ENERGY
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2020
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IF 6.082
Kun Fu,Chenxu Liu,Lemeng Wang,Xiayu Huang,Dong Fu
In this work, novel non-aqueous absorbents composed of 2-ethylhexan-1-amine (EHA) and glyme were proposed for CO 2 capture. The absorption performance of CO 2 in EHA + diglyme, EHA + triglyme and EHA + tetraglyme non-aqueous solutions was investigated and the viscosities ( η ) of the CO 2 -saturated absorbents were measured. Besides the experiments, kinetic models were applied to correlate the CO 2 absorption. The activation energy ( E a ) was obtained from Arrhenius equation , and the absorption mechanism was deduced. The results showed that both Lagergren model and Avrami model can accurately correlate and predict the time-dependent absorption amount, thus an optimized composition under which excellent absorption performance and relatively low η and E a can be simultaneously achieved was determined. Compared to water-based absorbents like MEA, the optimized non-aqueous absorbents take the advantages of better absorption performance and lower activation energy. Moreover, the glyme solvents have about 50% lower specific heat capacities and much higher boiling points (≥435 K) than water, which is expected to greatly reduce the sensible heat and the latent heat of the solvent during regeneration. Therefore, the proposed novel absorbents have promising industrial application potential in the CO 2 capture process.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Juan Lv,Sen Liu,Hao Ling,Hongxia Gao,Wilfred Olson,Qiang Li,Zain Ali Saleh Bairq,Zhiwu Liang
A new sulfolane/secondary amine biphasic absorbent, sulfolane/2-methylaminoethanol (MAE) solution, was developed for postcombustion CO2 capture (PCC). Surprisingly, using a 4M/5M sulfolane/MAE solution saves about 60% energy consumption (EC) for CO2 stripping when compared with traditional aqueous 5M monoethanolamine (MEA) solutions. First, we theoretically proved that MAE in sulfolane-based biphasic solution improves the CO2 absorption rate with high CO2 loading at the phase-changing point, which could be energy-saving for CO2 stripping. Based on a comprehensive comparison of the phase-changing behavior, nuclear magnetic resonance (NMR) spectra, absorption rate, and desorption performance, the 4M/5M sulfolane/MAE was determined to be the optimal molar ratio among six sulfolane/MAE biphasic solutions for CO2 capture. In addition, the absorption and desorption experiments with various temperatures revealed that relatively low temperature (ranging from 110 to 120 °C) was favorable for CO2 removal and energy-saving. Furthermore, the 4M/5M sulfolane/MAE solution achieved a very low energy consumption (EC) compared with that of 5M MEA solution, and the stripped CO2 amount is similar to that of 5M MEA and 5M MAE solutions.
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高影响因子
JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Yuan Wang,Hanzhi Wang,Tian C. Zhang,Shaojun Yuan,Bin Liang
A novel hierarchical porous carbon derived from poly(p-phenylenediamine) incorporated with reduced graphene oxide (rGO) is prepared for CO 2 capture and supercapacitors . In this synthesis, chemically in-situ oxidative polymerization and KOH chemical activation are employed with the controllable introduction of GO (GO/Polyphenylenediamine = 0–2 wt%). The obtained carbon material (APG-1%) with high surface area (860.4 m 2 g −1 ) and rich N content (7.91 wt%) exhibits excellent CO 2 capture ability (4.65 mmol g −1 at 298 K, 5 bar) and good electrochemical performance as a supercapacitor electrode with 158.5 F g −1 in 6 M KOH at a current density of 1 A g −1 . Even at a high current density of 10 A g −1 , a capacity of 115.2 F g −1 is still maintained. The rational addition of rGO provides an effective strategy of simultaneous improvement of CO 2 adsorption and capacitive performance.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Chenkai Jiang,Han Chen,Junliang Wang,Yao Shen,Jiexu Ye,Shihan Zhang,Lidong Wang,Jianmeng Chen
A biphasic solvent features high absorption capacity and low heat duty for CO2 capture. Phase separation behavior is essential to cut down energy penalty. Four phase splitting agents with different hydrophobicities, such as 1,3-dimethyl-2-imidazolidinone (DMI), 1-methyl-2-pyrrolidinone (NMP), N,N-dimethylformamide, and sulfolane, were dosed to biphasic solvents, triethylenetetramine and 2-(diethylamino)ethanol. Experimental results revealed that they can tune the phase separation behavior during CO2 absorption. Generally, under the same CO2 loading, the volume ratio of the rich phase increased with their hydrophobicity (log P), which accounts for over 50%. Moreover, their influences on absorption capacity, kinetics, and thermodynamics were also investigated. After dosing NMP, the heat duty was decreased by 22%. Furthermore, a phase splitting agent with a positive log P was more conducive to reducing the heat duty, and one with a negative log P enhanced the absorption rate. With DMI, the absorption rate was 114% higher than that of MEA at rich loading. The 13C NMR analysis showed that the agents were not involved in CO2 absorption and did not affect the reaction mechanism. Furthermore, quantum calculation was used to verify the reaction mechanism, confirming that the phase splitting agent increases the reaction equilibrium constant and makes it proceed more thoroughly.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Jie Ding,Wenxin Zhao,Letian Zi,Xin Xu,Qiang Liu,Qin Zhong,Yu Xu
This study is to convert renewable H 2 and increasingly concerned CO 2 to ethylene or C 2 H 4 over Fe 3.33 Co 1.67 K 5 /ZrO 2 and Fe 3.33 Co 1.67 K 5 /Al 2 O 3 catalysts. The ZrO 2 support provides amounts of surface oxygen vacancies (OVs) as well as stable and rich surface hydroxyl groups (-OH), which promotes the Fe 3.33 Co 1.67 K 5 /ZrO 2 catalysts with 5% Fe and Co loadings to achieve C 2 H 4 space time yield (STY) of 0.064 mmol C2H4 ∙m −2 cat ∙h −1 at 290 °C and 2.0 MPa, while the Fe 3.33 Co 1.67 K 5 /Al 2 O 3 catalysts only reach C 2 H 4 STY of 0.009 mmol C2H4 ∙m −2 cat ∙h −1 at 330 °C and 2 MPa Fe 3.33 Co 1.67 K 5 /ZrO 2 catalysts are very promising for converting the captured CO 2 and renewable H 2 to highly demanded C 2 H 4 . This work not only provides a guideline for developing efficient catalysts but also advances the mechanistic understanding of catalytic CO 2 hydrogenation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Weiwei Lu,Fengyang Ju,Kaisheng Yao,Xuefeng Wei
Conversion of CO2 into value-added fuels and chemicals faces the challenges of high overpotential, low selectivity for desired products, and sluggish multi-electron transfer kinetics. Plasmon-mediated electrocatalytic methods show potential for overcoming these problems. In this work, choosing Au nanoparticles (NPs) as the dual-functional material of the electrocatalyst and plasmonic support, methanol can be efficiently produced from CO2 reduction. The dependences of current density and Faradaic efficiency (FE) on the Au NP size, light wavelength, and light density are systematically investigated. The performance test results show that CH3OH with FE as high as 52% can be obtained at a potential of −0.8 V (vs RHE) when a 20.2 nm Au NP-modified glass carbon electrode is under excitation using 520 nm light with a light density of 120 mW/cm2. The performance results, along with the discrete dipole approximation calculation and electrochemical characterizations, suggest that the efficient activation of CO2 by plasmon-generated energetic electrons accounts for the enhanced conversion rate and the high selectivity for CH3OH production.
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RSC Advances
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2020
·Vol. 10
·期 31
·18192-18199
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IF 3.119
Zihao Yang,Taiheng Yin,Fengfan Zhang,Wei Wu,Meiqin Lin,Zhaoxia Dong,Juan Zhang
To study the microscopic dispersion state of CO2 in different ester solvents, the solubility, volume expansion coefficients and in situ Fourier transform infrared (FTIR) spectra of the CO2–ester system were measured. The results show that the solubility and expansion coefficient of CO2 in ester solvents decreases as the hydrocarbon chain increases. As the pressure increases, the infrared absorption peaks of CO2 and the functional groups characteristic of ester molecules shift, indicating that CO2 molecules interact with ester molecules and that CO2 would destroy the interactions between the ester molecules. The hydrocarbon chain length of the ester molecules has a significant effect on the infrared absorption peak of the CO2–ester system. As the hydrocarbon chain length increases, the CO2 absorption peak shift and peak shift of the carbonyl groups in the ester gradually decrease.
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PubMed
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Fang Li,Haiping Zhou,Jiajie Fan,Quanjun Xiang
Amine-functionalized graphitic carbon nitride (g-C 3 N 4 ) decorated with Au nanoparticles (CN/Au) was prepared by N 2 plasma treatment of g-C 3 N 4 powders impregnated with HAuCl 4 ·3H 2 O. Well-dispersed Au nanoparticles with a small particle size were deposited on g-C 3 N 4 nanosheets. In addition, the amino group was introduced into the CN/Au system. Without the addition of cocatalyst and sacrificial agent, CN/Au exhibited enhanced photocatalytic activity for CO 2 reduction under visible-light irradiation. CO and CH 4 evolution rates of CN/Au reached 28.3 and 1.3 μmol·h −1 ·g −1 , which were 7.6 and 2.6 times higher than those of pristine g-C 3 N 4 (CN-0), respectively. The enhanced activity can be explained by these factors. (1) The introduced amino group improved the adsorption capacity of CN/Au for CO 2 ; (2) the hot electrons generated by Au nanoparticles activated the surrounding electrons through energy transfer and caused local temperature to rise, increasing the efficiency of the photoreduction reaction of CO 2 ; (3) the Schottky junction between Au and g-C 3 N 4 promoted the migration of electrons from g-C 3 N 4 to Au nanoparticles, suppressing the recombination of the carriers. Time-of-flight secondary ion mass spectrometry confirmed the introduction of amino groups, and solid-state 13 C nuclear magnetic resonance spectra provided a support for inferring the position of the amino group.
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APPLIED ENERGY
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2020
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IF 8.848
Fuhuan Wang,Heping Xie,Tao Liu,Yifan Wu,Bin Chen
The electrochemical conversion of carbon dioxide into value-added chemicals and fuels using renewable energy sources is very promising and attractive in terms of both increasing energy utilization and environmental protection. Here we report a highly dispersed CuFe nitrogen–carbon framework as an efficient catalyst coated on carbon paper to form gas diffusion electrode for electrochemical CO 2 reduction. Such a electrode not only surmounts the disadvantage of single Cu or Fe electrode but also exhibits high selectivity, low overpotential and high energy efficiency for CO production. The as-fabricated electrode effectively converts CO 2 into CO with a low overpotential of 90 mV and high Faradaic efficiency over 90% at low applied potential range from −0.3 to −0.6 V (maximum 95.5% at −0.4 V, all potentials are converted to the reversible hydrogen electrode) with a high CO current density of 2.1 mA cm −2 at −0.5 V, as well extremely high energy efficiency of 78.3% at −0.4 V. It also exhibits robust stability during long-time electrolysis, with about 95% CO selectivity retained after 20 h electrolysis. The density functional theory computations unravel that the exceptionally high CO 2 electrocatalytic performance of the CuFe nitrogen–carbon electrode arises from its favorable local coordination environment and electronic structure giving rise to cooperative metal and pyridine N active sites for electrochemical CO 2 reduction to CO.
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FUEL
·
2020
·
IF 5.578
Jing Bai,Xiang Zhen,Kele Yan,Pan Li,Shuqi Fang,Chun Chang
Lots of thermodynamics and kinetics accelerators have been used in the process of mixture gas separation by hydrate method, but there is still lack of valid screening method for seeking reliable and effective hydrate promoters. In this work, the effects of additive molecular diameter on the hydrate phase equilibrium condition and the quantity of hydrogen bond donor and accepter of additive on the separation efficiency during CO 2 (40.0 mol%)/CH 4 hydrate formation process were investigated. The results demonstrated that the larger molecular diameter of additive in cyclopentane (CP), tetrahydrofuran (THF) and tetrahydrothiophene (THT) systems, the phase equilibrium promotion effect of additive is more significant. And the empirical equations were proposed for predicting the phase equilibrium condition of CO 2 /CH 4 hydrate under the impact of additive with different molecular diameters. Moreover, on account of the quantity of hydrogen bond donor and acceptor of additive were different, the degree of mutual dissolution between additive molecule and aqueous solution was different, so that the number of additive molecules that could participate in the formation of hydrate was different, which had a certain impact on the separation efficiency.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 27
·13806-13811
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IF 11.301
Xueyuan Wang,Muhammad Arsalan Ghausi,Rui Yang,Maoxiang Wu,Jiafang Xie,Yaobing Wang
Artificial leaves conduct photo(electro)chemical reactions for chemical and fuel production directly driven by sunlight/photovoltaic cells. Therefore, only in the presence of real-time sunlight can artificial leaves generate chemicals and fuels, limiting the prolonged production and flexible application of artificial leaves. In this work, by simply coupling a photovoltaic cell with a solid-state Zn–CO2 electrochemical cell as a new conceptual artificial leaf, continuous chemical production not only with sunlight but also in the dark was realized. In this conceptual artificial leaf, photo-generated electricity from the photovoltaic cell was pre-stored in the electrochemical cell during charge and CO2 reduction occurred in discharge. With pure CO2 supply, the conceptual artificial leaf achieved a solar-to-CO efficiency up to 15.2%, which surpassed that of the record artificial leaves and was among the highest efficiencies for artificial photosynthesis devices. This work provides possibilities for developing more universal-applied artificial leaves producing chemicals and fuels with ever-changing sunlight.
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高影响因子
COMPOSITES PART B-ENGINEERING
·
2020
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IF 7.635
Beibei Ma,Rijia Lin,Hui He,Qinghua Wu,Shuixia Chen
Hydrothermal is common process for synthesizing well-ordered mesoporous silica, however, it costs time and energy simultaneously. To improve the efficiency of synthesis process, it is necessary to propose a facile synthesis strategy with less time and energy requirement. In this study, an innovative non-hydrothermal method using NH 3 ∙H 2 O as catalyst after ripening step is developed to prepare SBA-15 with short mesochannels (SSBA-15) for the first time. The synthesis period of SSBA-15 framework was extremely shortened within 40 min under the optimized conditions (30 min of ripening step and 25% of NH 3 ∙H 2 O concentration), while obtained material exhibits well-ordered hexagonal pore structure and fine particle morphology of SSBA-15 (pore length of 250 ± 50 nm and mesopore size of 9.8 nm). This method can also be employed to synthesize conventional SBA-15 successfully. Moreover, the application of SSBA-15 as support of solid amine adsorbents on CO 2 adsorption and well-fitting of experimental CO 2 adsorption data with Avrami and intraparticle diffusion models reveal that the adsorbents combine the advantages of micro-mesoporous structure, short mesochannel and amine reagents (high affinity of CO 2 ), resulting in enhanced molecular diffusion, fast adsorption kinetics and high CO 2 adsorption capacity . Notably, the solid amine adsorbents exhibited excellent regeneration ability during ten adsorption-desorption cycles. This work opens up new opportunities in efficient preparation of materials that require hydrothermal process.
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