Mixed-Oxide Catalysts with Spinel Structure for the Valorization of Biomass: The Chemical-Loop Reforming of Bioethanol
Abstract
:1. Introduction
2. Spinels as Catalysts for the Chemical-Loop Reforming (CLR) of Bioethanol
- (a)
- Mn incorporation into Fe3O4 with generation of the corresponding ferrites showed its positive aspect on lowering the amount of coke that accumulated during the first step carried out with ethanol, see C %w (CHNS) in Table 4;
- (b)
- Mn incorporation also increased the H2/COx ratio, which follows from the previous statement. It is important to notice that the higher the H2/COx ratio, the more ‘pure’ is the H2 generated during the second step. For comparison, Fe3O4 itself accounts for H2/COx = 3.5, whereas MnFe2O4 (H2/COx = 15) and Co0.5Mn0.5Fe2O4 (H2/COx = 15) showed much higher values;
- (c)
- the incorporation of Cu (alone, or together with either Co or Mn) has a beneficial effect on the total amount of H2 produced from H2O, compared to Fe3O4. Hence, the best performance was shown by CuFe2O4 (Y-52%), Cu0.5Co0.5Fe2O4 (Y-46%) and Cu0.5Mn0.5Fe2O4 (Y-37%);
- (d)
- incorporation of Cu/Co led to the increase of the nH2/nEth ratio, as for CuFe2O4 (nH2/nEth = 1.2), and Cu0.5Co0.5Fe2O4 (nH2/nEth = 1.0). This can be correlated to the feasibility of producing H2 starting from bioethanol being based on the H2 vs ethanol heating values (referred to as LHV (Lower Heating Value), MJ/kg): 119, 96 and 28.86, respectively. In other words, the higher the nH2/nEth, the higher is the potential efficiency of the CLR process. Of course, there are many more aspects that have to be undertaken in order to calculate the actual cost of the CLR process, and to estimate a final price of H2 produced via CLR technology and compare it to the existing ones (not encompassed in this study).
- (a)
- Consecutive utilization of CoFe2O4, CuFe2O4 and Cu0.5Co0.5Fe2O4 ferrospinels as looping materials resulted in higher amounts of produced hydrogen (given in moles) which surpass the value obtained over the reference material—Fe3O4;
- (b)
- increasing the total tos from 20 to 60 min (which accounts the total time for the reduction/reoxidation step) leads to the decreasing of H2/COx ratio, which in its turn affects the final purity of the target gas—H2. However, this problem can be overcome by implementation of a three-step CLR process with the third step being carried out with air;
- (c)
- CuFe2O4 showed the higher nH2/nEth ratio of 1 (referring to the total value for three consecutive cycles) which was in fact twice as high as that obtained with Fe3O4 (nH2/nEth = 0.5);
- (d)
- on the other hand, under different conditions (not shown here), CoFe2O4 underwent the greatest extent of reduction during the first step, while being reoxidizable back to the spinel during the second step, and was able to maintain it throughout several repeated cycles. However, it showed the greater amount of accumulated coke, which formed CO when put in contact with steam during the second step;
- (e)
- coke formation remained an issue for M-modified ferrospinels, which means that avoiding completely carbon deposition and its further accumulation is not possible.
3. Other Materials as O-Carriers for Hydrogen Production via CLR
4. Conclusions
Funding
Conflicts of Interest
References
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Preparation Method | Reference |
---|---|
Coprecipitation | [9,10,11,12,13,14,15,16,17,18,19,20,21,22,23] |
Sol–gel | [24,25,26,27,28,29,30,31,32,33,34,35,36,37,38,39,40,41,42,43,44,45,46] |
Hydrothermal | [47,48,49,50,51,52,53,54,55] |
Solvothermal | [56,57,58,59,60] |
Microemulsion/Reverse micelles | [61,62,63,64,65,66,67,68] |
Template | [66,67,68,69,70,71,72] |
Mechanical milling | [73,74,75,76,77,78,79,80,81] |
Plasma | [82,83] |
Flux growth | [84,85,86] |
Solid phase | [87] |
Combustion | [88,89,90] |
Microwave combustion | [91,92,93] |
Microwave hydrothermal | [94,95,96] |
Pechini method | [97,98,99,100] |
Electrochemical | [101] |
Electrospinning | [102] |
Thermal treatment | [103,104] |
Ultrasonic wave-assisted ball milling | [105] |
Spray pyrolysis | [106] |
Aerosol | [107] |
Forced hydrolysis | [108] |
Glycol-thermal | [109] |
Refluxing | [110] |
Reaction | References |
---|---|
Oxidative cleavage of styrene to benzaldehyde with H2O2 | [5,49] |
Oxidation of cyclohexane to cyclohexanol/cyclohexanone with O2 or H2O2 | [6,7] |
Hydroxylation of benzene/phenol to phenol/diphenols with H2O2 | [111] |
Oxidation of vanyllol to vanillin with air | [112] |
Oxidation of benzyl alcohol to benzaldehyde with H2O2 | [113] |
Oxidation of monoterpenic alkenes with O2 | [114] |
Oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid (hmf to fdca) with H2O2 or O2 | [115,116,117] |
Oxidation of aniline to azoxybenzene with H2O2 | [118] |
Oxidation of toluene to benzaldehyde with H2O2 | [119] |
Oxidation of ethanol to acetaldehyde with O2 | [120] |
Oxidation of veratryl alcohol to veratryl aldehyde with O2 | [121] |
Ketonisation of butanol to heptanone | [122] |
Total oxidation of voc with air | [123] |
Friedel–crafts acylation | [124] |
Knoevenagel condensation | [125] |
Reduction of ketones | [126] |
Reduction of nitroarenes | [127] |
Methylation (alkylation) of phenolics, aniline, pyridine | [128] |
Methanol, ethanol reforming (by means of chemical-loop) | [129,130,131,132,133,134,135,136,137] |
Sample Name | SSA, m2/g | Crystallite Size, nm | Particle Size (dBET), nm |
---|---|---|---|
CuFe2O4 | 60 | 6.9 | 18.3 |
Cu0.5Co0.5Fe2O4 | 67 | 10.4 | 16.5 |
CoFe2O4 | 69 | 12 | 16.2 |
Co0.5Mn0.5Fe2O4 | 141 | 3.5 | 8 |
Cu0.5Mn0.5Fe2O4 | 112 | - | 10 |
MnFe2O4 | 165 | - | 6.9 |
Sample Name | C %W after 20 min Red. with Ethanol | H2/COX | Moles of H2/Moles of Ethanol (nH2/nEth) |
---|---|---|---|
CoFe2O4 | 11.6 | 6 | 0.5 |
Cu0.5Co0.5Fe2O4 | 16.3 | 3 | 1.0 |
CuFe2O4 | 6.9 | 3 | 1.2 |
Cu0.5Mn0.5Fe2O4 | 6.1 | 3 | 0.8 |
Co0.5Mn0.5Fe2O4 | 1.5 | 15 | 0.1 |
MnFe2O4 | 1.7 | 15 | 0.09 |
Fe3O4 | 5.3 | 3.5 | 0.7 |
Sample Name | H2/COX | Moles of H2/Moles of Ethanol |
---|---|---|
CoFe2O4 | 5 | 0.7 |
Cu0.5Co0.5Fe2O4 | 3 | 0.9 |
CuFe2O4 | 3 | 1.0 |
Fe3O4 | 3 | 0.5 |
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Vozniuk, O.; Tabanelli, T.; Tanchoux, N.; Millet, J.-M.M.; Albonetti, S.; Di Renzo, F.; Cavani, F. Mixed-Oxide Catalysts with Spinel Structure for the Valorization of Biomass: The Chemical-Loop Reforming of Bioethanol. Catalysts 2018, 8, 332. https://doi.org/10.3390/catal8080332
Vozniuk O, Tabanelli T, Tanchoux N, Millet J-MM, Albonetti S, Di Renzo F, Cavani F. Mixed-Oxide Catalysts with Spinel Structure for the Valorization of Biomass: The Chemical-Loop Reforming of Bioethanol. Catalysts. 2018; 8(8):332. https://doi.org/10.3390/catal8080332
Chicago/Turabian StyleVozniuk, Olena, Tommaso Tabanelli, Nathalie Tanchoux, Jean-Marc M. Millet, Stefania Albonetti, Francesco Di Renzo, and Fabrizio Cavani. 2018. "Mixed-Oxide Catalysts with Spinel Structure for the Valorization of Biomass: The Chemical-Loop Reforming of Bioethanol" Catalysts 8, no. 8: 332. https://doi.org/10.3390/catal8080332