Separation and Purification Technology最新文献_第9页

Nitrogen doping of porous carbons derived from CaCO3 nanofluids for enhanced CO2 adsorption. CaCO3纳米流体制备的多孔碳的氮掺杂增强CO2吸附。

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-27 DOI: 10.1016/j.seppur.2026.136961

Haiying Xiao , Mingdong Li , Ying Qin , Zhangfa TONG , Lishuo Li

Abstract

A sustainable and integrated strategy is developed for the synthesis of nitrogen-doped porous carbons (HNPCs) using organically modified CaCO₃ nanofluids as multifunctional precursors, and their CO₂ separation performance is systematically evaluated. Cubic and spherical CaCO₃ nanofluids were prepared using M2070 and KH560 as organic modifiers to form an organic crown-like structure, followed by programmed pyrolysis at 800 °C to obtain HNPCs. The obtained HNPCs exhibit well-developed porous structures with a high BET surface area of 777.3 m²·g⁻¹, a micropore volume of 0.0928 cm³·g⁻¹, and a nitrogen content of 2.79 wt% (elemental analysis). XPS analysis reveals that pyrrolic N (48.98%) and pyridinic N (26.47%) are the dominant nitrogen species, contributing to enhanced CO₂ adsorption affinity. The spherical CaCO₃-derived sample (SNPC(II)) shows superior CO₂ uptake capacities of 2.85 mmol·g⁻¹ at 25 °C and 3.98 mmol·g⁻¹ at 0 °C under 1 bar. The isosteric heat of adsorption ranges from 17.3 to 36.5 kJ·mol⁻¹, indicating a physisorption-dominated and energy-efficient process. Ideal Adsorbed Solution Theory predicts a CO₂/N₂ selectivity of 34.19 at 298 K and 1 bar. Fixed-bed breakthrough experiments using simulated flue gas (15 vol% CO₂/85 vol% N₂) demonstrate a CO₂ breakthrough time of 4631 s·g⁻¹, markedly longer than that of N₂ (342 s·g⁻¹). Moreover, SNPC(II) retains 98.7% of its initial CO₂ capacity after eight adsorption–desorption cycles, highlighting excellent cyclic stability.

摘要采用有机改性CaCO₃纳米流体作为多功能前驱体制备了氮掺杂多孔碳（HNPCs），并对其CO₂分离性能进行了系统评价。以M2070和KH560为有机改性剂制备立方和球形CaCO3纳米流体，形成有机冠状结构，然后在800℃下程序热解得到HNPCs。所得HNPCs具有良好的孔隙结构，BET表面积为777.3 m2·g−1，微孔体积为0.0928 cm3·g−1，含氮量为2.79 wt%（元素分析）。XPS分析表明，吡啶氮（48.98%）和吡啶氮（26.47%）是优势氮种，有助于增强CO 2的吸附亲和力。球形CaCO₃衍生样品（SNPC(II)）在1 bar下，在25℃下具有2.85 mmol·g−1的吸收率，在0℃下具有3.98 mmol·g−1的吸收率。等等吸附热范围为17.3 ~ 36.5 kJ·mol−1，表明该过程以物理吸附为主，节能高效。理想吸附溶液理论预测，在298 K和1 bar条件下，CO2/N2选择性为34.19。模拟烟气（15 vol% CO₂/85 vol% N₂）的固定床突破实验表明，CO₂的突破时间为4631 s·g−1，明显长于N₂的突破时间（342 s·g−1）。此外，SNPC（II）在8次吸附-解吸循环后仍能保持其初始CO₂容量的98.7%，表现出良好的循环稳定性。

{"title":"Nitrogen doping of porous carbons derived from CaCO3 nanofluids for enhanced CO2 adsorption.","authors":"Haiying Xiao , Mingdong Li , Ying Qin , Zhangfa TONG , Lishuo Li","doi":"10.1016/j.seppur.2026.136961","DOIUrl":"10.1016/j.seppur.2026.136961","url":null,"abstract":"<div><div>Abstract</div><div>A sustainable and integrated strategy is developed for the synthesis of nitrogen-doped porous carbons (HNPCs) using organically modified CaCO₃ nanofluids as multifunctional precursors, and their CO₂ separation performance is systematically evaluated. Cubic and spherical CaCO<sub>3</sub> nanofluids were prepared using M2070 and KH560 as organic modifiers to form an organic crown-like structure, followed by programmed pyrolysis at 800 °C to obtain HNPCs. The obtained HNPCs exhibit well-developed porous structures with a high BET surface area of 777.3 m<sup>2</sup>·g<sup>−1</sup>, a micropore volume of 0.0928 cm<sup>3</sup>·g<sup>−1</sup>, and a nitrogen content of 2.79 wt% (elemental analysis). XPS analysis reveals that pyrrolic N (48.98%) and pyridinic N (26.47%) are the dominant nitrogen species, contributing to enhanced CO₂ adsorption affinity. The spherical CaCO₃-derived sample (SNPC(II)) shows superior CO₂ uptake capacities of 2.85 mmol·g<sup>−1</sup> at 25 °C and 3.98 mmol·g<sup>−1</sup> at 0 °C under 1 bar. The isosteric heat of adsorption ranges from 17.3 to 36.5 kJ·mol<sup>−1</sup>, indicating a physisorption-dominated and energy-efficient process. Ideal Adsorbed Solution Theory predicts a CO<sub>2</sub>/N<sub>2</sub> selectivity of 34.19 at 298 K and 1 bar. Fixed-bed breakthrough experiments using simulated flue gas (15 vol% CO₂/85 vol% N₂) demonstrate a CO₂ breakthrough time of 4631 s·g<sup>−1</sup>, markedly longer than that of N₂ (342 s·g<sup>−1</sup>). Moreover, SNPC(II) retains 98.7% of its initial CO₂ capacity after eight adsorption–desorption cycles, highlighting excellent cyclic stability.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"391 ","pages":"Article 136961"},"PeriodicalIF":9.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146077284","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

Artificial intelligence-accelerated solvent screening for CO₂ capture in rotating packed beds: Economic impact and decision-support insights 旋转填料床中CO₂捕获的人工智能加速溶剂筛选：经济影响和决策支持见解

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-27 DOI: 10.1016/j.seppur.2026.137013

Mohammadu Bello Danbatta , Nasser Ahmed Al-Azri , Muhammad Abdul Qyyum , Nabeel Al-Rawahi

Rotating packed beds (RPBs) offer a compact and energy-efficient alternative to conventional absorbers for post-combustion CO₂ capture; however, their large-scale deployment is limited by the time and cost required for solvent evaluation and operational optimization. This study introduces an artificial intelligence-enabled framework that couples solvent selection with process-condition optimization to enhance CO₂ absorption performance in RPB systems. The framework combines machine-learning and reinforcement-learning methods to represent key RPB parameters, including revolution speed, gas–liquid flow ratios, solvent concentration, and temperature. It achieved a predictive accuracy of 92.8%, improving performance by more than 110% compared with conventional approaches, and enabled rapid identification of optimum solvent-operation pairs under realistic industrial ranges. The framework reduced evaluation time from weeks to hours while maintaining physical consistency and engineering reliability. When applied to process-level assessment, the AI-enabled configuration lowered capital and operating costs by 40% and 30%, respectively, and decreased the levelized cost of CO₂ capture from $63 to $40 per ton of CO₂. The economic advantage further widens under elevated energy prices, highlighting the framework's robustness and scalability. Integrating artificial intelligence with process-intensification principles, therefore, offers a practical pathway toward faster, cost-effective, and industrially viable RPB-based carbon capture.

旋转填充床（rpb）提供了一种紧凑和节能的替代传统的吸收器，用于燃烧后的二氧化碳捕获；然而，它们的大规模部署受到溶剂评估和操作优化所需的时间和成本的限制。本研究引入了一种人工智能框架，将溶剂选择与工艺条件优化相结合，以提高RPB系统的CO 2吸收性能。该框架结合了机器学习和强化学习方法来表示关键的RPB参数，包括转速、气液流量比、溶剂浓度和温度。与传统方法相比，该方法的预测准确率达到92.8%，提高了110%以上，并能够在实际工业范围内快速识别最佳溶剂操作对。该框架在保持物理一致性和工程可靠性的同时，将评估时间从数周减少到数小时。当应用于流程级评估时，启用人工智能的配置将资本和运营成本分别降低了40%和30%，并将二氧化碳捕获的平均成本从每吨63美元降至40美元。在能源价格上涨的情况下，经济优势进一步扩大，凸显了该框架的稳健性和可扩展性。因此，将人工智能与过程强化原理相结合，为实现更快、更具成本效益和工业上可行的基于rpb的碳捕获提供了一条切实可行的途径。

{"title":"Artificial intelligence-accelerated solvent screening for CO₂ capture in rotating packed beds: Economic impact and decision-support insights","authors":"Mohammadu Bello Danbatta , Nasser Ahmed Al-Azri , Muhammad Abdul Qyyum , Nabeel Al-Rawahi","doi":"10.1016/j.seppur.2026.137013","DOIUrl":"10.1016/j.seppur.2026.137013","url":null,"abstract":"<div><div>Rotating packed beds (RPBs) offer a compact and energy-efficient alternative to conventional absorbers for post-combustion CO₂ capture; however, their large-scale deployment is limited by the time and cost required for solvent evaluation and operational optimization. This study introduces an artificial intelligence-enabled framework that couples solvent selection with process-condition optimization to enhance CO₂ absorption performance in RPB systems. The framework combines machine-learning and reinforcement-learning methods to represent key RPB parameters, including revolution speed, gas–liquid flow ratios, solvent concentration, and temperature. It achieved a predictive accuracy of 92.8%, improving performance by more than 110% compared with conventional approaches, and enabled rapid identification of optimum solvent-operation pairs under realistic industrial ranges. The framework reduced evaluation time from weeks to hours while maintaining physical consistency and engineering reliability. When applied to process-level assessment, the AI-enabled configuration lowered capital and operating costs by 40% and 30%, respectively, and decreased the levelized cost of CO₂ capture from $63 to $40 per ton of CO₂. The economic advantage further widens under elevated energy prices, highlighting the framework's robustness and scalability. Integrating artificial intelligence with process-intensification principles, therefore, offers a practical pathway toward faster, cost-effective, and industrially viable RPB-based carbon capture.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"391 ","pages":"Article 137013"},"PeriodicalIF":9.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146077130","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 surface modification of 3D-printed biopolymer filter via acetone treatment for enhanced copper hexacyanoferrate immobilization and selective ammonium capture 丙酮处理对3d打印生物聚合物过滤器表面的简单改性，以增强六氰亚铁酸铜的固定化和选择性铵捕获

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-27 DOI: 10.1016/j.seppur.2026.137057

Narges Dehbashi Nia , Bokseong Kim , Yuhoon Hwang

Ammonium contamination poses a significant environmental concern due to its adverse impacts on aquatic ecosystems, including oxygen depletion, reproductive disorders in aquatic organisms, and the proliferation of harmful algal blooms that release toxic compounds. These effects deteriorate water quality and threaten ecosystem stability, underscoring the need for effective and selective ammonium removal strategies. In this study, copper hexacyanoferrate (CuHCF), a Prussian blue analogue with strong affinity for ammonium ions, was immobilized onto acetone-pretreated three-dimensional (3D)-printed polylactic acid (PLA) filters. Acetone pretreatment chemically etched the PLA surface, increasing surface porosity and hydrophilicity, thereby enhancing surface reactivity for subsequent functionalization and CuHCF immobilization. This surface engineering strategy enabled uniform and stable distribution of CuHCF particles on the biopolymer scaffold, resulting in improved adsorption performance and structural stability. The fabricated filter exhibited an ammonium adsorption capacity of 1.91 mg/g and maintained over 90% regeneration efficiency across five adsorption–desorption cycles. Continuous column experiments further demonstrated stable operation for up to 40 h without significant performance deterioration. Overall, this work presents a simple and scalable approach for fabricating 3D-structured adsorbents via acetone-assisted surface modification, offering a practical platform for selective ammonium recovery and resource-oriented water treatment applications.

铵污染由于其对水生生态系统的不利影响，包括氧气消耗，水生生物的生殖障碍以及释放有毒化合物的有害藻华的增殖，引起了重大的环境问题。这些影响使水质恶化，威胁生态系统的稳定，强调需要有效和选择性的铵去除策略。在这项研究中，六氰高铁酸铜（CuHCF）是一种对铵离子具有强亲和力的普鲁士蓝类似物，它被固定在丙酮预处理的三维（3D）打印聚乳酸（PLA）过滤器上。丙酮预处理化学蚀刻PLA表面，增加表面孔隙度和亲水性，从而提高表面反应性，为后续的功能化和CuHCF固定提供支持。这种表面工程策略使得CuHCF颗粒在生物聚合物支架上均匀稳定地分布，从而提高了吸附性能和结构稳定性。制备的过滤器对铵的吸附量为1.91 mg/g，在5次吸附-解吸循环中保持了90%以上的再生效率。连续柱实验进一步证明稳定运行高达40 h，没有明显的性能下降。总的来说，这项工作提出了一种简单且可扩展的方法，通过丙酮辅助表面改性来制造3d结构吸附剂，为选择性铵回收和资源型水处理应用提供了一个实用的平台。

{"title":"Facile surface modification of 3D-printed biopolymer filter via acetone treatment for enhanced copper hexacyanoferrate immobilization and selective ammonium capture","authors":"Narges Dehbashi Nia , Bokseong Kim , Yuhoon Hwang","doi":"10.1016/j.seppur.2026.137057","DOIUrl":"10.1016/j.seppur.2026.137057","url":null,"abstract":"<div><div>Ammonium contamination poses a significant environmental concern due to its adverse impacts on aquatic ecosystems, including oxygen depletion, reproductive disorders in aquatic organisms, and the proliferation of harmful algal blooms that release toxic compounds. These effects deteriorate water quality and threaten ecosystem stability, underscoring the need for effective and selective ammonium removal strategies. In this study, copper hexacyanoferrate (CuHCF), a Prussian blue analogue with strong affinity for ammonium ions, was immobilized onto acetone-pretreated three-dimensional (3D)-printed polylactic acid (PLA) filters. Acetone pretreatment chemically etched the PLA surface, increasing surface porosity and hydrophilicity, thereby enhancing surface reactivity for subsequent functionalization and CuHCF immobilization. This surface engineering strategy enabled uniform and stable distribution of CuHCF particles on the biopolymer scaffold, resulting in improved adsorption performance and structural stability. The fabricated filter exhibited an ammonium adsorption capacity of 1.91 mg/g and maintained over 90% regeneration efficiency across five adsorption–desorption cycles. Continuous column experiments further demonstrated stable operation for up to 40 h without significant performance deterioration. Overall, this work presents a simple and scalable approach for fabricating 3D-structured adsorbents <em>via</em> acetone-assisted surface modification, offering a practical platform for selective ammonium recovery and resource-oriented water treatment applications.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"391 ","pages":"Article 137057"},"PeriodicalIF":9.0,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048748","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

Model development and flux improvement for separating particle/macromolecule binary suspension by cross-flow microfiltration 交叉流微滤分离颗粒/大分子二元悬浮液的模型建立及通量改进

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137046

Su-En Wu , Ching-Ting Lin , Yen-Ting Chen

Seawater desalination is an essential approach to achieve a sustainable water supply amid increasing global water demand and freshwater scarcity. However, membrane fouling during pretreatment greatly impairs filtration performance and operational efficiency. Therefore, this study aims to develop a model to analyze and enhance flux performance during cross-flow microfiltration of a binary suspension containing inorganic particles and macromolecules in seawater pretreatment. The effects of cross-flow velocity and operational pressure on filtration flux, fouling resistance, cake properties, and solute rejection were examined. The results showed that cross-flow velocity exerted a stronger influence than transmembrane pressure (TMP), with higher velocities reducing cake resistance by up to 58.44% at 75 kPa owing to increased shear stress. An empirical model based on a force balance and resistance analysis was established, and semi-empirical equations were developed to predict filtration flux, cake thickness, and macromolecule rejection under various hydrodynamic conditions. Furthermore, a self-cleaning backwash strategy was evaluated, and a 12-min backwash cycle was found optimal for balancing fouling control and energy efficiency. These findings offer valuable insights into hydrodynamic behavior and fouling control, providing practical guidance for designing sustainable seawater pretreatment processes.

在全球用水需求不断增加和淡水短缺的情况下，海水淡化是实现可持续供水的重要途径。然而，预处理过程中的膜污染严重影响了过滤性能和操作效率。因此，本研究旨在建立一个模型来分析和提高海水预处理中含无机颗粒和大分子的二元悬浮液的交叉流微滤通量性能。考察了横流速度和操作压力对过滤通量、结垢阻力、滤饼性能和截留溶质的影响。结果表明，在75 kPa时，由于剪切应力的增加，横向流动速度对滤饼阻力的影响强于跨膜压力（TMP），较高的横向流动速度可使滤饼阻力降低58.44%。建立了基于力平衡和阻力分析的经验模型，并建立了半经验方程来预测不同水动力条件下的过滤通量、滤饼厚度和大分子截留。此外，对自清洁反冲洗策略进行了评估，并发现12分钟的反冲洗周期是平衡污染控制和能源效率的最佳选择。这些发现为水动力行为和污垢控制提供了有价值的见解，为设计可持续的海水预处理工艺提供了实用指导。

{"title":"Model development and flux improvement for separating particle/macromolecule binary suspension by cross-flow microfiltration","authors":"Su-En Wu , Ching-Ting Lin , Yen-Ting Chen","doi":"10.1016/j.seppur.2026.137046","DOIUrl":"10.1016/j.seppur.2026.137046","url":null,"abstract":"<div><div>Seawater desalination is an essential approach to achieve a sustainable water supply amid increasing global water demand and freshwater scarcity. However, membrane fouling during pretreatment greatly impairs filtration performance and operational efficiency. Therefore, this study aims to develop a model to analyze and enhance flux performance during cross-flow microfiltration of a binary suspension containing inorganic particles and macromolecules in seawater pretreatment. The effects of cross-flow velocity and operational pressure on filtration flux, fouling resistance, cake properties, and solute rejection were examined. The results showed that cross-flow velocity exerted a stronger influence than transmembrane pressure (TMP), with higher velocities reducing cake resistance by up to 58.44% at 75 kPa owing to increased shear stress. An empirical model based on a force balance and resistance analysis was established, and semi-empirical equations were developed to predict filtration flux, cake thickness, and macromolecule rejection under various hydrodynamic conditions. Furthermore, a self-cleaning backwash strategy was evaluated, and a 12-min backwash cycle was found optimal for balancing fouling control and energy efficiency. These findings offer valuable insights into hydrodynamic behavior and fouling control, providing practical guidance for designing sustainable seawater pretreatment processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137046"},"PeriodicalIF":9.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075608","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

Engineering a millimeter-scale packed bed reactor with porous calcium-alginate particles for intensified continuous-flow catalytic ozonation of ATZ 设计一个毫米级的多孔海藻酸钙填充床反应器，用于强化连续流催化臭氧氧化ATZ

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.136904

Yafang Zhang , Wenqi Fang , Gaoyan Shao , Yuming Tu , Chencan Du , Zhongqi Ren

The limited mass transfer efficiency at the three-phase interface remains a major challenge for the industrial application of catalytic ozonation processes. To address this kinetic limitation, this study proposes a catalytic system that combines structurally optimized Ca²⁺ cross-linked sodium alginate spheres (Ca@SA-LSR-PEG200) with a millimeter-scale packed bed reactor (mPBR). The mesoporous structure (32.61 nm) is formed through the incorporation of polyethylene glycol (PEG200) and liquid silica gel (LSR), which contributes to the mechanical stability. The integration of Ca@SA-LSR-PEG200 with the mPBR significantly improves the gas–liquid–solid contact efficiency, achieving 100% atrazine (ATZ) removal within a short residence time of 11 s. Compared to conventional bubble columns, the apparent rate constant (k = 0.81 s⁻¹) is enhanced by two to three orders of magnitude. Mechanism investigations reveal that the CaO sites and delocalized π electrons present in carbon defects facilitate the decomposition of ozone, thereby promoting the generation of reactive oxygen species (¹O₂, ·OH, ·O₂⁻), which are responsible for ATZ degradation. The system demonstrates excellent operational stability over a 100-h testing period, with an efficiency loss of less than 5%, primarily due to the protective role of the LSR framework in preventing metal leaching. This work offers valuable insights into the mass transfer limitations in catalytic ozonation and presents a scalable solution for the continuous removal of persistent organic pollutants.

在三相界面上有限的传质效率仍然是催化臭氧化工艺工业应用的主要挑战。为了解决这一动力学限制，本研究提出了一种催化系统，该系统将结构优化的Ca2+交联海藻酸钠球（Ca@SA-LSR-PEG200）与毫米级填充床反应器（mPBR）相结合。通过聚乙二醇（PEG200）和液态硅胶（LSR）的掺入，形成了32.61 nm的介孔结构，提高了材料的机械稳定性。Ca@SA-LSR-PEG200与mPBR的集成显著提高了气液固接触效率，在11 s的短停留时间内实现了100%的阿特拉津（ATZ）去除。与传统的气泡柱相比，表观速率常数（k = 0.81 s−1）提高了两到三个数量级。机理研究表明，碳缺陷中存在的CaO位点和离域π电子促进了臭氧的分解，从而促进了活性氧（1O2，·OH，·O2−）的生成，这些活性氧负责ATZ的降解。在100小时的测试期间，该系统表现出出色的运行稳定性，效率损失低于5%，这主要归功于LSR框架在防止金属浸出方面的保护作用。这项工作为催化臭氧化的传质限制提供了有价值的见解，并为持续去除持久性有机污染物提供了可扩展的解决方案。

{"title":"Engineering a millimeter-scale packed bed reactor with porous calcium-alginate particles for intensified continuous-flow catalytic ozonation of ATZ","authors":"Yafang Zhang , Wenqi Fang , Gaoyan Shao , Yuming Tu , Chencan Du , Zhongqi Ren","doi":"10.1016/j.seppur.2026.136904","DOIUrl":"10.1016/j.seppur.2026.136904","url":null,"abstract":"<div><div>The limited mass transfer efficiency at the three-phase interface remains a major challenge for the industrial application of catalytic ozonation processes. To address this kinetic limitation, this study proposes a catalytic system that combines structurally optimized Ca<sup>2+</sup> cross-linked sodium alginate spheres (Ca@SA-LSR-PEG200) with a millimeter-scale packed bed reactor (mPBR). The mesoporous structure (32.61 nm) is formed through the incorporation of polyethylene glycol (PEG200) and liquid silica gel (LSR), which contributes to the mechanical stability. The integration of Ca@SA-LSR-PEG200 with the mPBR significantly improves the gas–liquid–solid contact efficiency, achieving 100% atrazine (ATZ) removal within a short residence time of 11 s. Compared to conventional bubble columns, the apparent rate constant (<em>k</em> = 0.81 s<sup>−1</sup>) is enhanced by two to three orders of magnitude. Mechanism investigations reveal that the Ca<img>O sites and delocalized π electrons present in carbon defects facilitate the decomposition of ozone, thereby promoting the generation of reactive oxygen species (<sup>1</sup>O<sub>2</sub>, ·OH, ·O<sub>2</sub><sup>−</sup>), which are responsible for ATZ degradation. The system demonstrates excellent operational stability over a 100-h testing period, with an efficiency loss of less than 5%, primarily due to the protective role of the LSR framework in preventing metal leaching. This work offers valuable insights into the mass transfer limitations in catalytic ozonation and presents a scalable solution for the continuous removal of persistent organic pollutants.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 136904"},"PeriodicalIF":9.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075740","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

Rational molecular tuning of SPEEK membranes for high-performance zinc-iron flow batteries and electrodialysis 高性能锌铁液流电池和电渗析用SPEEK膜的合理分子调谐

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137041

Zhenle Gan , Xu He , Song Ge , Xuhao Wei , Wei Qian , Wu Kuang , Cuimiao Zhang , Chunli Song , Benfa Chu , Zhongbiao Zhang

The advancement of high-performance, low-cost ion exchange membranes (IEMs) is pivotal for enabling a sustainable energy future and ensuring safe water supplies. This study reports the synthesis and characterization of a sulfonated poly(ether ether ketone) (SPEEK) membrane through copolymerization with pre-sulfonated monomers and fluorene-based constituents. The synthetic strategy allows precise regulation of the sulfonation degree and improves membrane robustness. The obtained membranes exhibit an optimal combination of properties, including moderate water uptake, limited swelling, high ionic conductivity, along with excellent mechanical and thermal stability. The m-SPEEK-FDH membrane was systematically applied in two distinct technologies: Zinc‑iron redox flow batteries (AZIFB) and electrodialysis (ED). In AZIFB applications, the 0.6-SPEEK-FDH membrane demonstrates excellent performance. It achieves an energy efficiency exceeding 79.4% even at a high current density of 400 mA cm⁻². Meanwhile, it exhibits exceptional long-term cycling stability, maintaining an energy efficiency above 84.4% throughout a test of over 950 cycles that spanned 18 days at 200 mA cm⁻². The investigation demonstrates that ED with the treated 0.6-SPEEK-FDH also exhibits high desalination efficiencies (up to 97%) with low energy consumption (<4.5 kWh·kg⁻¹). The incorporation of rigid fluorene units with a tunable degree of sulfonation offers a viable approach to tailor-made CEMs, showcasing significant potential for both zinc‑iron flow batteries and electrodialysis processes.

高性能、低成本离子交换膜（IEMs）的发展对于实现可持续能源的未来和确保安全的水供应至关重要。本研究报道了通过预磺化单体和芴基组分共聚合成磺化聚醚醚酮（SPEEK）膜。该合成策略可以精确调节磺化程度，提高膜的鲁棒性。所获得的膜表现出最佳的性能组合，包括适度的吸水，有限的膨胀，高离子电导率，以及优异的机械和热稳定性。m-SPEEK-FDH膜系统地应用于两种不同的技术：锌-铁氧化还原液流电池（AZIFB）和电渗析（ED）。在AZIFB应用中，0.6-SPEEK-FDH膜表现出优异的性能。即使在400 mA cm−2的高电流密度下，其能量效率也超过79.4%。同时，它表现出优异的长期循环稳定性，在200毫安厘米−2下持续18天的超过950次循环测试中，能源效率保持在84.4%以上。研究表明，经处理的0.6-SPEEK-FDH的ED也具有高脱盐效率（高达97%）和低能耗（<4.5 kWh·kg−1）。结合具有可调磺化程度的刚性芴单元，为定制CEMs提供了一种可行的方法，展示了锌铁液流电池和电渗析工艺的巨大潜力。

{"title":"Rational molecular tuning of SPEEK membranes for high-performance zinc-iron flow batteries and electrodialysis","authors":"Zhenle Gan , Xu He , Song Ge , Xuhao Wei , Wei Qian , Wu Kuang , Cuimiao Zhang , Chunli Song , Benfa Chu , Zhongbiao Zhang","doi":"10.1016/j.seppur.2026.137041","DOIUrl":"10.1016/j.seppur.2026.137041","url":null,"abstract":"<div><div>The advancement of high-performance, low-cost ion exchange membranes (IEMs) is pivotal for enabling a sustainable energy future and ensuring safe water supplies. This study reports the synthesis and characterization of a sulfonated poly(ether ether ketone) (SPEEK) membrane through copolymerization with pre-sulfonated monomers and fluorene-based constituents. The synthetic strategy allows precise regulation of the sulfonation degree and improves membrane robustness. The obtained membranes exhibit an optimal combination of properties, including moderate water uptake, limited swelling, high ionic conductivity, along with excellent mechanical and thermal stability. The m-SPEEK-FDH membrane was systematically applied in two distinct technologies: Zinc‑iron redox flow batteries (AZIFB) and electrodialysis (ED). In AZIFB applications, the 0.6-SPEEK-FDH membrane demonstrates excellent performance. It achieves an energy efficiency exceeding 79.4% even at a high current density of 400 mA cm<sup>−2</sup>. Meanwhile, it exhibits exceptional long-term cycling stability, maintaining an energy efficiency above 84.4% throughout a test of over 950 cycles that spanned 18 days at 200 mA cm<sup>−2</sup>. The investigation demonstrates that ED with the treated 0.6-SPEEK-FDH also exhibits high desalination efficiencies (up to 97%) with low energy consumption (<4.5 kWh·kg<sup>−1</sup>). The incorporation of rigid fluorene units with a tunable degree of sulfonation offers a viable approach to tailor-made CEMs, showcasing significant potential for both zinc‑iron flow batteries and electrodialysis processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137041"},"PeriodicalIF":9.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075654","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

Probing the fouling induced by biomolecules of a polymer microfiltration membrane using 3D cryo-FIB/SEM 利用三维冷冻fib /SEM研究生物分子对聚合物微滤膜的污染

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137045

Hélène Roberge , Philippe Moreau , Estelle Couallier , Patricia Abellan

Membrane fouling is the main technical limitation to membrane filtration processes aimed at effectively separating valuable biomolecules from microalgae solutions. Although several fouling mechanisms have been proposed, they have rarely been directly observed. In this work, we demonstrate the direct nanometer-scale visualization of fouling both inside and on the surface of membranes. To mimic the microfiltration of real bioresource extracts, model solutions of lipids, proteins, and their mixtures were filtered, and the consecutively fouled membranes were analysed and reconstructed in 3D at high resolution using cryogenic focused ion beam coupled with scanning electron microscopy (cryo-FIB/SEM). Nanometer-scale analysis using deep learning segmentation tools (random forest combined with U-net model) uncovers membrane fouling mechanisms previously hypothesized, providing insights into how filtration depends on complex mixture composition. A quantitative analysis of the pores that are fouled or blocked, and open pores that can actively contribute to filtration is established. The methodology presented in this work provides directly probed, relevant information on membrane fouling structures that are scarcely accessible by other means, with broad applications to filtration processes in both industry and biotechnology research.

膜污染是膜过滤过程的主要技术限制，膜过滤过程旨在有效地从微藻溶液中分离有价值的生物分子。虽然提出了几种结垢机制，但它们很少被直接观察到。在这项工作中，我们展示了在纳米尺度上对膜内部和表面污垢的直接可视化。为了模拟真实生物资源提取物的微过滤，我们对脂质、蛋白质及其混合物的模型溶液进行了过滤，并利用低温聚焦离子束和扫描电镜（cro - fib /SEM）在高分辨率下对连续污染的膜进行了三维分析和重建。使用深度学习分割工具（随机森林与U-net模型相结合）的纳米尺度分析揭示了之前假设的膜污染机制，为过滤如何依赖于复杂的混合物组成提供了见解。对被污染或堵塞的孔隙和能够积极促进过滤的开放孔隙进行定量分析。在这项工作中提出的方法提供了直接探测的膜污染结构的相关信息，这些信息很难通过其他方式获得，在工业和生物技术研究的过滤过程中具有广泛的应用。

{"title":"Probing the fouling induced by biomolecules of a polymer microfiltration membrane using 3D cryo-FIB/SEM","authors":"Hélène Roberge , Philippe Moreau , Estelle Couallier , Patricia Abellan","doi":"10.1016/j.seppur.2026.137045","DOIUrl":"10.1016/j.seppur.2026.137045","url":null,"abstract":"<div><div>Membrane fouling is the main technical limitation to membrane filtration processes aimed at effectively separating valuable biomolecules from microalgae solutions. Although several fouling mechanisms have been proposed, they have rarely been directly observed. In this work, we demonstrate the direct nanometer-scale visualization of fouling both inside and on the surface of membranes. To mimic the microfiltration of real bioresource extracts, model solutions of lipids, proteins, and their mixtures were filtered, and the consecutively fouled membranes were analysed and reconstructed in 3D at high resolution using cryogenic focused ion beam coupled with scanning electron microscopy (cryo-FIB/SEM). Nanometer-scale analysis using deep learning segmentation tools (random forest combined with U-net model) uncovers membrane fouling mechanisms previously hypothesized, providing insights into how filtration depends on complex mixture composition. A quantitative analysis of the pores that are fouled or blocked, and open pores that can actively contribute to filtration is established. The methodology presented in this work provides directly probed, relevant information on membrane fouling structures that are scarcely accessible by other means, with broad applications to filtration processes in both industry and biotechnology research.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137045"},"PeriodicalIF":9.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075435","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

A two-step precipitation strategy for zinc recovery and magnesium control in sulfate solutions: process optimization and mechanistic insights 硫酸盐溶液中锌回收和镁控制的两步沉淀策略：工艺优化和机理见解

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-26 DOI: 10.1016/j.seppur.2026.137047

Zhimei Xia, Jing He, Caiyi Wang, Weihuan Xia, Shengjie Yi, Longgang Ye, Shufen Liu, Li Zhang, Yujie Hu

The accumulation of magnesium in zinc hydrometallurgy systems poses significant challenges to process efficiency and product quality. Existing removal methods often suffer from low selectivity, high energy consumption, or environmental concerns. This study proposes a novel two-step precipitation strategy using sodium bicarbonate for selective zinc recovery and magnesium control from purified zinc sulfate solution (PZSS). Under optimized conditions (1 mol/L NaHCO₃, 100% stoichiometric NaHCO₃ relative to Zn²⁺, 35 °C, 5 h, and 14 mL/min feed rate), Zn was recovered as ZnCO₃ with a high recovery rate of 99.86% and a low magnesium co-precipitation of only 1.64%. Subsequent magnesium removal using ammonia water achieved over 92% efficiency. The selective precipitation mechanism is attributed to the large solubility difference between ZnCO₃ and MgCO₃ under neutral pH conditions, coupled with the kinetic preference for ZnCO₃ nucleation, as elucidated by species distribution analysis, XRD, and SEM-EDS. This method provides an efficient, environmentally friendly alternative for magnesium management in zinc hydrometallurgy.

锌湿法冶金系统中镁的积累对工艺效率和产品质量提出了重大挑战。现有的去除方法往往存在选择性低、能耗高或环境问题。本研究提出了一种利用碳酸氢钠对纯化硫酸锌溶液（PZSS）进行选择性锌回收和镁控制的新型两步沉淀策略。优化条件为：NaHCO3浓度为1 mol/L， NaHCO3相对于Zn2+浓度为100%，加料温度为35℃，加料时间为5 h，加料速率为14 mL/min。在此条件下，锌以ZnCO3的形式回收，回收率高达99.86%，镁共析出率仅为1.64%。随后使用氨水去除镁的效率达到92%以上。通过物种分布分析、XRD和SEM-EDS分析，发现选择性沉淀机制是由于中性pH条件下ZnCO3和MgCO3的溶解度差异较大，加之动力学倾向于ZnCO3成核。该方法为湿法锌冶炼中镁的管理提供了一种高效、环保的替代方法。

{"title":"A two-step precipitation strategy for zinc recovery and magnesium control in sulfate solutions: process optimization and mechanistic insights","authors":"Zhimei Xia, Jing He, Caiyi Wang, Weihuan Xia, Shengjie Yi, Longgang Ye, Shufen Liu, Li Zhang, Yujie Hu","doi":"10.1016/j.seppur.2026.137047","DOIUrl":"10.1016/j.seppur.2026.137047","url":null,"abstract":"<div><div>The accumulation of magnesium in zinc hydrometallurgy systems poses significant challenges to process efficiency and product quality. Existing removal methods often suffer from low selectivity, high energy consumption, or environmental concerns. This study proposes a novel two-step precipitation strategy using sodium bicarbonate for selective zinc recovery and magnesium control from purified zinc sulfate solution (PZSS). Under optimized conditions (1 mol/L NaHCO<sub>3</sub>, 100% stoichiometric NaHCO<sub>3</sub> relative to Zn<sup>2+</sup>, 35 °C, 5 h, and 14 mL/min feed rate), Zn was recovered as ZnCO<sub>3</sub> with a high recovery rate of 99.86% and a low magnesium co-precipitation of only 1.64%. Subsequent magnesium removal using ammonia water achieved over 92% efficiency. The selective precipitation mechanism is attributed to the large solubility difference between ZnCO<sub>3</sub> and MgCO<sub>3</sub> under neutral pH conditions, coupled with the kinetic preference for ZnCO<sub>3</sub> nucleation, as elucidated by species distribution analysis, XRD, and SEM-EDS. This method provides an efficient, environmentally friendly alternative for magnesium management in zinc hydrometallurgy.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"391 ","pages":"Article 137047"},"PeriodicalIF":9.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146077286","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

Machine learning–driven identification of key factors governing hormone adsorption by agrifood waste–derived adsorbents 机器学习驱动的农业食品垃圾吸附剂对激素吸附的关键因素识别

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137033

Masud Parvez , Ahasanul Karim , Zarifeh Raji , Isa Ebtehaj , Hossein Bonakdari , Seddik Khalloufi

Hormone contamination in aquatic systems threatens human health and ecosystems, demanding efficient and sustainable separation strategies. This study aims to develop a machine learning (ML) framework to predict hormone adsorption using agrifood waste-derived adsorbents and to identify the key variables governing adsorption efficiency. A dataset of 604 observations with nine input variables was compiled from peer-reviewed studies. Three ensemble ML algorithms—Random Forest (RF), Least Squares Boosting, and M5 model trees—were evaluated across 511 models generated from all combinations of one to nine input variables. RF demonstrated the highest predictive accuracy, achieving a maximum test coefficient of determination (R²) of 0.976 and a minimum mean absolute error of 4.26 using eight input variables. Model robustness was assessed using a Combined Index (CI) integrating six statistical metrics, which decreased from a median value of 0.78 for single-input models to 0.0006 for the optimal eight-input configuration; the full nine-input model yielded CI = 0.0019. Bayesian optimization using the Expected Improvement per Second acquisition function further improved model performance, producing the highest test Nash–Sutcliffe efficiency (0.951) and the lowest normalized root mean square error (0.162) and ratio of root mean square error to standard deviation (0.221). Feature importance analysis identified initial concentration, contact time, pH, and adsorbent-to-solution ratio as the most influential predictors of adsorption efficiency. Hormone-specific analyses for 17β-estradiol (318 data points) and 17α-ethinylestradiol (106 data points) confirmed the robustness of these findings. The results show that optimized ML models support the design of sustainable adsorption-based hormone removal systems.

水生系统中的激素污染威胁着人类健康和生态系统，需要有效和可持续的分离策略。本研究旨在开发一个机器学习（ML）框架，以预测使用农业食品垃圾衍生吸附剂的激素吸附，并确定控制吸附效率的关键变量。从同行评议的研究中编译了604个观察结果和9个输入变量的数据集。三种集成ML算法——随机森林（RF）、最小二乘增强和M5模型树——在511个模型中进行了评估，这些模型是由1到9个输入变量的所有组合生成的。RF具有最高的预测精度，8个输入变量的最大检验决定系数（R2）为0.976，最小平均绝对误差为4.26。模型稳健性评估采用综合六个统计指标的综合指数（CI），从单输入模型的中位数0.78下降到最佳八输入配置的0.0006；完整的9个输入模型的CI = 0.0019。贝叶斯优化利用每秒预期改进（Expected Improvement per Second）获取函数进一步提高了模型的性能，产生最高的检验Nash-Sutcliffe效率（0.951），最低的归一化均方根误差（0.162）和均方根误差与标准差之比（0.221）。特征重要性分析表明，初始浓度、接触时间、pH值和吸附剂与溶液的比例是影响吸附效率的最重要因素。对17β-雌二醇（318个数据点）和17α-炔雌醇（106个数据点）的激素特异性分析证实了这些发现的稳健性。结果表明，优化的ML模型支持基于可持续吸附的激素去除系统的设计。

{"title":"Machine learning–driven identification of key factors governing hormone adsorption by agrifood waste–derived adsorbents","authors":"Masud Parvez , Ahasanul Karim , Zarifeh Raji , Isa Ebtehaj , Hossein Bonakdari , Seddik Khalloufi","doi":"10.1016/j.seppur.2026.137033","DOIUrl":"10.1016/j.seppur.2026.137033","url":null,"abstract":"<div><div>Hormone contamination in aquatic systems threatens human health and ecosystems, demanding efficient and sustainable separation strategies. This study aims to develop a machine learning (ML) framework to predict hormone adsorption using agrifood waste-derived adsorbents and to identify the key variables governing adsorption efficiency. A dataset of 604 observations with nine input variables was compiled from peer-reviewed studies. Three ensemble ML algorithms—Random Forest (RF), Least Squares Boosting, and M5 model trees—were evaluated across 511 models generated from all combinations of one to nine input variables. RF demonstrated the highest predictive accuracy, achieving a maximum test coefficient of determination (R<sup>2</sup>) of 0.976 and a minimum mean absolute error of 4.26 using eight input variables. Model robustness was assessed using a Combined Index (CI) integrating six statistical metrics, which decreased from a median value of 0.78 for single-input models to 0.0006 for the optimal eight-input configuration; the full nine-input model yielded CI = 0.0019. Bayesian optimization using the Expected Improvement per Second acquisition function further improved model performance, producing the highest test Nash–Sutcliffe efficiency (0.951) and the lowest normalized root mean square error (0.162) and ratio of root mean square error to standard deviation (0.221). Feature importance analysis identified initial concentration, contact time, pH, and adsorbent-to-solution ratio as the most influential predictors of adsorption efficiency. Hormone-specific analyses for 17β-estradiol (318 data points) and 17α-ethinylestradiol (106 data points) confirmed the robustness of these findings. The results show that optimized ML models support the design of sustainable adsorption-based hormone removal systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"391 ","pages":"Article 137033"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146077285","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

La vacancy-induced enhancement of CoO and oxygen vacancy for efficient chlorobenzene oxidation La空位诱导CoO和氧空位增强对氯苯的有效氧化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2026-01-25 DOI: 10.1016/j.seppur.2026.137035

Mingjiao Tian , Yaruo Zhao , Qin Yang , Changwei Chen , Han Xu , Dong Guo , Zeyu Jiang , Haohua Kang , Shan Ren , Chi He

The environmentally friendly purification of chlorinated volatile organic compounds (CVOCs) is a challenge in current air pollution control. Construction of active oxygen species on the catalyst surface is a promising strategy to promote the cleavage of CCl bond and the destruction of CVOC molecules. Herein, an oxygen-vacancy-rich perovskite-type 3LaCoO₃ catalyst was constructed for the efficient catalytic oxidation of chlorobenzene (CB). The partial removal of La in 3LaCoO₃ structure effectively modulates charge redistribution of Co sites, facilitating the Co³⁺/Co²⁺ redox cycle. Additionally, the La vacancy significantly enhanced the mobility of surface O₂²⁻, O₂⁻, and O⁻ species of 3LaCoO₃ along with the generation of oxygen vacancies, exhibiting the optimal oxygen activation capacity, which enhances the pathway: CB → phenolate species → C=C/CH₃/COOH → HCl/CO₂/H₂O and suppresses the formation of hazardous vinyl chloride, trichloroethane, dichloromethane, and chloroform. This study provides critical insights into the construction of oxygen vacancies and the development of active surface oxygen species for industrial CVOC stable and efficient elimination.

氯化挥发性有机物的环境友好净化是当前大气污染治理的一个挑战。在催化剂表面构建活性氧是促进CCl键断裂和破坏CVOC分子的一种很有前途的策略。本文构建了富氧空位钙钛矿型3LaCoO3催化剂，用于氯苯（CB）的高效催化氧化。3LaCoO3结构中La的部分去除有效地调节了Co位点的电荷再分配，促进了Co3+/Co2+的氧化还原循环。此外，La空位显著增强了3LaCoO3表面O22−、O2−和O−的迁移率，同时氧空位的生成，表现出最佳的氧活化能力，强化了CB→酚类物质→C=C/CH3/COOH→HCl/CO2/H2O的途径，抑制了有害物质氯乙烯、三氯乙烷、二氯甲烷和氯仿的生成。该研究为氧空位的构建和活性表面氧的开发提供了重要的见解，以稳定和有效地消除工业CVOC。

{"title":"La vacancy-induced enhancement of CoO and oxygen vacancy for efficient chlorobenzene oxidation","authors":"Mingjiao Tian , Yaruo Zhao , Qin Yang , Changwei Chen , Han Xu , Dong Guo , Zeyu Jiang , Haohua Kang , Shan Ren , Chi He","doi":"10.1016/j.seppur.2026.137035","DOIUrl":"10.1016/j.seppur.2026.137035","url":null,"abstract":"<div><div>The environmentally friendly purification of chlorinated volatile organic compounds (CVOCs) is a challenge in current air pollution control. Construction of active oxygen species on the catalyst surface is a promising strategy to promote the cleavage of C<img>Cl bond and the destruction of CVOC molecules. Herein, an oxygen-vacancy-rich perovskite-type 3LaCoO<sub>3</sub> catalyst was constructed for the efficient catalytic oxidation of chlorobenzene (CB). The partial removal of La in 3LaCoO<sub>3</sub> structure effectively modulates charge redistribution of Co sites, facilitating the Co<sup>3+</sup>/Co<sup>2+</sup> redox cycle. Additionally, the La vacancy significantly enhanced the mobility of surface O<sub>2</sub><sup>2−</sup>, O<sub>2</sub><sup>−</sup>, and O<sup>−</sup> species of 3LaCoO<sub>3</sub> along with the generation of oxygen vacancies, exhibiting the optimal oxygen activation capacity, which enhances the pathway: CB → phenolate species → C=C/CH<sub>3</sub>/COOH → HCl/CO<sub>2</sub>/H<sub>2</sub>O and suppresses the formation of hazardous vinyl chloride, trichloroethane, dichloromethane, and chloroform. This study provides critical insights into the construction of oxygen vacancies and the development of active surface oxygen species for industrial CVOC stable and efficient elimination.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"390 ","pages":"Article 137035"},"PeriodicalIF":9.0,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146075698","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