MATERIALS CHEMISTRY AND PHYSICS
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2017
·
IF 2.084
Yisong Wang,Tao Du,Ziyang Qiu,Yanli Song,Shuai Che,Xin Fang
Mesoporous ZSM-5 zeolite as the adsorbent supporting material was synthesized from rice husk ash (RHA), and then impregnated with polyethylenimine (PEI) for amine functional modification. A series of adsorbents (ZSM-5-PEI-X) with different PEI loading ratios were characterized by XRD , FTIR , TGA/DTG, nitrogen adsorption-desorption, SEM and EDX techniques. The measurement of the adsorption capacity at different temperatures was indicated that ZSM-5-PEI-30 had the highest adsorption capacity at 120 °C (1.96 mmol/g). The experimental data were fitted by adsorption kinetic models and isotherm models, indicated that fractional-order model and the Dual-site langmuir model can be used to describe the adsorption mechanism and predict the adsorption performance. The high CO 2 adsorption selectivity and regeneration stability suggested that this adsorbent is a potential candidate in the adsorption and separation of CO 2 in industrial flue gas .
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CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Jing Ouyang,Chenghui Zheng,Wei Gu,Yi Zhang,Huaming Yang,Steven L. Suib
To understand the effect of porous parameters and chemical components on CO 2 capturing performance of solid state amine absorbents and their kinetic parameters, a clay mineral-based CO 2 absorbent was prepared by impregnating five different liquid amines onto SiO 2 nanowire clusters from fibrous sepiolite (Sep). Characterization was conducted by XRD, SEM, FTIR, and N 2 adsorption–desorption isotherm, CO 2 adsorption performances were measured by TGA. After acid treatment, the raw Sep mineral changed into amorphous silica nanowires, and the largest S BET of the obtained SiO 2 nanowires reached 320 m 2 /g, which was 8 times larger than the pristine mineral. Amongst the adapted amines, tetraethylenepentamine (TEPA) showed superiority in the CO 2 adsorption capacity. The optimized adsorption capacity reached 3.7 mmol/g at 75 °C from a CO 2 + N 2 mixture on a ∼50 wt% TEPA loaded SiO 2 sample, and the capacity remained 3.6 mmol/g after ten circles of adsorption/desorption tests. The pore size and pore structure of the matrix, rather than the surface area, will obviously affect the adsorption ability of the product. Kinetic parameters for the CO 2 adsorption process fitted well with a fractional-order model, confirming that the CO 2 adsorption process by the solid absorbent should be a combination of both physical and chemical reactions. Results in this article provide detailed parameters for preparing and understanding these clay mineral based solid state CO 2 absorbents.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Wenhui Li,Xiaowa Nie,Xiao Jiang,Anfeng Zhang,Fanshu Ding,Min Liu,Zhongmin Liu,Xinwen Guo,Chunshan Song
Screening of various supports reveals that Co catalysts supported on ZrO 2 and Al 2 O 3 show good initial activity for CO 2 methanation. Co/ZrO 2 and Co/Al 2 O 3 catalysts prepared by impregnation with different metal loadings were further examined comparatively. The 10Co/ZrO 2 catalyst showed high activity with CO 2 conversion of 92.5% and CH 4 selectivity of 99.9% without deactivation after 300 h time on stream (TOS). However, the 10Co/Al 2 O 3 catalyst gave a lower CO 2 conversion of 77.8% which decreased to 38.6% after 300 h TOS. The catalysts were characterized by STEM/EDS (scanning transmission electron microscopy/energy-dispersive X-ray spectroscopy), in situ XRD(X-ray diffractometer), H 2 -TPR(temperature programmed reduction), XPS (X-ray photoelectron spectroscopy), chemisorption of H 2 , CO, CH 4 , CO 2 and NH 3 -TPD (temperature programmed desorption). Re-dispersion of Co species on the ZrO 2 support during reduction by H 2 was observed by STEM/EDS. New Co-Zr phase formed on the Co-ZrO 2 interface was directly observed by TEM for the first time; the Co/ZrO 2 catalyst exhibited high stability with high activity for CO 2 conversion. In situ XRD, H 2 -TPR and XPS results indicate the promoting effect of ZrO 2 on the reduction of Co 3 O 4 to Co metal along with the negative effect of Al 2 O 3 . The oxygen vacancies on the ZrO 2 detected by XPS may help to activate CO 2 and H 2 O and resist deactivation. Co/Al 2 O 3 catalyst deactivates rapidly due to coke deposition and spinel formation.
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NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 42
·期 1
·420-428
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IF 3.269
Fenglei Liu,Shuoyu Wang,Guorong Lin,Shuixia Chen
A hyper-cross-linked resin (PDVBpc) based solid amine adsorbent was synthesized by suspension polymerization of divinylbenzene (DVB) and a Friedel–Crafts alkylation reaction, followed by impregnation with tetraethylenepentamine (TEPA), for CO2 capture. The results showed that the specific surface area and pore volume of the initial porous polymer (PDVB) remarkably increased after the Friedel–Crafts alkylation reaction, which was beneficial for increasing the loading of TEPA and the adsorption of CO2. To determine the CO2 adsorption performance, certain factors, including the TEPA loading, flow rate, CO2 concentration and adsorption temperature, were investigated. The maximum adsorbed amount of CO2 (3.11 mmol g−1) was achieved at 25 °C and a CO2 concentration of 10 vol% when the flow rate was 30 mL min−1 and the TEPA loading was 30 wt%. The optimal TEPA loading could provide sufficient active sites for CO2 capture, whereas excessive loading may lead to aggregation of the adsorbent and blockage of pore channels. An increase in temperature was unfavourable for the adsorption of CO2, because the reaction between amine groups and carbon dioxide was exothermic. A high CO2 concentration would reduce the breakthrough time but would not affect the adsorption capacity for CO2. The experimental data fitted the Avrami model well at different temperatures, which indicated that both physisorption and chemisorption contributed to the adsorption of CO2. Thus, a promising material for the adsorption of CO2 was obtained via the functionalization with TEPA of a hyper-crosslinked resin.
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ENERGY & FUELS
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2017
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IF 3.091
Xin Sun,Caili Dai,Yongpeng Sun,Mingyong Du,Tao Wang,Chenwei Zou,Jiayuan He
Hydraulic fracturing has become an important stimulation technique for low/ultralow permeability reservoirs. Supercritical CO2 (SC-CO2), as a no water phase material of fracturing fluid, receives wide attention. Current researches on SC-CO2 fracturing fluid has mainly focused on its viscous properties and superiorities. However, little attention has been devoted to the interaction between SC-CO2 fracturing fluid and the oil reservoir during the fracturing process. Besides, in a low permeability reservoir, the wettability determines the oil recovery by imbibition, which is a main way to explore oil for a matrix. Therefore, it is crucial to study the wettability alteration on a low permeability oil reservoir introduced by SC-CO2 fracturing fluid. In this study, a contact angle goniometer was introduced to characterize the wettability alteration on low permeability cores by SC-CO2 fracturing fluid. Meanwhile, nuclear magnetic resonance T2 spectra, a scanning electron microscope, and a energy dispersive spectrometer were used to explain the mechanisms of wettability alteration and the adsorption of fracturing fluid was analyzed. In addition, spontaneous imbibition tests were conducted to definite the impact of wettability alteration on oil production. The results showed that the thickener in SC-CO2 fracturing fluid, fluid filter loss, and reservoir permeability were all responsible for wettability alteration on the core surface. With the increasing thickener contents and filter loss of fracturing fluid, cores turned to be intermediate and slightly water-wet from initial strongly water-wet, which was unfavorable for oil production.Comparatively low permeability cores which consist of more micro-small pores were more likely to make treated cores oleophilic, as well. Thickener adsorption was confirmed to be the main mechanism on wettability alteration by SC-CO2 fracturing fluid, which resulted in different pore surfaces, and thus a more oleophilic cores surface. On the basis of the results of spontaneous imbibition, strong lipophilicity cores corresponded to lower oil recovery, which illustrated that wettability alteration caused by SC-CO2 fracturing fluid was not favored for oil flow.
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ACS Sustainable Chemistry & Engineering
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2017
·
IF 5.951
Yan Gao,Lu Ye,Shuyan Cao,Hu Chen,Yanan Yao,Jian Jiang,Licheng Sun
Perovskite hydroxide CoSn(OH)6 nanoparticles were synthesized and used for the first time in the photocatalytic reduction of CO2 to CO. Under mild reaction conditions and using [Ru(bpy)3](PF6)2 as the photosensitizer, a high photocatalytic efficiency of 19.3 μmol for CO evolution with a high selectivity of 86.46% was obtained. The photocatalytic activity and CO selectivity were further improved by adding weak Brönsted acids, as proton sources, to the system.
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Nano Research
·
2024
·
IF 9.5
Zhang Guiru,Ji Ning,Lyu Shiheng,Ni Baoxin,Shen Peng,Ye Ke,Wang Yuting,Jiang Xuheng,Zhang Hai,Liu Xi,Wang Yongcheng,Jiang Kun
Electrochemically converting CO 2 into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions, yet largely limited to short-chained C 1 –C 3 products. Herein, we demonstrate a tandem artificial synthesis of biodegradable polyhydroxybutyrate (PHB) plastic from CO 2 building blocks. Batch synthesis of defects-enriched Bi catalyst is firstly demonstrated by plasma bombardment and following in situ electrochemical reduction, which delivers a HCOOH Faradaic efficiency above 80% at tunable concentration from 2 to 250 mM, an energy efficiency up to 41%, and a single-pass carbon conversion efficiency up to 60%. Annular dark field and second electron microscopic analysis, density functional theory (DFT) calcualtions, coupled with H-type and solid-state electrolyzer assessments, point out the vital role of defective and/or stepped Bi surface sites in promoting CO 2 -to-HCOOH conversion. Thereafter, as-synthesized high-purity HCOOH is used as the sole carbon source for C-chain growth within microbial fermentation reactor with Ralstonia eutropha , where activated formate dehydrogenase and increased metabolites related to Calvin–Benson–Bassham cycle are found to be responsible for the enhanced polyester accumulation.
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COLLOID AND POLYMER SCIENCE
·
2024
·Vol. 302
·期 7
·1011-1023
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IF 2.2
Yang Haiyan,Gong Yue,Wang Xinzhong,Chen Yuanyuan,Yu Dajiang
Polymer resin-based solid amine are prospective adsorbents used in removing CO 2 from biogas. Two commercial resins with different porous structures, AB-8 and ADS-17, were selected as supports to explore the influence of the support structures on adsorbent performance. It was discovered that macroporous channels greatly boost CO 2 adsorption at higher PEI loadings (≥ 30%), and their influence is more critical than total pore volume or specific surface area, though their impact is minimal at low PEI loadings. ADS-17-40% PEI demonstrated outstanding CO 2 adsorption of 208 mg·g −1 in its 16th cycle under specific operating conditions. Increasing gas flow rate to 200 mL·min −1 could promote CO 2 adsorption capacity and initial adsorption rate constant ( k 0 ) calculated by the deactivation model. The highest adsorption capacity was achieved at 55 °C, when the temperature ranged from 25 to 90 °C. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Longyun Zhang,Ganghua Zhou,Gaoran Chen,Heming Wang,Qian Zhao,Weiqin Yin,Jianjian Yi,Xingwang Zhu,Xiaozhi Wang,Xin Ning
The metal–organic frameworks (MOFs) rich in porous structures and their derivatives have been widely developed and applied to heavy metal adsorption. However, little attention has been paid to the subsequent treatment and reutilization of spent MOFs adsorbents. A potential feasible strategy is to develop MOFs-derived bimetallic catalysts for energy conversion. Herein, a bimetallic Ni-Cu 2 O-Cu/C nanocomposite (Ni-Cu/C) derived from spent Cu-based MOFs (CuBTC) adsorbents was fabricated and applied to improve the performance of photocatalytic CO 2 reduction. The results demonstrate that Ni doping could improve the charge transfer dynamics. The synthesized Ni-Cu/C catalyst exhibits a high CO yield (12.45 μmol g −1 h −1 ) in the pure water system in the absence of other photosensitizers and sacrificial agents, which is 2.05 folds higher compared to Cu/C. The CO 2 conversion selectivity of the synthesized Ni-Cu/C catalyst reaches up to 99.0%. The mechanism of photocatalytic CO 2 reduction reaction was further investigated by in-situ experiments and density functional theory calculation. The in-situ FT-IR characterization show that photogenerated electrons could effectively adsorb CO 2 to produce CO 2 − and optimize *CO immediate. This work not only emphasizes the unique design of bimetallic catalyst derived from spent MOFs adsorbent, but also contributes a feasible solution to its reutilization for enhanced CO 2 conversion.
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AICHE JOURNAL
·
2025
·
IF 4
Weilin Li,Rui Ma,Zheyang Liu,Zhehao Liu,Min Zhou,Baker Rhimi,Qiang Ma,Zhifeng Jiang,Weidong Shi
The insufficient light absorption capacity and severe photogenerated carrier recombination limit the overall efficiency of photocatalysts. Herein, we designed carbon-rich poly(heptazine imide) (PHI) by copolymerization of melamine and 2,4,6-triamine-pyrimidine with KCl/KI. This material has been demonstrated to markedly enhance the utilization rate of photons while simultaneously optimizing the charge efficiency of photogenerated electrons. The carbon-rich PHI showed a higher CO₂ reduction efficiency than the PHI, with a CO generation rate reaching 46.6 μmol g −1 h −1 . To overcome the obstacle of slow mass transfer, a flow reactor was designed in-house. The CO yield on carbon-rich PHI in the home-built flow reactor was found to be as high as 153 μmol g −1 h −1 , which is 3.3 times that observed in the batch reactor. The findings of the experimental study are in alignment with the results of the theoretical modeling, which was based on the finite volume analysis method.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2012
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IF 2.237
Jun Li,Chenjia You,Lifang Chen,Yinmei Ye,Zhiwen Qi,Kai Sundmacher
To reduce the high energy consumption and equipment corrosion in conventional processes of CO2 capture with aqueous amine solutions, the mixed nonaqueous solvents of monoethanolamine (MEA), diethanolamine (DEA), and diglycolamine (DGA) with polyethylene glycol (PEG) as cosolvent were explored for CO2 capture. The dynamic experiments of CO2 absorption and desorption were carried out to evaluate the performance of the studied nonaqueous solutions. It demonstrated that the mixed solutions of amines and PEG exhibited higher CO2 cyclic capacity and regeneration efficiency compared with the only aqueous amine solutions. Especially, the solution of 3 mol/L DGA-PEG200 exhibits a high cyclic capacity of 0.438 mol CO2/mol DGA and a high regeneration efficiency of 94.6%, which indicates its great potential in industrial application. Moreover, the very low vapor pressure of PEG helps the mixed solution for CO2 capture with reduced corrosion, energy consumption, and environmental pollution.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bin Jiang,Tong Lei,Weida Chen,Meisi Chen,Chen Lu,Feng Zhang,Zhibing Zhang
Due to the proton transfer between aqueous solution of protic ionic liquids (PILs) and N,N,N’,N’-tetramethyl-1,6-hexanediamine (TMHDA), the liquid–liquid phases are gradually transformed into one phase during the absorption which is restored to two phases by carbon dioxide desorption, thus both the absorption and desorption processes were effectively intensified by phase conversion. The experimental results showed that CO 2 load of TPH (composed of TMHDA, PILs and H 2 O) was 45% higher than that of PILs-H 2 O, as well as an obvious increase of absorption rate. Moreover, the regeneration energy consumption of TPH was only 2.10 GJ/tonCO 2 . The spectral analysis and molecular dynamics simulations revealed that the proton transfer was the key of phased conversion, and it was regulated by the synergistic interaction between PILs and TMHDA during the CO 2 capture process. This kind of phase conversion strengthening absorbent with low viscosity is a useful way to achieve low energy carbon dioxide capture.
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