SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Fan Liu,Yao Shen,Li Shen,Yuchi Zhang,Weiqi Chen,Qiaoli Wang,Sujing Li,Shihan Zhang,Wei Li
A novel sustainable amino functionalized ionic liquid (AFIL) organic solution of tetraethylene pentamine 5-amino-4-imidazolecarboxamide/n-propanol/ethylene glycol ([TEPAH][AICA]/NPA/EG) was proposed for CO 2 capture to reduce the regeneration energy consumption. The solution had an efficient absorption loading of 1.78 mol·mol −1 , and it still maintained a good recyclability after 10 cycles (regeneration efficiency > 88%). Under this condition, the regeneration energy consumption was 2.30 GJ·t −1 CO 2 , which was 39.5% lower than that of MEA/water. The absorption and desorption mechanisms were investigated by 13 C NMR. For CO 2 absorption reaction, N atom of [AICA] − combined with CO 2 to form the carbamate directly, while other amino groups followed the zwitterion formation and deprotonation. Then some carbamates combined with alcohol to form the alkyl carbonates. For CO 2 desorption reaction, both the alkyl carbonates and carbamates combined with AFILH + to decompose, but the alkyl carbonates decomposed completely and a small amount of carbamates remained, indicating that carbonate was easier to decompose than carbamate. The novel [TEPAH][AICA]/NPA/EG solution with low energy consumption and good recyclability, which provides a sustainable strategy for advancing carbon capture technologies.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2021
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IF 2.495
Xueteng Zhu,Hexia Deng,Gang Cheng
Photocatalytic reduction of CO 2 into fuels is a promising approach to address the energy crisis and global warming issues. In this work, g-C 3 N 4 -W 18 O 49 nanocomposite material was constructed by a simple solvothermal method. The W 18 O 49 nanorods have a good dispersion by coupling with the g-C 3 N 4 sheet. Under simulated sunlight irradiation, the g-C 3 N 4 -W 18 O 49 nanocomposite exhibited superior photocatalytic CO 2 reduction capability than that of g-C 3 N 4 and W 18 O 49 . The photo/electrochemical measurements demonstrated that the g-C 3 N 4 -W 18 O 49 heterojunction could accelerate the separation and migration of charge carries, thus improving the activity of photocatalytic reduction of CO 2 into CH 4 and CO.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Wenbo Chen,Zhenguo Zhang,Cancan Yang,Jing Liu,Hongcheng Shen,Kai Yang,Zhe Wang
In this work, we fabricated PIM-based mixed matrix membranes (MMMs) containing MOF-801/ionic liquid nanocomposites to enhance CO 2 separation performance of pure polymer membranes. All membranes and MOF-801/ionic liquid nanocomposites were prepared by solution casting method and wet impregnation, respectively. The samples were analyzed by SEM, XRD , FTIR, TGA and Nitrogen adsorption-desorption measurements. The nanocomposites are composed of metal-organic framework (MOF) MOF-801 and ionic liquid (IL) adsorption capacity. MOF-801 can well control the dispersion of IL in the polymer matrix , which is conducive to exposing more active sites in the nanocomposites to improve the CO 2 adsorption selectivity of MOF-801/ionic liquid nanocomposites. At the same time, the porous structure of nanocomposites also enhances the gas adsorption and diffusion, thereby improving the gas separation performance. Compared with pure PIM-1 membranes, the CO 2 permeability and CO 2 /N 2 selectivity of IL@MOF/PIM-5% MMMs was increased by 129% and 45% (CO 2 = 9420 Barrer, CO 2 /N 2 = 29）, respectively. Compared with MOF-801/PIM-1 MMMs, the permeability of CO 2 decreased slightly but the selectivity of CO 2 /N 2 increased from 27 to 29. The aging test showed that the CO 2 permeability of MMMs could remain above 70% after 90 days. The anti-plasticization performance of MMMs has also been significantly improved. The CO 2 separation performance of IL@MOF/PIM-5% MMMs significantly exceeded the 2008 Robeson upper bound, showing excellent gas separation performance and working stability.
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Yajian Duan,Chaojuan Li,Yaxin Hua,Shuai Wu,Yaqing Guo,Xiaogang Zhang,Yuqi Hu,Bin Yang,Yongnian Dai,Jin Shi
A novel membrane electrolysis cell has been designed to convert CO 2 into CO in organic electrolyte, with Cl 2 produced on the anode from NaCl oxidation in aqueous solution. The obtained CO and Cl 2 can be used as the feedstock to produce phosgene. Phosgene is a widely used acylating agent in a chemical industry, which can be used as feedstock to produce numerous high-value chemicals. Through this route, CO 2 can be converted into useful chemical, with huge economic profits created in this process. Our experiment results demonstrate that CO 2 can be efficiently converted into CO in our designed electrolyzer, and NaCl can be efficiently oxidized to Cl 2 . During long-term electrolysis process, NaHCO 3 is generated and accumulated between the membrane and the cathode. This phenomenon provides clear evidence for us to better understand the mechanism of CO 2 electro-reduction in organic electrolyte.
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高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Xin Li,Jingru Guan,Haopeng Jiang,Xianghai Song,Pengwei Huo,Huiqin Wang
Construction of multi-interface contact step-scheme (S-scheme) photocatalyst is a promising pathway to achieve high-electron transfer efficiency for photocatalytic CO 2 reduction. In this paper, g-C 3 N 4 nanosheets were selected as the main photocatalyst, rod-like CeO 2 (R-CeO 2 ) with unique Ce 4+ →Ce 3+ conversion property and rGO were loaded on the g-C 3 N 4 surface to construct 2D-1D-2D sandwich photocatalyst. The yields of CO and CH 4 were about 63.18 and 32.67 μmol/g after 4 h when the rGO/R-CeO 2 /g-C 3 N 4 was used as catalyst, which were about 4 and 6 times higher than that of pure CN, respectively. Cyclic experiments proved that the composite had excellent photocatalytic and material stability. Photoelectrochemical tests showed that the construction of S-scheme electron transfer model and the introduction of rGO can great enhance the electron transmission and separation of photogenerated electron-hole pairs. CO 2 adsorption test identified that the loading of R-CeO 2 and rGO obviously enhanced the CO 2 adsorption ability of pure g-C 3 N 4 . Density functional theory (DFT) calculations used to analyze the electron transfer path and the formation of the build-in electric field at the semiconductor interface. In-situ FTIR and 13 CO 2 element-tracer detection carried out to research the process of CO 2 photoreduction. A possible multi-interface contact S-scheme electron transfer mechanism for enhanced CO 2 photoreduction activity has been discussed.
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高影响因子
Journal of Physical Chemistry C
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2021
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IF 4.126
Fuyong Zhang,Wei Zhou,Xuewei Xiong,Yuhao Wang,Kang Cheng,Jincan Kang,Qinghong Zhang,Ye Wang
Catalytic transformation of CO2 into chemicals in large demand such as ethanol has attracted much research attention under the background of establishing carbon-neutral societies. Supported Rh catalysts are promising candidates for the hydrogenation of CO2 to ethanol but suffer from low ethanol productivity and poor catalyst stability. Here, we report that zeolite silicalite-1 embedded Na-promoted Rh nanoparticles (Na-Rh@S-1) demonstrate high productivity and stability for CO2 hydrogenation to ethanol. The ethanol selectivity of 24% was attained at a CO2 conversion of 10%, and the space-time yield of ethanol reached 72 mmol gRh–1 h–1, which outperformed most of the Rh-based catalysts reported to date. While a reference catalyst prepared by impregnation underwent deactivation, the Na-Rh@S-1 catalyst was stable for at least for 100 h owing to the confinement effect. The Na+ modifier played crucial roles in enhancing the CO2 conversion and ethanol selectivity by suppressing methane formation. The characterizations suggest that the presence of Na+ enables the coexistence of Rh0 and Rh+ and enhances CO2 adsorption, thus boosting ethanol formation. A comparative study between CO and CO2 hydrogenation reveals that the Na-Rh@S-1 catalyst is significantly more active and selective toward CO2 hydrogenation to ethanol.
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高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Xiangyu Li,Zhiqing Wang,Ru Feng,Jiejie Huang,Yitian Fang
If a large amount of fly ashes produced by coal-fired power plants was not treated harmlessly, it will pose a serious threat to the ecological environment. As one of the high-valued utilization technologies of fly ash, the technology of extracting aluminum from coal ash produces large quantities of waste residue after acid leaching nevertheless. It is an economic and environmentally friendly way to recycle alumina-extracted residue (AR) as solid sorbent to capture CO 2 . In this study, using AR as raw material, we synthesized PEI modified solid sorbents by novel “wet gel impregnation” method (WGI) to enhanced CO 2 capture. The effects of amine loading, adsorption temperature, and impregnation method on CO 2 adsorption capacity and kinetics were investigated by thermogravimetric analysis (TGA). On this basis, a possible double-layer adsorption model was proposed, i.e., the PEI adsorption layer on the outer surface of sorbents and the internal isolation layer. The ratio of the two layers changed with the variation in PEI loading and adsorption temperature, resulting in the difference of adsorption capacity. The maximum CO 2 adsorption capacity of 2.07 mmol/g was obtained under the amine loading of 40 wt% at 95 °C, and 100% CO 2 . Moreover, the stable adsorption capacity and high CO 2 selectivity were maintained in five repeated adsorption-desorption cycles.
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高影响因子
Journal of CO2 Utilization
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2019
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IF 5.189
Feiyang Hu,Sai Tong,Kun Lu,Cheng-Meng Chen,Fang-Yuan Su,Jian Zhou,Zhang-Hui Lu,Xuewen Wang,Gang Feng,Rongbin Zhang
The reduced oxide graphene (RGO) supported Ni-based catalysts is prepared and modified with ceria (Ni-Ce/RGO) for CO 2 methanation for the first time in the present work, and compared with the active carbon (AC) and γ-Al 2 O 3 supported samples. The results show that the catalytic activity of the samples without ceria follow the order Ni/RGO > Ni/γ-Al 2 O 3 > Ni/AC, vs . samples with ceria Ni-Ce/RGO > Ni-Ce/γ-Al 2 O 3 > Ni-Ce/AC. The activities of all samples were greatly improved after ceria modification. The Ni-Ce/RGO works the best for CO 2 methanation, which could reach the highest CO 2 conversion of 84.5% and the highest methane yield of 83.0% at 350 °C with atmospheric pressure. The excellent catalytic performance of Ni-Ce/RGO could be attributed to the special support effect of RGO and the ceria promotion effect. The support effect of RGO could be attributed to its large surface area and surface oxygen-containing functional groups, which results in stable anchoring of the active metal. The addition of ceria promotes the Ni dispersion on the supports as well as to accelerate the positive reaction due to the oxygen vacancies of ceria.
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高影响因子
RSC Advances
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2019
·Vol. 9
·期 46
·27050-27059
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IF 3.049
Xia Wang,Wulan Zeng,Hongyan Zhang,Dan Li,Hongjing Tian,Xiude Hu,Qian Wu,Chunling Xin,Xiaoyu Cao,Wenjing Liu
To reduce the cost of CO2 capture, polyethylene polyamine (PEPA), with a high amino density and relatively low price, was loaded into MCM-41 to prepare solid sorbents for CO2 capture from flue gases. In addition, methoxypolyethylene glycol (MPEG) was codispersed and coimpregnated with PEPA to prepare composite sorbents. The pore structures, surface functional groups, adsorption and regeneration properties for the sorbents were measured and characterized. When CO2 concentration is 15%, for 30, 40 and 50 wt% PEPA-loaded MCM-41, the equilibrium adsorption capacities were respectively determined to be 1.15, 1.47 and 1.66 mmol g−1 at 60 °C; for 30 wt% PEPA and 20 wt% MPEG, 40 wt% PEPA and 10 wt% MPEG, and 50 wt% PEPA and 5 wt% MPEG codispersed MCM-41, the equilibrium adsorption capacities were respectively determined to be 1.97, 2.22 and 2.25 mmol g−1 at 60 °C; the breakthrough and equilibrium adsorption capacities for 50 wt% PEPA and 5 wt% MPEG codispersed MCM-41 respectively reached 2.01 and 2.39 mmol g−1 at 50 °C, all values showed a significant increase compared to PEPA-modified MCM-41. After 10 regenerations, the equilibrium adsorption capacity for codispersed MCM-41 was reduced by 5.0%, with the regeneration performance being better than that of PEPA-loaded MCM-41, which was reduced by 7.8%. The CO2-TPD results indicated that the mutual interactions between PEPA and MPEG might change basic sites in MCM-41, thereby facilitating active site exposure and CO2 adsorption.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
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IF 5.107
Min Xiao,Ding Cui,Liangyu Zou,Qi Yang,Hongxia Gao,Zhiwu Liang
Three tertiary diamines, N , N , N' , N' -tetramethyl-1,2-ethanediamine, N , N , N ', N '- tetramethyl-1,3-propanediamine and N , N , N ', N '-tetramethyl-1,4-butanediamine, were investigated for application in post-combustion CO 2 capture. The acid-base properties of the diamines were studied through measuring pH values of the acidified amine solutions to obtain reaction constants and corresponding enthalpies/entropies of the reactions. Competitive formation of monoprotonated and diprotonated diamines was observed. CO 2 absorption using these diamine solutions was carried out through a continuous flow method. NMR spectroscopy was used to detect speciation of the bulk solution. Then a general evaluation of the diamines was made in comparison with the monoamines in terms of equilibrium CO 2 solubility and p Ka . The results demonstrated the potential of the structurally modified diamines to be promising bicarbonate forming absorbents in CO 2 absorption. Finally, the equilibrium CO 2 solubility of aqueous N , N , N' , N' -tetramethyl-1,2-ethanediamine solution was measured at a wider range of temperatures, CO 2 partial pressures and initial amine concentrations to establish a thermodynamic model. The model provided reasonable prediction of equilibrium CO 2 solubility and species concentration profiles.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xue Bai,Jinxin Liu,Yuhu Xu,Yue Ma,Zhanchao Liu,Jianming Pan
Conventional methods for preparing amidoxime-based hollow porous sorbents (HPS) for uranium (U(VI)) extraction usually use solution or emulsion process with surfactant and expensive pore template, so they cannot meet requirements of economic and environmentally friendly evaluation. Here, hollow porous microspheres functionalized with abundant amidoxime (AO-HP-MF) are prepared via CO 2 Pickering emulsion (or bubble) templated interfacial polymerization and assembly of site chains for highly efficient U(VI) extraction. For this strategy, in situ generated CO 2 bubbles are utilized as core template, SiO 2 nanoparticles serve dual roles of an emulsion stabilizer and pore template for polymer shell. Meanwhile, assembled polyvinyl polyamine (PEA) chains provide lots of sites for post-modification with amidoxime. Taking the advantages of well-defined hollow porous morphology, uniform size, and high-density of amidoxime, AO-HP-MF is expected to possess excellent adsorption capacity, fast equilibrium rate, and high selectivity. The equilibrium time and maximum adsorption capacity are 1.0 h and 553.3 mg g −1 at 298 K, respectively, and the monolayer chemisorption based on chelation between U(VI) and amidoxime is main mechanism of selective uranium extraction. Their uniform size may be associated with the pressure-dependent formation condition of in situ generated CO 2 bubbles, which is different from traditional emulsion templated microspheres with fairly irregular size. Most importantly, AO-HP-MF has remarkable selectivity for U(VI), even if massive amounts of Ca 2+ , Mg 2+ , Na + , Zn 2+ , and other ions exist in the simulated solution. Therefore, this work not only presents a new clue to fabricate high performance sorbents via simple bubble templates, but also provides a novel platform for U(VI) extraction.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 46
·18345-18354
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IF 3.069
Gaozhi Bai,Yu Han,Panpeng Du,Zhaoyang Fei,Xian Chen,Zhuxiu Zhang,Jihai Tang,Mifen Cui,Qing Liu,Xu Qiao
A highly efficient solid-amine adsorbent with excellent CO2 capacity from flue gas was successfully prepared using polyethyleneimine (PEI)-impregnated resin HPD450 in this study. The adsorbents were characterized by scanning electron microscopy (SEM), Fourier transforms infrared spectroscopy (FTIR), N2 adsorption–desorption, thermogravimetric analysis (TGA) techniques and elemental analysis (EA). The CO2 adsorption behaviors of the adsorbent were studied for their adsorption capacity, kinetics, thermodynamics and stability. The optimal adsorbent (HPD450/PEI-50) exhibited an excellent adsorption capacity of 4.44 mmol g−1 for pure CO2 and 3.62 mmol g−1 for 15 vol% CO2. Moreover, HPD450/PEI-50 retained an average capacity of 3.58 mmol g−1 under flue gas for 90 consecutive adsorption cycles. The adsorption/desorption process of CO2 on HPD450/PEI-50 was investigated using in situ FTIR. The capture of carbon dioxide in the simulated flue gas stream also demonstrated that moisture had a promoting effect on CO2 adsorption. This design of the high-performance HPD450/PEI-50 with a fantastic CO2 capacity could provide an up-and-coming candidate for CO2 capture from flue gas.
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高影响因子
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