SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Hong Zhu,Yan Huang,Simi Li,Lingkui Zhao,Junfeng Zhang
The most promising approach to tackling the greenhouse gases is CO 2 capture and storage (CCS), and amine solid adsorbents are the most widely investigated materials. In this work, Zr species as an accelerator promote CO 2 adsorption of the Pentatethylenehexamine (PEHA)/sepiolite (SEP) adsorbents. The adsorption rate, CO 2 adsorption capacity, and amine efficiency were significantly improved under various conditions (temperature, gas flow, and CO 2 concentration) by the introduction of the optimal content of Zr, the optimal HSEP-Zr 0.13 -PEHA 0.5 -600 adsorbent exhibited 1.80 mmol/g at 60 °C. Adsorption experiments combine with characterization (TG, XPS, NH 3 -TPD, SEM and TEM) exhibited that the introduction of Zr species were high dispersion on sepiolite, and Zr-O bond was formed in the structure of sepiolite. The acidity of the sepiolite supporter was enhanced by Zr which is benefit for amine loading. Above all resulted in the regeneration and thermal stability of the adsorbent were improved together. The economic evaluation results demonstrated that the adsorbent with Zr species is low-cost for large-scale post-combustion CO 2 capture.
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
MOLECULES
·
2024
·Vol. 29
·期 5
·1006
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IF 4.2
Xia Wang,Wulan Zeng,Peidan Hu,Shengxin Liu,Yuechao Lin,Zhaowen He,Chunling Xin,Xiangjun Kong,Jinghan Xu
Organic amine-modified mesoporous carriers are considered potential CO2sorbents, in which the CO2adsorption performance was limited by the agglomeration and volatility of liquid amines. In this study, four additives of ether compounds were separately coimpregnated with polyethylene polyamine (PEPA) into MCM-41 to prepare the composite chemisorbents for CO2adsorption. The textural pore properties, surface functional groups and elemental contents of N for MCM-41 before and after functionalization were characterized; the effects of the type and amount of additives, adsorption temperature and influent velocity on CO2adsorption were investigated; the amine efficiency was calculated; and the adsorption kinetics and regeneration for the optimized sorbent were studied. For 40 wt.% PEPA-loaded MCM-41, the CO2adsorption capacity and amine efficiency at 60 °C were 1.34 mmol/g and 0.18 mol CO2/mol N, when the influent velocity of the simulated flue gas was 30 mL/min, which reached 1.81 mmol/g and 0.23 mol CO2/mol N after coimpregnating 10 wt.% of 2-propoxyethanol (1E). The maximum adsorption capacity of 2.16 mmol/g appeared when the influent velocity of the simulated flue gas was 20 mL/min. In addition, the additive of 1E improved the regeneration and kinetics of PEPA-loaded MCM-41, and the CO2adsorption process showed multiple adsorption routes.
研究领域:
化学工程
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环境科学
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DOI
PubMed
高影响因子
FUEL
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2022
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IF 8.035
Huangyu Yan,Guojie Zhang,Ying Wang,Jun Liu,Guoqiang Li,Yuqiong Zhao,Ying Xu,Yongkang Lv
The low-cost of CO 2 adsorbent is crucial for realistic CO 2 adsorption application. In this paper, a series of green CO 2 adsorbents were prepared using tetraethylenepentamine (TEPA) functionalized blast furnace slag (BFS) as raw materials, which not only implemented the recycling of blast furnace slag solid waste, but also realized the low cost of amine adsorbents. A series of characterization analyses were performed on the synthesized hydrotalcite-like and hydrated calcium silicate green support materials. The effects of structures, TEPA loadings and adsorption temperatures on the material properties were investigated. The result shows that BFS10.5-50TEPA with more pores is an ideal adsorbent, its optimum adsorption capacity for CO 2 is 5.64 mmol/g at 80 ℃, and the amine efficiency is as high as 38.42 %. According to CO 2 -TPD analysis, the dominant CO 2 adsorption mechanism of BFS10.5-50TEPA were physisorption and weak chemisorption. Moreover, the adsorption kinetics and regeneration performances also studied. The results indicate that pseudo-first-order model and pseudo-second-order model are both not accurately at predicting experimental results, while the Avrami model can accurately predict the adsorption kinetics of CO 2 at both low adsorption temperature and high adsorption temperature. After 10 adsorption-desorption recycles, the CO 2 adsorption capacity of BFS10.5-50TEPA still maintain 5.02 mmol/g. This study provides a novel method for the preparation of solid amine adsorbents with high adsorption performance from low-cost solid waste.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Haitao Shi,Rong Cao,Haijun Zhang,Jiajia Yang,Yanlin Fu,Jiping Chen
Solid amine adsorbents represent a promising class of CO 2 sorbents, but their amine efficiency is limited by the inaccessibility of peripheral amines. The surface of mesocellular silica foam (MCF) is functionalized with the mixture of short-chain 3-Glycidyloxypropyl) triethoxysilane (GPTES) and long-chain Octadecyltrimethoxysilane (OTMS), forming pocket structures on the support surface, thereby exposing more amine sites and enhancing the amine efficiency of polyethylenimine (PEI). The resulting adsorbent demonstrates a high CO 2 adsorption capacity (5.02 mmol g −1 at 50 °C, 10 vol.% CO 2 , and 50%RH), high amine efficiency (0.43 at the dry condition), outstanding cyclic stability (0.5% performance decline per cycle under the conditions of dry CO 2 regeneration), and fast adsorption kinetics (15 min for adsorption saturation at 50 °C). First-principles calculations and CO 2 temperature-programmed desorption (TPD) experiments demonstrate that the introduction of GPTES and OTMS is beneficial to decreasing adsorption energy and forming paired carbamic acid states and ammonium carbamate states.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2016
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IF 2.567
Lihuo Zhang,Ni Zhan,Qing Jin,Honglai Liu,Jun Hu
Amine-impregnated solid sorbents have been approved as one of the promising sorbents for CO2 capture. However, the low adsorption rate seriously limits their real application. Herein, we synthesized the mesoporous multilamellar silica vesicle (MMSV) and used them as a novel support for the impregnation of polyethylenimine (PEI). The mesoporous multilamellar structure, as well as the presence of surfactant templates, significantly improved the dispersion of PEI in sorbents and hence improved both adsorption capacity and adsorption rate simultaneously. Among various MMSV-PEIs samples, MMSV(a)-PEI-60% showed the best CO2 adsorption capacity, up to 4.73 mmol/g in pure and dry CO2 flow at 90 °C, and even exhibited a 22% enhancement in humid CO2 flow at 75 °C. Moreover, it also presented good adsorption/desorption cyclic performance. The kinetic study showed that the second-order kinetic model fitted quite well for dynamic CO2 adsorption, and the adsorption rate constants revealed its faster adsorption rate and higher amine efficiency compared with most reported amine-impregnated sorbents.
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
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Yong Kong,Quan Liu,Zhiyuan Liu,Xiaodong Shen
Amine-functionalized silica aerogel globules (AFSAGs) were first synthesized via a simple ball drop casting method followed by amine grafting. The effect of grafting time on the structure and CO2 adsorption performance of the AFSAGs was investigated. The CO2 adsorption performance was comprehensively studied by breakthrough curves, adsorption capacity and rates, surface amine loading and density, amine efficiency, adsorption halftime, and cyclic stability. The results demonstrate that prolonging the grafting time does not lead to a significant increase in surface amine content owing to pore space blockage by superabundant amine groups. The CO2 adsorption performance shows obvious dependence on surface amine density, determined by both the surface amine content and specific surface area, and working temperature. AFSAGs with a grafting time of 24 h (AFSAG24) with a moderate surface amine density have optimal CO2 adsorption capacities, which are 1.78 and 2.14 mmol/g at 25 °C with dry and humid 400 ppm CO2, respectively. The amine efficiency of AFSAG24 with low CO2 concentrations, 0.38–0.63 with dry 400 ppm−1% CO2, is the highest among the reported amine-functionalized adsorbents. After estimation with different diffusion models, the CO2 adsorption process of AFSAG24 is governed by film diffusion and intraparticle diffusion. In the range of 1–4 mm, the ball size does not affect the CO2 adsorption capacity of AFSAG24 obviously. AFSAG24 offers significant advantages for practical direct air capture compared with its state-of-the-art counterparts, such as high dynamic adsorption capacity and amine efficiency, excellent stability, and outstanding adaptation to the environment.
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
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Luming Qi,Yu Han,Gaozhi Bai,Qing Liu,Zhaoyang Fei,Xian Chen,Zhuxiu Zhang,Jihai Tang,Mifen Cui,Xu Qiao
Amine adsorbents have been widely investigated for direct CO 2 capture from air. However, the low amine efficiency of the widely-studied amine sorbents is the critical factor to hinder the practical application under dry conditions. Herein, we developed the brush-like cetyltrimethylammonium chloride (CTAC) templating strategy to prepare micro-mesoporous silica nanoparticles (MMSN-X) and TEPA-functionalized adsorbents (MMSN-X/TEPA-Y). The character of samples was investigated by transmission electron microscopy , N 2 adsorption-desorption, Fourier transform infrared spectroscopy, thermal gravimetric analyzer and X-ray photoelectron spectroscopy. The adsorbent (MMSN-30/TEPA-50) with appropriate amount of brush-like CTAC exhibited higher CO 2 adsorption capacities (3.68 mmol/g adsorbent under simulated dry air conditions) than that of the adsorbents with none or less additives. The kinetic and thermodynamic model were applied to investigate the adsorption rate control factors and adsorption behavior of CO 2 adsorbents with brush-like CTAC. Moreover, with the effect of brush-like CTAC, the significant variation of adsorption product (conversion from carbamate (CO 2 /N = 0.5) to carbamic acid (CO 2 /N = 1)) was detected by in situ Fourier transform infrared spectroscopy . These results demonstrated that the combination of CO 2 and amine was altered in the presence of brush-like CTAC and thereby the amine efficiency was enhanced, which could be expected to be an efficient adsorbent for CO 2 from air in practical applications.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Haorui Liu,Xiaoqiong Wang,Shixun Chen,Shuixia Chen
A novel solid amine adsorbent with interconnect open-cell porous structure was successfully synthesized by crosslinking polyethyleneimine (PEI) with ethylene glycol diglycidyl ether (EGDE) via high internal phase emulsion (HIPE) polymerization. The preparation conditions were optimized. The adsorption performance of the prepared adsorbent for CO 2 was evaluated by fixed bed dynamic adsorption experiment. The results indicated that the optimal adsorbent PEI70K-E-HIPE-8 exhibited a record high CO 2 adsorption capacity of 14.22 mmol/g, amine efficiency of 83% and ratio of breakthrough capacity to equilibrium capacity of 0.92 (abbreviated as Q b /Q e ratio). Both adsorption capacity and adsorption kinetics are much better than those of PEI70K-E-gel-8 prepared without using HIPE template. The adsorbent also showed good CO 2 /CH 4 separation performance, a CH 4 productivity of 54.84 mmol/g could be obtained while using PEI70K-E-HIPE-8 to separated it from a 20 mL CO 2 /CH 4 (20:80, v:v) mixed gas, remarkably higher than that of PEI70K-E-gel-8 (0.28 mmol/g). PEI70K-E-HIPE-8 could keep a stable adsorption and separation performance after at lease 15 adsorption-desorption cycles. The superior CO 2 adsorption capacity and adsorption kinetics make it a promising candidate in practical CO 2 adsorption and CO 2 /CH 4 separation application.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子