Molecular Catalysis
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2025
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IF 4.9
Meilin Yin,Jingchen Li,Simai Peng,Daying Chen
The industrial implementation of CO 2 cycloaddition remains hindered by catalysts that require multi-step syntheses, co-catalysts or solvents, and yet offer limited recyclability and scalability. Here, we present a metal-free heterogeneous composite catalyst (PImBr@COF) prepared by a 6 h one-pot ship-in-bottle polymerization of imidazolium ionic liquids within the ordered nanochannels of an imine-linked triazine COF (HO-TAPT-COF). This strategy simultaneously embeds Br – nucleophiles, hydrogen-bond donors (-OH) and CO 2 -philic moieties (imine, triazine groups and imidazolium cations) into a crystalline porous scaffold, creating a cooperative activation environment for epoxide ring-opening and CO 2 coupling. The resulting catalyst achieves a CO 2 /N 2 selectivity boost from 14.2 to 24.7, maintains a CO 2 uptake of 50.6 mg g −1 , and delivers a 99.0 % yield of cyclochloroallyl carbonate under solvent- and cocatalyst-free conditions. Remarkably, both CO 2 capture and catalytic activity show negligible decay after ten cycles. Density functional theory calculations reveal that the confined ionic environment significantly lowers the energy barrier for epoxide activation. This work establishes a rapid, scalable and broadly applicable route for constructing multifunctional COF-based catalysts for sustainable CO 2 utilization.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jiangtao Peng,Xuanrong Wang,Ming Wen,Shengjie Jiu,Xia An,Xu Wu
The clay mineral-based composite was explored for adsorption of CO 2 , which was fabricated by impregnating monoethanolamine (MEA) on montmorillonite (Mont). The hydroxyl groups of Mont removed, and was found to be only physical loaded-amines after thermal treatment (T-Mont). The MEA molecules were well combined with the -OH surface of Mont, which enhanced stability and cyclability for CO 2 adsorption. The composite 40-MEA@Mont displayed excellent adsorption performance, and adsorption capacity reached 8.72 cm 3 ∙g −1 at room temperature. After eight cycles of CO 2 adsorption, the capacity of 40-MEA@Mont showed no noticeable changes compared to the first cycle, whereas 40-MEA@T-Mont was 15.19 % decline. The reason lies in the hydrogen bond interaction between amine and Mont matrix which was further confirmed by DFT calculation. Isosteric heat of adsorption analysis and in situ FT-IR manifested that CO 2 adsorption predominantly involved weak chemisorption on the composite 40-MEA@Mont. The CO 2 adsorption mechanisms of clay-based support can be controlled by adjusting the type of impregnated amines, and the layered montmorillonite loaded with amines can be a promising material for CO 2 adsorption at room temperature.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10493
·
IF 15.7
Zhang Zhiyong,Huang Qing,Xie Yangen,Zhang Boyang,Zhao Qi,Huang Xingmiao,Yang Na,Ji Hongwei,Chen Chuncheng,Sheng Hua,Zhao Jincai
Current CO 2 utilization depends on high-purity CO 2 , necessitating energy-intensive capture and purification from air. Herein, we present a practical system that selectively converts atmospheric CO 2 with ammonia into urea using solar energy as the sole input. This system is enabled by a heterostructure composed of an indium–porphyrin metal–organic framework and UiO-66-NH 2 , which harness ambient O 2 to promote rather than suppress CO 2 reduction. As a result, it achieves a CO production rate of 272.1 μmol·g −1 ·h −1 directly from air, which is competitive compared to the systems that rely on high-purity CO 2 . Moreover, coupling atmospheric CO 2 reduction with ammonia oxidation enables direct air-to-urea conversion with high selectivity. A scaled-up prototype operating under natural sunlight and open-air conditions achieves a urea production rate of 32.4 μmol·g −1 ·h −1 . This work integrates atmospheric CO 2 capture, solar-driven conversion, and product collection within a single, scalable platform, offering a practical route for carbon utilization under real-world conditions.
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LANGMUIR
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2025
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IF 3.9
Weiqiao Zhong,Zhichao Xia,Tingxi Zhang,Yuhuan Nie,Rong Lei,Lu Li,Qibin Chen
Switchable surfactants are an emerging class of environmentally friendly compounds that can be reversibly triggered between active and inactive states in response to external stimuli, enabling on-demand or on-command control over the interfacial properties. In this work, a type of imidazoline-based CO2-switchable surfactants was synthesized and systematically investigated. Structural characterization was performed by using Fourier transform infrared and 1H NMR spectroscopy, confirming the successful formation of long-chain alkyl imidazolines. Their surface activity and critical micelle concentration (CMC) were evaluated by measuring surface tension and interfacial tension, revealing strong adsorption behavior and efficient micellization. Conductivity and NMR analyses demonstrated the reversible transition between neutral and ionic forms under alternating CO2/N2 bubbling, confirming the robustness and repeatability of the switching process. The emulsification/demulsification cycles were repeated over multiple switching operations, where oil/water emulsions were stabilized by their bicarbonate salt forms with long-term stability, whereas the neutral forms induced rapid demulsification. These findings not only establish the fundamental interfacial behavior of imidazoline-based surfactants but also highlight their potential applications in enhanced oil recovery, chemical separation, drug delivery, and sustainable process design.
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Journal of Cleaner Production
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2025
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IF 10
Jubao Gao,Jinyu Bai,Lu Jia,Xueyi Song,Shujuan Wang,Yongqiang Ren,Shisen Xu
Global climate catastrophes driven by the greenhouse effect and rising CO 2 emissions highlight the urgent need for improved carbon-capture technologies. Deep eutectic solvents (DESs) have emerged as promising alternatives to ionic liquids and aqueous amines, but few studies assess the energy consumption of CO 2 capture with ternary DESs. The present study synthesized novel ternary DESs using cyclic amines as promoters, which were selected on the basis of their stability, slower consumption, and easier bond cleavage. The CO 2 capture performance of the resulting DESs was then investigated using spectroscopy and molecular dynamics simulations. The DES [ChCl][MEA]-5 %PZ exhibited the highest absorption capacity (0.290 g CO 2 /g), representing a 146 % increase over 30 wt % MEA, and an estimated regeneration efficiency of 88 %. Simulations showed that secondary amines strengthen intermolecular interactions and promote CO 2 uptake, consistent with experimental results. The results of both nuclear magnetic resonance and Fourier-transform infrared spectroscopy analyses indicate that CO 2 reacts with cyclic secondary amines to form carbamates, which enhance capture capacity. The heat of reaction was identified as the main contributor to regeneration energy. It is noteworthy that the regeneration energy for [ChCl][MEA]-5 %IM was 1.79 GJ/t CO 2 , which is approximately 60 % of that for 30 wt % MEA and is comparable to biphasic absorbents. In conclusion, these ternary DESs demonstrate considerable potential for energy-efficient CO 2 capture.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Li Jieyang,Zhang Huanlei,Luo Changhao,Cheng Dongbo,Xu Wanping,Lin Meng
Electrochemical conversion of CO 2 into fuels represents an important pathway for addressing the challenges of climate change and energy storage. However, large-scale applications remain hindered by the instability and inefficiency of CO 2 reduction systems, particularly under highly alkaline electrolytes and high current densities. One primary obstacle is the cathodic salt precipitation, which hinders mass transfer and blocks active sites limiting the lifespan of these systems. Here, we present a non-isothermal strategy that leverages a thermal gradient across the membrane electrode assembly to enhance electrochemical performance and suppress salt precipitation. By maintaining a cooler cathode and warmer anode, we exploit the Soret effect to drive cations away from the cathode, mitigating salting-out while boosting anodic activity and cathodic CO 2 solubility. The non-isothermal case has demonstrated over 200 h of stable operation at 100 mA cm −2 under highly alkaline conditions, outperforming conventional isothermal systems. Techno-economic analysis reveals reductions in CO 2 -to-CO production costs, supporting the scalability of this strategy. These findings enable the practical deployment of stable, high-efficiency CO 2 electrolysis systems.
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Carbon Capture Science & Technology
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2025
·
IF 10.5
Tingwei Wang,Xuelong Quan,Zhiqiang Sun,Zhao Sun
Excessive CO 2 emissions lead to a gradual increase in global average temperatures and an increased frequency of extreme weather events. Exploiting advanced materials for CO 2 capture has become a key issue of concern to all countries. In this study, a new biomass carbonization strategy, co-modification by H 2 O 2 and KOH, is proposed to prepare microporous biochar from pine sawdust with high CO 2 adsorption capacity. Results indicate that the co-modification strategy can produce biochar with a specific surface area as high as 3522.7 m 2 /g (with a micropore ratio of 90.3%), which increases by 56.7% compared to the biochar produced by biomass carbonization without H 2 O 2 treatment. The adsorption properties of the co-modification-derived biochar are investigated by CO 2 -TPD and TG, and the biochar exhibits a maximum CO 2 adsorption capacity of 6.60 mmol/g at 30°C and retains over 91.2% of this capacity after 10 cycles. It is revealed that H 2 O 2 -KOH modification can significantly promote the physisorption capacity of the biochar, highlighting the enhanced CO 2 capture efficiency due to alkaline hydrogen peroxide treatment on the biochar and its enhancement in CO 2 capture.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ya-Nan Jing,Xing-Liang Yin,Lei-Lei Li,Yan-Lan Wang,Jia Xue,Ze-Feng Xu,Da-Qiang Liu,Chuan-Wu Chen,Xiao-Jie Liu,Er-Kang Liu
CO 2 -to-high value-added chemicals via a photocatalytic route is of interest but strangled by the low efficiency. Herein, a novel Fe-TiO 2-x /TiO 2 S-scheme homojunction was designed and constructed by using a facile surface modification approach whereby oxygen vacancy (OV) and Fe introducing on the TiO 2 nanorod surface. The as-synthesized Fe-TiO 2-x /TiO 2 S-scheme homojunction exhibits positive properties on promoting photocatalytic CO 2 reduction: i) the nanorod structure provides numerous active sites and a radical charge transfer path; ii) the doped Fe and OV not only synergistically enhance light utilization but also promote CO 2 adsorption; iii) the Fe-TiO 2-x /TiO 2 S-scheme homojunction benefits photoexcited charge separation and retains stronger redox capacity. Thanks to those good characters, the Fe-TiO 2-x /TiO 2 homojunction exhibits superior CO 2 reduction performances with optimized CO/CH 4 generation rates of 122/22 μmol g -1 h −1 which exceed those of pure TiO 2 by more than 9.4/7.3 folds and most currently reported catalytic systems. This manuscript develops a facile and universal approach to synthesize well-defined homojunction and may inspire the construction of other more high-efficiency photocatalysts toward CO 2 reduction and beyond.
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Journal of Cleaner Production
·
2024
·
IF 9.7
Menglei Mao,Ruqing Chong,Feixue Sun,Rui Gao,Zihui Meng,Xinlong Fan,Wenfang Liu
Enzymatic conversion of CO 2 to formate is a highly significant pathway for CO 2 utilization, but current level of conversion efficiency remains unsatisfactory due to low solubility of CO 2 under mild conditions. CO 2 -philic materials can significantly augment the reaction by raising local concentration of substrate. Herein, the intercalated Ti 3 C 2 T x , nano-silica (SiO 2 ) and carbon nitride (CN) with abundant CO 2 adsorption sites were introduced to fabricate Ti 3 C 2 T x based nanocomposites, Ti 3 C 2 T x /SiO 2 /CN (TSCN), for the first time. As the controls, binary composites including Ti 3 C 2 T x /SiO 2 (TS), Ti 3 C 2 T x /CN (TCN) and SiO 2 /CN (SCN) were also studied. For each kind of material, the composition, structure, morphology, and application performance in the enzymatic CO 2 conversion were characterized and influencing factors were investigated. Among these composites, TSCN exhibited the best application performance and the enzyme reaction was accelerated up to 23.9 times that of the blank system. The value could reach as high as 35.3 after polyethyleneimine (PEI) modification. Following that, PEI modified composites were used as carrier of formate dehydrogenase (FDH) and apparent specific activity was up to 2.8 times that of free enzyme, which could retain 88.2% of the initial value after 10 cycles associated with the structural integrity. This work provides new impetus to CO 2 capture and conversion in a clean and mild way that shows bright application prospects.
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RSC Advances
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2025
·Vol. 15
·期 3
·1658-1664
·
IF 4.6
Xiuping Li,Jiaqi Wang,Bolin Yin,Kaihong Liu,Jingjing Zhao,Bo Jiang,Hexing Li
The hydrogenation of carbon dioxide into profitable chemicals is a viable path toward achieving the objective of carbon neutrality. However, the typical approach for hydrogenation of CO2 heavily relies on thermally driven catalysis at high temperatures, which is not aligned with the goals of carbon neutrality. Thus, there is a critical need to explore new catalytic methods for the high-efficiency conversion of CO2. Herein, we present a new class of catalysts, featuring phosphorus-doped amorphous ruthenium nanoparticles supported on copper nanoparticles, which capitalizes on the plasmonic effects of copper to achieve the photothermal transformation of CO2 to CO within a gas–solid flow system. Our findings indicated that the reaction efficiency in the presence of photothermal energy was over eight times greater than that with thermal energy alone. The catalyst system exhibited nearly 100% selectivity towards CO under mild conditions, with an impressive CO yield of 123.16 mmol g−1 h−1. This study highlights the significant potential of amorphous metal phosphides in photocatalytic CO2 hydrogenation under mild conditions and offers a fresh avenue for the robust catalysis of amorphous materials.
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Green Energy & Environment
·
2022
·
IF 12.781
Zhengshan Yang,Bowen Deng,Kaifa Du,Huayi Yin,Dihua Wang
Molten carbonate is an excellent electrolyte for the electrochemical reduction of CO 2 to carbonaceous materials. However, the electrolyte–electrode-reaction relationship has not been well understood. Herein, we propose a general descriptor, the CO 2 activity, to reveal the electrolyte–electrode-reaction relationship by thermodynamic calculations and experimental studies. Experimental studies agree well with theoretical predictions that both cations (Li + , Ca 2+ , Sr 2+ and Ba 2+ ) and anions (BO 2 − , Ti 5 O 14 8 − , Si O 3 2 − ) can modulate the CO 2 activity to control both cathode and anode reactions in a typical molten carbonate electrolyzer in terms of tuning reaction products and overpotentials. In this regard, the reduction of C O 3 2 − can be interpreted as the direct reduction of CO 2 generated from the dissociated C O 3 2 − , and the CO 2 activity can be used as a general descriptor to predict the electrode reaction in molten carbonate. Overall, the CO 2 activity descriptor unlocks the electrolyte–electrode-reaction relationship, thereby providing fundamental insights into guiding molten carbonate CO 2 electrolysis.
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FUEL
·
2020
·
IF 5.578
Bowen Lu,Zewu Zhang,Xiaoshan Li,Cong Luo,Yongqing Xu,Liqi Zhang
Cu catalysts have been widely used in CO 2 utilization due to their low reduction temperature and excellent CO 2 hydrogenation performance. It is important to well design Cu catalyst with high efficiency and durability for CO 2 hydrogenation. In this work, CuCe(rod) catalysts with various Cu contents were prepared. The physicochemical properties of the CuCe(rod) catalysts were described by XRD, TEM, N 2 -physisorption and H 2 -TPR.The effect of Cu content on catalytic performance of CO 2 hydrogenation with CuCe(rod) catalysts was also studied. Results showed that a high Cu content enhanced CO 2 conversion. The 40CuCe(rod) catalyst exhibited the best CO 2 conversion performance. At the reaction temperature of 400 °C, the CO production rate (CO 2 conversion) and CO selectivity based on the 40CuCe(rod) catalyst could reach 1.69 mol/g cat /h (41.1%) and nearly 100%, respectively. The analysis of kinetic measurements revealed that the activation energy of the 40CuCe(rod) catalyst was lower than that of other catalysts with different Cu contents during a reverse water–gas shift reaction. The lower activation energy and the interface structure of Cu-O x -Ce were closely related to CO 2 hydrogenation activity and remarkable stability for 96 h with minimal loss of CO 2 conversion activities.
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