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Solar Hydrogen Production Via a Samarium Oxide-Based Thermochemical Water Splitting Cycle

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Solar Hydrogen Production Via a Samarium Oxide-Based Thermochemical Water Splitting Cycle energies Article Solar Hydrogen Production via a Samarium Oxide-Based Thermochemical Water Splitting Cycle Rahul Bhosale 1,*, Anand Kumar 1, Fares AlMomani 1, Ujjal Ghosh 1, Mohammad Saad Anis 1, Konstantinos Kakosimos 2, Rajesh Shende 3 and Marc A. Rosen 4 1 Department of Chemical Engineering, College of Engineering, Qatar University, P. O. Box 2713, Doha 2713, Qatar; [email protected] (A.K.); [email protected] (F.A.); [email protected] (U.G.); [email protected] (M.S.A.) 2 Department of Chemical Engineering, Texas A&M University at Qatar, PO Box 23874, Doha 2713, Qatar; [email protected] 3 Department of Chemical and Biological Engineering, South Dakota School of Mines and Technology, Rapid City, SD 57701-3995, USA; [email protected] 4 Faculty of Engineering and Applied Science, University of Ontario Institute of Technology, 2000 Simcoe St. North, Oshawa, ON L1H 7K4, Canada; [email protected] * Correspondence: [email protected]; Tel.: +974-4403-4168 Academic Editor: Wei-Hsin Chen Received: 25 January 2016; Accepted: 18 April 2016; Published: 25 April 2016 Abstract: The computational thermodynamic analysis of a samarium oxide-based two-step solar thermochemical water splitting cycle is reported. The analysis is performed using HSC chemistry software and databases. The first (solar-based) step drives the thermal reduction of Sm2O3 into Sm and O2. The second (non-solar) step corresponds to the production of H2 via a water splitting reaction and the oxidation of Sm to Sm2O3. The equilibrium thermodynamic compositions related to the thermal reduction and water splitting steps are determined. The effect of oxygen partial pressure in the inert flushing gas on the thermal reduction temperature (TH) is examined. An analysis based on the second law of thermodynamics is performed to determine the cycle efficiency (hcycle) and solar-to-fuel energy conversion efficiency (hsolar´to´fuel) attainable with and without heat recuperation. The results indicate that hcycle and hsolar´to´fuel both increase with decreasing TH, due to the reduction in oxygen partial pressure in the inert flushing gas. Furthermore, the recuperation of heat for the operation of the cycle significantly improves the solar reactor efficiency. For instance, in the case where TH = 2280 K, hcycle = 24.4% and hsolar´to´fuel = 29.5% (without heat recuperation), while hcycle = 31.3% and hsolar´to´fuel = 37.8% (with 40% heat recuperation). Keywords: solar thermochemical; thermodynamics; hydrogen; water splitting; samarium oxide; computational analysis 1. Introduction Two concerns in many countries are long-term shortages of fossil fuels and the need to secure fuel supplies. Carbon dioxide emissions constitute another significant issue concerning all societies, as such emissions are considered the main cause of global warming and climate change, for which the consequences are predicted to be melting of glaciers, a sea level rise, and increased weather extremes. The CO2 emissions from fuel combustion were 32.1 Gt (billion metric tons) in 2015 [1]. As a consequence, it is important for countries to invest in and shift towards clean energy technologies such as solar energy. The conversion of solar energy to chemical energy in the form of an alternative fuel such as H2 provides a promising future sustainable energy pathway. Hydrogen can be produced with solar thermal energy via water splitting reactions. Hydrogen used in this manner is an energy carrier. Its advantages include a high energy density (on a mass basis) and non-polluting nature. Energies 2016, 9, 316; doi:10.3390/en9050316 www.mdpi.com/journal/energies Energies 2016, 9, 316 2 of 15 The metal oxide (MO)-based two-step solar thermochemical cycle is a potentially advantageous way to produce hydrogen via water splitting [2–4]. The main reactions involved in the MO based two-stepEnergies solar 2016, thermochemical 9, 316 water splitting cycle are as follows: 2 of 14 Reactionthermal energy 1: Solar via thermal water splitting dissociation reactions. of MO: Hydrogen used in this manner is an energy carrier. Its advantages include a high energy density (on a mass basis) and non‐polluting nature. The metal oxide (MO)‐based twoMO‐stepÑ solarMO thermochemicalreduced ` O2 cycle is a potentially advantageous (1) way to produce hydrogen via water splitting [2–4]. The main reactions involved in the MO based Reactiontwo‐step solar 2: Non-solar thermochemical water splittingwater splitting step: cycle are as follows: Reaction 1: Solar thermal dissociation of MO: MOreduced ` H2O Ñ MO ` H2 (2) MO → MOreduced + O2 (1) The MO-basedReaction 2: Non two-step‐solar solarwater thermochemical splitting step: water splitting cycle is beneficial because it avoids the formation of an explosive gaseous mixture of H and O (since both gases are produced in different MOreduced + H2O → MO2 + H2 (2) steps). Furthermore, the MO can be used in multiple thermochemical cycles as it is not consumed during anyThe of MO the‐ stepsbased involved.two‐step solar thermochemical water splitting cycle is beneficial because it Inavoids the past,the formation several MO-basedof an explosive redox gaseous systems mixture were of H theoretically2 and O2 (since and both experimentally gases are produced studied in as potentialdifferent thermochemical steps). Furthermore, water splitting the MO can reactions. be used These in multiple include thermochemical zinc oxide cycles cycles [2 –as11 it], ironis not oxide cyclesconsumed [12–15], tinduring oxide any cycles of the steps [16–18 involved.], terbium oxide cycles [19], mixed ferrite cycles [20–25], ceria cycles [26In–29 the], past, and perovskiteseveral MO‐based cycles redox [30– 32systems]. In thewere case theoretically of zinc andand experimentally tin oxide cycles, studied due as to the potential thermochemical water splitting reactions. These include zinc oxide cycles [2–11], iron oxide volatile nature of the MOs involved, the loss of reactive material due to high temperature operation is cycles [12–15], tin oxide cycles [16–18], terbium oxide cycles [19], mixed ferrite cycles [20–25], ceria inevitable.cycles In[26–29], the case and of perovskite the iron oxide,cycles [30–32]. ferrite, In ceria, the andcase perovskiteof zinc and cycles,tin oxide the cycles, complete due to reduction the of thevolatile MOs is nature not possible of the MOs and involved, hence a the lower loss of H 2reactiveproduction material is expecteddue to high (per temperature kg of metal operation oxide and per unitis inevitable. solar energy In the input). case of the Therefore, iron oxide, investigations ferrite, ceria, and of perovskite new thermochemical cycles, the complete cycles reduction aimed at H2 productionof the MOs via solar is not thermochemical possible and hence water a lower splitting H2 production are needed. is expected (per kg of metal oxide and Inper this unit paper, solar energy the thermodynamic input). Therefore, feasibility investigations of a novelof new samarium thermochemical oxide-based cycles aimed two-step at H2 solar thermochemicalproduction via water solar splittingthermochemical (Sm-WS) water cycle splitting is investigated. are needed. This is, to the best of the authors’ In this paper, the thermodynamic feasibility of a novel samarium oxide‐based two‐step solar knowledge, the first time that a Sm-WS cycle has been investigated for use in solar H2 production. Thermodynamicthermochemical modeling water splitting of the Sm-WS (Sm‐WS) cycle cycle is is performed investigated. (in This two is, sections) to the best using of the the authors’ commercial knowledge, the first time that a Sm‐WS cycle has been investigated for use in solar H2 production. thermodynamic HSC Chemistry software and databases [33]. In section one, the thermodynamic Thermodynamic modeling of the Sm‐WS cycle is performed (in two sections) using the commercial equilibriumthermodynamic compositions HSC Chemistry during the software solar thermal and databases reduction [33]. ofIn Sm section2O3 andone, thethe oxidationthermodynamic of Sm via waterequilibrium splitting are compositions determined. during The effectthe solar of thethermal oxygen reduction partial of pressure Sm2O3 and in the oxidation inert flushing of Sm gas via used insidewater a solar splitting reactor are during determined. thermal The reduction effect of ofthe Sm oxygen2O3 is partial examined. pressure Also, in thethe variationinert flushing in the gas Gibbs free energyused inside as a a function solar reactor of water during splitting thermal temperaturereduction of Sm (T2LO)3 for is examined. the H2 production Also, the variation step is estimated.in the In sectionGibbs two,free energy energy as and a function exergy of analyses water splitting of the Sm-WStemperature cycle (T areL) for carried the H2 out. production The solar step reactoris absorptionestimated. efficiency, In section the two, required energy solar and exergy energy analyses input, of radiation the Sm‐WS heat cycle losses, are carried the rate out. of The heat solar rejected by thereactor quench absorption unit and efficiency, the water the splitting required reactor, solar energy and theinput, solar-to-fuel radiation heat conversion losses, the efficiency rate of heat of the rejected by the quench unit and the water splitting reactor, and the solar‐to‐fuel conversion Sm-WS cycle are determined via computational thermodynamic modeling and the results are reported. efficiency of the Sm‐WS cycle are determined via computational thermodynamic modeling and the A typical Sm-WS cycle is presented in Figure1. results are reported. A typical Sm‐WS cycle is presented in Figure 1. Figure 1. Typical Sm‐WS cycle. Figure 1. Typical Sm-WS cycle. Energies 2016, 9, 316 3 of 15 To perform the thermodynamic calculations in a conventional way, we rely on the experimental or assessed data (which utilizes stability functions) published in thermodynamic books and scientific journals. This approach is time consuming due to the difficulty in locating the thermodynamic data in the published literature and also because the calculations involved are complicated. Furthermore, inconsistencies arising from the use of different standard and reference states make the final results uncomparable.
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