CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2024
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IF 3.1
Wu Yilu,Zheng Haolong,Xia Zihan,Fu Chengmin,Xu Feng,Yan Jian
The development of effective adsorbents with high amine efficiency and CO 2 adsorption almost unaffected by humidity is extremely challenging. In this study, we introduce an innovative solid amine adsorbent, TETA/DEA@FS, composed of triethylenetetramine (TETA) and diethanolamine (DEA) functionalized fumed silica (FS), which exhibits exceptional capability in selectively capturing trace CO 2 from N 2 . TETA/DEA@FS shows an exceptionally high capacity of CO 2 adsorption of 1.13 mmol/g at the temperature of 298 K and the pressure of 0.0004 bar (1 bar=100 kPa), and achieves an unprecedented CO 2 /N 2 IAST selectivity of 1.70×10 12 . TETA/DEA@FS exhibits high amine efficiency, with breakthrough experiments demonstrating that CO 2 adsorption remains nearly unaffected by humidity. Meanwhile, TETA/DEA@FS demonstrates rapid CO 2 adsorption kinetics and outstanding cyclic stability.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Luming Qi,Zhenyang Rong,Yeyang Ni,Linlin Zhang,Zhe Zhou,Qing Liu,Jihai Tang,Mifen Cui,Xu Qiao
The development of highly stable structured solid amine adsorbent is crucial for the large-scale deployment of CO 2 capture systems. Here, we report a structured solid amine adsorbent using the solid-liquid hybrid wrapping method, wherein a suspension of tetraethylenepentamine (TEPA) and ZSM-22 support is encapsulated within a calcium alginate film through freeze-drying. The textural properties of the structured adsorbents (SA@S/T X ) were investigated using scanning electron microscopy, N 2 adsorption-desorption, Fourier transform infrared spectroscopy, and thermal gravimetric analyzer. The CO 2 adsorption capacity of SA@S/T X displayed an initial increase followed by a decrease with increasing TEPA loading, and the adsorption rate exhibited a similar trend according to the pseudo-first-order model. The maximum adsorption capacity and adsorption rate ( k ) were observed to be 2.22 mmol/g and 0.98 min −1 (under conditions of pure CO 2 , 1 atm and 25 °C), respectively, at a TEPA content of 0.5. In addition, SA@S/T X exhibited good regeneration stability with a low loss in capacity of 10.8 % during 30 cycle of CO 2 adsorption–desorption tests, and high thermal stability with a low amine loss of 2.0 % under conditions of 100 °C and 12 h. These results demonstrate that the solid–liquid hybrid wrapping method effectively shapes the powdered adsorbent while significantly reducing TEPA volatilization, offering a possibility for the industrial applications of solid amine adsorbents.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Zhenyang Rong,Luming Qi,Xihua Xu,Linlin Zhang,Qing Liu,Zhaoyang Fei,Ming Xia,Mifen Cui,Xu Qiao
The industrialization of solid amine adsorbents requires the molding of the adsorbents, and the blockage or collapse of the pore structure caused by the molding process will inevitably affect the CO 2 adsorption performance. Herein, the structured solid amine adsorbent pellets (SA-T/M) were fabricated based on the crosslinking of alginate and Ca 2+ under mild conditions. The pelletized SA-T/M well preserved the pore structure of the original support, with only a 26.8 % diminution in specific surface area, which profited to a more uniform loading and dispersion of amine. Benefitting from the influence of pore structure on amine dispersion, SA-T/M achieved a pretty CO 2 adsorption capacity of 2.49 mmol g −1 . The hydroxyl group of alginates can form hydrogen bonds with the amines, which greatly improved the amine stability of the adsorbent and enabled SA-T/M to exhibit excellent cyclic stability. After 30 adsorption-desorption cycles, the adsorption capacity of SA-T/M merely decreased by 15.6 %. Considering the adsorption capacity and stability of structured adsorbents, the molding strategy with the assistance of alginate provides a potential path for the industrial application of solid amine adsorbent molding technique.
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
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Jiehan Lin,Wei Lu,Xiaoyu Shi,Qin Lu,Lei Wang,Hui He
Solid amine adsorbents cannot typically maintain desirable CO2 capture capacity while having ultralow regeneration temperatures. To address this issue, a novel thermoresponsive nanofiber-based solid amine adsorbent (TRCNF/PEIA) with high amino density and high content of thermoresponsive intelligent groups was designed and prepared using epichlorohydrin to rapidly cross-link polyethyleneimine (PEI) and a thermoresponsive cellulose nanofiber (TRCNF). The latter was obtained by grafting N-isopropylacrylamide (NIPAm) on the cellulose nanofiber (CNF) through Ce (IV)-initiated free radical polymerization. The as-prepared TRCNF/PEIA simultaneously showed high capture capacity (6.74 mmol/g) with water at 25 °C and a low regeneration temperature (60 °C). A comparison of the adsorption–desorption properties of TRCNF/PEIA with those of the PEIA, which was prepared using a procedure similar to that of TRCNF/PEIA but without TRCNF, showed that the thermoresponsive property of PNIPAm and the synergy of the hydroxyl groups of TRCNF/PEIA could facilitate CO2 complete desorption from the adsorbent at 60 °C, which was the lowest regeneration temperature to maintain the high adsorption capacity (≥6 mmol/g) of the adsorbents, based on the literature reports.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ENERGY
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2020
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IF 6.082
Chao Chen,Huifang Xu,Qingbin Jiang,Zhan Lin
Silica-supported amine adsorbents are extensively studied for CO 2 capture. However, rational design of silica materials with specific pore structures as amine supports for large CO 2 adsorption capacity , fast adsorption-desorption kinetics, easy regeneration, and good cyclic performance, still remains a challenge. Herein, we synthesize a series of ordered silicas with either bimodal or trimodal meso-macro porosities through a single- or double-templating route as supports for polyethylenimines (PEI) to make solid amine CO 2 adsorbents. Bimodal silicas with textural mesopores and interconnected macropores are ideal supports at medium amine loading, illustrated by significantly high amine efficiencies, e.g., 50BPEI (800)/PS-80-00 achieves a CO 2 uptake of 350 mg g −1 PEI at 75 °C, 1 bar, which is the one of the highest values among PEI/silica composites reported so far; however, further increase of amine loading leads to severe amine efficiency fading. In comparison, trimodal silicas with internal mesopores, textural mesopores, and interconnected macropores show outstanding performance at high amine loading, e.g., 70BPEI (800)/PS-80-187 exhibits a CO 2 adsorption capacity of 215 mg g −1 adsorbent at 75 °C, 1 bar, which is one of the highest values among reported PEI/silica composites. Moreover, we also study the correlations of the CO 2 adsorption capacity and kinetics, regeneration of adsorbent, and cyclic CO 2 adsorption-desorption performance with the PEI type, PEI loading amount, and operation temperatures. This work brings insight into factors affecting the CO 2 capture performance for amine-impregnated silica composites, providing an important guidance to design high-performance solid amine CO 2 adsorbents in the near future.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Journal of CO2 Utilization
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2019
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IF 5.189
Jing Chang,Chengming Hou,Donghai Wan,Xiuli Zhang,Bin Xu,Hongjing Tian,Xia Wang,Qingjie Guo
An alcoholamine, 2-[2-(dimethylamino)ethoxy]ethanol (DMAEE), was co-tethered with pentaethylenehexamine (PEHA) on the surfaces of the flue gas desulfurized gypsum (FGDG) carriers to synthesize a solid bi-amine adsorbent. The effects of temperature, loading of the blended amines, mass ratio of DMAEE to PEHA, CO 2 partial pressure on the CO 2 adsorption performance were discussed. The water of hydration contained in the FGDG carriers promoted the CO 2 adsorption capacity of the bi-amine adsorbent. Both the breakthrough time and the saturation adsorption capacity of the bi-amine adsorbent were distinctly higher than the DMAEE or PEHA singly tethered adsorbents. The adsorption capacity of the bi-amine adsorbent decreased by only 1.86% over twelve cycles. The isosteric heat of adsorption Q s t and the mean free energy of adsorption E f e was determined and both the values indicated that the adsorption was primarily chemisorption. In the kinetics analysis, Avrami model fitted best with the measured adsorption capacity. With the aid of the 13 C–NMR quantitative analysis results, the CO 2 adsorption mechanism of the bi-amine adsorbent in the presence of the water of hydration was revealed. For the bi-amine adsorbents supported on some porous carriers, FGDG particles were testified to replace up to 7 wt.% of montmorillonite clay or 7 wt.% of MCM–41 zeolite or 10.5 wt.% of ZSM–5 zeolite without any decrease in the CO 2 adsorption capacity.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Chemistry-An Asian Journal
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2016
·Vol. 11
·期 21
·3055-3061
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IF 4.592
Hui He,Linzhou Zhuang,Shuixia Chen,Hucheng Liu
Graphical Leave a gap ! A carbon dioxide imprinted solid amine adsorbent (IPEIA-R) with polyethylenimine (PEI) as a skeleton was conveniently prepared by using glutaraldehyde to cross-link carbon dioxide-preadsorbed PEI (see figure). The solid amine adsorbent showed a remarkable CO 2 adsorption capacity (8.56 mmol g −1 ) in the presence of water, owing to the high amine content and good swelling properties. A carbon dioxide imprinted solid amine adsorbent (IPEIA-R) with polyethylenimine (PEI) as a skeleton was conveniently prepared by using glutaraldehyde to cross-link carbon dioxide-preadsorbed PEI. As confirmed by FTIR, FT-Raman, and 13 C NMR spectroscopy, CO 2 preadsorbed on PEI could occupy the reactive sites of amino groups and act as a template for imprinting in the cross-linking process. The imino groups formed from the cross-linking reaction between glutaraldehyde and PEI could be reduced by NaBH 4 to form CO 2 -adsorbable amino groups. The adsorption results indicated that CO 2 imprinting and reduction of imino groups by NaBH 4 endowed the adsorbent with a higher CO 2 adsorption capacity. Compared with PEI-supported mesoporous adsorbents, the solid amine adsorbent with PEI as a skeleton can avoid serious pore blockage and CO 2 diffusion resistance, even with a high amine content. The solid amine adsorbent with PEI as a skeleton showed a remarkable CO 2 adsorption capacity (8.56 mmol g −1 ) in the presence of water at 25 °C, owing to the high amine content and good swelling properties. It also showed promising regeneration performance and could maintain almost the same CO 2 adsorption capacity after 15 adsorption–desorption cycles.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
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2023
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IF 5.3
Jinrui Zhang,Xiaoqiong Wang,Shixun Chen,Haorui Liu,Shuixia Chen
The adsorption capacity of a solid amine adsorbent for CO2 adsorption is often limited by the number of amino groups on the adsorbent surface. In this paper, a kind of ultrafine solid amine fiber (PSN) was prepared by direct electrospinning of polyethylenimine blends, which could provide plentiful amino groups on the fiber surface without further modification and would improve the CO2 adsorption capacity and amino utilization efficiency of the fibrous adsorbent. The effects of the adsorbent structure on the CO2 adsorption performance of PSN was investigated. The results indicated that the fibrous structure and higher outer surface area of PSN can greatly improve its adsorption capacity and adsorption rate for CO2. Under the simulated flue gas conditions (90% N2/10% CO2) at 25 °C, the CO2 adsorption capacity of PSN fiber is 2.10 mmol/g, and its CO2 adsorption capacity could reach 4.98 mmol/g at 75 °C. The diameter of the fiber obviously affects the CO2 adsorption behavior of the solid amine adsorbents; an increase of the fiber diameter would result in the decrease of the adsorption capacity of the adsorbents. PSN has good regeneration stability, and its CO2 adsorption performance remained almost unchanged after a number of regeneration cycles.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Fu Yang,Li-an Xing,Kwame Nana Opoku,Hongyao Zhao,Zhenxiao Wang,Ruiting Ni,Qiang Gao,Zengjing Guo,Feng Zeng,Aihua Yuan,Jianming Pan
The utilization of ambient low-pressure CO 2 adsorption for carbon neutrality initiatives holds great potential. However, conventional liquid amine absorption methods for CO 2 capture are plagued by high energy consumption and equipment corrosion issues. In this study, we present a novel approach using industrial waste silica fume (SF) as a precursor and tetraethylenepentamine (TEPA) as a chemical modifying agent to efficiently synthesize low-cost mesoporous solid amine adsorbents within the waste-derived mesoporous powder sorbents (MPS) series. Employing the static adsorption technique, the impact of both adsorption temperature and amine loading on the CO 2 adsorption efficacy was comprehensively investigated. The optimized sample, MPS-TEPA-30, demonstrated a superior CO 2 adsorption capacity, achieving 2.22 mmol g −1 at 323 K and 1 bar, a significant 6.8-fold increase compared to the unmodified MPS material (0.326 mmol g −1 ). Additionally, MPS-TEPA-30 demonstrated notable performance advantages, surpassing SBA15-TEPA-30 and MCM41-TEPA-30 with near 1.49- and 2.12-fold increases in adsorption capacity, respectively. Impressively, MPS-TEPA-30 exhibited remarkable adsorption ability beyond 1.5 mmol g −1 at ultralow pressures (<0.01 bar), suggesting its potential for ambient ultralow-pressure CO 2 capture. Moreover, MPS-TEPA-30 showed exceptional stability over multiple adsorption–desorption cycles, with only a marginal 6 % decrease in CO 2 capture efficiency after the seventh cycle. Thermogravimetric analysis confirmed the robust thermal stability of the amine-functionalized adsorbent (∼473 K), rendering it suitable for high-temperature adsorption–desorption processes. The Ideal Adsorbed Solution Theory (IAST) equation predicted an excellent adsorption selectivity of 1600 for the CO 2 /N 2 (1:1) mixture at 323 K and 10 mbar, underscoring the promising prospects of MPS-TEPA-30 in CO 2 capture and selective separation applications from ambient condition.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 12
·10016-10023
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IF 3.201
Fenglei Liu,Yizhu Kuang,Shuoyu Wang,Shuixia Chen,Wenhao Fu
A molecularly imprinted solid amine adsorbent was successfully synthesized via a facile crosslinking reaction based on polyethyleneimine (PEI) as the skeleton, glycol diglycidyl ether (GDGE) as cross-linker and CO2 molecules as template. FT-IR, FT-Raman, 13C NMR spectroscopy and TGA were employed to characterize the chemical structure and thermal stability of the solid amine adsorbent. The experimental results showed that the amine content of the molecularly imprinted polymer polyethyleneimine spheres (MIP-PEIs) could reach as high as 11.41 mmol g−1, and the material exhibited a lower CO2 diffusion resistance during CO2 adsorption. The CO2 adsorption capacity of MIP-PEIs (6.58 mmol g−1) was higher than that of non-imprinted NIP-PEIs (5.87 mmol g−1). The presence of water markedly increased the CO2 adsorption capacity by promoting the chemical adsorption of CO2 on the solid amine adsorbent. The pseudo-second order model could accurately describe the CO2 adsorption process on the MIP-PEIs from the beginning to the end. Moreover, this adsorbent also exhibited good regeneration performance, retaining almost the same adsorption amount of CO2 as the fresh material after ten adsorption–desorption cycles.
研究领域:
材料科学
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环境工程
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
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IF 7.4
Miaomiao Tan,Xiangyu Li,Yu Feng,Bing Wang,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang
The ordered mesoporous silica materials with large pore volume were prepared from the silica source extracted from fly ash by supercritical hydrothermal activation. This path has the advantages of low activation temperature, high silicon utilization, and matching of silicon source extraction and the hydrothermal synthesis process. The obtained mesoporous silica support was impregnated with 60 wt% tetraethylenepentamine (TEPA) to prepare excellent solid amine sorbent. The thermogravimetric results showed that the CO 2 adsorption capacity of sorbent could reach 5.17 mmol/g under 75 °C and dry pure CO 2 atmosphere. At the same time, the sorbent had fast adsorption kinetics (5.08 mmol/g in 10 min) and stable cycle performance. Consequently, the obtained sorbent is a promising candidate for carbon capture technologies.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Yangguan Chen,Jinrui Zhang,Haorui Liu,Xiaoqiong Wang,Shuixia Chen
Solid-amine adsorbents are promising CO 2 post-combustion adsorption materials to mitigate global warming. As one of the most important evaluation criteria, the CO 2 adsorption capacity of the adsorbent was determined by both kinetic and thermodynamic factors, while high temperature is good for mass transfer and low temperature is advantageous for equilibrium to move towards adsorption. In this study, surfactants were added into polyethylenimine (PEI) cryogel to enhance mass transfer and reduce the adsorption temperature, thereby promoting its adsorption capacity. With the addition of polyethylene glycol (PEG200), the CO 2 adsorption capacity reached a maximum value of 6.48 mmol/g at 65 °C, and the amine efficiency reached a maximum value of 0.52 mol C/mol N at 45 °C. Further characterization revealed that the addition of PEG not only enhanced the mass transfer, but also changed the chemisorption mechanisms, which were very similar to the effects of water. Besides, PEG would form hydrogen bonds with the PEI polymer network and showed stable regeneration capacity, thereby exhibiting a greater application potential.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）