Separation and Purification Technology最新文献_第10页

Iron-embedded S-scheme heterostructure nanocomposite K2Ti4O9/rGO for pollution control: Photocatalytic activity, stability, reaction intermediate, hazard profiling, and mechanism 用于污染控制的嵌铁 S 型异质结构纳米复合材料 K2Ti4O9/rGO：光催化活性、稳定性、反应中间体、危害分析和机理

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129801

The worsening environmental pollution caused by the misuse and careless management of pharmaceuticals has prompted many efforts to break down toxic antibiotics into harmless compounds. These substances, defined as representative emerging contaminants, can be harmful and cause allergic reactions when combined with coliform bacteria in soil or water environments. Layered titanate has attracted considerable attention for its potential to solve various environmental problems because of its unique material properties. This study examined newly fabricated layered titanate (K₂Ti₄O₉) nanobelts for the degradation of antibiotic tetracycline, one of the most widely used antibiotics, and high-strength coliform bacteria isolated from real wastewater. The K₂Ti₄O₉-reduced graphene oxide/Fe (KTO/rGO/α-Fe₂O₃) with a step scheme (S-Scheme) nanostructure was integrated by the simultaneous reduction of GO and α-Fe₂O₃. The toxicological relationships of nanomaterials were evaluated using the ecological structure–activity relations (ECOSAR) model, and the environmental impact of the photocatalytic degradation process was examined through a toxicity evaluation of the reaction intermediates. Under blue LED light, the nanocomposite removed 93 % of the tetracycline in 120 min. In addition, it was effective in real wastewater disinfection by inactivating 99 % of total coliforms within the same time frame, indicating the superior properties of the KTO/rGO/α-Fe₂O₃ S-Scheme nanocomposite. The heterostructure was confirmed by X-ray diffraction, ultraviolet diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and photoluminescence measurements. Gas chromatography-mass spectrometry confirmed the complete mineralization of tetracycline and the possible degradation pathway. These results highlight the potential for effectively controlling refractory pollutants in wastewater through the remarkable stability and cyclic performance of the new visible-light-driven photocatalyst.

药品的滥用和粗心大意的管理造成了日益严重的环境污染，促使许多人努力将有毒抗生素分解成无害化合物。这些物质被定义为具有代表性的新兴污染物，与土壤或水环境中的大肠菌群结合在一起时，可能会产生危害并引起过敏反应。层状钛酸酯因其独特的材料特性，具有解决各种环境问题的潜力，因而备受关注。本研究考察了新制备的层状钛酸酯（K2Ti4O9）纳米颗粒对抗生素四环素（最广泛使用的抗生素之一）和从实际废水中分离的高强度大肠菌群的降解作用。通过同时还原 GO 和 α-Fe2O3，集成了具有阶跃方案（S-Scheme）的 K2Ti4O9 还原氧化石墨烯/铁（KTO/rGO/α-Fe2O3）纳米结构。利用生态结构-活性关系（ECOSAR）模型评估了纳米材料的毒理学关系，并通过反应中间产物的毒性评估考察了光催化降解过程对环境的影响。在蓝色 LED 光下，纳米复合材料在 120 分钟内去除 93% 的四环素。此外，它在实际废水消毒中也很有效，在相同的时间内灭活了 99% 的总大肠菌群，这表明 KTO/rGO/α-Fe2O3 S-Scheme 纳米复合材料具有卓越的性能。异质结构通过 X 射线衍射、紫外漫反射光谱、X 射线光电子能谱、傅立叶变换红外光谱和光致发光测量得到了证实。气相色谱-质谱法证实了四环素的完全矿化和可能的降解途径。这些结果突出表明，这种新型可见光驱动光催化剂具有显著的稳定性和循环性能，有望有效控制废水中的难降解污染物。

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引用次数: 0

Surface reconstruction of sulfonated polysulfone ultrafiltration membrane with cellulose nanocrystals for enhancing anti-fouling performance 用纤维素纳米晶对磺化聚砜超滤膜进行表面重构以提高防污性能

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129815

The fouling issues of ultrafiltration membranes is one of limitations for their long-term effectiveness. Here, we developed an effective and environmentally friendly approach for constructing anti-fouling ultrafiltration membrane, achieved by the surface modification of sulfonated polysulfone (SPSF) ultrafiltration membrane with cellulose nanocrystals (CNCs). The composite ultrafiltration membrane was obtained by only filtering CNC suspension through SPSF ultrafiltration membrane, and showed good hydrophilicity that its water contact angle is only 53° which is much lower than that of SPSF ultrafiltration membrane (74°). Its retention rate for the pollutants with particle size greater than 10 nm is close to 100 %. Its water flux is almost twice that of SPSF ultrafiltration membrane under the sewage condition. After three cycles of filtering severe sewage, its flux recovery rate is still 95 %, far higher than that of SPSF ultrafiltration membrane (60 %). Therefore, the surface modification strategy of SPSF ultrafiltration membrane with CNCs is effective and green for improving the anti-fouling properties of ultrafiltration membranes, which is a valuable reference for enhancing the anti-fouling performance of ultrafiltration membranes from various materials. The as-prepared CNCs/SPSF ultrafiltration membrane has a promising application in the purification of wastewater containing hydrophobic particles.

超滤膜的污垢问题是其长期有效性的限制因素之一。在此，我们开发了一种有效且环保的方法来构建防污超滤膜，即用纤维素纳米晶（CNCs）对磺化聚砜（SPSF）超滤膜进行表面改性。该复合超滤膜仅通过 SPSF 超滤膜过滤 CNC 悬浮液而获得，具有良好的亲水性，其水接触角仅为 53°，远低于 SPSF 超滤膜的 74°。它对粒径大于 10 纳米的污染物的截留率接近 100%。在污水条件下，其水通量几乎是 SPSF 超滤膜的两倍。经过三个周期的严重污水过滤后，其通量恢复率仍高达 95%，远高于 SPSF 超滤膜的 60%。因此，采用 CNCs 对 SPSF 超滤膜进行表面改性的策略可有效、绿色地改善超滤膜的抗污性能，对提高各种材料超滤膜的抗污性能具有重要的参考价值。制备的 CNCs/SPSF 超滤膜在净化含有疏水颗粒的废水方面具有广阔的应用前景。

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引用次数: 0

Sugarcane bagasse derived composite sorbent for sorption based atmospheric water harvesting 甘蔗渣衍生复合吸附剂，用于基于吸附的大气水收集

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129820

The escalating global concern surrounding water scarcity is significantly impacting the quality of life, particularly in arid and land-locked regions. Sorption-based atmospheric water harvesting (AWH), employing a sorbent to capture atmospheric moisture, emerges as a sustainable solution to mitigate the global water crisis. However, developing efficient, eco-friendly, easily synthesised, and cost-effective sorbents poses a challenge. Herein, an efficient composite sorbent derived from waste sugarcane bagasse-based activated carbon (SBAC), impregnated with a low-cost hygroscopic CaCl₂ salt, has been prepared. The composite SBAC/CaCl₂ showed good performance across a wide working range between 10–90 % relative humidity, with water uptake ranging from 0.24 to 2.44 g/g. At moderate temperature and humidity (25 °C, 60 % RH), SBAC/CaCl₂ exhibited a water uptake of 1.2 g/g and achieved over 80 % of its equilibrium water uptake within 90 min. Also, the sorbent showed excellent solar driven desorption with desorption efficiencies reaching over 93 % and 85 % for 1 sun and 0.5 sun illumination, respectively, within 60 min. The sorption kinetics and adsorption isotherm showed excellent fit with the linear driving force model and Dubinin Astakhov isotherm model. The practical solar-driven atmospheric water harvesting performance of the SBAC/CaCl₂ composite was also successfully demonstrated using a custom-built device under outdoor conditions and the harvested water met the quality standards of drinking water. Furthermore, the prepared sorbent exhibited cyclic stability and storage reliability with no performance degradation even after repeated cycles. This work highlights the significant potential of waste biomass derived sorbents for sustainable AWH applications.

全球对水资源短缺的担忧不断升级，严重影响了人们的生活质量，尤其是在干旱和内陆地区。吸附式大气集水（AWH）利用吸附剂捕捉大气中的水分，是缓解全球水资源危机的一种可持续解决方案。然而，开发高效、环保、易于合成且成本效益高的吸附剂是一项挑战。在本文中，我们制备了一种高效的复合吸附剂，这种吸附剂取自废弃甘蔗渣基活性炭（SBAC），并浸渍了一种低成本的吸湿性 CaCl2 盐。SBAC/CaCl2 复合吸附剂在相对湿度为 10%-90% 的宽工作范围内表现出良好的性能，吸水率在 0.24 到 2.44 g/g 之间。在中等温度和湿度（25 °C，60 % 相对湿度）条件下，SBAC/CaCl2 的吸水率为 1.2 g/g，并在 90 分钟内达到平衡吸水率的 80 % 以上。此外，该吸附剂还表现出卓越的太阳光驱动解吸能力，在 60 分钟内，1 个太阳光照射和 0.5 个太阳光照射下的解吸效率分别达到 93% 和 85% 以上。吸附动力学和吸附等温线与线性驱动力模型和 Dubinin Astakhov 等温线模型非常吻合。在室外条件下，利用定制装置成功演示了 SBAC/CaCl2 复合材料的太阳能驱动大气水收集实用性能，收集的水符合饮用水质量标准。此外，所制备的吸水剂具有循环稳定性和储存可靠性，即使在反复循环后也不会出现性能下降。这项工作凸显了废弃生物质衍生吸附剂在可持续 AWH 应用中的巨大潜力。

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引用次数: 0

Principle of vanadium doping-induced MoS2 homojunction effect and mechanism analysis of antibacterial process under near-infrared light 掺钒诱导 MoS2 同质结效应的原理及近红外光下抗菌过程的机理分析

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129814

MoS₂ exhibits unique physical and chemical properties in its 1 T and 2H phases. Each phase has its inherent advantages and limitations. Although several biochemical properties of MoS₂ have been extensively reported, the specific impacts of these phases on photothermal and antibacterial performance, the feasibility of integrating the unique advantages of both phases and the underlying dominant bactericidal mechanisms are still largely unexplored. In this work, the electronic-structural relationships of 1 T- and 2H-MoS₂ were first simulated using density functional theory (DFT), which provided unique insights into how these phases affect performance. Based on these insights, a solid-state coupling interface and built-in electric field were designed between the two phases, and a 1 T/2H MoS₂ homojunction was synthesized using the hydrothermal method, achieving a higher carrier separation efficiency and exhibiting excellent photothermal and antibacterial properties. Subsequently, further attempts were made to adjust the electronic structure by doping vanadium atoms. This doping not only introduces additional electrons to facilitate electron transfer but also further enhances the antibacterial capability by creating surface defects that increase the number of active sites. Finally, the synergistic antibacterial mechanism of this system was thoroughly investigated through detailed experiments and DFT theoretical analysis. The design of the homojunction, the introduction of defects, and the incorporation of heteroatoms were discussed in this paper, which pave the way for the rational design strategy of advanced two-dimensional materials and can be extended to other polycrystalline materials.

MoS2 的 1 T 相和 2H 相具有独特的物理和化学特性。每种相都有其固有的优势和局限性。尽管 MoS2 的一些生物化学特性已被广泛报道，但这些相态对光热和抗菌性能的具体影响、整合两种相态独特优势的可行性以及潜在的主导杀菌机制在很大程度上仍未得到探索。在这项工作中，首先使用密度泛函理论（DFT）模拟了 1 T 和 2H-MoS2 的电子结构关系，从而为了解这些相如何影响性能提供了独特的见解。在此基础上，设计了两相之间的固态耦合界面和内置电场，并利用水热法合成了 1 T/2H MoS2 同质结，实现了更高的载流子分离效率，并表现出优异的光热和抗菌性能。随后，研究人员进一步尝试通过掺杂钒原子来调整电子结构。这种掺杂不仅引入了额外的电子以促进电子转移，还通过产生表面缺陷增加了活性位点的数量，从而进一步增强了抗菌能力。最后，通过详细的实验和 DFT 理论分析，对该系统的协同抗菌机制进行了深入研究。本文讨论了同质结的设计、缺陷的引入和杂原子的结合，为先进二维材料的合理设计策略铺平了道路，并可推广到其他多晶材料。

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引用次数: 0

Yolk-Shell Pst@SiO2 decorated with functional guests: A new solid-phase extractant for highly effective separation of no carrier added 177Lu 用功能客体装饰的卵黄壳Pst@SiO2：高效分离无载体添加 177Lu 的新型固相萃取剂

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129802

With the rapid development of ¹⁷⁷Lu-related radiopharmaceuticals, there is an urgent need for large-scale production of ¹⁷⁷Lu efficiently. In this work, we employed yolk-shell Pst@SiO₂ to accommodate 2-ethylhexyl 2-ethylhexylphosphonic acid (HEH[EHP]), obtaining a material with ideal microstructure and adequate functionality to isolate Lu from Yb effectively. ¹⁷⁷Lu isolation on HEH[EHP]-Pst@SiO₂ dynamic column has been demonstrated to be influenced by various parameters such as the initial target solution, the eluent property, and the separation temperature. Most importantly, an effective separation process including primary separation and secondary purification has been established based on plenty of simulated experiments and radioactively tracing investigations. As a result, NCA ¹⁷⁷Lu with high radionuclide and radiochemical purity (≥99.99 %) and excellent decontamination factor (10⁴) from Yb can be acquired in good recovery (>60%). This work provides not only a candidate for NCA ¹⁷⁷Lu production but also some important hints for the separation of other heavy lanthanides.

随着177Lu相关放射性药物的快速发展，177Lu的大规模高效生产迫在眉睫。在这项工作中，我们采用卵黄壳Pst@SiO2容纳2-乙基己基膦酸（HEH[EHP]），获得了一种具有理想微观结构和足够功能的材料，可有效地从镱中分离出Lu。在 HEH[EHP]-Pst@SiO2 动态色谱柱上分离 177Lu 的过程受到多种参数的影响，如初始目标溶液、洗脱液性质和分离温度。最重要的是，在大量模拟实验和放射性追踪调查的基础上，建立了包括一级分离和二级纯化的有效分离过程。因此，可以从镱中获得放射性核素和放射化学纯度高（≥99.99 %）、去污因子（104）优良（60%）的 NCA 177Lu。这项工作不仅为生产 NCA 177Lu 提供了一个候选方案，还为分离其他重镧系元素提供了一些重要提示。

{"title":"Yolk-Shell Pst@SiO2 decorated with functional guests: A new solid-phase extractant for highly effective separation of no carrier added 177Lu","authors":"","doi":"10.1016/j.seppur.2024.129802","DOIUrl":"10.1016/j.seppur.2024.129802","url":null,"abstract":"<div><div>With the rapid development of <sup>177</sup>Lu-related radiopharmaceuticals, there is an urgent need for large-scale production of <sup>177</sup>Lu efficiently. In this work, we employed yolk-shell Pst@SiO<sub>2</sub> to accommodate 2-ethylhexyl 2-ethylhexylphosphonic acid (HEH[EHP]), obtaining a material with ideal microstructure and adequate functionality to isolate Lu from Yb effectively. <sup>177</sup>Lu isolation on HEH[EHP]-Pst@SiO<sub>2</sub> dynamic column has been demonstrated to be influenced by various parameters such as the initial target solution, the eluent property, and the separation temperature. Most importantly, an effective separation process including primary separation and secondary purification has been established based on plenty of simulated experiments and radioactively tracing investigations. As a result, NCA <sup>177</sup>Lu with high radionuclide and radiochemical purity (≥99.99 %) and excellent decontamination factor (10<sup>4</sup>) from Yb can be acquired in good recovery (>60%). This work provides not only a candidate for NCA <sup>177</sup>Lu production but also some important hints for the separation of other heavy lanthanides.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320334","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

High metal-loaded sub-nanocluster catalyst enhanced Fenton-like reaction activity for emerging contaminants degradation by generating high-valent copper 高金属负载亚纳米簇催化剂通过生成高价铜增强了新污染物降解的 Fenton 类反应活性

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-20 DOI: 10.1016/j.seppur.2024.129794

High-valent copper (Cu(III)) species are crucial intermediates in CH bond functionalization within both the biological and biomimetic processes, facilitated by copper enzymes and stabilized by multicopper oxidases. Herein, a nitrogen-doped copper sub-nanocluster catalyst (SNC) featured a high metal content (29.1 wt%) and uniform Cu distribution was synthesized by carbonizing the nanosheet-like metal–organic framework (MOF), enhancing bisphenol A degradation by activating peroxymonosulfate (PMS) to generate Cu(III). The degradation performance of the SNC outperformed the catalyst carbonized with the bulk-like MOF and matched the reported single-atom catalysts counterparts. Nitrogen doping decreased the electrons of Cu3d orbital, enhancing its bonding with the oxygen atom within the PMS molecule, thus promoting Cu(III) generation. The Cu-SNC/PMS system also showed robust resistance against anions, pH changes, and diverse water matrices. Importantly, it can selectively degrade electron-rich pollutants through oxygen atom transfer by Cu(III). This study provided new perspectives into SNC preparation, the controlled formation of high-valent metal species, and their role in Fenton-like reactions for pollutants degradation.

高价铜（Cu(III)）物种是生物和仿生过程中 CH 键官能化的关键中间体，由铜酶促进并由多铜氧化酶稳定。本文通过碳化纳米片状金属有机框架（MOF），合成了一种氮掺杂铜亚纳米簇催化剂（SNC），该催化剂具有金属含量高（29.1 wt%）和铜分布均匀的特点，通过激活过一硫酸盐（PMS）生成铜（III）来提高双酚 A 的降解性能。SNC 的降解性能优于用块状 MOF 碳化的催化剂，与已报道的单原子催化剂性能相当。氮的掺入减少了 Cu3d 轨道的电子，增强了其与 PMS 分子中氧原子的结合，从而促进了 Cu(III) 的生成。Cu-SNC/PMS 系统还对阴离子、pH 值变化和各种水基质表现出强大的耐受性。重要的是，它可以通过 Cu（III）的氧原子转移选择性地降解富电子污染物。这项研究为 SNC 的制备、高价金属物种的可控形成及其在污染物降解的 Fenton 类反应中的作用提供了新的视角。

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引用次数: 0

Synthesis of bifunctional silica aerogels for robust and simultaneous removal of Hg(II) and malachite green: Performance and mechanism 合成双功能二氧化硅气凝胶，用于同时强效去除汞（II）和孔雀石绿：性能与机理

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-19 DOI: 10.1016/j.seppur.2024.129773

The pollution of heavy metal ions and dyes to water endanger the ecosystem and public health. Adsorption has been widely used for the removal of water pollutants because of its low cost and simple operation. Herein, a family of nitrogen- and sulfur-containing bifunctional silica aerogels with different structure and composition were prepared for robust and simultaneous removal of Hg(II) and malachite green (MG). The optimal adsorption pH for Hg(II) and MG are 6 and 10, and the maximum adsorption capacity are 215.35 and 1227.14 mg·g⁻¹. The adsorption kinetic and isotherm process can be described by pseudo-second-order and Langmuir model. The aerogels can simultaneous removal Hg(II) and MG efficiently. They also exhibit impressive affinity and adsorption selectivity for Hg(II) and MG with the existence of multiple contaminants and high saline environments. Adsorption mechanism implies the adsorption for Hg(II) mainly depends on the interaction with amino and sulfur groups, while the binding of MG mainly depends on the formation of hydrogen bonds. The aerogels display satisfactory adsorption performance in real water sample and good reusability. The regeneration rate can maintain 91.50 % and 90.23 % for Hg(II) and MG after five regeneration cycles. The work may provide efficient bifunctional silica aerogels for the simultaneous decontamination metal ions and dyes with practical application.

重金属离子和染料对水的污染危及生态系统和公众健康。吸附法因其成本低、操作简单而被广泛应用于去除水污染物。本文制备了一系列具有不同结构和组成的含氮和含硫双功能二氧化硅气凝胶，用于同时强效去除汞（II）和孔雀石绿（MG）。Hg(II) 和 MG 的最佳吸附 pH 值分别为 6 和 10，最大吸附容量分别为 215.35 和 1227.14 mg-g-1。吸附动力学和等温线过程可用伪二阶和 Langmuir 模型描述。气凝胶能同时有效地去除 Hg（II）和 MG。在多种污染物和高盐度环境下，气凝胶对 Hg(II) 和 MG 的亲和力和吸附选择性也令人印象深刻。吸附机理表明，对 Hg（II）的吸附主要取决于与氨基和硫基的相互作用，而对 MG 的结合主要取决于氢键的形成。气凝胶在实际水样中显示出令人满意的吸附性能和良好的可重复使用性。经过五个再生周期后，气凝胶对 Hg(II) 和 MG 的再生率分别保持在 91.50% 和 90.23%。这项工作可为同时净化金属离子和染料提供高效的双功能二氧化硅气凝胶，并具有实际应用价值。

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引用次数: 0

Ultrathin 2D/2D MoS2/Bi2WO6 S-scheme heterojunction for boosting photocatalytic degradation of ciprofloxacin 促进环丙沙星光催化降解的超薄二维/二维 MoS2/Bi2WO6 S 型异质结

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-19 DOI: 10.1016/j.seppur.2024.129768

A series of 2D/2D MoS₂/Bi₂WO₆ S-scheme heterojunctions consisting of ultrathin MoS₂ nanosheets (MS, 1.6 nm) and ultrathin Bi₂WO₆ nanosheets (BWO, 1.5 nm) were developed for photocatalytic degradation of ciprofloxacin. The samples with 5 % mass ratio of MS (5 %MS/BWO) exhibits the almost complete degradation of ciprofloxacin (≈100 %) under visible light. It is evidenced that the formation of S-scheme heterojunction with close interfacial interaction facilitates the photoinduced carrier separation and the generation of surface acid sites. The activation of ciprofloxacin molecules is realized through the coordinately interaction of C-N and C=O with the surface W sites. Moreover, the OVs in BWO side is a convenient pathway for activated of O₂, embodying in the generation of •O₂⁻ and •OH under visible light over photocatalyst. Such an association of charge transfer mechanism with coordination activation shows the enhanced photocatalytic performance toward ciprofloxacin. This work provides a motivation which designs an S-scheme heterojunction photocatalyst with the ability to activate the specific group in molecules to comprehend the degradation of antibiotics.

研究人员开发了一系列由超薄 MoS2 纳米片（MS，1.6 纳米）和超薄 Bi2WO6 纳米片（BWO，1.5 纳米）组成的二维/二维 MoS2/Bi2WO6 S 型异质结，用于光催化降解环丙沙星。在可见光下，质量比为 5% 的 MS（5%MS/BWO）样品几乎完全降解了环丙沙星（≈100%）。事实证明，S 型异质结的形成与紧密的界面相互作用促进了光诱导的载流子分离和表面酸性位点的生成。环丙沙星分子的活化是通过 C-N 和 C=O 与表面 W 位点的配位相互作用实现的。此外，BWO 侧的 OV 是活化 O2 的便捷途径，在光催化剂上的可见光作用下产生 -O2- 和 -OH。这种电荷转移机制与配位活化的结合增强了对环丙沙星的光催化性能。这项工作提供了一种设计 S 型异质结光催化剂的动机，这种光催化剂具有激活分子中特定基团的能力，可以理解抗生素的降解。

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引用次数: 0

Humic substances and inorganic ions synergistically precipitate at the gas–liquid interface in a simulation experiment of direct-contact heat and mass transfer processes 在直接接触传热和传质过程的模拟实验中，腐殖质和无机离子在气液界面协同沉淀

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-19 DOI: 10.1016/j.seppur.2024.129787

Direct-contact heat and mass transfer processes are widely employed in saline wastewater treatment. However, these processes are accompanied by serious ultrafine particle emission, a phenomenon associated with the solute’s transition across the gas–liquid interface. A thorough comprehension of the solute’s behavior at this gas–liquid interface is vital for clarifying the crossing process and guiding particle control strategies. Here, solutions containing saturated inorganic ions and humic substances were evaporated to analyze their behaviors at the gas–liquid interface in an experimental simulation of direct-contact heat and mass transfer processes. It was found that these substances co-precipitated at this interface. Humic substances can bind with inorganic ions via chemical bonds, monovalent ions through cation-π interactions, and divalent ions through electrostatic and chelation interactions. Moreover, humic substances can act as nucleation sites for precipitating inorganic crystals. These distinctive binding mechanisms caused a synergistic relationship between humic substances and inorganic ions during precipitation. Amidst precipitation, humic substances with high humification degrees and large molecular weights were predominantly enriched. Inorganic ions, comprising over 93% of the total precipitate mass, constituted the principal constituents. Among these, Na⁺, with an enrichment factor of 2.10, precipitated more readily at the gas–liquid interface compared to divalent ions. These conclusions concerning the binding mechanisms of humic substances and inorganic ions, along with their precipitation characteristics, were validated in the submerged combustion evaporation process of membrane-concentrated leachate.

直接接触传热和传质过程被广泛应用于含盐废水处理中。然而，这些过程伴随着严重的超细颗粒排放，这种现象与溶质跨越气液界面的转变有关。透彻理解溶质在气液界面上的行为对于澄清穿越过程和指导颗粒控制策略至关重要。在此，我们蒸发了含有饱和无机离子和腐殖质的溶液，在直接接触传热和传质过程的实验模拟中分析了它们在气液界面上的行为。结果发现，这些物质在该界面上共沉淀。腐殖质可通过化学键与无机离子结合，通过阳离子-π相互作用与一价离子结合，通过静电和螯合作用与二价离子结合。此外，腐殖质还可以作为无机晶体沉淀的成核场所。这些独特的结合机制使腐殖质与无机离子在沉淀过程中产生了协同作用。在沉淀过程中，主要富集的是腐殖化程度高、分子量大的腐殖质。无机离子是主要成分，占沉淀物总质量的 93% 以上。其中，富集系数为 2.10 的 Na+ 比二价离子更容易在气液界面沉淀。这些关于腐殖质和无机离子的结合机制及其沉淀特性的结论在膜浓缩浸出液的浸没燃烧蒸发过程中得到了验证。

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引用次数: 0

Synergistic integration of zeolite engineering and fixed-bed column design for enhanced biogas upgrading: Adsorbent synthesis, CO2/CH4 separation kinetics, and regeneration assessment 沸石工程与固定床塔设计的协同整合，促进沼气提质：吸附剂合成、CO2/CH4 分离动力学和再生评估

IF 8.1 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2024-09-19 DOI: 10.1016/j.seppur.2024.129772

Biogas, a renewable energy vector derived from anaerobic digestion of organic waste, requires CO₂ separation to enhance its calorific value for engine fuel. This study integrates CO₂/CH₄ separation in biogas using a novel approach integrating dual chemically-activated zeolites and fixed-bed column purification. Biogas produced via CSTR/ultrafiltration (69 % CH₄, 30 % CO₂, 14 ppm H₂S) was further upgraded using HCl + NaOH and H₂SO₄ + NaOH activated zeolites. Optimal absorption capacity of 97.77 ± 0.01 % was achieved at 140 mesh, 60-minute H₂SO₄ + NaOH activation, 2-hour calcination (400 °C), and 200 mL/min flow rate. Breakthrough was observed at 18.12 min. Langmuir isotherm (R² = 0.9992) and Elovich kinetics (R² = 0.9846) best described the adsorption process. XRD analysis showed significant crystal size reduction post-activation (53.31 nm to 16.90 nm). Notably, BET analysis revealed enhanced surface properties surface area of 286.71 m²/g, pore volume of 0.213 cc/g, and pore diameter of 3.532 Å. An innovative dual-column system with non-isothermal TSA protocol optimized CO₂ adsorption (30 mins) and desorption (17 mins, 40 °C, 100 mL/min), yielding superior near-pure methane biogas (99.29 % CH₄, 0.66 % CO₂, trace H₂S). A methane loss of 2.75 % during upgrading demonstrated high CO₂ selectivity. This synergistic approach presents a promising solution for sustainable biogas purification and engine fuel applications.

沼气是一种从有机废物厌氧消化中提取的可再生能源，需要进行二氧化碳分离以提高其作为发动机燃料的热值。本研究采用一种新型方法，将双重化学活化沸石和固定床柱净化结合起来，对沼气中的 CO2/CH4 进行分离。通过 CSTR/超滤产生的沼气（69 % CH4、30 % CO2、14 ppm H2S）使用 HCl + NaOH 和 H2SO4 + NaOH 活性沸石进行进一步提纯。在 140 目、60 分钟 H2SO4 + NaOH 活化、2 小时煅烧（400 °C）和 200 mL/min 流速条件下，达到了 97.77 ± 0.01 % 的最佳吸收能力。在 18.12 分钟时观察到突破。朗缪尔等温线（R2 = 0.9992）和埃洛维奇动力学（R2 = 0.9846）对吸附过程进行了最佳描述。XRD 分析表明，活化后晶体尺寸明显缩小（从 53.31 nm 减小到 16.90 nm）。创新的双柱系统与非等温 TSA 协议优化了二氧化碳吸附（30 分钟）和解吸（17 分钟，40 °C，100 mL/分钟），产生了优质的近纯甲烷生物气（99.29 % CH4、0.66 % CO2、痕量 H2S）。在提纯过程中，甲烷损失为 2.75%，这表明二氧化碳具有很高的选择性。这种协同方法为可持续的沼气净化和发动机燃料应用提供了一种前景广阔的解决方案。

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