APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Jun Cheng,Leiqing Hu,Yannan Li,Jianzhong Liu,Junhu Zhou,Kefa Cen
To research effects of CO 2 absorption capacity and type of CO 2 absorbent on the CO 2 separation and free-volume properties of facilitated transport membranes, two types of CO 2 absorbents, namely monoethanolamine (MEA) and ionic liquids (ILs:[P 66614 ][Triz] and [P 66614 ][2-Op]), were adopted. The CO 2 absorption capacities of MEA, [P 66614 ][Triz] and [P 66614 ][2-Op] were about 0.561 mol CO 2 per mol, 0.95 mol CO 2 per mol and 1.60 mol CO 2 per mol, respectively. All mean free-volume hole radiuses of membranes decreased after blending CO 2 absorbents. After polymer membrane blended with two ILs, number of free-volume hole increased, resulting in modest increase of the fractional free volume. Both CO 2 permeability and selectivity increased after blending MEA and ILs. The increasing range of CO 2 permeability corresponded with CO 2 absorption capacity of CO 2 absorbents, and membrane blending with [P 66614 ][2-Op] showed the highest CO 2 permeability of 672.1 Barrers at 25 °C. Pebax/PEGDME membrane blending with MEA obtained the highest CO 2 /H 2 and CO 2 /CH 4 selectivity at 17.8 and 20.5, respectively.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
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2017
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IF 2.991
Lei Bao,Shuyi Fang,Dongdong Hu,Yuan Zong,Ling Zhao,Weikang Yuan,Tao Liu
Several amphiphilic nonfluorinated polymers, poly(vinyl acetate)-block-poly(dimethylaminoethyl methacrylate) (PVAc -b- PDMAEMA) and poly(vinyl acetate- alt -diethyl maleate) (PVDBM) -b- PDMAEMA with different ratios of CO 2 -philic and hydrophilic groups, were synthesized using RAFT/MADIX polymerization and ATRP. Stability measurements revealed that PVDBM 8 -b- PDMAEMA 22 could emulsify 80% CO 2 in H 2 O, with stable CO 2 -in-water (C/W) emulsions observed for more than 48 h under 20.0 MPa at 25 °C, which was 20 times longer than PVAc -b- PDMAEMA did. The optimal degree of polymerization (DP) for CO 2 -philic groups in PVDBM- b -PDMAEMA was 8, because increasing the DP of PVDBM increased the CO 2 -philicity, whereas increased molecular weight limited the miscibility in water. Molecular dynamics simulations were applied to determine the hydrophilic/CO 2 -philic balance (HCB). It was found that enhanced CO 2 -philic tails widened the HCB range, and the optimal range of the HCB was varied with CO 2 -philic tail types. Both experimental and simulation results demonstrated that enhancing the CO 2 -philicty of surfactant tails can improve the stability of C/W emulsions.
研究领域:
材料科学
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化学工程
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高分子化学
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DOI
高影响因子
Energy Technology
·
2021
·Vol. 9
·期 8
·2100205
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IF 3.631
Zipeng Zeng,Aya Gomaa Abdelkader Mohamed,Xiang Zhang,Yaobing Wang
Although metal–N-doped carbons are promising electrocatalysts for CO 2 -to-CO conversion due to their high conversion efficiency and current density, their commercial application is still challenging due to their narrow potential/current range. In general, a wide potential/current electrocatalyst is in high demand for industrial CO 2 electrocatalysis. Controllable strategy to tune N configurations toward pyridinic-enriched metal–N x active sites is attractive. The synergetic effect of the ability of pyridinic N to capture Lewis acidic CO 2 and the characteristics of Ni–N active sites to inhibit the hydrogen evolution reaction (HER) can achieve a wide potential window, which has high practical value. Herein, the well-chosen precursors resulting in a pyridinic-enriched Ni–N x site can selectively catalyze CO 2 toward CO generation in aqueous media with a high Faradaic efficiency (FE) of 100% with an overpotential of 680 mV. Continuous CO FE > 90% was recorded under a wide range of potentials without decay. Motivated by its practical characteristics in CO 2 electrocatalysts, a Zn–CO 2 battery is assembled achieving a CO 2 –CO conversion efficiency of more than 90% in a wide discharge current window. Therefore, the results highlight that pyridinic-enriched Ni–N x holds great promise as simultaneous CO-selective electrocatalyst by suitably tuning M–N configurations as new perspective strategy.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
DOI
高影响因子
Soft Matter
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2019
·Vol. 15
·期 30
·6107-6115
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IF 3.399
Ruiqin Wang,Mengxin Zhang,Ying Guan,Mao Chen,Yongjun Zhang
CO2-monitoring plays an important role in medicine, environmental sciences, and food industries. Here, a new CO2-responsive hydrogel film was fabricated from branched polyethyleneimine (BPEI) and partially oxidized dextran (PO-Dex) via layer-by-layer (LBL) assembly, based on the in situ Schiff base reaction between the two polymers. The swelling behaviours of the films were studied using Fabry–Perot fringes on their reflection spectra. Like ordinary hydrogels, the BPEI/PO-Dex films swell in water. In addition, they swell to a larger degree when CO2 is introduced, due to the reaction between CO2 and the amino groups in BPEI. The CO2-induced swelling can be reported by the shift of the Fabry–Perot fringes on their reflection spectra; therefore, the BPEI/PO-Dex film can be used as an optical sensor for dissolved CO2. In the new sensor, the BPEI/PO-Dex film acts as a CO2-sensing material and Fabry–Perot cavity simultaneously. The introduction of ordered structure is no longer required. The response of the sensor to CO2 is linear and reversible. Unlike other hydrogel-based sensors that suffer from a slow response, the new sensor can respond to CO2 quickly, making it applicable for real-time, continuous monitoring of CO2 levels in solution.
研究领域:
材料科学
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环境科学
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医学
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食品工业
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jian Guan,Xiangzeng Wang,Jingcheng Du,Quansheng Liang,Wen He,Ying Liu,Ji Ma,Chunwei Zhang,Jiangtao Liu
Polymers of intrinsic microporosity (PIMs) are promising candidates for carbon dioxide (CO 2 ) separation and capture from flue gas or natural gas. PIM-1, which has excellent gas permeation properties over the Robeson upper bound (1991), has been widely functionalized to further enhance the CO 2 permeability or selectivity. In this work, a simple and readily processive surface modification method has been proposed via hydrolysis of the PIM-1 membrane. The two hydrolysis processes by the acid method, amidation and carboxylation processes, have been conducted to functionalize the surface of PIM-1 membranes forming N A -PIM-1 and C A -PIM-1 membranes. The TGA, FT-IR spectra and NMR results verify that the composition and structure inside the PIM-1 membrane remain unchanged. XPS and NMR spectra demonstrate that the nitrile group at the surface was successfully functionalized with an amine group or carboxyl group. The CO 2 permeability and CO 2 /N 2 selectivity of the N A -PIM-1 membrane both increased to 4593.2 Barrer and 28.5, respectively. Another advantage of N A -PIM-1 membranes is the coordination site from introduced nitrogen atoms with zinc ions to form N A -PIM-1-Zn, which could further react with PEI to introduce amine-rich groups on the surface of the PIM-1 membrane. The CO 2 /N 2 selectivity of the N A -PIM-1-Zn-PEI membrane coated with PEI on the surface increases 45.4% compared to the unmodified PIM-1 membranes, with CO 2 permeability decreasing only 15.5% compared to the unmodified PIM-1 membrane. The N A -PIM-1 and N A -PIM-1-Zn-PEI membranes both surpass the Robeson upper bound (2008) even under mixed gas feeding, suggesting that surface modification of PIM-1 is a promising approach for CO 2 capture from natural gas and flue gas.
研究领域:
材料科学
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环境工程
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 1
·94
·
IF 4
Fuhai Zhang,Jing Xiong,Xiaoxiao Yu,Lei Wang,Tongyu Wu,Zhendong Yu,Minmeng Tang,Haiyan Liu,Yanhong Chao,Wenshuai Zhu
As a promising member of the carbon nitride family, nitrogen-rich g-C3N5has attracted significant attention because of its excellent light absorption performance. Nevertheless, its practical application in photocatalytic CO2reduction is hindered by severe photogenerated charge recombination and limited CO2adsorption capacity. Constructing a heterojunction has emerged as an effective strategy to mitigate charge recombination, thereby enhancing the photocatalytic performance of the catalyst. Herein, a series of CdS/g-C3N5-X heterojunction catalysts were prepared via an in situ hydrothermal approach. The obtained heterojunction catalysts exhibited a novel coral reef-like morphology which facilitated the exposure of additional active sites, thereby enhancing the adsorption and activation of CO2. Moreover, studies have shown that CdS can be anchored to the surface of g-C3N5through C-S bonds, forming a built-in electric field at the interface, which accelerated the separation and transfer of photogenerated charges. Consequently, the resulting heterojunction materials demonstrated high efficiency in photocatalytic CO2reduction with H2O as a sacrificial agent. In particular, CdS/g-C3N5-0.2 exhibited the maximum photocatalytic performance up to 22.9 μmol·g−1·h−1, which was 6 times and 3 times that of unmodified g-C3N5and CdS, respectively. The results indicated that the increased active sites and enhanced charge separation of the Cd/g-C3N5-0.2 catalyst were the primary reasons for its improved photocatalytic CO2reduction performance. This work provides a novel heterojunction-based photocatalyst for efficient CO2photocatalytic reduction, offering insights into the preparation of high-performance photocatalysts for sustainable energy applications.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Qi Gao,Bo Wang,Japan Trivedi,Xingguang Xu,Shuai Liu
CO2-responsive foam (CRF) is a highly promising candidate for CO2-enhanced oil recovery (CO2-EOR) because it displays higher stability than the surfactant-stabilized foam owing to the formation of robust wormlike micelles (WLMs) upon exposure to CO2. In this work, the nanoparticle-enhanced CO2-responsive foam (NECRF) was properly prepared using lauryl ether sulfate sodium (LES)/diethylenetriamine/nano-SiO2, and its interfacial properties and EOR potential were experimentally and numerically assessed, aiming to explore the feasibility and effectiveness of NECRF as a novel CO2-EOR technique. It was found that the interfacial expansion elastic modulus increased 6-fold after CO2 stimulation. The modulus continued to increase with the introduction of nano-SiO2 owing to the pronounced synergistic effect of WLMs and nanoparticles. In addition to increasing the viscosity of the foaming liquid, WLMs and nano-SiO2 enhanced the shearing resistance of the NECRF as well. Calculations demonstrated that both the coarsening rate and the size distribution uniformity coefficient of NECRF were markedly lower than that of the LES foam, which subsequently inhibited NECRF decay and greatly improved its dynamic stability. Besides, molecular dynamics simulation revealed that adding inorganic salts to NECRF could notably enhance the foaming performance due to the intensified hydration of surfactant head groups and reduced binding energy of neighboring molecules. Nuclear magnetic resonance-assisted core flooding experiments validated the exceptional capacity of NECRF to sweep the low-permeability region and improve the conformance profile. Overall, these findings may provide valuable insights into the development and application of novel materials and strategies for the CO2-EOR.
研究领域:
石油工程
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Ji Liu,Yuan-gu Xia,Meng-fan Liu,Bin Hu,Hong-jin Zhang,Ji-hong Li,Zhen-xi Zhang,Qiang Lu
Nitrogen oxides are the major pollutants in solid fuel/waste combustion processes, which can be reduced by unburned or additive chars. The surface char–NO reaction is significantly influenced by CO 2 , whereas the impact mechanism is far from conclusive. Herein, fixed-bed experiments and computational methods were adopted to elucidate the role of CO 2 on char–NO reaction. Experimentally, CO 2 exhibited an inhibitive impact on NO reduction at 873 K but a promotive influence at 1023 K and 1173 K. According to the detection of outlet CO, characterization of char, and density function theory (DFT) calculations, CO and gasified char derived from char–CO 2 gasification are both responsible for the promotive effect at 1173 K, which offers a clear image of the gasification mechanism conjectured in previous work. More importantly, a CO 2 -mediated oxygen rearrangement (CO 2 -MOR) mechanism has been found and confirmed for the first time, which can well explain the experimental results observed at 873 K and 1023 K. The adsorbed CO 2 can intervene in the oxygen rearrangement on the char surface to alter the NO reduction behaviors. The present study offers a comprehensive insight into the roles of CO 2 in the heterogeneous reduction of NO on char surface.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
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IF 4.507
Hailong Li,Mingyu Qu,Yingchao Hu
Li 4 SiO 4 has been demonstrated as a promising adsorbent for CO 2 capture. However, Li 4 SiO 4 adsorbents from the conventional solid-state method usually exhibit dense microstructures and, thus, poor CO 2 capture performance. Treating Li 4 SiO 4 with organic acids has been proved effective to improve the microstructures. The commonly used acids such as acetic acid, citric acid and gluconic acid are too expensive, restricting the application of this modification technique. In addition, in the typical Li 4 SiO 4 -based CO 2 capture looping system, CO 2 usually exists in the desorption reactor. However, the effect of the existence of CO 2 at the desorption stage on adsorption performance has been rarely studied. Focusing on these two issues, this work employed pyroligneous acid (PA), a low-cost by-product of the fast pyrolysis of biomass, to modify the microstructures of Li 4 SiO 4 . It was found that modification by pyroligneous acid (PA) successfully improved the microstructures and enhanced the surface area of Li 4 SiO 4 adsorbent. As a result, the obviously improved CO 2 adsorption performance was achieved. In addition, the test results under CO 2 -containing desorption atmospheres indicated that the existence of CO 2 at the desorption stage decreased the adsorption performance due to the severe sintering caused by the existence of CO 2 at the desorption stage.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
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2022
·
IF 8.321
Ye Qu,Yanglin Chen,Yifei Ye,Ping Xu,Jianmin Sun
Heterogenization of homogeneous catalysts without the loss of activity is still a huge challenge. Herein, homogeneous [HTMG][His][I] amino acid ionic liquid (IL), consisting of 1,1,3,3-tetramethylguanidine cation, histidine anion and iodine anion, were introduced into the pore channels of SBA-15 substrate with the assistance of supercritical CO 2 (scCO 2 ) media. Due to its low viscosity, high diffusivity and absence of surface tension, scCO 2 enabled [HTMG][His][I] to highly disperse in SBA-15 pore channels. Surprisingly, [HTMG][His][I]/SBA-15 heterogeneous catalyst displayed higher CO 2 cycloaddition activity (95% propylene carbonate yield) than equivalent molar pristine [HTMG][His][I] homogeneous catalyst (69% propylene carbonate yield) under the identical conditions. The significantly enhanced activity was resulted from the synergistic effect of [HTMG][His][I] and SBA-15 support. Moreover, [HTMG][His][I]/SBA-15 performed outstanding universality of various epoxides and reusability. This work developed a promising strategy to heterogenization of homogeneous IL catalyst assisted by scCO 2 as synthetic media and provided an efficient catalyst for CO 2 conversion.
研究领域:
化学工程
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催化材料
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Mingjie Cheng,Bo Gao,Xiaoli Zheng,Wenzhuo Wu,Weiqian Kong,Pengfei Yan,Zubin Wang,Bin An,Yunpeng Zhang,Qingchao Li,Qun Xu
Exploring a facile, rapid and efficient route to produce metal-organic frameworks (MOFs) with highly accessible active sites is of great importance for catalysis. Here we demonstrate the CO 2 coordination can drive low temperature rapid synthesis of porphyrin-based bismuth-MOFs (Bi-PMOFs) by utilizing synergistic physical and chemical properties of supercritical CO 2 (SC-Bi-PMOFs). The molecular-level role of scCO 2 in the synthesis of SC-Bi-PMOFs have been investigated through a series of characterizations including in-situ time-dependent infrared spectroscopy, wherein chemical coordination of CO 2 promotes to fabricate 2D SC-Bi-PMOFs nanosheets. Moreover, the formation of Cu-PMOFs and Fe-PMOFs proves the universal scCO 2 strategy for synthesizing PMOFs. Density functional theory (DFT) calculations together with experiments results confirm the SC-Bi-PMOFs with abundant active sites guarantee efficient ligand-to-metal charge transfer and reduction efficiency of CO 2 . The high-efficiency utilization of CO 2 for synthesizing a series of MOFs and subsequent catalysis on photocatalytic CO 2 reduction for valuable chemicals realize the carbon recycle.
研究领域:
材料科学
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环境科学
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化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Min Deng,Jing Wei,Zikang Qin,Zheng Yan,Junfeng Zheng,Lin Yang,Lu Yao,Wenju Jiang,Zhongde Dai
Styrene-butadiene-styrene triblock copolymer (SBS) has attracted increasing research attention due to its low cost, excellent mechanical properties, and superior gas permeability performance. In this work, a series of novel SBS doped membranes were prepared by introducing polyphosphoric acid (PPA), lithium 2,2,2- trifluoroacetate (TFALi), and 1,3-dichloro-1,1,3,3-tetraisopropyldisiloxane (Siloxane-Cl) into SBS as dopants. The results indicated that the addition of dopants into SBS membranes simultaneously enhanced the CO 2 permeability and CO 2 /N 2 selectivity of SBS membranes. Specially, doping Siloxane-Cl expanded the d-spacing, introduced flexible siloxane (Si-O) groups to enlarge molecular spaces, and formed more crosslinked network structure. Therefore, the SBS/Siloxane-20 membrane showed an approximately 4-fold increase CO 2 permeability compared to the pristine SBS membranes (from 203.3 to 842.9 barrer), accompanied by an increase in CO 2 /N 2 selectivity from 15.8 to 22.0. The obtained membranes also exhibited attractive anti-plasticization and anti-physical aging properties, no obvious decline in CO 2 permeability and/or CO 2 /N 2 selectivity can be observed after 1-week continuous permeation test, making them promising candidates for CO 2 /N 2 separation.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）