in capturing carbon dioxide (CO<sub>2</sub>) and are expected to help alleviate the pressing issue of global warming. This study utilizes experimental approaches and molecular dynamics(MD) simulation to research the process of CO<sub>2</sub> capture with amine-based DESs. The DESs, composed of methyltriphenylphosphonium bromide (MTPPB) and methyldiethanolamine (MDEA) as the hydrogen bond acceptor (HBA) and donor (HBD), respectively, were evaluated for their physical properties and CO<sub>2</sub> absorption capacity. Additionally, the impact of different water contents and temperatures on CO<sub>2</sub> absorption was investigated. Results demonstrated that HBD quantity negatively correlates with viscosity while positively correlating with CO<sub>2</sub> solubility. The water content of the DESs ranged from 10 wt% to 50 wt%, leading to a progressive reduction in viscosity, while the CO<sub>2</sub> absorption capacity initially decreased and then increased. The DES with a molar ratio of 1:16 had the lowest viscosity of 10.5 mPa.s and the greatest CO<sub>2</sub> absorption of 0.1004 g CO<sub>2</sub>/g DES at 50 wt% water content and 303.15 K, causing significant savings in solvent costs. MD simulations were utilized to explore the microscopic interactions among HBA, HBD, CO<sub>2</sub>, and water, revealing that the addition of 50 wt% water does not affect the structure of the DES. The experimental and computational studies presented in this study illustrate that the introduction of a specific quantity of water to DESs and selecting suitable temperatures can enhance CO<sub>2</sub> capture efficiency, providing theoretical support for industrial application of CO<sub>2</sub> capture.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"70 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The optimal conditions for extracting turmeric essential oil (CEO) using ionic liquid ultrasound-assisted hydrodistillation (IL-U-HD) were determined in this study. In this context, the CEO extraction yield reached 6.88 %, significantly higher than that of hydrodistillation (HD), ultrasound-assisted hydrodistillation (U-HD), and ionic liquid-assisted hydrodistillation (IL-HD). The extraction kinetics, GC–MS compositional analysis, cell viability, and antioxidant properties of the extracted CEO indicate enhanced cell viability and antioxidant properties when extracted by IL-U-HD. Additionally, the compositional fractions exhibited an increase while improving extraction efficiency by 22 % compared to HD. To explore the efficient extraction mechanism at the molecular level, cellobiose and ar-turmerone were established as model molecules representing the primary constituents of the plant cell wall and CEO, respectively. Their interaction with ILs was investigated using quantum chemical calculations (QC) and wavefunction analysis. The results revealed that [EMIM][Tf2N] formed hydrogen bond (HB) interactions with cellobiose and exhibited strong van der Waals (vdW) interactions as well as HB interactions with ar-turmerone, leading to a significant enhancement in CEO extraction.
本研究确定了使用离子液体超声辅助水蒸馏（IL-U-HD）萃取姜黄精油（CEO）的最佳条件。在此条件下，姜黄精油的萃取率达到 6.88%，明显高于水蒸馏法（HD）、超声波辅助水蒸馏法（U-HD）和离子液体辅助水蒸馏法（IL-HD）。萃取动力学、气相色谱-质谱（GC-MS）成分分析、细胞存活率和萃取 CEO 的抗氧化特性表明，采用 IL-U-HD 萃取时，细胞存活率和抗氧化特性均有所提高。此外，与 HD 相比，萃取效率提高 22%的同时，成分馏分也有所增加。为了在分子水平上探索高效萃取机制，将纤维生物糖和 ar-turmerone 确定为模型分子，分别代表植物细胞壁和 CEO 的主要成分。利用量子化学计算（QC）和波函数分析研究了它们与 IL 的相互作用。结果表明，[EMIM][Tf2N] 与纤维生物糖形成氢键（HB）相互作用，与 ar-turmerone 表现出强烈的范德华（vdW）相互作用和氢键相互作用，从而显著提高了 CEO 的提取率。
{"title":"Ionic liquid ultrasound-assisted hydrodistillation high efficiency extraction of turmeric (Curcuma longa L.) essential oil and study of its extraction mechanism","authors":"Yu Chen, Huayang Yu, Yaxuan Liu, Yuxin Guo, Xiaoli Wang, Yang Wang, Chuanrun Li, Yichun Dong, Yanyan Guo","doi":"10.1016/j.seppur.2024.130504","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130504","url":null,"abstract":"The optimal conditions for extracting turmeric essential oil (CEO) using ionic liquid ultrasound-assisted hydrodistillation (IL-U-HD) were determined in this study. In this context, the CEO extraction yield reached 6.88 %, significantly higher than that of hydrodistillation (HD), ultrasound-assisted hydrodistillation (U-HD), and ionic liquid-assisted hydrodistillation (IL-HD). The extraction kinetics, GC–MS compositional analysis, cell viability, and antioxidant properties of the extracted CEO indicate enhanced cell viability and antioxidant properties when extracted by IL-U-HD. Additionally, the compositional fractions exhibited an increase while improving extraction efficiency by 22 % compared to HD. To explore the efficient extraction mechanism at the molecular level, cellobiose and <em>ar</em>-turmerone were established as model molecules representing the primary constituents of the plant cell wall and CEO, respectively. Their interaction with ILs was investigated using quantum chemical calculations (QC) and wavefunction analysis. The results revealed that [EMIM][Tf<sub>2</sub>N] formed hydrogen bond (HB) interactions with cellobiose and exhibited strong van der Waals (vdW) interactions as well as HB interactions with <em>ar</em>-turmerone, leading to a significant enhancement in CEO extraction.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"21 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637895","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Actual industrial emissions usually contain multiple aromatic VOCs, but little is known about adsorption and oxidation behaviors of multicomponent aromatic VOCs over catalysts, which limits the practical application of catalytic oxidation technology. Herein, the adsorption and oxidation of toluene and o-xylene mixture generated during paint production over Pt-based supported catalysts (Pt/NiO, Pt/Co3O4, Pt/Nb2O5 and Pt/CeO2) were investigated. Pt/Nb2O5 and Pt/CeO2 catalysts significantly promoted the oxidation of mixture. However, Pt/NiO and Pt/Co3O4 catalysts exhibited more difficulties in degrading mixed VOCs. Characterization results revealed that Pt/NiO and Pt/Co3O4 possessed higher percentage of surface adsorbed oxygen. Pt/Nb2O5 and Pt/CeO2 had more surface lattice oxygen, Pt0 species and acid sites. The weak competitive adsorption over Pt/Nb2O5 and Pt/CeO2 catalysts might be related to their acidic and electronic properties. In situ experiments proved that surface adsorbed oxygen and surface lattice oxygen of Pt/CeO2 could oxidize toluene and o-xylene simultaneously at lower temperature. However, the depleted oxygen species on Pt/Co3O4 could not be replenished in time due to the strong competitive adsorption and different oxidation mechanisms. This study uncovers the mixing effect of toluene and o-xylene over Pt/MOx catalysts, which provides a guiding direction towards the development of catalysts for efficient degradation of multicomponent VOCs.
{"title":"Unraveling the opposite behaviors of Pt/MOx catalysts for toluene and o-xylene mixture oxidation: Modulating mixing effect by optimization supports","authors":"Qiuling Wang, Jing Li, Song Wu, Jingping Feng, Jiali Lu, Zuliang Wu, Erhao Gao, Wei Wang, Jiali Zhu, Shuiliang Yao, Nanhua Wu","doi":"10.1016/j.seppur.2024.130536","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130536","url":null,"abstract":"Actual industrial emissions usually contain multiple aromatic VOCs, but little is known about adsorption and oxidation behaviors of multicomponent aromatic VOCs over catalysts, which limits the practical application of catalytic oxidation technology. Herein, the adsorption and oxidation of toluene and o-xylene mixture generated during paint production over Pt-based supported catalysts (Pt/NiO, Pt/Co<sub>3</sub>O<sub>4</sub>, Pt/Nb<sub>2</sub>O<sub>5</sub> and Pt/CeO<sub>2</sub>) were investigated. Pt/Nb<sub>2</sub>O<sub>5</sub> and Pt/CeO<sub>2</sub> catalysts significantly promoted the oxidation of mixture. However, Pt/NiO and Pt/Co<sub>3</sub>O<sub>4</sub> catalysts exhibited more difficulties in degrading mixed VOCs. Characterization results revealed that Pt/NiO and Pt/Co<sub>3</sub>O<sub>4</sub> possessed higher percentage of surface adsorbed oxygen. Pt/Nb<sub>2</sub>O<sub>5</sub> and Pt/CeO<sub>2</sub> had more surface lattice oxygen, Pt<sup>0</sup> species and acid sites. The weak competitive adsorption over Pt/Nb<sub>2</sub>O<sub>5</sub> and Pt/CeO<sub>2</sub> catalysts might be related to their acidic and electronic properties. <em>In situ</em> experiments proved that surface adsorbed oxygen and surface lattice oxygen of Pt/CeO<sub>2</sub> could oxidize toluene and o-xylene simultaneously at lower temperature. However, the depleted oxygen species on Pt/Co<sub>3</sub>O<sub>4</sub> could not be replenished in time due to the strong competitive adsorption and different oxidation mechanisms. This study uncovers the mixing effect of toluene and o-xylene over Pt/MOx catalysts, which provides a guiding direction towards the development of catalysts for efficient degradation of multicomponent VOCs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"129 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610318","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.seppur.2024.130543
Zi-Yi Zhao, Si-Jia Wang, Long-Bo Mi, Ming Lu, Jing-Jing Li, Guoliang Liu, Xiao-Qin Liu, Lin-Bing Sun
Hyper-cross-linked polymers (HCPs) feature excellent pore structures, ultra-high stability, and ease of preparation, making them promising candidates for visible-light-driven selective organic sulfide oxidation. Developing new HCPs of good performance is of great significance in the endeavor. Perylene diimide (PDI) exhibits excellent visible light absorption properties due to its high planar conjugated structure, showing potential as a monomer for photocatalytic HCP synthesis. In this study, we report the construction of two HCPs, named NUT-18 and NUT-18-Me, employing the Friedel-Crafts alkylation reaction using PDI derivatives as monomers. Both HCPs possess high specific surface area (reaching up to 811 and 828 m2/g) and photoactivity. Consequently, NUT-18 and NUT-18-Me demonstrated photocatalytic efficiency, with conversion and selectivity exceeding 98 % in the various organic sulfides’ photocatalytic oxidation. Notably, the photocatalytic performance is well-maintained even after 5 cycles, indicating good recyclability. Investigation of the catalytic mechanisms revealed that the selective catalytic oxidation of sulfides is based on the synergistic promotion of dual pathways for electron and energy transfer. This research highlights the potential of PDI molecules in designing and synthesizing porous materials as promising photocatalysts.
{"title":"Perylene diimide-based hyper-cross-linked polymers for visible-light-driven selective organic sulfide oxidation","authors":"Zi-Yi Zhao, Si-Jia Wang, Long-Bo Mi, Ming Lu, Jing-Jing Li, Guoliang Liu, Xiao-Qin Liu, Lin-Bing Sun","doi":"10.1016/j.seppur.2024.130543","DOIUrl":"https://doi.org/10.1016/j.seppur.2024.130543","url":null,"abstract":"Hyper-cross-linked polymers (HCPs) feature excellent pore structures, ultra-high stability, and ease of preparation, making them promising candidates for visible-light-driven selective organic sulfide oxidation. Developing new HCPs of good performance is of great significance in the endeavor. Perylene diimide (PDI) exhibits excellent visible light absorption properties due to its high planar conjugated structure, showing potential as a monomer for photocatalytic HCP synthesis. In this study, we report the construction of two HCPs, named NUT-18 and NUT-18-Me, employing the Friedel-Crafts alkylation reaction using PDI derivatives as monomers. Both HCPs possess high specific surface area (reaching up to 811 and 828 m<sup>2</sup>/g) and photoactivity. Consequently, NUT-18 and NUT-18-Me demonstrated photocatalytic efficiency, with conversion and selectivity exceeding 98 % in the various organic sulfides’ photocatalytic oxidation. Notably, the photocatalytic performance is well-maintained even after 5 cycles, indicating good recyclability. Investigation of the catalytic mechanisms revealed that the selective catalytic oxidation of sulfides is based on the synergistic promotion of dual pathways for electron and energy transfer. This research highlights the potential of PDI molecules in designing and synthesizing porous materials as promising photocatalysts.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"246 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.seppur.2024.130429
Zhouyi Chen , Xiao Zhang , Yue Shen , Wusong Geng , Chengyun Gong , Yunxia Zhang , Guozhong Wang
The enhancement of ion uptake capacity and electron transport process in the hybrid capacitive deionization (HCDI) Faraday electrode material is achieved by bridging Na2MnSiO4 (NMS) with acidified carbon nanotubes (HCNT). Herein, NMS@HCNT composites with three-dimensional conductive network structure were synthesized by the sol–gel method and subsequent thermal treatment. The NMS@HCNT Faraday electrode material displayed a high desalination capacity of 52.84 mg/g and a satisfactory mean salt adsorption rate of 6.89 mg/g/min, which are significantly higher than the desalination capacity (30.06 mg/g) and mean salt adsorption rate (4.35 mg/g/min) of NMS. This excellent desalination performance is mainly attributed to the fact that HCNT in the NMS@HCNT material not only acts as a highway for electron transport, but also increases the specific surface area of the material, which provide more ion-accessible surfaces and active sites to facilitate charge transfer and ion uptake capacity during desalination, thus effectively enhancing the HCDI performance of the electrode material. This study offers valuable insights into the design of HCDI electrode materials for high-efficiency desalination.
{"title":"Boosting ion uptake and electron transport through bridging Na2MnSiO4 with acidified carbon nanotubes for enhanced hybrid capacitance deionization","authors":"Zhouyi Chen , Xiao Zhang , Yue Shen , Wusong Geng , Chengyun Gong , Yunxia Zhang , Guozhong Wang","doi":"10.1016/j.seppur.2024.130429","DOIUrl":"10.1016/j.seppur.2024.130429","url":null,"abstract":"<div><div>The enhancement of ion uptake capacity and electron transport process in the hybrid capacitive deionization (HCDI) Faraday electrode material is achieved by bridging Na<sub>2</sub>MnSiO<sub>4</sub> (NMS) with acidified carbon nanotubes (HCNT). Herein, NMS@HCNT composites with three-dimensional conductive network structure were synthesized by the sol–gel method and subsequent thermal treatment. The NMS@HCNT Faraday electrode material displayed a high desalination capacity of 52.84 mg/g and a satisfactory mean salt adsorption rate of 6.89 mg/g/min, which are significantly higher than the desalination capacity (30.06 mg/g) and mean salt adsorption rate (4.35 mg/g/min) of NMS. This excellent desalination performance is mainly attributed to the fact that HCNT in the NMS@HCNT material not only acts as a highway for electron transport, but also increases the specific surface area of the material, which provide more ion-accessible surfaces and active sites to facilitate charge transfer and ion uptake capacity during desalination, thus effectively enhancing the HCDI performance of the electrode material. This study offers valuable insights into the design of HCDI electrode materials for high-efficiency desalination.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"359 ","pages":"Article 130429"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610268","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-14DOI: 10.1016/j.seppur.2024.130515
Chenghua Fan , Dongbo Wang , Yuyan Feng , Qingge Feng , Dachao Ma , Qiming Wang , Ying Lu , Wenqiang Yang
The advanced oxidation system involving periodate (PI) has demonstrated effective degradation capabilities for certain organic pollutants in water. A critical aspect of this process is the efficient activation of periodate. In this experiment, carbon vacancy-containing graphitic carbon nitride (Cv-CN) was prepared through a simple high-temperature calcination method, and Mn atoms were uniformly dispersed on its surface, forming Mn-Cv-CN. The presence of carbon vacancies modulated the electron density around the single-atom Mn, significantly enhancing the activation efficiency of PI. Surface-anchored Mn atoms with carbon vacancies in carbon nitride/periodate (Mn-Cv-CN/PI) system degraded 99% of sulfamethoxazole (SMX) within 25 min. Various degradation factors for SMX, including O2−, 1O2, IO3, OH, and electron transfer processes, were detected, with O2− identified as the primary reactive oxygen species (ROS). PI was activated by acquiring electrons from active sites, generating a substantial amount of O2− to catalytically transform the pollutants. Liquid chromatography-mass spectrometry was used to analyze the possible degradation pathways and intermediates of SMX. Multiple experiments demonstrated that the Mn-Cv-CN/PI system showed promising potential in treating water containing recalcitrant antibiotics. The findings provided a novel strategy for efficiently activating PI with single-atom catalysts to remove refractory pollutants from water.
{"title":"Efficient activation of periodate for sulfamethoxazole degradation by modulating charge density in single-atom Mn regions via carbon vacancies in carbon nitride","authors":"Chenghua Fan , Dongbo Wang , Yuyan Feng , Qingge Feng , Dachao Ma , Qiming Wang , Ying Lu , Wenqiang Yang","doi":"10.1016/j.seppur.2024.130515","DOIUrl":"10.1016/j.seppur.2024.130515","url":null,"abstract":"<div><div>The advanced oxidation system involving periodate (PI) has demonstrated effective degradation capabilities for certain organic pollutants in water. A critical aspect of this process is the efficient activation of periodate. In this experiment, carbon vacancy-containing graphitic carbon nitride (C<sub>v</sub>-CN) was prepared through a simple high-temperature calcination method, and Mn atoms were uniformly dispersed on its surface, forming Mn-C<sub>v</sub>-CN. The presence of carbon vacancies modulated the electron density around the single-atom Mn, significantly enhancing the activation efficiency of PI. Surface-anchored Mn atoms with carbon vacancies in carbon nitride/periodate (Mn-C<sub>v</sub>-CN/PI) system degraded 99% of sulfamethoxazole (SMX) within 25 min. Various degradation factors for SMX, including <img>O<sub>2</sub><sup>−</sup>, <sup>1</sup>O<sub>2</sub>, <img>IO<sub>3</sub>, <img>OH, and electron transfer processes, were detected, with <img>O<sub>2</sub><sup>−</sup> identified as the primary reactive oxygen species (ROS). PI was activated by acquiring electrons from active sites, generating a substantial amount of <img>O<sub>2</sub><sup>−</sup> to catalytically transform the pollutants. Liquid chromatography-mass spectrometry was used to analyze the possible degradation pathways and intermediates of SMX. Multiple experiments demonstrated that the Mn-C<sub>v</sub>-CN/PI system showed promising potential in treating water containing recalcitrant antibiotics. The findings provided a novel strategy for efficiently activating PI with single-atom catalysts to remove refractory pollutants from water.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"359 ","pages":"Article 130515"},"PeriodicalIF":8.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610317","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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