RSC Advances
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2020
·Vol. 10
·期 13
·7751-7757
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IF 3.119
Xiaoyan Chen,Xiaoyan Luo,Jiaran Li,Rongxing Qiu,Jinqing Lin
In this study, a variety of functionalized ILs with dual sites including amino acid group (AA) and basic anion (R) were synthesized to investigate the suppression and cooperation between the sites in CO2 absorption. The basic anions selected in this study with different basicity include sulfonate (Su), carboxylate (Ac), imidazolium (Im), and indolium (Ind). These ILs ([P66614]2[AA–R]) were applied to CO2 absorption. The results present that CO2 capacity increases first and then decreases later with the continuous increase in the activity of the anion site. Combined with CO2 absorption experiments, IR and NMR spectroscopic analyses and DFT calculation demonstrate that the ability of one site to capture CO2 would be suppressed when the activity of another site is much stronger. Thus, the cooperation of dual site-functionalized ILs and high CO2 capacity might be achieved through balancing the two sites to be equivalent. Based on this point, [P66614]2[5Am–iPA] was further synthesized by taking the advantage of the conjugated benzene ring. As expected, [P66614]2[5Am–iPA] showed capacity as high as 2.38 mol CO2 per mol IL at 30 °C and 1 bar without capacity decrease even after 10 times recycling performance of CO2 absorption and desorption.
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FOOD CHEMISTRY
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2020
·
IF 6.306
Yating Lu,Dong Li,Li Li,Tarun Belwal,Yanqun Xu,Xingyu Lin,Zhenhua Duan,Zisheng Luo
Degreening is widely used in citrus fruit to extend the market season for economic gains and increase the consumer acceptance. Elevated CO 2 was exogenously applied to Satsuma mandarins ( Citrus unshiu Marc. ) for degreening and its effect on pigment metabolism was investigated. The results revealed 15% CO 2 treatment accelerated the citrus fruit peel color change along with the chlorophyll degradation, β-cryptoxanthin and flavonoids accumulation. The expression of CitSGR , CitNYC , CitChlase , CitPPH , CitPAO and CitRCCR genes involved in chlorophyll metabolism and a set of genes involved in producing β, β-xanthophylls were up-regulated by elevated CO 2 . For flavonoid metabolism, the up-regulated expressions of CitPAL , CitCHS and CitCHI partly explained the increased total flavonoids content. These results showed that 15% CO 2 treatment improved the visual appearance of citrus fruits due to its impact on pigment metabolism and also maintained their nutritional value, thus could be employed as a potential commercial technique for citrus degreening.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
·
IF 7.864
Fan Liu,Yao Shen,Li Shen,Cheng Sun,Liang Chen,Qiaoli Wang,Sujing Li,Wei Li
To achieve low regeneration energy consumption and viscosity, a novel amino-functionalized ionic liquid [TEPAH][2-MI] combined with organic solvents has been proposed for CO2 capture in this work. The results demonstrated that the absorption loading of [TEPAH][2-MI]/N-propanol (NPA)/ethylene glycol (EG) was 1.72 mol·mol–1 (28 wt %, 257 g·L–1), which was much higher than that of monoethanolamine/water, and the regeneration efficiency was maintained at 90.7% after the fifth regeneration cycle. The viscosities of the solution were only 3.66 and 7.65 mPa·s before and after absorption, respectively, which were significantly lower than those of traditional nonaqueous absorbents. The reaction mechanism investigated via 13C NMR and quantum calculations summarized that CO2 first reacted with the amino group of [TEPAH]+ to form the carbamates through the zwitterion formation and protonation process, while CO2 reacted with the N atom of [2-MI]− to directly form the carbamate. Then, some of them further reacted with NPA and EG to form the carbonates. Moreover, Nπ and Nτ tautomers of [TEPAH][2-MI] could convert into each other continuously when CO2 was absorbed. During CO2 desorption, the carbamates and carbonates reacted with AFILH+ to decompose and released CO2 directly.
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ENERGY & FUELS
·
2020
·
IF 3.421
Yang Zhang,Xun Gong,Yang Peng,Erwei Leng,Yang Li,Xiaomin Li
In this work, sorbent pellets were prepared based on six synthetic powdery sorbents. CO2 uptake tests and kinetic analysis were carried out to screen sorbent pellets. Experimental results showed that the CO2 capture capacity of sorbent pellets was lower than that of powdery sorbents, which was mainly attributed to reduced Brunauer–Emmett–Teller (BET) specific surface area caused by pore structure damage during the pelletization process. However, the sorbent pellet CaSi75p containing 75 wt % CaO and 25 wt % Ca2SiO4 was less affected by pelletization than other sorbent pellets, which can be explained by the formation of cracks and pores that resulted from the crystalline change of Ca2SiO4 during the calcination–carbonation cycles. Among all of the sorbent pellets, CaSi75p showed the highest CO2 capture capacities of 0.531 g/g and 0.26 g/g in the first and 25th cycles. The performance of sorbent pellets was improved by adding cellulose as a pore-forming material. The reaction rate constants for all sorbents in each cycle were calculated. The experimental and kinetic data indicated that CaSi75p was an excellent sorbent even without adding cellulose.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Qingshuo Li,Hao Yang,Mengqing Li,Kexin Zhao,Baogen Duan,Chen Zhang,Hongxia Wang,Congzhen Qiao,Haibo Chang,Tong Lin
The cycloaddition of CO2 with epoxide has been a promising way to fix CO2. Developing efficient, low-cost catalysts for this reaction is highly desired. In this paper, we report a novel cocatalyst system that consists of acrylamide and KI for the synthesis of propylene carbonate using CO2 and propylene oxide as starting materials. Different amides (i.e., acrylamide, benzamide, nicotinamide, acetamide, N-isopropylacrylamide, N-tert-butylacrylamide, and N,N-dimethylacrylamide) were combined with different potassium halides to investigate their catalysis capability. KI/acrylamide showed the highest efficiency, and a synergetic effect occurred between acrylamide and KI. At the KI: acrylamide ratio of 1:1 (mol/mol) and concentration of 2.5 mol% for both of them (based on PO), the reaction reached a yield of 95.3%. The catalytic system applies to the cycloaddition reaction using different epoxides. The reaction mechanism was proposed.
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ACS Omega
·
2020
·
IF 2.87
Yanxue Gu,Yucui Hou,Shuhang Ren,Ying Sun,Weize Wu
CO2 emission from flue gas is an important issue threatening human survival. Deep eutectic solvents (DESs), which have many unique properties, have been studied for CO2 capture. However, water can be absorbed by DESs during the absorption of CO2, which may increase the energy cost during the desorption of CO2. In this work, a new kind of hydrophobic functional DES formed by polyamine hydrochloride and thymol was synthesized and used for CO2 capture. It had been found that these DESs could efficiently capture CO2 even at low partial pressures. The CO2 capacity of [TEPA]Cl-thymol (n[TEPA]Cl/nthymol = 1:3) was high up to 1.355 mol CO2/mol DES at 40 °C and 101.3 kPa. Interestingly, these DESs were still hydrophobic after saturated with CO2. The CO2 absorption capacity increased with a decrease of temperature and an increase of CO2 partial pressure. Regeneration results showed that no obvious loss in the capacity could be found after five absorption/desorption cycles of these DESs. The Fourier transform infrared (FT-IR) spectra indicated that CO2 could interact with amino in the DESs by the formation of carboxylate. Moreover, the equilibrium constant and Henry’s law constant in chemical absorption and physical absorption were studied.
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JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Shuangshuang Lin,Haiming Hua,Jiyang Li,Peng Zhang,Jinbao Zhao
We have found that the formation of passivation film plays a major role in the negative shift of the decomposition voltage in the hydrogen-generating process. Both the hydrolysis of weak acid ions and the decarboxylation reaction of carboxylate can make the LiCO 2 CH 3 produce a passivation film to inhibit the water decomposition to a certain extent. As for the LiCO 2 CF 3 without hydrolysis of weak acid ion, it can be highly possible to facilitate the introduction of CO 2 via its carboxylate specific decarboxylation reaction, and further produce lithium carbonate passivation film as well. However, the water decomposition voltage in the oxygen-producing process is more dependent on the properties of lithium salt anions. Those with strong electron-absorbing groups such as the trifluoromethyl are more likely to effectively endue the aqueous electrolyte with a high oxidative decomposition potential . Moreover, the concentration of LiCO 2 CF 3 aqueous electrolyte can reach up to 28 mol kg −1 , and hence the electrochemical stability window of this water-base electrolyte can be expanded to about 3.0 V. This work provides a new idea for the selection of high concentration lithium salt.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Jie Gao,Haizhuo Mao,Hua Jin,Chen Chen,Armin Feldhoff,Yanshuo Li
Membrane-based separation technology has evolved as a competitive approach for CO 2 capture from flue gas (mainly N 2 ). To achieve high separation performance, three partially NH 2 -, OH- and CH 3 OH- functionalized mixed-linker-ZIF-7 were successfully synthesized, and incorporated into polyether-block-amide (Pebax® 2533) polymer to form mixed-matrix membranes (MMMs). As evidenced by the CO 2 adsorption isotherms , introducing functional groups in the ZIF-7 framework was indeed beneficial for CO 2 adsorption. All MMMs composed of ZIF-7-NH 2 , ZIF-7-OH and ZIF-7-CH 3 OH offered better CO 2 /N 2 separation performance than the parent ZIF-7-Pebax® 2533 membrane, suggesting the positive effect of functionalized ZIF-7 fillers on the gas separation performance. Among the three functionalized ZIF-7 based MMMs, the ZIF-7-OH-Pebax MMMs exhibited the best performance for CO 2 /N 2 separation, which might be ascribed to the highest adsorption selectivity of CO 2 over N 2 predicted by ideal adsorbed solution theory (IAST) for ZIF-7-OH fillers. The 14% ZIF-7-OH-Pebax MMM showed high CO 2 permeability of 273 Barrer and CO 2 /N 2 separation factor of 38, which increased by 60% and 145% as compared with the neat Pebax membrane. The strategy of preparing functionalized MOFs with strong affinity for CO 2 provides an effective method to develop MMMs for highly efficient CO 2 separation.
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Chemistry-An Asian Journal
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2020
·Vol. 15
·期 14
·2153-2159
·
IF 4.056
Zhihong Zhuang,Yicheng Zhang,Liang Hu,Hangjun Ying,Weiqiang Han
Graphical A thiol-assisted one-pot method by using 3-mercaptopropionic acid (MPA) to synthesize carbon-supported metal nanoparticles catalysts for efficient electrocatalytic reduction of carbon dioxide (CO 2 RR) has been reported. The synthesized Au−MPA/C catalyst achieves a FE CO of 96.2% with a CO current density of −11.4 mA/cm 2 , which is much higher than that over Au foil or MPA-free Au/C. The typical preparation route of carbon-supported metallic catalyst is complex and uneconomical. Herein, we reported a thiol-assisted one-pot method by using 3-mercaptopropionic acid (MPA) to synthesize carbon-supported metal nanoparticles catalysts for efficient electrocatalytic reduction of carbon dioxide (CO 2 RR). We found that the synthesized Au−MPA/C catalyst achieves a maximum CO faradaic efficiency (FE) of 96.2% with its partial current density of −11.4 mA/cm 2 , which is much higher than that over Au foil or MPA-free carbon-supported Au (Au/C). The performance improvement in CO 2 RR over the catalyst is probably derived from the good dispersion of Au nanoparticles and the surface modification of the catalyst caused by the specific interaction between Au nanoparticles and MPA. This thiol-assisted method can be also extended to synthesize Ag−MPA/C with enhanced CO 2 RR performance.
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Catalysts
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2020
·Vol. 10
·期 6
·715
·
IF 3.52
Yong He,Ye Yuan,Zhihua Wang,Longlong Liu,Jiaxin Tan,Jiahao Chen,Kefa Cen
The gasification experiments of coal chars with CO2were carried out isothermally, with K, Ca, Ni, and Zn chloride catalysts, adopting a thermal gravimetric analyzer (TGA) from 800 to 1100 °C. The kinetic characteristic of the samples were described using the volumetric model (VM), the grain model (GM), and the random pore model (PRM). The morphology patterns of the samples were tested applying X-ray diffraction (XRD) and the catalytic mechanisms concerning the phase changes were proposed. The results confirm that the gasification rate and char reactivities are enhanced by K, Ca and Ni chlorides, while ZnCl2inhibited the process. The catalysis ability shows the following cation order: Ca > K > Ni > Zn. Among the models described above, PRM was proven to give the best fitting value and hence adopted to kinetics parameters calculation. The activation energies in promoting conditions were lower than that of the uncatalyzed cases. In view of the catalytic mechanism, the K metals tend to form intermediate complexes and repeatedly connect with coal char, while the Ca species may follow the oxidation-reduction mechanism and the Ni metals catalyze the gasification process.Keywords:char gasification;catalytic kinetics;catalytic mechanisms;metal chlorides
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 39
·2002092
·
IF 16.836
Facai Wei,Tingting Wang,Xiaolin Jiang,Yan Ai,Anyang Cui,Jing Cui,Jianwei Fu,Jiangong Cheng,Lecheng Lei,Yang Hou,Shaohua Liu
Currently, the precise control of the architecture and surface of functional materials for high-performance still remains a great challenge. Here, a feasible approach is presented to synchronously manipulate mesoporous surface and dimensionality of SnO 2 catalysts into hierarchically mesoporous nanosheets and nanospheres within one simple reaction system. By adjustment of the hydrophobic chain length of different fluorinated surfactants, 0D SnO 2 nanospheres with average size of 165 nm, and 2D SnO 2 ulthrathin nanosheets with thickness of 22.5 nm with the distinct dimensionalities are separately obtained (one stone, two birds), both of which are well decorated with ordered mesopore arrays on their surfaces (pore size of 16 nm). The following calcination gave rise to the formation of hierarchically mesopores (5 and 16 nm, respectively) with high crystallization and improved surface area (96.8 m 2 g −1 ). The resultant mesoporous SnO 2 nanosheets as catalyst for CO 2 electroreduction reaction (CO 2 RR) exhibit excellent selectivity, with a high Faraday efficiency (FE) of HCOOH reaching up to 90.0% at −1.3 V and C 1 FE of 97.4% at −1.2 V versus reversible hydrogen electrode, as well as long-term stability, which is among the best performance compared to reported SnO 2 materials, thanks to the collective contributions of the unique architecture and mesoporous structure.
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Hui Ning,Dianliang Guo,Xiaoshan Wang,Zhonghao Tan,Wenhang Wang,Zhongxue Yang,Linqing Li,Qingshan Zhao,Jian Hao,Mingbo Wu
Developing of economic and efficient catalysts is critical for the application of electroreduction of carbon dioxide to highly valuable chemicals. Herein, we present a facile method to synthesize N-doped hieratically porous carbon through pyrolysis of petroleum pitch followed by ammonia etching. We found mesopores are favored formation by removing of asphaltene from petroleum pitch during the carbonation process. Simultaneously, ammonia etching can not only increase the pyridinic-N content, but also upgrade the ratio of meso- to micro- pores of carbon materials. Using the N-doped hieratically porous carbon as catalyst for carbon dioxide electroreduction, the Faradaic efficiency of carbon monoxide reaches 83% at −0.9 V vs. the reversible hydrogen electrode (RHE) in 0.1 M KHCO 3 . This superior performance is attributed to the synergistic effects of highly pyridinic-N content in conjunction with the hieratically porous architecture, rendering abundant exposed and accessible active sites for electroreduction of CO 2 . Our work provides a new strategy for the large-scale preparation of high-performance, low-cost catalysts for CO 2 electroreduction.
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