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Operational Strategy of a Two-Step Thermochemical Process for Solar Hydrogen Production

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Operational Strategy of a Two-Step Thermochemical Process for Solar Hydrogen Production international journal of hydrogen energy 34 (2009) 4537–4545 Available at www.sciencedirect.com journal homepage: www.elsevier.com/locate/he Operational strategy of a two-step thermochemical process for solar hydrogen production Martin Roeb*, Martina Neises, Jan-Peter Sa¨ck, Peter Rietbrock, Nathalie Monnerie, Ju¨rgen Dersch, Mark Schmitz, Christian Sattler German Aerospace Center – DLR, Institute of Technical Thermodynamics, Solar Research, Linder Hoehe, 51147 Cologne, Germany article info abstract Article history: A two-step thermochemical cycle process for solar hydrogen production from water has Received 28 February 2008 been developed using ferrite-based redox systems at moderate temperatures. The cycle Received in revised form offers promising properties concerning thermodynamics and efficiency and produces pure 18 August 2008 hydrogen without need for product separation. Accepted 18 August 2008 The process works by cycling stationary ferrite-coated monoliths through sequential Available online 15 October 2008 oxidation and reduction steps at 1073 and 1473 K, respectively. By using two such mono- liths in parallel, it is possible to quasi-continuously produce hydrogen. A prototype solar Keywords: reactor and peripherals suitable to proof the process concept were developed and have Thermochemical cycle been successfully tested in DLR’s solar furnace in Cologne. Repeated cycling operation is Ferrites possible with a reproducible amount of hydrogen produced. In most cases, a distinct decay Solar thermal of the amount of the evolved hydrogen is observed from cycle to cycle due to inhomoge- Water splitting neous heating of the monolithic absorber in the very first cycles and due to disappearance Iron oxide of the porosity and the associated loss of surface area in later cycles. Results from experimental campaigns with the prototype reactor and simulations with a corresponding reactor model support the development and verification of a process strategy for the continuous production of hydrogen in a larger scale. The tasks include the enhancement of long-term stability of the redox system, the development of an operational strategy and finally the design and development of a 100 kWth pilot reactor to demonstrate the feasibility of the process on top of a solar tower under real conditions. ª 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved. 1. Introduction and reactor design. Therefore, solar chemistry focuses on thermochemical cycles which proceed in several steps and Thermal splitting of water using concentrated solar energy is enable hydrogen generation at moderate temperatures which an attractive and completely renewable way to produce are manageable by using state-of-the-art engineering mate- hydrogen. However, because of thermodynamic restrictions, rials. The most interesting thermochemical cycle is the two- acceptable yields in the direct thermal splitting of water can step water splitting cycle using redox systems. During the only be achieved at temperatures above 2500 K. Such high first step of this cycle (the water splitting) the reduced and temperatures impose extraordinary demands on materials therefore activated material is oxidised by taking oxygen * Corresponding author. Tel.: þ49 2203 6012673; fax: þ49 2203 4141. E-mail address: [email protected] (M. Roeb). 0360-3199/$ – see front matter ª 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.ijhydene.2008.08.049 4538 international journal of hydrogen energy 34 (2009) 4537–4545 Nomenclature 2. Testing of solar reactor in the solar furnace DLR German Aerospace Center EC European Commission To realise the continuous supply of hydrogen, a quasi- MO metal oxide continuous operating reactor was built at the DLR. It consists of two separate chambers with fixed honeycomb absorbers in from water and producing hydrogen according to the both chambers as shown in Fig. 1a. While in one chamber the reaction: water splitting reaction takes place at temperatures around 1073 K, the other is being regenerated at temperatures of up to / 1473 K. During the water splitting reaction, water vapour (1) MOreduced þ H2O MOoxidised þ H2 diluted with nitrogen is passed through the reaction chamber In the next step (the regeneration step) the material is while during the regeneration the chamber is flushed with reduced again, setting some of its lattice oxygen free accord- pure nitrogen. ing to the reaction: The water splitting process needs significantly less solar power than the regeneration step. Therefore in the first / campaigns with the two-chamber reactor an optical dimin- (2) MOoxidised MOreduced þ O2 isher was used to attenuate the incoming radiation accord- One major advantage is that hydrogen and oxygen are ingly: a metallic mesh was moved in an alternating way in produced in separate steps, i.e. no separation of hydrogen and front of the left or right reaction chamber according to the oxygen is needed. completion of the two half cycles. In the most recent Several redox materials consisting of oxide pairs of multi- campaign, the diminisher was replaced by a newly developed lamellae shutter providing much more flexibility with respect valent metals (e.g. Fe3O4/FeO [1–3],Mn3O4/MnO [4]) or systems of metal oxide/metal (e.g. ZnO/Zn [5]) have been evaluated. to separate adjustment of power and flux density in the two Recently a lot of attention has been paid to ferrites and mixed chambers. The lamellae shutter can regulate separately the metal ferrites [6–9] and different approaches on solar receiver two different temperatures in both chambers needed for concepts for using mixed ferrites [10–12] have been developed. the hydrogen production and the regeneration (Fig. 1b). The In the scope of the project HYDROSOL and the consecutive segment shutter is installed 1000 mm in front of the focus of project HYDROSOL-2, both funded by the EC [14], mixed iron oxides have been used as the reducing material. The basic idea of the HYDROSOL project was to combine a support structure capable of achieving high temperatures when heated by concentrated solar radiation with a redox pair system suitable to carry out water dissociation and for regeneration at these temperatures. That means the complete operation of the whole process (water splitting and regeneration of the metal oxide) can be achieved by a single solar energy converter. The iron oxides have been fixed on ceramic monolithic structures, which are placed inside a solar receiver reactor. Two solar prototype receiver reactors have been designed, built and tested in the solar furnace of DLR in Cologne. With the first reactor, in which a single coated monolith is located in a single reaction chamber, the feasibility of solar chemical hydrogen production by redox systems coated on ceramic- support structures has been shown [13]. With the second reactor, a two-chamber setup, the continuous supply of hydrogen to downstream units was possible by operating both chambers in parallel but in different modes [14]. The goal of the ongoing work is to develop and build an optimized pilot plant (100 kWth) for solar hydrogen production based on this novel reactor concept. The project involves further scale-up of this technology and its effective coupling with solar central receiver systems in order to exploit and demonstrate all potential advantages. Specific challenging problems to be solved include the enhancement and optimi- sation of the metal oxide-ceramic-support system with respect to long-time stability under multi-cycle operation and the development and construction of a complete pilot dual absorber/receiver/reactor unit in a scale of 100 kWth and its Fig. 1 – a) Vertical-horizontal cut of two-chamber reactor coupling to a solar heliostat field. (conti reactor); b) schematic view of the lamellae shutter. international journal of hydrogen energy 34 (2009) 4537–4545 4539 the solar furnace of DLR in Cologne and is divided into two cycle rather quickly, the rear part of the absorber heats up parts. One part regulates the temperature in the left reactor more slowly and gets slightly hotter from cycle to cycle. chamber and the other part the temperature in the right Therefore the part of the honeycomb reaching a temperature reactor chamber. Each side of the lamellae shutter can be level sufficient for effective regeneration increases moved separately and simultaneously by a stepping motor. throughout the day. The amount of regenerated metal oxide The most recent experimental series in the solar furnace of per cycle increases (see also Section 3.2). DLR was first of all aiming at the evaluation of different Between the second and the third day, the mean hydrogen coating materials, especially concerning their long-term flow rate dropped about 50%. This is partly due to the variation stability and capability to produce constant hydrogen output of experimental parameters on the third day. In particular, over several cycles. Secondly, the experimental series aimed most of the cycles that day were conducted with reduced half- at the development of process parameters and operational cycle times as well for regeneration as for water splitting. But strategies for the pilot plant which has been set up at the this effect alone is not sufficient enough to explain the extent Plataforma Solar de Almerı´a(PSA). The strategy for operating of the decrease. Such a massive drop of the hydrogen flow rate the prototype reactor in the solar furnace is taken as a model as seen after
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