1. |
- Dahlin, Sandra, et al.
(author)
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Effect of biofuel- and lube oil-originated sulfur and phosphorus on the performance of Cu-SSZ-13 and V2O5-WO3/TiO2 SCR catalysts
- 2021
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In: Catalysis Today. - : Elsevier B.V.. - 0920-5861 .- 1873-4308. ; 360, s. 326-339
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Journal article (peer-reviewed)abstract
- Two different SCR catalysts, V2O5-WO3/TiO2 and Cu-SSZ-13, were exposed to biodiesel exhausts generated by a diesel burner. The effect of phosphorus and sulfur on the SCR performance of these catalysts was investigated by doping the fuel with P-, S-, or P + S-containing compounds. Elemental analyses showed that both catalysts captured phosphorus while only Cu-SSZ-13 captured sulfur. High molar P/V ratios, up to almost 3, were observed for V2O5-WO3/TiO2, while the highest P/Cu ratios observed were slightly above 1 for the Cu-SSZ-13 catalyst. Although the V2O5-WO3/TiO2 catalyst captured more P than did the Cu-SSZ-13 catalyst, a higher degree of deactivation was observed for the latter, especially at low temperatures. For both catalysts, phosphorus exposure resulted in suppression of the SCR performance over the entire temperature range. Sulfur exposure, on the other hand, resulted in deactivation of the Cu-SSZ-13 catalyst mainly at temperatures below 300-350 °C. The use of an oxidation catalyst upstream of the SCR catalyst during the exhaust-exposure protects the SCR catalyst from phosphorus poisoning by capturing phosphorus. The results in this work will improve the understanding of chemical deactivation of SCR catalysts and aid in developing durable aftertreatment systems.
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2. |
- Ge, Yaxin, et al.
(author)
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Effects of used bed materials on char gasification : Investigating the role of element migration using online alkali measurements
- 2022
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In: Fuel processing technology. - : Elsevier. - 0378-3820 .- 1873-7188. ; 238
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Journal article (peer-reviewed)abstract
- Online alkali measurements using surface ionization are employed to study alkali release during heating of used industrial fluidized bed materials and gasification of biomass-based char and bed material mixtures. The alkali release from the bed materials starts at 820 °C and increases with temperature, the time a bed material has experienced in an industrial process, and in the presence of CO2. Online alkali measurement during heating of char mixed with used bed material shows significant alkali uptake by the char. Complementary SEM-EDS studies confirm the alkali results and indicate that other important inorganic elements including Si, Mg, and Ca also migrate from the bed material to the char. The migration of elements initially enhances alkali release and char reactivity, but significantly reduces both during the final stage of the gasification. The observed effects on char gasification become more pronounced with increasing amount of bed material and increasing time the material experienced in an industrial process. The ash-layer on the used bed material is concluded to play an important role as a carrier of alkali and other active components. The char and bed material systems are closely connected under operational conditions, and their material exchange has important implications for the thermal conversion.
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3. |
- Yu, Xiaowen, et al.
(author)
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Hydrogen Evolution Linked to Selective Oxidation of Glycerol over CoMoO4—A Theoretically Predicted Catalyst
- 2022
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In: Advanced Energy Materials. - : Wiley. - 1614-6832 .- 1614-6840. ; 12:14
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Journal article (peer-reviewed)abstract
- Electrochemical valorization of biomass waste (e.g., glycerol) for production of value-added products (such as formic acid) in parallel with hydrogen production holds great potential for developing renewable and clean energy sources. Here, a synergistic effort between theoretical calculations at the atomic level and experiments to predict and validate a promising oxide catalyst for the glycerol oxidation reaction (GOR) are reported, providing a good example of designing novel, cost-effective, and highly efficient electrocatalysts for producing value-added products at the anode and high-purity hydrogen at the cathode. The predicted CoMoO4 catalyst is experimentally validated as a suitable catalyst for GOR and found to perform best among the investigated metal (Mn, Co, Ni) molybdate counterparts. The potential required to reach 10 mA cm−2 is 1.105 V at 60 °C in an electrolyte of 1.0 ᴍ KOH with 0.1 ᴍ glycerol, which is 314 mV lower than for oxygen evolution. The GOR reaction pathway and mechanism based on this CoMoO4 catalyst are revealed by high-performance liquid chromatography and in situ Raman analysis. The coupled quantitative analysis indicates that the CoMoO4 catalyst is highly active toward C—C cleavage, thus presenting a high selectivity (92%) and Faradaic efficiency (90%) for formate production.
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4. |
- Zacharias, Savannah C., et al.
(author)
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Exploring Supramolecular Gels in Flow-Type Chemistry-Design and Preparation of Stationary Phases
- 2021
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In: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 0888-5885 .- 1520-5045. ; 60:28, s. 10056-10063
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Journal article (peer-reviewed)abstract
- Two major challenges facing chemical synthesis are product isolation and catalyst recovery. One method to overcome these challenges is to perform the synthesis in a flow system with a catalytic stationary phase. However, the polymeric catalytic materials used in flow systems are often laborious to produce. In this study, we investigate a novel supramolecular gel as a catalytic stationary phase material. The gel is based on a modular, easy to synthesize, oxotriphenylhexanoate (OTHO) gelator comprised of a catalytic unit designed to catalyze the Knoevenagel reaction. The catalytic organogel enhances the rate of product formation and can be reused five times. Use of the OTHO to construct catalytic gels is a flexible technique that can be utilized to improve product isolation and reduce wastage of the catalyst.
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5. |
- Jogi, Ramakrishna, et al.
(author)
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Understanding the formation of phenolic monomers during fractionation of birch wood under supercritical ethanol over iron based catalysts
- 2020
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In: Journal of the Energy Institute. - : Elsevier. - 1743-9671 .- 1746-0220. ; 93:5, s. 2055-2062
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Journal article (peer-reviewed)abstract
- The liquefaction of biomass in ethanol, at the critical point, has high potential due to low temperature and pressure (243 °C, 63 bar) when compared with water (374 °C, 220 bar). The current study deals with the fractionation of birch wood powder which was liquefied under supercritical ethanol over acidic or non-acidic catalysts, 5 wt % Fe-Beta-H-150 and 5 wt % Fe–SiO2, respectively. Based on the results, the reaction mechanism for the formation of lignin degradation products was proposed. The main phenolic product was isoeugenol over 5 wt % Fe-Beta-H-150 while intermediate products, i.e. such as coniferyl, and sinapyl alcohol, 4-propenyl syringol, syringaresinol, as well as syringyldehyde reacted rapidly further. The thermodynamic analysis was performed by Joback approach and using Gibbs-Helmholtz equation supporting the obtained results.
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6. |
- Mukesh, Chandrakant, et al.
(author)
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Production of C-14 Levulinate Ester from Glucose Fermentation Liquors Catalyzed by Acidic Ionic Liquids in a Solvent-Free Self-Biphasic System
- 2020
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In: ACS Omega. - : American Chemical Society (ACS). - 2470-1343. ; 5:10, s. 4828-4835
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Journal article (peer-reviewed)abstract
- Herein, we present the C-14 levulinate ester of 2,3-butanediol as the product of sugar fermentation liquors. The designed Brønsted acidic ionic liquid (BAIL) catalysts enable self-induced phase separation with ester products, and the role of anions has been investigated. Esterification reactions were carried out by 2,3-butanediol (2,3-BDO) and levulinic acid in solvent-free media and low temperatures (60–105 °C). For comparison, sulfuric acid, amberlite IR-120, and sulfonic acid-functionalized pyridinium ionic liquids with different anions were utilized as a catalyst upon esterification reaction. The diester product, namely, butane-2,3-diyl bis(4-oxopentanoate), was formed with a good yield (85%) and selectivity (85%) after complete conversion of 2,3-BDO in 24 h at 80 °C. The low yield (8%) of the monoester was observed. The monoester and diester were separated by a liquid–liquid extraction method. The ester products were characterized by various instrumental techniques such as 1H and 13C NMR, GC–FID, LC–MS, and FT-IR spectroscopy. The Hammett acidity functions of BAILs were determined from UV–vis spectroscopy. The catalyst was successfully recycled and reused in the processes. The spent BAILs were reused in six consecutive cycles with only a ∼7% diminished diester yield and selectivity. The produced levulinate ester will be useful as biofuel additives, solvents, plasticizers, and other applications.
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7. |
- Wang, Kai, et al.
(author)
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A one-carbon chemicals conversion strategy to produce precursor of biofuels with Saccharomyces cerevisiae
- 2023
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In: Renewable Energy. - : Elsevier BV. - 0960-1481 .- 1879-0682. ; 208, s. 331-340
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Journal article (peer-reviewed)abstract
- Utilization of one-carbon chemicals such as CO2, formate, and methanol by microorganisms can enable the sustainable production of fuels and chemicals. However, the low conversion efficiency of these chemicals by microorganisms is a major challenge. To address this, we designed a one-carbon strategy that can utilize CO2 and its derivative formate. Here, a platform yeast strain with improved formate utilization and NAD(P)H production was constructed and evaluated for its ability to produce free fatty acids (FFAs). Based on 13C-marked analysis, the one-carbon assimilation efficiency of the platform strain reached 11.24%. Through continuous optimization, under conditions of glucose feeding the formate utilization rate of the final strain reached 0.48 g/L/h, with the final titer of FFAs reached 10.1 g/L, which represented improvements of 21.8 times and 33.7 times, respectively. As such, the produced FFAs can be easily transformed into biodiesel by combining them with downstream technologies in future research.
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8. |
- Yahia, Mohamed, et al.
(author)
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Effect of incorporating different ZIF-8 crystal sizes in the polymer of intrinsic microporosity, PIM-1, for CO2/CH4 separation
- 2021
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In: Microporous and Mesoporous Materials. - : Elsevier. - 1387-1811 .- 1873-3093. ; 312
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Journal article (peer-reviewed)abstract
- Effective and economical carbon dioxide-methane separation (CO2/CH4) is highly desirable in several industries such as sweetening natural gases and renewable natural gas (RNG) from biogas and landfills. Among the different separation technologies, membrane separation has been shown to have lower cost of production and lower CH4 losses. In this study, Zeolitic Imidazole Frameworks (ZIF-8) crystals with sizes varying from 45 nm to 450 nm were synthesized and incorporated in the polymer of intrinsic microporosity, PIM-1, to form mixed matrix membranes (MMMs). The structure, morphology, and physicochemical properties of the MMMs were characterized by 1H NMR, FTIR, XRD, TGA, and SEM. ZIF-8 crystal size was controlled using the concentration of sodium formate. The influence of the ZIF-8 crystal size on MMMs was studied by sorption, gas permeability, and aging of the membranes. The MMMs with ZIF-8 crystals of 120 nm particle diameter yielded the greatest improvement in gas transport properties; the CO2/CH4 selectivity-CO2 permeability was 11.4 and 9700 Barrer compared to PIM-1 with 6.4 and 9300 Barrer respectively. The former is near the Robeson 2008 upper bound, while PIM-1 is on the 1991 upper bound. After 40 days of aging, selectivity increased and permeability decreased; the changes were parallel to the Robeson upper bounds indicating increased polymer packing and diffusivity selectivity.
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9. |
- Balachandran, Srija, et al.
(author)
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Comparative study for selective lithium recovery via chemical transformations during incineration and dynamic pyrolysis of EV li-ion batteries
- 2021
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In: Metals. - : MDPI AG. - 2075-4701. ; 11:8
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Journal article (peer-reviewed)abstract
- Selective leaching of Li from spent LIBs thermally pretreated by pyrolysis and incineration between 400 and 700 °C for 30, 60, and 90 min followed by water leaching at high temperature and high L/S ratio was examined. During the thermal pretreatment Li2CO3 and LiF were leached. Along with Li salts, AlF3 was also found to be leached with an efficiency not higher than 3.5%. The time of thermal pretreatment did not have a significant effect on Li leaching efficiency. The leaching efficiency of Li was higher with a higher L/S ratio. At a higher leaching temperature (80 °C), the leaching of Li was higher due to an increase in the solubility of present Li salts. The highest Li leaching efficiency of nearly 60% was observed from the sample pyrolyzed at 700 °C for 60 min under the leaching condition L/S ratio of 20:1 mL g−1 at 80 °C for 3 h. Furthermore, the use of an excess of 10% of carbon in a form of graphite during the thermal treatment did not improve the leaching efficiency of Li.
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10. |
- Achour, Abdenour, 1980, et al.
(author)
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Towards stable nickel catalysts for selective hydrogenation of biomass-based BHMF into THFDM
- 2023
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In: Journal of Environmental Chemical Engineering. - : Elsevier BV. - 2213-3437 .- 2213-2929. ; 11:2
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Journal article (peer-reviewed)abstract
- Selective transformation of BHMF (2,5-bis(hydroxymethyl)furan) to THFDM (tetrahydrofuran-2,5-dimethanol) over a variety of structured Ni/Sx-Z1−x catalysts was investigated. The effects of support, Ni loading, solvent, temperature, pressure, and particle size on the conversion and selectivity were studied. Among them, the 10 wt% Ni catalyst supported on the SiO2:ZrO2 weight ratio of 90:10 (10NiS90Z10) exhibits the best performance in terms of BHMF conversion and THFDM selectivity. Its good performance was attributed to its well-balanced properties, that depend upon the ZrO2 content of the support in combination with SiO2, the active Ni sites-support interaction, and acidity/basicity ratio of each catalyst resulting in different Ni dispersions. Importantly, the 10NiS90Z10 catalyst showed a stable selectivity to THFDM (>94%), with 99.4% conversion of BHMF during 2 h reaction time. Poor catalytic activity resulted from excessive ZrO2 content (>10 wt%). The structural, textural, and acidity properties of NiSi100−y-Zry catalysts, tuned by selectively varying the Ni amount from 5 to 15 wt%, were critically investigated using numerous material characterization techniques. Catalyst recycling experiments revealed that the catalyst could be recycled several times without any measurable loss of catalytic activity.
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