Oxidative steam reforming of ethanol on rhodium catalyst – I: Spatially resolved steady-state experiments and microkinetic modeling

Baruah, Renika; Dixit, Marm; Parejiya, Anand; Basarkar, Pratik; Bhargav, Atul; Sharma, Sudhanshu

doi:10.1016/j.ijhydene.2017.03.168

Cited by 18 publications

(9 citation statements)

References 66 publications

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“…It is evident that theoretical studies have focused on the decomposition pathways of ethanol, while all previously reported microkinetic models on ethanol conversion towards syngas are over noble metals, namely Pt [19,26] and Rh [27]. It is recognised though that the high cost of the latter poses significant economic difficulties to the commercial implementation of the process.…”

Section: Introductionmentioning

confidence: 99%

“…In the work of Koehle et al[26], again a Pt catalyst was studied, but for ethanol partial oxidation, so understandably the high temperature oxidative conditions led to the surface pathways being substantially different to those discussed above, with ethanol activation proceeding primarily through dehydration. Similarly, the work of Baruah et al[27], focusing on the oxidative steam reforming of ethanol on Rh, proposed dehydroxylation (C-O cleavage) as the initial ethanol activation step, although again for a different reaction and conditions. In the current work, in parallel to the main pathway to CH 3 CHOH*, ethanol…”

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confidence: 97%

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Microkinetic modelling and reaction pathway analysis of the steam reforming of ethanol over Ni/SiO2

Afolabi

Kechagiopoulos

2019

International Journal of Hydrogen Energy

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Hydrogen production via the steam reforming of biomass-derived ethanol is a promising environmental alternative to the use of fossil fuels and a means of clean power generation. A microkinetic modelling study of ethanol steam reforming (ESR) on Nickel is presented for the first time and validated with minimal parameter fitting against experimental data collected over a Ni/SiO2 catalyst. The thermodynamically consistent model utilises Transition State Theory and the UBI-QEP method for the determination of kinetic parameters and is able to describe correctly experimental trends across a wide range of conditions. The kinetically controlling reaction steps are predicted to occur in the dehydrogenation pathway of ethanol, with the latter found to proceed primarily via the formation of 1-hydroxyethyl. CC bond cleavage is predicted to take place at the ketene intermediate leading to the formation of CH2 and CO surface species. The latter intermediates proceed to react according to methane steam reforming and water gas shift pathways that are enhanced by the presence of water derived OH species. The experimentally observed negative reaction order for water is explained by the model predictions via surface saturation effects of adsorbed water species. The model results highlight a possible distinction between ethanol decomposition pathways as predicted by DFT calculations on Ni close-packed surfaces and ethanol steam reforming pathways at the broad range of experimental conditions considered.

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Section: Introductionmentioning

confidence: 99%

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confidence: 97%

Microkinetic modelling and reaction pathway analysis of the steam reforming of ethanol over Ni/SiO2

Afolabi

Kechagiopoulos

2019

International Journal of Hydrogen Energy

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“…New concepts of self-sustained electrochemical promotion catalysts for partial oxidation of heavy hydrocarbons were also proposed in References [5,15]. Baruah et al [16] developed a microkinetic model for the ethanol oxidative steam-reforming process, and it can be used in CFD software. However, these research studies did not take maximization hydrogen production of ethanol reforming as the objective function to obtain the optimal operating parameters.…”

Section: Introductionmentioning

confidence: 99%

Process Modeling, Optimization, and Heat Integration of Ethanol Reforming Process for Syngas Production with High H2/CO Ratio

Xiang

Yuan

2019

Processes

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The process modeling, parameter optimization, and heat integration of reforming ethanol to hydrogen is conducted in this paper. Modeling results show that the optimum reaction pressure for ethanol steam reforming is 1 bar. When the 7.4:1 is selected as a moderate water/ethanol ratio, the optimum reaction temperature is about 755 °C. As for heat integration, the composite curve and optimum heat-exchange network are given out by pinch technology, of which adding a heat exchanger can reduce 10,833 kW of heating duty and 10,833 kW of cooling duty and make the energy saving reach about 57.4%. Another two heat-integration plans are proposed for the ethanol steam-reforming process, to further decrease the high-level heat duty. Finally, similar heat integration was also carried out for the oxidative steam reforming, and the system is autothermal when the oxygen/ethanol is about 0.5:1 on the basis of above steam-reforming process, while the hydrogen molar purity is decreased from 69% to 66%.

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“…[4,5] These methods often suffered from serious limitations such as substrate scope and recyclability of the catalyst. [7,8] The contemporary advancement over the decades in heterogeneous rhodium metal catalysis has led in substantial improvement to overcome the drawbacks in the developed reduction processes. [7,8] The contemporary advancement over the decades in heterogeneous rhodium metal catalysis has led in substantial improvement to overcome the drawbacks in the developed reduction processes.…”

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confidence: 99%

“…in 1,4-dioxane (0.5 mL) at 100 8C, we got 27% yield of the product 2 a in 2 h ( Table 1, entry 1). Subsequently other bases such as K 2 CO 3 , KO t Bu, and NaOH were screened and 10-70% yields of the desired product were observed respectively (Table 1, entries [5][6][7][8]. Subsequently other bases such as K 2 CO 3 , KO t Bu, and NaOH were screened and 10-70% yields of the desired product were observed respectively (Table 1, entries [5][6][7][8].…”

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confidence: 99%

Supported Rhodium Nanoparticles Catalyzed Reduction of Nitroarenes, Arylcarbonyls and Aryl/Benzyl Sulfoxides using Ethanol/Methanol as In Situ Hydrogen Source

2018

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A facile reduction reaction of nitroarenes, aryl carbonyls and aryl/benzyl sulfoxides was performed under polystyrene supported rhodium (Rh@PS) catalyzed conditions using ethanol/methanol as in situ hydrogen source. The catalyst Rh@PS played a pivotal role in the oxidation of ethanol/methanol in the presence of traces of aerial oxygen and base to produce hydrogen gas, enough for further reduction reaction. Transmission electron microscopy (TEM) analysis indicated that the average particle size of the Rh nanoparticles (NPs) lies between 2-3 nm; this is responsible for its high catalytic activity. The advantages of Rh@PS are its catalytic activity, easy preparation, recovery, recyclability for several runs, and low metal leaching during reaction.

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Oxidative steam reforming of ethanol on rhodium catalyst – I: Spatially resolved steady-state experiments and microkinetic modeling

Cited by 18 publications

References 66 publications

Microkinetic modelling and reaction pathway analysis of the steam reforming of ethanol over Ni/SiO2

Microkinetic modelling and reaction pathway analysis of the steam reforming of ethanol over Ni/SiO2

Process Modeling, Optimization, and Heat Integration of Ethanol Reforming Process for Syngas Production with High H2/CO Ratio

Supported Rhodium Nanoparticles Catalyzed Reduction of Nitroarenes, Arylcarbonyls and Aryl/Benzyl Sulfoxides using Ethanol/Methanol as In Situ Hydrogen Source

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