ACS Applied Materials & Interfaces
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2025
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IF 8.2
Xiaoyu Shi,Yang Yang,Xu Liu,Jingwen Wang,Fangming Jin
The current carbon capture and utilization (CCU) technologies suffer from energy-intensive processes due to conventional alkaline-based capture methods requiring significant energy input for regeneration and material cycling. In Earth’s carbonate weathering process within Karst systems, CO2 is sequestered and transformed through interaction with CaCO3. Inspired by this natural process, here, we propose an integrated CO2 capture–conversion strategy using geologically abundant carbonates as low-cost absorbents. We demonstrate that CO2 absorbed by carbonates can be efficiently hydrogenated in situ to formate in a one-pot system at 140 °C using a nonprecious cobalt–copper (CoCu) catalyst, achieving 21% yield of formate with diluted CO2 emissions (as low as 50 000 ppm, representative of typical industrial exhaust). Co facilitates the formation of a Cu+/Cu0 interfacial structure, leading to an enhancement of the hydrogenation efficiency. Density functional theory calculations show that the Cu+/Cu0 interface serves as the primary active site for H2 adsorption and activation to H*, which then promotes the reduction of bicarbonate (HCO3–) to formate. Furthermore, the interface between Co and Cu lowers the energy barrier for HCO3– adsorption, leading to its enhanced reduction by H*. This work offers a new pathway for simultaneous CO2 capture and catalytic conversion, advancing sustainable and energy-efficient CCU technologies.
研究领域:
环境化学
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催化化学
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碳中和技术
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可持续能源
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地球化学
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工业废气处理
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产品关联
DOI
PubMed
高影响因子
APPLIED ENERGY
·
2022
·
IF 11.446
Rui-Long Wang,Ming-Jia Li,Dong Li,Yi-Wen Yang
In this paper, a novel microalgal attached membrane photobioreactor based on the modified polyvinylidene difluoride (PVDF) / polyvinyl pyrrolidone (PVP) composite membrane for microalgae direct air carbon capture is developed and optimized. The Computational Fluid Dynamics (CFD) simulation, molecular dynamic study (MDS) and experimental study are adopted to investigate the synergy between light transmission and fluid flow, CO 2 transmission mechanism inside the membrane and microalgae cells. The modified composite membrane is proposed and processed to improve the carbon sequestration rate of the microalgal attached membrane photobioreactor (AM-PBR). First, the synergy angle between the light transmission direction and fluid flow direction of the flat-plate photobioreactor (FP-PBR) is analyzed. To improve the synergy of light and fluid flow, the AM-PBR is proposed. Secondly, for the MDS part, the models of PVDF membrane and polytetrafluoroethylene (PTFE) membrane are developed. A three-layer simulation model is proposed to reveal the transmission mechanism of CO 2 from the gas-liquid layer to the microalgae cell membrane layer. Several parameters including CO 2 diffusion coefficient, CO 2 concentration profile and velocity profile of CO 2 are analyzed to compare the performance of different membranes and working conditions. Then, for verification of the simulation work, AM-PBR experiments are designed. To further enhance the CO 2 transmission and microalgae attached performance, different PVDF/PVP composite membranes are assessed. The carbon sequestration rate of the modified membrane is improved according to the experiments. Finally, the novel microalgae membrane photobioreactor with the modified PVDF/PVP membrane is developed and the carbon sequestration rate of the PBR system is improved. The results showed that the best ratio for PVDF and PVP is 2:1 with 20 wt% solution, and with this modified membrane the carbon sequestration rate of the PVDF/PVP-based AM-PBR is 18.61% higher than the original PVDF-based AM-PBRs. The proposed novel AM-PBR is especially useful for low-concentration CO 2 direct air carbon capture.
研究领域:
环境科学
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生物技术
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产品关联
DOI
高影响因子
Industrial Chemistry & Materials
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2025
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IF 11.9
Bocheng Yu,Muqing Yang,Yijian Qiao,Yaozu Wang,Yongqing Xu,Xuan Bie,Qinghai Li,Yanguo Zhang,Shuzhuang Sun,Hui Zhou
Integrated carbon capture and utilization (ICCU) has emerged as a promising strategy toward carbon neutrality. However, most existing studies rely on simulated flue gas compositions, neglecting the impact of common impurities such as sulfur oxides (SOx) and nitrogen oxides (NOx), thereby limiting the practical industrial applicability of ICCU technologies. Herein, we systematically investigate the effects of SO2 and NO2 at various concentrations on the adsorption-catalysis performance based on a representative Ni-Ca dual functional material (DFM) in ICCU-dry reforming of methane (ICCU-DRM) process. Exposure to 100 ppm SO2 showed negligible influence on catalytic activity but markedly inhibited carbon deposition. Further increasing the SO2 concentration to 500 ppm led to complete deactivation of the DFM. NO2 exhibited a similar concentration-dependent trend to SO2, albeit with a comparatively lower impact. Mechanistic analysis revealed that both SO2 and NO2 promote the formation of a coating layer of calcium-containing compounds on the surface of Ni nanoparticles, accounting for the part or total deactivation. These findings offer critical insights into the industrial applications of ICCU systems under realistic flue gas conditions.
研究领域:
化学工程
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环境科学
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能源技术
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
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2024
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IF 2.7
Yu Bin Wang,Jie Rui Yu,Xiao Xian Zhang,Hao Chen,Han Bang Ruan,Guo Hua Yang
Ammonia carbon capture is characterized by low corrosion, resistance to oxidation and degradation, and low energy consumption for regeneration. However, it also presents challenges such as a slow absorption rate and notable ammonia escape. Current ammonia decarbonization research primarily focuses on the flue gas from power plants, which differs in composition from ship exhaust gas. To address this, we constructed a small carbon absorption test bench and used a mixture of CO 2 and N 2 as the ship exhaust gas. Ammonia solution and alcohol served as absorbents and additives, respectively, to explore the effects of the additive hydroxyl number, the concentrations of the additive and ammonia solution, and the reaction temperature on carbon loading, absorption rate, and ammonia escape. Results indicated that n-propanol was most effective in inhibiting ammonia escape, and a low concentration of ammonia solution was more suitable for absorbing CO 2 . Specifically, when the concentration of ammonia was 4% and the concentration of n-propanol was 0.2 mol/L, the cumulative ammonia escape was reduced by 34% compared to the scenario without additives. Additionally, the carbon loading and average absorption rate reached 0.49 mol CO 2 /mol NH 3 and 2.33 × 10 −3 mol·kg −1 ·min −1 , respectively, representing increases of 34.2 and 60.7%. However, as the reaction temperature increased, the effectiveness of n-propanol in enhancing ammonia absorption diminished. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Processes
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2018
·Vol. 6
·期 4
·35
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IF 1.279
Pingping He,Xingchi Qian,Zhaoyang Fei,Qing Liu,Zhuxiu Zhang,Xian Chen,Jihai Tang,Mifen Cui,Xu Qiao
A series of carbon aerogels were synthesized by polycondensation of resorcinol and formaldehyde, and their structure was adjusted by managing solution concentration of precursors. Carbon aerogels were characterized by X-ray diffraction (XRD), Raman, Fourier transform infrared spectroscopy (FTIR), N2adsorption/desorption and scanning electron microscope (SEM) technologies. It was found that the pore structure and morphology of carbon aerogels can be efficiently manipulated by managing solution concentration. The relative micropore volume of carbon aerogels, defined by Vmicro/Vtol, first increased and then decreased with the increase of solution concentration, leading to the same trend of CO2adsorption capacity. Specifically, the CA-45 (the solution concentration of precursors is 45 wt%) sample had the highest CO2adsorption capacity (83.71 cm3/g) and the highest selectivity of CO2/N2(53) at 1 bar and 0 °C.Keywords:carbon aerogels;concentration;structure manipulation;CO2capture
研究领域:
材料科学
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环境工程
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产品关联
DOI
高影响因子
ENERGY
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2023
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IF 9
Run Qi,Zhaohao Li,Hongyuan Zhang,Hongming Fu,Heng Zhang,Dan Gao,Haiping Chen
Membrane absorption is a promising CO 2 capture technology, which is limited by the high cost of membrane materials. Coal fly ash (CFA)-based ceramic membrane as an alternative material for membrane modules can effectively reduce the preparation cost. In this study, CFA-based ceramic membrane with superhydrophobic properties is prepared by depositing SiO 2 nanoparticles and grafting 1H, 1H, 2H, 2H-perfluorooctyltriethoxysilane (POTS). Characters including pore size distribution, porosity and N 2 flux of superhydrophobic membrane are performed. The superhydrophobic modified ceramic membrane is applied to CO 2 capture experiments using ethanolamine (MEA) solution as the absorbent. The result shows that the contact angle of the modified ceramic membrane reaches 155.0°, which significantly improves the anti-wetting properties of the membrane surface . The CO 2 capture experiment demonstrates a maximum capture efficiency of 97.45% and a mass transfer rate of 21.17 mol/(m 2 ·h). In addition, the superhydrophobic modified ceramic membrane exhibits excellent thermal and chemical stability, sustaining high performance even after 8 h of continuous operation. This study provides the theoretical and empirical foundation for the application of CFA-based superhydrophobic ceramic membranes in CO 2 capture.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
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2025
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IF 5.1
Jiang Liu,Longyu Wang,Wenzhao Sun,Runhu Li,Yuanshui Zhen,Shiyuan Guo,Bo Wang,Xingguang Xu
The escalating global demand for energy and the urgent need to mitigate climate change have spurred the development of next generation carbon capture utilization and storage (CCUS) techniques. This study introduces novel amine-functionalized silica nanoparticles (PEI@SiO2-KH550 NPs) as a high-performance CO2 carrier for CCUS applications. The nanoparticles were synthesized via a facile two-step modification process: grafting 3-aminopropyltriethoxysilane (KH550) onto silica nanoparticles, followed by coating with polyethyleneimine (PEI). This design significantly enhances CO2 absorption capacity by enriching the surface amine groups, so more CO2 will be carried into the target formation, interact with the oil and be stored underground. The resultant nanofluid (0.8 wt% concentration) demonstrated exceptional CO2 uptake (∼100 cm3 under ambient conditions in 40 minutes) and dispersion stability (zeta potential: +38.21 mV). Rheological analyses revealed its shear-thinning behavior, ensuring injectivity in porous media. Remarkably, CO2-saturated nanofluid reduced the dynamic interfacial tension (IFT) between crude oil and water from 19.24 mN m−1 to 7.82 mN m−1, primarily attributed to nanoparticle adsorption at the oil–water interface and in situ generation of surface-active carbamates. In addition, the pressure drop experiment revealed that the presence of PEI@SiO2-KH550 in the aqueous phase could significantly promote the CO2 diffusion rate and facilitate the mass transfer. Besides, molecular dynamics simulations demonstrated that PEI@SiO2-KH550 enhanced the CO2 saturated-nanofluid/crude oil interaction through impacting the interfacial energy (IFE), the radial distribution function (RDF) of light and heavy oil components, the interface thickness and the CO2 diffusion coefficient. Core flooding experiments validated the dual effectiveness of the developed nanofluid, achieving 79.8% oil recovery (10% higher than the carbonated water) and 48.6% CO2 sequestration rate (16.7% higher than carbonated water). The innovation lies in the nanoparticles' scalable synthesis, dual functionality (CO2 capture and interfacial modification), and compatibility with harsh reservoir conditions. This work may provide enlightening insights for integrating CO2-enhanced oil recovery (EOR) with CO2 geological storage, advancing next-generation CCUS technology.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Mengxiang Fang,Ying Xie,Yan Shao,Xiaoming Xu,Yang Xia,Man Mou,Ximing Hu,Tao Wang,Zihao Liu
The steel industry generates 7–9 % of the world’s anthropogenic carbon emissions. Carbon capture, utilization, and storage (CCUS) technologies for low carbon emissions from the steel industry have attracted research attention. Chemical absorption is the most mature and widely used carbon capture method, and reducing the energy consumption of this technology is currently a research hotspot. This work focused on the development of amine blends suitable for carbon capture in a top gas recycling-oxygen blast furnace (TGR-OBF) for low-carbon steelmaking and further reduction of carbon emissions. The effects of piperazine (PZ) and its derivatives on methyldiethanolamine (MDEA) activation were explored. PZ and 2-(piperazin-1-yl)ethanamine (AEP) most significantly activated MDEA. The best absorption and regeneration performance was achieved with aqueous amine solutions at the MDEA:PZ and MDEA:AEP ratios of 5:3 and 1:1, respectively. Blast furnace gas is rich in CO, and we verified that CO does not significantly affect the overall performance of the aqueous amine solution. The maximum absorption rate of the developed MAA absorbent was similar to that of 30 wt% monoethanolamine (MEA), and at 20 % and 35 % CO 2 , the cyclic capacities were 1.57 and 1.47 times greater than that of 30 wt% MEA, while the maximum regeneration rates were 2.13 and 1.92 times greater than those of 30 wt% MEA, respectively. A bench-scale CO 2 capture experiment performed at a flow rate of 4 Nm 3 /h verified the scale-up application potential of the absorbent. The regeneration energy of MAA under the optimal operating conditions was 2.86 GJ/ton CO 2 , which was 28.5 % lower than that of 30 wt% MEA. Moreover, MAA displayed a lower latent heat and lower reaction heat. The developed MAA absorbent has great adaptability and low regeneration energy and is expected to be applied in the steel industry to effectively reduce blast furnace carbon emissions.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Shuai Wang,Chunliang Shang,Yimin Deng,Jan Baeyens,Tatiana V. Plisko,Alexandr V. Bildyukevich,Tejraj M Aminabhavi,Xinying Liu,Mahluli Moyo,Helei Liu
The mass transfer plays a decisive role in screening and evaluation of amine solvents as well as in designing and scale-up of CO 2 capture. The influence of different operating parameters on mass transfer processes in CO 2 capture by EAE-1DMA2P amine solution was thoroughly investigated using a small-scale packed column. The mass transfer mechanism of EAE-1DMA2P amine solution in the capture of CO 2 was discussed by determining both mass transfer control steps and the reaction region between CO 2 and amine solvent, which provided a theoretical guidance for subsequent development of new solvents for large-scale applications. In addition, based on the experimental observations of K G a v , a prediction model for K G a v of EAE-1DMA2P composite amine solution was established by comparing two empirical models viz., Kohl-Riesenfeld-Astarita and Sheng of which Kohl-Riesenfeld-Astarita model provided a better fitting of the experimental results. The commonly used amine solvents and EAE-1DMA2P composite solvents were further compared and analyzed in terms of packed column size design and solvent consumption. The required packed column volume using EAE-1DMA2P composite solvent was only 4.95 m 3 , while the EAE-1DMA2P composite solvent has the smallest solvent consumption among all the solvents, indicating that this solvent has a lower operating cost than the other solvents, suggesting better industrial application.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Lingyu Shao,Feng Xu,Zhicheng Wu,Chang Liu,Chengjin Pan,Yifan Wang,Zhengda Yang,Tao Wang,Longchao Yao,Chenghang Zheng,Xiang Gao
Advancement of the absorbent for CO 2 capture is essential in optimizing the performance and reducing the negative environmental effects associated with this technology. Despite ammonia's promise as an absorbent, the volatility limits its practical application and creates potential environmental pollution . Therein, we assess various additives (amino acids, carbonates, and alkanolamines) for ammonia-based solvents using multi-stage circulation absorber from the viewpoints of aerosol emission, ammonia emission, and CO 2 capture efficiency. Experimental findings reveal that ammonia volatilization can be inhibited by the protonation of free ammonia by carboxyl groups and the formation of hydrogen bonding between amino/hydroxyl groups and ammonia, with ammonia emission reduced by 21.7 %, aerosol emission reduced by 26.5 %, and CO 2 capture efficiency increased to a maximum of 87.8 % under the condition of adding histidine . Moreover, the experiment highlights a positive correlation between total ammonia emission and aerosol concentration/diameter. Additionally, tests combining source abatement with water wash exhibit up to 50.5 % aerosol removal efficiency and up to 76.6 % ammonia removal efficiency. To further mitigate emissions, a comprehensive approach is proposed, achieving an 84.4 % reduction in ammonia emission and a 61.9 % reduction in aerosol emission. Finally, a method for recycling ammonia for desulfurization is suggested.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Sen Liu,Hao Ling,Juan Lv,Hongxia Gao,Yanqing Na,Zhiwu Liang
The sulfolane was, surprisingly, found to be a universal phase-splitting solvent in a serial of aqueous primary alkanolamine solution for CO2 removal; the reaction product of carbamate and hydrophilicity of amine can be the key factor for triggering phase change; also, the phase change can have a significant effect on CO2 capture performance. To comprehensively understand the effect of phase change on absorption, stripping, and phase separation performance, MEA sulfolane-based solution was chosen as a typical biphasic system for investigation. First, the experimental results revealed that the phase change can dramatically decrease the absorption rate and lead to less CO2 capacity in absorption processes. Second, the enriched MEA in separated solution can substantially decrease the energy consumption for CO2 stripping but exorbitant concentration of MEA can significantly reduce the CO2 removal efficiency in a quasicycle of absorption and desorption processes. Third, the phase separation rate of emulsion of MEA/sulfolane solution can be obviously improved by the increasing temperature, and fortunately, the increasing temperature had less effect on miscible solubility of MEA and sulfolane in two separated phases. Finally, on consideration of the absorption rate, energy consumption, and phase separation rate, a new technological process was proposed for CO2 capture using primary alkanolamine sulfolane-based solution to achieve the goal of relative high CO2 removal efficiency and energy saving.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Qing Sun,Qingqiao Zhao,Lifang Zhang,Fengjun Ming,Weidong Zhang
Water lean solvents have received growing attention for CO2 capture due to their low solvent evaporation and potential for energy saving. The previous study mainly focused on the organic diluent selection and paid less efforts on the amine effect. In this study, 11 types of amines with representative structures were selected to explore the effect of amine on CO2 loading and CO2 distribution with poly(ethylene glycol) dimethyl ether (NHD) as organic diluent. Based on the cyclic loading and reaction heat comparison, N-ethylethanolamine (EAE) was selected and the EAE/NHD water lean solvent was constructed. The liquid–liquid phase separation was found in the EAE/NHD/H2O system with more than 95% CO2 concentrated in the lower phase, which yielded high cyclic loading and benefited regeneration energy consumption. The water content effect was further investigated in terms of CO2 cyclic loading and phase separation behaviors, suggesting that EAE/NHD/H2O with a mass ratio of 3:6:1 exhibited the excellent performance of 3.03 mol·kg–1 cyclic loading and 2.27 GJ·t–1 CO2 regeneration energy consumption. 13C NMR and quantum chemistry calculations were conducted to explain the reaction route and phase change mechanism. The large difference between the ion–dipole interaction of ion–H2O and the molecule–molecular interaction of ion-NHD was regarded as the main reason for phase separation. The long-term tests indicated the cycling stability and low corrosivity of EAE/NHD/H2O, as exhibited by the stable CO2 cyclic loading during 8 runs of absorption–desorption and lower corrosivity rate of carbon steel than 30 wt % MEA aqueous solution.
研究领域:
化学工程
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环境科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子