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吸附 11

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Fabrication of coconut shell-derived porous carbons for CO adsorption application

《化学科学与工程前沿（英文）》 2023年第17卷第8期页码 1122-1130 doi: 10.1007/s11705-022-2292-6

摘要： Biomass-derived porous carbons have been considered as the most potential candidate for effective CO₂ adsorbent thanks to being widely-available precursor and having highly porous structure and stable chemical/physical features. However, the biomass-derived porous carbons still suffer from the poor optimization process in terms of the synthesis conditions. Herein, we have successfully fabricated coconut shell-derived porous carbon by a simple one-step synthesis process. The as-prepared carbon exhibits advanced textual activity together with well-designed micropore morphology and possesses oxygen-containing functional groups (reached 18.81 wt %) within the carbon matrix. Depending on the different activating temperatures (from 700 to 800 °C) and KOH/biomass mass ratios (from 0.3 to 1), the 750 °C and 0.5 mass ratio were found to be enabling the highest CO₂ capture performance. The optimal adsorbent was achieved a high CO₂ uptake capacity of 5.92 and 4.15 mmol·g⁻¹ at 0 and 25 °C (1 bar), respectively. More importantly, as-prepared carbon adsorbent exhibited moderate isosteric heat of adsorption and high CO₂/N₂ selectivity. The results were revealed not only the textural feature but also the surface functional groups critically determine the CO₂ capture performance, indicating coconut shell-derived porous carbon has a considerable potential as a solid-state adsorbent for the CO₂ capture.

关键词： porous carbons CO₂ adsorption KOH activation single step reaction biomass

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Tuning porosity of coal-derived activated carbons for CO2 adsorption

《化学科学与工程前沿（英文）》 2022年第16卷第9期页码 1345-1354 doi: 10.1007/s11705-022-2155-1

摘要： A simple method was developed to tune the porosity of coal-derived activated carbons, which provided a model adsorbent system to investigate the volumetric CO₂ adsorption performance. Specifically, the method involved the variation of the activation temperature in a K₂CO₃ induced chemical activation process which could yield activated carbons with defined microporous (< 2 nm, including ultra-microporous < 1 nm) and meso-micro-porous structures. CO₂ adsorption isotherms revealed that the microporous activated carbon has the highest measured CO₂ adsorption capacity (6.0 mmol∙g^–1 at 0 °C and 4.1 mmol∙g^–1 at 25 °C), whilst ultra-microporous activated carbon with a high packing density exhibited the highest normalized capacity with respect to packing volume (1.8 mmol∙cm⁻³ at 0 °C and 1.3 mmol∙cm^–3 at 25 °C), which is significant. Both experimental correlation analysis and molecular dynamics simulation demonstrated that (i) volumetric CO₂ adsorption capacity is directly proportional to the ultra-micropore volume, and (ii) an increase in micropore sizes is beneficial to improve the volumetric capacity, but may lead a low CO₂ adsorption density and thus low pore space utilization efficiency. The adsorption experiments on the activated carbons established the criterion for designing CO₂ adsorbents with high volumetric adsorption capacity.

关键词： coal-derived activated carbons porosity CO₂ adsorption molecular dynamics

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Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

《能源前沿（英文）》 2023年第17卷第4期页码 545-554 doi: 10.1007/s11708-023-0867-7

摘要： The effect of oxygen vacancies on the adsorption and activation of CO₂ on the surface of different phases of ZrO₂ is investigated by density functional theory (DFT) calculations. The calculations show that the oxygen vacancies contribute greatly to both the adsorption and activation of CO₂. The adsorption energy of CO₂ on the c-ZrO₂, t-ZrO₂ and, m-ZrO₂ surfaces is enhanced to 5, 4, and 3 folds with the help of oxygen vacancies, respectively. Moreover, the energy barrier of CO₂ dissociation on the defective surfaces of c-ZrO₂, t-ZrO₂, and m-ZrO₂ is reduced to 1/2, 1/4, and 1/5 of the perfect surface with the assistance of oxygen vacancies. Furthermore, the activation of CO₂ on the ZrO₂ surface where oxygen vacancies are present, and changes from an endothermic reaction to an exothermic reaction. This finding demonstrates that the presence of oxygen vacancies promotes the activation of CO₂ both kinetically and thermodynamically. These results could provide guidance for the high-efficient utilization of CO₂ at an atomic scale.

关键词： CO₂ activation oxygen vacancies ZrO₂ different phases

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Parametric study on the mixed solvent synthesis of ZIF-8 nano- and micro-particles for CO adsorption:

Alireza Hadi, Javad Karimi-Sabet, Abolfazl Dastbaz

《化学科学与工程前沿（英文）》 2020年第14卷第4期页码 579-594 doi: 10.1007/s11705-018-1770-3

摘要： The room temperature synthesis of ZIF-8 micro- and nano-particles was investigated using a mixed methanol-water solvent system. ZIF-8 particles of good quality and high crystallinity were obtained. Response surface methodology was used to determine the effect of the synthesis conditions on the ZIF-8 yield, particle size distribution, and mean particle size. The ligand/metal salt molar ratio followed by the amount of sodium formate (the deprotonating agent) and then the amount of water (i.e., the composition of the mixed solvent) respectively had the largest effects on both the ZIF-8 yield and particle size. Results showed that mixing of solvents with different strengths in producing ZIF-8 crystals is a practical method to size-controlled synthesis of ZIF-8 particles. This method is more favorable for industrial-scale ZIF-8 synthesis than using excess amounts of ligands or chemical additives (like sodium formate). In addition, ZIF-8 samples with different mean particle sizes (100, 500, and 1000 nm) were used for CO adsorption and the mid-sized ZIF-8 particles had the highest adsorption capacity.

关键词： metal organic frameworks zeolitic imidazolate frameworks ZIF-8 response surface methodology Box Behnken design CO adsorption

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CO, N, and CO/N mixed gas injection for enhanced shale gas recovery and CO geological storage

《能源前沿（英文）》 2023年第17卷第3期页码 428-445 doi: 10.1007/s11708-023-0865-9

摘要： In this work, using fractured shale cores, isothermal adsorption experiments and core flooding tests were conducted to investigate the performance of injecting different gases to enhance shale gas recovery and CO₂ geological storage efficiency under real reservoir conditions. The adsorption process of shale to different gases was in agreement with the extended-Langmuir model, and the adsorption capacity of CO₂ was the largest, followed by CH_4, and that of N₂ was the smallest of the three pure gases. In addition, when the CO₂ concentration in the mixed gas exceeded 50%, the adsorption capacity of the mixed gas was greater than that of CH₄, and had a strong competitive adsorption effect. For the core flooding tests, pure gas injection showed that the breakthrough time of CO₂ was longer than that of N₂, and the CH₄ recovery factor at the breakthrough time (

R C H 4

) was also higher than that of N₂. The

R C H 4

of CO₂ gas injection was approximately 44.09%, while the

R C H 4

of N₂ was only 31.63%. For CO₂/N₂ mixed gas injection, with the increase of CO₂ concentration, the

R C H 4

increased, and the

R C H 4

for mixed gas CO₂/N₂ = 8:2 was close to that of pure CO₂, about 40.24%. Moreover, the breakthrough time of N₂ in mixed gas was not much different from that when pure N₂ was injected, while the breakthrough time of CO₂ was prolonged, which indicated that with the increase of N₂ concentration in the mixed gas, the breakthrough time of CO₂ could be extended. Furthermore, an abnormal surge of N₂ concentration in the produced gas was observed after N₂ breakthrough. In regards to CO₂ storage efficiency (

S s t o r a g e - C O 2

), as the CO₂ concentration increased,

S s t o r a g e - C O 2

also increased. The

S s t o r a g e - C O 2

of the pure CO₂ gas injection was about 35.96%, while for mixed gas CO₂/N₂ = 8:2,

S s t o r a g e - C O 2

was about 32.28%.

关键词： shale gas gas injection competitive adsorption enhanced shale gas recovery CO₂ geological storage

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Effect of co-existing organic compounds on adsorption of perfluorinated compounds onto carbon nanotubes

Shubo DENG,Yue BEI,Xinyu LU,Ziwen DU,Bin WANG,Yujue WANG,Jun HUANG,Gang YU

《环境科学与工程前沿（英文）》 2015年第9卷第5期页码 784-792 doi: 10.1007/s11783-015-0790-1

摘要： Co-existing organic compounds may affect the adsorption of perfluorinated compounds (PFCs) and carbon nanotubes in aquatic environments. Adsorption of perfluorooctane sulfonate (PFOS), perfluorooctane acid (PFOA), perfluorobutane sulfonate (PFBS), and perfluorohexane sulfonate (PFH S) on the pristine multi-walled carbon nanotubes (MWCNTs-Pri), carboxyl functionalized MWCNTs (MWCTNs-COOH), and hydroxyl functionalized MWCNTs (MWCNTs-OH) in the presence of humic acid, 1-naphthol, phenol, and benzoic acid was studied. Adsorption kinetics of PFOS was described well by the pseudo-second-order model and the sorption equilibrium was almost reached within 24 h. The effect of co-existing organic compounds on PFOS adsorption followed the decreasing order of humic acid>1-naphthol>benzoic acid>phenol. Adsorbed amounts of PFOS decreased significantly in the presence of co-existing or preloaded humic acid, and both adsorption energy and effective adsorption sites on the three MWCNTs decreased, resulting in the decrease of PFOS adsorption. With increasing pH, PFOS removal by three MWCNTs decreased in the presence of humic acid and phenol. The adsorbed amounts of different PFCs on the MWCNTs increased in the order of PFBS

关键词： perfluorinated compounds carbon nanotubes competitive adsorption humic acid perfluorooctane sulfonate (PFOS)

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Integrated adsorption and absorption process for post-combustion CO

Gongkui Xiao, Penny Xiao, Andrew Hoadley, Paul Webley

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 483-492 doi: 10.1007/s11705-020-1964-3

摘要： This study explored the feasibility of integrating an adsorption and solvent scrubbing process for post-combustion CO capture from a coal-fired power plant. This integrated process has two stages: the first is a vacuum swing adsorption (VSA) process using activated carbon as the adsorbent, and the second stage is a solvent scrubber/stripper system using monoethanolamine (30 wt-%) as the solvent. The results showed that the adsorption process could enrich CO in the flue gas from 12 to 50 mol-% with a CO recovery of >90%, and the concentrated CO stream fed to the solvent scrubber had a significantly lower volumetric flowrate. The increased CO concentration and reduced feed flow to the absorption section resulted in significant reduction in the diameter of the solvent absorber, bringing the size of the absorber from uneconomically large to readily achievable domain. In addition, the VSA process could also remove most of the oxygen initially existed in the feed gas, alleviating the downstream corrosion and degradation problems in the absorption section. The findings in this work will reduce the technical risks associated with the state-of-the art solvent absorption technology for CO capture and thus accelerate the deployment of such technologies to reduce carbon emissions.

关键词： vacuum swing adsorption monoethanolamine post-combustion CO₂ capture integrated process

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Efficient CO

Yanxia Wang, Xiude Hu, Tuo Guo, Jian Hao, Chongdian Si, Qingjie Guo

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 493-504 doi: 10.1007/s11705-020-1967-0

摘要： In this work, nitrogen-doped porous carbons (NACs) were fabricated as an adsorbent by urea modification and KOH activation. The CO adsorption mechanism for the NACs was then explored. The NACs are found to present a large specific surface area (1920.72–3078.99 m ·g ) and high micropore percentage (61.60%–76.23%). Under a pressure of 1 bar, sample NAC-650-650 shows the highest CO adsorption capacity up to 5.96 and 3.92 mmol·g at 0 and 25 °C, respectively. In addition, the CO /N selectivity of NAC-650-650 is 79.93, much higher than the value of 49.77 obtained for the nonnitrogen-doped carbon AC-650-650. The CO adsorption capacity of the NAC-650-650 sample maintains over 97% after ten cycles. Analysis of the results show that the CO capacity of the NACs has a linear correlation ( = 0.9633) with the cumulative pore volume for a pore size less than 1.02 nm. The presence of nitrogen and oxygen enhances the CO /N selectivity, and pyrrole-N and hydroxy groups contribute more to the CO adsorption. Fourier transform infrared spectra analysis indicates that CO is adsorbed onto the NACs as a gas. Furthermore, the physical adsorption mechanism is confirmed by adsorption kinetic models and the isosteric heat, and it is found to be controlled by CO diffusion. The CO adsorption kinetics for NACs at room temperature and in pure CO is in accordance with the pseudo-first-order model and Avramís fractional-order kinetic model.

关键词： porous carbon CO₂ adsorption nitrogen-doped adsorption mechanism kinetics

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Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporous

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

《化学科学与工程前沿（英文）》 2011年第5卷第2期页码 264-273 doi: 10.1007/s11705-010-1007-6

摘要： Adsorption of pure CO and N and separation of CO /N mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations. Fully atomistic models of MFI and MFI/MCM-41 are constructed and characterized. A bimodal pore size distribution is observed in MFI/MCM-41 from simulated small- and broad-angle X-ray diffraction patterns. The density of MFI/MCM-41 is lower than MFI, while its free volume and specific surface area are greater than MFI due to the presence of mesopores. CO is preferentially adsorbed than N , and thus, the loading and isosteric heat of CO are greater than N in both MFI and MFI/MCM-41. CO isotherm in MFI/MCM-41 is similar to that in MFI at low pressures, but resembles that in MCM-41 at high pressures. N shows similar amount of loading in MFI, MCM-41 and MFI/MCM-41. The selectivity of CO over N in the three adsorbents decreases in the order of MFI>MFI/MCM-41>MCM-41. With increasing pressure, the selectivity increases in MFI and MFI/MCM-41, but decreases in MCM-41. The self-diffusivity of CO and N in MFI decreases as loading increases, while in MFI/MCM-41, it first increases and then drops.

关键词： adsorption diffusion CO₂ flue gas zeolite micro/mesoporous composite

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Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

《环境科学与工程前沿（英文）》 2021年第15卷第5期 doi: 10.1007/s11783-021-1397-3

摘要：

• Synthesis of NS-CNTS is used in a high desulfurization performance.

关键词： Dibenzothiophene (DBT) Tertiary methyl mercaptan Adsorption Carbon nano tube (CNT) Desulfurization Doping

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Experimental study on capturing CO 2 greenhouse gas by mixture of ammonia and soil

Ying WU, Yifei WANG, Qinghua ZENG, Xin GONG, Zunhong YU,

《化学科学与工程前沿（英文）》 2009年第3卷第4期页码 468-473 doi: 10.1007/s11705-009-0257-7

摘要： This paper presents our study on removal of carbon dioxide (CO) greenhouse gas emissions by using the mixture of ammonia and soil. CO capture capacity using this method is 15% higher than the sum of ammonia chemical absorption capacity and soil physical adsorption capacity. Scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) are utilized to study this synergism. The removal effect is not only reflected in ammonia chemical reaction with CO. CO can also be absorbed by ammonium bicarbonate (NHHCO) crystal, which is the main component of the product, or wrapped in the pore of the crystal or packed in the gap between the crystal and the soil. CO can be permanently deposited as carbonated minerals in the subsoil earth layers.

关键词： electron microscopy product physical adsorption capacity spectroscopy

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Detection of CO

Veselina Georgieva, Richard Retoux, Valerie Ruaux, Valentin Valtchev, Svetlana Mintova

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 94-102 doi: 10.1007/s11705-017-1692-5

摘要： Detection of oxygen and carbon dioxide is important in the field of chemical and biosensors for atmosphere and biosystem monitoring and fermentation processes. The present study reports on the preparation of zeolite films doped with iron nanoparticles for detection of CO and O in gas phase. Pure nanosized LTL type zeolite with monomodal particle size distribution loaded with iron (Fe-LTL) was prepared under hydrothermal condition from colloidal precursor suspensions. The zeolite was loaded with iron to different levels by ion exchange. The Fe-LTL suspensions were used for preparation of thin films on silicon wafers via spin coating method. The reduction of the iron in the zeolite films was carried out under H flow (50% H in Ar) at 300 °C. The presence of iron nanoparticles is proved by ultra-violet-visible spectroscopy. The properties of the films including surface roughness, thickness, porosity, and mechanical stability were studied. In addition, the loading and distribution of iron in the zeolite films were investigated. The Fe-LTL zeolite films were used to detect O and CO in a concentration dependent mode, followed by IR spectroscopy. The changes in the IR bands at 855 and 642 cm (Fe–O–H and Fe–O bending vibrations) and at 2363 and 2333 cm (CO asymmetric stretching) corresponding to the presence of O and CO , respectively, were evaluated. The response to O and CO was instant, which was attributed to great accessibility of the iron in the nanosized zeolite crystals. The saturation of the Fe-LTL films with CO and O at each concentration was reached within less than a minute. The Fe-LTL films detected both oxygen and carbon dioxide in contrast, to the pure LTL zeolite film.

关键词： zeolite films detection of CO₂ and O₂ adsorption

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Encapsulation of 2-amino-2-methyl-1-propanol with tetraethyl orthosilicate for CO2 capture

Sidra Rama, Yan Zhang, Fideline Tchuenbou-Magaia, Yulong Ding, Yongliang Li

《化学科学与工程前沿（英文）》 2019年第13卷第4期页码 672-683 doi: 10.1007/s11705-019-1856-6

摘要： Carbon capture is widely recognised as an essential strategy to meet global goals for climate protection. Although various CO capture technologies including absorption, adsorption and membrane exist, they are not yet mature for post-combustion power plants mainly due to high energy penalty. Hence researchers are concentrating on developing non-aqueous solvents like ionic liquids, CO -binding organic liquids, nanoparticle hybrid materials and microencapsulated sorbents to minimize the energy consumption for carbon capture. This research aims to develop a novel and efficient approach by encapsulating sorbents to capture CO in a cold environment. The conventional emulsion technique was selected for the microcapsule formulation by using 2-amino-2-methyl-1-propanol (AMP) as the core sorbent and silicon dioxide as the shell. This paper reports the findings on the formulated microcapsules including key formulation parameters, microstructure, size distribution and thermal cycling stability. Furthermore, the effects of microcapsule quality and absorption temperature on the CO loading capacity of the microcapsules were investigated using a self-developed pressure decay method. The preliminary results have shown that the AMP microcapsules are promising to replace conventional sorbents.

关键词： carbon capture microencapsulated sorbents emulsion technique low temperature adsorption and absorption

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Optimization of electrochemically synthesized Cu

Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi

《化学科学与工程前沿（英文）》 2020年第14卷第2期页码 233-247 doi: 10.1007/s11705-019-1893-1

摘要： Cu (BTC) , a common type of metal organic framework (MOF), was synthesized through electrochemical route for CO capture and its separation from N . Taguchi method was employed for optimization of key parameters affecting the synthesis of Cu (BTC) . The results indicated that the optimum synthesis conditions with the highest CO selectivity can be obtained using 1 g of ligand, applied voltage of 25 V, synthesis time of 2 h, and electrode length of 3 cm. The single gas sorption capacity of the synthetized microstructure Cu (BTC) for CO (at 298 K and 1 bar) was a considerable value of 4.40 mmol·g . The isosteric heat of adsorption of both gases was calculated by inserting temperature-dependent form of Langmuir isotherm model in the Clausius-Clapeyron equation. The adsorption of CO /N binary mixture with a concentration ratio of 15/85 vol-% was also studied experimentally and the result was in a good agreement with the predicted value of IAST method. Moreover, Cu (BTC) showed no considerable loss in CO adsorption after six sequential cycles. In addition, artificial neural networks (ANNs) were also applied to predict the separation behavior of CO /N mixture by MOFs and the results revealed that ANNs could serve as an appropriate tool to predict the adsorptive selectivity of the binary gas mixture in the absence of experimental data.

关键词： Cu₃(BTC)₂ electrochemical synthesis CO₂ adsorption Taguchi optimization ANN modeling

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Activated carbons and amine-modified materials for carbon dioxide capture –– a review

Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU

《环境科学与工程前沿（英文）》 2013年第7卷第3期页码 326-340 doi: 10.1007/s11783-013-0510-7

摘要： Rapidly increasing concentration of CO in the atmosphere has drawn more and more attention in recent years, and adsorption has been considered as an effective technology for CO capture from the anthropogenic sources. In this paper, the attractive adsorbents including activated carbons and amine-modified materials were mainly reviewed and discussed with particular attention on progress in the adsorbent preparation and CO adsorption capacity. Carbon materials can be prepared from different precursors including fossil fuels, biomass and resins using the carbonization-activation or only activation process, and activated carbons prepared by KOH activation with high CO adsorbed amount were reviewed in the preparation, adsorption capacity as well as the relationship between the pore characteristics and CO adsorption. For the amine-modified materials, the physical impregnation and chemical graft of polyethylenimine (PEI) on the different porous materials were introduced in terms of preparation method and adsorption performance as well as their advantages and disadvantages for CO adsorption. In the last section, the issues and prospect of solid adsorbents for CO adsorption were summarized, and it is expected that this review will be helpful for the fundamental studies and industrial applications of activated carbons and amine-modified adsorbents for CO capture.

关键词： adsorption capacity CO₂ capture activated carbon amine-impregnated adsorbents

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标题作者时间类型操作

Fabrication of coconut shell-derived porous carbons for CO adsorption application

期刊论文

Tuning porosity of coal-derived activated carbons for CO2 adsorption

期刊论文

Enhanced performance of oxygen vacancies on CO adsorption and activation over different phases of ZrO

期刊论文

Parametric study on the mixed solvent synthesis of ZIF-8 nano- and micro-particles for CO adsorption:

Alireza Hadi, Javad Karimi-Sabet, Abolfazl Dastbaz

期刊论文

CO, N, and CO/N mixed gas injection for enhanced shale gas recovery and CO geological storage

期刊论文

Effect of co-existing organic compounds on adsorption of perfluorinated compounds onto carbon nanotubes

Shubo DENG,Yue BEI,Xinyu LU,Ziwen DU,Bin WANG,Yujue WANG,Jun HUANG,Gang YU

期刊论文

Integrated adsorption and absorption process for post-combustion CO

Gongkui Xiao, Penny Xiao, Andrew Hoadley, Paul Webley

期刊论文

Efficient CO

Yanxia Wang, Xiude Hu, Tuo Guo, Jian Hao, Chongdian Si, Qingjie Guo

期刊论文

Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporous

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

期刊论文

Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

期刊论文

Experimental study on capturing CO 2 greenhouse gas by mixture of ammonia and soil

Ying WU, Yifei WANG, Qinghua ZENG, Xin GONG, Zunhong YU,

期刊论文

Detection of CO

Veselina Georgieva, Richard Retoux, Valerie Ruaux, Valentin Valtchev, Svetlana Mintova

期刊论文

Encapsulation of 2-amino-2-methyl-1-propanol with tetraethyl orthosilicate for CO2 capture

Sidra Rama, Yan Zhang, Fideline Tchuenbou-Magaia, Yulong Ding, Yongliang Li

期刊论文

Optimization of electrochemically synthesized Cu

Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi

期刊论文

Activated carbons and amine-modified materials for carbon dioxide capture –– a review

Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU

期刊论文

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