Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123910
·
IF 7.5
Wenhao Hou,Jiaqi Xing,Lina Qiao,Yun Ju,Yaqi Liu,Jing He,Wenwen Wei,Jie Jiang,Hong Zhang
Water microdroplets possess energetic interfaces that can promote the reduction and utilization of carbon dioxide (CO 2 ). However, the mechanism by which acidity modulates CO 2 interfacial reactions in microdroplets remains unclear. Herein, CO 2 fixation in pyruvate-containing microdroplets was investigated over a pH range of 1.5–10.1. Online mass spectrometry showed that acidic conditions significantly enhance the reaction between CO 2 and pyruvate, particularly in smaller droplets and at lower pyruvate concentrations. A similar promotion was observed for another α-keto acid, α-ketoglutaric acid. Mechanistic analysis suggests that electrostatic attraction between interfacial anions (Cl - and OH - ) and protons amplifies the interfacial electric field at the air-water interface, which drives CO 2 fixation rather than conventional proton catalysis. These findings highlight the critical role of acidity in interfacial CO 2 -related chemistry and may help improve the understanding of environmentally relevant microdroplet carbon processes.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Kai Zhu,Zhenmao Zhang,Xinyin Bai,Fangfang Chang,Qing Zhang,Ge Li,Zhengyu Bai
Electrochemical pre-reconstruction creates CuO/Cu 2 O/Cu/CeO 2 @C heterointerfaces. • Carbon confinement stabilizes multivalent Cu interfaces during CO 2 electroreduction. • CeO 2 modulates the electronic structure and interfacial charge distribution of Cu. • Reconstructed interfaces tune the thermodynamics of *CO and *OCCO formation. • Ethanol Faradaic and cathodic energy efficiencies reach 75.6% and 30.9% at −0.9 V vs. RHE. The electrochemical CO 2 reduction reaction (CO 2 RR) to ethanol provides a carbon–neutral route for the sustainable production of value-added chemicals, yet achieving high ethanol selectivity remains challenging. Herein, we report a Ce-containing Cu-based oxide precursor embedded in a carbon framework, which undergoes electrochemical pre-reconstruction to form CuO/Cu 2 O/Cu/CeO 2 @C heterostructure featuring active multi-heterointerfaces. By optimizing the Ce content, the reconstructed catalyst delivers a high ethanol Faradaic efficiency of 75.6% and an energy efficiency of 30.9% at −0.9 V versus the reversible hydrogen electrode in a flow-cell reactor, outperforming most reported Cu-based CO 2 RR electrocatalysts. Comprehensive structural characterizations reveal that the carbon confinement layer mitigates excessive reduction of Cu species and stabilizes the multivalent Cu interfacial environment during CO 2 RR, while CeO 2 modulates the local electronic structure and induces interfacial charge redistribution over Cu sites. In situ characterization combined with theoretical calculations further reveals that interfacial environment modifies the relative thermodynamics of *CO and *OCCO formation. This work provides profound insights into interfacial charge-redistribution-mediated ethanol selectivity and provides a design strategy for high-performance advanced Cu-based CO 2 RR electrocatalysts. Download: Download high-res image (80KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Feiyu Zhu,Yudong Ding,Xinglu Feng,Yujia Gan,Xun Zhu,Min Cheng,Qiang Liao
Hydrophobic DES integrates CO 2 cycloaddition and catalyst recycling. • Polarity evolution drives aqueous extraction of carbonate products. • Water extraction gives 93% recovery and > 97% yield over five cycles. • DFT reveals a water-tolerant decanol-assisted ring-opening pathway. • Catalyst-as-raffinate design enables reaction–separation integration. Homogeneous catalysts offer high activity for CO 2 fixation, yet their separation from polar carbonate products remains a persistent barrier to catalyst recycling. Here, we report an integrated catalysis–separation system based on a catalyst-as-raffinate strategy, exploiting the polarity increase inherent to the CO 2 cycloaddition of epoxides. A hydrophobic deep eutectic solvent composed of trioctylmethylammonium bromide and decanol was constructed as both the catalytic medium and the recyclable low-polarity raffinate phase. During the conversion of glycidol to glycerol carbonate, the reaction-induced polarity shift promotes product partitioning into water during extraction, while retaining the catalyst in the hydrophobic phase. Product extraction reached 93%, and the recovered catalyst maintained glycerol carbonate yields above 97% over five consecutive catalytic–extraction cycles. DFT and energy-decomposition analyses show that residual water is thermodynamically accommodated within the hydrogen-bonding catalytic network, whereas the decanol-assisted ring-opening pathway remains kinetically favored by avoiding excessive exchange repulsion in the rate-determining transition state. These features enable stable catalytic performance during aqueous recycling. Across different epoxides, extraction efficiency correlates with the product–DES polarity difference. This work establishes reaction-induced polarity evolution as a design principle for coupling homogeneous catalysis with product separation and catalyst recycling. Download: Download high-res image (101KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Jing Fan,Pengfei Jin,Guohua Wu,Fenhong Song,Long Ma
Twelve ternary DESs were prepared for efficient and regenerable CO 2 capture. • AA-PZ-EG (1:1:8) reached 0.18876 mol mol −1 at 303.15 K and 810 kPa. • CO 2 solubility was accurately correlated with a maximum AAD of 0.299%. • FTIR verified physical dissolution coupled with amine-assisted chemical capture. • DES2 retained >80% regeneration efficiency after three capture-release cycles. To address the greenhouse effect and climate change caused by excessive CO 2 emissions, the development of efficient, green, and regenerable CO 2 absorbents has become a major research focus in the fields of energy and environmental science. In this study, twelve ternary deep eutectic solvents (DESs) were synthesized from acetamide, piperazine, 1,4-diazabicyclo[2.2.2]octane (DABCO), ethylene glycol, and diethylene glycol via a one-step heating and stirring method. The density, viscosity, potential ecotoxicity of the constituent components, CO 2 absorption performance, and short-term cyclic performance were systematically investigated. With increasing temperature, the prepared DESs exhibited an approximately linear decrease in density, while their viscosity displayed a temperature-dependent reduction consistent with Arrhenius behavior. Ecological Structure-Activity Relationships (ECOSAR) screening suggested relatively low predicted aquatic toxicity for most of the individual components, whereas the ecotoxicity of the complete DES mixtures remains to be assessed experimentally. Among the twelve ternary DESs, DES2, which exhibits combined physical dissolution and reversible chemical interactions at the PZ sites, showed the best CO 2 absorption performances, with a CO 2 uptake of 0.1294 g CO 2 /g DES at 303.15 K and 810 kPa. The CO 2 solubility data were correlated using the Jou and Mather equation within the investigated temperature and pressure ranges, and the model showed good agreement with the experimental data. Moreover, DES2 (AA:PZ:EG = 1:1:8) retained over 80% of its initial CO 2 absorption capacity after three consecutive absorption–desorption cycles, indicating favorable short-term cyclic performance. Download: Download high-res image (162KB) Download: Download full-size image
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JOURNAL OF MEMBRANE SCIENCE
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2026
·
IF 8.8
Jincheng Peng,Lu Tang,Yihao Xiao,Xinxi Huang,Wanbin Li
MOFs are nested into intrinsic micropores of membranes by in situ confined growth. • Rigid MOF units interact with polymer chains and suppress polymer relaxation. • MOFs can reconstruct pore architectures and environments for improving selectivity. • Membranes exhibit enhanced aging resistance and separation performance. • After 180-d aging, CO 2 permeability and CO 2 /N 2 selectivity are 3240 Barrer and 47.3. Polymers of intrinsic microporosity (PIMs) with abundant interconnected pathways are promising for fabricating CO 2 capture membranes with exceptional permeability, but their applications are hindered by the issues of physical aging and insufficient selectivity. In this study, we report in situ confined growth of pore-nested metal-organic frameworks (MOFs) within the intrinsic micropores of PIM membranes as scaffolds to reconstruct their pore architectures for addressing the issues of aging and selectivity. Through a simple two-step immersion process for precursor immobilization followed by coordination, the pore-nested MOFs are constructed within the cavities and homogeneously distributed throughout the membranes. As rigid MOF units interact with polymer chains, suppress polymer segmental relaxation, reinforce polymer matrices, and regulate transport pathways, the rigidified membranes exhibit simultaneously enhanced aging resistance and separation performance, with selectivity markedly increasing from 14.6 to 40.3. After natural aging for 180 days, the membranes still retain a CO 2 permeability of 3240 Barrer, 92.3% of the initial value, alongside a CO 2 /N 2 selectivity of 47.3. This study offers a viable route to reshape transport channels via confined synthesis within micropores for designing high-performance and anti-aging separation membranes. Download: Download high-res image (387KB) Download: Download full-size image
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Wang Shichong,Wang Xinran,Wang Shuanjin,Xiao Min,Han Dongmei,Guo Hui,Huang Sheng,Meng Yuezhong
Photovoltaic
(PV) encapsulants play a pivotal role in ensuring
the long-term reliability of solar modules by protecting sensitive
cells from moisture ingress, mechanical stress, and ultraviolet (UV)
degradation. However, conventional encapsulant materials, such as
ethylene-vinyl acetate, polyolefin elastomer, and polyvinyl butyral,
exhibit several inherent limitations, including a high water vapor
transmission rate, poor delamination resistance, and easy formation
of optical haze under long-term UV irradiation in hygrothermal conditions.
To address these challenges, we herein design a CO 2 -derived
aliphatic polycarbonate-based thermoplastic polyurethane (TPU) as
a PV encapsulant, which combines high transmittance (>90.5%), flexibility,
superior water vapor barrier properties (WVP < 12.42 g·mm
m –2 day –1 ), moisture insensitivity,
and strong adhesion to PV glass and backsheet substrates. More specifically,
the multiblock TPU is synthesized via the polyaddition of poly(propylene
carbonate)diol, polyether diol, hexamethylene diisocyanate, and 1,4-butanediol.
Upon optimizing the chemical composition and incorporating proper
additives (e.g., silicone coupling agents, UV absorbers, antioxidants),
the encapsulant achieves enhanced interfacial adhesion with a peel
strength of 87.2 N cm –1 and maintains a residual
peel strength of 73.4 N cm –1 following accelerated
UV aging. Additionally, the adhesion mechanism based on TPU is proposed
and preliminarily elucidated. This study tackles key challenges in
photovoltaic module encapsulation by developing this high-performance
alternative material, demonstrating significant potential for large-scale
industrial applications.
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Science Advances
·
2026
·Vol. 12
·期 29
·
IF 13.9
Pan Zhu,Lixuan Ma,Xudong Yang,Xiao-Hong Yi,Jundong Wang,Chunlu Ding,Xin Li,Meng Lin,Wen Liu,Chong-Chen Wang,Huazhang Zhao,Zishuai Zhang
Conventional carbon dioxide (CO 2 ) capture systems are constrained by limited uptake capacity and energy-intensive regeneration. Here, we formulate a microporous carbon capture solution (MCCS) by dispersing a permanent-porosity framework (ZIF-67) in a liquid absorbent, coupling solvent-excluded physisorption with chemical uptake and boosting the CO 2 capture capacity by ∼45%. Instead of bulk thermal stripping, we implement interfacial, microbubble-activated regeneration (MAR) with a decreased monoethanolamine (MEA) loss rate by ∼38%. Microbubble activation refreshes gas-liquid-solid contact to liberate 100% physiosorbed CO 2 , whereas microbubble-collapse events that mechanically trigger contact electrocatalysis (CEC), enabling interfacial hydroxyl radicals (•OH) that cleave carbamates under mild conditions and regenerates a substantial additional 37 to 55% of chemically absorbed CO 2 . Theoretical analyses reveal that •OH is the key species governing CO 2 regeneration in the CEC-MAR process through oxidative carbon-nitrogen bond cleavage, followed by •H-assisted intermediate reduction to regenerate the amine. To approach engineering relevance, we realize kilogram-scale zeolitic imidazolate framework (ZIF) synthesis under ambient conditions using simple mechanical stirring, providing scalable MCCS inventory to enable (i) continuous delivery of high-purity CO 2 (1437 millimoles over 200 minutes) from a laboratory-scale integrated system and (ii) direct electroreduction to carbon monoxide (CO) with a faradaic efficiency (FE CO ) of 51% without CO 2 supply. More broadly, it establishes a porous-liquid, interfacial-regeneration paradigm that decouples capacity from stoichiometry and enables electrified, continuous CO 2 capture, regeneration, and utilization under scalable, low-temperature conditions.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jie Liu,Kaiyu Li,Shizhen Gao,Guohua Wu,Jing Fan
Efficient photocatalytic CO 2 reduction is limited by rapid carrier recombination and sluggish interfacial kinetics. Here, NiFe-LDH/ZnCdS (ZCS) heterostructures were fabricated by hydrothermal synthesis followed by electrostatic self-assembly. Mott–Schottky analysis, XPS, photoelectrochemical measurements, and density functional theory calculations collectively reveal staggered band alignment and interfacial charge redistribution, supporting a type-II charge-transfer pathway with improved carrier separation. The optimized 15NiFe-LDH/ZCS produced CO, CH 4 , C 2 H 4 , and C 2 H 6 at 16.54, 8.30, 1.22, and 4.70 μmol g −1 h −1 , respectively, while maintaining stable activity over 16 h. The enhancement originates from intimate interfacial contact, stronger visible-light harvesting, faster charge transport, and increased accessible active sites. These results establish a practical heterostructure-design strategy for multi-electron photocatalytic CO 2 conversion.
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产品关联
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Journal of Environmental Chemical Engineering
·
2026
·
IF 7.5
Hui Liu,Chao Yuan,Jianfeng Wang,Tongsheng Zhang,Binjie Zhou,Penghao Xin,Suping Cui
Carbon capture with chemical absorption method represents a critical pathway toward carbon neutrality in industry. However, its application faces challenges including high capture energy requirement for CO 2 desorption and limited CO 2 utilization routes. This study employed diethanolamine (DEA) as a CO 2 absorbent to prepare CO 2 –absorbed DEA (termed DEA–CO 2 ) with different CO 2 absorption amount. DEA–CO 2 was employed to modulate cement strength development, bypassing the energy-intensive CO 2 desorption step. Effects of DEA–CO 2 on cement hydration and the microstructure of the hardened cement pastes were investigated to reveal the regulation mechanism by in-situ carbonation. Results demonstrate that DEA-CO 2 additions show the potential to enhance 3d and 28d strength. Optimal performance occurs with 0.15% DEA and 0.22% CO 2 (D0.15%C0.22%), elevating 3d and 28d compressive strength by 15.3% and 29.3%, respectively. The enhancement is attributed to the accelerated hydration of aluminates and silicates by DEA–CO 2 to achieve a more condensed structure. Moreover, carbonation in cement pastes by DEA–CO 2 effectively mitigates the retardation effect of 0.15% DEA on early cement hydration. However, in the presence of DEA–CO 2 , the accelerated reaction of C 3 A with gypsum delays C 3 S hydration, especially for D0.15%C1.32%. It is hypothesized that the precipitated CaCO 3 or CaCO 3 –AFm on the surface of cement particles also inhibits further silicates hydration. Therefore, D0.15%C1.32% reduces the compressive strength before 28d. These results confirm the potential of utilizing DEA–CO 2 without desorption to optimize the strength development of cementitious materials, provided that the CO 2 dosage is carefully controlled.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Zhen Sun,Chenming Zhou,Teng Wang,Zhixin Gao,Jin Sun,Renquan Hu,Meng Yan,Zhaolin Na,Ran Su,Yong Yang
Photocatalytic CO2 reduction offers a green strategy to alleviate climate change and address the energy crisis. In this work, indium oxysulfide subnanocoils with a thickness of 0.9 nm were successfully synthesized via a facile solvothermal method. Adjusting the sulfur content not only modulates the band structure and energy level positions but also enables precise control over the morphology of the as-prepared products. The optimized indium oxysulfide subnanocoils exhibit excellent photocatalytic activity for CO2 reduction, with a CO evolution rate of 61.731 μmol h–1 g–1, which ranks among the best performances for indium-based materials reported to date. The enhancement of photocatalytic performance can be attributed to the exceptionally high surface atomic exposure ratio of the unique subnanometer coiled structure. Meanwhile, the sulfur substitution-induced S–O coordination significantly reduces the average valence state of indium, narrows the band gap, and improves the reduction capability of photogenerated electrons. This study provides a feasible approach for the development of high-performance subnanoscale photocatalysts for CO2 reduction.
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PubMed
高影响因子
ENERGY & FUELS
·
2026
·
IF 6
Yanshuang Xiong,Zhiwei Jian,Ian Jimmy Madatta,Yang Liu,Jinrui Ding
Electroreduction of carbon dioxide (CO2) to produce multicarbon products (C2+) holds immense potential for reducing carbon emissions and realizing high-valued CO2 utilization. However, the development of efficient catalysts still remains challenging. Cuprous oxide (Cu2O) has been identified as a promising candidate, yet its C2+ selectivity and stability require further improvement. In this study, we, for the first time, blended Cu2O with cerium oxide (CeOx) nanoparticles, forming a Cu2O/CeOx hybrid catalyst which greatly enhanced the selectivity and durability for C2+ production. The optimized catalyst achieved a remarkable carbon product Faradaic efficiency (FE) of 79.6% and a C2+ product FE of 58% (±2.4%) in an H-type electrolytic cell. Our findings provide a novel strategy for significantly improving the selectivity, efficiency, and catalyst stability of CO2 electroreduction.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Shuangshuang Yang,Zhicun Chu,Bo Gao,Xiaoli Zheng,Ichiro Imae,Jun Chen,Qun Xu
We report herein the typical conductive polymer poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) to be successfully modified onto single-walled carbon nanotubes (SWCNTs) using a supercritical carbon dioxide (SC CO2) antisolvent-induced polymer epitaxy method, and the role of the experimental temperature of SC CO2 on the modification process was systematically investigated. PEDOT:PSS/SWCNTs composites with optimal modification prepared at 80 °C and 15 MPa were used as functional fillers, and functional temperature-sensitive composite hydrogels of PEDOT:PSS/SWCNTs/poly-N-isopropylacrylamide (PNIPAM) were successfully prepared. With the help of Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction, transmission electron microscopy (TEM), scanning electron microscopy (SEM), and other characterization means, the chemical composition and microscopic morphology of the composite hydrogel were systematically analyzed. The composite hydrogel exhibits reversible temperature-sensitive responsiveness, transitioning from a transparent swollen state at room temperature to an opaque collapsed state at 32 °C, and demonstrates strong adhesion to various substrates, including glass, plastic, metal, and skin. Meanwhile, the near-infrared (NIR) photothermal conversion properties of this hydrogel were evaluated, showing a significant and uniform temperature increase upon NIR irradiation. The drug release behavior was assessed in vitro after loading the hydrophilic anticancer drug 5-fluorouracil (5-FU) with the stimulation of NIR light, achieving an accelerated and on-demand release. Our experimental results indicate that the pore size increases with the increase of the addition of PEDOT:PSS/SWCNTs, enabling the precise controlled release of 5-FU. This work provides new insights and experimental support for the design of intelligent drug delivery systems.
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