ACS Applied Materials & Interfaces
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2017
·
IF 7.504
Shiming Zhang,Dingguan Wang,Qianhao Pan,Qinyuan Gui,Shenglong Liao,Yapei Wang
Solid materials for CO2 capture and storage have attracted enormous attention for gaseous separation, environmental protection, and climate governance. However, their preparation and recovery meet the problems of high energy and financial cost. Herein, a controllable CO2 capture and storage process is accomplished in an emulsion-templated polymer foam, in which CO2 is breathed-in under dark and breathed-out under light illumination. Such a process is likely to become a relay of natural CO2 capture by plants that on the contrary breathe out CO2 at night. Recyclable CO2 capture at room temperature and release under light irradiation guarantee its convenient and cost-effective regeneration in industry. Furthermore, CO2 mixed with CH4 is successfully separated through this reversible breathing in and out system, which offers great promise for CO2 enrichment and practical methane purification.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2016
·
IF 1.207
Xiaoqing Wang,Libo Li,Jiangfeng Yang,Jinping Li
Two isomeric metal–organic frameworks (MOFs) with 2-dimensional (2D) and 3-dimensional (3D) topologies both comprised of Cu(II) and OTf (OTf = trifluoromethanesulfonate) ions were synthesized and characterized. The CO 2 , CH 4 and N 2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at 0.1 MPa. The results showed that the 2D MOF exhibited a higher selectivity for CO 2 from CO 2 /CH 4 and CH 4 from CH 4 /N 2 compared to the 3D MOF, even though it possessed a lower surface area and pore volume. The higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered MOFs. Dynamic separation experiments using CO 2 /CH 4 and CH 4 /N 2 mixtures on the two MOFs proved that the 2D MOF had a longer elution time than the 3D MOF as well as better separation abilities.
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JOURNAL OF POROUS MATERIALS
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2016
·Vol. 24
·期 3
·591-599
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IF 1.385
Li Yanyan,Na Wei,Wang Hua,Gao Wengui
A series of Au–CuO/SBA-15 catalysts with 1–3 wt% Au and 30 wt% CuO were successfully prepared for CO 2 hydrogenation to methanol by chemical reduction and the following impregnation. The influence of Au content on the physicochemical properties of Au–CuO/SBA-15 catalysts was investigated in terms of ICP-AES, N 2 physisorption, XRD, TEM, N 2 O titration, XPS and H 2 –TPR technique. The results showed that the as-prepared Au–CuO/SBA-15 catalysts exhibited higher catalytic activity than CuO/SBA-15 catalyst. 2 % Au–CuO/SBA-15 catalyst showed the best catalytic activity with 13.5 % methanol selectivity and 24.2 % CO 2 conversion for CO 2 hydrogenation to methanol. The addition of Au NPs played an important role in improving the catalytic activity for CO 2 hydrogenation to methanol, which may be attributed to the interaction between Au and CuO.
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POLYMER
·
2016
·
IF 3.586
Jin Wang,Hongming Zhang,Yuyang Miao,Lijun Qiao,Xianhong Wang,Fosong Wang
UV-curable waterborne polyurethanes (CO 2 -UV-WPUs) with CO 2 -polyols as soft segment were firstly synthesized. In addition to the good mechanical performance, the coexistence of carbonate and ether moieties in soft segment assured the excellent hydrolysis resistance of CO 2 -UV-WPU compared with polybutylene adipate glycol based waterborne polyurethane (PBA-UV-WPU). Its retention of tensile strength reached 88% after 15 h immersion in 1.5% sodium hydroxide solution, while that of PBA-UV-WPU completely lost its mechanical property. The double bond density primarily governed the mechanical performance of CO 2 -UV-WPU, when it increased from 0.93 mmol/g to 2.4 mmol/g, the tensile strength increased from 29 MPa to 67 MPa, while elongation at break decreased from 150% to 9.6%, accompanied by the reduction of maximum water swelling percentage from 26.7% to 14.5%. The introduction of CO 2 -polyol as soft segment not only created a route to produce UV-curable waterborne polyurethane from CO 2 , but also provided polyurethane with novel value-added performance like good hydrolysis resistance. Moreover, the thermal/mechanical performance and hydrophilicity of CO 2 -UV-WPUs could be conveniently adjusted by controlling molecular weight of CO 2 -polyols, ensuring the application feasibility of CO 2 -UV-WPU.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
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2017
·Vol. 131
·期 2
·1499-1507
·
IF 1.953
Lyu Jiaxun,Hu Dongdong,Liu Tao,Zhao Ling
The non-isothermal curing kinetics of epoxy resin system consisting of diglycidyl ether of bisphenol A (DGEBA) and m-xylylenediamine (MXDA) were investigated by high-pressure differential scanning calorimetry at different heating rates of 5, 10, 15 and 20 K min −1 under compressed carbon dioxide (CO 2 ) of 0.1–8 MPa. The activation energies were determined by isoconversional Kissinger–Akahira–Sunose method and Vyazovkin numerical method, and the average values decreased from 53.5 to 46.8 and 54.1 to 44.5 kJ mol −1 , respectively, when the CO 2 pressure increased from 0.1 to 8 MPa. It is indicated that the curing reaction of epoxy resin occurs more easily under higher-pressure CO 2 due to the promoted molecular movement, especially in the supercritical state. The non-isothermal curing kinetics were investigated by n th-order model and two-parameter autocatalytic model (Šesták–Berggren model), and the latter one analyzed by Málek method exhibited good agreement with the experimental data except the initial and final stages of the curing reaction.
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Journal of Energy Chemistry
·
2017
·
IF 2.594
Haiying Ran,Jiexin Wang,Ahmed A. Abdeltawab,Xiaochun Chen,Guangren Yu,Yinghao Yu
We synthesized one quaternary ammonium polymeric ionic liquids (PILs)P[VBTHEA]Cl and three imidazolium PILs of P[VEIm]Br, P[VEIm]BF 4 , P[VEIm]PF 6 by free-radical polymerization in solution. These PILs were characterized by FT-IR, 1 H-NMR, 13 C-NMR, TGA, XRD and SEM. Their CO 2 adsorption capacities were measured under different pressures and temperatures by constant-volume technique. It was observed that quaternary ammonium PILs of P[VBTHEA]Cl have higher adsorption capacity for CO 2 than those imidazolium PILs, following P[VBTHEA]Cl > P[VEIm]PF 6 > P[VEIm]BF 4 > P[VEIm]Br, which may be ascribed to higher positive charge density on ammonium cation than that on imidazolium cation and thus stronger interaction with CO 2 , consistent with the results from dual-mode adsorption model that ammonium PILs have much higher CO 2 bulk absorption than imidazolium PILs. CO 2 adsorption capacity of P[VBTHEA]Cl is 9.02 mg/g under 295 K and 1 bar, which is comparable to that of some other PILs, and is much higher than that of the corresponding ILs monomer . These PILs have good adsorption selectivity for CO 2 over N 2 and regeneration efficiency.
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BIOMASS & BIOENERGY
·
2024
·
IF 5.8
Yonghui Xu,Yufei Liu,Wei Zhan,Dingle Zhang,Yiyun Liu,Yi Xu,Zhengshun Wu
This study explores the transformation of peanut shells, an abundant agricultural waste, into high-efficiency activated carbon for CO 2 capture using a two-step pyrolysis and K 2 CO 3 activation method. Observations indicated that with an increasing impregnation ratio, the activated carbon demonstrates remarkable improvements in structural properties, achieving specific surface areas and pore volumes of 1150.02 m 2 /g and 0.46 cm 3 /g, respectively. Among the prepared samples, the activated carbon obtained with a peanut shell to K 2 CO 3 impregnation mass ratio of 1:2 exhibits superior CO 2 adsorption capacity at 1 bar, with values of 3.76 mmol/g at 25 °C and 5.70 mmol/g at 0 °C. The CO 2 adsorption isotherms of the activated carbon conform to the Langmuir and Freundlich models. These results demonstrate the potential of this method in addressing environmental concerns, particularly in mitigating CO 2 emissions, and highlight the broader application prospects of biomass-derived activated carbon in environmental management.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Zhaoxing Wu,Zhengxiong Wu,Yulai Zhao,Linxi Hou
The electrochemical reduction of CO2 to produce high-value multicarbon products represents a challenging yet highly desirable process, particularly due to the inefficient C–C coupling observed in current electrocatalysts. In this study, Cu2+ and Co2+ were introduced into ZIF-8 as precursors to synthesize a series of Co- and CuCo-doped carbon nanostructure materials with varying Co-to-Cu ratios. X-ray diffraction and X-ray photoelectron spectroscopy (XPS) analyses confirmed the successful doping of metal Co in the form of Co–Nx, while Cu was partly doped as nanoparticles attached to the carbon substrate surface and partly as single atoms forming Cu–Nx. Transmission electron microscopy and energy-dispersive X-ray spectroscopy analyses revealed uniform distribution of elemental Co and Cu on the carbon substrate, with Cu loaded as nanocluster on the surface. Linear sweep voltammetry tests indicated that Cu/CoCu-Nx-C composites exhibited enhanced reactivity toward CO2 reduction compared to other samples. At −0.19 V (vs RHE), the Faradaic efficiencies (FEs %) of C2H4, C2H6, CH4, CO, and H2 over Cu/CoCu-Nx-C were 29.7, 8.6, 20.2, 9.8, and 31.5%, respectively. The influence of Co and Cu doping modes on the selectivity of electrocatalytic reduction products was investigated. Results showed that Cu/CoCu-Nx-C exhibited a higher FE of C2 compared to Cu/Cu–Nx-C, with nearly 10 times higher C2 current density. Mechanistic insights from acid-etching experiments and XPS revealed a synergistic interaction between metallic Co and Cu, promoting the generation of multicarbon products. Co–Nx improved *CO coverage, facilitating subsequent C–C coupling on neighboring Cu–Nx. Additionally, CH4 production was attributed to the (111) crystalline facets in the Cu nanocluster and isolated Cu–Nx. Overall, this research provides an important understanding of the creation of straightforward and effective catalysts for the reduction of CO2. It holds considerable potential for the production of hydrocarbons using carbon dioxide.
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AICHE JOURNAL
·
2024
·Vol. 70
·期 8
·e18471
·
IF 3.5
Xiaoyu Wang,Fangxu Fan,Yongchao Sun,Jingfa Zhang,Canghai Ma,Gaohong He
Polymer-based membrane technology holds immense promise for CO 2 separation. However, it faces persistent challenges, including the high CO 2 pressure-induced plasticization and permeability-selectivity trade-offs, which significantly hinder the development of polymeric membranes. To tackle this issue, we synthesized a novel polyimide 6FDA-DAT:DABA(6FDD) containing triptycene and carboxylic groups. Upon de-carboxylation induced cross-linking, the membrane demonstrated a simultaneous enhancement of gas permeability and selectivity. Specifically, compared to the uncross-linked 6FDD, the 400°C-24 h cross-linked membrane exhibited a remarkable increase in CO 2 permeability by 177% (93.1 Barrer) and a significant rise in CO 2 /CH 4 selectivity by 47% (57.5), reaching the CO 2 /CH 4 upper bound. More importantly, the cross-linked membrane displayed vastly improved CO 2 plasticization resistance, withstanding up to 42 bar of CO 2 feed pressure. The design of decarboxylated cross-linked membranes in this work paves the way for creating high-performing and plasticization-resistant membranes with potential applications in high-pressure CO 2 separations.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yingnan Ma,Na Liu,Yulu Zhang,Zhen Xu,Juan Chen,Hong Wu,Jianqiang Meng
The gutter layer of thin film composite membranes (TFCMs) promotes the formation of ultrathin top layers. MOFs nanosheets gutter layer is an efficient strategy for building gas separation TFCMs while suffers from such an issue that gas molecules transport between interlayer thus making it difficult to fully utilize the excellent molecule sieving ability of MOFs. In this work, both MOFs nanosheets and continuous MOFs gutter layers were constructed to prepare TFCMs for CO 2 separation. The polyamide top layer with irregular structure was formed on MOFs gutter layer by interfacial polymerization. The physical and chemical properties as well as separation performance of different TFCMs were further compared. Benefitting from the denser structure and stronger hydrophobicity of continuous ZIF-8 gutter layer, the obtained top layer showed more regular structure with ultrathin thickness (≈30 nm). At the same time, due to the ZIF-8 gutter layer provided additional and stable CO 2 selectivity, the CO 2 permeance reached 588.2 GPU with the selectivity of CO 2 /N 2 and CO 2 /CH 4 of 49.8 and 52.3, which surpassed the 2008 Robeson upper bound. We believe that such a membrane design based on continuous MOFs gutter layers is a promising approach for high-performance gas separation membranes.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Qi Tan,Yiwen Liu,Ruifeng An,Heping Wu,Zhiqiang Tian,Bingliang Gao
Reducing greenhouse gas emissions is a crucial step in mitigating global warming. Carbon dioxide (CO 2 ) represents one of the most pivotal greenhouse gases contributing to climate change. Many researchers are actively engaged in the development of effective and reversible CO 2 absorbents to control and reduce CO 2 gas emissions. In this paper, we synthesized a series of molecular solvents (MSs) based on the superbase 1,5-diazabicyclo [4.3.0]-5-nonene (DBN) and used them for CO 2 capture. The CO 2 capture capacity of MSs composed of DBN and different alcohols was systematically investigated, with DBN-Methanol (1:1.25) demonstrating superior absorption performance by achieving a maximum absorption capacity of 0.263 g CO 2 /g MS. The effects of temperature, pressure, the molar ratio of the hydrogen bond acceptor (HBA) to hydrogen bond donor (HBD), and moisture on the absorption process were studied. The experimental results were corroborated by NMR spectra analysis and FTIR spectra analysis, confirming that these MSs can effectively react with CO 2 to produce carbonate and carbamate compounds through synergistic absorption involving hydroxyl group as primary component and amino group as secondary component. In addition, it is worth noting that the MSs studied in this work exhibit only glass transition at low temperatures and transform into ionic liquids (ILs) after capturing CO 2 , resulting in a significant increase in conductivity and demonstrating considerable electrochemical potential.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Dandan Hao,Ping Wang,Ju Liu,Huanhui Zhan,Tiantian Zhou,Bo Fu
MOF-199 is considered to be an excellent CO 2 adsorbent owing to its substantial specific surface area, suitable pore structure and abundant sorption sites. However, powdered MOF-199 is prone to agglomeration and has poor recyclability. Herein, we proposed a MOF-199-based adsorbent by combining the MOF synthesis process with traditional papermaking process. Through such a design, MOF-199 particles are adhered on the surface of wood pulp fiber. The sufficient hydroxyl groups and electrostatic forces of cellulose facilitates the homogeneous and tight adhesion of MOF crystals. The optimal MP-4 sample demonstrated a high CO 2 adsorption capacity (1.80 mmol·g ‐−1 at 25 °C) and good CO 2 /N 2 selectivity (30.06). Moreover, the composite sorbent can be easily regenerated. The adsorption mechanism was analyzed by the density functional theory approach. The simulation results showed that the carboxyl functional groups with a large number of oxygen atoms and active metal sites are the key to boost the CO 2 adsorption performance.
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