CHEMICAL ENGINEERING SCIENCE
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2025
·
IF 4.3
Min Zhou,Ningbo Yu,Qiang Sun,Hongxia Gao,Jinhang Fan,Zhiwu Liang
This study systematically investigates how steric architecture governs CO 2 absorption kinetics by analyzing six sterically modulated amines in aqueous and ethanol solutions. The stopped-flow apparatus was employed to determine pseudo-first-order kinetic constants (k 0 ) for CO 2 absorption by six sterically hindered amines with varying spatial configurations in aqueous and ethanol solutions within 293.15–308.15 K. The kinetic model based on the zwitterion mechanism outperforms the base-catalyzed hydration mechanism in predictive accuracy, with average absolute relative deviations (AARD) of 1.45–3.31 % in aqueous solutions and 2.28–2.58 % in ethanol solutions. Density functional theory (DFT) calculations reveal that increased molecular steric hindrance diminishes the nucleophilicity of amine-N atoms; the strengthened interactions of –OH groups concurrently facilitate the formation of intramolecular hydrogen bonding, which collectively amplify steric hindrance and thereby diminish reaction kinetics. In addition, ethanol’s strong solvation effects further diminish amine reactivity toward CO 2 , resulting in significantly lower absorption rates in ethanol-based systems compared to aqueous environments. These findings elucidate the complex interplay between steric hindrance, solvent dependence and CO 2 absorption kinetics, providing theoretical guidelines for optimizing design of CO 2 absorbent.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Mazhar Khan,Zeeshan Akmal,Muhammad Tayyab,Seemal Mansoor,Muhammad Adnan Zeb,Amir Zeeshan,Muhammad Mubashir Khan,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
The synergistic integration of redox reactions in the photocatalyst poses a significant challenge for CO 2 photoreduction. Addressing this issue requires the design of spatially proximate redox sites while effectively suppressing charge recombination at these sites. This work offers a pioneering tactic that exploits synergistic redox reactions in close atomic proximity. The deliberate incorporation of palladium and indium into TiO 2 , where the Pd site assists in hole accumulation, accelerates water dissociation, and generates highly active H* species. Meanwhile, adjacent In sites capture photogenerated electrons from TiO 2 , producing reactive intermediates by activating CO 2 . The synergistic incorporation of Pd and In accelerates redox functionality, boosts charge carrier separation, and mitigates recombination at closely situated redox sites. Comprehensive characterizations, including in-situ XPS and FTIR, strengthen these innovative outcomes. The optimized Pd 0.5 -In 1 /TiO 2 photocatalyst achieves nearly 100 % selectivity of CH 4 with a production rate of 30.5 µmol g -1 h −1 without the use of any sacrificial reagent, demonstrating a 25-fold improvement compared to pristine TiO 2 . In-situ infrared spectroscopy further validates that the synergistic doping of metal ions promotes the formation of *CH 3 O and *CHO, key intermediates in the production of CH 4 . This investigation provides valuable insight into the intricate design of coupled redox active sites.
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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
·
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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Chem Catalysis
·
2025
·
IF 11.6
Xiaoxiong Huang,Linping Qian,Yujin Ji,Wenzhe Niu,Yuncheng Hu,Liangyao Xue,Jingjing Li,Shuanglong Huang,Jiaqi Zhang,Youyong Li,Bo Zhang
The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) in pure water is one of the most promising strategies for avoiding crystallization in conventional electrolytes. Here, we sought to modify the catalyst of dispersed single-atom nickel (Ni) sites on an ultrathin nitrogen-doped carbon nanosheet (Ni–N–C) by using amino groups (Ni–N–C–NH 2 ). The obtained Ni–N–C–NH 2 catalysts exhibited a peak turnover frequency of 11.1 s −1 with >90% CO selectivity and ultrastable durability of 100 h of continuous operation and achieved two to three times greater current density than Ni–N–C. Operando spectroscopic evidence combined with theory studies suggested that the improved CO selectivity originates from the synergistic effect of the amino groups and Ni–N–C. The introduced amino groups with the surface property of the electron donor upshift the d -band center of Ni and favor CO 2 capture and proton-coupled electron transfer, ultimately enabling highly efficient operation of the CO 2 RR on Ni–N–C catalysts.
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Frontiers of Environmental Science & Engineering
·
2025
·Vol. 19
·期 8
·1-14
·
IF 6.4
Yang Zhouzhou,Zheng Xudong,Ji Biao,Xu Zihuai,Bao Sifan,Sun Wei,Mei Jinfeng,Rong Jian,Li Zhongyu
Utilization of carbon-based materials is crucial for mitigating CO 2 emissions. However, practical materials for CO 2 capture remain challenging due to limitations in adsorption capacity and rate. Inspired by the unique structural features of biomass materials, high-performance hierarchical porous carbon was prepared using vascular plants. The ordered arrangement structure effectively improved the adsorption capacity and rate of the material by optimizing the pore structure. Potassium hydroxide (KOH) was used as an activator to synthesize microporous carbon with an ordered hierarchical structure. The properties of hierarchical porous carbon were characterized. The experimental results indicate that porous carbon prepared from loofah complex has excellent CO 2 adsorption capacity. The highest adsorption capacity is 4.09 mmol/g when the activation temperature is 700 °C. The selectivity (15/85) for the binary gas mixture CO 2 /N 2 was 20, and the recoverability was good after 10 cycles. The hierarchical porous carbon derived from loofah showed excellent adsorption performance and has potential in various applications.
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Mineral Processing and Extractive Metallurgy Review
·
2016
·
IF 1.56
Zijian Su,Yuanbo Zhang,Bingbing Liu,Jun Chen,Guanghui Li,Tao Jiang
Calcite (CaCO3), one of the main impurities, has an uncertain effect on the volatilization behavior of tin oxide in the tin-bearing iron ore concentrates during the selective reduction volatilization process. In this study, natural calcite powders were added into the tin-bearing iron ore concentrates to investigate tin volatilization behavior affected by CaCO3 under different roasting temperature, CO content, and roasting time. In addition, the effect of CaCO3 on the phase transformation of SnO2 was determined using XRD, SEM-EDS combined with thermodynamics calculation. The results indicated that CaCO3 had a significantly adverse effect on the Sn volatilization ratio, because Ca2SnO4 was easily formed under CO-CO2 atmosphere. It was also found from the study that the generation of SnO(s) was the most critical intermediate for promoting the formation of Ca2SnO4.
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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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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2024
·
IF 3.7
Xiaofei Xu,Xiaolong Li,Zhi Li,Da Zhang
An experimental study of single carbon dioxide (CO 2 ) bubbles ascending in aqueous solutions of carboxymethyl cellulose (CMC) is performed as a means to obtain further understanding of the rising behavior and mass transfer of soluble bubbles in shear-thinning non-Newtonian fluids. High-speed photography and digital image processing technique are employed to quantify the characteristic parameters of the bubble rising process. The rising behavior of single CO 2 bubbles in a Newtonian fluid (tap water) is measured as a reference. It has been found that the rheology of the liquid phase significantly influenced the rising behavior of the bubbles. In CMC aqueous solutions, CO 2 bubbles mostly followed a straight rising path characterized by increasing aspect ratio and decreasing vertical velocity. Increase in initial bubble size led to bubble deformation in less concentrated CMC aqueous solutions which resulted in an irregular rising path. The evolution of bubble equivalent diameter can be mainly divided into two stages: a fast reduction stage followed by a slow one. Meanwhile, the variation of liquid-side mass transfer coefficient k L of CO 2 bubbles in tap water and CMC aqueous solution with different weight percentages is discussed. The mobility of gas-liquid interface is considered to have significant impact on gas-liquid mass transfer. A dimensionless correlation considering the rheology of the liquid phase is proposed to describe the evolution of the motion and deformation of single soluble CO 2 bubbles in infinite stagnant shear-thinning non-Newtonian liquids.
研究领域:
流体力学
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化学工程
·
多相流
·
传质过程
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非牛顿流体动力学
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气泡动力学
·
环境工程
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危险品化学品经营许可证（带存储）