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Constructing a solar-driven capture material for iodide removal from aquatic radio waste
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132237
Rui Jiao, Yiwan Si, Pengzhi Ma, Jiyan Li, Zhaoqi Zhu, Hanxue Sun, An Li
Radioactive elements have recently received much attention considering that it does serious harm to the human and environment. The solar-driven adsorption coupled interface evaporation process is a more efficient method for treating volatile radioactive iodide ions. Herein, a newly induced capture strategy was designed to obtain efficient solar-driven adsorption coupled interface evaporation material for high performance treatment of iodide ions via skillfully molecular design and pore size regulate process, in which 1,3-dichloroisoquinoline with smaller block structures serving as the trapper. In addition, the unique π-π interactions of conjugated microporous polymers (CMPs), as well as the excellent water transport channel penetrated by hydrogel, contribute to the capture of target ions. In this paper, the hollow microspheres CMPs-1 exhibited the highest iodide adsorption capacity (15.96 mg g−1), reaching equilibrium after 7 h of static adsorption in a 0.10 mmol L-1 iodide ions solution. Under 1 sun, CMP-based porous composite hydrogel PCH-CMP-1 realized outstanding pure water interfacial evaporation rate (2.42 kg m−2h−1), which exceeded the evaporation rate reported in many other literatures. Based on the iodine adsorption capacity of CMPs-1 and the excellent interfacial evaporation ability of PCH-CMP-1, PCH-CMP-1 had a good interfacial evaporation rate for iodide ions solutions (1.50 kg m−2h−1), and the distillate did not contain iodide ions, in which some are adsorbed by the PCH-CMP-1 and some remain in the solution. With its extraordinary pore structure and excellent interfacial evaporation ability, the PCH-CMP-1 demonstrates the potential of an excellent solar-driven adsorption coupled interface evaporation materials for treating radioactive iodine.
{"title":"Constructing a solar-driven capture material for iodide removal from aquatic radio waste","authors":"Rui Jiao,&nbsp;Yiwan Si,&nbsp;Pengzhi Ma,&nbsp;Jiyan Li,&nbsp;Zhaoqi Zhu,&nbsp;Hanxue Sun,&nbsp;An Li","doi":"10.1016/j.seppur.2025.132237","DOIUrl":"10.1016/j.seppur.2025.132237","url":null,"abstract":"<div><div>Radioactive elements have recently received much attention considering that it does serious harm to the human and environment. The solar-driven adsorption coupled interface evaporation process is a more efficient method for treating volatile radioactive iodide ions. Herein, a newly induced capture strategy was designed to obtain efficient solar-driven adsorption coupled interface evaporation material for high performance treatment of iodide ions via skillfully molecular design and pore size regulate process, in which 1,3-dichloroisoquinoline with smaller block structures serving as the trapper. In addition, the unique π-π interactions of conjugated microporous polymers (CMPs), as well as the excellent water transport channel penetrated by hydrogel, contribute to the capture of target ions. In this paper, the hollow microspheres CMPs-1 exhibited the highest iodide adsorption capacity (15.96 mg g<sup>−1</sup>), reaching equilibrium after 7 h of static adsorption in a 0.10 mmol L<sup>-1</sup> iodide ions solution. Under 1 sun, CMP-based porous composite hydrogel PCH-CMP-1 realized outstanding pure water interfacial evaporation rate (2.42 kg m<sup>−2</sup>h<sup>−1</sup>), which exceeded the evaporation rate reported in many other literatures. Based on the iodine adsorption capacity of CMPs-1 and the excellent interfacial evaporation ability of PCH-CMP-1, PCH-CMP-1 had a good interfacial evaporation rate for iodide ions solutions (1.50 kg m<sup>−2</sup>h<sup>−1</sup>), and the distillate did not contain iodide ions, in which some are adsorbed by the PCH-CMP-1 and some remain in the solution. With its extraordinary pore structure and excellent interfacial evaporation ability, the PCH-CMP-1 demonstrates the potential of an excellent solar-driven adsorption coupled interface evaporation materials for treating radioactive iodine.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132237"},"PeriodicalIF":8.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471045","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}
引用次数: 0
Sub-Nano Gaδ+ clusters confined by porous carbon spheres and coupled with SnS2 for efficient photocatalytic extraction of uranium
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132195
Yuehua Pan , Yingxue Pang , Hao Fu , Zhenyu Cai , Yuxiang Deng , Zhiwei Huang , Donglou Ren , Yuezhou Wei , Xinpeng Wang
Extracting uranium from uranium waste streams, particularly utilizing zero-carbon emission photochemistry, emerges as a promising and sustainable strategy. Herein, we construct an SS@Ga/PCS composite photocatalyst, consisting of SnS2 nanosheets as well as a metal − support produced by confining sub-nano Gaδ+ clusters in the hollow porous carbon spheres (PCS). The Gaδ+ clusters are innovatively introduced as active sites with localized hole capability to simultaneously improve visible light response and carrier separation. In-situ characterizations and theoretical calculations reveal that Gaδ+ clusters induced metal-support interaction (MSI) by optimizing the electronic structure in the PCS host; In addition, Gaδ+ clusters act as plasma excitation elements to enhance the visible light responsiveness and carrier separation of SS@Ga/PCS. Ultimately, the inhomogeneous photocatalysis of uranium extraction achieved superior performance as compared to the pure components, corresponding to an encouraging removal rate of 97.87 % and a photo-extraction capacity of up to 1867.30 mg g−1 in 50 mL of uranium waste solution, as well as a wide-concentration window adaptability and excellent catalytic robustness. More significantly, this ingenious nano-confined strategy extends the design ideas of highly dispersed sub-nanometallic cluster co-catalysts and stimulates the study of the availability of abundant reactive active sites combined with monomer strong interactions, which provides a novel insight into the mechanism of photocatalytic uranium extraction.
{"title":"Sub-Nano Gaδ+ clusters confined by porous carbon spheres and coupled with SnS2 for efficient photocatalytic extraction of uranium","authors":"Yuehua Pan ,&nbsp;Yingxue Pang ,&nbsp;Hao Fu ,&nbsp;Zhenyu Cai ,&nbsp;Yuxiang Deng ,&nbsp;Zhiwei Huang ,&nbsp;Donglou Ren ,&nbsp;Yuezhou Wei ,&nbsp;Xinpeng Wang","doi":"10.1016/j.seppur.2025.132195","DOIUrl":"10.1016/j.seppur.2025.132195","url":null,"abstract":"<div><div>Extracting uranium from uranium waste streams, particularly utilizing zero-carbon emission photochemistry, emerges as a promising and sustainable strategy. Herein, we construct an SS@Ga/PCS composite photocatalyst, consisting of SnS<sub>2</sub> nanosheets as well as a metal − support produced by confining sub-nano Ga<sup>δ+</sup> clusters in the hollow porous carbon spheres (PCS). The Ga<sup>δ+</sup> clusters are innovatively introduced as active sites with localized hole capability to simultaneously improve visible light response and carrier separation. In-situ characterizations and theoretical calculations reveal that Ga<sup>δ+</sup> clusters induced metal-support interaction (MSI) by optimizing the electronic structure in the PCS host; In addition, Ga<sup>δ+</sup> clusters act as plasma excitation elements to enhance the visible light responsiveness and carrier separation of SS@Ga/PCS. Ultimately, the inhomogeneous photocatalysis of uranium extraction achieved superior performance as compared to the pure components, corresponding to an encouraging removal rate of 97.87 % and a photo-extraction capacity of up to 1867.30 mg g<sup>−1</sup> in 50 mL of uranium waste solution, as well as a wide-concentration window adaptability and excellent catalytic robustness. More significantly, this ingenious nano-confined strategy extends the design ideas of highly dispersed sub-nanometallic cluster co-catalysts and stimulates the study of the availability of abundant reactive active sites combined with monomer strong interactions, which provides a novel insight into the mechanism of photocatalytic uranium extraction.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132195"},"PeriodicalIF":8.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471046","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}
引用次数: 0
Recent progress on customizable multi-dimensional carbon-supported metal–organic frameworks (Cx/MOFs) composites for efficient adsorption of gases and vapors
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132203
Weiqiu Huang , Yuning Li , Xufei Li , Zhaoqiang Zhang , Yuhao Lu , Mingguo Peng , Xinya Wang , Yankang Zhou
Metal-organic frameworks (MOFs), a novel adsorbent with ultra-high porosity, customizable pore size and chemistry, have gained wide attentions for adsorbing and separating gases and vapors. However, some parent MOFs are usually unsatisfied when facing the complex environmental conditions, such as humidity, gas/vapor mixtures. To break these dilemmas, multi-dimensional carbon, 1D carbon nanotube (CNT), 2D graphene (GR), 3D porous carbon (PC), supported MOFs composites (Cx/MOFs, x termed as the dimension of carbon) have been developed. In this review, the types and synthetic strategies of Cx/MOFs are distinguished and classified based on the dimension and function of Cx, respectively, and the assessment methods are also put forward to identify the compounds or composites. Due to the synthetic effect between Cx and MOFs, the resulted Cx/MOFs composites not only enhanced the water stability of pristine MOFs, but also regenerated additional characteristics like customized pores around interfaces, which further improved the adsorption and separation abilities for gases and vapors, such as greenhouse gases (CO2, CH4), fuel gases (CH4, H2), toxic gases and vapors (SO2, H2S, NH3 and various condensative volatile organic compounds (VOCs)). In addition, the future prospects in the fields of adsorption and separation on Cx/MOFs are emphasized and pictured.
{"title":"Recent progress on customizable multi-dimensional carbon-supported metal–organic frameworks (Cx/MOFs) composites for efficient adsorption of gases and vapors","authors":"Weiqiu Huang ,&nbsp;Yuning Li ,&nbsp;Xufei Li ,&nbsp;Zhaoqiang Zhang ,&nbsp;Yuhao Lu ,&nbsp;Mingguo Peng ,&nbsp;Xinya Wang ,&nbsp;Yankang Zhou","doi":"10.1016/j.seppur.2025.132203","DOIUrl":"10.1016/j.seppur.2025.132203","url":null,"abstract":"<div><div>Metal-organic frameworks (MOFs), a novel adsorbent with ultra-high porosity, customizable pore size and chemistry, have gained wide attentions for adsorbing and separating gases and vapors. However, some parent MOFs are usually unsatisfied when facing the complex environmental conditions, such as humidity, gas/vapor mixtures. To break these dilemmas, multi-dimensional carbon, 1D carbon nanotube (CNT), 2D graphene (GR), 3D porous carbon (PC), supported MOFs composites (C<sub>x</sub>/MOFs, x termed as the dimension of carbon) have been developed. In this review, the types and synthetic strategies of C<sub>x</sub>/MOFs are distinguished and classified based on the dimension and function of C<sub>x</sub>, respectively, and the assessment methods are also put forward to identify the compounds or composites. Due to the synthetic effect between C<sub>x</sub> and MOFs, the resulted C<sub>x</sub>/MOFs composites not only enhanced the water stability of pristine MOFs, but also regenerated additional characteristics like customized pores around interfaces, which further improved the adsorption and separation abilities for gases and vapors, such as greenhouse gases (CO<sub>2</sub>, CH<sub>4</sub>), fuel gases (CH<sub>4</sub>, H<sub>2</sub>), toxic gases and vapors (SO<sub>2</sub>, H<sub>2</sub>S, NH<sub>3</sub> and various condensative volatile organic compounds (VOCs)). In addition, the future prospects in the fields of adsorption and separation on C<sub>x</sub>/MOFs are emphasized and pictured.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132203"},"PeriodicalIF":8.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471084","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}
引用次数: 0
Surface sulfur functionalized defects on the synergistic and competitive effects of CO2 and H2O adsorption: Density functional theory study
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132191
Bin Zhou, Tai Feng, Dingtong Liu, Hao Wang, Yueyang Wang, Cuiping Wang, Jun Li
Heteroatom doping can significantly enhance the CO2 adsorption capacity of carbon-based materials, but it also increases the hydrophilicity of the carbon matrix. This can lead to the competitive adsorption of CO2 and H2O becoming more pronounced in humid environments. In this study, the co-adsorption behaviors of H2O and CO2 on carbon surfaces modified with various sulfur functional groups were investigated at the molecular level using density functional theory. The adsorption mechanisms were comprehensively analyzed through IGMH, QTAIM, EDA-FF, and charge transfer analysis. ESP analysis revealed that the absolute values of the local maxima and minima of the water molecules’ electrostatic potential were higher than those of CO2, indicating that water molecules exhibit greater adsorption stability and hydrogen bonding capability on highly polar functional groups. QTAIM analysis identified the specific interaction pathways and strengths between the atoms of CO2 and H2O, while IGMH analysis showed that the interactions between CO2, H2O, and the porous carbon are primarily weak van der Waals forces. EDA-FF results indicate that electrostatic and dispersive interactions are the dominant forces in the co-adsorption of CO2 and H2O. The enhanced adsorption stability of CO2 in the co-adsorption system is mainly due to the additional unsaturated carbon sites created by basal defects, which significantly strengthen the van der Waals interactions of CO2. Additionally, hydrogen bonding between CO2 and H2O further promotes CO2 adsorption energy. This study underscores the critical role of sulfur functionalization in modulating adsorption behavior on carbon surfaces and provides valuable theoretical insights for designing advanced adsorbent materials capable of synergistically adsorbing multi-component gases.
掺杂杂原子可显著提高碳基材料的二氧化碳吸附能力,但同时也会增加碳基质的亲水性。这可能导致二氧化碳和水的竞争吸附在潮湿环境中变得更加明显。本研究采用密度泛函理论,在分子水平上研究了经各种硫官能团修饰的碳表面对 H2O 和 CO2 的共吸附行为。通过 IGMH、QTAIM、EDA-FF 和电荷转移分析全面分析了吸附机理。ESP 分析表明,水分子静电势的局部最大值和最小值的绝对值均高于 CO2,这表明水分子在高极性官能团上表现出更高的吸附稳定性和氢键能力。QTAIM 分析确定了 CO2 和 H2O 原子间的特定相互作用途径和强度,而 IGMH 分析表明 CO2、H2O 和多孔碳之间的相互作用主要是弱范德华力。EDA-FF 结果表明,静电作用和分散作用是 CO2 和 H2O 共吸附的主要作用力。共吸附体系中 CO2 吸附稳定性增强的主要原因是基底缺陷产生了额外的不饱和碳位点,从而大大加强了 CO2 的范德华相互作用。此外,CO2 和 H2O 之间的氢键作用也进一步提高了 CO2 的吸附能。这项研究强调了硫功能化在调节碳表面吸附行为中的关键作用,并为设计能够协同吸附多组分气体的先进吸附材料提供了宝贵的理论见解。
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引用次数: 0
Efficient removal of emulsified oil from water by lipase functionalized bio-catalytic graphene oxide sponges 利用脂肪酶功能化生物催化氧化石墨烯海绵高效去除水中的乳化油
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132241
Mahsa Moayedi, Yalda Majooni, Nariman Yousefi
Conventional water treatment methods struggle to tackle the oil contamination in the form of resilient emulsified droplets, measuring less than 20 μm in wastewater, due to their robust stability. The absence of economically feasible technologies capable of managing these small oil droplets leads to their prolonged existence in water, causing drastic impact on marine life, ecosystem, and public health. As such, there is an urgent need for advanced technologies capable of efficiently removing emulsified oil droplets with minimal residue. The main reason for emulsion stability is the interaction between surfactants and the oil–water interfaces. In this study, we biologically degraded surfactants to disrupt the interfacial layer between water and oil droplets, ultimately leading to destabilizing the highly stable emulsions. We combined the biocatalytic activity of lipase with the high adsorption capacity of reduced graphene oxide (rGO) to treat highly stable emulsified oil. Lipase activity was enhanced after being immobilized on the hydrophobic rGO sponges, compared to its free form, due to the enzyme structural changes. Our results demonstrate that the immobilized lipase effectively degraded the emulsion stabilizer (Tween 20), while the generated metabolites and combined oil droplets were adsorbed by the highly adsorptive rGO sponges. These synergistic mechanisms resulted in more than 96 % removal of emulsified crude oil.
传统的水处理方法难以处理废水中小于 20 μm 的弹性乳化油滴形式的油类污染,因为它们具有很强的稳定性。由于缺乏经济可行的技术来管理这些小油滴,导致它们长期存在于水中,对海洋生物、生态系统和公众健康造成严重影响。因此,迫切需要能够有效去除乳化油滴并将残留物降至最低的先进技术。乳液稳定性的主要原因是表面活性剂与油水界面之间的相互作用。在这项研究中,我们通过生物降解表面活性剂来破坏水和油滴之间的界面层,最终导致高度稳定的乳液失去稳定性。我们将脂肪酶的生物催化活性与还原氧化石墨烯(rGO)的高吸附能力相结合,处理高度稳定的乳化油。由于酶的结构发生了变化,与游离态相比,固定在疏水性 rGO 海绵上的脂肪酶活性得到了增强。我们的研究结果表明,固定化脂肪酶能有效降解乳化稳定剂(吐温 20),而生成的代谢物和组合油滴则被吸附性极强的 rGO 海绵吸附。这些协同机制使乳化原油的去除率超过 96%。
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引用次数: 0
Algal carbon quantum dots/Bi2MoO6 S-scheme heterojunction with enhanced visible-light photocatalytic degradation for ciprofloxacin
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132196
Jiaxin Liu, Lili Ji, Qianrui He, Shaohong Zang, Jiaxing Sun, Hao Yang, Teng Dong, Tongxin Liu, Huihui Wu, Xingyu Chen, Zebin Zhong, Xu Deng
The formation of S-scheme heterojunctions offers a viable strategy for enhancing photocatalytic efficiency in tackling organic contaminants. However, the green, low-cost, easy-to-synthesize S-scheme heterojunction is critical to further large-scale production. In this study, we successfully developed a new, eco-friendly, and cost-effective S-scheme heterojunction photocatalyst, Carbon quantum dots prepared from Sargassum horneri / Bi2MoO6 (SCQDs/BMO) utilizing an in-situ hydrothermal method. Carbon quantum dots derived from marine macroalga Sargassum horneri (SCQDs) are integrated with Bi2MoO6 semiconductors to formulate the groundbreaking catalytic material. The results affirm that SCQDs’ incorporation generated an internal electric field (IEF) at SCQDs-BMO interfaces, significantly enhancing charge separation. Moreover, SCQDs act as electron capturers to enhance carrier separation. At the same time, during the composite process, the carbon dots can reduce Bi3+ to Bi0. The high conductivity of Bi further enhances the electron transport capability of the system, working synergistically with the internal electric field to promote the separation and migration of charge carriers. This optimization improves the interfacial charge transfer pathway between BMO and SCQDs. Thus, SCQDs/BMO exhibits superior photocatalytic degradation for ciprofloxacin (CIP) under visible light, up to 97.7 % in 180 min, whose rate constant is 2.6 times that of BMO. The primary active agents, including ·O2/·OH, produced on the surface of SCQDs/BMO are crucial in the photodegradation of CIP. The potential intermediates, degradation pathways, and underlying mechanisms have been clearly outlined. This study offers an efficient and environmentally friendly method of developing high-activity S-scheme heterojunction photocatalysts for treating antibiotics wastewater.
S 型异质结的形成为提高光催化处理有机污染物的效率提供了一种可行的策略。然而,绿色、低成本、易合成的 S 型异质结对于进一步的大规模生产至关重要。在这项研究中,我们利用原位水热法成功开发出了一种新型、环保、高性价比的 S 型异质结光催化剂--从马尾藻中制备的碳量子点/Bi2MoO6(SCQDs/BMO)。从海洋大型藻类马尾藻(Sargassum horneri)中提取的碳量子点(SCQDs)与 Bi2MoO6 半导体相结合,形成了突破性的催化材料。研究结果表明,SCQDs 的加入在 SCQDs-BMO 界面产生了内电场 (IEF),显著增强了电荷分离。此外,SCQDs 还可作为电子捕获器,增强载流子分离。同时,在复合过程中,碳点可以将 Bi3+ 还原成 Bi0。Bi 的高导电性进一步增强了系统的电子传输能力,与内部电场协同作用,促进电荷载流子的分离和迁移。这种优化改善了 BMO 和 SCQD 之间的界面电荷转移途径。因此,在可见光条件下,SCQDs/BMO 对环丙沙星(CIP)的光催化降解效果显著,180 分钟内降解率高达 97.7%,其速率常数是 BMO 的 2.6 倍。SCQDs/BMO 表面产生的主要活性剂(包括 -O2-/-OH)是 CIP 光降解的关键。研究清楚地概述了潜在的中间产物、降解途径和基本机制。这项研究为开发用于处理抗生素废水的高活性 S 型异质结光催化剂提供了一种高效、环保的方法。
{"title":"Algal carbon quantum dots/Bi2MoO6 S-scheme heterojunction with enhanced visible-light photocatalytic degradation for ciprofloxacin","authors":"Jiaxin Liu, Lili Ji, Qianrui He, Shaohong Zang, Jiaxing Sun, Hao Yang, Teng Dong, Tongxin Liu, Huihui Wu, Xingyu Chen, Zebin Zhong, Xu Deng","doi":"10.1016/j.seppur.2025.132196","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132196","url":null,"abstract":"The formation of S-scheme heterojunctions offers a viable strategy for enhancing photocatalytic efficiency in tackling organic contaminants. However, the green, low-cost, easy-to-synthesize S-scheme heterojunction is critical to further large-scale production. In this study, we successfully developed a new, eco-friendly, and cost-effective S-scheme heterojunction photocatalyst, Carbon quantum dots prepared from <em>Sargassum horneri</em> / Bi<sub>2</sub>MoO<sub>6</sub> (SCQDs/BMO) utilizing an in-situ hydrothermal method. Carbon quantum dots derived from marine macroalga <em>Sargassum horneri</em> (SCQDs) are integrated with Bi<sub>2</sub>MoO<sub>6</sub> semiconductors to formulate the groundbreaking catalytic material. The results affirm that SCQDs’ incorporation generated an internal electric field (IEF) at SCQDs-BMO interfaces, significantly enhancing charge separation. Moreover, SCQDs act as electron capturers to enhance carrier separation. At the same time, during the composite process, the carbon dots can reduce Bi<sup>3+</sup> to Bi<sup>0</sup>. The high conductivity of Bi further enhances the electron transport capability of the system, working synergistically with the internal electric field to promote the separation and migration of charge carriers. This optimization improves the interfacial charge transfer pathway between BMO and SCQDs. Thus, SCQDs/BMO exhibits superior photocatalytic degradation for ciprofloxacin (CIP) under visible light, up to 97.7 % in 180 min, whose rate constant is 2.6 times that of BMO. The primary active agents, including ·O<sub>2</sub><sup>−</sup>/·OH, produced on the surface of SCQDs/BMO are crucial in the photodegradation of CIP. The potential intermediates, degradation pathways, and underlying mechanisms have been clearly outlined. This study offers an efficient and environmentally friendly method of developing high-activity S-scheme heterojunction photocatalysts for treating antibiotics wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"30 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143473401","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}
引用次数: 0
The influence mechanism of cross-linking agent relative molecular mass on in-situ cross-linking in PES membrane matrix
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132199
Zhiyao Du , Hao Zhang , Jingguo She , Jiahui Li , Haifu Gao , Ziping Song , Wangwang Guan , Hongjin Yan , Chunrui Wu , Xiaolong Lu
In this paper, three cross-linking agents with varying relative molecular mass (RMM) were used to initiate in-situ cross-linking reaction in polyether sulfone (PES) membrane matrix, novel PES membranes were prepared through non-solvent induced phase separation (NIPS). Thereafter, the mechanism underlying cross-linking agent RMM’s influence on membrane structure and properties was analyzed. The results indicated that for the same proportion of dope solution system, cross-linking agents with smaller RMM will have more molar mass epoxy groups participating in the ring-opening reaction, which can form more hydroxyl groups in the subsequent cross-linking reaction, leading to a significant improvement in the hydrophilicity of PES membrane. Meanwhile, system with lower RMM of cross-linking agent had faster double diffusion rate in phase separation, and the larger most probable pore size formed in our modified membrane will further improve the permeation flux. The cross-linking network generated by the membrane formation system with low RMM of the cross-linking agent was more complete, and this modified membrane had a tensile strength maintained at 3.5Mpa. Relative to the original PES membrane, our optimal modified membrane has fourfold increased permeation flux, reaching 667.8 L·m−2·h−1. Meanwhile, BSA rejection of the membrane can be maintained at 96.7 %. Our modified membrane has improved antifouling efficiency, exhibiting persistent hydrophilicity during the 21-day washing experiment.
本文采用三种不同相对分子质量(RMM)的交联剂在聚醚砜(PES)膜基中引发原位交联反应,通过非溶剂诱导相分离(NIPS)制备了新型 PES 膜。随后,分析了交联剂 RMM 对膜结构和性能的影响机理。结果表明,在相同比例的掺杂溶液体系中,RMM 较小的交联剂会有更多摩尔质量的环氧基团参与开环反应,从而在后续的交联反应中形成更多的羟基,使 PES 膜的亲水性显著提高。同时,交联剂 RMM 较低的体系在相分离中的双重扩散速度更快,而改性膜形成的更大的最可能孔径将进一步提高渗透通量。交联剂 RMM 较低的成膜体系生成的交联网络更完整,改性膜的抗拉强度保持在 3.5 兆帕。与原始 PES 膜相比,我们的最佳改性膜的渗透通量提高了四倍,达到 667.8 L-m-2-h-1。同时,膜对 BSA 的排斥率可保持在 96.7%。我们的改性膜提高了防污效率,在 21 天的洗涤实验中表现出持久的亲水性。
{"title":"The influence mechanism of cross-linking agent relative molecular mass on in-situ cross-linking in PES membrane matrix","authors":"Zhiyao Du ,&nbsp;Hao Zhang ,&nbsp;Jingguo She ,&nbsp;Jiahui Li ,&nbsp;Haifu Gao ,&nbsp;Ziping Song ,&nbsp;Wangwang Guan ,&nbsp;Hongjin Yan ,&nbsp;Chunrui Wu ,&nbsp;Xiaolong Lu","doi":"10.1016/j.seppur.2025.132199","DOIUrl":"10.1016/j.seppur.2025.132199","url":null,"abstract":"<div><div>In this paper, three cross-linking agents with varying relative molecular mass (RMM) were used to initiate in-situ cross-linking reaction in polyether sulfone (PES) membrane matrix, novel PES membranes were prepared through non-solvent induced phase separation (NIPS). Thereafter, the mechanism underlying cross-linking agent RMM’s influence on membrane structure and properties was analyzed. The results indicated that for the same proportion of dope solution system, cross-linking agents with smaller RMM will have more molar mass epoxy groups participating in the ring-opening reaction, which can form more hydroxyl groups in the subsequent cross-linking reaction, leading to a significant improvement in the hydrophilicity of PES membrane. Meanwhile, system with lower RMM of cross-linking agent had faster double diffusion rate in phase separation, and the larger most probable pore size formed in our modified membrane will further improve the permeation flux. The cross-linking network generated by the membrane formation system with low RMM of the cross-linking agent was more complete, and this modified membrane had a tensile strength maintained at 3.5Mpa. Relative to the original PES membrane, our optimal modified membrane has fourfold increased permeation flux, reaching 667.8 L·m<sup>−2</sup>·h<sup>−1</sup>. Meanwhile, BSA rejection of the membrane can be maintained at 96.7 %. Our modified membrane has improved antifouling efficiency, exhibiting persistent hydrophilicity during the 21-day washing experiment.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132199"},"PeriodicalIF":8.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470841","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}
引用次数: 0
Construction of a novel dual-cathode flow-through heterogeneous electro-Fenton system for enhanced mass transfer during H2O2 production and activation in cefoperazone degradation
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132235
Chaoran Shao, Songyu Ren, Yanyu Zhang, Zhenjun Wen, Aimin Wang, Zhongguo Zhang
To accelerate the feasibility and practical considerations of the in situ generated H2O2, a sequential dual-cathode heterogeneous electro-Fenton (HEF) system was implemented for various pollutants degradation, in which an activated carbon fiber (ACF) cathode was used to produce H2O2 in situ and an FeOCl nanosheets loaded onto ACF felt (ACF@FeOCl) cathode was employed to accelerate reactive oxygen species (ROS) generation by activating H2O2. A novel flow-through dual-cathode HEF system was utilized by using an ACF cathode for H2O2 production and an FeOCl nanosheets loaded onto ACF felt (ACF@FeOCl) cathode for simultaneously producing and activating H2O2. The sequential dual-cathode system can generate 711.6 μM OH via in situ produce H2O2 and completely degrade antibiotic cefoperazone (CFPZ) at neutral pH, achieving a 50 mg L−1 CFPZ removal of 100.0 % within 60 min and TOC removal of 60.0 % within 180 min. The electron spin resonance (ESR) spectrum and radical quenching tests certified that the predominant ROS were OH and 1O2 responsible for CFPZ degradation. Notably, over 10 cycles the degradation rate maintained at 100.0 % within 60 min, while the TOC removal efficiency only decreasing from 60.0 % to 51.6 % after 180 min. The UPLC-QQQ-MS results and density functional theory (DFT) was employed to propose reasonable degradation pathways of CFPZ. Ultimately, the toxicological simulation via ECOSAR assessment revealed that the toxicity of the intermediate products during CFPZ degradation appeared a declining trend. These findings collectively demonstrate that the ACF/ACF@FeOCl-HEF system was an efficient and cost-effective technology by in situ electrocatalytic synthesis of H2O2 and the activation of H2O2 to yield reactive oxygen species for the treatment of recalcitrant organic contaminants.
{"title":"Construction of a novel dual-cathode flow-through heterogeneous electro-Fenton system for enhanced mass transfer during H2O2 production and activation in cefoperazone degradation","authors":"Chaoran Shao, Songyu Ren, Yanyu Zhang, Zhenjun Wen, Aimin Wang, Zhongguo Zhang","doi":"10.1016/j.seppur.2025.132235","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132235","url":null,"abstract":"To accelerate the feasibility and practical considerations of the in situ generated H<sub>2</sub>O<sub>2</sub>, a sequential dual-cathode heterogeneous electro-Fenton (HEF) system was implemented for various pollutants degradation, in which an activated carbon fiber (ACF) cathode was used to produce H<sub>2</sub>O<sub>2</sub> in situ and an FeOCl nanosheets loaded onto ACF felt (ACF@FeOCl) cathode was employed to accelerate reactive oxygen species (ROS) generation by activating H<sub>2</sub>O<sub>2</sub>. A novel flow-through dual-cathode HEF system was utilized by using an ACF cathode for H<sub>2</sub>O<sub>2</sub> production and an FeOCl nanosheets loaded onto ACF felt (ACF@FeOCl) cathode for simultaneously producing and activating H<sub>2</sub>O<sub>2</sub>. The sequential dual-cathode system can generate 711.6 μM <sup>•</sup>OH via in situ produce H<sub>2</sub>O<sub>2</sub> and completely degrade antibiotic cefoperazone (CFPZ) at neutral pH, achieving a 50 mg L<sup>−1</sup> CFPZ removal of 100.0 % within 60 min and TOC removal of 60.0 % within 180 min. The electron spin resonance (ESR) spectrum and radical quenching tests certified that the predominant ROS were <sup>•</sup>OH and <sup>1</sup>O<sub>2</sub> responsible for CFPZ degradation. Notably, over 10 cycles the degradation rate maintained at 100.0 % within 60 min, while the TOC removal efficiency only decreasing from 60.0 % to 51.6 % after 180 min. The UPLC-QQQ-MS results and density functional theory (DFT) was employed to propose reasonable degradation pathways of CFPZ. Ultimately, the toxicological simulation via ECOSAR assessment revealed that the toxicity of the intermediate products during CFPZ degradation appeared a declining trend. These findings collectively demonstrate that the ACF/ACF@FeOCl-HEF system was an efficient and cost-effective technology by in<!-- --> <!-- -->situ electrocatalytic synthesis of H<sub>2</sub>O<sub>2</sub> and the activation of H<sub>2</sub>O<sub>2</sub> to yield reactive oxygen species for the treatment of recalcitrant organic contaminants.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"37 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471047","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}
引用次数: 0
Adsorptive membranes of cellulose acetate CA/SiO2/UiO-66(Zr) for the removal of protein bound uremic toxins 用于去除与蛋白质结合的尿毒症毒素的醋酸纤维素 CA/SiO2/UiO-66(Zr) 吸附膜
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132244
Diogo dos Reis Barradas, Moisés Luzia Pinto, Maria Norberta de Pinho, Miguel Minhalma
One of the strong limitations of hemodialysis is the fact that protein bound uremic toxins (PBUTs), such as p-Cresyl Sulfate (pCS), are not filtered out, remaining in the patient’s bloodstream, leading to a worsening of the chronic kidney disease (CKD).In the present work, the MOF (Metal Organic Framework) UiO-66(Zr) is incorporated into CA/SiO2 membranes in order to increase their capacity to remove uremic toxins, that preferentially bind to plasma proteins, such as pCS. The casting solutions for membrane synthesis by phase inversion combined with sol–gel method are prepared with 1%, 1.5%, 2% and 2.5% of MOF to yield CA22/SiO2 membranes with these contents.The four membranes containing increasing MOF contents showed an increase of hydraulic permeability ranging from 14.38 to 33.82 kg/h/m2/bar and of molecular weight cut-off ranging from 3.5 to 14.7 kDa.Adsorption isotherms were constructed at 37 °C for pCS on UiO-66(Zr) and on Bovine Serum Albumin (BSA) and for all the four membranes incorporating MOF. It was concluded that the membrane adsorption, per MOF mass, decreases with increasing MOF content. The Langmuir and Freundlich parameters were calculated for each case. Finally, a last adsorption isotherm was carried out on pCS in the presence of both UiO-66(Zr) and BSA, where with 5 mg/mL of UiO-66(Zr) it was possible to reduce the bounding of the toxin to the protein by around 50 %.
{"title":"Adsorptive membranes of cellulose acetate CA/SiO2/UiO-66(Zr) for the removal of protein bound uremic toxins","authors":"Diogo dos Reis Barradas, Moisés Luzia Pinto, Maria Norberta de Pinho, Miguel Minhalma","doi":"10.1016/j.seppur.2025.132244","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132244","url":null,"abstract":"One of the strong limitations of hemodialysis is the fact that protein bound uremic toxins (PBUTs), such as p-Cresyl Sulfate (pCS), are not filtered out, remaining in the patient’s bloodstream, leading to a worsening of the chronic kidney disease (CKD).In the present work, the MOF (Metal Organic Framework) UiO-66(Zr) is incorporated into CA/SiO<sub>2</sub> membranes in order to increase their capacity to remove uremic toxins, that preferentially bind to plasma proteins, such as pCS. The casting solutions for membrane synthesis by phase inversion combined with sol–gel method are prepared with 1%, 1.5%, 2% and 2.5% of MOF to yield CA22/SiO<sub>2</sub> membranes with these contents.The four membranes containing increasing MOF contents showed an increase of hydraulic permeability ranging from 14.38 to 33.82 kg/h/m<sup>2</sup>/bar and of molecular weight cut-off ranging from 3.5 to 14.7 kDa.Adsorption isotherms were constructed at 37 °C for pCS on UiO-66(Zr) and on Bovine Serum Albumin (BSA) and for all the four membranes incorporating MOF. It was concluded that the membrane adsorption, per MOF mass, decreases with increasing MOF content. The Langmuir and Freundlich parameters were calculated for each case. Finally, a last adsorption isotherm was carried out on pCS in the presence of both UiO-66(Zr) and BSA, where with 5 mg/mL of UiO-66(Zr) it was possible to reduce the bounding of the toxin to the protein by around 50 %.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"13 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471088","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}
引用次数: 0
Enhancing antifouling and catalytic cleaning Abilities of fabrics for efficient Oil-Water separation
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132239
Zhiying He, Xiran Yang, Zhibin Zeng, Junjie Zheng, Xu Guo, Mei Zhu, Wei Chen, Haokun Zhang, Qing Xu, Qian Zhang, Peng Zhao, Lin Chen, Sudong Yang, Ya Liu
Efficient oil–water separation is critical for environmental sustainability, yet conventional materials often lack the dual antifouling and catalytic self-cleaning capabilities required for long-term performance. This study introduces a novel approach by engineering a biomimetic polyacrylonitrile (PAN)/MnO2 composite fabric through in situ hydrothermal growth of MnO2 nanosheets, creating a hierarchical micro/nanostructure inspired by natural systems. This design uniquely integrates passive antifouling (via superhydrophilic surface and microbubble-induced repulsion) with active catalytic cleaning driven by reactive oxygen species (ROS) generated during hydrogen peroxide decomposition. The composite fabric achieves remarkable separation performance under gravity: a “water-removing” flux of 29,806.4 L m–2h–1 and an “oil-removing” flux of 3,580.4 L m–2h–1, while maintaining > 99.8 % oil rejection efficiency across diverse oil–water mixtures. Crucially, the synergistic passive-active antifouling mechanism effectively mitigates irreversible fouling, a persistent challenge in conventional membranes. This work advances catalytic self-cleaning technologies by demonstrating how biomimetic structural design and multifunctional chemistry can synergize to address complex oil–water separation challenges, offering a transformative solution for environmental remediation.
{"title":"Enhancing antifouling and catalytic cleaning Abilities of fabrics for efficient Oil-Water separation","authors":"Zhiying He, Xiran Yang, Zhibin Zeng, Junjie Zheng, Xu Guo, Mei Zhu, Wei Chen, Haokun Zhang, Qing Xu, Qian Zhang, Peng Zhao, Lin Chen, Sudong Yang, Ya Liu","doi":"10.1016/j.seppur.2025.132239","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132239","url":null,"abstract":"Efficient oil–water separation is critical for environmental sustainability, yet conventional materials often lack the dual antifouling and catalytic self-cleaning capabilities required for long-term performance. This study introduces a novel approach by engineering a biomimetic polyacrylonitrile (PAN)/MnO<sub>2</sub> composite fabric through in situ hydrothermal growth of MnO<sub>2</sub> nanosheets, creating a hierarchical micro/nanostructure inspired by natural systems. This design uniquely integrates passive antifouling (via superhydrophilic surface and microbubble-induced repulsion) with active catalytic cleaning driven by reactive oxygen species (ROS) generated during hydrogen peroxide decomposition. The composite fabric achieves remarkable separation performance under gravity: a “water-removing” flux of 29,806.4 L m<sup>–2</sup>h<sup>–1</sup> and an “oil-removing” flux of 3,580.4 L m<sup>–2</sup>h<sup>–1</sup>, while maintaining &gt; 99.8 % oil rejection efficiency across diverse oil–water mixtures. Crucially, the synergistic passive-active antifouling mechanism effectively mitigates irreversible fouling, a persistent challenge in conventional membranes. This work advances catalytic self-cleaning technologies by demonstrating how biomimetic structural design and multifunctional chemistry can synergize to address complex oil–water separation challenges, offering a transformative solution for environmental remediation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"65 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471104","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}
引用次数: 0
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Separation and Purification Technology
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