AICHE JOURNAL
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2026
·
IF 4
Ningbo Yu,Shaofei Wang,Min Zhou,Min Xiao,Bo Jin,Hongxia Gao,Zhiwu Liang
Amine-based water-lean solvents serve as energy-efficient absorbents for carbon dioxide (CO 2 ) capture but face paradoxical kinetic challenges, where the mixed solvents inconsistently accelerate or decelerate reaction rates across amine classes. By integrating stopped-flow kinetics, molecular dynamics simulations, and electrostatic potential analysis, we elucidate water modulates CO 2 absorption in mixed absorbents systems via amine-specific solvent encapsulation effect for the first time. For primary amines (e.g., monoethanolamine, MEA), water preferentially hydrates nucleophilic nitrogen atoms, forming steric barriers that impede CO 2 access and suppress kinetics with increasing hydration. Conversely, secondary amines (e.g., methylaminoethanol, MAE) exhibit oxygen-directed hydration, which weakens nitrogen solvation and enhances electrostatic CO 2 -amine interactions, accelerating kinetics. A zwitterion-based kinetic model quantifies these solvent-induced activation energy shifts, revealing a universal mechanism validated across diverse solvent systems. This work establishes molecular design principles for tailoring water-lean absorbents, bridging the critical gap between solvent engineering and reaction pathways to advance energy-efficient carbon capture technologies.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Yongjun Mao,Yudian Zhu,Xudong Wang,Jianming Liu,An-Ping Zeng
The synthesis of amino acids from CO2 as the sole carbon source is a critical goal for sustainable biomanufacturing, offering a green alternative to conventional production methods plagued by greenhouse gas emissions and resource competition. Here, we construct a highly efficient cell-free enzymatic platform for the direct biosynthesis of aspartate from CO2. Our integrated platform couples a carbon-fixing module using the modified reductive glycine pathway (rGlyP) with a custom-designed synthesis cascade that condenses two glycine molecules into aspartate, driven by glycine oxidase and a redesigned b-hydroxyaspartate cycle (BHAC). A key challenge in this multienzyme system is achieving pathway synergy. To address this, we employed an enzyme-constrained static model to rationally design the optimal stoichiometry of the five-enzyme cascade. This computational approach not only boosted the final aspartate yield by over 25% but was also essential in identifying glycine oxidase (Bs-ThiO) as the primary rate-limiting bottleneck. Through systematic optimization of enzymes, reaction conditions, and feeding strategies, the system finally achieved accumulation of 17.3 mM aspartate (2.3 g/L) within 2 h, reaching an exceptional 92% of the model-predicted theoretical yield. This study establishes a powerful and sustainable platform for green amino acid production and showcases the significant potential of combining computational design with cell-free engineering to advance the frontier of CO2-based biomanufacturing.
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ACS Catalysis
·
2026
·
IF 13.6
Xianglong Meng,Yanjiao Wang,Ruiping Deng,Soryong Chae,Chunzheng Wang,Girolamo Giordano,Zifeng Yan,Hailing Guo,Svetlana Mintova
A strategy for synthesizing bimetallic catalysts confined within zeolite frameworks, offering a promising approach for stabilizing metal species under harsh reaction conditions, is disclosed. A dual-stage synthesis strategy including alkali etching to open the channels of Silicalite-1 (S-1) zeolite, exposing internal hydroxyl defects that serve as anchoring sites for Cu and Zn species, is presented. This was followed by a dry-gel conversion encapsulation step to yield Cu-ZnO@S-1 catalyst. The competitive occupation of these sites by Cu and Zn facilitates the formation of high-density Cu-ZnO interfaces. Under reaction conditions of 3 MPa and 250 °C, the catalyst achieves a methanol selectivity above 99.2% and a space-time yield (STY) of 2.1 g gCu–1 h–1, nearly four times higher than that of copper-containing catalyst (Cu@S-1, 0.54 g gCu–1 h–1) and significantly outperforming the sample prepared by conventional impregnation (Cu-ZnO/S-1, 1.6 g gCu–1 h–1). The oxygen-deficient Cu-ZnO1–x sites at the Cu-ZnO interface are further demonstrated to serve as genuine active centers for methanol synthesis. The methanol formation reaction proceeds via the formate pathway, and the high density of Cu-ZnO1–x sites effectively lowers the activation barrier for the hydrogenation of *HCOO to *H2COO.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Ning Zhang,Chuanlong Jin,Shangping Wang,Junjiang Bao,Xiaopeng Zhang,Gaohong He
Abatract A polymer of intrinsic microporosity (PIM) membrane that commonly remains both highly permeable and mechanically robust under aggressive CO 2 feeds is still an unmet challenge. Here this work proposes a novel crosslinking strategy with dual-function compensation that simultaneously preserves free volume and enhances CO 2 dissolution for microporous membrane preparation. Amino-functionalized ZIF-8 (ZIF-8-NH 2 ) nanoparticles are dispersed in bromomethylated PIM (PIM-BM) and subsequently thermally crosslinked via Hofmann alkylation. The incorporated ZIF-8-NH 2 therefore acts simultaneously as covalent crosslinking nodes that restrict chain mobility and suppress physical aging/plasticization, and permanent CO 2 -philic pores (0.34 nm) that compensate the free volume loss upon crosslinking network formation. The optimal c-PIM/ZIF-9 wt% membrane exhibits an exceptional CO 2 permeability 6803.53 Barrer as well as CO 2 /N 2 selectivity of 29 with equimolar mixed gas. Meanwhile, the membrane also demonstrates remarkable resistance to both physical aging and plasticization. This work presents a novel strategy that offers a promising avenue for developing high-performance microporous membranes for particle carbon capture.
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ChemCatChem
·
2026
·Vol. 18
·期 2
·e01743
·
IF 3.9
Yunjie Xie,Bowen Xu,Yi Liu,Feng Zeng,Chalachew Mebrahtu
Herein, we present a concept for CO 2 -assisted direct aqueous-phase hydrogenation of sodium acetate to ethanol, offering a salt-tolerant approach that circumvents energy-intensive acidification and simplifies biomass valorization. The reaction was performed over highly dispersed Pt on the CoAlPt (CAP) catalyst, which improves H 2 activation and drives hydrogen spillover, thereby increasing the reactive surface hydrogen species while mitigating excessively strong H adsorption that suppresses activity under alkaline conditions. The CAP catalyst achieved 90.88% ethanol selectivity with a productivity of 3.63 mmol·g −1 ·h −1 at 180°C without CO 2 addition. Introducing CO 2 (0.1 MPa) increased ethanol productivity to 4.92 mmol·g −1 ·h −1 by converting OH − to HCO 3 − and shifting acetate speciation toward molecular acetic acid, which is more readily hydrogenated. The results obtained in this concept study highlight the potential of using CO 2 as a promoter for direct acetate hydrogenation towards a sustainable strategy for converting acetate-rich aqueous streams to ethanol and other value-added products. Graphical CoAlPt (CAP) catalyst enables an efficient aqueous-phase hydrogenation of acetate to ethanol with 90.88% selectivity. Introducing a controlled amount of CO 2 led to a two-way synergistic promotion between acetate and CO 2 hydrogenation, where balanced OH − /HCO 3 − species further enhance ethanol and methane formation.
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CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 4.3
Wenwei Wu,Shuai Wang,Can Lv,Tejraj Aminabhavi,Ozge Yuksel Orhan,Helei Liu
In this study, a novel mixed amine biphasic absorbent composed of DETA, 1DMA2P, and H 2 O was constructed for CO 2 capture. Physical properties of the biphasic absorbent were calculated over the temperature range of 298.15 K to 313.15 K, while its CO 2 absorption kinetics were investigated in a stirred tank reactor. Based on different reaction mechanisms of the primary amine DETA and the tertiary amine 1DMA2P with CO 2 , the overall reaction rate constant (k ov ) and the second-order reaction rate constant (k 2 ) of the biphasic solvent were calculated. Using Arrhenius equation, the activation energies of DETA and 1DMA2P solutions in the biphasic absorbent were calculated to be 19.37 kJ/mol and 51.45 kJ/mol, respectively, both lower than those of pure solutions. 13 C NMR data and quantum chemical calculations indicate the generation of highly polar products with increasing CO 2 flow rate, prompting the phase transition in homogeneous solution. DETA and its products dissolved in aqueous phase form the CO 2 -rich phase. The less polar 1DMA2P interacted less strongly with DETA products and separated into upper layer of the solution due to its lower density than the DETA-related products.
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FUEL
·
2026
·
IF 7.5
Wenjing Wang,Mingnv Guo,Yulin Chen,Yuxuan Guo,Jiahao Liu,Ziqi Wang,Zhongqing Yang
A W 18 O 49 /Bi 2 MoO 6 heterojunction photocatalyst with favorable photothermocatalytic activity was constructed in this study. Its physicochemical properties were characterized and analyzed, and its photothermocatalytic performance was evaluated through catalytic activity tests conducted under full solar spectrum conditions. The results show that W 18 O 49 /Bi 2 MoO 6 exhibits superior photothermal catalytic activity compared to single Bi 2 MoO 6 and W 18 O 49 . Among them, the W 18 O 49 /Bi 2 MoO 6 heterojunction with a mass ratio of 7 % has the highest CO yield, reaching 140.03 µmol/g, which is 7.5 times higher than that of pure W 18 O 49 . The interaction between W 18 O 49 and Bi 2 MoO 6 endows W 18 O 49 /Bi 2 MoO 6 with good photogenerated carrier separation and migration efficiency, as well as photothermal catalytic activity. This provides ideas for designing photocatalysts with efficient photothermal catalytic CO 2 reduction.
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Nanoscale
·
2026
·
IF 5.1
Qi Chen,Yanming Li,Hui Shi,Wenbin Ma,Chunzhen Yang,Changli Li,Jingfu He
Multi-carbon (C2+ ) products from electrocatalytic CO2 reduction (CO2 RR) hold significant industrial value. Tandem Cu-based catalytic systems can markedly improve C2+ selectivity, but their performance is often limited by suboptimal spatial configurations. In this study, we fabricate layer-stacked Ag/CuO and array-patterned Ag/CuO catalysts with tunable array spacings (200, 400, and 800 μm) to decouple CO generation and consumption, thereby enabling precise regulation of * CO flux. The array-patterned Ag/CuO systems markedly outperform layer-stacked designs, indicating that lateral CO diffusion is more effective than longitudinal diffusion.Moreover, C 2+ selectivity strongly depends on array spacing, with the best performance achieved at 400 μm (Ag-CuO-400), reaching a Faradaic efficiency (FE) of 63% for ethylene at 300 mA/cm 2 in a neutral electrolyte. Through operando infrared microscopy, we visualize the * CO coverage distribution in real time, revealing an effective lateral CO diffusion length of approximately 200 μm. This corresponds to an optimal balance between * CO supply and C-C coupling activity on the Ag-CuO-400 catalyst. This work underscores the significance of anisotropic * CO transport and provides a design strategy for spatially structured tandem catalysts.
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高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Hao Wang,Jiabao Yang,Yipu Xu,Yucai Qin,Shutao Xu,Guanghui Zhang,Zhongmin Liu,Xinwen Guo
As environmental and energy issues become increasingly apparent, the tandem catalytic hydrogenation of CO2 for direct hydrocarbon production has attracted significant attention. However, zeolite deactivation caused by metal migration severely hampers its development. This work reveals that for the In2O3/ZSM-5 catalyst in CO2 hydrogenation, indium species preferentially migrate to the external surface of ZSM-5 and interact with hydroxyl groups (e.g., Brønsted acid sites (BAS) and SiOH) via solid-state ion exchange, which is related to the subsequent poisoning of BAS within micropores. Based on this insight, a surface engineering strategy was developed by grafting silane onto the external surface, which significantly enhanced the resistance to indium poisoning. After a 22-h reaction, the silane-modified catalyst (In2O3/ZSM-5-SiPr) retained nearly all of its strong acid sites and maintained a C2+ hydrocarbon selectivity of >92.0%. However, the unmodified catalyst suffered a 60% loss of the number of strong acid sites and yielded 0% C2+ selectivity. The derived 0.6Si/In2O3/ZSM-5-SiPr achieved a C2+ selectivity of >92.0% with a space-time yield (STY) of 3.66 mmol goxide–1 h–1, which is more than 2.6 times higher than that of the reported powder-mixed In2O3 tandem catalysts, and demonstrated stability for over 260 h under harsh conditions. This strategy is generally applicable to multiple zeolites with varying Si/Al ratios and topologies. This work provides a universal approach for designing stable and highly active tandem catalysts resistant to metal migration during CO2 hydrogenation.
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ACS Catalysis
·
2026
·
IF 13.1
Can Cheng,Yaolin Wang,Jia-nan Wang,Haomiao Xu,Wenjun Huang,Zhisong Liu,Wei Li,Yuyang Li,Zan Qu,Xin Tu,Naiqiang Yan
Plasma-catalytic CO2 hydrogenation to CO offers a promising route for carbon-neutral chemical synthesis. However, its advancement is constrained by low energy efficiency and limited mechanistic insight. Here, we developed an oxygen vacancy-engineered Pd-WO3–x catalyst supported on nickel foam (NF), which exhibits enhanced performance in ambient plasma-driven CO2 conversion. The system leverages the conductive properties of NF to spatially divide the discharge zone into streamer and filamentary discharge zones, thereby enhancing plasma activation and interfacial charge transfer. Catalyst characterization reveals that Pd plays a critical role in stabilizing metastable oxygen vacancies (OVs) within WO3–x, which function as electron reservoirs to promote CO2 dissociation into CO. Density functional theory calculations and in situ spectroscopic studies confirm that Pd facilitates H2 dissociation, while vibrationally excited CO2 generated in the plasma gas phase preferentially adsorbs at OV sites. At a specific energy input of 33.6 kJ L–1, the system demonstrates superior performance, achieving 54.9% CO2 conversion with 99.8% selectivity toward CO, surpassing typical plasma-catalytic benchmarks. The catalyst exhibited good stability over 100 h of continuous operation, with a slight decrease in CO2 conversion (<10%) and nearly unchanged CO selectivity (>99%) due to strong metal–support interactions and the conductive nature of NF. This work demonstrates that OV engineering provides a promising strategy for designing efficient plasma-catalytic systems for CO2 conversion.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2017
·
IF 2.726
Qiaoyan Shang,Shuqian Xia,GuanWei Cui,Bo Tang,Peisheng Ma
Carbon dioxide enhanced oil recovery (CO 2 EOR) process is widely used in petroleum industry in recent years. But it has some shortcomings, such as early gas breakthrough, fingering, asphaltene precipitations, because of the low viscosity and density of CO 2 . These problems can be resolved by adding some common solvents as chemical modifiers in CO 2 flooding. In this work, ethanol was chosen as the chemical modifier. The effects of ethanol on the equilibrium interfacial tension (IFT) of paraffin + CO 2 systems were investigated with different ethanol contents, temperature range 60–100 °C and pressure range 5.06–14.60 MPa, respectively. New correlation for predicting the IFTs of paraffin + modified CO 2 systems were proposed based on 150 experimental IFT values. The square of correlation coefficient ( R 2 ), root mean square error ( RMSE ) and average absolute relative deviations ( AARD ) were 0.9948, 0.15 and 2.49%, respectively. The paraffin IFTs for modified CO 2 and pure CO 2 flooding were compared by the IFT average absolute decrease ratio ( AADR ).
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International Journal of Electrochemical Science
·
2023
·Vol. 13
·期 4
·3613-3624
·
IF 1.5
Yong Xiang,Chen Li,Zhengwei Long,Canwen Zhang,Zhongli Ji
Although steel corrosion in a SO 2 -containing atmospheric environment has been extensively investigated, its electrochemical behavior still needs to be addressed, especially when it coexists with CO 2 in a carbon capture, utilization and storage system. In this work, electrochemical experiments with 316L stainless steel corrosion in a CO 2 -saturated solution were conducted by adding different amounts of SO 2 to a solution at 25 °C under different pH conditions. The effect of SO 2 on the cathodic reactions of 316L stainless steel corrosion in a CO 2 -saturated solution was investigated by electrochemical methods, including potentiodynamic sweep, linear polarization resistance and electrochemical impedance spectroscopy. The results showed that the presence of SO 2 increased the cathodic limiting current and corrosion rates of 316L stainless steel at the same pH. There was a “second-wave” phenomenon that appeared before the second limiting current and this new “wave” was demonstrated to be related to the direct reduction of both hydrate of SO 2 and bisulfite on the steel surface.
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