Validation of the H2 production stage via SER under relevant conditions for the Ca/Cu reforming process practical application

Grasa, Gemma; Navarro, M.V.; López, José Manuel; Díez-Martín, L.; Fernández, José R.; Murillo, R.

doi:10.1016/j.cej.2017.04.134

Cited by 30 publications

(29 citation statements)

References 66 publications

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“…The thermal integration of the Ca-Cu looping process on a large scale has been also evaluated [37,38] The experimental viability of the main reaction stages of the Ca-Cu looping process has been demonstrated in lab-scale fixed-bed reactors within the framework of the ASCENT project [46]. Grasa et al [47] studied the SER operation at different pressures using a mixture of a commercial reforming catalyst and a calcium-based sorbent. Both materials exhibited excellent performances after repetitive oxidation-reductionreforming cycles.…”

Section: Introductionmentioning

confidence: 99%

Study of the calcination of CaCO3 by means of a Cu/CuO chemical loop using methane as fuel gas

2019

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The Ca-Cu looping process allows a H 2-rich product gas to be obtained on the basis of the sorption enhanced reforming (SER) concept, while generating a concentrated stream of CO 2 suitable for geological storage or industrial use. Previous works have demonstrated that the Cu/CuO chemical loop provides a feasible alternative for regenerating the CO 2-sorbent required for the SER with potentially low energy penalties. In this work, the CuO reduction/CaCO 3 calcination operation, which is the key stage of the Ca-Cu looping process, is experimentally demonstrated in a fixed-bed reactor at TRL4 using pure methane as fuel gas. The effect of the temperature of the solids bed on the operation is also evaluated. A detailed characterization of both CuOand CaO-based materials resulting from the experiments has been carried out, revealing only minor changes in their textural properties, which demonstrates their high stability after successive oxidation-carbonation-reduction/calcination cycles.

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Section: Introductionmentioning

confidence: 99%

Study of the calcination of CaCO3 by means of a Cu/CuO chemical loop using methane as fuel gas

2019

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“…Finally, the calcination of CaCO 3 and simultaneous reduction of CuO is carried out in the step C (1 bar, <1173 K). In a recent work, the H 2 production stage of the Ca/Cu process was validated under relevant experimental conditions [21]. In this research a gas stream containing 95%vol H 2 was obtained at 923 K using a space velocity of 2.5 kg CH 4 h −1 kg cat −1 , high enough to allow the process scaling up.…”

Section: Introductionmentioning

confidence: 99%

Determination of the oxidation kinetics of high loaded CuO-based materials under suitable conditions for the Ca/Cu H2 production process

Díez-Martín

Grasa

Murillo

et al. 2018

Fuel

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In this work, the oxidation reaction of high loaded CuO-based materials was investigated under atmospheric and pressurized conditions. The oxygen transport capacity of the materials was firstly tested in the TGA and no losses greater than 5% were observed along 100 oxidation/reduction cycles. The kinetic parameters governing the oxidation reactions of the selected CuO-based materials were determined using a shrinking core model with chemical reaction control. The experimental results suggested that a SCM with chemical reaction control is able to predict the oxidation conversion of high loaded CuO-based materials in powder and pellet form. On the other hand, the effect of total pressure on materials reactivity was analyzed. The kinetic parameters obtained under atmospheric conditions were applied to fit the experimental data obtained under pressurized conditions. The results confirmed that the pressure has not an important effect on the oxidation kinetics of high loaded CuO-based materials and the parameters obtained at atmospheric pressure can be applied to study the oxidation under pressurized conditions.

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“…Reaction stages involving Ca and Cu solids have been experimentally studied at laboratory scale [22,23] and simultaneous CuO reduction/CaCO3 calcination up to TRL4 [24]. The experimental studies on SER stage under relevant conditions of the process are currently scarce nevertheless high H2 production efficiencies have been corroborated for a mixture of CO2-sorbent with fresh or aged reforming catalyst at different mass hourly space velocities and pressures [25]. The basic Ca/Cu looping process consists of a sequence of three main reaction steps (see Figure 1), which are adiabatically carried out in fixed-bed reactors operating in parallel at different reaction steps to make a continuous looping operation feasible.…”

Section: Introductionmentioning

confidence: 99%

Catalyst evaluation for high-purity H2 production by sorption-enhanced steam-methane reforming coupled to a Ca/Cu process

Navarro

López

Garcı́a

et al. 2017

Journal of Power Sources

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The operational limits of a commercial nickel-based catalyst under the conditions of a sorption-enhanced steam-methane reforming process coupled to a Ca/Cu chemical loop are investigated for high-purity H 2 production in a cyclic operation. The performance of the reforming catalyst is tested by means of a high number of oxidation-reductionreforming cycles. After 100 oxidation-reduction cycles, this catalyst retains its exceptional reforming activity. The methane conversion values are close to the thermodynamic equilibrium under very demanding conditions: temperature between 500 ºC-700 ºC and mass hourly space velocity of 8.8 kgCH 4 h-1 kgcat-1. After 200 cycles, the sample shows reduction in its reforming activity in line with a lower dispersion of the Ni species. Sintering of Ni nanocrystals is evidenced during the oxidation-reduction multi-cycles. The performance of the catalyst after 200 oxidationreduction cycles mixed with a CaO-based CO 2 sorbent is studied under optimal conditions calculated for the sorption-enhanced reforming process coupled to a Ca/Cu cycle (temperature of 650 ºC, steam/methane ratio of 4, sorbent/catalyst ratio of 4 and space velocity of 0.75 kgCH 4 h-1 kgcat-1). Remarkably, an equilibrium value over 92 vol.% H 2 concentration is achieved, highlighting this catalyst as a promising candidate for the next steps of the process development.

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Validation of the H2 production stage via SER under relevant conditions for the Ca/Cu reforming process practical application

Cited by 30 publications

References 66 publications

Study of the calcination of CaCO3 by means of a Cu/CuO chemical loop using methane as fuel gas

Study of the calcination of CaCO3 by means of a Cu/CuO chemical loop using methane as fuel gas

Determination of the oxidation kinetics of high loaded CuO-based materials under suitable conditions for the Ca/Cu H2 production process

Catalyst evaluation for high-purity H2 production by sorption-enhanced steam-methane reforming coupled to a Ca/Cu process

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