Separation and Purification Technology最新文献

{"title":"A novel strategy for simultaneous removal of hardness, suspended solids and organics from fracturing wastewater: Efficiency, mechanism and application","authors":"Yabo Shang,&nbsp;Yadong Wang,&nbsp;Junwei Huang,&nbsp;Juan Shi,&nbsp;Lu Xu,&nbsp;Keqian Li,&nbsp;Pengkang Jin,&nbsp;Xin Jin","doi":"10.1016/j.seppur.2025.132735","DOIUrl":"10.1016/j.seppur.2025.132735","url":null,"abstract":"<div><div>The coexistence of high hardness, turbidity, and organic matter in oilfield fracturing wastewater presents significant challenges for its reuse and the efficiency of conventional treatment methods. The accumulation of hardness-causing ions, suspended solids (SS), and organic pollutants complicates treatment processes, reducing both efficiency and sustainability in wastewater management. A practical solution is essential to enable large-scale reuse of oilfield wastewater while minimizing environmental impacts. This study introduced an innovative nucleation crystallization pelleting (NCP) process for the simultaneous removal of hardness, organic matter, and SS from wastewater. The method employed pre-added seeds with active sites, facilitating the deposition of Ca²⁺ and Mg²⁺ as CaCO₃, Mg(OH)₂, and Mg_0.03Ca_0.97CO₃ via Na₂CO₃ and NaOH addition. Organic matter was removed by co-precipitation and surface complexation, while SS adhered to the particle surface due to hydrodynamic action. Under optimal conditions (4200 mg/L Na₂CO₃, 1400 mg/L NaOH, 7.5 % seed filling rate, and 80 m/h up-flow velocity), the three-stage NCP system achieved removal efficiencies of 95.6 % for total hardness, 90.1 % for TSS, and a 31.1 % reduction in COD, with effluent hardness consistently remaining below 300 mg/L. These results satisfied the requirement that the total concentration of Ca²⁺ and Mg²⁺ ions in the field-prepared fracturing fluid remains below 150 mg/L. The process demonstrated stability across three reuse cycles, confirming the seeds’ reliability, efficiency, and reproducibility. A pilot-scale NCP system with a treatment capacity of 50 m³/h was developed, and 120 h of continuous operation demonstrated stable effluent quality. Dense pellets (∼1.2 mm) formed during the treatment required no additional processing. The findings confirmed that the NCP system effectively and reliably treats oilfield fracturing wastewater, achieving substantial removal of hardness, SS, and organic pollutants. The formation of dense pellets without generating sludge underscored its practicality for large-scale applications. This study offers a scalable and sustainable solution to wastewater treatment challenges, paving the way for broader adoption of NCP technology in industrial settings.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132735"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758031","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}

{"title":"Synergistic effect of oxygen vacancies and Z-scheme in Ag3PO4/FeSnO(OH)5 for ultrafast degradation of indomethacin via photogenerated h+","authors":"Haijun Chen ,&nbsp;Chunli Kang ,&nbsp;Shiyi Zhao ,&nbsp;Zhuowen Wang ,&nbsp;Haiyang Liu ,&nbsp;Deming Dong ,&nbsp;Jiao Qu ,&nbsp;Na Zheng ,&nbsp;Xiuyi Hua","doi":"10.1016/j.seppur.2025.132802","DOIUrl":"10.1016/j.seppur.2025.132802","url":null,"abstract":"<div><div>Ineffective separation of photo-carriers and slow photoreaction rates seriously limit the decontamination effectiveness of the photocatalyst. To overcome these limitations, herein, the oxygen vacancies modified Z-scheme Ag₃PO₄/FeSnO(OH)₅ heterojunction was designed with FeSnO(OH)₅ as a co-catalyst. In this photosystem, Ag₃PO₄ and FeSnO(OH)₅ function as oxidation and reduction centers of Ag₃PO₄/FeSnO(OH)₅ photocatalysts, respectively. Importantly, oxygen vacancies in the Z-scheme heterojunction provide an effective charge transport pathway, which not only inhibits the photocorrosion of Ag₃PO₄ but also reduces electron-hole recombination, significantly boosting the photocatalytic decontamination performance and long-term stability of the Ag₃PO₄/FeSnO(OH)₅ photocatalyst. Remarkably, the Ag₃PO₄/FeSnO(OH)₅ photocatalyst demonstrated outstanding photocatalytic performance, 100% degrading indomethacin (IDM) under visible light in just 30 min through the main generation of h⁺ that attacks the active atoms of IDM, prominently outperforming other counterparts. Besides, three principal degradation pathways were proposed, and the toxicity of the degradation products was significantly reduced. The Ag₃PO₄/FeSnO(OH)₅ exhibited high photocatalytic degradation efficacy across different qualities of water. This research offers an oxygen vacancy modified engineering combined with a Z-scheme heterojunction strategy for constructing extraordinary photocatalysts for environmental purification.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132802"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758025","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}

{"title":"OGCN-modified thin-film nanocomposite membranes for efficient capture and enrichment of rare earth ions","authors":"Siwei Yu ,&nbsp;Xindong Li ,&nbsp;Lijinhong Huang ,&nbsp;Zhaohuang Zhong ,&nbsp;Jianghui Jia ,&nbsp;Luo Bao ,&nbsp;Qinyan Zhu ,&nbsp;Wentai Wu ,&nbsp;Wanfu Huang","doi":"10.1016/j.seppur.2025.132738","DOIUrl":"10.1016/j.seppur.2025.132738","url":null,"abstract":"<div><div>Conventional methods for recovering ionic rare earth elements are complex, and involve multiple phase transitions that reduce production efficiency. Therefore, simplified and more efficient recovery processes are urgently needed. In this study, we developed thin-film nanocomposite (TFN) membranes modified with oxidized graphite-phase carbon nitride (OGCN) to achieve high-efficiency capture and enrichment of rare earth ions. Graphitic carbon nitride was synthesized via thermal polymerization and then transformed into OGCN nanoparticles through a hydrogen peroxide-assisted hydrothermal process. These nanoparticles were embedded into a polyetherimide (PEI) mixed matrix membrane (MMM), and a TFN membrane (PA-MMM(PEI-OGCN)) was fabricated using piperazine as the aqueous phase and trimesoyl chloride as the organic phase via interfacial polymerization. PA-MMM(PEI-OGCN) exhibited high water flux (38.6 L·m⁻²·h⁻¹) and effective rare earth ion rejection, with La³⁺, Y³⁺, and Nd³⁺ rejection rates all exceeding 95 %. The OGCN modification significantly enhanced the hydrophilicity and surface charge density of the membranes, improving their capacity to capture and enrich rare earth ions. Under different volume reduction factors (VRF), the PA-M2 membrane consistently showed higher rare earth ion rejection compared to the PA-M0 membrane. At a VRF of 10, the PA-M2 membrane increased rare earth ion concentration from 0.242 to 1.285 g/L, and kept rare earth loss in the permeate below 65 mg and significantly lower than the 80 mg observed with the PA-M0 membrane. The PA-M2 membrane demonstrated excellent stability and fouling resistance during long-term operation. In conclusion, OGCN-modified TFN membranes offer great potential for efficient separation and recovery of rare earth ions, and present broad applications in resource sustainability and environmental protection.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132738"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758027","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}

{"title":"Peroxymonosulfate activation by iron-cluster-modified Mn single atom catalyst for ciprofloxacin removal: Non-radical pathway dominated by 1O2 and high-valent metal–oxygen species","authors":"Ying Xiong ,&nbsp;Yanting Zhou ,&nbsp;Yuanyuan Liu ,&nbsp;Xin Zhou ,&nbsp;Zhijian Du ,&nbsp;Ruxin Men ,&nbsp;Jiajia Wang","doi":"10.1016/j.seppur.2025.132730","DOIUrl":"10.1016/j.seppur.2025.132730","url":null,"abstract":"<div><div>Atomic clusters have been recognized for boosting interactions with single-atom sites and activating peroxymonosulfate (PMS) to degrade pollutants. However, research on the synergies between different metals in these clusters and their impact on enhancing single-atom activity remains limited. This paper introduces an iron-cluster-modified manganese single-atom catalyst (FeMn_ac-NC) exhibiting exceptional catalytic activity. At low doses of the catalyst (FeMn_ac-NC, 0.05 g/L) and the oxidant (PMS, 0.2 g/L), the FeMn_ac-NC/PMS system recorded an impressive removal efficiency of 91.0 % in 5 min, exhibiting a <em>k_obs</em> of 0.1038 min⁻¹. Within this system, the active oxygen species identified included singlet oxygen and high-valent metal–oxygen species. X-ray photoelectron spectroscopy analysis revealed a significant presence of pyrrolic nitrogen in the material, which binds with Mn to create the primary active site. Based on calculations using the density functional theory, the redox cycling between iron clusters and manganese single atoms has been proved to improve the activation efficiency of the system. The system demonstrates high tolerance to environmental media containing anions and dissolved organic matter, showing notable degradation performance over a wide pH range. This research provides valuable insights for the development of high-performance catalysts that is well-suited for practical environmental purification applications.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132730"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745453","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}

{"title":"Feasibility exploration and performance assessment of extractive distillation processes for separation of different high concentration feed compositions based on multi-objective optimization","authors":"Hui Wang,&nbsp;Jing Pan,&nbsp;Jinlong Li,&nbsp;Zhixia Xu,&nbsp;Ruimin Zhang,&nbsp;Tan Dai,&nbsp;Qing Ye","doi":"10.1016/j.seppur.2025.132818","DOIUrl":"10.1016/j.seppur.2025.132818","url":null,"abstract":"<div><div>The separation of azeotropic mixtures with high concentration composition has received increasing attention in recent years. This paper investigates the feasibility of different distillation processes to separate the ternary mixtures with a high concentration composition when the high-concentration composition is stable node or non-stable node. When the high concentration composition is stable node, the conventional three-column ED process (CTC), the four-column ED process with a preconcentration column (FCPC) and the three-column ED process with a combined distillation column (TCDC) can separate the mixtures. When the high concentration composition is non-stable node, only the CTC can separate the mixtures. Taking the NPA/THF/water system in which NPA and water are stable nodes, THF is non-stable node as an example, the results show that the TCDC process gets the best energy saving and cost reduction. Compared with the CTC processes of 0.8 water /0.1 NPA /0.1THF and 0.8 NPA /0.1 water /0.1THF systems, the TCDC processes reduce the energy consumption by 53.53 % /46.01%, the TAC by 57.49% /57.43%, the CO2 emissions by 60.12%/57.52% and the entropy generation 57.74%/45.31%.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132818"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758029","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}

{"title":"Rational design of a small peptidomimetic ligand to capture a viral spike protein","authors":"Carlos Filipe Santos Costa ,&nbsp;Iana Lychko ,&nbsp;Carolina Mota Natal ,&nbsp;Arménio Jorge Moura Barbosa ,&nbsp;Ana Margarida Gonçalves Carvalho Dias ,&nbsp;Ana Cecília Afonso Roque","doi":"10.1016/j.seppur.2025.132778","DOIUrl":"10.1016/j.seppur.2025.132778","url":null,"abstract":"<div><div>The availability of purified antigenic proteins is critical to develop agents to prevent, diagnose, or treat infectious diseases. In this context, antigenic proteins are produced by recombinant expression in host cells and further purified, typically by chromatographic methods. Chromatographic steps that allow the one-step capture of the antigenic protein are important to streamline the purification train. Here, we present the design and development of an adsorbent bearing a synthetic affinity ligand to capture the SARS-CoV-2 spike protein, used as a model antigenic protein. A 120-ligand combinatorial library was designed <em>in silico</em> and then synthesised in solid phase, and both were computationally and experimentally screened for binding to the spike protein. One lead ligand was selected for yielding &gt; 95 % binding, and 64–73 % recovery of original strain spike protein, its receptor-binding domain (RBD), and Omicron BA.5 variant spike protein. An enrichment factor of 15 was found when capturing the spike protein from a clarified supernatant sample. Complementary molecular dynamics simulations allowed a better understanding of the interactions between the lead ligand and the spike protein, which mainly consist of hydrophobic interactions, some hydrogen bonds and salt bridges formed with an important ligand carboxyl group. Overall, the methodology is a fast and efficient platform to develop affinity ligands for the purification of antigenic proteins in future pandemics.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132778"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Two novel [CuxIy]n-based MOFs with high BET surface area for efficient MTO products separation","authors":"Xueyue Yu,&nbsp;Baobing Tang,&nbsp;Zhaohui Shi,&nbsp;Zhiwei Liu,&nbsp;Xu Liu,&nbsp;Lirong Zhang,&nbsp;Yunling Liu","doi":"10.1016/j.seppur.2025.132796","DOIUrl":"10.1016/j.seppur.2025.132796","url":null,"abstract":"<div><div>Here, by utilizing mixed molecular building block strategy, two novel [Cu_xI_y]_n-based MOFs materials, <strong>JLU-MOF205</strong> and <strong>JLU-MOF206</strong> were successfully constructed by employing HPYBZ (HPYBZ = 4-(4-pyridyl) benzoic acid) and HPYA (HPYA = 3-(4-pyridyl) acrylic acid) organic ligands. Both MOFs possess typical [Cu_xI_y] clusters and copper paddlewheel building units, <strong>JLU-MOF205</strong> exhibits a unique 2D + 2D → 3D perpendicular polycatenated framework. <strong>JLU-MOF206</strong> presents better structural stability compared to <strong>JLU-MOF205</strong>, which resulted in improving water stability, high Brunauer-Emmett-Teller (BET) surface area and extra open metal sites. Additionally, both [Cu_xI_y]_n-based MOFs demonstrate superior adsorption of C₃H₆ over C₂H₄, thereby achieving excellent C₃H₆/C₂H₄ selectivity. Breakthrough experiments confirmed their outstanding performance in separating C₃H₆/C₂H₄ binary mixtures, enabling the one-step purification of C₂H₄ and the recovery of C₃H₆. <strong>JLU-MOF205</strong> samples can extract 43.65, 64.70, and 172.23 L kg⁻¹ of high-purity (99.9 %) C₂H₄ from C₃H₆/C₂H₄ mixtures in different ratios (50/50, 20/50, and 10/90), respectively. For <strong>JLU-MOF206</strong>, it is also possible to extract 113.53, 230.79, and 501.28 L kg⁻¹ of high-purity (99.9 %) C₂H₄, respectively. Moreover, their excellent separation selectivity and high reusability surpass many known MOFs materials, making them ideal candidate adsorbents for industrial separation applications.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132796"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745447","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}

{"title":"Mechanism of NO electrocatalytic reduction over the MoS2-based single atom catalyst: A DFT investigation","authors":"Yang-wen Wu,&nbsp;Han-wen Wang,&nbsp;Zheng-long Wu,&nbsp;Xiong Zhang,&nbsp;Yao Dong,&nbsp;Zhuang Hu,&nbsp;Yue Lv,&nbsp;Xin-yue Zhou,&nbsp;Li Zhao,&nbsp;Bing Zhang,&nbsp;Qiang Lu","doi":"10.1016/j.seppur.2025.132813","DOIUrl":"10.1016/j.seppur.2025.132813","url":null,"abstract":"<div><div>The emission of Nitric Oxide (NO) is a critical issue in the area of global environmental pollution. The electrocatalytic reduction of Nitric Oxide (NORR) for controlling NO pollution and generating ammonia has attracted significant attention in recent years, wherein the transition metal single atom catalyst (SAC) exhibits especially decent performance. However, the interaction mechanism between reactants and the NORR catalyst remains unclear at the current stage. Herein, this study explored the NORR mechanism on the MoS₂-based transition metal SACs. Density functional theory calculations were employed to determine the superior SAC catalyst for NORR by evaluating the electrochemical stability, adsorption performance, and NORR reactivity. Results showed that Mn-MoS₂ exhibited excellent performance in terms of electrochemical stability and NO adsorption. Based on electronic structure analysis, Mn altered the electronic state distribution of MoS₂, enhancing charge transfer intensity. Hybridization of different orbitals indicated the stronger interaction between Mn and NO, promoting the adsorption of NO on the surface of MoS₂. Calculation of Gibbs free energy of NORR steps confirmed that Mn-MoS₂ reduced the energy barrier of the rate determining step in NORR and accelerated the reaction process. This study provides a theoretical foundation for the development of advanced SACs, emphasizing the promising role of Mn in enhancing catalytic efficiency.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132813"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745450","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}

{"title":"Facile and economic modified method for CaO-based particles with straw as additive: Improving CO2 adsorption performance and cyclic stability","authors":"Xuehua Shen ,&nbsp;Ruirui Zhang ,&nbsp;Ruiheng Zhang ,&nbsp;Feng Xie ,&nbsp;Han Hua ,&nbsp;Pengju Wang ,&nbsp;Feng Yan ,&nbsp;Zewei Quan ,&nbsp;Zuotai Zhang","doi":"10.1016/j.seppur.2025.132820","DOIUrl":"10.1016/j.seppur.2025.132820","url":null,"abstract":"<div><div>CaO-based sorbents represent a highly viable solution for post-combustion CO₂ capture, with granulation commonly employed to mitigate elutriation in fluidized-bed reactors. Nonetheless, granulation markedly increases the density of these sorbents, thereby impairing their CO₂ uptakes and cyclic stability. In this study, a cost-effective strategy was developed by incorporating various pore-forming agents (agar, urea, straw, and biochar) into CaO-based particles (denoted as CaO+C+A, CaO+C+U, CaO+C+S, and CaO+C+B) to enhance their adsorption performance and durability. The findings revealed that the mechanical strength of uncalcined CaO-based particles remained unaltered by the incorporation of additives, whereas only the CaO+C+S particle maintained acceptable compressive strength (17.1 N) and a low attrition rate (6.6 %) after calcination. Compared with the CaO+C+A particle, the compressive strength of CaO+C+S particle was increased by 87.5 % and the attrition rate was decreased by 22.8 %. Meanwhile, the CaO+C+S particle exhibited the highest CO₂ adsorption performance, achieving 541 mg/g within 10 min, alongside outstanding cyclic stability, maintaining 217 mg/g after 20 cycles. This represents a 17.4 % increase in initial adsorption and a 25.3 % improvement in long-term stability compared to the control particle. These advancements are attributed to straw’s role in facilitating pore formation, refining CaO crystal size, and increasing the proportion of high-melting-phase (CaAl₄Si₂O₁₁). The first two factors markedly enhance the diffusion kinetics conditions and thus improving the CO₂ adsorption performance of CaO-based particles. Combined, these three factors enhance resistance to sintering by creating spatial physical barriers and increasing the melting point. This study offers a straightforward and cost-efficient modification approach to improve the CO₂ adsorption performance and durability of CaO-based particles.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132820"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745448","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}

{"title":"Ion-island induced spatially separated active sites in poly(ionic liquid)s for efficient CO2 fixation into cyclic carbonates","authors":"Mengqian Fu ,&nbsp;Tianyu Guo ,&nbsp;Shuaifei Liu ,&nbsp;Qianmeng Zhao ,&nbsp;Wen Liu ,&nbsp;Yunong Li ,&nbsp;Zifeng Yang ,&nbsp;Wei Hua ,&nbsp;Qian Su ,&nbsp;Weiguo Cheng","doi":"10.1016/j.seppur.2025.132815","DOIUrl":"10.1016/j.seppur.2025.132815","url":null,"abstract":"<div><div>Carbon dioxide (CO₂) conversion into carbonates <em>via</em> cycloaddition with epoxides represents a promising approach for achieving carbon neutrality and advancing clean energy technologies. However, it remains challenging to design efficient heterogeneous catalysts that achieve high catalytic activity comparable to homogeneous components with minimal dosage under mild conditions. From the perspective of maintaining intrinsic activity while realizing sufficient exposure of active sites, this work presents a new strategy to construct efficient heterogeneous catalysts based on ion-island induced spatially separated active sites in hyper cross-linked poly(ionic liquid)s (HPILs). By optimizing the Friedel-Crafts alkylation and ionization in specific directions, we synthesized a series of HPILs featuring ion-island architectures with spatially separated active sites. Intriguingly, it was discovered that the electron-withdrawing ionic liquids induced unidirectional polymerization into ion-islands, and the electron-rich triphenylphosphine (PPh₃) tended to cross-link multidirectional forming networks, which co-regulated the distributions of ion-islands and therein inter-ion interaction. Remarkably, HPIL-3 with peripherally distributed ion-islands demonstrated exceptional catalytic efficiency (TOF = 1451.1 h⁻¹) for CO₂ and propylene oxide (PO) at 90 °C with 0.05 mol% Br^- <strong>(</strong>relative to PO<strong>).</strong> Combining EPS and in-situ DRIFTS analysis revealed that the quaternary phosphine cations (P⁺) and Br^- synergistically activated both CO₂ and PO molecules, thereby accelerating the cycloaddition process.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"366 ","pages":"Article 132815"},"PeriodicalIF":8.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745452","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}