ENERGY & FUELS
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2015
·
IF 2.79
Hongyan Tang,Yi Zhang,Feng Wang,Huapeng Zhang,Yuhai Guo
Membrane wetting is the main obstacle for carbon dioxide (CO2) capture on long-term operation. In order to understand wetting, polytetrafluoroethylene (PTFE) hollow fiber membranes were fabricated through paste extrusion, stretching, and sintering processes. CO2 capture performance over 180 days was performed. It indicates no obvious deterioration of CO2 flux over 180 days. Subsequently, further investigation was performed through immersion of PTFE hollow fiber membranes in different absorbent solutions. Results of Fourier transform infrared (FTIR) spectroscopy, energy-dispersive spectroscopy (EDS), and variations of membrane weight showed the PTFE polymer kept good stability in the absorbent solutions over 24 weeks. Scanning electron microscopy (SEM) images indicated the pore sizes of the PTFE hollow fiber membranes did not markedly enlarge during immersion, which was proved by pore size distributions. Contact angle measurements indicated no obvious reduction (8° reduction) in the membrane hydrophobicity over 24 weeks. Values of the contact angle relied on the surface tension values of the absorbent solutions. AFM images showed that immersion imposed a negative influence on the roughness values, which was the same order as the contact angle. The results suggested that none of the absorbent molecules entered the interior of the PTFE polymer. PTFE hollow fiber membranes may be a promising alternative for CO2 capture on long-term operation.
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CATALYSIS TODAY
·
2015
·
IF 3.893
Xiao-Fang Liu,Qing-Wen Song,Shuai Zhang,Liang-Nian He
Carboxyl-containing organocatalysts, e.g. EDTA (ethylenediaminetetraacetic acid) in combination with nucleophilic halide such as n Bu 4 NBr were demonstrated to be efficient catalyst systems for the synthesis of cyclic carbonates from CO 2 and a broad range of epoxides in excellent yield and selectivity. Thanks to synergistic effects of carboxylic groups and bromide anion, the cycloaddition reaction proceeded smoothly at 5 bar CO 2 under mild reaction conditions. Interaction of carboxylic groups in EDTA with the epoxide via hydrogen bonding presumably facilitates the ring-opening of the epoxide by the nucleophile e.g. bromide. In particular, multiple carboxylic groups in one molecule i.e. EDTA could more effectively activate the epoxide and stabilize the alkoxide intermediate through multi-site hydrogen bonding in comparison with monocarboxylic acid. Moreover, the carboxylic acid like EDTA used in this study represents a cheap, commercially available, environmentally benign, metal-free catalyst for CO 2 conversion. Thus, this catalytic protocol could have potential application for catalytic fixation of CO 2 into value-added chemicals.
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Journal of CO2 Utilization
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2014
·
IF 0
Qingzhao Shi,Lishuai Jing,Weihong Qiao
Poor solubility of heavy hydrocarbons in CO 2 has limited the application of CO 2 -EOR (enhanced oil recovery) in modern oil recovery industry to some extent. Therefore, it is crucial to investigate the solubility regularity of different hydrocarbons in supercritical carbon dioxide (scCO 2 ) in the first place. In this paper, our objective is to explore the solubility of n -alkanes (C 6 H 14 –C 18 H 38 ) in scCO 2 . To measure cloud point pressures, the experiment utilizes high-pressure view chamber, and results for accuracy and repeatability of the experimental method and instrument are evidently positive. Then, cloud point pressures for n -alkanes from 318 K to 343 K show a proximately linear and positive correlation with the temperature; they also increase with expanding chain length of n -alkanes. In addition, the result of x (molar fraction of n -alkane at cloud point pressure) indicates that x has a positive correlation with the pressure at identical temperature, and when pressure is constant, temperature increase will reduce x . Finally, relationship studies between density of CO 2 and x reveal that, density of CO 2 has a positive influence on the solubility of n -alkane, and the Chrastil model corrects ln ρ and ln S data. The measured data align with the Chrastil model, with a maximum AARD value of 9.85%.
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JOURNAL OF MEMBRANE SCIENCE
·
2015
·
IF 5.056
Xueqin Li,Zhongyi Jiang,Yingzhen Wu,Haiyang Zhang,Youdong Cheng,Ruili Guo,Hong Wu
Composite membranes were fabricated by incorporating carboxylic acid nanogels (CANs) into a Pebax MH 1657 matrix for potential applications in CO 2 /CH 4 (or N 2 ) separation. CANs were synthesized by precipitation polymerization of N-isopropylacrylamide (NIPAM), acrylic acid (AA) monomer and N,N′-methylenebisacrylamide (BIS) crosslinker. The incorporation of CANs simultaneously tailored favorable water environment and increased CO 2 transport sites within the membranes. With increasing CANs loading, the homogeneously dispersed CANs in the Pebax matrix offered more favorable water environment and the additional carboxyl group sites for efficient CO 2 transport, thus constructing interconnected preferential CO 2 transport passageways. The Pebax-CANs-30 composite membrane exhibited the highest gas separation performance, with the CO 2 /CH 4 and CO 2 /N 2 selectivities of 33 and 85 respectively, and a CO 2 permeability of 2026 Barrer (1 Barrer=10 −10 cm 3 (STP) cm/(cm 2 s cmHg), well surpassing the Robeson's upper bound limit reported in 2008. This effort will give rise to a new option to tailor water environment and increase CO 2 transport sites for fabricating high-performance CO 2 separation membranes .
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2015
·Vol. 17
·期 15
·10080-10085
·
IF 4.493
Zhaoming Liu,Yadong Hu,Hongqing Zhao,Yang Wang,Xurong Xu,Haihua Pan,Ruikang Tang
Living organisms such as corals can carry out CO2 looping efficiently via biomineralization under ambient conditions. Inspired by this natural process, we establish a solution system of calcium acetate–ethanol–water (Ca(Ac)2–C2H5OH–H2O) for CO2 chemical looping at constant room temperature. The CO2 capture is achieved by its reaction with Ca(Ac)2 to form calcium carbonate (CaCO3) mineral and HAc in the binary solvent with a high C2H5OH content. However, an increase in the H2O content in the system triggers acetic acid (HAc)-induced CaCO3 dissolution to release CO2. The system can be recovered for CO2 capture readily by the replenishment of C2H5OH. This biomimetic mineralization-based CO2 capture/release is controlled by the ionization states of the electrolytes, and is precisely regulated in the C2H5OH–H2O binary solvent. Our attempt highlights the fundamental principle of solution chemistry in reaction control and provides a bioinspired strategy for CO2 capture/release with very low cost and easy availability.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2014
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IF 2.063
Yan Cao,Yunxia Zhao,Zijian Lv,Fujiao Song,Qin Zhong
New composites of UiO-66 and graphene oxide (GO) were synthesized and tested as CO 2 adsorbents at room temperature. The materials and the parent composite components were characterized using X-ray diffraction (XRD), thermo-gravimetric analysis (TGA), nitrogen adsorption–desorption isotherm analysis, scanning electron microscopy (SEM), and FT-IR spectroscopy. The CO 2 isotherms on the UiO-66/GO composites and the UiO-66 were measured by a static volumetric method separately. Experiments of multiple adsorption/desorption cycles were conducted to estimate reversibility of CO 2 on the UiO-66/GO. The results showed that the BET surface area of the composites was higher than that of the parent UiO-66, and the adsorption capacities of CO 2 on the composites were greatly higher than that on the UiO-66 sample. The composite UiO-66/GO-5 exhibited the maximum CO 2 uptake of 3.37 mmol/g at 298 K and 1 bar, which increased by 48% in comparison with that of the UiO-66, and was much higher than those of the conventional activated carbons and the zeolites. The CO 2 adsorption capacity was dependent on the BET surface area and the micropore volume of the composites. Finally, the adsorption/desorption cycle experiment revealed that the adsorption performance of UiO-66/GO-5 was fairly stable, without noticeable degradation in the adsorption capacity of CO 2 after 6 cycles. Therefore, this kind of composites has a potential application on CO 2 capture technologies to mitigate global warming.
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Polymer Chemistry
·
2015
·Vol. 6
·期 43
·7580-7585
·
IF 5.52
Shunjie Liu,Yuyang Miao,Lijun Qiao,Yusheng Qin,Xianhong Wang,Xuesi Chen,Fosong Wang
A CO2-based oligo(carbonate-ether) tetraol was synthesized in a controlled manner by immortal copolymerization of carbon dioxide (CO2) and propylene oxide (PO) in the presence of 1,2,4,5-benzenetetracarboxylic acid (btcH4) catalyzed by using a zinc–cobalt double metal cyanide (Zn–Co–DMC) catalyst. The number average molecular weight (Mn) of the tetraol was in a good linear relationship with the molar ratio of PO and btcH4 (PO/btcH4), and hence can be precisely controlled. Besides, the rapid chain transfer in immortal copolymerization afforded the tetraol with a narrow polydispersity index (PDI) of 1.08 at a Mn of 1400 g mol−1. Notably, the weight fraction of the byproduct propylene carbonate (WPC) was reduced to as low as 4.0 wt%, which is the lowest Wpc ever reported for the synthesis of branched polyols. The structure of the oligo(carbonate-ether) tetraol was confirmed, providing new evidence for the effect of the acidity (pKa1 value) of the chain transfer agent (CTA) on the initial catalytic mechanism. The acid only acts as the CTA directly participating in the copolymerization via the chain transfer reaction when its pKa1 value is higher than that of adipic acid (pKa1 = 4.43). However, when its pKa1 value is lower than that of succinic acid (pKa1 = 4.2), it acts as the initiate-transfer agent, which first initiates PO homopolymerization to an oligo-ether polyol, and then the in situ formed polyol acts as a new CTA for the copolymerization.
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ChemNanoMat
·
2017
·Vol. 3
·期 8
·560-568
·
IF 2.937
Xinglong Pan,Jianqiang Zhang,Qingzhong Xue,Xiaofang Li,Degong Ding,Lei Zhu,Tianchao Guo
Graphical As a novel filler , 1 D multi-walled carbon nanotube/graphene oxide nanoribbons (MWCNT@GONRs) with low oxidation degree can enhance the gas-separation performance of mixed matrix membranes (MMMs) due to the synergistic effect of the MWCNTs core and GONRs shell. 1 D multi-walled carbon nanotube/graphene oxide nanoribbon (MWCNT@GONRs) hybrids were prepared using a chemical method as fillers for Pebax-based mixed matrix membranes (MMMs) with excellent CO 2 separation performance. Herein, the GONRs shell provided a selective barrier and large gas adsorption area, which contributed to enhancement of gas selectivity, while MWCNTs core with smooth internal surface acted as a rapid transport channel, which improved the gas permeability. It is found that MMMs with 1 wt % loading showed the highest separation factor (80 for CO 2 /N 2 and 23 for CO 2 /CH 4 ) and high CO 2 permeability, far surpassing the upper bound line. Therefore, the synergistic effect of the MWCNTs core and GONRs shell in MWCNT@GONRs nanohybrids can effectively enhance the gas-separation performance of MMMs at low loading. The unique microstructures, ease of synthesis and low filled loading make MWCNT@GONRs promising candidates in post-combustion and sustainable chemistry.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2017
·
IF 3.615
Xingzhong Guo,Li Ding,Kazuyoshi Kanamori,Kazuki Nakanishi,Hui Yang
A novel CO 2 sorbent was prepared by modifying polyethyleneimine (PEI) on hierarchically porous silica (HPS) monoliths with well-defined macro-mesopores through wet impregnation method. HPS monoliths before and after functionalization were characterized by scanning electron microscopy (SEM), differential thermal analysis/thermogravimetry (DTA/TG), fourier transform infrared spectroscopy (FT-IR) and nitrogen adsorption/desorption analysis (BET), and the CO 2 adsorption-regeneration properties of as-synthesized sorbents were investigated by thermogravimetric analysis (TG). The effects of loaded PEI amount as well as adsorption temperature and CO 2 partial pressure on the CO 2 adsorption performance of the as-prepared sorbents were also studied. The results showed that the porous structure of HPS-PEI sorbents was preserved after functionalization, while the specific surface area and pore volume decreased with increasing amount of amines to some extent. The use of PEI had a remarkable improvement on the CO 2 adsorption capacity. With the increasing amount of PEI loaded, the CO 2 adsorption capacity improved significantly. The highest CO 2 adsorption capacity of 2.44 mmol (g sorbent) −1 was obtained at 75 °C in the CO 2 partial pressure of 100 kPa for the HPS loaded with 60 wt% PEI. Adsorption/desorption cycles indicated that the PEI-modified HPS sorbents had a good stability and regeneration.
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International Journal of Electrochemical Science
·
2024
·
IF 1.3
Wenhui Dong,Xinyuan Sun,Qianqian Niu,Yun Zhu,Baokang Jin
Phenylacetic acid derivatives, including 1-naphthaleneacetic acid, hold crucial applications in various domains. Traditional synthesis methods often involve intricate steps or the use of expensive and polluting heavy metal catalysts. This paper presents an electrochemical approach for efficiently producing valuable compounds like 1-naphthaleneacetic acid and other phenylacetic acid analogs through the reduction of benzyl halides, such as 1-chloromethyl naphthalene, in the presence of CO 2 . At the same time as preparing phenylacetic acid, the resource utilization of CO 2 is realized. Six kinds of carboxy analogs were synthesized by potentiostatic electrolysis of benzyl halides in acetonitrile with CO 2 as a co-reactant and tetraethyl ammonium tetrafluoroborate as an electrolyte. The electrochemical reduction products were confirmed structurally through NMR, mass spectrometry, and other techniques. The Faraday electrolysis efficiencies ranged from 82 % to 94 %, with 72.5–92.9 % conversions. The study delves into the electron transfer mechanism using cyclic voltammetry and in situ FT-IR spectroelectrochemistry. The reduction process on silver electrodes under a CO 2 atmosphere was identified as an irreversible two-electron process, generating a monovalent anion that attacks CO 2 to yield the respective carboxyl analogs.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Lulu Zhao,Huilin Hou,Shuo Wang,Lin Wang,Yang Yang,Chris R. Bowen,Jinguo Wang,Ziyi Liao,Dongjiang Yang,Ruifang Yan,Weiyou Yang
Despite the development of a range of photocatalysts for CO 2 reduction, the practical applications are significantly limited by low conversion efficiencies and their reliance on sacrificial agents, which are rooted in thermodynamic and kinetic challenges related to CO 2 conversion. Here, the engineering of Co single atoms in ultrathin single-crystal BiOCl nanosheets for boosted photocatalytic CO 2 reduction is reported. The engineering of Co atoms modulates the distribution of photogenerated charges at the catalyst surface, controlling key surface reaction dynamics and suppressing surface electron-hole recombination. This modulation also improves light absorption and enhances CO 2 adsorption and activation, leading to more efficient surface reactions. Notably, CO 2 is stably adsorbed onto the (001) face of BiOCl through a Bi-O-C(= O)-Co-O coordination unit, which lowers the activation energy for CO 2 reduction and reduces the formation energy of COOH − intermediates. As a result, the BiOCl photocatalysts achieve a CO formation rate of 183.9 µmol g −1 h −1 , when irradiated with a 300 W Xe lamp without cocatalysts or sacrificial agents. It represents an ≈13-fold increase compared to that of pristine BiOCl, and surpasses most reported Bi-based photocatalysts to date. Current work provides valuable insights into engineering of single atoms for developing advanced CO 2 -reduction photocatalysts.
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LANGMUIR
·
2024
·
IF 3.7
Xinzi Wu,Jiawei Ruan,Lifang Chen,Zhiwen Qi
The development of aqueous absorbents for CO2 capture is significantly important to reduce global industrial gas emissions through high regeneration efficiency and low energy consumption. Herein, we newly designed and prepared a dihydroxylated ionic liquid (IL) bis(2-hydroxyethyl)dimethylammonium 1,2,4-triazole ([N1,1,2OH,2OH][TZ]) for highly efficient CO2 absorption through anion–cation cooperative interactions. A superior capacity of 1.33 mol of CO2 per mol of IL and excellent reversibility have been achieved by the introduction of dihydroxy sites on the ammonium-based Tz IL. 1H and 13C nuclear magnetic resonance, Fourier transform infrared, and quantum chemical calculations demonstrate bihydroxyl-cooperative absorption of CO2 via hydrogen bond interaction between the cation and anion of the IL. The theory calculation shows that IL displays a superlow reactive absorption enthalpy, favorable to the reversible CO2 absorption, which can maintain an initial absorption capacity of 98.5% with the cycle numbers of 100, implying the facile regeneration and superlow energy consumption. Thus, the functionalized ILs toward group cooperative gas absorption and excellent reversibility may open a door to designing new materials for enhancing CO2 absorption and utilization.
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