The idling of equipment caused by prolonged cooling times is a significant challenge impeding the upscaling application of temperature vacuum swing adsorption (TVSA) for carbon dioxide (CO2) capture from industrial flue gas. Increasing the adsorption temperature is a promising approach to reducing cooling times, mitigating equipment idling, and improving operational efficiency. However, maintaining CO2 purity and recovery rates at elevated adsorption temperatures remains unexplored. Through experimental and simulation studies, this work systematically optimized the operation parameters of a pilot-scale two-bed eight-step TVSA system to ensure its feasibility at a high adsorption temperature 343 K, a temperature that is 40 K higher than the optimal operation temperature of 13X-APG adsorbent and can warrant the continuous operation of the TVSA process. After optimization, CO2 purity of 95.08 % and recovery of 91.84 % were achieved under the conditions of an adsorption time of 380 s, an adsorption temperature of 343 K, a regeneration temperature of 393 K, a regeneration pressure of 11 kPa, and a purge gas flow rate of 0.083 m/s, which is comparable to the performance of low-temperature TVSA process. The effects of key operating parameters such as feed time (260–360 s), adsorption temperature (343–363 K), desorption temperature (383–403 K), vacuum (7–12 kPa) and purge gas flow rate (0–0.166 m/s) on the process performance were systematically examined. By resolving the issue of equipment idling, this study extends the practical applicability of the TVSA process in industrial scenarios.
{"title":"Enhanced CO2/N2 separation via optimized temperature/vacuum swing adsorption (TVSA) Processes: Experimental and simulation studies","authors":"Zhongru Zhou, Hao Ling, Yunlei Zhao, Hailong Li, Zequn Yang, Xiayi Hu","doi":"10.1016/j.seppur.2025.132051","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132051","url":null,"abstract":"The idling of equipment caused by prolonged cooling times is a significant challenge impeding the upscaling application of temperature vacuum swing adsorption (TVSA) for carbon dioxide (CO<sub>2</sub>) capture from industrial flue gas. Increasing the adsorption temperature is a promising approach to reducing cooling times, mitigating equipment idling, and improving operational efficiency. However, maintaining CO<sub>2</sub> purity and recovery rates at elevated adsorption temperatures remains unexplored. Through experimental and simulation studies, this work systematically optimized the operation parameters of a pilot-scale two-bed eight-step TVSA system to ensure its feasibility at a high adsorption temperature 343 K, a temperature that is 40 K higher than the optimal operation temperature of 13X-APG adsorbent and can warrant the continuous operation of the TVSA process. After optimization, CO<sub>2</sub> purity of 95.08 % and recovery of 91.84 % were achieved under the conditions of an adsorption time of 380 s, an adsorption temperature of 343 K, a regeneration temperature of 393 K, a regeneration pressure of 11 kPa, and a purge gas flow rate of 0.083 m/s, which is comparable to the performance of low-temperature TVSA process. The effects of key operating parameters such as feed time (260–360 s), adsorption temperature (343–363 K), desorption temperature (383–403 K), vacuum (7–12 kPa) and purge gas flow rate (0–0.166 m/s) on the process performance were systematically examined. By resolving the issue of equipment idling, this study extends the practical applicability of the TVSA process in industrial scenarios.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385255","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}
Low-temperature SCR denitrification technology requires catalysts with both NOx oxidation and NH3 adsorption capabilities. However, most catalysts, such as MnOx and MnO2/TiO2, with the problems of narrow activity temperature windows and low sulfur resistance. Herein, the mesoporous amorphous oxide catalysts Smα-MnTiOx are successfully synthesized by a solvothermal method. The catalyst displays excellent low-temperature activity and sulfur tolerance, with a denitrification conversion of over 90 % within the range of 160°C to 350°C. Furthermore, the denitrification conversion was maintained at more than 98 % for 8 h at 250°C and 50 ppm SO2 atmosphere. The reducibility capacity and surface acidity of Smα-MnTiOx catalysts are improve by the doping of Sm, thus facilitating the adsorption and activation of NH3 and O2, which is beneficial for the improvement of catalytic activity. The in-situ DRIFTS shows the abundant chemisorbed oxygen on the surface of Smα-MnTiOx favors NO2 generation, and the doping of Sm extended the temperature range of NO2 (50–250 ℃),which promotes the reaction towards the Fast-SCR reaction pathway at low temperatures. The combined effect of E-R mechanism and Fast-SCR reaction successfully broaden the denitration temperature window of Smα-MnTiOx catalysts. Furthermore, the interaction between Mn and Sm species effectively inhibits the electron transfer from Mn to SO2, which reduces the generation of metal sulfate and protect the active sites of the catalyst. This study provides new ideas for the improvement of denitrification catalysts with sulfur tolerance, water resistance and upper and lower catalytic activity.
{"title":"Construction of mesoporous amorphous Smα-MnTiOx with high deNOx performance and sulfur Tolerance: Insight into the synergistic Sulfur-Resistant effect between Manganese-Samarium species","authors":"Xuewu Hou, Jitong Wang, Cheng Ma, Wenming Qiao, Licheng Ling","doi":"10.1016/j.seppur.2025.132030","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132030","url":null,"abstract":"Low-temperature SCR denitrification technology requires catalysts with both NO<sub>x</sub> oxidation and NH<sub>3</sub> adsorption capabilities. However, most catalysts, such as MnO<sub>x</sub> and MnO<sub>2</sub>/TiO<sub>2</sub>, with the problems of narrow activity temperature windows and low sulfur resistance. Herein, the mesoporous amorphous oxide catalysts Sm<sub>α</sub>-MnTiO<sub>x</sub> are successfully synthesized by a solvothermal method. The catalyst displays excellent low-temperature activity and sulfur tolerance, with a denitrification conversion of over 90 % within the range of 160°C to 350°C. Furthermore, the denitrification conversion was maintained at more than 98 % for 8 h at 250°C and 50 ppm SO<sub>2</sub> atmosphere. The reducibility capacity and surface acidity of Sm<sub>α</sub>-MnTiO<sub>x</sub> catalysts are improve by the doping of Sm, thus facilitating the adsorption and activation of NH<sub>3</sub> and O<sub>2</sub>, which is beneficial for the improvement of catalytic activity. The in-situ DRIFTS shows the abundant chemisorbed oxygen on the surface of Sm<sub>α</sub>-MnTiO<sub>x</sub> favors NO<sub>2</sub> generation, and the doping of Sm extended the temperature range of NO<sub>2</sub> (50–250 ℃),which promotes the reaction towards the Fast-SCR reaction pathway at low temperatures. The combined effect of E-R mechanism and Fast-SCR reaction successfully broaden the denitration temperature window of Sm<sub>α</sub>-MnTiO<sub>x</sub> catalysts. Furthermore, the interaction between Mn and Sm species effectively inhibits the electron transfer from Mn to SO<sub>2</sub>, which reduces the generation of metal sulfate and protect the active sites of the catalyst. This study provides new ideas for the improvement of denitrification catalysts with sulfur tolerance, water resistance and upper and lower catalytic activity.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"26 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375817","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132052
Yingying Fan, Junjie Liu, Xu Han
Photocatalytic generation of oxidative free radicals is an effective method to eliminate viruses and bacteria in air. Nevertheless, the underlying mechanisms governing the gas-phase sterilization remain unclear. In this study, the self-doped Bi2.15WO6 was synthesized to prepare the Bi2.15WO6 coating. In the presence of Bi2.15WO6 coating, the average logarithmic degradation efficiencies (LDEs) are 3.82 and 3.07 for E. coli and S. aureus, respectively under UV illumination for 12.9 s, indicating its desirable sterilization efficiencies. In addition, the sterilization rates of E. coli and S. aureus slightly decrease by 3 % and 6 % after 30-repeated cycles, indicating the high stability of this catalytic coating. The 2,7-dichlorofluorescein (DCF) fluorescence experiments and SEM analysis indicate that reactive oxygen species (ROS) produced by Bi2.15WO6 have effectively destroyed cell structure to achieve the complete inactivation. The N,N-diethyl-p-phenylenediamine sulfate (DPD) and radical trapping experiments further reveal that H2O2 is the primary oxidizing species, and its yield is linearly proportional to the LDE values. The produced H2O2 is further decomposed to •OH under UV irradiation to kill bacteria. Raman analysis confirms the presence of the intermediate species of surface ≡Bi-OO•superoxo and/or ≡Bi-OOH peroxo groups on Bi2.15WO6, which are the precursors of H2O2. In addition, the 3-D filter facilitates sterilization by the Bi2.15WO6 in that it prolongs the duration of free radical via physically intercepting bioaerosols, thus apparently improving the degradation rate. This study provides new insights on the sterilization mechanism involved in the gas-phase photocatalytic processes.
{"title":"Important contributions of in-situ produced H2O2 during photocatalytic sterilization of air by self-doped Bi2.15WO6","authors":"Yingying Fan, Junjie Liu, Xu Han","doi":"10.1016/j.seppur.2025.132052","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132052","url":null,"abstract":"Photocatalytic generation of oxidative free radicals is an effective method to eliminate viruses and bacteria in air. Nevertheless, the underlying mechanisms governing the gas-phase sterilization remain unclear. In this study, the self-doped Bi<sub>2.15</sub>WO<sub>6</sub> was synthesized to prepare the Bi<sub>2.15</sub>WO<sub>6</sub> coating. In the presence of Bi<sub>2.15</sub>WO<sub>6</sub> coating, the average logarithmic degradation efficiencies (<em>LDEs</em>) are 3.82 and 3.07 for <em>E. coli</em> and <em>S. aureus</em>, respectively under UV illumination for 12.9 s, indicating its desirable sterilization efficiencies. In addition, the sterilization rates of <em>E. coli</em> and <em>S. aureus</em> slightly decrease by 3 % and 6 % after 30-repeated cycles, indicating the high stability of this catalytic coating. The 2,7-dichlorofluorescein (DCF) fluorescence experiments and SEM analysis indicate that reactive oxygen species (ROS) produced by Bi<sub>2.15</sub>WO<sub>6</sub> have effectively destroyed cell structure to achieve the complete inactivation. The <em>N,N</em>-diethyl-p-phenylenediamine sulfate (DPD) and radical trapping experiments further reveal that H<sub>2</sub>O<sub>2</sub> is the primary oxidizing species, and its yield is linearly proportional to the <em>LDE</em> values. The produced H<sub>2</sub>O<sub>2</sub> is further decomposed to •OH under UV irradiation to kill bacteria. Raman analysis confirms the presence of the intermediate species of surface ≡Bi-OO•superoxo and/or ≡Bi-OOH peroxo groups on Bi<sub>2.15</sub>WO<sub>6</sub>, which are the precursors of H<sub>2</sub>O<sub>2</sub>. In addition, the 3-D filter facilitates sterilization by the Bi<sub>2.15</sub>WO<sub>6</sub> in that it prolongs the duration of free radical via physically intercepting bioaerosols, thus apparently improving the degradation rate. This study provides new insights on the sterilization mechanism involved in the gas-phase photocatalytic processes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"29 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375536","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}
Most wastewater treatment plants (WWTPs) encounter the problem of insufficient carbon sources. Particularly, the removal of organic pollutants is severely affected by carbon limitation and thus requires the use of external carbon sources in the secondary biological treatment process, which considerably increases operating costs. Even after the secondary treatment of high-concentration organic wastewater, the effluent still contains various organic substrates, such as low molecular weight organic acids and carbohydrates, etc., which can be used as carbon sources in the process of nitrogen and phosphorus removal. Effective separation and recovery of organic carbon sources in high-concentration organic wastewater are crucial to realize the resource utilization of organic carbon sources. In this study, a novel sandwich-structure thin-film composite (TFC) nanofiltration membrane was synthesized via chemically bonding polyvinyl alcohol (PVA) to form an interlayer and surface modification by Fe3+ and tannic acid (TA) chelating coordination on the polyamide (PA) layer. The design promoted the deposition of metal polyphenol networks on the PA layer, exposing more chelating sites while reducing the force resistance generated by deposition. The interlayer improved the permeability of the membrane, and the deposition of Fe–TA complexes enhanced membrane separation efficiency. Compared with the TFC-Fe membrane, the resulting membrane (PVA-TFC-Fe) showed a 56.42 % increase in permeability and enhanced rejection of inorganic salts and small-molecule organic carbon sources. Compared with the retention of the TFC-control membrane, that of PVA-TFC-Fe for small-molecule carbon sources, namely, acetic acid, propionic acid, and butyric acid, increased by 19.05 %, 17.34 %, and 15.67 %, respectively, and exhibited long-term operational stability.
{"title":"Novel nanofiltration composite membrane with a sandwich-structure of polyvinyl alcohol interlayer and Fe3+-tannic acid polyamide layer for carbon source recovery","authors":"Xiujuan Hao, Yukai Hu, Rijian Quan, Xiayu Xu, Xin Liu, Yukun Li, Jiayu Tian","doi":"10.1016/j.seppur.2025.132047","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132047","url":null,"abstract":"Most wastewater treatment plants (WWTPs) encounter the problem of insufficient carbon sources. Particularly, the removal of organic pollutants is severely affected by carbon limitation and thus requires the use of external carbon sources in the secondary biological treatment process, which considerably increases operating costs. Even after the secondary treatment of high-concentration organic wastewater, the effluent still contains various organic substrates, such as low molecular weight organic acids and carbohydrates, etc., which can be used as carbon sources in the process of nitrogen and phosphorus removal. Effective separation and recovery of organic carbon sources in high-concentration organic wastewater are crucial to realize the resource utilization of organic carbon sources. In this study, a novel sandwich-structure thin-film composite (TFC) nanofiltration membrane was synthesized via chemically bonding polyvinyl alcohol (PVA) to form an interlayer and surface modification by Fe<sup>3+</sup> and tannic acid (TA) chelating coordination on the polyamide (PA) layer. The design promoted the deposition of metal polyphenol networks on the PA layer, exposing more chelating sites while reducing the force resistance generated by deposition. The interlayer improved the permeability of the membrane, and the deposition of Fe–TA complexes enhanced membrane separation efficiency. Compared with the TFC-Fe membrane, the resulting membrane (PVA-TFC-Fe) showed a 56.42 % increase in permeability and enhanced rejection of inorganic salts and small-molecule organic carbon sources. Compared with the retention of the TFC-control membrane, that of PVA-TFC-Fe for small-molecule carbon sources, namely, acetic acid, propionic acid, and butyric acid, increased by 19.05 %, 17.34 %, and 15.67 %, respectively, and exhibited long-term operational stability.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"2 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385253","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132011
Bolong Zhao , Yonggang Sun , Guangsuo Yu , Min Xu , Juan Zhang , Duoning Zhao , Yulong Ma
Nitrogen doping plays a crucial role in activating the Fenton catalytic activity of transition metal oxides. However, the mechanism by which nitrogen doping sites influence the properties of these oxides remains unclear. We successfully incorporated nitrogen atoms into the internal lattice of MnFe2O4 spinel through thermal activation and identified two major doping sites: interstitial nitrogen (Nint) and substitutional nitrogen (Nsub). Through in-situ DIRFTS experiments and DFT calculations, we proposed a unique mechanism. Both sites can effectively activate the catalytic activity of the oxides, but Nsub is particularly effective in altering the electron distribution of Mn elements within the lattice. This alteration promotes the transformation of superoxide (•O2–/•OOH) to H2O2, thereby further enhancing catalytic activity. Compared to un-doped MnFe2O4, experimental results obtained using MnFe2O4N0.4 as the catalyst demonstrated that the degradation rate constant of tetracycline in simulated wastewater increased from 0.0072 min−1 to 0.2745 min−1. Furthermore, the degradation rate of tetracycline reached 98.7 %. For real wastewater experiments, the COD removal rate was 77.4 %, and the mineralization rate was 62.5 %. This study offers new insights into the design of nitrogen-doped transition metal oxide catalysts.
{"title":"Igniting the catalytic activity of Mn-Fe spinel for Fenton reactions: The doped nitrogen atoms in the interstitial sites and substitutional sites","authors":"Bolong Zhao , Yonggang Sun , Guangsuo Yu , Min Xu , Juan Zhang , Duoning Zhao , Yulong Ma","doi":"10.1016/j.seppur.2025.132011","DOIUrl":"10.1016/j.seppur.2025.132011","url":null,"abstract":"<div><div>Nitrogen doping plays a crucial role in activating the Fenton catalytic activity of transition metal oxides. However, the mechanism by which nitrogen doping sites influence the properties of these oxides remains unclear. We successfully incorporated nitrogen atoms into the internal lattice of MnFe<sub>2</sub>O<sub>4</sub> spinel through thermal activation and identified two major doping sites: interstitial nitrogen (N<sub>int</sub>) and substitutional nitrogen (N<sub>sub</sub>). Through <em>in-situ</em> DIRFTS experiments and DFT calculations, we proposed a unique mechanism. Both sites can effectively activate the catalytic activity of the oxides, but N<sub>sub</sub> is particularly effective in altering the electron distribution of Mn elements within the lattice. This alteration promotes the transformation of superoxide (•O<sub>2</sub><sup>–</sup>/•OOH) to H<sub>2</sub>O<sub>2</sub>, thereby further enhancing catalytic activity. Compared to un-doped MnFe<sub>2</sub>O<sub>4</sub>, experimental results obtained using MnFe<sub>2</sub>O<sub>4</sub>N<sub>0.4</sub> as the catalyst demonstrated that the degradation rate constant of tetracycline in simulated wastewater increased from 0.0072 min<sup>−1</sup> to 0.2745 min<sup>−1</sup>. Furthermore, the degradation rate of tetracycline reached 98.7 %. For real wastewater experiments, the COD removal rate was 77.4 %, and the mineralization rate was 62.5 %. This study offers new insights into the design of nitrogen-doped transition metal oxide catalysts.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132011"},"PeriodicalIF":8.1,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375818","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132042
Xiaodong Zhang, Ziwei Shen, Hao Lyu, Zuming Liu, Jinsheng Sun
Industrial methanol distillation systems typically use a fusel oil side-draw to maintain product purity; however, fusel oil is a hazardous byproduct that poses significant safety risks. This study proposes an alternative strategy that processes diluted alcohol instead of fusel oil to mitigate safety concerns and meet regulatory requirements. Four configurations were evaluated, combining forward and backward multi-effect heat integration schemes with fusel oil side-draw and diluted alcohol strategies. A simultaneous optimization algorithm was employed to optimize process parameters and heat integration structures. The results show that the diluted alcohol strategy outperforms fusel oil side-draw configurations in terms of total annual cost and methanol recovery rates, demonstrating its economic and operational advantages. Furthermore, the optimized configurations achieved lower unit steam consumption than values reported in the literature, highlighting the energy efficiency of the proposed approach. To enhance decarbonization potential, heat pump-based electrification strategies were assessed, including mechanical vapor recompression (MVR), flash vapor circulation (FVC), and FVC combined with bottom flashing (FVC-BP). Despite their low coefficient of performance, these strategies offer significant carbon reduction potential, achieving up to 95.5 % emission reductions in countries with low grid carbon intensity, such as Norway, and 54.3 % in countries with high grid carbon intensity, such as China.
{"title":"Energy-efficient and sustainable methanol distillation: Exploring diluted alcohol strategies, multi-effect heat integration, and heat pump-based electrification for carbon reduction","authors":"Xiaodong Zhang, Ziwei Shen, Hao Lyu, Zuming Liu, Jinsheng Sun","doi":"10.1016/j.seppur.2025.132042","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132042","url":null,"abstract":"Industrial methanol distillation systems typically use a fusel oil side-draw to maintain product purity; however, fusel oil is a hazardous byproduct that poses significant safety risks. This study proposes an alternative strategy that processes diluted alcohol instead of fusel oil to mitigate safety concerns and meet regulatory requirements. Four configurations were evaluated, combining forward and backward multi-effect heat integration schemes with fusel oil side-draw and diluted alcohol strategies. A simultaneous optimization algorithm was employed to optimize process parameters and heat integration structures. The results show that the diluted alcohol strategy outperforms fusel oil side-draw configurations in terms of total annual cost and methanol recovery rates, demonstrating its economic and operational advantages. Furthermore, the optimized configurations achieved lower unit steam consumption than values reported in the literature, highlighting the energy efficiency of the proposed approach. To enhance decarbonization potential, heat pump-based electrification strategies were assessed, including mechanical vapor recompression (MVR), flash vapor circulation (FVC), and FVC combined with bottom flashing (FVC-BP). Despite their low coefficient of performance, these strategies offer significant carbon reduction potential, achieving up to 95.5 % emission reductions in countries with low grid carbon intensity, such as Norway, and 54.3 % in countries with high grid carbon intensity, such as China.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375537","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132033
Hong-Chan Jiang, Shi-Ming Li, Qing-Ling Ni, Liu-Cheng Gui, Xiu-Jian Wang
In the petrochemical industry, the efficient one-step adsorption separation of ethylene (C2H4) and ethane (C2H6) is a favored but challenging technical task. This highlights the importance of upgrading functional group design standards to create physical adsorbent materials that combines superior C2H6 adsorption capacity and excellent C2H6/C2H4 selectivity to meet the demanding needs of industry. Herein, we presented a strategy that tuning the pore environment of nonpolar metal–organic frameworks (MOFs) via installing additional polar functional binding sites in the pores to boost C2H6/C2H4 separation performance. By introducing methyl and fluorine as functional sites into carboxylic ligands, we successfully designed and synthesized two novel MOFs, named GNU-3-Me and GNU-3-F. The pore size and physical and chemical properties of the two MOFs were carefully regulated. We found that the GNU-3-F has an optimized aperture and pore surface environment, with a high C2H6 uptake (92.55 cm3 cm−3 at 1 bar and 298 K) and an outstanding equimolar C2H6/C2H4 selectivity (2.1), superior to most C2H6 selective MOFs. Computational studies show this excellent C2H6 absorption capacity and selectivity in GNU-3-F mainly roots in its well-designed pore size and fluorine modified pore environment. These properties work together to significantly improve its affinity and distinguish ability to C2H6 molecules in GNU-3-F. The breakthrough experiments finally demonstrate that GNU-3-F can efficiently separate C2H6/C2H4 mixtures under ambient conditions.
{"title":"Pore engineering in double-wall MOFs through immobilizing functional bonding sites for boosting efficient ethane/ethylene separation","authors":"Hong-Chan Jiang, Shi-Ming Li, Qing-Ling Ni, Liu-Cheng Gui, Xiu-Jian Wang","doi":"10.1016/j.seppur.2025.132033","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132033","url":null,"abstract":"In the petrochemical industry, the efficient one-step adsorption separation of ethylene (C<sub>2</sub>H<sub>4</sub>) and ethane (C<sub>2</sub>H<sub>6</sub>) is a favored but challenging technical task. This highlights the importance of upgrading functional group design standards to create physical adsorbent materials that combines superior C<sub>2</sub>H<sub>6</sub> adsorption capacity and excellent C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity to meet the demanding needs of industry. Herein, we presented a strategy that tuning the pore environment of nonpolar metal–organic frameworks (MOFs) via installing additional polar functional binding sites in the pores to boost C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> separation performance. By introducing methyl and fluorine as functional sites into carboxylic ligands, we successfully designed and synthesized two novel MOFs, named <strong>GNU-3-Me</strong> and <strong>GNU-3-F</strong>. The pore size and physical and chemical properties of the two MOFs were carefully regulated. We found that the <strong>GNU-3-F</strong> has an optimized aperture and pore surface environment, with a high C<sub>2</sub>H<sub>6</sub> uptake (92.55 cm<sup>3</sup> cm<sup>−3</sup> at 1 bar and 298 K) and an outstanding equimolar C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (2.1), superior to most C<sub>2</sub>H<sub>6</sub> selective MOFs. Computational studies show this excellent C<sub>2</sub>H<sub>6</sub> absorption capacity and selectivity in <strong>GNU-3-F</strong> mainly roots in its well-designed pore size and fluorine modified pore environment. These properties work together to significantly improve its affinity and distinguish ability to C<sub>2</sub>H<sub>6</sub> molecules in <strong>GNU-3-F</strong>. The breakthrough experiments finally demonstrate that <strong>GNU-3-F</strong> can efficiently separate C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> mixtures under ambient conditions.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375539","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.131972
Mingming Wang, Jie Wang, Guorui Wu, Qi Shen, Wei Zhang, Jia Guo, Linfeng Huang, Liang Feng, Chunyan Yuan, Feiyun Sun
Developing resilient and stable carbon-based metal catalysts for activating peroxymonosulfate (PMS) has attracted great attention in the advanced oxidation processes (AOP) area for removing organic pollutants in wastewater. This study synthesized CoFe2S4/CNTs (CFS-CNTs) nanocomposites using hydrothermal technique, which can activate PMS for efficient degradation of tetracycline (TC). A detailed characterization of the synthesized catalysts was conducted, and their catalytic performance was assessed by varying parameters such as catalyst dosage, PMS concentration, pH, and the presence of co-existing substances. The results demonstrated that CFS-CNTs showed excellent TC removal efficiency and reusability, even showing satisfactory degrading performance for various surface water matrices. The superior activities of the prepared catalysts are attributed mainly to the synergistic interaction of the bimetallic sulfides and CNTs. This synergy aids in the uniform dispersion of the catalysts and increases the availability of catalytic sites, which are essential in producing more active species. Free radical quenching experiments, chemical probe analyses, and electron paramagnetic resonance (EPR) demonstrated that SO4·− and 1O2 were the primary reactive oxygen species generated during the reaction environment. X-ray photoelectron spectroscopy (XPS) and electrochemical assessments also indicate that carbon nanotubes also functioned as high-speed charges, facilitating channels to achieve rapid electron transfer and accelerating the cycling of metal valence states. The TC degradation pathways, intermediate toxicity assessment, and CFS-CNTs/PMS system response mechanisms were also proposed. These findings provide new insights into the application of metal sulfides in PMS systems for the treatment of wastewater containing refractory organic pollutants.
{"title":"CoFe2S4-modified CNTs catalyst to activate peroxymonosulfate under a wide range pH for high-efficient tetracycline degradation via radical and non-radical paths","authors":"Mingming Wang, Jie Wang, Guorui Wu, Qi Shen, Wei Zhang, Jia Guo, Linfeng Huang, Liang Feng, Chunyan Yuan, Feiyun Sun","doi":"10.1016/j.seppur.2025.131972","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131972","url":null,"abstract":"Developing resilient and stable carbon-based metal catalysts for activating peroxymonosulfate (PMS) has attracted great attention in the advanced oxidation processes (AOP) area for removing organic pollutants in wastewater. This study synthesized CoFe<sub>2</sub>S<sub>4</sub>/CNTs (CFS-CNTs) nanocomposites using hydrothermal technique, which can activate PMS for efficient degradation of tetracycline (TC). A detailed characterization of the synthesized catalysts was conducted, and their catalytic performance was assessed by varying parameters such as catalyst dosage, PMS concentration, pH, and the presence of co-existing substances. The results demonstrated that CFS-CNTs showed excellent TC removal efficiency and reusability, even showing satisfactory degrading performance for various surface water matrices. The superior activities of the prepared catalysts are attributed mainly to the synergistic interaction of the bimetallic sulfides and CNTs. This synergy aids in the uniform dispersion of the catalysts and increases the availability of catalytic sites, which are essential in producing more active species. Free radical quenching experiments, chemical probe analyses, and electron paramagnetic resonance (EPR) demonstrated that SO<sub>4</sub>·<sup>−</sup> and <sup>1</sup>O<sub>2</sub> were the primary reactive oxygen species generated during the reaction environment. X-ray photoelectron spectroscopy (XPS) and electrochemical assessments also indicate that carbon nanotubes also functioned as high-speed charges, facilitating channels to achieve rapid electron transfer and accelerating the cycling of metal valence states. The TC degradation pathways, intermediate toxicity assessment, and CFS-CNTs/PMS system response mechanisms were also proposed. These findings provide new insights into the application of metal sulfides in PMS systems for the treatment of wastewater containing refractory organic pollutants.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"23 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375542","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132050
Sun Hae Ra Shin, Ambalavanan Jayaraman, Praveen K. Thallapally
Recycling halogen gas from spent nuclear fuel is desirable for improving economic feasibility of molten salt reactors and beneficial for various industrial processes. In this review, we discuss the current progress of various types of porous adsorbents designed for halogen gas uptake (exclusively F2, Cl2, and Br2) and address challenges associated with industrial application. We believe that this review will provide both fundamental and practical insights for adsorbent design in the field of halogen gas capture.
{"title":"Recent advances in the capture of halogen gas by porous adsorbents: A review","authors":"Sun Hae Ra Shin, Ambalavanan Jayaraman, Praveen K. Thallapally","doi":"10.1016/j.seppur.2025.132050","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132050","url":null,"abstract":"Recycling halogen gas from spent nuclear fuel is desirable for improving economic feasibility of molten salt reactors and beneficial for various industrial processes. In this review, we discuss the current progress of various types of porous adsorbents designed for halogen gas uptake (exclusively F<sub>2</sub>, Cl<sub>2</sub>, and Br<sub>2</sub>) and address challenges associated with industrial application. We believe that this review will provide both fundamental and practical insights for adsorbent design in the field of halogen gas capture.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"16 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375816","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 : 2025-02-10DOI: 10.1016/j.seppur.2025.132041
Miao Wang , Kai Wang , Zhiliang Jin
To address the limitations of CoMoO4 photocatalysts (e.g., high recombination rate of photogenerated electron-hole pairs and low light energy utilization), a novel CoMoO4/AgVO3 photocatalyst enriched with oxygen vacancies (OV) was constructed and the photocatalytic hydrogen production ability under visible light irradiation was investigated. The experimental results indicate that the hydrogen production efficiency of CoMoO4/AgVO3-30 reaches 3049.28μmol g−1h−1, which is 5.07 times higher than that of CoMoO4 and 8.89 times higher than that of AgVO3. Based on the XPS, UPS and DFT characterization results, it can be inferred that, since the work function of CoMoO4 compared to is lower than that of AgVO3, the electrons of CoMoO4 undergo transfer AgVO3 when the two are in contact, thus optimizing the energy band structure. In-situ XPS results further reveal that under photoexcitation conditions, the electrons of CoMoO4 are continuously transferred to AgVO3, consistent with the S-scheme electron transfer mechanism, which facilitates the spatial separation of photogenerated carriers and holes. Furthermore, the abundant OV in CoMoO4/AgVO3 enhances the capture of photogenerated electrons and promotes the hydrogen evolution reaction. S-scheme electron transfer mechanism synergizes with abundant OV to boost photocatalytic hydrogen evolution activity.
{"title":"Construction of novel CoMoO4/AgVO3 heterojunction with abundant oxygen vacancies for efficient photocatalytic hydrogen evolution","authors":"Miao Wang , Kai Wang , Zhiliang Jin","doi":"10.1016/j.seppur.2025.132041","DOIUrl":"10.1016/j.seppur.2025.132041","url":null,"abstract":"<div><div>To address the limitations of CoMoO<sub>4</sub> photocatalysts (e.g., high recombination rate of photogenerated electron-hole pairs and low light energy utilization), a novel CoMoO<sub>4</sub>/AgVO<sub>3</sub> photocatalyst enriched with oxygen vacancies (O<sub>V</sub>) was constructed and the photocatalytic hydrogen production ability under visible light irradiation was investigated. The experimental results indicate that the hydrogen production efficiency of CoMoO<sub>4</sub>/AgVO<sub>3</sub>-30 reaches 3049.28μmol g<sup>−1</sup>h<sup>−1</sup>, which is 5.07 times higher than that of CoMoO<sub>4</sub> and 8.89 times higher than that of AgVO<sub>3</sub>. Based on the XPS, UPS and DFT characterization results, it can be inferred that, since the work function of CoMoO<sub>4</sub> compared to is lower than that of AgVO<sub>3</sub>, the electrons of CoMoO<sub>4</sub> undergo transfer AgVO<sub>3</sub> when the two are in contact, thus optimizing the energy band structure. In-situ XPS results further reveal that under photoexcitation conditions, the electrons of CoMoO<sub>4</sub> are continuously transferred to AgVO<sub>3</sub>, consistent with the S-scheme electron transfer mechanism, which facilitates the spatial separation of photogenerated carriers and holes. Furthermore, the abundant O<sub>V</sub> in CoMoO<sub>4</sub>/AgVO<sub>3</sub> enhances the capture of photogenerated electrons and promotes the hydrogen evolution reaction. S-scheme electron transfer mechanism synergizes with abundant O<sub>V</sub> to boost photocatalytic hydrogen evolution activity.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132041"},"PeriodicalIF":8.1,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375813","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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