JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2020
·Vol. 31
·期 22
·20495-20512
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IF 2.22
Jiang Haopeng,Li Xin,Chen Songtao,Wang Huiqin,Huo Pengwei
g-C 3 N 4 quantum dots (CN QDs)-decorated mesoporous CeO 2 composite photocatalyst was prepared by hydrothermal method. The characterized results exhibit that the CN QDs are successfully coupled with mesoporous CeO 2 , and the photoelectronic response is effectively enhanced. The photocatalytic activity was tested by CO 2 reduction, and the results showed that when the loading of CN QDs was 0.75 wt%, the composite photocatalyst has the best photocatalytic activity. After 10 h of UV irradiation, the yields of CO and CH 4 were 22.48 µmol/g and 15.81 µmol/g, respectively. Some of the electrons generated within m-CeO 2 participated in the CO 2 reduction reaction and some were transferred to CN QDs through the two-phase interface to participate in the CO 2 catalytic reaction. The oxygen vacancies in m-CeO 2 can adsorb CO 2 and the introduced CN QDs can excite more oxygen vacancies with m-CeO 2 heterostructure, thereby adsorbing more CO 2 and photoreduction electrons.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Jianfei Xiao,Yuan Wang,Tian C. Zhang,Shaojun Yuan
A novel porous carbon derived from glucose and dicyandiamide incorporated with reduced graphene oxide (rGO) was prepared for CO 2 capture and supercapacitors . In this synthesis, one-pot hydrothermal and KOH activation were employed to obtain reducing graphene oxide/N-doped porous carbon (rGO/NPC) composites. Among the rGO/NPC composites derived, the sorbent rGO/NPC-600-2-1 (1 represents the addition amount of graphene oxide is 1% of the total mass of glucose and dicyandiamide, 2 represents the mass ratio of potassium hydroxide to the precursor of carbon composite material is 2 and 600 means activation temperature is 600 °C) had a large surface area of 865.1 m 2 g −1 , a rich nitrogen doping amount of 7.07 wt%, and a high CO 2 capture ability of 5.77 mmol/g at 298 K. Additionally, the as-synthesized rGO/NPC-600-2-1 was used as a supercapacitor electrode, providing a specific capacitance 210.8 F g −1 in 6 M KOH electrolyte under ambient conditions and excellent charge and discharge long cycle stability (circa 100% capacitance retention at a current density of 10 A g −1 after 10000 cycles). Even at a high current density of 20 A g −1 , a capacity of 141.1 F g -1 is still maintained. The results above suggested that the rGO/NPC composites are applicable candidates for both electrochemical energy storage and CO 2 capture.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Hucheng Zhang,Jianji Wang
In recent years, metal–organic frameworks (MOFs) have been explored as emulsifiers for the fabrication of Pickering emulsions and then used for hybrid material synthesis and interface catalysis. Nevertheless, stimuli-responsive Pickering emulsions stabilized by MOFs have been rarely reported so far, although they are of great importance for fundamental research studies and practical applications. Herein, for the first time, triethylenetetramine (TETA)-functionalized MOFs (ZIF-90/TETA) have been designed, synthesized, and used for fabricating CO2-/N2-response Pickering emulsions. It is shown that even at the ZIF-90/TETA content of 0.25 wt %, the functional MOF can still efficiently emulsify n-hexane and water to form a high internal phase Pickering emulsion. Importantly, the Pickering emulsion can be easily and reversibly switched between emulsification and demulsification by bubbling of CO2 and N2 alternatively at atmospheric pressure. The possible mechanism of the CO2/N2 switchable emulsion is investigated by zeta potential, water contact angle, interfacial tension, 13C NMR spectroscopy, and an optical microscope. It is found that the acid–base reaction of CO2 with TETA anchored on the surface of ZIF-90 leads to the production of hydrophilic ammonium bicarbonate and carbamate, which results in the emulsification of the Pickering emulsion. However, when N2 is bubbled to remove CO2, the reverse reaction takes place to cause the demulsification of the Pickering emulsion. Moreover, the CO2/N2 switchable Pickering emulsion has been successfully used as a microreactor for Knoevenagel reactions to demonstrate a highly efficient integration of chemical reaction, product separation, and ZIF-90/TETA recycling for a sustainable chemical process.
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Chemistry-An Asian Journal
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2020
·Vol. 15
·期 14
·2153-2159
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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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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
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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 Materials Chemistry A
·
2020
·Vol. 8
·期 14
·6524-6531
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IF 11.301
Jiadong Li,Feng Wei,Changchang Dong,Wei Mu,Xiaojun Han
Indium oxide (In2O3)-based photocatalysts have great potential in photocatalytic CO2 reduction. Nevertheless, their photocatalytic activity is inhibited by rapid electron–hole recombination. Hence, a novel Z-scheme ternary hierarchical ZnFe2O4/RGO/In2O3 photocatalyst is fabricated for photocatalytic conversion of CO2 to CO and CH4. The CO production rate reaches up to 35.4 μmol g−1 under 4 h of illumination using a 20ZFO/10RGO/IO catalyst, which is 3.9 times and 9.8 times higher than those using bare In2O3 and bare ZnFe2O4, respectively. The CH4 production rate is 7.8 μmol g−1, which is 4.3 fold and 2.4 fold higher, respectively, compared to those from bare In2O3 and bare ZnFe2O4. The enhancement of photocatalytic CO2 reduction was ascribed to a Z-scheme mechanism of the hierarchical catalysts by introducing RGO in-between In2O3 and ZnFe2O4 to promote charge separation and realize efficient utilization of the high-energy electrons and holes. The oxygen-defect of ZnFe2O4 also facilitates the adsorption and activation of CO2. This work provides new insights to design ternary In2O3-based hierarchical photocatalysts with a rational Z-scheme photocatalytic mechanism to improve the CO2 conversion efficiency.
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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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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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RSC Advances
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2020
·Vol. 10
·期 13
·7751-7757
·
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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