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Nuclear Production of Hydrogen, Fourth Information Exchange ...

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PREDICTING THE ENERGY EFFICIENCY OF A RECUPERATIVE BAYONET DECOMPOSITION REACTOR<br />

Predicting the energy efficiency <strong>of</strong> a recuperative bayonet decomposition<br />

reactor for sulphur-based thermochemical hydrogen production*<br />

Maximilian B. Gorensek, Tommy B. Edwards<br />

Computational Sciences Directorate, Savannah River National Laboratory<br />

Aiken, SC, USA<br />

Abstract<br />

High-temperature decomposition <strong>of</strong> sulphuric acid is a major step for sulphur-based thermochemical<br />

cycles such as hybrid sulphur and sulphur-iodine. It is generally also the most energy-intensive, so<br />

that the overall heat requirement for this step can determine whether a particular decomposition<br />

reactor or flow sheet design is practical.<br />

A recuperative bayonet sulphuric acid decomposition reactor has been designed by researchers at<br />

Sandia National Laboratories (SNL) that features all-silicon carbide (SiC) construction for the heated<br />

parts, can be made from readily available SiC shapes, makes the most use <strong>of</strong> heat recuperation, and<br />

has all <strong>of</strong> its fluid connections at sufficiently low temperatures that conventional seal materials can be<br />

used. Bench-scale experiments using electric resistance heaters as the energy source have verified that<br />

the design functions as intended.<br />

The purpose <strong>of</strong> this work was to apply a pinch analysis to the SNL concept, using a statistically<br />

designed set <strong>of</strong> computer model experiments to establish the limiting performance (heating target) <strong>of</strong><br />

the reactor as a function <strong>of</strong> operating conditions. Mapping out the limiting performance helped ascertain<br />

the practical operating range, allowing the reactor to be integrated into conceptual flow sheets. Seven<br />

input variables were considered: temperature (48 to 150°C), pressure (10 to 90 bar), and acid<br />

concentration (30 to 90 wt.%) <strong>of</strong> the feed; process fluid temperatures at the inlet (600 to 740°C) and the<br />

outlet (750 to 900°C) <strong>of</strong> the catalyst bed; temperature approach to equilibrium <strong>of</strong> the decomposition<br />

reaction in the catalyst bed (-25 to 0°C); and minimum temperature difference for recuperative heat<br />

transfer (10 to 100°C). Of particular interest was the effect <strong>of</strong> temperature, which will be limited by<br />

the operating temperature <strong>of</strong> the nuclear reactor heat source.<br />

A space-filling Latin Hypercube Design was used to generate model control variable input sets that<br />

were spread throughout factor space. Statistical tools were used to develop models from the results <strong>of</strong><br />

the simulation “experiments” and to suggest additional simulation points to explore regions <strong>of</strong> interest.<br />

Over 130 different sets <strong>of</strong> control variables were eventually simulated.<br />

Results indicate that practical operation (high temperature heat target < 400 kJ/mol SO 2 ) requires acid<br />

feed concentrations in excess <strong>of</strong> 65 wt.% H 2 SO 4 . The optimum (lowest achievable high temperature<br />

heat target <strong>of</strong> 321 kJ/mol SO 2 ) occurs at roughly 80 wt.% H 2 SO 4 at the highest pressure (90 bar) and<br />

highest peak process temperature (900°C). As the peak process temperature is decreased from 900°C,<br />

the heating target increases. Below peak process temperatures <strong>of</strong> about 700°C, heating targets well in<br />

excess <strong>of</strong> 400 kJ/mol SO 2 are predicted. This means that HTGR operating below 800°C reactor outlet<br />

temperature will not allow efficient bayonet operation. Feed and catalyst bed inlet temperatures had<br />

no effect on the heat target. Not surprisingly, a zero value <strong>of</strong> the decomposition reaction temperature<br />

approach to equilibrium and 10°C minimum temperature difference for recuperative heat transfer was<br />

found to be best.<br />

* The full paper being unavailable at the time <strong>of</strong> publication, only the abstract is included.<br />

NUCLEAR PRODUCTION OF HYDROGEN – © OECD/NEA 2010 199

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