CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xuandong Wang,Jie He,Liang Mao,Xiaoyan Cai,Chuanzhi Sun,Mingshan Zhu
Photocatalytic CO 2 conversion to valuable fossil fuels has been demonstrated to be a promising approach to reduce emissions of CO 2 and produce renewable energy, which primarily depends on developing the high efficiency of charge separation photocatalysts. Herein, CsPbBr 3 , one typical kind of all-inorganic perovskite nanocrystal, is immobilized on monolayer MoS 2 nanosheets to construct a new and ideal CsPbBr 3 /MoS 2 photocatalyst in the application of CO 2 photoreduction. In comparison with pure CsPbBr 3 , CsPbBr 3 /MoS 2 heterostructures possessed a specific electric field to more efficiently separate charges and generated more active sites for facilitating CO 2 activation, resulting in 3.0 and 2.4 times yields for CO 2 photoreduction to CH 4 and CO, respectively. Detailed characterization methods such as photoluminescence, surface photovoltage spectroscopy and theory calculations indicate the vivid illustrations of photogenerated carries separation which contributes to improving photocatalytic CO 2 conversion efficiency. The present investigation is anticipated to provide a new way for fabricating highly efficient perovskite-based photocatalyst in solar-energy-driven applications.
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ENERGY
·
2020
·
IF 6.082
Rujie Wang,Shanshan Liu,Qiangwei Li,Shihan Zhang,Lidong Wang,Shanlong An
Blended amine solvents are considered potential alternatives to monoethanolamine for CO 2 capture, for the fast absorption kinetics of primary/secondary amine and low regeneration penalty of tertiary amine. In this research, blended amine solvents comprising N,N-dimethylcyclohexylamine (DMCA) and N-methylcyclohexyamine (MCA) were proposed. CO 2 absorption increased the polarity of the products and ensured the absorbent remained homogenous throughout the absorption/desorption cycles. Through quantum chemical calculation, the low stability of MCA-carbamate was confirmed by a ΔΔG 3 value of −6.41 kcal/mol, and a possible reaction route from carbamate to bicarbonate was revealed. Thus, the CO 2 capacity of DMCA-MCA reached 0.875–0.985 mol CO 2 /mol amine. Moreover, MCA exhibited considerably low forward energy barrier for zwitterion formation (2.7 kcal/mol), and the CO 2 absorption of DMCA could be accelerated through the proton transfer reaction with the MCA-zwitterion. Accordingly, the total mass transfer coefficient of CO 2 in DMCA-MCA approached 2.02 × 10 −10 mol/cm 2 s Pa, which was 1.2-fold higher than that of 5 M MEA. The total regeneration energy of DMCA-MCA blend was estimated at 2.20 GJ/t CO 2 , which was 44.9% lower than 5 M MEA. This study developed a novel DMCA-MCA blended solvent with rapid absorption rate, huge CO 2 capacity and efficient regeneration for CO 2 capture.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
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IF 2.627
Bo-Yun Liu,Min-Jie Chen,Liang Yang,Bo Zhao,Tao Xia,Gang-Gang Chang
The engineering of highly efficient and stable heterogeneous catalysts for catalytic conversion of CO 2 to high value-added products is highly desirable but presents a great challenge. Herein, we reported the synthesis of a series of multifunctional IL@H-Zn/Co-ZIF composite catalysts with a unique porous hollow capsule structure and encapsulated amino-functionalized ionic liquids (ILs). The unique hollow capsule structure of IL@H-Zn/Co-ZIF provides sufficient space for loading active ILs ([C 2 NH 2 Mim + ][Br − ]) and fast mass transfer of substrate molecules during catalysis. Furthermore, the microporous Zn-ZIF shell can effectively avoid the leaching of active ILs. Benefiting from the unique hollow structure, the resultant IL@H-Zn/Co-ZIF demonstrated excellent catalytic performance (>95% yield), and good recyclability (still remained about 90% activities after 5 cycles) when applied in the CO 2 cycloaddition reaction under solvent and co-catalyst free conditions.
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ENERGY & FUELS
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2020
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IF 3.421
Cui-Ping Ye,Rui-Nan Wang,Xia Gao,Wen-Ying Li
To screen the efficient media for CO2 capture of flue gas from power plants, a strategy for improving the CO2 capture capacity by dual functionalized ionic liquids (ILs) with multiple active sites is proposed. Three phosphonium dual functionalized ILs ([aP4443][2-Np], [aP4443][2-Op], and [aP4443][Triz]) have been prepared. The sorption capacities of the synthesized ILs under pure CO2 atmosphere and the supported ILs under different loading amounts from 10 to 50%, temperatures of 30–80 °C, and CO2 partial pressure varied from 10 to 15% were determined. Fourier transform infrared (FTIR) spectroscopy was applied to reveal the interaction between CO2 and ILs, and the pseudo-second-order model and the intraparticle diffusion model were used for a better understanding of the CO2 adsorption behavior. The results showed that a high capacity up to 1.88 mol of CO2/mol of IL for [aP4443][2-Np] is achieved, and 30% IL–MCM-41 can reach 3.19 mmol/g with excellent reversibility under the atmosphere of CO2:N2 (15%:85%) at 30 °C and 0.1 MPa. Raising the temperature or decreasing the CO2 concentration is not conducive to improving the CO2 capacity. FTIR spectroscopy demonstrated that the amino and hydroxyl react with CO2 to form NHCOO– or CO3–. Combined with the activation energy calculation, the kinetic analysis revealed that the CO2 capture of supported ILs is an internal diffusion controlled physical adsorption.
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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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Membranes
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2021
·Vol. 11
·期 2
·118
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IF 4.106
Chunwei Zhang,Menglong Sheng,Yaoqiang Hu,Ye Yuan,Yulong Kang,Xiao Sun,Tao Wang,Qinghua Li,Xisen Zhao,Zhi Wang
CO2enhanced oil recovery (CO2-EOR) technology is a competitive strategy to improve oil field economic returns and reduce greenhouse gas emissions. However, the arbitrary emissions or combustion of the associated gas, which mainly consists of CO2and CH4, will cause the aggravation of the greenhouse effect and a huge waste of resources. In this paper, the high-performance facilitated transport multilayer composite membrane for CO2/CH4separation was prepared by individually adjusting the membrane structure of each layer. The effect of test conditions on the CO2/CH4separation performance was systematically investigated. The membrane exhibits high CO2permeance of 3.451 × 10−7mol·m−2·s−1·Pa−1and CO2/CH4selectivity of 62 at 298 K and 0.15 MPa feed gas pressure. The cost analysis was investigated by simulating the two-stage system. When the recovery rate and purity of CH4are 98%, the minimum specific cost of separating CO2/CH4(45/55 vol%) can be reduced to 0.046$·Nm−3CH4. The excellent short-to-mid-term stability indicates the great potential of large industrial application in the CH4recovery and CO2reinjection from oilfield associated gas.Keywords:oilfield associated gas;CO2capture;multilayer composite membrane;facilitated transport;CO2/CH4separation
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhenggang Wang,Jianwei Yuan,Renhao Li,Haipeng Zhu,Jingui Duan,Yanan Guo,Gongping Liu,Wanqin Jin
Compared with traditional separation methods, membrane-based technology shows advantages in energy efficiency for natural gas purification. To overcome the performance trade-off of conventional polymeric membranes, in this study, ZIF-301 MOF was employed as novel filler to fabricate 6FDA-DAM polyimide mixed-matrix membranes (MMMs) for CO 2 /CH 4 separation. A solvent exchange approach was proposed to remove the high-boiling-point solvent used for fabricating the MMMs. The microstructures and physico-chemical properties of the ZIF-301 fillers and ZIF-301/6FDA-DAM MMMs were characterized by SEM, EDX, XRD, IR, TGA, DSC and high-pressure sorption isotherms. The CO 2 /CH 4 transport properties through the MMMs were evaluated by permeation measurement at various feed pressures and analyzed by solution-diffusion model. The results showed that the incorporation of ZIF-301 into 6FDA-DAM enhanced both the CO 2 permeability and CO 2 /CH 4 selectivity, attributing to the preferential CO 2 sorption and aperture molecular sieving effect of the ZIF-301 filler. The MMM with optimal ZIF-301 loading of 20 wt% exhibited CO 2 permeability of 891 barrer and CO 2 /CH 4 of 29.3 that surpassed the 2008 Robeson upper-bound, suggesting that ZIF-301 based membrane could be a potential candidate for natural gas purification.
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Reaction Kinetics Mechanisms and Catalysis
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2020
·Vol. 132
·期 1
·417-429
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IF 1.52
Xie Qi,Miao Changxi,Lei Tianqi,Hua Weiming,Yue Yinghong,Gao Zi
Dehydrogenation of ethane assisted by CO 2 has been investigated over Au catalyst supported on Y-doped CeO 2 nanorod. The catalysts were characterized by XRD, TEM, N 2 adsorption, XPS, TG, H 2 -TPR and Raman spectroscopy. Enhanced activity can be obtained after the proper Y doping. The optimal catalyst Au/Ce 0.9 Y 0.1 exhibits an ethane conversion of 20.9% and nearly 100% selectivity to ethylene without any evident tendency of deactivation in 50 h. The reducibility of surface oxygen species is found to play a key role in the dehydrogenation assisted by CO 2 , which can be improved by proper Y doping into CeO 2 nanorod. The promoting effect of CO 2 on activity is evident over Au/Ce 0.9 Y 0.1 catalyst, due to the quick transformation of H 2 product into H 2 O by the reverse water gas shift reaction. The catalyst stability is also improved by the addition of CO 2 , attributed to the elimination of coke by Bouduoard reaction.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Shasha Wang,Junfeng Miao,Mengshuai Liu,Lihui Zhang,Zhenfa Liu
Novel microporous carbon xerogels (CX-HMTAs) with different morphologies and well-developed porosity were successfully fabricated. The hierarchical pore, surface structure, and nitrogen content could be easily controlled by adjusting the amount of hexamethylenetetramine (HMTA). The samples as-obtained exhibited high micropore volume and large specific surface area, which were applied as supercapacitor electrodes and CO 2 capture materials. The CX-HMTA4 with a moderate concentration of HMTA (0.72 %) afforded the highest CO 2 adsorption capability with 4.21 mmol g −1 at 273 K and 1 bar, and excellent ideal adsorption solution theory (IAST) selectivity with 70 for CO 2 /N 2 capture at 298 K. Moreover, the CX-HMTA4 were simultaneously conducted as a supercapacitor electrode, and gave a maximum specific capacitance of 161 F g -1 and high stability (retained 99.4 % capacity after 1000 cycles) in 6 M KOH electrolyte at 1 A g -1 , showed a great advance when compared with most reported benchmark carbon materials. The multifunctional porous carbon materials presented herein were facilely prepared without any activation, exhibiting considerable potentials for large-scale gas adsorption/separation and electrochemical energy storage.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ke Guo,Xiaoli Zhu,Lianlian Peng,Yanghe Fu,Rui Ma,Xinqing Lu,Fumin Zhang,Weidong Zhu,Maohong Fan
The conversion of CO 2 into valuable chemicals utilizing solar energy is one of the most promising approaches to solve the problems associated with global warming and energy shortage. Considering more and more covalent organic frameworks (COFs) that have been reported, the great potential of COFs as photocatalysts for CO 2 reduction is still appreciated to a limited extent. In the current work, Ru nanoparticles (NPs) loaded ketoamine-based COF (TpPa-1) catalysts, named Ru/TpPa-1, were developed for the photocatalytic reduction of CO 2 upon visible-light irradiation for the first time. Compared with TpPa-1, Ru/TpPa-1 catalysts exhibit a significantly enhanced activity for the photoreduction of CO 2 . In combination with the results from some extensive characterizations, it is found that the interactions between the Ru NPs and TpPa-1 can enhance the visible-light harvesting and create a new way to extend the service life of photo-generated charge carriers via facilitating the electron transfer through the loaded Ru NPs. The current investigation, therefore, provides a photocatalytic approach for CO 2 fixation, enriches the theory of photocatalysis, and enlarges the application of COF-based materials.
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Journal of Materials Chemistry A
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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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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ge Xie,Nuoya Zhou,Yujie Gao,Shuo Du,Hongyao Du,Juan Tao,Lianbin Zhang,Jintao Zhu
Acceleration of skin wound healing is an important aspect of wound treatment. The use of carbon dioxide (CO 2 ) has been recognized as one of the most effective ways to improve microcirculation and to benefit wound healing, while the need of the specialized equipment and the uncontrollable delivery of gas CO 2 might restrict such strategy in wide applications. Herein, we develop a photothermal hydrogel for the on-demand and localized delivery of CO 2 to accelerate skin wound healing by combining thermoresponsive block copolymer (BCP) of Pluronic F127 and carbon nanoparticles (CNPs) with amino groups, which can be used for loading CO 2 precursor of bicarbonate for controlled release. We show that by rationally optimizing the content of the thermoresponsive BCP in the photothermal hydrogel, a liquid-to-solid transition triggered by the body temperature can be achieved. Under light irradiation, the CNPs can convert light into heat, triggering the decomposition of the bicarbonate, and the photothermal hydrogel can thus locally release CO 2 in the wound site. Wound healing can be accelerated by improving local microcirculation disturbance and increasing tissue oxygen concentration. This study provides a new opportunity for local CO 2 supplement for accelerating wound healing.
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