International Journal of Greenhouse Gas Control
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2015
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IF 3.946
Xia Wang,Qingjie Guo,Jun Zhao,Linlin Chen
A CO 2 sorbent was prepared by immobilizing a mixture of tetraethylenepentamine (TEPA) and 2-amino-2-methyl- l -propanol (AMP) onto MCM-41. The prepared composites were characterized by N 2 adsorption–desorption, Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), and thermogravimetric analysis (TGA) techniques. CO 2 adsorption–desorption experiments were conducted in a self-assembled fixed bed reactor under the simulated flue gas component of 15 vol.% CO 2 /85 vol.% N 2 . The promoting effects of AMP on the adsorption performance and amine efficiency of TEPA modified MCM-41 were studied. In addition, the effects of the adsorption temperature and the feed flow rate on the CO 2 adsorption process were investigated. Further, the regenerability of the sorbent was studied by performing fifteen adsorption–desorption cycles over the temperature range of 70 °C (adsorption) to 100 °C (desorption). Among the prepared sorbents, MCM-41 modified with 30 wt.% TEPA and 30 wt.% AMP (MCM-41-TEPA30%-AMP30%) showed rapid adsorption kinetics and the maximum CO 2 adsorption capacity of 3.01 mmol-CO 2 /g-sorbent at 70 °C. Moreover, the MCM-41-TEPA30%-AMP30% sorbent exhibited good regenerability and thermal stability. The results demonstrate that the MCM-41-TEPA30%-AMP30% sorbent is a promising CO 2 sorbent.
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 Sustainable Chemistry & Engineering
·
2021
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IF 8.198
Weiyang Yuan,Shuzhen Chen,Changlei Qin,Dawid Piotr Hanak,Xu Zhou
CO2 adsorption is an important approach to control the excessive CO2 emission from energy and industrial plants and mitigating the greenhouse effect. As an acknowledged high-temperature adsorbent, Li4SiO4 shows advantages in capturing a large amount of CO2 with a fast reaction rate and excellent cyclic stability. However, its CO2 adsorption capacity would be significantly affected by the flue gas impurities, such as SO2 and O2. The underlying reaction mechanism of such impurities and Li4SiO4 is still unclear. For this reason, this work studied the reaction path and kinetics between Li4SiO4 and SO2 through experiments, thermodynamic calculations, and characterizations. The results showed that Li4SiO4 reacts with SO2 to produce Li2SiO3 and Li2SO4 in the presence of O2 at 500–700 °C and forms Li2SiO3 and Li2SO3 in the absence of O2 at 500–682 °C. Furthermore, this study revealed a very low activation energy of 7.47 kJ/mol for Li4SiO4 sulfation in the presence of O2 in the kinetic-controlled stage, and the value goes up to 249.7 kJ/mol in the diffusion-controlled stage. These results will provide valuable references for the industrial applications of CO2 adsorption by Li4SiO4.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Processes
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2023
·Vol. 11
·期 4
·1075
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IF 3.5
Zhaochen Huang,Guoqiang Huang
Usually, the ion implantation gases used in semiconductor production are required to be extremely high in purity. Due to the presence of trace CO2in electronic special gas BF3, the quality of the material is significantly affected, which makes it crucial to impose control on CO2content. Unlike a series of blank adsorbents reported in other studies, the zinc-loaded adsorbents prepared in this study are intended for the adsorption of CO2from CO2/BF3. Firstly, the materials were characterized by XRD, BET, SEM-EDS and TG-DSC analysis, etc., and the breakthrough curves of the adsorbents as obtained under different preparation conditions were investigated at 20 °C and 200 kPa. The results show that the adsorption performance reached the optimal level when the activation temperature was 450 °C and a 13X molecular sieve was impregnated by 0.15 mol/L Zn(NO3)2. Moreover, compared with the Zn-13X, the breakthrough time was reduced to 69% and 44% in two adsorption cycles, respectively. Finally, FTIR was used to reveal the adsorption mechanism of the carbonates produced by CO2adsorption. It was found that the adsorption performance was affected by the irreversible reduction in the number of active sites due to the continuous formation of polydentate carbonate during adsorption and regeneration.Keywords:CO2adsorption;13X molecular sieve;carbonate species
研究领域:
材料科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
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IF 6.735
Yufang Wu,Zhenqiang Lv,Xin Zhou,Junjie Peng,Yuning Tang,Zhong Li
We report a bifunctional SBU-tuning strategy that simultaneously enhances the selective CO 2 adsorption capacity of Cu-BTC and its structural stability under moisture. A series of Gly@Cu-BTCs were prepared by grafting glycine (Gly) to the secondary building units (SBUs) of the commercially available Cu-BTC through the nano-seed assistant ultrafast room temperature synthesis. N 2 isotherms evidenced higher BET specific surface area and pore volume of Gly@Cu-BTCs than that of Cu-BTC. Hence, Gly 0.3 @Cu-BTC exhibited a superior CO 2 capacity of 5.4 mmol/g at ambient conditions, which is 12% higher than that of Cu-BTC. Besides, the adsorptive selectivity of Gly 0.3 @Cu-BTC for the equimolar CO 2 /CH 4 and CO 2 /N 2 mixtures was separately up to 8.53 and 59.38, being 11% and 15% higher compared to that of Cu-BTC. More importantly, the stability of Gly 0.3 @Cu-BTC against moisture was improved. After 10 days’ exposure in 55% relative humidity, Gly 0.3 @Cu-BTC preserved 80% of its original CO 2 capacity, while only 9% CO 2 capacity remained for Cu-BTC. In addition, negligible CO 2 capacity loss of Gly 0.3 @Cu-BTC was observed in the subsequent 10 days in moisture after the initial exposure. Gly 0.3 @Cu-BTC exhibited excellent regenerability, and its CO 2 desorption efficiency reached up to 98% based on the consecutive adsorption-desorption cycles. The origination of the improved stability under moist of Gly 0.3 @Cu-BTC was interpreted with DFT calculation. The bifunctional SBU-tuning strategy demonstrated in this work enables the potential adsorptive separation application of Cu-BTC under moist working condition.
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
NANO
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2024
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IF 1
Xuecong Ma,Linlin Geng,Yu Li,Jianwen Wei,Lei Liao,Dunqiu Wang
Micro/mesoporous materials are low-cost functional materials with the potential for CO 2 adsorption. Modifying micro/mesoporous materials is significant for enhancing CO 2 adsorption and their high-value utilization. Herein, the micro/mesoporous material of composite molecular sieve ZSM-5/MCM-48 (ZM) was synthesized by a two-step crystallization method using cetyltrimethylammonium bromide as a template, tetraethyl orthosilicate as a silicon source and ZSM-5 seed as part of silicon aluminum source. Tetraethylenepentamine (TEPA) and polyethyleneimine (PEI) were used as impregnation modifiers to modify ZM with amine groups. The results showed that with the increase of amine loadings, both ZM-T60 (Impregnated with TEPA) and ZM-P60 (Impregnated with PEI) functionalized adsorbents exhibited the best adsorption capacities of 4 . 9 7 mmol ⋅ g − 1 and 3 . 2 8 mmol ⋅ g − 1 at 60, respectively, when the loading of ZM sample was 60%. The adsorption kinetic analysis showed that the adsorption of CO 2 by ZM-T60 and ZM-P60 was a chemisorption-dominated process accompanied by physical adsorption. After 10 adsorption/desorption cycles, the CO 2 adsorption capacity of ZM-T60 and ZM-P60 decreased by 8.7% and 2.6%, respectively. This work demonstrates that impregnation modification of the composite molecular sieve to achieve efficient CO 2 adsorption has practical application significance.
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
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Chunying Liu,Li Lv,Kun Liu,Junsu Jin,Jianguo Mi,Yongqiang Ren,Shisen Xu
By coupling CALF-20 on ZIF-7 via in situ crystallization in the confined micrometer-sized pores of poly(acrylates), a novel composite, namely, CALF-20-on-ZIF-7@poly(acrylates), has been synthesized for the simultaneous removal of CO2 and H2S from IGCC feed gas. Within this coupled crystal, CALF-20, known for its strong adsorption capacity and excellent stability toward CO2 and H2S, serves as the outer layer crystal to shift the adsorption/desorption hysteresis loop of inner ZIF-7 to beyond atmosphere pressure. Under high pressure, CO2 and H2S are automatically adsorbed. Upon reducing the pressure to the atmospheric level, CO2 is automatically released, while H2S remains temporarily due to its high adsorption energy. After about 150 cycles of CO2 adsorption/desorption of the kilogram-scale composite, H2S approaches saturation and is then removed by vacuuming. Since the content of H2S in IGCC feed gas is trivial, the total energy consumption for the composite regeneration is 0.16 MJ/kg (CO2). After 600 consecutive cycles, the CO2 adsorption capability of the composite decreases by 0.41%, demonstrating excellent cyclic stability.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jinsong Shi,Jianguo Xu,Hongmin Cui,Nanfu Yan,Runhan Yan,Yaqing Weng
Porous carbon is a very promising type of CO 2 adsorbent due to its excellent stability, low cost, and tunable physicochemical properties. In the current work, N-doped hierarchically porous carbon was synthesized with the assistance of NaCl template and KHCO 3 activation. A series of carbons with three dimensional and interconnected micro- meso -macroporous structure were successfully prepared. Effects of synthesis conditions on textural properties and N-doping were analyzed and discussed with details. The carbons also exhibited high surface area (725–2423 m 2 /g) and N content (1.49–7.93 wt%). CO 2 adsorption properties were studied with a combined experimental and theoretical approach. At 25 °C and 1 bar, the carbons exhibited CO 2 uptake up to 4.22 mmol/g and CO 2 /N 2 selectivity up to 25.6. Grand canonical Monte Carlo (GCMC) simulation was employed to further elucidate the different roles played by N-doping and textural properties during CO 2 adsorption. Effects of various N-functionalities located in pores with different sizes on CO 2 adsorption were thus revealed. The present study presents a novel strategy for controlled synthesis of porous carbons, and provides helpful insights into their CO 2 adsorption behaviors.
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
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 32
·13755-13763
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IF 3.288
Xia Wang,Wulan Zeng,Wenjing Liu,Xiaoyu Cao,Chunhui Hou,Qi Ding,Yaxuan Lü
The design and development of low-cost sorbents is vital for CO2 capture from flue gases. In this study, the lignite char from Ordos coal (SE) was treated by a one-step KOH activation method to prepare microporous activated carbons for CO2 adsorption. The textural pore properties, surface functional groups and element contents of SE before and after activation were characterized and discussed; the effects of the mass ratio of KOH to SE, activation temperature and time, as well as the adsorption temperature on CO2 adsorption for prepared porous sorbents were investigated and optimized; the isosteric heat of adsorption and adsorption kinetics for the optimized sorbent were further calculated and fitted. When the mass ratio of KOH to SE was 1 : 1, the activation temperature and time were 700 °C and 120 min respectively, and the sorbent of K/SE700(120) showed an adsorption capacity of 1.35 mmol g−1 at 20 °C, which dropped by 2.96% after ten regenerations. The Langmuir adsorption isotherms fitted the adsorption data of K/SE700(120) well, and the isosteric heats of adsorption were 11–13 kJ mol−1, showing the physisorption characteristic. In addition, the good fit of the adsorption data to the Avrami model suggested that there are multiple adsorption routes for K/SE700(120).
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
ADSORPTION SCIENCE & TECHNOLOGY
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2022
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IF 4.373
Zhijuan Zhang,Pengwei Li,Ting Zhao,Yuanhan Xia
The ZIF-8 crystals were successfully postsynthetically modified using methylamine (MA), ethylenediamine (ED), and N, N-dimethylethylenediamine (MMEN) to improve their adsorption performance toward CO2. Results showed that, compared with the original ZIF-8, the BET specific surface area of MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 has increased by 118.2%, 92.0%, and 29.8%, respectively. In addition, their total pore volume increased separately by 130.8%, 100%, and 48.7%. The adsorption capacities of CO2 on the amine-modified ZIF-8 samples followed the order . The CO2 adsorption capacities at 298 K on MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 were increased by 118.2%, 90.2%, and 29.8%, respectively. What is more, the CO2/N2 selectivities calculated using an IAST model of the amine@ZIF-8 samples at 0.01 bar and 298 K were also significantly improved and followed the order , which increased by 173.0%, 121.4%, and 22.6%, respectively. The isosteric heat of CO2 adsorption () on the MA-ZIF-8, MMEN-ZIF-8, and ED-ZIF-8 all becomes higher, while of N2 on these samples was slightly lower in comparison with that on the ZIF-8. Furthermore, after six recycle runs of gravimetric CO2 adsorption-desorption on MA-ZIF-8, the adsorption performance of CO2 is still very good, indicating that the MA-ZIF-8 sample has good regeneration performance and can be applied into industrial CO2 adsorption and separation.
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
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Jeremiah Amesimeku,Yucheng Zhao,Ke Li,Jinlou Gu
The creation of innovative porous materials for CO 2 capture and separation is proving extremely relevant for environmental sustainability and global warming mitigation. In this study, modified Ce-UiO-66 MOFs were synthesized in 10 min using simultaneous microwave and ultrasound irradiation method. The porosity of the MOF was altered using the soft-templating approach. This strategy resulted in the construction of a hierarchically micro-mesoporous structure with an average mesopore size of 11.10 nm. The as-obtained MOFs, abbreviated as CUT, were characterized with SEM, XRD , FTIR, TGA , BET, and evaluated as CO 2 adsorbents. The results displayed preserved crystal structure, higher thermal stability up to 570 °C. The heightened diffusion of CO 2 molecules to the micropores promoted by mesopore channels, endued CUT with an over-all CO 2 adsorption uptake of 2.53 mmol/g at 273 K at 1 bar outperforming equivalent Ce-UiO-66 MOFs. Notably, the CUT adsorbent showed improved CO 2 /N 2 IAST selectivity (34.2 vs 24.6) and CO 2 isosteric heat of adsorption ( Q st = 30.15 vs 25 kJ/mol) in contrast to pristine UiO-66 (Zr).
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
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Haiqian Zhao,Jiuyang Jia,Jiaxin Ying,Mingqi He,Zekun Sun,Xing Zhang,Zhonghua Wang,Wei Zhou
Utilizing flue gas as feedstock for CO 2 electro−reduction systems is a promising technology to address problems caused by excessive CO 2 emissions. However, the O 2 contained in the flue gas has a significant adverse effect on the CO 2 reduction. Herein, a facile strategy was proposed to suppress the influence of O 2 by constructing a CO 2 −enriched region. N−doping was demonstrated to be an efficient way to enhance CO 2 adsorption selectivity over O 2 on activated carbon. The N−doped activated carbon achieved 3.7 times increase in CO 2 adsorption selectivity over O 2 than that before modification under simulated flue gas atmosphere (75 %N 2 + 15 %CO 2 + 10 %O 2 ). The distinction in adsorption mechanism between CO 2 and O 2 was revealed by quantum chemistry study. The increased polarity of the carbon materials favored CO 2 adsorption and had less impact on O 2 adsorption. The electrostatic interaction between CO 2 and carbon material was demonstrated to be enhanced after the introduction of pyridinic N and pyrrolic N, which led to an improvement in the CO 2 adsorption capacity. The dispersion interaction, which fully regulated O 2 adsorption, was weakened due to the deviation of the O 2 adsorption position. This study provided a reference for the subsequent development of CO 2 selective adsorption materials.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Chemical Science
·
2018
·Vol. 9
·期 14
·3426-3437
·
IF 9.063
Xinyu Li,Zhi-Jian Zhao,Liang Zeng,Jiubing Zhao,Hao Tian,Sai Chen,Kang Li,Sier Sang,Jinlong Gong
La2O3 exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO2 adsorbed on La2O3 and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO2 adsorption and activation over La2O3. Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La2O3via tuning CO2 adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La2O2CO3 on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO2 adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）