Chinese Journal of Chemical Engineering最新文献_第2页

Functionalized solvents containing conjugated ligands for the separation of α-olefins 含共轭配体的功能化溶剂用于α-烯烃的分离

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-07-22 DOI: 10.1016/j.cjche.2026.06.018

Xinying Li, Shuying Wang, Shuai Zheng, Zhiyong Zhou, Chencan Du, Yuming Tu, Zhongqi Ren

{"title":"Functionalized solvents containing conjugated ligands for the separation of α-olefins","authors":"Xinying Li, Shuying Wang, Shuai Zheng, Zhiyong Zhou, Chencan Du, Yuming Tu, Zhongqi Ren","doi":"10.1016/j.cjche.2026.06.018","DOIUrl":"10.1016/j.cjche.2026.06.018","url":null,"abstract":"<div><div><em>α</em>-Olefins are important basic chemical raw materials. Metal-based coordination-functionalized solvents that leverage π-complexation with olefins can significantly improve the performance of olefin separation. In this study, AgBF<sub>4</sub> was used as the coordination metal salt and maleic anhydride (MA), a conjugated five-membered compound, was employed as the organic ligand, to design and synthesize a functionalized solvent (AgBF<sub>4</sub>:MA (1:3)) for the efficient separation of 1-hexene. This solvent exhibited a selectivity of up to 1559.31 for the 1-hexene/<em>n</em>-hexane system, a distribution coefficient of 3.9754 for 1-hexene, good cycling stability, and high separation selectivity for various unsaturated/saturated hydrocarbon systems. Fourier transform infrared spectroscopy and Raman spectroscopy, together with quantum chemical calculations, revealed that the carbonyl group in the MA ligand coordinates with Ag<sup>+</sup> in a monodentate manner. Meanwhile, the uncoordinated carbonyl enhances the electron-withdrawing ability of the ligand through the conjugated double bond. This reduces the electron density on Ag<sup>+</sup> and significantly strengthening its π-complexation ability with 1-hexene. Modulating the electronic properties of the metal center through ligand conjugation provides new insights for designing efficient olefin separation processes.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 118-129"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Swirling flow reorganization and heat transfer enhancement in a vortex tube with a diameter-transformed vortex generator 直径变换涡发生器涡流管内旋流重组与强化换热

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-08-06 DOI: 10.1016/j.cjche.2026.07.019

Chunhua Zhang, Cong Zhou, Bona Lu, Junjie Liu, Wei Wang, Lijun Zhang, Guoqing Wang

{"title":"Swirling flow reorganization and heat transfer enhancement in a vortex tube with a diameter-transformed vortex generator","authors":"Chunhua Zhang, Cong Zhou, Bona Lu, Junjie Liu, Wei Wang, Lijun Zhang, Guoqing Wang","doi":"10.1016/j.cjche.2026.07.019","DOIUrl":"10.1016/j.cjche.2026.07.019","url":null,"abstract":"<div><div>The twisted-tape based vortex tube is recognized as a promising reactor for the highly energy-intensive steam cracking process. This study develops a short-length twisted tape, hereinafter termed the diameter-transformed vortex generator (DTVG), to reorganize decaying swirling flow through the coupling of bulk rotating flow and longitudinal vortices. Computational fluid dynamics with the RNG <em>k</em>–<em>ε</em> turbulence model was used to investigate macroscopic transport behavior, vortex structure evolution, sectional thermal–hydraulic performance and entropy generation. Based on vortex evolution, the DTVG vortex tube can be divided into induction, twin vortex and single vortex decay sections. This sectional swirling flow reorganization transforms the induction section into a vortex regulation region rather than a strong mixing region, while shifting the main heat transfer benefit to the twin vortex decay section. There, robust helical longitudinal vortex pairs promote wall-to-core transport, and near-wall shear renews the thermal boundary layer, yielding the highest Nusselt number and performance evaluation criterion values of 306.753 and 1.163, respectively. Entropy generation analysis further provides thermodynamic evidence for this functional transformation: compared with hollow twisted tape and conventional twisted tape, DTVG shows reductions of 21.7% and 21.3% in global entropy generation, with frictional entropy generation decreasing by 42.3% and 43.4%, indicating suppressed premature dissipation of mechanical energy during vortex initiation.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 281-294"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148996960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Scalable fabrication of Janus particles and interfacial engineering thereby Janus粒子的可伸缩制造及其界面工程

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-07-22 DOI: 10.1016/j.cjche.2026.06.017

Jiye Yang, Dayin Sun, Zhenzhong Yang

引用次数: 0

Formation mechanisms and mass transfer characteristics of solid–electrolyte interphase in lithium batteries 锂电池固-电解质界面形成机理及传质特性

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-08-14 DOI: 10.1016/j.cjche.2026.07.025

Jialin Li, Xueyi Yan, Boquan Li, Chen Ling, Xueqiang Zhang, Jiaqi Huang

{"title":"Formation mechanisms and mass transfer characteristics of solid–electrolyte interphase in lithium batteries","authors":"Jialin Li, Xueyi Yan, Boquan Li, Chen Ling, Xueqiang Zhang, Jiaqi Huang","doi":"10.1016/j.cjche.2026.07.025","DOIUrl":"10.1016/j.cjche.2026.07.025","url":null,"abstract":"<div><div>The solid–electrolyte interphase (SEI) remains the most central yet enigmatic factor determining the performance of lithium (Li) batteries. As a nanoscale layer composed of insoluble electrolyte decomposition products between the anode and electrolyte, the SEI serves two key functions in governing battery performance: passivating the anode against further electrolyte reactions and enabling Li-ion transport across the interface. The simultaneous fulfillment of these two functions, in which reactions and mass transfer are intrinsically coupled, considerably complicates the understanding of the role of the SEI. Furthermore, the sensitivity of the SEI to air and electron beams poses additional challenges for its characterization and understanding. Consequently, a thorough understanding of SEI formation reactions and associated mass transport characteristics is imperative for the continued advancement of Li batteries. Herein, we first elucidate the formation mechanism of the SEI, covering the generation of reduction products, nucleation and growth, and evolution, as well as the resulting composition and structural models. The mass transfer characteristics of the SEI are then systematically summarized, with emphasis on grain-boundary-mediated and nanopore-confined transport pathways. Subsequently, representative strategies for regulating the SEI to achieve improvement in passivation capability and ion transport are introduced. Finally, we offer insights into future research directions for deepening the fundamental understanding of SEI-related scientific issues and enabling rational SEI design.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 130-142"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Intensification of mass transport in key materials for hydrogen production by anion exchange membrane water electrolysis 阴离子交换膜电解制氢关键材料的质量输运强化

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-08-01 DOI: 10.1016/j.cjche.2026.07.009

Dongcheng Lin, Jing Liu, Zhuofan Zheng, Baoguo Wang

{"title":"Intensification of mass transport in key materials for hydrogen production by anion exchange membrane water electrolysis","authors":"Dongcheng Lin, Jing Liu, Zhuofan Zheng, Baoguo Wang","doi":"10.1016/j.cjche.2026.07.009","DOIUrl":"10.1016/j.cjche.2026.07.009","url":null,"abstract":"<div><div>Anion exchange membrane water electrolysis (AEMWE) has approached the threshold of industrial deployment over the past decade, offering the precious-metal-free chemistry of alkaline systems combined with high current density comparable to proton exchange membrane cells. However, component-level progress has consistently outpaced assembled-device durability. Reported degradation rates span nearly two orders of magnitude across groups using nominally similar materials, pointing to coupled failure mechanisms at the assembly level that single-component optimization cannot resolve. This review interprets the gap through a coupled-loop degradation model. Three self-sustaining feedback loops are proposed to operate in parallel at the membrane electrode assembly (MEA) level. The chemical failure loop is driven by hydroxide and radical attack on the polyelectrolyte, the mechanical failure loop by hydration-induced stress and microcrack propagation, and the structural failure loop by catalyst-ionomer interfacial debonding. Correspondingly, the mechanical, chemical, and structural enhancement dimensions each target one loop at its initiation site. Commercial durability requires simultaneous intervention across all three loops, rather than sequential optimization of any one. Mass transport intensification provides a unifying design framework for AEMWE, guiding catalyst, ionomer, and interface architecture. We survey recent progress in membrane chemistry and catalyst architecture, draw on parallel fields to identify promising materials for MEA fabrication, and highlight the challenges remaining in bridging laboratory demonstrations to commercial-scale deployment.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 246-268"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Reaction kinetics and process intensification of peroxycarbonate synthesis in a microreactor system 微反应器系统合成过氧碳酸盐的反应动力学及过程强化

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-05-22 DOI: 10.1016/j.cjche.2026.03.042

Lei Chen, Heng Fang, Jilei Han, Zhuo Chen, Dong Chen, Jianhong Xu

{"title":"Reaction kinetics and process intensification of peroxycarbonate synthesis in a microreactor system","authors":"Lei Chen, Heng Fang, Jilei Han, Zhuo Chen, Dong Chen, Jianhong Xu","doi":"10.1016/j.cjche.2026.03.042","DOIUrl":"10.1016/j.cjche.2026.03.042","url":null,"abstract":"<div><div><em>tert</em>-Butyl peroxy-2-ethylhexyl carbonate (TBEC) is widely used as a curing agent in unsaturated polyester molding processes. However, its conventional batch synthesis suffers from limitations in mass and heat transfer efficiency and presents considerable thermal safety hazards. In this work, the synthesis of TBEC was intensified by performing the peroxidation of 2-ethylhexyl chloroformate (2-EHCF) using <em>tert</em>-butyl hydroperoxide (TBHP) in a microreactor system. The reaction characteristics, including the main peroxidation and competing hydrolysis, were elucidated through batch experiments. Apparent kinetics were subsequently determined in the microreactor under intrinsic kinetic control that confirmed by Hatta number analysis. Results show the reaction order of 2-EHCF, NaOH and TBHP are 0.42, −0.02 and 3.82 respectively. The pre-exponential factor and activation energy are 16 L<sup>3.2</sup>·mol<sup>−</sup><sup>3.2</sup>·s<sup>−1</sup> and 26.1 kJ·mol<sup>−1</sup> respectively. Response surface methodology was then employed to optimize the process parameters and predict TBEC yield. Guided by these findings, a novel process that integrates continuous-flow microreaction with a room-temperature staged aging step was developed. The proposed strategy enhanced the TBEC yield from 94% to 98%, demonstrated significant process intensification by reducing the total processing time by nearly 40% through enhanced mass/heat transfer, doubled the space-time yield, and enabled safe operation across a broader temperature range. This study provides a scalable framework for intensifying similar hazardous processes with slow kinetics.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 80-94"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Stepwise direct lithium extraction from unconventional brines using phosphorus- and diketone-based systems 采用基于磷和二酮的系统逐步从非常规盐水中直接提取锂

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-08-14 DOI: 10.1016/j.cjche.2026.07.026

Jianfeng Zhang, Hongbo Sun, Meng Wei, Wanghai He, Chenglong Wei, Jiong Jiao, Marco Wenzel, Jan J. Weigand, Huizhou Liu, Liangrong Yang

{"title":"Stepwise direct lithium extraction from unconventional brines using phosphorus- and diketone-based systems","authors":"Jianfeng Zhang, Hongbo Sun, Meng Wei, Wanghai He, Chenglong Wei, Jiong Jiao, Marco Wenzel, Jan J. Weigand, Huizhou Liu, Liangrong Yang","doi":"10.1016/j.cjche.2026.07.026","DOIUrl":"10.1016/j.cjche.2026.07.026","url":null,"abstract":"<div><div>With the rapid development of lithium batteries, energy storage and controlled nuclear fusion, the demand for lithium is increasing rapidly. Direct lithium extraction from unconventional brines (<em>e.g.</em>, oilfield brines) is becoming increasingly critical. However, unlike traditional high Mg/Li salt lake brines, these systems typically contain high concentrations of calcium ions, which further increases the difficulty of lithium separation. To address these challenges, this study proposes two novel extraction systems that enable direct lithium extraction from brines with high concentrations of magnesium, calcium and sodium through a stepwise process. First, a triphenyl phosphate-tetraphenylborate synergistic system achieves 84% lithium recovery from simulated raw brine. By employing a strategy combining lithium stripping with <em>in-situ</em> precipitation of magnesium and calcium ions, the separation factors for Li/Mg and Li/Ca reach 178 and 1528, respectively. Single crystal structure analysis reveals the separation mechanism of lithium from magnesium and calcium by the organophosphorus extractant at the molecular level for the first time, and mass spectrometry analysis verifies the selective migration behavior of lithium ions during the extraction process. The resulting alkaline lithium solution is further treated with a novel diketone system, achieving a single-stage lithium extraction efficiency of 89% and a Li/Na separation factor of 415. The two-step strategy achieves an overall lithium recovery of 80% from raw brine, significantly higher than the conventional process. The obtained lithium carbonate is confirmed as battery-grade by XRD and composition analysis. This work provides molecular insights for designing novel lithium extractants and offers a new approach for direct lithium extraction from raw brines.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 236-245"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Super-tough PBS/lignin composites with aging resistance, antibacterial activity, and biodegradability 超韧PBS/木质素复合材料具有耐老化，抗菌活性和可生物降解性

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-07-29 DOI: 10.1016/j.cjche.2026.07.003

Tao Hu, Xue Yi Jia, Umay Amara, Weifeng Liu, Dong Yu Zhu, Xueqing Qiu

{"title":"Super-tough PBS/lignin composites with aging resistance, antibacterial activity, and biodegradability","authors":"Tao Hu, Xue Yi Jia, Umay Amara, Weifeng Liu, Dong Yu Zhu, Xueqing Qiu","doi":"10.1016/j.cjche.2026.07.003","DOIUrl":"10.1016/j.cjche.2026.07.003","url":null,"abstract":"<div><div>Poly(butylene succinate) (PBS) is a biodegradable renewable polyester widely used in agricultural films, packaging, and disposable products. Nonetheless, its inherent brittleness, high production cost, and limited functionality restrict broader practical applications. In this study, we proposed a biomass-modified PBS composite by synergistically employing fractionated lignin (AL-EtOAc) and thioctic acid (TA) through high-temperature melt blending. The lignin dispersion and the compatibilization of TA aided the formation of a flexible–rigid interlocking network with multiple cross-linked interfaces. The resultant architecture pointedly improved mechanical properties with tensile strength up to 36 MPa and elongation break at 1332.4%, which is 22-fold higher than neat PBS (60.04%). In addition, the composites demonstrated multifunctional performance, encompassing UV shielding, UV aging resistance, antibacterial activity, photothermal antibacterial effects, and biodegradability. Further, soil burial tests further confirmed that the incorporation of lignin and TA as natural compounds significantly accelerated the biodegradation rate of the PBS composites, achieving a mass loss of 18.14% after 16 weeks, which was six times higher than that of neat PBS. This work reveals a robust fabrication strategy for high-performance, multifunctional PBS-based biodegradable plastic, showing a great potential for sustainable packaging and agricultural applications.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 215-225"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148948055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Hydrogen oxidation anode for sustainable reductive electrosynthesis 用于可持续还原电合成的氢氧化阳极

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-08-18 DOI: 10.1016/j.cjche.2026.08.005

Siyun Dai, Wenyan Liu, Wen Liu, Xili Cui, Yiming Mo, Huabin Xing

{"title":"Hydrogen oxidation anode for sustainable reductive electrosynthesis","authors":"Siyun Dai, Wenyan Liu, Wen Liu, Xili Cui, Yiming Mo, Huabin Xing","doi":"10.1016/j.cjche.2026.08.005","DOIUrl":"10.1016/j.cjche.2026.08.005","url":null,"abstract":"<div><div>Organic electroreductive synthesis often needs to pair with sacrificial anodic reactions, such as metal dissolution or solvent decomposition, thus compromising the scalability and sustainability. Herein, we report a general and sustainable hydrogen oxidation anode enabled by a palladium (Pd) membrane to pair with various reductive electrosynthesis. The Pd membrane anode integrates multiple functions, including dissociative hydrogen adsorption, transmembrane diffusion, and electrochemical hydrogen atom oxidation. This configuration physically separates hydrogen gas chamber and electrolyte chamber, providing a “traceless” electron sink and proton source to pair with cathodic reactions. Thermodynamic and kinetic studies revealed that the anodic reaction is governed by dissociative adsorption and electrochemical oxidation steps, which are tunable <em>via</em> catalyst morphology and electrolyte engineering. Steady-state hydrogen oxidation current density can reach 5.4 mA·cm<sup>−2</sup> at a low oxidation potential (−0.21 V vs. Fc/Fc<sup>+</sup>) in nonaqueous electrolytes, sufficient to drive the majority of reported nonaqueous electroreductive protocols while maintaining the innocent role as a counter electrode reaction. The stability of palladium membrane anode was tested over 170-h continuous electrolysis. The generality of this strategy was demonstrated in two representative reductive transformations, including electrochemical nitroarene reduction and cross-electrophile coupling. These findings establish the Pd membrane anode as a broadly applicable alternative to sacrificial anodic reactions for sustainable nonaqueous reductive electrosynthesis.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 1-11"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148859051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Heterogenizing homogeneous cocatalysts within ordered-mesoporous Core@microporous shell UiO-66 nanoreactors for efficient and size-selective CO2 cycloaddition with epoxides 在有序介孔Core@microporous壳层UiO-66纳米反应器中制备均相助催化剂，用于环氧化物与CO2的高效和尺寸选择性环加成

IF 3.5 3区工程技术

Chinese Journal of Chemical Engineering Pub Date : 2026-09-01 Epub Date: 2026-07-28 DOI: 10.1016/j.cjche.2026.06.016

Shoukang Xiao, Ze Qin, Junying Chen, Liyu Chen, Kui Shen

{"title":"Heterogenizing homogeneous cocatalysts within ordered-mesoporous Core@microporous shell UiO-66 nanoreactors for efficient and size-selective CO2 cycloaddition with epoxides","authors":"Shoukang Xiao, Ze Qin, Junying Chen, Liyu Chen, Kui Shen","doi":"10.1016/j.cjche.2026.06.016","DOIUrl":"10.1016/j.cjche.2026.06.016","url":null,"abstract":"<div><div>The cycloaddition of CO<sub>2</sub> with epoxides represents a promising strategy for mitigating CO<sub>2</sub> emissions. However, most heterogeneous catalytic systems still rely on homogeneous halogen-based cocatalysts to achieve desirable activities, which significantly complicates subsequent product purification and separation. Herein, we report a facile strategy to heterogenize homogeneous Br-based cocatalysts by encapsulating them into within stable UiO-66-based core–shell nanoreactors for efficient CO<sub>2</sub> fixation. Specifically, ordered mesoporous Ce-based UiO-66 (OM-UiO-66) was first synthesized <em>via</em> a soft-template method. The homogeneous Br-based cocatalyst was then adsorbed into the mesopores of OM-UiO-66, followed by epitaxial growth of a microporous Ce-based UiO-66 shell with controllable thickness to complete the encapsulation, thereby yielding a size-selective nanoreactor that possesses both 0.6 nm sieving channels and 10 nm reaction channels. Importantly, the synergistic interactions among the high concentration of the cocatalyst confined in the mesopores, the abundant Lewis acidic Ce sites on the pore walls, the mesoporous microenvironment that facilitates the enrichment of CO<sub>2</sub> and epoxide substrates, and the judiciously controlled thickness of the microporous shell collectively impart the as-prepared nanoreactor with high catalytic activity, excellent recyclability, and remarkable substrate size selectivity for the cycloaddition of CO<sub>2</sub> with epoxides under ambient conditions. This work not only develops a novel strategy for the efficient fixation of CO<sub>2</sub> <em>via</em> the heterogenization of homogeneous catalysts with a novel MOF-based core–shell architecture, but also provides a compelling paradigm for the heterogenization of other homogeneous catalysts.</div></div>","PeriodicalId":9966,"journal":{"name":"Chinese Journal of Chemical Engineering","volume":"97 ","pages":"Pages 24-32"},"PeriodicalIF":3.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148938438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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