Separation and Purification Technology最新文献

Catalytic combustion of propane over second metal-modified Ru supported on CeO2 nanosheet 在 CeO2 纳米片支撑的第二金属改性 Ru 上催化燃烧丙烷

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-29 DOI: 10.1016/j.seppur.2024.129874

Among the CeO₂ supported noble metal catalysts, Ru/CeO₂ shows the highest activity for propane combustion. However, Ru/CeO₂ catalysts still exhibit some problems such as poor thermal stability and high temperature volatilization loss of Ru species. In this work, based on electronic structure modification and acid-base-redox property regulation, the active Ru component in Ru/CeO₂ was modified with a second element to prepare for propane (C₃H₈) combustion. Activity test and characterizations illustrated that all the selected elements reduce the C₃H₈ combustion activity due to a corresponding reduction in active Ru-O-Ce species. With the addition of Cs with strong electron-donating leads to the stabilization of Ce³⁺ within the CeO₂, consequently diminishing its redox capabilities thus exhibits suboptimal activity and stability. However, the moderately electron-donating alkaline earth metal Ba stabilizes the low-cost Ru species and improves the thermal stability. In contrast, the strongly electron-withdrawing element Nb reduces the stability of low-valence Ru species and leads to the easy loss of Ru at high temperatures. However, the prepared NbRu/CeO₂ catalyst shows better resistance to chlorine poisoning and CO₂ due to the enhancement of acidity. Finally, the reaction pathway for propane oxidation was thoroughly investigated by in-situ DRIFTS over the modified Ru/CeO₂ catalysts. The addition of Cs improves Ru′ dispersion, which in turn facilitates the oxidation of propane to propanol. With the addition of Ba, the conversion of carboxylic acid species to acid ester species is accelerated. While the addition of Nb lead to a decrease in the variety of adsorbates.

在 CeO2 支持的贵金属催化剂中，Ru/CeO2 对丙烷燃烧的活性最高。然而，Ru/CeO2 催化剂仍然存在一些问题，如热稳定性差和高温下 Ru 物种挥发损失。在这项工作中，基于电子结构修饰和酸碱氧化还原特性调节，用第二种元素修饰了 Ru/CeO2 中的活性 Ru 成分，为丙烷（C3H8）燃烧做准备。活性测试和表征结果表明，由于活性 Ru-O-Ce 物种的相应减少，所有选定元素都会降低 C3H8 的燃烧活性。加入强电子负载的 Cs 会导致 Ce3+ 稳定在 CeO2 中，从而削弱其氧化还原能力，使其活性和稳定性都不理想。然而，中等电子负载的碱土金属 Ba 能稳定低成本的 Ru 物种，并提高热稳定性。相反，强吸电子元素 Nb 会降低低价 Ru 物种的稳定性，并导致 Ru 在高温下容易流失。不过，由于酸性增强，制备的 NbRu/CeO2 催化剂对氯中毒和 CO2 的耐受性更好。最后，通过在改性 Ru/CeO2 催化剂上进行原位 DRIFTS，对丙烷氧化的反应途径进行了深入研究。Cs 的加入改善了 Ru′ 的分散，从而促进了丙烷氧化成丙醇。加入 Ba 后，羧酸类物质向酸酯类物质的转化速度加快。而添加 Nb 会导致吸附剂种类减少。

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引用次数: 0

The enhanced mechanism of ZnIn2S4-CoFe2O4-BC activated peroxomonosulfate under visible light for the degradation of fluoroquinolones 可见光下 ZnIn2S4-CoFe2O4-BC 活化过硫酸单胞菌降解氟喹诺酮类药物的增强机制

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-29 DOI: 10.1016/j.seppur.2024.129927

Visible light is a sustainable method for activation peroxomonosulfate (PMS). In this study, the ZnIn₂S₄-CoFe₂O₄-BC (ZIS-CFO-BC) composite photocatalytic material was synthesized by two-step hydrothermal and solvothermal methods to enhanced the efficiency of sunlight utilization. The morphology analysis revealed ZIS and CFO particles are uniformly dispersed on the Biochar (BC) surface, forming a stable heterojunction interface. A 96.39 % removal of enrofloxacin (ENR, 2 mg/L) was achieved within a 30 min period by the Vis/ZIS-CFO-BC system. According to the quenching and EPR tests, SO₄^•−, h⁺, •OH, and ¹O₂ were identified as the primary active species. Valence changes were observed for both Co and Fe, indicating that this is primary site for PMS activation. The findings of the cycling and co-existing ions experiments illustrate that ZIS-CFO-BC exhibits remarkable potential for various applications. This research presents a new recyclable green material that efficiently utilizes sunlight to enhance the Fenton-like system.

可见光是活化过硫酸盐（PMS）的一种可持续方法。本研究采用水热法和溶解热法两步合成了 ZnIn2S4-CoFe2O4-BC （ZIS-CFO-BC）复合光催化材料，以提高太阳光的利用效率。形貌分析表明，ZIS 和 CFO 颗粒均匀地分散在生物炭（BC）表面，形成了稳定的异质结界面。在 30 分钟内，Vis/ZIS-CFO-BC 系统对恩诺沙星（ENR，2 mg/L）的去除率达到 96.39%。根据淬灭和 EPR 测试，确定 SO4--、h+、-OH 和 1O2 为主要活性物种。Co 和 Fe 的价态都发生了变化，表明这是 PMS 活化的主要部位。循环和共存离子实验的结果表明，ZIS-CFO-BC 在各种应用领域都具有显著的潜力。这项研究提出了一种新型可回收绿色材料，它能有效利用阳光来增强类似芬顿的系统。

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引用次数: 0

Techno-economic insights into one-pot bacterial astaxanthin extraction and sustainable therapeutic product development using natural solvent mixtures 利用天然混合溶剂提取单锅细菌虾青素和开发可持续治疗产品的技术经济见解

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-29 DOI: 10.1016/j.seppur.2024.129926

The increasing demand for sustainable and safe products is driving the replacement of synthetic pigments with natural alternatives in the cosmetics industry. Additionally, the use of green solvents, such as natural solvent mixtures (NaSoMix), is essential to minimize the environmental impact of extraction processes. This study explores the innovative application of NaSoMix for extracting astaxanthin-rich extracts (ARE) from the bacterium Paracoccus carotinifaciens, a promising source of natural colorants and antioxidants. By employing menthol-based natural deep eutectic solvents (NaDES) combined with bio-based solvents, viz., ethyl acetate and ethanol, the research achieved remarkable ARE extraction yields of up to 1.3 mg/mL using conventional procedures. Notably, process intensification through microwave-assisted extraction resulted in a 400 % increase in ARE recovery yields compared to traditional methods. The therapeutic soaps formulated with these ARE extracts exhibited significant antioxidant activity, achieving a 75 % reduction in DPPH• free radical signals, and maintained excellent color stability over a month, with minimal perceptual changes. Safety assessments confirmed the non-irritating properties of the therapeutic soaps, with an irritation score of 0 at low ARE concentrations. Furthermore, an economic analysis revealed a highly favorable Internal Rate of Return (IRR) of 183 % and a Return on Investment (ROI) of 2890 %, underscoring the commercial viability of this sustainable approach. Overall, this study highlights the effectiveness and safety of utilizing NaSoMix for extracting high-value compounds and formulating innovative therapeutic cosmetic products, aligning with consumer preferences for natural ingredients while promoting environmental sustainability and economic feasibility.

化妆品行业对可持续和安全产品的需求日益增长，推动了天然替代品对合成颜料的替代。此外，使用绿色溶剂（如天然混合溶剂 (NaSoMix)）对于最大限度地减少萃取过程对环境的影响至关重要。本研究探索了 NaSoMix 在从 Paracoccus carotinifaciens 细菌中提取富含虾青素的提取物 (ARE) 中的创新应用，这是一种很有前景的天然着色剂和抗氧化剂来源。通过采用薄荷醇基天然深共晶溶剂（NaDES）与生物基溶剂（即乙酸乙酯和乙醇）相结合的方法，该研究利用传统工艺实现了高达 1.3 mg/mL 的显著虾青素提取率。值得注意的是，与传统方法相比，通过微波辅助萃取强化工艺使 ARE 的回收率提高了 400%。用这些 ARE 提取物配制的治疗皂具有显著的抗氧化活性，可减少 75% 的 DPPH 自由基信号，并在一个月内保持良好的颜色稳定性，感观变化极小。安全评估证实了治疗皂的无刺激特性，在低浓度 ARE 的情况下刺激性为 0。此外，经济分析表明，该方法的内部收益率（IRR）为 183%，投资回报率（ROI）为 2890%，非常可观，凸显了这种可持续方法的商业可行性。总之，这项研究强调了利用 NaSoMix 提取高价值化合物和配制创新治疗化妆品的有效性和安全性，符合消费者对天然成分的偏好，同时促进了环境的可持续发展和经济可行性。

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引用次数: 0

Mechanochemistry assisted oxidative desulfurization of high-sulfur petroleum coke over HPMo coupled binary deep eutectic solvent 高硫石油焦在 HPMo 耦合二元深共晶溶剂上的机械化学辅助氧化脱硫过程

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129882

As the product in the coking of residual oil, the high-sulfur petroleum coke (HSPC, S > 3.0 wt%) has drawn increasing interest for the preparation of graphite electrodes in the steelmaking industry in recent years. How to effectively reduce the sulfide content of HSPC to produce low-sulfur petroleum coke (LSPC, S < 1.0 wt%) with high value is the research hotspot, but remains a huge challenge in the petroleum processing industry. Herein, a novel mechanochemistry-assisted HSPC oxidative desulfurization strategy was proposed with the amide based binary deep eutectic solvent (DES) as the extractant and solvent, and commercial grade phosphomolybdic acid (HPMo) and H₂O₂ used as catalyst and oxidant, respectively. The novelty of this method lied in the pretreatment of petroleum coke by ball milling, which increased the specific surface area of HSPC, thereby exposing more sulfur sites for the accessibility and reaction with H₂O₂ and reactive sites, and thereafter significantly enhancing the desulfurization rate of HSPC. The sulfur content of HSPC can be remarkably decreased from 4.46 wt% to 0.51 wt% under the reaction temperature of 60 °C due to the coupling effect between HPMo and DES, which represents the record-high desulfurization rate (88.6 %) and is strikingly higher that the state-of-the-art catalysts reported under the similar conditions so far. This work proposes a new avenue for design and preparation of advanced desulfurization catalyst for petroleum coke in the future.

作为渣油焦化的产物，高硫石油焦（HSPC，S > 3.0 wt%）近年来在炼钢行业制备石墨电极中越来越受到关注。如何有效降低 HSPC 中的硫化物含量，生产出高附加值的低硫石油焦（LSPC, S < 1.0 wt%）是研究的热点，但在石油加工行业仍是一个巨大的挑战。本文提出了一种新型机械化学辅助 HSPC 氧化脱硫策略，以酰胺基二元深共晶溶剂（DES）为萃取剂和溶剂，以商业级磷钼酸（HPMo）和 H2O2 分别为催化剂和氧化剂。该方法的新颖之处在于通过球磨对石油焦进行预处理，增加了 HSPC 的比表面积，从而暴露出更多的硫位点，以便与 H2O2 和反应位点进行接触和反应，从而显著提高了 HSPC 的脱硫率。由于 HPMo 与 DES 之间的耦合效应，在 60 °C 的反应温度下，HSPC 的硫含量可从 4.46 wt% 显著降至 0.51 wt%，脱硫率（88.6%）创历史新高，大大高于迄今为止在类似条件下报道的最先进催化剂。这项工作为今后设计和制备先进的石油焦脱硫催化剂开辟了一条新途径。

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引用次数: 0

Comparative study for removal of potentially toxic metals from the groundwater of Lakhanpur Area, Odisha, India by using two different hydrogels 使用两种不同水凝胶去除印度奥迪沙拉坎普尔地区地下水中潜在有毒金属的比较研究

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129915

In this work, we collected eight groundwater samples from various important locations from Lakhanpur area, Odisha, India. The concentration of various metal ions (Fe^3+, Ni^2+, Cd^2+, and Zn²⁺) present in the collected water samples was analyzed through an atomic absorption spectrometer (AAS). Two hydrogels, such as PVA/CH and PVA/AA, are synthesised by adopting sol–gel polymerization technique using CH, AA, and PVA. Both the hydrogels were characterized by using FT-IR, XRD, SEM/EDS, XPS, and TGA. We adopted suitable methodology to carry out studies on the antibacterial properties, swelling behaviour, and adsorption of the water samples. The adsorption study was done for the separation of potentially toxic metal ions at various intervals of time using two hydrogels. It was observed that the capability of adsorption rate increases with increases in adsorbent dosage and the rate of adsorption, which is faster at the initial time and then gradually decreases up to 180 min. The adsorption capacity of both hydrogels follows the order Zn²⁺ > Ni²⁺> Fe³⁺> Cd²⁺ ions. The results revealed that the adsorption capability of the PVA/CH hydrogel is higher than that of PVA/AA, signifying their use efficiently for the elimination of potentially toxic metal ions from metal-contaminated water.

在这项研究中，我们从印度奥迪沙拉坎普尔地区的多个重要地点采集了 8 个地下水样本。通过原子吸收光谱仪 (AAS) 分析了采集水样中各种金属离子（Fe3+、Ni2+、Cd2+ 和 Zn2+）的浓度。采用溶胶-凝胶聚合技术，使用 CH、AA 和 PVA 合成了两种水凝胶，如 PVA/CH 和 PVA/AA。这两种水凝胶都通过傅立叶变换红外光谱、XRD、SEM/EDS、XPS 和 TGA 进行了表征。我们采用适当的方法对水样品的抗菌特性、溶胀行为和吸附性进行了研究。吸附研究是利用两种水凝胶在不同时间间隔内分离可能有毒的金属离子。研究发现，随着吸附剂用量和吸附速率的增加，吸附速率的能力也随之增加。两种水凝胶的吸附能力依次为 Zn2+；Ni2+；Fe3+；Cd2+。结果表明，PVA/CH 水凝胶的吸附能力高于 PVA/AA 水凝胶，这表明它们可有效去除金属污染水中的潜在有毒金属离子。

{"title":"Comparative study for removal of potentially toxic metals from the groundwater of Lakhanpur Area, Odisha, India by using two different hydrogels","authors":"","doi":"10.1016/j.seppur.2024.129915","DOIUrl":"10.1016/j.seppur.2024.129915","url":null,"abstract":"<div><div>In this work, we collected eight groundwater samples from various important locations from Lakhanpur area, Odisha, India. The concentration of various metal ions (Fe<sup>3+,</sup> Ni<sup>2+,</sup> Cd<sup>2+,</sup> and Zn<sup>2+</sup>) present in the collected water samples was analyzed through an atomic absorption spectrometer (AAS). Two hydrogels, such as PVA/CH and PVA/AA, are synthesised by adopting sol–gel polymerization technique using CH, AA, and PVA. Both the hydrogels were characterized by using FT-IR, XRD, SEM/EDS, XPS, and TGA. We adopted suitable methodology to carry out studies on the antibacterial properties, swelling behaviour, and adsorption of the water samples. The adsorption study was done for the separation of potentially toxic metal ions at various intervals of time using two hydrogels. It was observed that the capability of adsorption rate increases with increases in adsorbent dosage and the rate of adsorption, which is faster at the initial time and then gradually decreases up to 180 min. The adsorption capacity of both hydrogels follows the order Zn<sup>2+</sup> > Ni<sup>2+</sup>> Fe<sup>3+</sup>> Cd<sup>2+</sup> ions. The results revealed that the adsorption capability of the PVA/CH hydrogel is higher than that of PVA/AA, signifying their use efficiently for the elimination of potentially toxic metal ions from metal-contaminated water.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358712","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

Facile fabrication of robust cork-inspired superhydrophobic aerogel for continuous oil spill and emulsion absorption 轻松制造用于持续吸收溢油和乳化液的坚固软木塞启发式超疏水气凝胶

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129888

Although superhydrophobic aerogels are widely used in oil–water separation, traditional vertical channel aerogels often struggle to achieve flexibility, robustness, and superhydrophobicity simultaneously. Inspired by cork wood, carboxylated nitrile rubber was selected as the soft phase, while a polymethylsiloxane layer served as the rigid phase, resulting in the successful preparation of a robust superhydrophobic aerogel. The aerogel featured a honeycomb-like structure with a multimodal pore size distribution. It exhibited excellent superhydrophobicity, with a contact angle of about 155.5° and a rolling angle of approximately 2°. Even under various extreme conditions, the aerogel maintained a contact angle exceeding 150°, showcasing excellent stability. Additionally, it showed excellent mechanical properties, with only around 10 % irreversible damage after 1000 compression cycles at 30 % strain. Therefore, the aerogel exhibited excellent adsorption performance, with an absorption capacity of 0.909 mL/cm³, and an average absorption rate of 0.848 mL/s. Even after 100 cycles, it retained excellent recovery capabilities, proving effective in various practical oil–water separation scenarios. Most importantly, this method was simple, easy to operate, customizable, and cost-effective, laying the foundation for widespread industrial applications.

虽然超疏水气凝胶被广泛应用于油水分离领域，但传统的垂直通道气凝胶往往难以同时实现柔性、坚固性和超疏水性能。受软木的启发，我们选择了羧基丁腈橡胶作为软相，聚甲基硅氧烷层作为硬相，从而成功制备出了坚固的超疏水气凝胶。气凝胶具有多模态孔径分布的蜂窝状结构。它具有出色的超疏水性能，接触角约为 155.5°，滚动角约为 2°。即使在各种极端条件下，气凝胶也能保持超过 150° 的接触角，显示出卓越的稳定性。此外，气凝胶还具有出色的机械性能，在应变为 30% 的条件下压缩 1000 次后，只有约 10% 的不可逆损伤。因此，气凝胶具有出色的吸附性能，吸附容量为 0.909 mL/cm3，平均吸附速度为 0.848 mL/s。即使在 100 次循环后，气凝胶仍能保持出色的回收能力，在各种实际油水分离应用中证明了其有效性。最重要的是，这种方法简单、易于操作、可定制且具有成本效益，为广泛的工业应用奠定了基础。

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引用次数: 0

Constructing oxygen-deficient Cu/WO3/TNT heterojunction film for improved photocatalytic decomposition of toluene and bacteria: From bench-scale study to enlarged reactor test 构建缺氧的 Cu/WO3/TNT 异质结薄膜以改进甲苯和细菌的光催化分解：从台架研究到扩大反应器试验

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129919

A robust and active photocatalyst that can effectively decompose indoor air pollutants is highly demand. In this study, we have fabricated Cu and WO₃ modified titania nanotube (Cu/WO₃/TNT) with oxygen vacancies to enhance photocatalytic decomposition of toluene and bacteria under light irradiation. The roles of WO₃ and Cu modification on TNT film have been investigated through photoelectrochemical (PEC) measurements and photocatalytic decomposition of pollutants. The results demonstrate that the deposition of Cu (about 2.5 %) and WO₃ (about 1.1 %) onto TNT film, as well as concurrent formation of oxygen vacancies, effectively enhance PEC response and photocatalytic activity of TNT film. Under UV–visible light irradiation, the optimized Cu/WO₃/TNT catalyst can effectively degrade toluene by approximately 95.0 % in 90 min, while over 99.9 % of E. coli bacteria can be inactivated by the photocatalyst under visible light irradiation. Both Cu/WO₃ deposition and oxygen vacancy formation improve light absorption and charge carrier separation of the TNT film for pollutants degradation. Oxygen plays a crucial role in the toluene degradation process, with O₂/^•O₂⁻ activation considered as a key step for subsequent oxidation of toluene or benzyl radical. Whereas, the main oxidants for bacteria inactivation during the process are identified as ¹O₂ and h⁺. Scaled-up experiments (∼1.0 m³ reactor for toluene degradation and ∼ 0.1 m³ reactor for gas phase bacteria inactivation) prove that the the optimized Cu/WO₃/TNT film is a promising photocatalyst for indoor air purification under UV–visible light irradiation.

人们亟需一种能有效分解室内空气污染物的坚固而活跃的光催化剂。在这项研究中，我们制备了具有氧空位的 Cu 和 WO3 修饰二氧化钛纳米管（Cu/WO3/TNT），以增强其在光照射下对甲苯和细菌的光催化分解能力。通过光电化学（PEC）测量和污染物的光催化分解，研究了 WO3 和 Cu 修饰在 TNT 薄膜上的作用。结果表明，在 TNT 薄膜上沉积 Cu（约 2.5%）和 WO3（约 1.1%），并同时形成氧空位，可有效提高 TNT 薄膜的光致电化学响应和光催化活性。在紫外-可见光照射下，优化的 Cu/WO3/TNT 催化剂可在 90 分钟内有效降解甲苯约 95.0%，而在可见光照射下，光催化剂可灭活 99.9% 以上的大肠杆菌。Cu/WO3 沉积和氧空位的形成都改善了 TNT 薄膜的光吸收和电荷载流子分离，从而实现污染物降解。氧气在甲苯降解过程中起着至关重要的作用，O2/-O2-活化被认为是随后甲苯或苄基自由基氧化的关键步骤。而在这一过程中，细菌失活的主要氧化剂是 1O2 和 h+。放大实验（1.0 立方米的反应器用于甲苯降解，0.1 立方米的反应器用于气相细菌灭活）证明，优化的 Cu/WO3/TNT 薄膜是一种很有前途的光催化剂，可用于紫外可见光照射下的室内空气净化。

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引用次数: 0

In situ synthesis of Nb-modified AFI topology molecular sieve and its modulation on the formantion of high-efficiency catalyst for 4,6-dimethyldibenzothiophene hydrodesulfurization Nb 改性 AFI 拓扑分子筛的原位合成及其对 4,6-二甲基二苯并噻吩加氢脱硫高效催化剂形成的调控作用

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129914

Herein, molecular sieves with Nb and Si modified AFI-type structures were successfully synthesized in situ via a hydrothermal synthesis method. Subsequently, the corresponding NiW catalysts modified by the molecular sieve were obtained through incipient co-impregnation. The performance of NiW catalysts for 4,6-dimenthyldibenzothiophene (4,6-DMDBT) was comprehensively investigated. A series of characterizations demonstrated that Nb species were uniformly distributed within the AFI framework. This not only resulted in an increase in the acidic sites of both molecular sieves and hybrid-support (NbSAPO-5-alumina), but also effectively modulated the interaction between hybrid support and active metals. This led to a higher stacking numbers, which facilitated the sulfidation of W and Ni species, ultimately promoting the formation of more active edge sites on WS₂ slabs. This resulted in the catalyst NiW/NbSAPOA achieving a significantly higher desulfurization ratio of 95.8 % for 4,6-DMDBT at 280 ℃. Furthermore, the catalyst NiW/NbSAPOA exhibited the highest turnover frequency of 9.17 × 10⁻⁴ s⁻¹, and markedly enhanced selectivity for the direct desulfurization pathway in 4,6-DMDBT HDS.

在此，通过水热合成法成功地在原位合成了具有 Nb 和 Si 修饰 AFI 型结构的分子筛。随后，通过萌发共浸渍法获得了分子筛修饰的相应 NiW 催化剂。研究人员全面考察了 NiW 催化剂对 4,6-二甲基二苯并噻吩（4,6-DMDBT）的性能。一系列表征结果表明，铌物种均匀地分布在 AFI 框架中。这不仅增加了分子筛和混合支撑（NbSAPO-5-氧化铝）的酸性位点，还有效调节了混合支撑与活性金属之间的相互作用。这导致了更高的堆叠数，有利于 W 和 Ni 的硫化，最终促进在 WS2 板上形成更多的活性边缘位点。这使得催化剂 NiW/NbSAPOA 在 280 ℃ 下对 4,6-DMDBT 的脱硫率显著提高，达到 95.8%。此外，催化剂 NiW/NbSAPOA 的翻转频率最高，达到 9.17 × 10-4 s-1，并显著提高了 4,6-DMDBT 加氢脱硫过程中直接脱硫途径的选择性。

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引用次数: 0

Novel polyarylene sulfide sulfone/amide tertiary amine membranes for organic solvent nanofiltration 用于有机溶剂纳滤的新型聚芳硫醚砜/酰胺叔胺膜

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-28 DOI: 10.1016/j.seppur.2024.129909

The development of membrane materials that are fouling-resistant and capable of achieving molecular separation from organic solvents is essential for industrial development. The strategy of introduction of zwitterionic compound amine oxide (AO) was proved to be an effective route. So, in this study, TA unit was introduced into polyarylene sulfide sulfone (PASS) molecular chain, then a facile one-step oxidation was conducted to convert the tertiary amine (TA) units in the membrane molecular chain to AO units. Through the oxidation treatment, the anti-fouling performance of the membranes was greatly improved with the Frr up to 95 % and F_ir down to 10 %, indicating the potential for long-term filtration. Interestingly, with the oxidation process, the thioether (−S–) units in the polymer chain were found to oxidize to strong polar sulfone groups (−SO₂–). Thus the rigidity of the molecular chain and the intermolecular interaction was significant enlarged, and the solvent resistance of the membrane was further enhanced. Also it is interesting that the membranes were transferred from ultrafiltration to loose nanofiltration membranes after the oxidation treatment. Then the oxidized membranes were conducted to organic solvent nanofiltration. The O-PASS/ATA membrane demonstrated a notable retention effect for dyes in ethanol, N, N-Dimethylformamide (DMF) and N-methyl-2-pyrrolidone (NMP). The retention of Congo red was maintained at a level exceeding 95 %, while the permeance remained stable at a range of 7–16 L m⁻²h⁻¹ bar⁻¹. This work presents an effective method for the preparation of nanofiltration membranes for organic solvents and demonstrates significant potential for achieving molecular separation in organic solvents.

开发抗污且能从有机溶剂中实现分子分离的膜材料对工业发展至关重要。引入齐聚物氧化胺（AO）的策略被证明是一种有效的途径。因此，本研究在聚芳醚砜（PASS）分子链中引入 TA 单元，然后进行简单的一步氧化，将膜分子链中的叔胺（TA）单元转化为 AO 单元。通过氧化处理，膜的防污性能大大提高，Frr 达到 95%，Fir 降低到 10%，显示出长期过滤的潜力。有趣的是，在氧化过程中，聚合物链中的硫醚（-S-）单元被氧化成强极性的砜基团（-SO2-）。因此，分子链的刚性和分子间的相互作用显著增强，膜的耐溶剂性也进一步提高。同样有趣的是，经过氧化处理后的膜从超滤膜转移到了松散的纳滤膜上。然后，氧化膜被用于有机溶剂纳滤。O-PASS/ATA 膜在乙醇、N, N-二甲基甲酰胺（DMF）和 N-甲基-2-吡咯烷酮（NMP）中对染料的截留效果显著。刚果红的保留率保持在 95% 以上，而渗透率在 7-16 L m-2h-1 bar-1 的范围内保持稳定。这项研究提出了一种制备有机溶剂纳滤膜的有效方法，并展示了在有机溶剂中实现分子分离的巨大潜力。

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引用次数: 0

Switchable deep eutectic solvents for the extraction of phlorizin and trilobatin from sweet tea (Lithocarpus litseifolius (Hance) Chun) 从甜茶（Lithocarpus litseifolius (Hance) Chun）中提取氯嗪和三叶皂苷的可切换深共晶溶剂

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-27 DOI: 10.1016/j.seppur.2024.129898

Switchable deep eutectic solvents (SDESs) have recently been developed to improve the recovery and reuse of the extractants. In this work, temperature-induced SDESs were prepared and used for the extraction of flavonoids (representative phlorizin and trilobatin) from sweet tea (Lithocarpus litseifolius (Hance) Chun). These SDESs solution can switch between solution and sediment depending on the temperature, and the phase diagram of SDESs solution had been drawn. Their temperature-responsive characteristics were studied by various characterizations, including variable-temperature FT-IR, variable-temperature ¹H NMR, and variable-temperature dynamic light scattering (DLS). SDES-1 (Benzamide: Malic acid = 2:1) was screened as the optimal extractant, and the major factors affecting the extraction process were studied by single-factor experiments and optimized by response surface methodology (RSM). The extraction yields for phlorizin and trilobatin were 114.72 and 12.56 mg/g, respectively. Moreover, the recoveries for phlorizin and trilobatin reached 98.46 % and 94.64 %, respectively. This study thus provides an environmentally sound strategy for extracting bioactive compounds from plant resources.

为了提高萃取剂的回收率和重复利用率，最近开发出了可切换深共晶溶剂（SDES）。本研究制备了温度诱导型深共晶溶剂（SDESs），并将其用于甜茶（Lithocarpus litseifolius (Hance) Chun）中黄酮类化合物（具有代表性的叶绿素和三叶皂苷）的萃取。这些 SDESs 溶液可随温度在溶液和沉淀之间切换，并绘制了 SDESs 溶液的相图。通过变温傅立叶变换红外光谱、变温 1H NMR 和变温动态光散射（DLS）等多种表征方法研究了它们的温度响应特性。筛选出 SDES-1（苯甲酰胺：苹果酸=2:1）为最佳萃取剂，通过单因素实验研究了影响萃取过程的主要因素，并采用响应面法（RSM）进行了优化。结果表明，氯嗪和三叶皂苷的萃取率分别为 114.72 和 12.56 mg/g。此外，氯嗪和三叶皂苷的回收率分别达到了 98.46 % 和 94.64 %。因此，这项研究为从植物资源中提取生物活性化合物提供了一种无害环境的策略。

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