ACS Catalysis
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2024
·
IF 11.3
Decun Luo,Chun-Ran Chang,Zhun Hu
In this study, tetrabutylammonium bromide (TBAB) with a cationic radius of 4.94 Å was encapsulated in ZIF-8 with a pore size of 3.4 Å by a one-step method. The TBAB@ZIF-8 catalyst showed superior catalytic activity on the reaction of CO2 with propylene oxide (PO) than TBAB and the zeolitic imidazolate framework, respectively, showing a synergistic effect. The synergist effect was related with the compensation effect between the adsorption of CO2 and the loop-opening of PO, where ZIF-8 provided the active sites for CO2 adsorption and Br– in TBAB promoted the opening of the loop of PO. The catalytic performance of TBAB@ZIF-8 illustrated a volcano curve with the increase of the TBAB content. The addition of TBAB could have resulted in a positive effect on the loop-opening of PO. However, excessive TBAB hindered mass transfer and reduced the CO2 adsorption of ZIF-8, which was certified by the CO2 adsorption test. Diffuse reflectance infrared Fourier transform spectroscopy results showed that TBAB@ZIF-8 catalysts proceed in a new reaction pathway and that the rate-determining step of the reaction was the opening of the loop of PO. These results provided a guideline for the development of immobilization of homogeneous catalysts for CO2 fixation.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
JOURNAL OF CRYSTAL GROWTH
·
2019
·
IF 1.573
Zheng Li,Dong-Liang Zhong,Wei-Yan Zheng,Jin Yan,Yi-Yu Lu,Da-Tong Yi
This work presents a morphological and kinetic investigation of tetra- n -butyl ammonium bromide (TBAB) or tetra- n -butyl phosphonium bromide (TBPB) semiclathrate hydrates formed with a CO 2 + CH 4 gas mixture at the stoichiometric concentration (2.57 mol%). A 3-stage procedure was proposed and employed in the experiments. All experiments were performed at 2.8 MPa and a subcooling of 12 K was used as driving force for hydrate nucleation and growth. It was found that the shapes of hydrate crystals formed in TBPB and TBAB solutions were quite different. Besides, the TBPB semiclathrate hydrate grew laterally at gas/liquid interface and quickly covered the interface while the TBAB semiclathrate hydrate initially formed around the gas/liquid interface and then sank to the reactor bottom. As a consequence, gas uptake and the rate of hydrate growth obtained in TBAB solutions were higher than that in TBPB solutions. It was also found that CO 2 content in hydrate phase, CO 2 recovery, and separation factor obtained in TBAB solutions were higher than those obtained in TBPB solutions. Therefore, TBAB semiclathrate hydrate formed at the stoichiometric concentration and quiescent conditions will be a promising approach to improve the hydrate based CO 2 separation from the CO 2 + CH 4 gas mixture.
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
ENERGY
·
2022
·
IF 8.857
Xiaoya Zang,Jing Wang,Yong He,Xuebing Zhou,Deqing Liang
Tetrabutylammonium bromide (TBAB) is a typical thermodynamic additive that can enhance the hydrate equilibrium temperature . Additionally, semi-clathrate hydrates formed from TBAB solutions exhibit reasonable CO 2 adsorption performance. In this study, TBAB hydrates were synthesized to determine their carbon capture capacity from a ternary gas mixture of CH 4 /CO 2 /N 2 (0.5/0.4/0.1). We measured the effect of temperature, pressure, and TBAB mass fractions (0.05–0.2) on the formation of gas hydrates, which were analyzed using Raman spectroscopy, powder X-ray diffraction (PXRD), and cryo-scanning electron microscopy (Cryo-SEM). With a 0.05 TBAB aqueous solution, the maximum recovery factor of CH 4 was 1.646 at 290.1 K and 7.0 MPa, whereas the maximum CO 2 split ratio was 0.454 at a pressure of 7.0 MPa and temperature of 280.1 K. Furthermore, the cryo-SEM images revealed that the addition of TBAB significantly increased the specific surface area of the hydrate crystals compared with the pure water system. PXRD and Raman spectroscopy showed that the hydrate structure transformed from a SI to a semi-clathrate hydrate. The hydrate samples formed from the 0.05 TBAB solution were found to be type A and B, leading to greater gas consumption. These results are expected to provide support for hydrate gas separation technology.
研究领域:
化学工程
·
材料科学
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DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yimao Shen,Zhi Li,Jingtao Hu,Yue Zhang,Tianduo Li,Guangjin Chen
Gas hydrate technology is a new gas storage method developed in recent years and has great application potential. Due to the slow formation kinetics of hydrate and the low actual gas storage density, it is a promising method to prepare the fixed bed filled with wet porous materials to inducing adsorption-hydration coupling effect, so as to improve the gas storage efficiency. In this study, various additives including THF, TBAB and diesel oil were added to the water-bearing activated carbon fixed bed to improve its gas storage capacity. Our experimental results show that the addition of THF or TBAB can significantly promote the gas storage performance of the bed. At the optimum concentration of THF (7.5 wt%), the gas storage density of bed (S b ) and gas storage capacity of hydrate (S w ) were 128.66 V/V b and 194.26 V/V w , which are 2.89 times and 3.07 times higher than those of wet activated carbon fixed bed without additives, respectively. When 5 wt% TBAB was added, the S b and S w were increased by 1.86 times and 1.87 times, respectively. Moreover, using diesel to establish gas channels in the fixed bed to improve the gas mass transfer between the bulk gas phase and the fixed bed can also significantly improve the gas storage performance of the bed. When the oil-carbon ratio (R o ) is 0.5, the S b and S w are 97.97 V/V b and 172.77 V/V w , respectively. However, further increasing the amount of diesel oil will not significantly improve the gas storage density of the bed due to the volume increase of the bed caused by the addition of diesel. When both diesel oil and THF are added to the water-containing fixed bed, the effect will be not significantly better than that of the bed with diesel oil or THF alone because the two accelerators compete with each other. Finally, the gas release and decomposition speed of the water-bearing fixed bed with / without 7.5 wt%THF are investigated. The results show that the final gas recovery of the bed with 7.5 wt% THF could reach 95.01 %, indicating a good application prospect.
研究领域:
化学工程
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能源技术
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DOI
高影响因子
Energies
·
2018
·Vol. 11
·期 2
·399
·
IF 2.676
Rong Li,Xiao-Sen Li,Zhao-Yang Chen,Yu Zhang,Chun-Gang Xu,Zhi-Ming Xia
Tetra-n-butyl ammonium bromide (TBAB) was widely used in the research fields of cold storage and CO2hydrate separation due to its high phase change latent heat and thermodynamic promotion for hydrate formation. Agglomeration always occurred in the process of TBAB hydrate generation, which led to the blockage in the pipeline and the separation apparatus. In this work, we screened out a kind of anti-agglomerant that can effectively solve the problem of TBAB hydrate agglomeration. The anti-agglomerant (AA) is composed of 90% cocamidopropyl dimethylamine and 10% glycerol, which can keep TBAB hydrate of 19.3–29.0 wt. % in a stable state of slurry over 72 h. The microscopic observation of the morphology of the TBAB hydrate particles showed that the addition of AA can greatly reduce the size of the TBAB hydrate particles. CO2gas separation experiments found that the addition of AA led to great improvement on gas storage capacity, CO2split fraction and separation factor, due to the increasing of contact area between gas phase and hydrate particles. The CO2split fraction and separation factor with AA addition reached up to 70.3% and 42.8%, respectively.Keywords:CO2separation;TBAB;IGCC;anti-agglomerant;micromorphology;hydrate
研究领域:
化学工程
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环境科学
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材料科学
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DOI
高影响因子
Processes
·
2024
·Vol. 12
·期 11
·2315
·
IF 2.8
Yang Ge,Haihong Chen,Rui Qin,Haiyuan Yao,Ting Huang,Xin Lv,Huiyong Liang,Shi Shen
During marine oil–gas extraction, significant amounts of carbon dioxide (CO2) gas are often produced. Effectively separating these associated CO2gases during extraction has become a critical technical challenge. Therefore, this paper aims to enhance the efficiency of CO2hydrate-based capture technology and conduct relevant research. The goal is to increase the driving force for hydrate formation by combining the traditional thermodynamic additive TBAB with pressure modulation and to improve the hydrate formation rate through the use of multiple kinetic promoters. This paper presents the initial investigation into the effect of the thermodynamic accelerator tetrabutylammonium bromide (TBAB) on the characteristics of CO2hydrate formation. The promotion effects of TBAB solutions with varying mass concentrations (3%, 5%, 7.5%, 10%) and reaction pressures (3 MPa, 4 MPa) were subjected to a systematic analysis, and the optimal conditions were identified as 4 MPa and a 5 wt% TBAB concentration. Subsequently, the impact of combining TBAB with kinetic promoters (SDS, nano Al2O3, L-methionine, L-leucine) on CO2hydrate generation characteristics was further investigated. In this paper, the effect of a single promoter on the generation characteristics of CO2hydrate was investigated, and the efficient carbon trapping ability of the complex promoter was verified, which provides theoretical support for the application of CO2trapping technology using the hydrate method.
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
Petroleum Science
·
2023
·
IF 5.6
Xingxun Li,Ming Liu,Qingping Li,Weixin Pang,Guangjin Chen,Changyu Sun
The natural gas hydrate has become one of the most promising future green energy sources on the earth. The natural gas hydrates mostly exist in the sediments with porous structure, so a solid understanding of the hydrate formation and growth processes in the porous medium is of significance for the exploitation of natural gas hydrate. The micro-packed bed device is one of the efficient microfluidic devices in the engineering field, but it has been rarely used for the hydrate-based research. In this study, a transparent micro-packed bed device filled with glass beads was developed to mimic the porous condition of sediments, and used to in-situ visualize the hydrate formation and growth habits in the pore spaces under both static and dynamic conditions. For the static experiment, two types of hydrate growth patterns in porous medium were observed and identified in the micro-packed bed device, which were the grain-coating growth and pore-filling growth. For the dynamic condition, the hydrate formation, growth, distribution habits and hydrate blockage phenomena in the pore spaces were in-situ visually captured. The impacts of flowrate and subcooling on the pressure variation of the micro-packed bed and the duration of the hydrate growth under dynamic flow condition in pores were in-situ monitored and analyzed. The higher flowrate could result in the faster hydrate growth and more severe blockage in pores, but the effect of subcooling condition might be less significant at the high flowrate.
研究领域:
能源工程
·
水合物科学
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微流控技术
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多孔介质流动
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天然气水合物
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2018
·
IF 1.712
Yaling Luo,Changjun Liu,Hairong Yue,Siyang Tang,Yingming Zhu,Bin Liang
The selective oxidation of cyclopentene by aqueous H 2 O 2 using H 3 PW 12 O 40 and tetrabutyl ammonium bromide (TBAB) as a phase transfer catalyst has been investigated. The results show that the presence of TBAB significantly improved the oxidation selectivity of cyclopentene. The effects of the reaction conditions on the conversion of cyclopentene were investigated in detail. The optimal reaction conditions are as follows: the H 3 PW 12 O 40 to TBAB molar ratio, 1:1–1:3; H 3 PW 12 O 40 to cyclopentene molar ratio, 0.54:100–0.64:100; and molar ratio of H 2 O 2 to cyclopentene, 1.6:1. The conversion reached to 59.8% in 4 h at 35.0 °C, while the selectivity of glutaraldehyde was 38.0% and the selectivity of 1,2-cyclopentanediol was 55.6%. In addition, a route for oxidation of cyclopentene by aqueous H 2 O 2 using a heteropoly acid and quaternary ammonium salt as a phase transfer catalyst was proposed.
研究领域:
化学工程
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催化化学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 46
·22143-22150
·
IF 3.925
Yanwen Guo,Xingjian Liu,Bing Hu
A novel supported deep eutectic solvent (DES) TBAB/PEG-200 was prepared by loading DES TBAB/PEG-200 onto mesoporous silica by the sol–gel method. The properties of the supported deep eutectic solvent TBAB/PEG-200 were characterized by FT-IR, XRD, SEM, BET analysis, and TG. The adsorption oxidation desulfurization system was studied using environmentally friendly H2O2 as an oxidant and typical heterocyclic sulfide dibenzothiophene (DBT) was dissolved in n-octane as a simulated oil. After the optimization of preset experimental parameters, the DBT content in the simulated oil could be removed deeply and effectively under the optimal reaction conditions m(25%-DES/SiO2) = 0.20 g, T = 60 °C, O/S = 14, t = 60 min. The catalyst was reused more than 9 times with no significant decrease in the desulfurization rate. Finally, the possible adsorption oxidative desulfurization mechanism was proposed.
研究领域:
材料科学
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环境工程
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催化化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
·
2026
·
IF 6.6
Zhen Xu,Zheng Liu,Lina Meng,Yuan Lu,Feng Chen,Yiwei Wang,Qiang Sun,Xuqiang Guo
The semi-clathrate hydrate of tetrabutylammonium bromide (TBAB) is a promising phase change material for high-density cold energy storage. However, its disordered adhesion on heat exchange surfaces remains an unresolved challenge. This study explores the coupled impact dynamics and hydrate phase change of TBAB solution droplets on metallic surfaces with varying wettability. A multi-field coupled experimental apparatus was established, utilizing high-speed imaging, infrared thermometry, and a PSO-based Young-Laplace fitting algorithm. The results indicate that the classical model underestimates the maximum spreading factor (
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产品关联
DOI
高影响因子
Environmental Progress & Sustainable Energy
·
2025
·
IF 2.3
Zhengxiong Jiang,Zhitao Han
With the aim to develop wet denitration process for marine application, it is still challenging to simultaneously achieve high-efficiency NO x removal from flue gas and low nitrate concentration in scrubbed solution. Herein a novel two-step method was proposed to solve this issue: phosphate buffer solution (PBS) with organic additive was used to absorb NO x efficiently from flue gas, and in next step, Na 2 SO 3 as a reductant was added in the scrubbed solution to reduce NO x off-line. Five typical organic additives were chosen to compose with PBS. The tetrabutylammonium bromide and phosphate buffer solution (TBAB/PBS) composite solution exhibited superior NO x absorption performance. Furthermore, the effects of TBAB concentration, NO x oxidation degree, solution pH, temperature and O 2 concentration on NO x absorption performance of TBAB/PBS composite solution were investigated systematically, and a high NO x absorption efficiency of >90% could be achieved. It was mainly attributed to a physical complex between PBS and NO 2 , N O 3 − $$ N{O}_3^{-} $$ , N O 2 − $$ N{O}_2^{-} $$ , together with a mass transfer enhancement by TBAB. A long-run test showed that nitrate concentration was much lower than the limit value of IMO. Cyclic absorption and regeneration tests confirmed that Na 2 SO 3 could effectively regenerate the scrubbed solution in the absence of O 2 .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaoya Zang,He Li,Yubao Zhang,Yong Chen,Yong He,Nengyou Wu,Xuebing Zhou,Deqing Liang
To enhance the CO 2 separation efficiency of hydrate-based gas separation (HBGS) technology, the kinetic process of hydrate formation from synthesized CH 4 /CO 2 /N 2 gas mixtures in the presence of cyclopentane (CP) and tetra-n-butyl ammonium bromide (TBAB) and gas separation efficiency were studied at an initial pressure of 7.0 MPa and temperatures ranging from 275.1 to 290.1 K. The crystallographic properties of the mixed hydrates were also evaluated by Raman, powder X-ray diffraction(XRD) and cryo-scanning electron microscop(cryo-SEM). Results showed that the combination of CP and TBAB tended to inhibit the separation efficiency compared with pure CP. The maximum CH 4 recovery was 1.37 and the CO 2 split ratio was 0.791 when using CP and TBAB solution. The order of CO 2 split ratio in the different systems followed the order SDS > CP > TBAB/CP > CP/SDS > TBAB. Meanwhile, the adsorption capacity and gas consumption also decreased with an increase in TBAB concentration. Raman and XRD tests revealed that sI, sII, and semi-clathrate hydrates were found to coexist after hydrate formation and no other types of hydrates was formed. CH 4 could only enter the small cages (5 12 ) of the hydrate. SEM images showed that the hydrate crystals were ellipsoid-shaped with different sizes and stacked together to form a globular structure, suggesting that the specific surface area of the hydrate crystals enhanced with the increasing of TBAB concentration. These findings can be used to evaluate the feasibility of applying TBAB and CP in HBGS technology.
研究领域:
化学工程
·
环境科学
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DOI
高影响因子
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