Separation and Purification Technology最新文献_第7页

Electrospun HKUST-1@PAN nanofibers membranes for efficient thorium ion enrichment via spatial confinement effect 静电纺HKUST-1@PAN纳米纤维膜通过空间约束效应高效富集钍离子

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136389

Xiang-He Kong , Ding-Ding Wang , Cheng-Cheng Zhu , Cui Wang , Lei Lei , Hong-Sheng Liu , Wen-Bo Lan , Hong-Qing Wang

As uranium reserves deplete, thorium emerges as a key alternative, making its recovery from mining wastewater a pivotal step for resource sustainability and environmental remediation. In this study, HKUST-1@PAN composite nanofiber membranes were prepared using the electrostatic spinning technique to uniformly load HKUST-1 onto polypropylene (PAN) polymer membranes for the enrichment of radioactive Th(IV). The HKUST-1@PAN nanofiber membrane with 40 wt% MOF loading exhibited superior Th(IV) adsorption performance, achieving a highest capacity of 303.95 mg g⁻¹ at the initial concentration (C₀) of 200 mg L⁻¹ and pH = 3. This nanofiber membrane demonstrates high ionic strength tolerance and rapid adsorption kinetics, achieving equilibrium within just 20 min. Thermodynamic analyses confirm that the adsorption process is both endothermic and spontaneous. Dynamic membrane filtration experiments showed the membrane achieved 98 % removal of low-concentration Th(IV) (20 mg L⁻¹). Furthermore, the adsorption mechanism was thoroughly analyzed through SEM, XPS, FT-IR, and DFT calculations, revealing that the pore confinement effect of HKUST-1 affords specific adsorption sites for Th(IV). The incorporation of PAN with HKUST-1 maintains the hierarchical porous architecture of the MOFs while overcoming the inherent solid-liquid separation issue of powdered adsorbents. This work highlights the promising application of MOFs-incorporated nanocomposite membranes as efficient platforms for radioactive thorium extraction from aqueous waste streams.

随着铀储量的枯竭，钍成为一种重要的替代品，从采矿废水中回收钍成为资源可持续性和环境修复的关键步骤。本研究采用静电纺丝技术制备HKUST-1@PAN复合纳米纤维膜，将HKUST-1均匀负载在聚丙烯（PAN）聚合物膜上，富集放射性Th（IV）。在初始浓度（C0）为200 mg L−1、pH = 3的条件下，HKUST-1@PAN纳米纤维膜对Th（IV）的吸附性能最高，达到303.95 mg g−1。这种纳米纤维膜具有高离子强度耐受性和快速吸附动力学，在20分钟内达到平衡。热力学分析证实吸附过程是吸热自发的。动态膜过滤实验表明，该膜对低浓度Th(IV) （20 mg L−1）的去除率达到98%。此外，通过SEM、XPS、FT-IR和DFT计算深入分析了吸附机理，发现HKUST-1的孔约束效应为Th（IV）提供了特定的吸附位点。PAN与HKUST-1的结合保持了mof的分层多孔结构，同时克服了粉状吸附剂固有的固液分离问题。本研究强调了mofs纳米复合膜作为高效萃取废水中放射性钍的平台的应用前景。

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引用次数: 0

Enhanced NH3-SCR performance over Phosphotungstic acid-modified Mn-based LDO catalysts 磷钨酸修饰的mn基LDO催化剂提高了NH3-SCR性能

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136404

Yang Deng , Na Zhu , Miaoqin Zhou

Mn-based catalysts have gained significant attention for the low-temperature selective catalytic reduction of NO_x with NH₃ (NH₃-SCR). However, their industrial application was hindered by poor H₂O resistance, low N₂ selectivity, and a narrow operational temperature window. In this work, MnFeAlO_x catalysts were prepared using the layered double hydroxides (LDHs)-derived oxide method. Additionally, a strategy involving polyoxometallic acid was employed to further boost the SCR activity of Mn-based layered double oxides (LDOs) catalysts. The incorporation of uniformly dispersed phosphotungstic acid (HPW) adjusted the oxidation properties and improved the catalysts' ability to adsorb and store NH₃. The optimal Mn₁Fe_0.5Al_0.5–10 %HPW catalyst exhibited a wider active temperature range (100–300 °C), higher N₂ selectivity and better H₂O resistance. Transient reactions and in situ DRIFTS analyses revealed that nitrate decomposition was the primary pathways for N₂O formation, a process that was inhibited by HPW, resulting in improved catalytic performance. This enhancement approach has the potential to inform the development of high-performance, highly selective low-temperature NH₃-SCR catalysts for use in industrial denitration processes.

锰基催化剂在NH3低温选择性催化还原NOx （NH3- scr）方面得到了广泛关注。然而，它们的抗水性能差，对N2的选择性低，工作温度窗窄，阻碍了它们的工业应用。在这项工作中，采用层状双氢氧化物（LDHs）衍生的氧化物方法制备了MnFeAlOx催化剂。此外，采用多金属氧酸策略进一步提高了锰基层状双氧化物（LDOs）催化剂的SCR活性。均匀分散磷钨酸（HPW）的加入调节了催化剂的氧化性能，提高了催化剂对NH3的吸附和储存能力。优选的Mn1Fe0.5Al0.5-10 %HPW催化剂具有较宽的活性温度范围（100-300 ℃）、较高的N2选择性和较好的耐水性能。瞬态反应和原位漂移分析表明，硝酸盐分解是N2O生成的主要途径，HPW抑制了这一过程，从而提高了催化性能。这种增强方法有可能为工业脱硝过程中使用的高性能、高选择性低温NH3-SCR催化剂的开发提供信息。

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引用次数: 0

MOF-derived S-scheme g-C₃N₄/Fe₂O₃ heterojunction with intercalated carbon for enhanced multifunctional photocatalysis mof衍生的S-scheme g-C₃N₄/Fe₂O₃插层碳异质结增强多功能光催化

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136390

Sandip Padhiari , Manamohan Tripathy , Swati Panigrahi , Pragnyashree Aparajita , Ugrabadi Sahoo , Monalisa Mishra , Swarna M. Patra , G. Hota

For better exciton separation and high catalytic activity, the most trailblazing stratagem is to frame S-scheme heterojunction photocatalytic systems through a simple repeatable synthetic strategies. In context to the above, a solvothermal followed by thermal annealing method was developed to convert type-II g-C₃N₄/MIL-53 (Fe) (g-C₃N₄/ML) into nanostructured S-scheme g-C₃N₄/Fe₂O₃ (g-C₃N₄/FO) under N₂ atmosphere at 500 °C. During the thermal annealing process of g-C₃N₄/ML, as revealed from the XRD, Raman, TEM, and XPS analysis, the MOF structures of MIL-53 (Fe) (ML) were destroyed. They were transformed to g-C₃N₄/FO with a thin layer of amorphous carbon around the developed α-Fe₂O₃ (FO) nanoparticles. The intercalated carbon between the g-C₃N₄ nanosheets and FO nanoparticles functions as an electron donor/acceptor, which converts g-C₃N₄/ML type-II heterojunction to g-C₃N₄/FO S-scheme heterojunction. When the photocatalytic activity of the developed nanocatalysts are scrutinized, it shows outstanding photocatalytic performance, which is 4.1, 2.9 and 4.5 folds times higher than g-C₃N₄/ML for bromoxynil degradation (97.3 %), As(III) oxidation (93.35 %), and H₂ evolution (5336.53 μmol g⁻¹ h⁻¹) reactions under visible light. It is also observed from the cytotoxicity studies that the obtained photocatalyst degraded toxic bromoxynil pesticide into non-toxic byproducts. This amplified photocatalytic activity can be attributable to the change in spatial charge carrier migrations from type-II to S-scheme followed by superior light absorption capacity and improved separation efficiency of the photogenerated charge carriers.

为了获得更好的激子分离和更高的催化活性，最具开创性的策略是通过简单的可重复合成策略构建s -图式异质结光催化体系。在此基础上，采用溶剂热法和热退火法，在500 ℃的N2气氛下，将ii型g-C3N4/MIL-53 (Fe) （g-C3N4/ML）转化为纳米结构的S-scheme g-C3N4/Fe2O3 （g-C3N4/FO）。在g-C3N4/ML的热退火过程中，通过XRD、Raman、TEM和XPS分析发现MIL-53 (Fe) （ML）的MOF结构被破坏。它们在α-Fe2O3 （FO）纳米颗粒周围包裹一层非晶碳，转变为g-C3N4/FO。在g-C3N4纳米片和FO纳米颗粒之间插入的碳作为电子供体/受体，将g-C3N4/ML型异质结转化为g-C3N4/FO s型异质结。对所制备的纳米催化剂的光催化活性进行了考察，结果表明，在可见光下对溴腈降解（97.3% %）、As（III）氧化（93.35 %）和H2析出（5336.53 μmol g−1 h−1）反应的光催化性能分别是g- c3n4 /ML的4.1、2.9和4.5倍。从细胞毒性研究中还观察到，所制备的光催化剂可将有毒溴虫腈农药降解为无毒副产物。这种增强的光催化活性可归因于空间载流子从ii型向s型迁移的变化，随之而来的是优越的光吸收能力和光生载流子分离效率的提高。

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引用次数: 0

A metal-carboxylate chains metal-organic framework decorated with N/O binding sites for MTO productions separation 金属-羧酸盐链金属-有机框架修饰的N/O结合位点为MTO产物分离

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136367

Wenxuan Feng, Qiang Zhang, Xin Lian, Tong-Liang Hu

As key building blocks in the chemical industry, ethylene (C₂H₄) and propylene (C₃H₆) are the primary target products of the methanol-to-olefins (MTO) process, which offers a promising alternative to traditional petroleum-based routes for olefin production. The separation of C₂H₄ and C₃H₆ constitutes a critical step in this process. Herein, we present a metal-carboxylate chains MOF (NUM-21), possessing suitable pore aperture and the presence of nitrogen/oxygen (N/O) binding sites distributed within the pore channels, which enables the effective capture of C₃H₆ and direct C₂H₄ purification from binary C₃H₆/C₂H₄ mixtures. The NUM-21a (activated NUM-21) exhibits a significantly higher C₃H₆ adsorption capacity (54.6 cm³ g⁻¹) compared to C₂H₄ (42.1 cm³ g⁻¹) at 298 K and 1 bar. Dynamic breakthrough experiments further demonstrated the effective separation of C₃H₆/C₂H₄ mixtures with varying compositions over NUM-21a. Grand Canonical Monte Carlo (GCMC) simulations revealed that C₃H₆ molecules exhibit stronger interactions with the framework than C₂H₄. Moreover, NUM-21 displays excellent recyclability and cycling stability under ambient pressure conditions. This work highlights the significance of rational MOF design for gas separation and offers valuable insights for the efficient separation of MTO products.

乙烯（C2H4）和丙烯（C3H6）作为化学工业的关键组成部分，是甲醇制烯烃（MTO）工艺的主要目标产品，它为传统的石油制烯烃路线提供了一个有希望的替代方案。C2H4和C3H6的分离是这一过程的关键步骤。本文提出了一种金属-羧酸盐链MOF (NUM-21)，具有合适的孔径和分布在孔通道内的氮/氧（N/O）结合位点，可以有效捕获C3H6，并从C3H6/C2H4二元混合物中直接纯化C2H4。在298 K和1 bar条件下，活化后的NUM-21a对C3H6的吸附量（54.6 cm3 g−1）明显高于C2H4（42.1 cm3 g−1）。动态突破实验进一步证明了不同组分的C3H6/C2H4混合物在NUM-21a上的有效分离。大规范蒙特卡罗（GCMC）模拟表明，C3H6分子与框架的相互作用比C2H4更强。此外，NUM-21在环境压力条件下表现出优异的可回收性和循环稳定性。本研究突出了合理的MOF设计对气体分离的重要性，为MTO产品的高效分离提供了有价值的见解。

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引用次数: 0

Synergistic enhancement of molecular oxygen activation for BPA degradation via joule heating and Cu-doped MnO2: Efficiency and mechanism 焦耳加热和cu掺杂MnO2协同增强分子氧活化降解双酚a的效率和机理

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136383

Huiqi Lv, Ziyang Ding, Yuhuan Jia, Weilin Guo

The efficient degradation of bisphenol A (BPA) critically depends on the development of high-performance catalysts and advanced oxidation technologies. In this study, we developed a novel Joule-heating assisted system using carbon felt supported copper doped MnO₂ (CMC) as conductor and catalyst for synergistic catalytic degradation of BPA. Cu-doping significantly improves the electrical conductivity of MnO₂ and its ability to form reactive oxygen species (ROS). Concurrently, applied Joule heating elevated the system temperature to 70.7 °C with 90 min at 9 V, further boosting degradation efficiency by activating molecular oxygen. Correspondingly, over 95 % of BPA (20 mg/L) is removed after 90 min with an electric energy consumption of only 5.36 kJ per milligram of BPA. This value is significantly lower than that required by conventional water bath heating to the same temperature. Mechanistic analyses indicate that the primary route for free radical generation during Jule heating is the catalytic activation of O₂ on the surface rather than direct thermal activation. In summary, this research establishes an energy-efficient degradation strategy that utilizes Joule heating in combination with a Cu-MnO₂ catalyst to effectively treat typical organic pollutants found in wastewater.

双酚A （BPA）的高效降解取决于高性能催化剂和先进氧化技术的发展。在这项研究中，我们开发了一种新的焦耳加热辅助系统，以碳毡支撑的铜掺杂MnO2 （CMC）为导体和催化剂，协同催化降解BPA。cu的掺杂显著提高了MnO2的电导率和生成活性氧（ROS）的能力。同时，应用焦耳加热将系统温度提高到70.7°C，在9 V下加热90分钟，通过激活分子氧进一步提高降解效率。相应的，在90分钟后，超过95%的BPA （20 mg/L）被去除，每毫克BPA的电能消耗仅为5.36 kJ。这个值明显低于传统水浴加热到相同温度所需的值。机理分析表明，巨乐加热过程中自由基产生的主要途径是表面O2的催化活化，而不是直接的热活化。综上所述，本研究建立了一种节能降解策略，利用焦耳加热与Cu-MnO₂催化剂相结合，有效地处理废水中的典型有机污染物。

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引用次数: 0

Tannic acid regulates electron transfer of iron-biochar composites in immobilized bioreactors for efficient removal of nitrate, nickel, and ibuprofen: Performance and potential mechanisms 单宁酸调节铁-生物炭复合材料在固定化生物反应器中高效去除硝酸盐、镍和布洛芬的电子转移：性能和潜在机制

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136391

Tianmeng Li , Xue Li , Junfeng Su , Shuyu Liu , Yihan Bai , Xuru Lu , Xuan Li

Complex pollution and insufficient carbon-to‑nitrogen ratios are major challenges currently facing wastewater treatment plants. Ferrous-driven denitrification offers an effective solution for treating low carbon-to‑nitrogen (C/N) ratio wastewater, but this process is often constrained by slow electron transfer rates. Therefore, this study prepared a hydrothermally activated tannic acid -modified iron-biochar composite (TA-Fe-BC). Using polyvinyl alcohol (PVA) and sodium alginate (SA) as media, the composite was embedded with the strain Zoogloea sp. ZP7 as a biocarrier to operate a bioreactor. Hydrothermally activated TA generates quinone groups, thereby enhancing electron transfer efficiency. The reactor achieved an excellent nitrate removal efficiency of 97.83 % at HRT = 4 h, C/N= 2, and pH = 7. Furthermore, trace nickel (Ni²⁺) and ibuprofen (IBP) in wastewater were likely removed primarily through adsorption by microbial-produced extracellular polymeric substances (EPS) and bio‑iron precipitation. Community analysis indicated that TA-Fe-BC addition promoted Pseudomonadota enrichment. Concurrently, the bioreactor harbored diverse microbial communities performing ferrous oxidation (Dechloromonas, Zoogloea) and iron reduction (Alicycliphilus, Geothrix). KEGG database analysis revealed that TA-Fe-BC promoted the upregulation of genes involved in iron and nitrogen cycling. This study provides a novel approach for the efficient treatment of wastewater with low C/N ratios.

复杂的污染和碳氮比不足是污水处理厂目前面临的主要挑战。铁驱动反硝化为处理低碳氮比（C/N）废水提供了有效的解决方案，但该过程通常受到电子转移速率缓慢的限制。因此，本研究制备了一种水热活化单宁酸修饰铁-生物炭复合材料（TA-Fe-BC）。以聚乙烯醇（PVA）和海藻酸钠（SA）为培养基，以Zoogloea sp. ZP7为生物载体包埋该复合材料，操作生物反应器。水热活化的TA生成醌基团，从而提高电子传递效率。当HRT = 4 h, C/N= 2, pH = 7时，反应器的硝酸盐去除率为97.83%。此外，废水中的微量镍（Ni2+）和布洛芬（IBP）可能主要通过微生物胞外聚合物（EPS）吸附和生物铁沉淀来去除。群落分析表明，TA-Fe-BC的加入促进了假单胞菌的富集。同时，该生物反应器还拥有多种微生物群落，可进行亚铁氧化（decchloromonas, Zoogloea）和铁还原（Alicycliphilus, Geothrix）。KEGG数据库分析显示，TA-Fe-BC促进了铁和氮循环相关基因的上调。本研究为低碳氮比废水的高效处理提供了一条新途径。

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引用次数: 0

Molecular-level determination of chloride-induced shifts in DOM transformation in UV/H2O2 and UV/PDS systems 在UV/H2O2和UV/PDS体系中，氯离子诱导DOM转变的分子水平测定

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136396

Zhepei Gu, Feiyan Fang, Xiaoyu Wang, Qibin Li

High chloride (Cl⁻) concentrations in wastewater complicate the transformation of dissolved organic matter (DOM) during advanced oxidation processes (AOPs). This study investigated the impact of Cl⁻ on the transformation of Suwannee River natural organic matter (SRNOM), a highly unsaturated and aromatic DOM certified reference material, in ultraviolet-activated hydrogen peroxide (UV/H₂O₂) and ultraviolet-activated peroxydisulfate (UV/PDS) systems. The inhibitory effect of Cl⁻ on DOM removal was more significant in the UV/PDS system; at 56.4 mM Cl⁻, total organic carbon removal decreased by 22.81 %. Ultrahigh-resolution mass spectrometry showed that Cl⁻ promoted the formation of highly oxygenated, highly unsaturated, and phenolic (HO-HUPh) compounds while suppressing their further degradation to aliphatic (Ali) species. This effect occurred in both systems but was stronger in the UV/PDS system because Cl⁻ shifted the dominant reactive species from SO₄^•− to reactive chlorine species (RCS, e.g., Cl₂^•−), whereas hydroxyl radicals remained dominant in the UV/H₂O₂ system. Reactive chlorine species enhanced oxygen addition to DOM but impeded decarboxylation and dealkylation, leading to the accumulation of HO-HUPh intermediates. The UV/PDS system also generated more potentially toxic chlorinated organic byproducts than the UV/H₂O₂ system (558 vs. 406 molecular formulas). These findings provide a basis for optimizing AOPs for chloride-rich wastewater.

在深度氧化过程（AOPs）中，废水中高浓度的氯离子（Cl−）使溶解有机物（DOM）的转化复杂化。研究了Cl−对苏万尼河天然有机质（SRNOM）在紫外线活化过氧化氢（UV/H2O2）和紫外线活化过硫酸氢盐（UV/PDS）体系中转化的影响。SRNOM是一种高度不饱和的芳香DOM标准物质。在UV/PDS体系中，Cl−对DOM去除的抑制作用更为显著；在56.4 mM Cl−时，总有机碳去除率下降22.81 %。超高分辨率质谱分析表明，Cl−促进了高氧、高不饱和和酚类（HO-HUPh）化合物的形成，同时抑制了它们进一步降解为脂肪族（Ali）物质。这种效应在两种体系中都存在，但在UV/PDS体系中更强，因为Cl -将主要的活性物质从SO4•−转移到活性氯（RCS，例如Cl2•−），而羟基自由基在UV/H2O2体系中仍然占主导地位。活性氯增强了DOM的氧加成，但阻碍了脱羧和脱烷基，导致HO-HUPh中间体的积累。与UV/H2O2系统相比，UV/PDS系统产生的潜在毒性氯化有机副产物更多（分子式558 vs 406）。研究结果为富氯废水AOPs的优化提供了依据。

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引用次数: 0

Metal-free porous N, S co-doped carbon catalyst for H2S selective oxidation: enhanced elemental sulfur selectivity and mechanisms 无金属多孔N， S共掺杂碳催化剂用于H2S选择性氧化：增强单质硫选择性及其机理

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136392

Yuan Li , Sisi Pan , Hongyan Li , Ying Zhao , Jie Zhao , Ping Ning , Kai Li

The selective oxidation of H₂S into elemental sulfur is considered as one promising method for the removal of this undesired gas. Second heterogeneous atom introducing into N doped carbocatalyst skeleton shows their potential on the enhancement of selectivity. We developed a novel N, S co-doped porous carbon with high pyridinic content and mesoporous pore structure for H₂S selective oxidation. The experimental results showed that the optimized catalyst exhibits excellent durability about 133 h with 100 % conversion and 95 % elemental sulfur selectivity at 180 °C. Kinetic study and density functional theory calculation reveals that sulfur doping could regulate the electronic structure of N atom on the carbocatalyst surface and further weaken the interactions between N active site and H₂S molecule, then prevent deep oxidation of H₂S. The work provides a strategy for atomic-level modulation of non-metal doping catalysts, enabling selective oxidation process for efficient and durable desulfurization.

选择性氧化H2S成单质硫被认为是一种很有前途的方法来去除这种不需要的气体。在N掺杂碳催化剂骨架中引入第二种非均相原子，显示了其提高选择性的潜力。我们开发了一种新型的N， S共掺杂多孔碳，具有高吡啶含量和介孔孔结构，用于H2S选择性氧化。实验结果表明，优化后的催化剂在180℃下具有优异的耐久性，转化率为100%，单质硫选择性为95%。动力学研究和密度泛函理论计算表明，硫掺杂可以调节碳催化剂表面N原子的电子结构，进一步削弱N活性位点与H2S分子的相互作用，从而阻止H2S的深度氧化。这项工作为非金属掺杂催化剂的原子级调制提供了一种策略，使选择性氧化过程高效持久地脱硫成为可能。

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引用次数: 0

Corrigendum to “Photothermal nanotube enhanced thermomorphic absorbents for efficient low-temperature CO2 release” [Sep. Purif. Technol. 374 (2025) 133704] “光热纳米管增强的热致吸收剂用于有效的低温二氧化碳释放”的勘误表[9月Purif]。科技. 374 (2025)133704]

IF 8.6 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136268

Junjie Yuan, Wenchuan Niu, Qi An, Gaofeng Deng, Zhichao Wang, Jubao Gao

The authors regret that the necessary supporting documentation was not uploaded.

发件人感到遗憾的是，没有上传必要的证明文件。

引用次数: 0

Simulation study on the morphological characteristics and adsorption mechanism of CO₂ adsorption by coal 煤吸附CO₂的形态特征及吸附机理的模拟研究

IF 9 1区工程技术 Q1 ENGINEERING, CHEMICAL

Separation and Purification Technology

Pub Date : 2025-12-05 DOI: 10.1016/j.seppur.2025.136398

Yansheng Wang , Yaqing Zhang , Ling Qiao , Cunbao Deng , Lamei Liu , Angang Lv , Qingsheng Xu , Zhixin Jin

Sealing CO₂ in coal mine goafs is a cost-effective way to reduce carbon emissions, but the microscopic behavior of CO₂ adsorption in coal is still poorly understood. Therefore, the molecular simulations are used to examine the morphology and mechanisms of CO₂ adsorption under various conditions. Results show dry coal follows the Langmuir model for CO₂ adsorption. In water-bearing coal, hydrogen bonding between water and CO₂ temporarily increases adsorption at 5 % moisture. Properties of the CO₂ adsorption layer—density, thickness, and stability—vary with temperature, pressure, pore size, and moisture, with thickness from 3.35 to 5.5 Å, densities from 1.07 to 3.21 g/cm³, and diffusion coefficients from 0.352 to 6.566 Å²/ps. In dry coal, CO₂ prefers adsorption sites capable of forming hydrogen bonding, then other polar sites, and surface sites; environmental conditions mainly affect the last sites. The first two adsorption sites are occupied by water in water-bearing coal, but then water forms clusters instead of occupying the last adsorption sites. Adsorption of water reduces density but stabilizes the CO₂ adsorption layer. When these sites are occupied by water, the CO₂ adsorption layer shifts backward, weakening the electrostatic interactions. However, the thickness of CO₂ adsorption layer is prevented from changing by hydrogen bonding between water and CO₂. This research provides theoretical guidance for CO₂ sequestration in underground coal mine goafs.

在煤矿采空区封存CO 2是一种经济有效的碳减排方法，但对煤中CO 2吸附的微观行为仍知之甚少。因此，通过分子模拟来研究不同条件下CO₂吸附的形态和机理。结果表明，干煤对CO₂的吸附符合Langmuir模型。在含水煤中，水和CO₂之间的氢键暂时增加5%水分时的吸附。CO2吸附层的密度、厚度和稳定性随温度、压力、孔径和湿度的变化而变化，其厚度为3.35 ~ 5.5 Å，密度为1.07 ~ 3.21 g/cm3，扩散系数为0.352 ~ 6.566 Å2/ps。在干煤中，CO₂优先于能够形成氢键的吸附位点，其次是其他极性位点和表面位点；环境条件主要影响最后一个站点。含水煤的前两个吸附位被水占据，但随后水形成团簇而不是占据最后的吸附位。水的吸附降低了密度，但稳定了CO2吸附层。当这些位置被水占据时，CO₂吸附层向后移动，减弱静电相互作用。然而，水与二氧化碳之间的氢键作用阻止了二氧化碳吸附层厚度的变化。该研究为煤矿井下采空区CO₂固存提供了理论指导。

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引用次数: 0