ENERGY
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2022
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IF 8.857
Haorui Liu,Shuoyu Wang,Xiaoqiong Wang,XiaoJing Feng,Shuixia Chen
A novel stable porous solid amine adsorbent with three-dimensional interpenetrating network structure was prepared by polymerization of divinylbenzene using high internal phase emulsion (HIPE) template method , and followed by further introducing polyethyleneimine (PEI) by impregnation-crosslinking method. Fixed bed dynamic adsorption experiment proved that under wet condition, the former exhibited not only a higher capacity of 6.22 mmol/g but also a better adsorption kinetics process with faster adsorption rate and longer lag in breakthrough point, which makes it potential to be used in gas separation. In CO 2 /CH 4 separation experiment, PolyHIPE-PE30-4 showed a CO 2 /CH 4 separation selectivity of 253 at 298 K and 1 bar, and meanwhile exhibited an extra-high operating capacity. The pure methane productivity of PolyHIPE-PE30-4 was 24.1 mmol/g from CO 2 /CH 4 (80:20, v/v) mixed gas, 4.5 times to that of PE30-4 gel (5.36 mmol/g). Significantly, PolyHIPE-PE30-4 could maintain an excellent regeneration performance after at least 7 cycles, while PolyHIPE-P30 exhibited a remarkably decrease in adsorption capacity after only three adsorption-desorption process in wet condition, demonstrating the advantage of impregnation-crosslinking method for amine functionalization. The superior CO 2 adsorption capacity and regeneration stability, combined with its superior adsorption kinetics property make it a broad prospect in the field of CO 2 /CH 4 separation.
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DOI
高影响因子
FUEL
·
2021
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IF 6.609
Xinjie Luo,Pengfei Zheng,Ke Gao,Bing Wei,Yujun Feng
Water-alternating-CO 2 gas (WAG) flooding is a common technique to enhance oil recovery via improving CO 2 sweep efficiency, but serious gas channeling may still occur, especially in reservoirs with strong heterogeneity, due to a poor blocking capacity of aqueous slugs to the “channeling” pathway induced by their low viscosity. Herein, a copolymer whose aqueous solution viscosity can be increased by both heat and CO 2 was developed and added into the aqueous slug to control gas channeling and increase oil recovery during enhanced WAG processes. The copolymer was synthesized by grafting poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) onto the triblock copolymer, Pluronic F127, PEO 100 -PPO 65 -PEO 100 . The aqueous copolymer solutions can be thickened/gelled by heating due to the formation of micelles as the physical cross-link and their entanglements even at a concentration as low as 0.2 wt%, and viscosified by bubbling CO 2 thanks to expanded copolymer coils caused by electrostatic repulsion-induced chain extension of protonated PDMAEMA chains. Notably, thermo- and CO 2 -triggered viscosifying can work synergistically and they are completely reversible upon cyclically heating/cooling the copolymer solutions and bubbling/removing CO 2 into/from the aqueous phase, respectively. In WAG flooding tests using two parallel cores, gas channeling was mitigated by blocking high-permeability cores due to in-situ thermo-induced gelation and CO 2 -triggered thickening of copolymer slugs, thus diverting chase fluids into unswept low-permeability cores and enhancing 21–22% total oil recovery than the conventional and HAPM-enhanced WAG modes. Importantly, owing to the characteristics of low initial viscosity, single component, and thermo-gelation, this dually-responsive copolymer possesses high injectivity and satisfactory gelation control. This work could enlighten the design of novel dual/multiple stimuli-thickening polymers used for channeling control and enhanced oil recovery.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Dan Li,Cuiping Li
A class of CO2-binding organic liquids (CO2-BOLs) composed of 1,1,3,3-Tetramethylguanidine (TMG) and Glycerol (Gly) and Gly’s amino derivatives were developed for highly efficient and reversible CO2 capture. These CO2-BOLs exhibited high gravimetric CO2 solubility up to 0.196 g CO2·g–1 at 313.2 K and 1.0 atm, superior to most functionalized ILs and other absorbents. The influential factors of CO2 absorption, such as components of CO2-BOLs, absorption temperature, and CO2 partial pressure together with water contents were investigated, and the recyclability of CO2-BOLs was verified to be excellent. The absorption mechanism of CO2-BOLs was explored with the help of spectral analysis, quantum chemical calculation, and thermodynamic analysis. All the results revealed that chemisorption took place once these CO2-BOLs were exposed to CO2, and alkyl guanidine carbonates were produced. Besides, it is illustrated that introducing the amino group to Gly could reduce the nucleophilic reactivity of CO2-BOLs, along with the absorption enthalpy simultaneously.
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高影响因子
APPLIED ENERGY
·
2018
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IF 7.9
Xiaowen Zhang,Helei Liu,Zhiwu Liang,Raphael Idem,Paitoon Tontiwachwuthikul,Mohammed Jaber Al-Marri,Abdelbaki Benamor
The aim of this work is to find a potential way for great decrease in CO 2 capture energy requirement. Here, for the first time, a series of bifunctional Al 2 O 3 /HZSM-5 catalysts (Al-ZSM) were prepared by the combined precipitation ultrasound method and used for the CO 2 desorption process. All the investigated catalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrometry (FT-IR), N 2 adsorption–desorption, ammonia and CO 2 temperature programmed desorption (NH 3 /CO 2 -TPD) and pyridine-adsorption infrared spectroscopy (Py-IR). The regeneration behaviors of a 5 M monoethanolamine (MEA) solvent with four Al-ZSM catalysts were studied at an initial CO 2 loading of 0.5 mol CO 2 /mol amine and the temperature of 96 °C. The results reveal that all the catalysts improve the CO 2 desorption performance, the Al-ZSM catalysts show higher catalytic performance than the single catalysts Al 2 O 3 and HZSM-5, and the Al-ZSM can reduce the heat duty by 23.3–34.2% as compared with the catalyst-free test. The use of Al-ZSM in the MEA regeneration process improves the desorption performance by 2–3 times in comparison with the blank run. A possible dual sites mechanism of CO 2 desorption with Al-ZSM is suggested. The excellent performance of Al-ZSM can be attributed to their enhanced Brϕnsted acid sites (BAS), mesopore surface area (MSA) and basic sites, which resulted from the good synergistic reaction between the Al 2 O 3 and HZSM-5, and the base treatment for HZSM-5. Besides, the stability test of the Al-ZSM was conducted. Based on the results, the Al-ZSM demonstrate a superior catalytic performance for the rich amine regeneration process, and present an excellent cyclic stability, explicitly have the potential to be a promising industrial catalyst for CO 2 capture. Furthermore, the dual sites catalytic CO 2 desorption over bifunctional catalysts will open a new path to design better catalysts for the rich amine solution regeneration process to increase the desorption performance, reduce the regeneration energy consumption, and thus further decreasing the operation costs of CO 2 capture.
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DOI
高影响因子
APPLIED ENERGY
·
2018
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IF 7.9
Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang
To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Daofei Lv,Renfeng Shi,Yongwei Chen,Yang Chen,Houxiao Wu,Xin Zhou,Hongxia Xi,Zhong Li,Qibin Xia
A water resistant zirconium–porphyrin metal–organic framework PCN-222 was synthesized for selectively separating CO2/CH4 and CO2/N2. Isotherms of CO2, CH4, and N2 on PCN-222 at low and high pressures were respectively measured. At 298 K, CO2 uptakes at 100 and 3000 kPa were 1.16 and 13.67 mmol/g, respectively. At 298 K and 100 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities separately reached 4.3 and 73.7. At 298 K and 3000 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities were 4.7 and 32.8, respectively. Importantly, breakthrough experiments confirmed that PCN-222 could achieve the effective separation of CO2/CH4 (both 50:50 and 10:90) and CO2/N2 (both 50:50 and 15:85) gas mixtures. The dynamic regeneration experiments showed that PCN-222 maintained its initial CO2 adsorption capacity after five cycles of CO2 adsorption–desorption. This work suggested that PCN-222 was a potential candidate for selectively separating CO2/N2 and CO2/CH4.
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高影响因子
ACS Applied Materials & Interfaces
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2018
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IF 8.097
Ebrahim Ataeivarjovi,Zhigang Tang,Jian Chen
In this present work, a novel approach has been proposed by which a solvent absorption and membrane desorption methods can significantly reduce the carbon dioxide (CO2) emission and energy consumption. In this method, the CO2 capture processing is based on the combination of membrane and physical solvent. Here, dimethyl carbonate and polydimethylsiloxane (PDMS)–SiO2 nanocomposite were used as the physical solvent and desorption membrane, respectively. However, the main focus of this research was on the CO2 desorption behavior of PDMS–SiO2 hybrid membrane. To do so, the influence of the operating conditions and membrane properties on the pervaporation process to capture CO2 have been investigated. The PDMS–SiO2 hybrid membrane containing 10 wt % SiO2 was the most effective membrane. Results revealed that increase in CO2 concentration from 1.5 to 3 wt % led to decrease in the selectivity from 94 to 47 and increase in flux from 1.7 to 5.38 (kg/m2·h). In addition, an increase in temperature increased the flux and reached the highest level (8.17 kg/m2·h) at 40 °C. However, the selectivity decreased to 36.13. It was found that the addition of SiO2 nanoparticles to the PDMS membrane not only enhanced the membrane performance but also decreased the energy consumption about 75% compared with gas stripping method and mass transfer about 49% compared with pure PDMS membrane. Finally, these results illustrated that such a novel technique used for pervaporation separation process is a green and promising alternative to separate CO2 from the physical solvent.
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DOI
PubMed
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Yongsheng Tan,Qi Li,Liang Xu,Chikezie Chimere Onyekwena,Tao Yu,Lifeng Xu
Nanoparticles effectively enhance the CO2 geological storage capacity by altering wettability during CO2–brine–rock interactions, which significantly impacts the CO2 residual trapping and migration in reservoirs. However, the effect of nanoparticles on CO2–brine–rock interactions in carbonate formations is poorly understood. Therefore, in this study, the impact of SiO2 nanoparticles (SNPs) on CO2–brine–rock interactions was evaluated under supercritical CO2 conditions (60 °C and 12 MPa) by analyzing wettability, conducting X-ray diffraction, scanning electron microscopy analyses, measuring weight loss, and performing low-field nuclear magnetic resonance (LFNMR) tests. The results indicated that (a) both CO2–brine–rock interactions and SNPs–CO2–brine–rock interactions can alter the wettability of carbonate rock surfaces from oil-wet to water-wet and that the carbonate rock became more water-wet after SNPs addition; (b) CO2–brine–rock interactions primarily involved the dissolution of calcite in carbonate rocks under acidic conditions, but SNPs–CO2–brine–rock interactions were more intense; (c) based on LFNMR analysis, the pores of the carbonate core in this study were divided into small pores (T2 < 5 ms) and large pores (T2 > 5 ms), with CO2–brine–rock interactions occurring mainly in the large pores of the carbonate cores but with enhanced interactions in small pores; (d) CO2 solubility in solution after CO2–brine–rock interactions increased with increasing pressure and eventually reached equilibrium, and this trend was observed both in the CO2–brine–rock system and the SNPs–CO2–brine–rock system. However, the CO2 solubility in the SNPs–CO2–brine–rock system was greater than that in the CO2–brine–rock system.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Ziyi Li,Jia Xiong,Hang Song,Shuchang Liu,Yufei Huang,Yangqiang Huang,Geoffrey I. N. Waterhouse,Ziyun Wang,Yu Mao,Zhiwu Liang,Xiao Luo
To enhance the photocatalytic efficiency of ZIF-67 (Zeolitic Imidazolate Framework-67), we integrated it with Ti 3 C 2 T x MXene through in-situ synthesis and assessed the effects of different MXene concentrations on photocatalytic activity. We identified ZIF-67/Ti 3 C 2 T x MXene as the optimal catalyst (denoted as ZT-450), yielding CO, CH 4 , and H 2 at 62.7, 6.7, and 7.3 μmol g −1 , respectively. The CO productive rate achieved by ZT-450 exhibits a substantial enhancement, outperforming both ZIF-67 and Ti 3 C 2 T x by factors of 16.1 and 4.8, respectively. After introducing Ti 3 C 2 T x in ZIF-67, CO 2 adsorption ability achieves 127.90 μmol g −1 , much higher than those of pure ZIF-67 and Ti 3 C 2 T x . Combining Density Functional Theory (DFT) calculations, we established that introducing Ti 3 C 2 T x in ZIF-67 facilitates rapid electron transfer and improves light absorption, CO 2 activation. In-situ DRIFTS measurements of photocatalytic CO 2 reduction reaction (CO 2 RR) on ZIF-67/Ti 3 C 2 T x MXene composite were employed to reveal the emergence of intermediates such as *COOH, *CHO, *OCH 3 , etc ., and elucidate the mechanism accordingly. This research contributes to the advancement of photocatalytic CO 2 RR, offering insights into applying Ti 3 C 2 Tx MXene in photocatalysis.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xi Tang,Bin Xu,Wufeng Jiang,Xiaoshan Li,Ge Gao,Fan Wu,Cong Luo,Liqi Zhang
Piperazine (PZ) derivatives which have been widely used in CO 2 capture technology exhibit stable physicochemical properties, such as resistance to thermal degradation and low regeneration energy consumption. Both two parameters of CO 2 absorbents, low CO 2 absorption heat (ΔH abs ) and large CO 2 equilibrium solubility (α e ), are important to CO 2 capture performance. However, the influence of functional group types of PZ derivatives on their CO 2 capture performance remained unclear. This research aimed to study the functional group influence on the ΔH abs and α e by PZ derivatives with two amines using experimental and quantum chemical methods. The results indicated that PZ derivatives with the ethyl side chain had larger ΔH abs and α e than those with the methyl side chain. The presence of the hydroxy group in PZ derivatives reduced the ΔH abs and the α e . The presence of cyclic methyl side chains on the N atom of PZ derivatives decreased the ΔH abs and increased α e at the same time. The findings show that PZ derivatives with cyclic methyl side chains, steric hindrance effect, and no hydroxy group are favorable for CO 2 capture. Among the eight PZ derivatives, TEDA with lower ΔH abs (48.99 kJ/mol) and higher α e (0.917 mol CO 2 /mol amine) is an excellent absorbent. The results of this study are very important for screening efficient and low-energy consumption absorbents for CO 2 capture.
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高影响因子
Fundamental Research
·
2024
·
IF 5.7
Na Chu,Xiaobing Wu,Ziyue Zhao,Xue Zheng,Yilin Lu,Ying Pu,Yue Wang,Jiayi Cai,Lixia Zhang,Xiaohong He,Daping Li,Raymond Jianxiong Zeng,Yangyang Yu,Yong Jiang
The demand for converting CO 2 into fuels or chemicals is on the rise to achieve a carbon-efficient circular economy. Biohybrid CO 2 electrolysis shows potential for increasing production rates and diversifying product spectra by combining electrocatalysts and microbial catalysts. However, it is important to note that utilizing a shared catholyte for biohybrid CO 2 electrolysis has not demonstrated significant performance improvements to date. In this study, we developed a biohybrid CO 2 electrolysis system utilizing a solid electrolyte operating in an external mode. The produced formic acid was extracted and used as an intermediate for microbial conversion. Impressively, the solid-electrolyte CO 2 electrolysers obtained a remarkable total Faraday efficiency of 81.4% for formic acid production. In-situ mechanism studies unveiled metallic tin as the probable real active site, prompting further exploration of strategies to boost the activity and stability of electrocatalysts. In the bioconversion step, we achieved a noteworthy 8-day duration for generating bioelectricity, nearly 100% electron recovery for biomethane production, and 90.8% for acetate generation. Additionally, when ethanol was co-fed, a C 6 specificity of 41.1% was observed for the generation of medium-chain fatty acids (MCFAs). This study presents groundbreaking experimental data that demonstrates the numerous advantages of utilizing hybrid systems as advanced synthesis techniques.
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DOI
高影响因子
RESOURCES CONSERVATION AND RECYCLING
·
2024
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IF 11.2
Yuguang Mao,Xiang Hu,Sarra Drissi,Wei Chen,Caijun Shi
To address the challenge posed by the carbonation product layer formed on recycled cement paste powder (RCPP) on the efficiency and degree of carbonation, CO 2 -loaded monoethanolamine (MEA) “microcapsules” were used. The CO 2 within MEA was released by heating after the formation of the dense carbonation products layer on RCPP to provide an additional internal CO 2 source to penetrate into the uncarbonated layer. Results showed that using CO 2 dissolved in 15 %, 30 %, and 45 % MEA aqueous solution increased the carbonation degree of RCPP by 10.8 %, 11.2 %, and 13.8 %, respectively, compared to RCPP wet carbonated in water. In addition to calcite, vaterite and aragonite were observed in the CO 2 -loaded MEA carbonated RCPP. The long-term compressive strength of cement pastes with 30 % CO 2 -loaded MEA carbonated RCPP increased, and the porosity decreased compared to cement paste with RCPP wet carbonated in water. However, MEA negatively affected the early compressive strength of the cement paste.
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DOI
高影响因子
危险品化学品经营许可证（带存储）