ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
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IF 6.653
Lidong Wang,Yifeng Zhang,Rujie Wang,Qiangwei Li,Shihan Zhang,Meng Li,Jie Liu,Bo Chen
A novel phase splitter, namely, sulfolane, was proposed to advance the traditional monoethanolamine (MEA) absorption technology for CO2 capture by simultaneously promoting the absorption rate and lowering heat duty. The phase-splitting phenomenon was observed after the CO2 loading level had exceeded 0.73 mol CO2/L, thereby generating a CO2-rich MEA upper layer and a lower layer containing sulfolane. Sulfolane facilitated CO2 absorption because of its strong affinity with acid gases, which resulted in an absorption rate 2.7 times higher than that of the conventional MEA process. The process simulation using Aspen Plus indicated that the regeneration heat with the MEA/sulfolane mixture as a solvent substantially decreased to 2.67 GJ/t-CO2, which was 31% lower than that of the conventional MEA process (3.85 GJ/t-CO2). Moreover, the sensible heat and vaporization heat of MEA/sulfolane were markedly decreased by 62.4% and 47.9%, which could be ascribed to the decreased stripping volume and relatively high CO2 partial pressure caused by liquid–liquid phase separation. The proposed system is proved to be a promising candidate for the advancement of CO2 capture techniques with high CO2 absorption capacity, rapid absorption rate, and low-energy penalty.
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高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 3
·589-596
·
IF 9.405
Ying Wang,Jingjing Zhang,Qingli Qian,Bernard Baffour Asare Bediako,Meng Cui,Guanying Yang,Jiang Yan,Buxing Han
CO2 transformation is an important topic in green chemistry, and methanol homologation using CO2 is a promising route to produce ethanol. In this work, we studied this reaction using different homogeneous catalytic systems. It was found that a [RuCl2(CO)3]2/Co4(CO)12 bimetallic catalyst using LiI as a promoter and N-ethyl-2-pyrrolidone (NEP) as the solvent was very effective under mild conditions. The reaction could proceed efficiently at 160 °C, which is much lower than that reported before. The turnover frequency (TOF) of ethanol based on Ru was as high as 7.5 h−1 and the selectivity of ethanol in total products could reach 65.0 C-mol%, which are obviously higher than those reported in the literature. Ethanol was synthesized through cascade catalysis of a reverse water gas shift (RWGS) reaction and methanol homologation with syngas (CO/H2). The outstanding performance of the catalytic system originated from the excellent cooperation of the components. The catalyst could be reused at least five times without any obvious decrease of the catalytic performance. The effect of the solvent on this reaction was studied systematically. The mechanism was also discussed based on isotope labeling tests.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
IF 11.698
Weiyi Chen,Bin Han,Chen Tian,Xueming Liu,Shujie Liang,Hong Deng,Zhang Lin
Reducing carbon dioxide (CO 2 ) to various value-added chemical products by photocatalysis could effectively alleviate the serious problems of global warming and energy shortages. Currently, most commonly prepared photocatalysts present poor performance under visible light irradiation. In this study, we adopted a facile, scalable and controllable approach to prepare ultrathin two-dimensional (2D) porous Co 3 O 4 catalysts (Co 3 O 4 -NS) by air calcining of the ultrathin metal-organic framework (MOFs) nanosheet templates to validly reduce CO 2 with a Ru-based photosensitizer under visible light irradiation. Benefitting from the structural nature of MOFs precursors, the calcined Co 3 O 4 -NS inherit the morphology of 2D and well-developed porosity, which support the transport of electrons, enhance the adsorption of CO 2 molecules, and render abundant catalytic sites for CO 2 activation. As a result, the CO generation rate is approximately 4.52 μmol·h −1 with selectivity of 70.1%, which is superior to the Co 3 O 4 bulk catalysts (Co 3 O 4 -BK). Additionally, density functional theory (DFT) calculations reveal that the model of Co 3 O 4 monolayer has stronger CO 2 adsorption energy than that of the Co 3 O 4 bulk, which is beneficial for the CO 2 -to-CO conversion. This MOF-engaged strategy provides new insight into the controlled synthesis of advanced ultrathin holey nanosheets to improve the efficiency of photocatalytic CO 2 reduction.
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Journal of CO2 Utilization
·
2018
·
IF 5.503
Xu Jiang,Faliang Gou,Chenze Qi
A series of C 2 v -symmetric diphenylporphyrin complexes containing a metal ion (Mg, Al, Mn, Fe, Co, Zn) have been synthesized and applied as catalysts for the solvent-free cycloaddition of epoxides and carbon dioxide under atmospheric pressure and mild temperature, in concert with phenyltrimethylammonium tribromide (PTAT) as a co-catalyst. The activity of these catalysts deeply relies on their coordinated metal species. [5,15-Diphenylporphyrin]manganese(III) chloride ( DPP-MnCl ) has been found to be the most effective catalyst under optimal reaction conditions. It's worth mentioning that the cycloaddition of phenyl glycidyl ether (GPE) and CO 2 proceeded successfully by DPP-MnCl /PTAT even at 25 °C and atmospheric pressure. Moreover, preliminary kinetic investigations of this cycloaddition were carried out by using catalysts DPP-MnCl , DPP-CoCl and DPP-Zn , revealing that the (phenoxymethyl)ethylene carbonate (PEC) formation with the lowest activation energy is catalyzed by DPP-MnCl . Furthermore, a Lewis acid-base dual cooperative catalytic mechanism has been carefully proposed in light of the catalyst systems and the experimental results.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Zihan Qu,Hong Wu,Yue Zhou,Leixin Yang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Ning Zhang,Yutao Liu,Zhongyi Jiang
Membranes with fast CO 2 transport pathways have attracted intense attention due to their outstanding CO 2 permeability, showing potential for industrial application. Regulating the spatial distribution of CO 2 -philic groups in polymer-based membranes is expected to be a promising strategy to achieve the fast CO 2 transport pathways. In membrane matrix, the interconnected network of concentrated domains of CO 2 facilitated transport groups provides membranes with specific CO 2 transport pathways and finally leads to their high separation performance. In this study, a novel kind of polyelectrolyte membrane, quaternary ammonium polysulfone with interconnected ionic clusters, is prepared to enhance the CO 2 permeability. The hydrophilic quaternary ammonium groups tend to aggregate spontaneously to create ionic clusters. Furthermore, under humidified conditions, these ionic clusters are connected by water to form an ionic cluster network in the membrane matrix. The ionic cluster network plays the crucial role in accelerating the selective transport for CO 2 molecules over CH 4 by the reversible interaction between CO 2 and ion pairs. By tuning the quaternization degree of polysulfone, a series of polyelectrolyte membranes with different size of ionic clusters were developed. Membranes with hydrated ionic clusters (5–9 nm) show dramatic enhancement in CO 2 separation performance, especially in CO 2 permeability. The as-prepared quaternary ammonium polysulfone membrane with 8.98 nm ionic clusters exhibited the high CO 2 permeability of 1109.44 Barrer and a high CO 2 /CH 4 selectivity of 29.70, which exceeds 2008 Robeson upper bound limit. The optimized separation performance of QA-PSf membranes is attractive for potential application such as CO 2 capture from flue gas and natural gas.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 15
·4152-4158
·
IF 9.405
Bernard Baffour Asare Bediako,Qingli Qian,Jingjing Zhang,Ying Wang,Xiaojun Shen,Jinbiao Shi,Meng Cui,Guanying Yang,Zhen Wang,Shengrui Tong,Buxing Han
Synthesis of ethanol from cheap and renewable CO2 is of great importance, but is still a challenge. Because it involves CO2 hydrogenation with simultaneous C–C bond formation, and the synergy of two or more transition metals is usually required for catalyzing the reaction effectively. Moreover, higher temperature is needed to drive the reaction. In this work, we found that the monometallic Ru3(CO)12 catalyst could efficiently catalyze the synthesis of ethanol from CO2, methanol and H2 in the ionic liquid, 1-butyl-3-methylimidazolium chloride ([bmim]Cl), using LiCl and LiI as promoters. Ethanol could form at 120 °C, which is among the lowest temperatures reported to date. A detailed study indicated that ionic liquids play an important role in monometallic catalysis. High ethanol selectivity and activity were obtained under optimized conditions. In addition, the catalyst could be easily recycled and the TON of ethanol reached 180 after five cycles. To our knowledge, this is the first time that an ionic liquid has been used as a reaction medium to produce ethanol using CO2 and H2.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2019
·
IF 6.97
Sachin Mane,Yu-Xia Li,Xiao-Qin Liu,Lin-Bing Sun
The use of porous carbons for selective CO2 separation attracts increasing attention. Owing to low thermostability of porous polymers, low yield is the major concern of porous carbons. To obtain porous carbons with high yield, the development of thermostable porous polymers is highly expected. Herein, high yielded (70% for 700 °C and 64% for 800 °C) Sn-doped porous carbons (SnPCs) have been constructed through KOH-assisted carbonization of Sn-containing polymer. Notably, SnPC-700 (218.5 mg·g–1) demonstrates higher CO2 adsorption capacity than the reference sample prepared without KOH, SnPC-700r (188.3 mg·g–1), indicating the importance of KOH-assisted activation. Carbonization temperature has an effect on the adsorption capacity of resultant materials, and high carbonization temperature leads to better adsorption capacity on CO2. SnPC-800 is able to capture 242.8 mg·g–1 of CO2, which is better than some benchmarks including BILP-7 (193.0 mg·g–1), PAF-1–450 (196.4 mg·g–1), and FCTF-1 (205.5 mg·g–1). More importantly, SnPC-800 demonstrates good selectivity of CO2 over CH4 (31.1). Thus, high yield and good performance upon CO2 adsorption capacity and selectivity over CH4 make SnPCs attractive candidates for the removal of CO2 from natural gas.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Zihao Yang,Wei Wu,Zhaoxia Dong,Meiqin Lin,Shuwei Zhang,Juan Zhang
The establishment of a miscible phase between CO 2 and crude oil can significantly improve CO 2 flooding efficiency. However, the minimum miscibility pressure (MMP) between CO 2 and crude oil is usually higher than the fracture pressure of the formation, how to reduce the MMP between CO 2 and crude oil is very important, and there are fewer related studies. Our inspiration for reducing MMP comes from the unique dispersion characteristics of CO 2 in alcohol, the intermolecular force of crude oil may decrease due to the existence of alcohols. In this paper, the CO 2 solubility and the oil volume expansion with adding a variety of alcohols (1-butanol, 1-pentanol and 1-hexanol) were measured by a visible high temperature and high pressure cell from 7 MPa to 20 MPa at 343.15 K. The MMP between CO 2 and crude oil is predicted by measuring the interfacial tension (IFT) between CO 2 and crude oil from 2 MPa to 43.3 MPa at 343.15 K. The results showed that the CO 2 solubility in crude oil and the oil volume expansion were greatly improved due to the addition of alcohols. Especially 1-butanol, 1-pentanol and 1-hexanol were mixed by 8:1:1(volume ratio), 5% (volume ratio) alcohols mixture was added to the crude oil, the CO 2 solubility in crude oil increased by 28.74% at 345.15 K and 19 MPa, and the volume expansion coefficient of crude oil also increased by 4.45% at 345.15 K and 14 MPa. It is encouraging to note that the MMP between CO 2 and crude oil decreases by 9.21% after adding 5% alcohols mixture into crude oil. This article is able to provide a new technique for reducing the MMP between CO 2 and crude oil in the field of enhanced oil recovery.
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高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2019
·
IF 3.073
Suresh Mutyala,Madhavi Jonnalagadda,Harisekhar Mitta,Raveendra Gundeboyina
MIL-101 (Cr) was synthesized by a hydrothermal method and used as support to prepare a series of polyethylenimine (PEI) incorporated MIL-101 (Cr) by wet impregnation method. All characterization results revealed that the structure of MIL-101 (Cr) was well-maintained by the incorporation of polyethylenimine and confirmed the presence of PEI within MIL-101 (Cr). The CO 2 adsorption studies were carried out in a fixed bed reactor from 30 to 90 °C, 1 bar. The adsorption of CO 2 has been increased by the incorporation of PEI. It was due to the chemical interaction between the NH 2 and CO 2 groups to form a carbamate. The high CO 2 adsorption capacity 3.81 mmol g −1 was shown by 70 wt% PEI loaded MIL-101 (Cr) at 75 °C, 1 bar, because of more number of NH 2 groups and a high number of CO 2 molecules diffusion. Its adsorption capacity was 4.7 times higher than the adsorption capacity of MIL-101 (Cr) (0.80 mmol g −1 ). Moreover, in moisture condition, CO 2 adsorption capacity was increased to 4.4 mmol g −1 by the formation of ammonium bicarbonate and showed good adsorption stability throughout each adsorption-desorption cycle. The Avrami adsorption kinetic model was well fitted with experimental breakthrough CO 2 adsorption data of MIL-101 (Cr)-PEI-70. It suggested that the adsorption of CO 2 on PEI incorporated material was chemical adsorption.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Liying An,Shenfang Liu,Linlin Wang,Jiayi Wu,Zhenzhen Wu,Changdan Ma,Qiankun Yu,Xin Hu
In this work, graphene-derived N-enriched porous carbons were synthesized by urea modification and KOH activation of thermally shocked graphene oxide. The prepared sorbents were characterized by various techniques and investigated as potential CO2 capture materials. The as-prepared sorbents possess high CO2 adsorption capacity of 2.40 mmol/g (25 °C) and 3.24 mmol/g (0 °C) at 1 bar, which is higher than most graphene-based carbons reported previously. The nitrogen incorporation and narrow microporosity are the two major factors that determine CO2 uptake for these graphene-derived carbonaceous adsorbents under ambient conditions. The adsorption kinetic data of the optimized sample were well-described by the classical Fick’s diffusion model with a high CO2 diffusion rate. The fast CO2 adsorption kinetics can be attributed to the short diffusion paths of this sample, which is composed of thin layers of graphene sheets. Moreover, these graphene-derived sorbents also demonstrate excellent stability and recyclability, high selectivity of CO2 over N2, suitable heat of adsorption, and excellent dynamic CO2 capture capacity. As a result, these graphene-derived porous carbons deserve consideration for removal of CO2 from exhausted flue gas.
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JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Jinhui Zhang,Qingping Xin,Xu Li,Mingya Yun,Rui Xu,Shaofei Wang,Yifan Li,Ligang Lin,Xiaoli Ding,Hui Ye,Yuzhong Zhang
Mixed matrix membranes (MMMs) are challenged by the non-ideal interfacial morphologies that leads to the weakened gas separation performances and mechanical strength . Filler surface modification with organosilanes is an effective approach to build the linkage between polymer and the fillers. In this study, we fabricated MMMs by introducing aminosilane functionalized graphene oxide (f-GO) nanosheets into Pebax ® 1657 matrix. The introduction of f-GO decreased the crystallinity and increased chain mobility of Pebax matrix. Benefiting from the improved filler dispersion, semi-interpenetrated Pebax chains in the Si-O-Si network at the interface, and the high intrinsic mechanical strength of GO, the MMMs exhibit a 1.7-times higher Young's modulus and 1.1-times higher break strength. The amino groups on GO help to construct a facilitated transport pathway along the polymer-filler interface. With greatly improved CO 2 separation performances in dry state, the membranes exhibited even higher performances in humidified state. Particularly, Pebax/f-GO-0.9% membrane showed a high CO 2 permeability of 934.3 Barrer, and a CO 2 /CH 4 selectivity of 40.9, a CO 2 /N 2 selectivity of 71.1, surpassing the Robeson upper bound and quite promising for carbon capture.
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高影响因子
Small
·
2019
·Vol. 15
·期 17
·1900289
·
IF 10.856
Hao Dong,Lei Zhang,Lulu Li,Wanyu Deng,Congling Hu,Zhi-Jian Zhao,Jinlong Gong
The electroreduction of CO 2 to CO provides a potential way to solve the environmental problems caused by excess fossil fuel utilization. Loading transition metals on metal oxides is an efficient strategy for CO 2 electroreduction as well as for reducing metal usage. However, it needs a great potential to overcome the energy barrier to increase CO selectivity. This paper describes how 8.7 wt% gold nanoparticles (NPs) loaded on CeO x nanosheets (NSs) with high Ce 3+ concentration effectively decrease the overpotential for CO 2 electroreduction. The 3.6 nm gold NPs on CeO x NSs containing 47.3% Ce 3+ achieve CO faradaic efficiency of 90.1% at −0.5 V in 0.1 m KHCO 3 solution. Furthermore, the CO 2 electroreduction activity shows a strong relationship with the fractions of Ce 3+ on Au-CeO x NSs, which has never been reported. In situ surface-enhanced infrared absorption spectroscopy shows that Au-CeO x NSs with high Ce 3+ concentration promote CO 2 activation and *COOH formation. Theoretical calculations also indicate that the improved performance is attributed to the enhanced *COOH formation on Au-CeO x NSs with high Ce 3+ fraction.
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高影响因子
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