LANGMUIR
·
2022
·
IF 4.331
Yangguan Chen,Guorong Lin,Haorui Liu,Jinrui Zhang,Shuixia Chen
Solid amine adsorbents are promising materials to mitigate global warming. In this study, a commercially available melamine-formaldehyde sponge was adopted as a support to prepare a kind of solid amine adsorbent using polyethylenimine as a functional component and ethylene glycol diglycidyl ether as a cross-linker. The adsorbent, with abundant tunnels and a high amine loading amount, had a high adsorption capacity. When the amine loading was 89.6 wt%, the as-prepared adsorbent showed a high adsorption capacity of 7.29 mmol/g at 20 °C in the presence of water. The spent adsorbent could be easily regenerated by heating it at 90 °C, resulting in lower energy consumption. It has been proved by the Avrami model that physical and chemical adsorption coexist in the adsorption of CO2 on this adsorbent. Simulation with the intraparticle diffusion model has revealed that the rate-controlling step in the adsorption process was the gas film diffusion period when the adsorption temperature was below 30 °C, while it was the adsorption equilibrium period when the adsorption temperature was above 30 °C.
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高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 101
·期 5
·2510-2517
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IF 2.5
Wenan Sun,Zhongcong Zhao,Junjie Xiong,Yujian Rong,Jin Bao,Baolei Liu,Zhihao Chen
The hydrophobic associating polymer (MXN-1) was used as a foam stabilizer with optimized supporting additives to solve the problem of high friction in foam fracturing fluid. The basic formula was 0.3% MXN-1 + 0.08% sodium dodecyl sulphate (SDS) + 0.3% B-14 + 1% potassium chloride (KCl) + 0.03% ammonium persulphate (APS). The friction reduction, sand-carrying capacity, gel-breaking performance, and core damage of the fracturing fluid system were studied. The results showed that the proposed system had a unique friction reduction advantage compared with the cross-linked guar gum foam fracturing fluid, and the friction reduction percent reached 62% at a high flow rate. The surface tension of the gel breaking solution was lower than 25 mN/m, and the residue content was about 7 mg/L.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Caili Dai,Peng Liu,Mingwei Gao,Zhiyuan Liu,Changlong Liu,Yining Wu,Xiangyu Wang,Shichun Liu,Mingwei Zhao,Hui Yan
Supercritical carbon dioxide (SC-CO 2 ) dry fracturing is considered to be an ideal choice for low permeability, tight and other unconventional reservoir development, because SC-CO 2 has the characteristics of inhibiting water sensitivity damage and improving flowback efficiency. However, the low viscosity of SC-CO 2 limits its application. At present, the most effective way is to thicken CO 2 with thickeners. In this work, seven heptadecafluorodecyl acrylate/styrene (HFDA/STY) copolymers were synthesized, their solubility and thickening properties in SC-CO 2 were evaluated. With the increase of phenyl content in the copolymer, the dissolution pressure and thickening ability of the copolymer in SC-CO 2 increased. The solubility pressure of P(HFDA 0.70 -co-STY 0.30 ) reached 22.2 MPa at 5 wt%, and the viscosity of SC-CO 2 was increased by 297 times. The increase of temperature leads to the increase of molecular thermal motion, which leads to the increase of solubility pressure but the opposite of thickening ability. Molecular dynamics (MD) simulation method was used to reveal the thickening mechanism of SC-CO 2 . The MD simulation results show that fluorocarbon headgroups in copolymers can significantly reduce its dissolution pressure and phenyl group plays the key role in improving the viscosity of CO 2 , which is consistent with laboratory experiment results.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Shujie Liang,Gongchang Zeng,Xiaohui Zhong,Hong Deng,Zuqi Zhong,Zhang Lin,Jianlin Huang
Photoreduction of diluted CO 2 is an effective strategy for the sustainable and environmentally friendly development of energy. In this study, lattice strain in NiSe is modulated through the control of the Ni concentration for the photoreduction of diluted CO 2 . Refined XRD data and the results of the Williamson–Hall analysis indicate that the lattice strain is induced by lattice distortion caused by an absence of Ni atoms in the crystal lattice . In pure CO 2 , the cumulative CO yield and selectivity of Ni 1−x Se nanoflowers reached approximately 19.39 µmol and 90.7 % in 3 h, respectively. For lower CO 2 concentrations of 0.1 and 0.05 atm, the CO selectivity of Ni 1−x Se was approximately 72.7 % and 61.7 %, respectively. On characterization of the synthesized nanoflowers , we deduced that the lattice-strained Ni 1−x Se exhibited a favorable electronic band structure that improved the separation efficiency of the photogenerated carriers . DFT calculations results revealed that the lattice strain significantly facilitated the adsorption and activation of CO 2 , which resulted in highly efficient CO 2 photoreduction. This study provides an effective strategy for the design and synthesis of high-performance catalysts based on the modification of their crystal structures.
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Processes
·
2021
·Vol. 9
·期 9
·1638
·
IF 2.847
Yonggang Ma,Xin Chen,Dehui Han,Zhe Zhao,Wenting Lu
A CO2-responsive composite of multiwall carbon nanotube (MWCNT) coated with polydopamine (PDA) and polydimethylamino-ethyl methacrylate (PDMAEMA) was prepared. The PDA was first self-polymerized on the surface of carbon nanotube. 2-bromoisobutyryl bromide (BiBB) was then immobilized by PDA and then initiated the ATRP of DMAEMA on the carbon nanotube surface. The resulting composite was characterized by Fourier-transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). The CO2-responsive test was performed by bubbling CO2into the mixture of MWCNT-PDA-PDMAEMA composite in water. A well-dispersed solution was obtained and the UV-Vis transmittance decreased dramatically. This is attributed to the reaction between PDMAEMA and CO2. The formation of ammonium bicarbonates on the surface of carbon nanotubes leads to the separation of nanotube bundles. This process can be reversed as the removal of CO2by bubbling N2.Keywords:CO2-responsive;polymer;multiwall carbon nanotube (MWCNT);composite;ATRP
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Mengyang Xu,Xiaoxue Zhao,Haopeng Jiang,Songtao Chen,Pengwei Huo
Converting carbon dioxide into valuable chemicals is seen as a promising strategy for slowing global warming while enriching energy supplies. Photocatalysts derived from Metal-Organic Frameworks (MOFs) can not only overcome the problem of poor stability of MOFs, but also inherit the advantages of MOFs to some extent. Herein, carbon doped In 2 O 3 (C-In 2 O 3 ) hollow tubular is synthesized by calcination of MIL-68(In) as sacrificial template. Then C-In 2 O 3 and g-C 3 N 4 are hydrothermal to obtain C-In 2 O 3 /g-C 3 N 4 heterojunction . The unique hollow tubular structure, carbon doping and type-II heterojunction of C-In 2 O 3 /g-C 3 N 4 expand the light absorption capacity and promote the separation of photogenerated electron-hole pairs, thus significantly improve the activity of photocatalytic reduction of CO 2 . Among them, C-In 2 O 3 /g-C 3 N 4 -5 shows the highest CO 2 reduction activity towards CO (153.42 μmol/g/h) and CH 4 (110.31 μmol/g/h).
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ChemSusChem
·
2021
·Vol. 15
·期 1
·e202102010
·
IF 8.928
Han Zhang,Yu Yang,Yongxiang Liang,Jun Li,An Zhang,Han Zheng,Zhigang Geng,Fengwang Li,Jie Zeng
Graphical Lend me your EORs : Electrochemical oxidation-reduction (EOR) processing of a Cu-based metal-organic framework results in the formation of sub-nanometer Cu clusters that retains the organic linkers for highly selective and durable electrosynthesis of methane from the electrochemical CO 2 reduction reaction. Electrochemical CO 2 methanation powered by renewable electricity provides a promising approach to utilizing CO 2 in the form of a high-energy-density, clean fuel. Cu nanoclusters have been predicted by theoretical calculations to improve methane selectivity. Direct electrochemical reduction of Cu-based metal-organic frameworks (MOFs) results in large-size Cu nanoparticles which favor multi-carbon products. This study concerns an electrochemical oxidation-reduction method to prepare Cu clusters from MOFs. The derived Cu clusters exhibit a faradaic efficiency of 51.2 % for CH 4 with a partial current density of >150 mA cm −2 . High-resolution microscopy, in situ X-ray absorption spectroscopy, in situ Raman spectroscopy, and a range of ex situ spectroscopies indicate that the distinctive CH 4 selectivity is due to the sub-nanometer size of the derived materials, as well as stabilization of the clusters by residual ligands of the pristine MOF. This work offers a new insight into steering product selectivity of Cu by an electrochemical processing method.
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高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 1
·243-257
·
IF 2.081
Zhang Wenfei,Zhou Qulan,Qi Ji,Li Na
Cu 2 O films were prepared using an improved solution immersion method, whereas ZnO/Cu 2 O films were prepared using an electrodeposition method. Then, the pure Cu 2 O film electrodes and ZnO/Cu 2 O film electrodes were used to reduce CO 2 to CH 3 OH. The crystal structure, morphology, particle size, and specific surface area of pure Cu 2 O films prepared under different immersion times and ZnO/Cu 2 O films prepared under different deposition times and Zn 2+ concentrations were analyzed using X-ray diffraction, scanning electron microscopy, and Brunauer–Emmett–Teller analysis. The electrolytic activity of the pure Cu 2 O film electrodes and ZnO/Cu 2 O film electrodes were studied. Under the same reaction conditions, the ZnO/Cu 2 O film electrode with the Zn 2+ concentration of 0.05 M and the deposition time of 30 min had the highest total CH 3 OH yield of 315.656 μmol/cm 2 and the fastest formation rate of 52.609 μmol/(cm 2 h), and its faradaic efficiency was 45%, which was remarkably higher than that of pure Cu 2 O film electrodes under the same reaction conditions. This study highlighted that ZnO nanoparticles had a very good promotion of electrolytic CO 2 reduction on Cu 2 O film.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Debo He,Wenji Ruan,Jibiao Li,Jiupai Ni,Chengsheng Ni
The large-scale integration of intermittent renewable energies into the power grid could reduce the CO 2 emission from the combustion of fossil fuel, but it requires energy storage techniques to balance the energy production and demand. The electrolysis of CO 2 that converting electricity into chemicals/fuels provides a sustainable way of energy storage and CO 2 reduction. Solid oxide electrolysis cell (SOEC) operating at around 800 °C was able to provide highly efficient transformation of CO 2 because the high temperature was able to decrease the energy demand and increase the activation of CO 2 than room temperature electrolysis. In this study, Mo-doped ferrite perovskite , La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 , was studied as the cathode of an SOEC for the direct electrolysis of CO 2 at 800 °C. Cell with La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode showed a significantly higher current density during CO 2 electrolysis than the one with La 0.55 Sr 0.45 FeO 3 cathode. Compared with the parent La 0.55 Sr 0.45 FeO 3 cathode that will subject to a superficial decomposition into Fe 0 and SrO or SrCO 3 at an elongated cathodic bias of − 1.4 V, Mo-doping will induce the production of Ruddlesden-Popper phase ( e.g. (La,Sr) 2 (Mo,Fe)O 4 , Fe-Mo-O oxides and Fe 0 ). La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode was found to an unobvious current decrease at − 1.1 V, but a cell degradation was found under a high bias of − 1.4 V. During the 97 h’ aging under a cathodic bias (−1.4 V), the reduced molybdenum cation in La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 was found to be less mobile than Fe 3+/2+ , La 3+ or Sr 2+ , and the perovskite with Fe-deficit region were also found to be important for the activation of CO 2 and dissociation of CO in the electrochemical process.
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Advanced Science
·
2021
·Vol. 9
·期 4
·2104138
·
IF 16.806
Aya Gomaa Abdelkader Mohamed,Enbo Zhou,Zipeng Zeng,Jiafang Xie,Dunfeng Gao,Yaobing Wang
Electrochemical CO 2 reduction (ECR) is one of the promising CO 2 recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO 2 to formate, while CO evolution selectivity is largely controlled. Selective formate is detected with Faradaic efficiency (FE HCOOH ) of ≈95% at an outstanding partial current density of 47 mA cm –2 in a conventional H-Cell. Zn(Pb) is further investigated in an electrolyte-fed device achieving a superior conversion rate of ≈100 mA cm –2 representing a step closer to practical electrocatalysis. The in situ analysis demonstrates that the Pb incorporation plays a crucial role in CO suppression stem from the generation of the Pb–O–C–O–Zn structure rather than the CO-boosted Pb–O–C–Zn. Density functional theory (DFT) calculations reveal that the alloying effect tunes the adsorption energetics and consequently modifies the electronic structure of the system for an optimized asymmetric oxo-bridged intermediate. The alloying effect between Zn and Pb controls CO selectivity and achieves a superior activity for a selective CO 2 -to-formate reduction.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Jiehong He,Shaoshuai Chang,Haoran Du,Bo Jiang,Wenzhao Yu,Zhenwu Wang,Weiwei Chu,Lanfang Han,Jian Zhu,Hexing Li
The hydrogenation of carbon dioxide (CO 2 ) to formic acid (FA) has been considered as a promising approach to utilize CO 2 and realize carbon-neutral energy supply. Development of efficient heterogeneous catalysts is an interesting yet challenging task. In this work, a reliable amorphous NiRu 0.1 B catalyst was presented and displayed a sufficient catalytic activity for the hydrogenation of CO 2 into FA. The amorphous structure of catalysts provided abundant dangling bonds and unsaturated atoms for enhancement of the reactant gas adsorption. Moreover, the electron-donating effect of B element is crucial for creating active electron-rich metal centres, which is proposed to facilitate the formation of the M H for activating CO 2 molecules. Owing to synergistic effect of amorphous structure and electron-donating, amorphous NiRu 0.1 B catalysts show a higher activity and stability than that of Ni-B and crystalline Ni-B at low temperature. This work not only exhibits a facile method to prepare amorphous bimetallic catalysts, also demonstrates that amorphous metals are promising heterogeneous catalysts for the hydrogenation of CO 2 to FA.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2021
·Vol. 27
·期 3
·269-277
·
IF 0
Shi Han,Cheng Yingying,Kang Peng
The metal oxide/nitrogen-doped carbon (NC) compounds zirconium oxide/NC (ZrO 2 /NC) and cerium oxide/NC (CeO 2 /NC) were synthesized via the pyrolysis of polyaniline on the metal oxide surface. The characterization of the ZrO 2 /NC and CeO 2 /NC catalysts showed more active CO 2 reduction reaction activity than that of NC catalyst without metal oxide. Gas chromatography analysis revealed that CO and H 2 were the primary products, and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography. The maximum Faraday efficiency of ZrO 2 /NC reached 90% at − 0.73 V (vs. RHE), with the current density of CO at 5.5 mA/cm 2 ; this Faraday efficiency value was higher than that of NC (41%), with the current density of CO at 3.1 mA/cm 2 . The interaction between the metal oxide and carbon allowed the efficient formation of defect sites, especially imine-type nitrogen, strengthening the adsorption of the key reaction intermediate CO 2 •− and thus promoting the CO 2 reduction reaction.
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