CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Qingnan Wang,Yueyangchao Yu,Longjie Liu,Yi Ye,Xinglei Zhao,Chongshan Yin,Bin Liu,Shaofei Wang
Efficient separation of CO 2 from CH 4 is a critical unit operation for biogas upgrading and achieving carbon neutrality goals. While mixed-matrix membranes (MMMs) offer an energy-efficient alternative to traditional separation processes, their industrial deployment is often restricted by engineering challenges, specifically filler agglomeration and non-selective interfacial defects. Herein, we report a novel MOF (metal–organic framework) gel network templated polymerization strategy that effectively circumvents these limitations. In this approach, a continuous, pre-formed network of UiO-66 MOF gel serves as a structural scaffold, within which the 6FDA-ODA polyimide matrix is directly polymerized. This method fosters exceptional interfacial adhesion and uniform dispersion of the filler, successfully eliminating non-selective defects. The resulting MMMs exhibit remarkable gas separation performance, with the optimal membrane (MA-0.075, with 1.6 wt% UiO-66 gel loading) achieving a CO 2 permeability of 30.9 Barrer and a CO 2 /CH 4 selectivity of 135.5 under mixed-gas conditions. This represents enhancements of 212 % and 162 %, respectively, over the pristine 6FDA-ODA polyimide membrane, surpassing the 2008 Robeson upper bound. Furthermore, the membrane demonstrated excellent operational stability over 120 h. This work provides a scalable fabrication route for advanced MMMs, demonstrating significant potential for energy-efficient gas separation applications.
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JOURNAL OF MEMBRANE SCIENCE
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2026
·
IF 8.8
Yingnan Ma,Zhen Xu,Yulu Zhang,Zixuan Guo,Juan Chen,Panliang Zhang,Kewen Tang
This study innovatively proposed an in-situ confined polymerization strategy of trimesoyl chloride (TMC) and piperazine (PIP) within MOFs nanosheets, successfully constructing a thin film nanocomposite (TFN) separation membrane with excellent interfacial compatibility. The method employed MOFs nanosheets as confined templates to achieve bottom-up in-situ construction of a continuous and dense polyamide matrix. By precisely controlling the number of polymerization cycles, the MOFs content in the functional layer was effectively regulated from 83.3 wt% to 42.6 wt%. Benefiting from the molecular-level interfacial compatibility between MOFs and the polymer phase, as well as the synergistic effect of efficient solution diffusion and fine molecular sieving mechanisms, the TFN membranes demonstrated significantly enhanced CO 2 separation performance, CO 2 permeance reached 1688.3 GPU with selectivities of 36.4 for CO 2 /N 2 and 38.9 for CO 2 /CH 4 , which surpassed the Upper bound (2008 and 2019). The TFN membranes exhibited outstanding long-term operational stability (selectivity fluctuation <3.6%) under rigorous conditions including prolonged 14-day continuous testing and variable temperature (35-75 °C) and pressure (0.1-0.5 MPa) conditions. This work provided a new paradigm for the precise design and scalable fabrication of gas separation membranes, opening new avenues for the development of high-performance separation membranes.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2026
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IF 4.6
Guoliang Li,Wei Gao,Junpeng Liu,Haipeng Jiang
Aluminum nanoparticles (ANPs) are promising energetic materials owing to their high energy density and advanced reactivity, but they are also prone to explosion. In this study, a polydimethylsiloxane-containing dry-water suppressant (PDMS@DW) is prepared, and the inhibitory effects of CO 2 and PDMS on ANP oxidation and explosion are evaluated using thermal analysis and dust-explosion experiments. The particle-surface reaction inhibition mechanism is elucidated by ReaxFF MD simulations. The experiments show that PDMS@DW significantly weakens oxidation heat release, increases the apparent activation energy, and delays the oxidation process, while the introduction of CO 2 or PDMS@DW markedly reduces both maximum explosion pressure and pressure rise rate. ReaxFF MD results reveal that CO 2 and PDMS suppress the formation of an oxygen-rich, negatively charged environment on the outer surface of the Al 2 O 3 -shell, thereby inhibiting the thermal diffusion of shell-O and core-Al atoms towards the inner shell interface, ultimately slowing down the melting of the Al-core. Based on the temperature rise rate, ANP combustion in O 2 /CO 2 atmospheres is partitioned into surface combustion, slow combustion and self-sustaining combustion. Surface combustion is identified as the dominant phase responsible for overpressure generation during ANP explosions. Atomic displacement analysis indicates surface combustion is governed primarily by reactions between external-O and both shell-Al and exposed core-Al atoms. CO 2 most effectively suppresses this critical stage. In contrast, PDMS promote the formation of a C/Si-containing coating on the particle surface, enabling inhibition throughout the entire combustion process; hence, ANPs in CO 2 /PDMS mixed systems do not enter the self-sustaining combustion stage within the same timescale. Novelty and significance statement This work employs ReaxFF MD simulations to investigate the ignition and combustion of ANP in CO 2 /PDMS atmosphere, revealing the critical stage and atomistic mechanisms associated with overpressure formation in nano-Al dust explosion. The simulation results are qualitatively supported by the experimental observations. The study clarifies the apparent dual behavior of CO 2 —enabling self-sustained combustion of ANP while simultaneously suppressing dust explosions—and, for the first time, reveals the suppression mechanisms of ANP ignition and combustion at the atomic scale. The research methodology and insights presented herein provide a theoretical foundation for the rational design of advanced dust explosion suppression materials.
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Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·123544
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IF 7.5
Zihao Wei,Yulin Qin,Mengbo Zou,Lin Jia,Haorun Li,Yuekun Zhang,Jinyu Wang,Zeyu Guo,Hao Wu,Zeyu Zhang,Shanghong Zeng
The rational surface regulation of Cu electrocatalysts through doping foreign components has emerged as a feasible pathway in electrochemical CO 2 reduction reaction. Herein, the catalysts comprising the Cu 0 -Sm 3+ -Cu + sites are reported to explore the doping-driven the alteration of surface structure and properties. The incorporation of Sm with oxygen affinity in Cu 2 O/Cu decreases the crystallite sizes and evokes lattice expansion of Cu 2 O and Cu to generate surface defects. The interaction of Cu 0 , Sm 3+ and Cu + promotes dual-carbon production by stabilizing Cu + and enhancing *CO coverage and water dissociation. Our findings therefore reveal the role of Sm in promoting beneficial changes of Cu-based electrocatalysts.
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Journal of Materials Chemistry A
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2026
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IF 9.2
Rong Wang,Xinyi Yuan,Qingxiang Ma,Yan Wang,Jucang Ke,Xiaopeng Li,Xinhua Gao,Jian Sun,Tian-sheng Zhao
The oxidative dehydrogenation of propane with CO2 (CO2-ODHP) technology is recognized as a promising new route for propylene production, owing to its advantages in energy saving, high yield, and environmental friendliness. However, the inherent complexity of the reaction system and catalyst structures has led to ongoing debates regarding its activation mechanisms and reaction pathways. Thus, the development of high-performance catalysts capable of synergistic activation of propane and CO2 with simultaneous high propylene selectivity continues to be a key objective and challenge. This study aimed to investigate the catalytic activity of Pt-based catalysts supported on CeOx nanoclusters for the CO2-ODHP reaction, from the perspective of enhancing CO2 adsorption and activation. Experimental results demonstrate that the oxygen-rich defect structure on the CeOx nanoclusters significantly promotes the activation and dissociation of CO2. Furthermore, the incorporation of Sn effectively enhances the dispersion of Pt species and their surface electron density, thereby further strengthening the strong adsorption and activation of propane while simultaneously facilitating the desorption of propylene. Following continuous operation for 5 h at 550 °C, the 0.5Pt2.0Sn/CeOx-SiO2 catalyst demonstrated superior catalytic performance, achieving a propane conversion of 45.3% and a propylene selectivity of 93.6%. Based on in situ DRIFTS analysis, a possible reaction mechanism for CO2-ODHP on this catalyst is proposed. The findings of this study provide crucial theoretical guidance and practical references to further advance high-performance Pt-based catalysts for CO2-ODHP reactions.
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Chem Catalysis
·
2026
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IF 10.7
Yunshuo Wu,Xiaole Weng,Haiqiang Wang,Zhongbiao Wu
CO 2 -assisted oxidative dehydrogenation of propane (CO 2 -ODHP) is a promising route for propylene production and CO 2 utilization, but catalyst sintering under harsh reaction and coke-burning conditions limits industrial deployment. Here, we report a practical regeneration strategy in which non-thermal H 2 plasma rapidly restores Au/MoS 2 catalysts that were deactivated by sintering at 600°C. The plasma treatment regioselectively reconstructs supported Au nanoparticles into raft-like Au domains enriched in unsaturated Au δ+ sites and stabilized by strong Au−S interactions, and this effect results in a 6.3-fold increase in propylene yield. The regenerated catalyst shows industrially relevant propylene productivity, high operational stability, and repeated regenerability. Mechanistic studies indicate that the Au rafts, electronically promoted by subsurface sulfur, facilitate propane C−H activation while accelerating hydrogen spillover and propylene desorption. These findings establish plasma-driven catalyst reconstruction as an effective regeneration strategy for light-alkane dehydrogenation and sustainable olefin production.
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Catalysis Science & Technology
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2026
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IF 4
Guoqing He,Yonghao Liang,Li Guo,Qianqian Zhang,Ying Xie,Zefan Hu,Jialing Chen,Xiaoqin Wu,Ran Zhang
Metal-organic frameworks (MOFs) exhibit promising catalytic potential for various reactions owing to their unique structure composed of designable metal-oxo clusters bridged by organic linkers, modifiable frameworks, and intrinsic porosity. Currently, defective MOFs are gaining considerable attention due to their accessible Lewis acid sites, tunable ligands, and superior performance compared with pristine MOFs. In this work, we have developed an amino-functionalized UiO-66 with ligand defects, denoted as UiO-66-DABAx (where x represents the molar percentage of 3,4-diaminobenzoic acid (DABA) relative to the total linker content), which enables an efficient pathway for the cycloaddition reaction of CO2 with epoxides under mild conditions. The increased density of Lewis acid sites and the presence of amino-functionalized ligands synergistically facilitate the ring-opening of epoxides and CO2 adsorption. Compared with pristine UiO-66, UiO-66-DABAx exhibits a stronger affinity for CO2. More importantly, UiO-66 modified with 20 mol% DABA (UiO-66-DABA20) exhibits optimal catalytic activity in the CO2 cycloaddition reaction, yielding a cyclic carbonate of 95%. This study paves a promising strategy for the chemical fixation of CO2 into cyclic carbonates using amino-functionalized defective UiO-66 as a potential heterogeneous catalyst under mild reaction conditions.
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Journal of Materials Chemistry A
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2026
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IF 9.2
Shilin Wei,Weiqi Liu,Lang Xu
This study systematically investigates how lanthanoid elements and electromagnetic fields unite to enhance the performance of nickel-based catalysts in the electrocatalytic carbon dioxide reduction reaction. First, we synthesized and analyzed 14 lanthanoid-doped Ni nanoparticle catalysts. The results show that doping with lanthanoids effectively modulates the nickel electronic structure, raising the CO faradaic efficiency from 72.8% in the undoped case to generally over 90% for all lanthanoid-doped catalysts. Further research reveals that applying electric and magnetic fields produces an equivalent effect on current density: the higher the external magnetic or electric field strength, the higher the current density. Finally, the performance enhancements from both the internal factor, electronic structure modulation, and external factors, magnetic or electric fields, were found to be unified under one core idea – the promotion of charge-transfer processes. Consequently, this study presents unique perspectives on the unity in the diversity of factors governing the catalytic performance.
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BIORESOURCE TECHNOLOGY
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2026
·
IF 8.2
Li Sun,Cao Zhenzhou,Cui Jixian,Huang Liuyang,Qi Xiaonan,Wei Yanjie,Li Xianhui
Developed Fe 2 O 3 NPs-embedded membranes to overcome gas–liquid mass transfer limits. • Fe 2 O 3 NPs raise surface area and add C O groups, thereby enhancing CO 2 adsorption. • Fe 2 O 3 NPs-nanofiber membranes enhance biomass, CO 2 fixation, and delay decline. • Fe 2 O 3 NPs promote stable biofilm formation, enhancing initial attachment and growth. • Fe 2 O 3 NPs enhance ATP, photosynthesis and XDLVO adhesion for CO 2 fixation performance. Algae-based carbon capture and utilization (CCU) technique offers a sustainable strategy for CO 2 mitigation, but its efficiency is often limited by poor gas–liquid mass transfer and unstable carbon availability. Here, this study developed an iron oxide nanoparticle (Fe 2 O 3 NPs)-incorporated electrospun nanofiber membrane to enhance CO 2 capture and microalgal fixation. Results revealed that the Fe 2 O 3 NPs was able to reduce fiber diameter, refine pore architecture, and increase specific surface area, thereby the improved CO 2 adsorption. In Chlorella cultivation, the final biomass concentration and CO 2 biofixation rate of modified membrane increased by respective 11.6%±1.2% and 14.3% compared with that of pristine nanofibers. Furthermore, the modified membrane significantly promoted the early-stage biofilm formation, yielding biofilms that were 47.9% thicker, denser, and exhibited increased rougher surface. Nanoparticle-induced “microhooks”, together with enhanced EPS secretion, strengthened algal attachment, increased cell density, and improved spatial homogeneity, thus creating a favorable microenvironment for rapid biofilm development. Cellular analyses demonstrated that membranes modified with Fe 2 O 3 NPs increased intracellular ATP by 45.6%, superoxide dismutase activity by 39.9%, and specific growth rate by 41.8% compared to the blank controls, indicating enhanced metabolic activity and stress resistance. Physicochemical characterization further showed that a reduction in electrostatic repulsion and an increase in hydrophobicity. Meanwhile, Lifshitz-van der Waals (U LW ) and Lewis acid-base (U AB ) interaction energies increased by approximately twofold and 2.74-fold, respectively. These changes synergistically enhanced initial algal adhesion and attachment stability, facilitating CO 2 enrichment. In summary, this work elucidates the synergistic bio-physicochemical mechanisms underlying nanoparticle-modified membranes and specify their potential for advancing efficient microalgae-based CCUS technologies. Download: Download high-res image (191KB) Download: Download full-size image
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ACS Catalysis
·
2026
·Vol. 16
·期 15
·14667-14679
·
IF 13.6
Qi Yuntao,Xue Lei,Zhao Shichao,Deng Tiansheng,Qin Yong,Zhang Bin
The hydrogenation of CO 2 to CO represents a promising synthetic pathway to replace coal gasification and methane reforming. Ru-based catalysts showed high activity in CO 2 hydrogenation but lower CO selectivity due to competing methanation reactions. Here, we reported a surface sulfur (S) decoration strategy to shift the methanation to 99% selectivity for CO on the Ru/TiO 2 catalyst in CO 2 hydrogenation. The optimized 2%Ru/TiO 2 -SO catalyst achieved a CO 2 conversion of 57.9% with 100% CO selectivity at 550 ° C, and it operated stably even in a reaction gas containing an H 2 S impurity. Notably, even after high-temperature oxidation treatment at 800 ° C, the 2%Ru/TiO 2 -SO catalyst still retains high CO selectivity (>98.2%). Structural characterization confirms strong S–Ru interactions between S species and Ru nanoparticles in S-decorated catalysts, with highly dispersed S species bonded to the Ru surface as S 2− , thereby leaving the surface Ru atoms in an electron-deficient state. Mechanistic studies reveal that CO was formed via direct dissociation of CO 2 on this 2%Ru/TiO 2 -SO catalyst. The adsorption strength of CO* species and H 2 activation capacity were significantly suppressed on S-decorated catalysts featuring electron-deficient Ru species, thus inhibiting the deep hydrogenation of CO and enabling exclusive CO generation. The surface S decoration strategy employed here will provide insights and guidance for the design of supported metal catalysts with tunable selectivity in other heterogeneous catalytic hydrogenation reactions, particularly those operating at high temperatures.
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ACS Catalysis
·
2026
·Vol. 16
·期 15
·15348-15362
·
IF 13.6
Rhimi Baker,Harrath Karim,Liu Yifan,Liu Zheyang,Zhou Min,El-Khodary Sherif A.,Shi Weidong,Jiang Zhifeng
Photocatalytic CO 2 reduction to C 2 H 4 remains challenging due to inefficient multielectron transfer and sluggish C−C coupling kinetics. Herein, we demonstrate that precise engineering of metal−organic framework (MOF) nodes establishes dual-functional active sites that synergistically drive C−C coupling and H 2 O activation. A hybrid photocatalyst is constructed by integrating a porphyrinic MOF (Fe-MOFBPy), featuring axially coordinated bipyridine ligands that modulate paddlewheel Fe−N nodes, with carbon nitride (CN) to form a heterojunction. Controlled linker depletion introduces defects that generate coordinatively unsaturated Fe sites and enable rational tuning of Fe−N bonding. Combined density functional theory and ab initio molecular dynamics simulations reveal that the Fe−N bond acts as a dual-functional site, where the N atom facilitates H 2 O activation and proton transfer, while the Fe center promotes *CO + *CHO coupling toward C 2 intermediates. In contrast, defective MOFs with reduced Fe−N coordination form Fe−O sites that exhibit inferior activity due to inefficient H 2 O activation. Notably, the intrinsic flexibility of the Fe−N bond lowers the kinetic barrier for H 2 O dissociation. Consequently, the catalyst achieves a C 2 H 4 production rate of 24.5 μmol g −1 h −1 with an 87.1% electron-based selectivity, outperforming analogous systems. This work provides a blueprint for designing dual-functional sites in MOFs for solar-driven C 2 H 4 synthesis.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Hanlin Wang,Xianglin Chen,Yafei Guo,Pu Huang,Antian Wang,Jingyi Shi,Huaxiang Gao,Ruilin Wang,Chuanwen Zhao
Electrochemical CO 2 reduction to syngas driven by renewable energy offers a sustainable alternative to conventional fossil-fuel-based processes, while maintaining a stable H 2 /CO ratio under the inherently fluctuating potentials remains a substantial challenge. In this study, a series of supported Zn catalysts are fabricated by electrodepositing Zn onto Cu foil substrates, with a systematic investigation into the effects of deposition current density (−5 to −20 mA/cm 2 ) and deposition time (10 to 20 min) on catalyst structure and performance. Characterization results reveal that, with increasing deposition parameters, Zn species evolve from discrete nanoplates into an interwoven network of wrinkled structures, accompanied by decreased work function and charge transfer resistance. The synthesized catalysts exhibit a favorable balance in activity toward the electrochemical CO 2 reduction reaction (eCO 2 RR) and hydrogen evolution reaction (HER), thereby enabling highly tunable syngas production with H 2 /CO ratios ranging from 0.5 to 5.4. Notably, the Cu-Zn catalysts demonstrate remarkable stability in syngas composition, maintaining a nearly constant H 2 /CO ratio across a wide potential window of −1.11 to −1.41 V vs. reversible hydrogen electrode (RHE). Furthermore, the Cu-Zn-10–10 catalyst exhibits excellent durability under fluctuating voltage conditions over 24 h, highlighting its potential for seamless integration with intermittent green electricity. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations indicate that the Cu-Zn bimetallic sites moderately enhance *CO adsorption, inhibiting its rapid desorption. Moreover, the energy barriers of eCO 2 RR and HER show little variation with potential, which collectively ensure the stability of the H 2 /CO ratio within the range of −1.11 to −1.41 V vs. RHE.
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