Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·123026
·
IF 7.5
Xiaoqing Xiong,Jinglong Li,Meiyu Zhen,Dongyan Liu,Yujian Li,Chang Wang,Ziyi Lu,Xingyu Wu,Huanda Zheng,Hongjuan Zhao
Photodynamic antibacterial therapy (PDAT) is recognized as a promising antibacterial strategy with high antibacterial efficiency and good biosafety. Porphyrin-based covalent organic frameworks (Por-COFs) with porous conjugated structures and exceptional stability serve as ideal platforms for high-performance in PDAT. Nevertheless, Por-COF synthesis faces crystallinity loss during post-synthetic purification. Here, Por-COFs were synthesized via one-pot reaction with the assistance of supercritical carbon dioxide (scCO 2 ), using 2,5-dihydroxyterephthalaldehyde and 5,10,15,20-tetrakis(4-aminophenyl) porphyrin (TAPP) as monomers, acetic acid (HOAc) as catalyst, and N , N -dimethylformamide (DMF) as co-solvent. The effects of volume ratio of DMF and HOAc ( V (DMF): V (HOAc)), scCO 2 pressure, temperature, and reaction time on the Por-COF morphology and crystallization were investigated. It showed that optimal Por-COFs-HP, with good crystallization, adsorption capacity, photosensitizing reactive oxygen species (ROS) activity and excellent photodynamic antibacterial rates against Staphylococcus aureus ( S. aureus ), Escherichia coli ( E. coli ), Pseudomonas aeruginosa ( P. aeruginosa ), and Staphylococcus epidermidis ( S. epidermidis ) was synthesized under the conditions of V (DMF): V (HOAc)= 8:7, 8 MPa, 70 °C, and 72 h. Por-COFs-HP was incorporated into nylon-66 (PA66) via interfacial polymerization combined with in-situ pulling spinning-coupled twisting to fabricate Por-COFs-HP@PA66 yarns and interwoven fabrics. Photosensitive properties and antibacterial rates of the resultant yarns and fabrics verified the retention of Por-COFs-HP’s excellent antibacterial activity after fabrication into the PA66 matrix. This study establishes a scCO 2 -assisted synthesis route for Por-COFs, and provides key technical references for the development and practical application of COFs-based antibacterial textiles.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
YiKai Wang,Zixue Zhao,Long Shi,Tianyi Zhou,Haohan Wan,Gang Zhang,Chuanrong Liu,Wenju Jiang,Lin Yang,Lu Yao,Junfeng Zheng,Zhongde Dai,Bart Van der Bruggen
Secondary interfacial polymerization tailors RO/NF TFCs for CO 2 capture. • A PEI secondary layer mitigates nonselective defects and enhances selectivity. • Mixed-gas tests show about 200 GPU CO 2 permeance with CO 2 /N 2 selectivity about 75. • Reversible 50 ppm SO 2 response; performance is retained after cycling. • PIP-based membranes show higher gas-separation performance than MPD-based analogues. Interfacial polymerization (IP), most commonly based on PIP/TMC and MPD/TMC chemistries, is the foundation for polyamide (PA) thin film composite (TFC) membranes used in water treatment. However, the reaction is rapid and diffusion-limited, which restricts control of the selective layer and often produces structural heterogeneity that lowers selectivity in gas separations. Here, we demonstrate that secondary interfacial polymerization (SIP) can be used to retrofit these liquid-separation membranes for CO 2 capture by creating an interfacial polyethyleneimine (PEI) repair layer that seals and reconstructs nonselective defects in situ. Under optimized conditions, the SIP membrane achieves ~200 GPU CO 2 permeance and ~75 CO 2 /N 2 selectivity (>2× the baseline). PEI seals nonselective voids inside the selective layer and forms an amine-rich, CO 2 -philic transport interface, so CO 2 permeance remains nearly unchanged even though the effective selective-layer thickness increases from 236 nm to 319 nm for the SIP-PIP membrane. The PEI overlayer also improves durability: after 50 ppm SO 2 exposure, CO 2 permeance decreased from 196 to 165 GPU and recovered to 185 GPU upon returning to SO 2 -free feed, and membranes retained >90% of initial performance after repeated pressure and temperature cycling. Notably, PIP-based membranes consistently show higher permeance and selectivity than MPD-based membranes, which is opposite to their ranking in aqueous separations, suggesting that solution-diffusion transport dominates under gas-phase operation. Overall, these results provide a scalable defect-repair strategy for low-cost repurposing of mature IP-based water-treatment membranes into CO 2 capture membranes. Download: Download high-res image (224KB) Download: Download full-size image
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高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 6
·155
·
IF 2.5
Hu Xinhui,Quan Yanhong,Li Haidong,Ren Jun
CO 2 activation represents a pivotal step in the CO 2 cycloaddition reaction with propylene oxide (PO) to form propylene carbonate (PC). This study prepared a chlorine-functionalized strongly alkaline polystyrene (CPS) catalyst via copolymerization and a TEAB/SiO 2 catalyst via silane coupling for CO 2 cycloaddition reactions. The CPS catalyst achieves nearly complete PO conversion (99.8%) with high selectivity (99.6%) towards PC and maintains a PC yield > 94% even after 10 reaction cycles. In contrast, the TEAB/SiO 2 exhibits rapid deactivation, with the PC yield declining from 66.8% to 5.1% after three cycles. Dynamically, the CPS catalyst exhibited a marked reduction in activation energy (20.1 kJ·mol −1 ) compared to TEAB/SiO 2 (32.9 kJ·mol −1 ), corroborating CO 2 activation through covalently anchored quaternary ammonium groups, which benefited from the higher alkalinity (2.65 mmol·g −1 ). Moreover, the outstanding stability of the CPS catalyst arises from the robust crosslinked framework of polystyrene and divinylbenzene. This work provides a strategic approach for designing alkaline catalysts and establishes a novel pathway to develop high-performance alternatives to ionic liquids for CO 2 activation in the cycloaddition reaction between CO 2 and PO. Graphical The alternative text for this image may have been generated using AI.
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AICHE JOURNAL
·
2026
·
IF 4.4
Qi Liu,Tong Luo,Guowei Ma,Beiqi Sun,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Formulating superior absorbent by amine blending is a vital strategy for CO 2 capture. However, the blend of different amines may affect their chemical stabilities and hinder the long-term operation of CO 2 capture system. This work studied the stability of amine blends composed of 1-amino-2-propanol (1AP) and various tertiary amines, aiming to reveal their influence on thermal degradation. The addition of 1AP reduced the thermal stability of tertiary amines, as 1AP accepts alkyl groups from the protonated tertiary amines. Density functional theory (DFT) was used to verify the proposed thermal degradation mechanism of blended amines. The computational results suggest that the increase in blended amine loss was closely related to the decrease of the free energy barriers for the alkylation reactions between tertiary amine and 1AP. In addition, the thermal stability of blended amines associated with amine protonation degree in solution based on the 13 C NMR analysis.
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高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Xingwu Zhai,Yuchun Liu,Tianchen Wei,Leyi Su,Jing Zhang,Liang Wu,Yuxin Xiao,Tianqi Liu,Xinyun Wang,Cong Han,Zhaodi Fan,Min Zhou
The practical implementation of Li─CO 2 batteries is constrained by the challenging decomposition of Li 2 CO 3 . While cleaving C─O bonds is predominantly focused on, Li─O cleavage is the initial and rate-limiting step. The Li─O bond strength is a key descriptor for this process, which involves increasing the population of its antibonding orbital. The HOMO of Li 2 CO 3 is composed of O p -orbitals that couple with d -orbitals of transition metals. Herein, over-coordination of metal sites modulates the electronic distribution in metal d -orbitals and promotes O p -orbital polarization, converting symmetric metal pairs into asymmetric pairs. This resulting localized dipole moment induces an asymmetric interfacial polarized electron density distribution and targeted bond polarization. The dipole at asymmetric sites polarizes O p -orbitals and promotes electron transfer into the Li─O antibonding orbital. Using WB as proof-of-concept, this asymmetry electronic polarization increases the population of Li─O antibonding orbitals and weakens their interaction. This results in a markedly low decomposition energy barrier of 0.53 eV for Li 2 CO 3 and an ultralow charge voltage of 2.99 V. The battery also exhibits stable operation for 500 h at 120°C with high energy efficiency (74.43%). This work highlights local dipole engineering and establishes electronic asymmetry-mediated activation for efficient Li─CO 2 batteries.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Jiawei Wang,Jiacheng Li,Fumin Wang,Xubin Zhang,Shuai Liu,Shuai Niu,Liang Chen,Xu Wu
Stabilizing the Cu δ+ (1 < δ < 2) valence state during CO 2 reduction reaction (CO 2 RR) process is essential to enhance the C-C coupling and further promote the conversion of CO 2 into value-added C 2+ products. Herein, we propose a new strategy to stabilize the Cu δ+ under the synergistic effect of 4f orbital and oxygen vacancies (O v ) through the construction of Ce doped CuO with enriched O v via symbiotic strategy (CuCeO-O v ). Theoretical calculations and experimental results show the derived gradient orbital coupling O v -[Ce 4f-O 2p-Cu 3d] unit with Ce 4f as electron buffer as well as O v as electron supply station can facilitate the electron itinerancy during CO 2 RR process, which is beneficial to reinforce the Cu-O covalency and inhibit peroxidation of Cu δ+ , thus endowing CuCeO-O v with a highly active (Faradaic efficiency of C 2 H 4 reaches 51% at −1.3 V vs. RHE) and stable bidirectional self-regulating capability (the current density and FE of C 2 H 4 show virtually no attenuation even after 13 h) simultaneously. This work not only gives a profound insight to the synergistic effect of dopants and O v in metal oxides but also provides new guidance to structural design of high-performance insert materials.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122829
·
IF 7.5
Peijun Li,Weicong Xu,Xing Wang,Chao Liu,Anze Ning,Qingwen Chen,WulejiasiI Aerxin,Tao Li,Haowei Huang,Rui Xiao
The electrochemical conversion of CO₂ into gaseous hydrocarbon fuels (CH₄ and C₂H₄) has become a prominent research focus, relying heavily on high-performance catalysts. In this study, commercial pure Cu foil was etched with FeCl₃, utilizing a simple etching approach to alter the etching time (30 s, 60 s, 90 s, and 120 s) to reconstruct the Cu foil surface and form active centers such as grooves and cube-like Cu nanoparticles. The hydrogenation of the *CO intermediate and C–C coupling were facilitated by these features, thereby promoting the formation of gaseous hydrocarbon products during CO₂ electroreduction. By varying the etching time, the groove morphology and the size, surface area, and roughness of the cube-like Cu nanoparticles were systematically tuned. The Cu foil electrode etched for 60 s exhibited the highest surface area and roughness, together with cube-like Cu nanoparticles of approximately ∼43.89 nm, thereby providing optimal active sites for *CO adsorption and selective hydrocarbon formation. At −1.2 V versus RHE, a total hydrocarbon Faradaic efficiency (FE) of 64.94% was achieved, including 33.34% for CH₄ and 31.60% for C₂H₄. These results demonstrate an effective strategy for promoting selective hydrocarbon production during CO₂ electroreduction.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Xiangji Zhou,Zhilong Zheng,Jian Zhang,Jiapeng Ji,Xiaolong Zhang
The precise control of product selectivity in the electrochemical CO 2 reduction reaction (ECR) toward specific multi-carbon (C 2+ ) compounds remains a significant challenge. This work demonstrates that incorporating germanium (Ge) into copper (Cu) nanoparticles to form a solid solution effectively tunes the surface electronic states of Cu, thereby steering the C 2+ product distribution from ethylene toward ethanol. First-principles calculations predict that an optimal Ge content (Cu 94 Ge 6 ) optimizes the Cu 3d orbital hybridization and shifts the d-band center, strengthening the adsorption of the critical * CH 2 CHO intermediate and favoring its hydrogenation pathway. Experimentally, the Cu 94 Ge 6 catalyst exhibits an ethanol-to-ethylene ratio of ∼1.8, significantly higher than that of pure Cu (∼0.6). Comprehensive characterization, including in situ ATR-FTIR and quasi in situ XPS, reveals that the Ge-induced electronic modulation enhances the adsorption of COCHO/CH 2 CHO intermediates and promotes the presence of isolated interfacial water, which collectively facilitates ethanol formation. This study presents a viable strategy for regulating C 2+ product selectivity through solid-solution electronic engineering in Cu-based electrocatalysts.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Hengyu Li,Yang Liu,Qinghai Long,Chao Liu,Huawang Zhao,Zuoming Zhou,Guohua Jing,Bihong Lv
Amine-based CO 2 capture technologies face major hurdles in large-scale industrial deployment due to the high energy demand for solvent regeneration. Solid acid catalysts enable low-temperature desorption via proton transfer acceleration to reduce energy consumption, yet their practical deployment is hindered by active site leaching and deactivation, undermining stability and reliability. In this study, an acid-functionalized ionic liquid (AFIL), [DBAEH][AlCl 4 ], is introduced as a homogeneous catalyst to intensify CO 2 desorption from CO 2 -loaded MEA solutions at low temperatures. Its introduction accelerated the MEA regeneration rate by 64.46% and improved the overall regeneration efficiency by 26.87%. In addition, the AFIL effectively lowered the thermal energy demand during CO 2 desorption, reducing the relative regeneration heat duty by 17.00%. Notably, the catalyst maintained stable performance over ten consecutive absorption–desorption cycles, which indicate that the AFIL catalyst delivers superior catalytic performance and operational stability. Mechanistic insights derived from FT-IR and 13 C NMR characterizations suggested that the Brønsted acid sites (BASs) serve as proton donors, while the Lewis acid sites (LASs) promote C N bond scission, collectively enhancing carbamate breakdown and the deprotonation of protonated amines. Furthermore, the acid sites exhibit excellent stability against deactivation under catalytic conditions, rendering regeneration or replacement unnecessary. This dual–acid catalytic mechanism provided a promising avenue for lowering the regeneration heat load and operational expenses associated with industrial CO 2 capture processes.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Bin Xu,Xiaoyi Gao,Xi Tang,Xiaoshan Li,Cong Luo,Fan Wu,Wen Chen,Liqi Zhang
In gas purification processes, absorption in packed columns is one of the most commonly used and highly efficient methods for gas removal. However, the prediction of mass transfer performance in packed columns often suffers from significant uncertainties, which has long been a critical challenge in industrial design, process analysis, and simulation. To address this issue, the present study introduces the concept of ineffective porosity (ε u ) and systematically evaluates its role in improving the prediction accuracy of mass transfer performance in packed columns. First, the value of ε u was determined using the Billet inverse calculation method, and the results demonstrated an approximately linear relationship between ε u and the liquid holdup (H). Subsequently, experiments were conducted to examine the effects of operating parameters on the effective interfacial area (a v ) and mass transfer performance. Incorporating ε u into the a v model reduced the absolute average deviation (AAD) from 13.9% to 9.6%. Similarly, the incorporation of ε u into various mass transfer models has been shown to enhance their predictive accuracy. Finally, the mass transfer mechanism of CO 2 absorption by amine solutions was explored, demonstrating that the process is controlled by reaction kinetics. These findings not only highlight the critical role of ineffective porosity in mass transfer modeling but also provide methodological guidance for the precise design, process optimization, and industrial application of packed columns.
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Wenli Wu,Ming Chen,Chuanfu Wang,Yuxin Jin,Gang Xie,Xinyang He,Daiqi Ye,Limin Chen
CO 2 -assisted oxidative dehydrogenation of ethane (CO 2 -ODHE) has attracted growing attention as a promising route for the effective utilization of shale gas and CO 2 to produce ethylene. A 1.5 wt% Co/TiZrO 4 catalyst was identified highly effective for the CO 2 -ODHE reaction, achieving an ethane conversion of 43.7%, an ethylene yield of 27.9% and a CO 2 conversion of 20.1% at 650 ℃ − performances that surpasses many reported non-Cr-based transition metal catalysts. Based upon our recently developed analytical method for quantitative elucidation of ethane-CO 2 reaction pathways, combined characterization using powder X-ray diffraction (XRD), hydrogen temperature-programmed reduction (H 2 -TPR), in-situ Raman, in-situ NO adsorption diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and quasi in-situ X-ray photoelectron spectroscopy (XPS) revealed that Co 3+ species exhibited higher intrinsic activity than Co 2+ for ethane dehydrogenation. More importantly, this study provide first evidence for a temperature dependent reaction mechanism- from a Mars-van Krevelen mechanism at low temperature, to a coupled direct dehydrogenation (DDHE) and reverse water gas shift (RWGS) mechanism at intermediate temperatures, and finally to dry reforming of ethane (DRE) at high temperature. These mechanistic insights establised a robust foundation for the rational design of highly selective and thermally stable catalysts for efficient ethylene production via CO 2 -ODHE.
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高影响因子
MACROMOLECULES
·
2026
·
IF 5.7
Jinyu Li,Yongchao Sun,Tianyou Li,Zeyuan Gao,Fangxu Fan,Lu Bai,Gaohong He,Canghai Ma
Thermally rearranged (TR) polymers have emerged as promising candidates for gas separation membranes but often suffer from poor resistance to CO2-induced plasticization. In this study, rigid biphenyl (TMB) units were introduced into the polyimide backbone, and bromine atoms were incorporated into the polymer side chains to enable controlled cross-linking. The polymers underwent in situ debromination during thermal rearrangement, transforming into cross-linked PBO networks to enhance both permeability and selectivity. The optimized 50%-Br-6FTA-PBO(1:1) membrane exceeded the 2008 Robeson upper bounds for CO2/CH4 and H2/CH4 separations, as well as the 2018 upper bound for CO2/CH4 mixed gas separation. Moreover, the cross-linked network structure conferred excellent antiplasticization performance under CO2 pressures up to 600 psi and maintained stable gas separation properties over 1000 h of aging. This work provides a universal strategy for designing TR membranes that possess high permeability, high selectivity, excellent anti-CO2 plasticization performance, and long-term stability.
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高影响因子
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