international journal of hydrogen energy 34 (2009) 737744

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Global warming potential of the sulfuriodine process using life cycle assessment methodology
William C. Lattina, Vivek P. Utgikarb,*
a b

Department of Environmental Sciences, University of Idaho, Idaho Falls, ID 83402, United States Department of Chemical Engineering, University of Idaho, Idaho Falls, ID 83402, United States

article info
Article history: Received 10 June 2008 Received in revised form 7 October 2008 Accepted 22 October 2008 Available online 6 December 2008 Keywords: Life cycle analysis Sulfuriodine cycle Nuclear production of hydrogen

abstract
A life cycle assessment (LCA) of one proposed method of hydrogen production thermochemical water-splitting using the sulfuriodine cycle couple with a very high-temperature nuclear reactor is presented in this paper. Thermochemical water-splitting theoretically offers a higher overall efciency than high-temperature electrolysis of water because heat from the nuclear reactor is provided directly to the hydrogen generation process, instead of using the intermediate step of generating electricity. The primary heat source for the SI cycle is an advanced nuclear reactor operating at temperatures corresponding to those required by the sulfuriodine process. This LCA examines the environmental impact of the combined advanced nuclear and hydrogen generation plants and focuses on quantifying the emissions of carbon dioxide per kilogram of hydrogen produced. The results are presented in terms of global warming potential (GWP). The GWP of the system is 2500 g carbon dioxide-equivalent (CO2-eq) per kilogram of hydrogen produced. The GWP of this process is approximately one-sixth of that for hydrogen production by steam reforming of natural gas, and is comparable to producing hydrogen from wind- or hydro-electric conventional electrolysis. 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.

1.

Introduction

Several thermochemical processes have been proposed for large-scale production of hydrogen using heat from nuclear reactors, including the sulfuriodine cycle (SI), UT-3 method (University of Tokyo), hybrid sulfur, and Ispra Mark 9 process. The sulfuriodine cycle, combined with a new-generation nuclear reactor as the source of heat for the process, is being studied extensively for implementation and deployment in the United States and throughout the world [1]. Life-cycle assessments (LCAs) have been conducted for several of these processes [24]. Because each uses different methodologies and assumptions, comparison of results is difcult.

The goal of this life-cycle assessment is to evaluate the environmental impacts of producing hydrogen using the sulfuriodine thermochemical cycle and a nuclear reactor heat source. The LCA will identify and quantify signicant environmental aspects and assess their impacts. The assessment can be used stand-alone or may be compared with similar life-cycle assessments.

1.1. Thermochemical hydrogen production and the sulfuriodine cycle

The decision to use the SI cycle is based partially on a study performed by General Atomics, University of Kentucky, and

* Corresponding author. Tel.: 1 208 282 7720; fax: 1 208 282 7950. E-mail address: vutgikar@if.uidaho.edu (V.P. Utgikar). 0360-3199/$ see front matter 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.ijhydene.2008.10.059

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Sandia National Laboratories [1]. That study ranked twentyve thermochemical processes using qualitative parameters, such as the number of chemical reactions involved, the number of chemical separations necessary, number and abundance of chemicals involved, process parameters (e.g., temperature and pressure), availability of data, and the number of reports and studies published. Each parameter was assigned a weighting-factor and assigned a numerical score. The sum of the individually weighted values was summed for a total process score. Two processes were selected for nal consideration: the UT-3 cycle and the sulfuriodine cycle. The U.S. Department of Energys Nuclear Hydrogen Initiative funded research on the sulfuriodine cycle, the hybrid sulfur cycle, and the calciumbromine cycle. The sulfuriodine cycle was selected for further development based on its higher predicted efciency. However, the study neglects some industrial-scale issues, like heat exchangers and the size of equipment, and it tends to over-penalize the cycles lacking relevant thermodynamic data [17]. For example, the SI cycle requires a heat source capable of operating at over 1000  C reactor vessel outlet temperature, which results in peak fuel temperatures of 1200  C. Since current-generation light-water reactors operate nominally at less than 350  C, a new-generation advanced high-temperature reactor (AHTR) must be designed [13].

The boundary of the hydrogen plant subsystem includes construction and operation of the physical plant, acquisition of raw materials for the thermochemical process (i.e., water, iodine and sulfuric acid), including the method of production for each chemical used in the process, the energy required for extraction and rening, and its relative abundance. The interface between the two subsystems is a heat transfer loop consisting of an intermediate heat exchanger (IHX) and heat transfer medium (helium gas). This LCA does not include liquefaction, storage and distribution of hydrogen product in the analysis since those operations are independent of the method of production and depend upon the intended use of the product. End-use of the hydrogen product is also excluded from the study since a single purpose would be presumed for the product (e.g., transportation using fuel cells or internal combustion engines) and would not represent the current uses of hydrogen (production of ammonia fertilizer and hydrogenation of petrochemicals).

2.2.

Life cycle inventory

2.

Life cycle assessment (LCA)

The LCA process is dened in the ISO 14040 series of standards and includes goal and scope denition (dening the system under consideration), inventory analysis (identifying and quantifying system input and output), impact assessment (assessing the effects of the activities), and interpretation (evaluating the results) [5].

Once the system boundaries are established, inputs to the system (i.e., inventory) must be dened. Major inputs to the system being studied include materials of construction for the reactor and hydrogen plant, such as concrete, structural steel, stainless steel, and other materials; nuclear fuel; reactor coolant; feed material for the process (iodine, sulfuric acid, and water); fossil fuels and electricity necessary for construction; and energy and materials needed to operate the facility (replacement nuclear fuel, electricity, fossil fuels and electricity, make-up helium gas, process materials, and water).

2.2.1.

Nuclear reactor inventory

2.1.

System denition

Denition of system boundaries has signicant impact on the outcome of an LCA. This LCA denes the boundaries of the hydrogen production system as the nuclear reactor and the hydrogen plant subsystems. The system is analyzed for a functional unit of production of 1 kg of hydrogen. For the system being considered, one or more 600 MW(th) AHTR reactor modules are coupled to a hydrogen production plant [30]. The analysis of the nuclear reactor includes mining, milling, conversion and enrichment of uranium ore; fabrication and transportation of nuclear fuel; construction, operation and decommissioning of the nuclear power plant; and nuclear waste disposal [6]. Some studies do not include disposal of radioactive waste and spent nuclear fuel in the analysis; however, operation of one nuclear reactor for 20 years results in over 35 ton of heavy metal for disposal or reprocessing, not a trivial amount when the large number of nuclear reactors required to support a hydrogen economy is considered. All of the thermal energy from the nuclear reactor is transferred to the thermochemical process through an intermediate heat exchanger (IHX). Additional energy is necessary to operate the reactor and hydrogen plant auxiliary systems [7].

Since the advanced high-temperature nuclear reactor (VHTR) is currently in the conceptual stage of design, it is assumed that advanced nuclear plants are equivalent to existing nuclear plants with regard to quantities and types of materials of construction, although there are differences in construction (e.g., containment and connement structures, shielding, etc.) [3]. This assumption is conservative and provides an upper bound for calculations. Therefore, emissions from materials of construction and construction activities are assumed to be similar. Concrete and steel represent greater than 95% of the materials used for construction of a nuclear reactor plant. Anigstein et al. estimate a 1970-vintage 1000 MW(e) (3000 MW(t)) pressurized water reactor nuclear power plant contains 34,811 metric tons of steel [8]. The reactor and associated systems account for 18,364 ton, with the remainder in the turbine building and electrical generation equipment. Bryan and Dudley, as cited in Peterson, estimate 190 cubic yards of concrete per megawatt of capacity for the same plant [9,10]. Although the sizes of individual reactor components may vary differently (i.e., geometrically for vessels and piping), for conservatism, a linear relationship is assumed between plant size and power capacity. Therefore, the reference 600 MW(t) advanced nuclear plant contains roughly 1/5 of the material as a 3000 MW(th) plant. This results in approximately 3675 metric tons of steel, and 114,000 cubic yards (209,760 ton) of concrete. At the end of the plants 30-year life it will be decontaminated, decommissioned and disposed as waste.

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The core of a 1000 MW(th) reactor contains 75 ton of enriched uranium fuel [13]. Assuming the core loading is proportional to rated power, the 600 MW(t) reference plant contains 45 ton of enriched uranium. To operate at elevated temperatures necessary to support the SI cycle, a new type of nuclear fuel with high-temperature coating is being developed [39]. Advanced nuclear reactors will be designed to achieve higher fuel burn-up which will reduce the quantity of nuclear fuel required, and the quantity of spent fuel to be disposed. Newer fuel enrichment technology (gas centrifuge) requires forty times less energy than the current method (gaseous diffusion) [6]. In 2002, 55% of fuel produced worldwide used gaseous diffusion, and 45% used gas centrifuge for enrichment, whereas all of the fuel produced in the U.S. is by gaseous diffusion [4]. The worldwide trend is to use gas centrifuge technology for all enrichment [6]. Consequently, the emissions associated with future nuclear fuel production, consumption and disposal should be lower for the advanced nuclear plant. To maintain efcient operation, about onethird of the spent nuclear fuel will be removed from the reactor every year and replaced with fresh fuel [13]. Helium is used as a reactor coolant and heat transfer medium in the nuclear reactor and the hydrogen production plant. It is chemically stable, has a relatively high specic heat capacity, and has negligible cross-section for neutron absorption and capture [10]. It is recovered commercially from natural gas deposits by low-temperature cryogenic fractional distillation. It may be present in natural gas at concentrations of up to 7% by volume [31]. In 2006, 170 million cubic meters of helium were produced worldwide [32]. For the purpose of this study, the VHTR is assumed to contain 3.685 tons of helium as reactor coolant, based on similarity to the Fort St. Vrain hightemperature gas reactor [11]. Alternative designs may use different coolant systems. For example, Forsberg proposes to use molten uoride salt coolant, based on higher specic heat capacity and smaller component piping [12]. Large pipe size increases heat loss and cost. In addition to the heat produced by the reactor, approximately 100 MW(e) additional power is required to operate pumps, compressors, and auxiliary equipment associated with the nuclear reactor and the hydrogen generation plant [26]. This study assumes that power is obtained from the U. S. distribution grid, and is generated using the mix of sources identied in the Mid-Western United States [21]. However, if this power would be provided by a nuclear reactor, the resultant GHG emissions would be signicantly lower.

A signicant difference among thermochemical processes involves the chemicals used in the processes. For example, the UT-3 cycle uses bromine, calcium, and iron. Ispra Mark 9 uses iron and chlorine. Hybrid sulfur uses sulfuric acid coupled with electrolysis, whereas the SI process uses sulfuric acid and iodine. Since energy is required to circulate the material through the plant, processes using liquid or gas are preferred over those using solid materials. Iodine is one of the essential elements necessary in the SI cycle. In the United States, iodine is extracted from subsurface brine associated with natural gas and oil deposits [20]. Energy must be supplied to pump the brine, compress air for the blowout process, to purify and crystallize the product. The current cost of iodine is $17.03 per kg [20]. Although the stoichiometric amount of iodine required for the SI cycle is 2120 ton, bench-scale experiments indicate a need for approximately 10,000 ton of material [17]. Worldwide production of iodine is roughly 18,000 ton per year [33]. Assuming nominal process losses of iodine (lifetime 10%), a signicant percentage of the current worlds production of iodine is involved in the inventory of one hydrogen plant. The other substance required in the SI cycle is sulfuric acid. The reference plant will contain about 100 ton of high-purity sulfuric acid. Sulfuric acid is one of the most widely used chemicals in industry. Although much of the sulfuric acid in use is recovered from industrial processes, high-purity sulfuric acid is produced from oxidation of sulfur and sulfur dioxide [40]. For every mole of hydrogen produced, one mole of highpurity water must be consumed in a stoichiometric reaction. For the reference plant producing 200 ton of hydrogen per day, 1.77E 7 metric tons of water are consumed over the 30 year life of the plant. Bench-scale experiments demonstrate that water must also be supplied in excess up to eight times the required amount for the reaction to proceed [27].

2.2.3.

Intermediate heat exchanger (IHX) inventory

2.2.2.

Hydrogen generation plant inventory

The reference hydrogen plant produces 200 ton of hydrogen per day of operation. Assuming a capacity factor of 0.9, about 1.97E 9 kg of hydrogen are produced over the 30-year life of the plant. Hydrogen product is available at the plant gate as a compressed gas at 346 psia and 99.6% purity [35]. Spath and Mann have estimated types and quantities of materials of construction for a hydrogen generation plant using steam reforming of natural gas [28]. Assuming similar construction for the SI cycle, the plant requires 3272 ton of steel, and approximately 10,242 ton of concrete (cement with aggregate). They further estimate that materials of construction and decommissioning account for 0.4% of total GHG emissions.

Design of an IHX capable of operating at the required temperature (1000  C) poses an engineering challenge, requiring advanced design and materials. Since designs for the IHX are still conceptual, the type of heat exchanger (e.g., blade, printed circuit), types and quantities of materials are not known at this time. For reference, the Calder-Hall reactor has four Inconel heat exchangers, each 18 feet in diameter, 70feet high, and each weighing 200 ton. Some advanced, hightemperature resistant materials proposed for the IHX include SiC and Inconel 600H [34]. Silicon carbide requires more energy to produce (180 MJ/kg), therefore the contribution from the IHX to the total emissions would increase over more conventional materials [22].

2.2.4.

Emissions inventory

The total emissions from the proposed system will be the sum of the emissions from the nuclear power plant and the SI hydrogen generation plant subsystems. A summary of lifecycle emissions from several different studies of nuclear power plants are shown in Table 1. Primary focus is on carbon dioxide emissions and global warming potential (GWP) since they have global impacts. Acidication, measured as grams of SO2-equivalent, is a regional effect and results must be interpreted for the specic geographic area of concern [42].

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Table 1 Life cycle emissions inventory from nuclear power plants Author
Koch [23] Meier [24] Krewitt [25] CRIEPI [43] British Energy [6]

CO2 (g/kWh)
259 17 19.7 22 5.05

SO2 (mg/kWh)
350 Not reported 32 Not reported 10

NOx (mg/kWh)
2100 Not reported 70 Not reported 20

2.3.

Life cycle inventory assessment

Life cycle assessment of each subsystem uses data such as specic energy consumption (MJ/kg) or specic emission factors (grams of emissions per kilogram of product). Those quantities are then summed to yield total emissions for the nuclear hydrogen generation system.

2.3.1.

Nuclear reactor plant inventory assessment

Total energy used in the production of steel is estimated to range from 25.5 GJ/ton for mild steel, to 100 GJ/ton required for specialty and stainless steel [15,22]. Mild steel can be prepared from secondary scrap steel in a modern, efcient electric arc furnace. Nuclear-grade steel (meeting nuclear quality assurance standards) requires primary steel produced from primary sources. Using a mid-point value of 60 GJ/ton results in 2.21E 5 GJ required for the 3675 metric tons of steel in the nuclear plant. Coking coal, used for primary steel production, emits 0.111 kg CO2/MJ [21]. This results in emissions of 8.17E 6 kg CO2-eq to produce the steel necessary for a nuclear plant. Since 1.97E 9 kg of hydrogen are produced over the 30-year life of the plant, the specic carbon emission for steel is 4.15 g CO2-eq/kg of hydrogen produced. Alternatively, Worrell estimates emission of 0.50.82 ton CO2/ton steel. Using the higher estimate results in 1.53 g CO2/kg H2, about one-half of the calculated value. The primary fuel for production of cement is coal. Portland cement production requires 4.896.33 MJ per kilogram of cement [14]. With the addition of sand and aggregate, production of concrete requires a total of 0.893 MJ/kg [15,16]. For 209,760 ton of concrete contained in the nuclear plant, this represents 1.87E 8 MJ, which results in emission of 4.76E 7 kg CO2-eq. For 1.97E 9 kg of hydrogen produced over the life of the plant, the specic carbon emission for concrete is 24.2 g CO2-eq/kg of hydrogen produced. The total calculated emissions from steel and concrete are 24.2 g CO2-eq/kg H2. Since this represents about 95% of the emissions from construction, the total emissions are 25.5 g CO2-eq/kg H2. Emissions from decontamination and decommissioning are assumed to be 10% of that from construction [35]. This adds 2.6 g CO2-eq/kg H2, for total emission of 28.1 g CO2-eq/kg H2 from plant construction and decommissioning. Mining and milling of uranium ore result in 1.85 g CO2/kWh [6]. The contribution to emissions from enrichment is dependent upon the type of process used. Enrichment by gas centrifuge adds 0.43 g CO2/kWh, whereas gaseous diffusion uses forty times the energy, resulting in 17.2 g CO2/kWh [19]. Using these values, the contribution of emissions from nuclear fuel is either 1372.18 g CO2/kg H2 if gaseous diffusion

is used, or 164.23 g CO2/kg H2 if a gas centrifuge is used. This reactor is assumed to be constructed in the U.S. Since gaseous diffusion is used to produce all of the uranium fuel in the U.S., the higher value is used in this LCA. Information regarding specic energy consumption and emissions for helium is not reported in the literature, and existing life cycle inventory databases are not sufciently mature to include all substances of interest. Lacking specic data, an alternative method of calculating GHG emissions is necessary. It is reasonable to assume that for commonly available substances, the cost of the commodity (less a reasonable amount for prot and overhead) is directly proportional to the energy required for production. The cost of helium in the U.S. is regulated by statute at $1.965 per m3 for government supply. Commercial prices range $2.42 2.63 per m3 [20]. With a density of 0.0001785 g/cm3, each cubic meter of helium contains 0.1785 kg. Thus, the regulated price of helium is $11.00/kg, and the commercial price ranges from $13.56 to 14.73 per kilogram. Natural gas is the primary energy for production of helium and sells for $0.60 per therm (105.5 MJ). Using the regulated price of helium and CO2 emissions for natural gas results in 29 MJ/kg He, and 0.5 kg CO2-eq/kg He. Assuming the reactor inventory is 3.685 ton (3.69E 3 kg), the gross energy requirement for the helium coolant inventory is 1.06E 5 MJ, which results in emission of 1.84E 6 g CO2-eq. For 1.97E 9 kg of hydrogen produced over the life of the plant, the specic carbon emission from helium is 9.34E 4 g CO2-eq/ kg H2. Assuming the hydrogen plant has the same volume of helium as the reactor, and assuming 10% loss per year from the system, the total specic carbon emission for helium is 0.002 g CO2-eq/kg of hydrogen produced. Operation of the nuclear and hydrogen plants requires an additional 100 MW(e) of electricity [26]. If this power is obtained from the grid in the U.S., which primarily uses coal for electrical generation, this would result in an additional 7804 g CO2-eq/kg H2. In Europe, or U.K., electricity is generated primarily from nuclear power. The same 100 MW(e) would result in only 60.6 g CO2-eq/kg of hydrogen.

2.3.2.

Hydrogen plant inventory assessment

Spath and Mann estimate construction of a plant for steam reforming of natural gas requires 3272 ton of steel, and 10,242 ton of concrete [28]. They have calculated total emissions from this plant at 11,888 g CO2/kg H2. Construction of an SI cycle plant and the steam reforming plant is assumed similar for the purpose of this LCA. A value of 0.4% is provided as the contribution to emissions from plant construction and decommissioning, yielding 47.55 g CO2/kg H2. Data regarding specic energy consumption and specic emissions for the production of iodine are lacking in the literature. The same method used to determine emissions from helium can be applied to the iodine inventory. The cost of iodine is reported as $17.03 per kilogram [20]. If energy is supplied totally by natural gas, production of 1 kg of iodine requires 97 MJ. Heat from recycled brine could conceivably supply 50% of the process energy, which would reduce the specic energy requirement range to 49 MJ/kg of iodine. Resultant CO2 emission would be 1.8/kg CO2-eq/kg I2. The hydrogen plant inventory of iodine is 2120 ton, based on the stoichiometric reaction. Using 49 MJ/kg yields 1.04E 8 MJ, and

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5.77E 9 g CO2-eq for the life of the plant. Adding the contribution from 10% process loss over the entire life of the plant results in 0.33 g CO2-eq per kilogram of hydrogen. The U.S. Environmental Protection Agency reports an emission factor of 4.05 kg carbon dioxide emitted per metric ton of sulfuric acid produced [40]. The initial inventory of H2SO4 in the hydrogen plant is 100 ton. The assumed loss rate is 1% per year of operation, therefore 130 ton of sulfuric acid is necessary to operate the process. This yields 526 kg of CO2 over the life of the plant, or 5.26E-4 g CO2-eq/kg H2. In order to supply high purity water as the source of hydrogen requires 315 kWh/m3. Assuming the density of water is 1 g/cm3, 1.77E 7 m3 of water are used over the life of the plant. Reverse osmosis purication requires 315 kWh/m3 (18309150 g CO2/m3) resulting in 16.482.18 g CO2/kg H2. Because of their relative size and importance, the contributions from intermediate heat exchangers are calculated separately from the nuclear and hydrogen plants. Based on the size of the Calder-Hall reactor heat exchangers, 800-tons of Inconel alloy are required for fabrication. Using a value of 60 GJ/ton to produce steel results in 4.8E 7 MJ required, and emission of 1.76E 9 g CO2-eq. The production of 1.97E 9 kg H2 yields a contribution of 0.89 g CO2-eq/kg H2.

2.3.3.

Resource depletion

There is consensus that resource depletion should be considered in life cycle analyses. The impacts of resource management (i.e., extraction and processing) and depletion may surpass other aspects of the life cycle [37]. In order to produce 1 ton of hydrogen requires circulation of large quantities of material, from 500 to 10,000 ton depending upon the material [17]. Iron, chlorine, and calcium are relatively abundant and easily produced in quantities required. Bromine and iodine, on the other hand, are less abundant and require energy-intensive separation techniques. Scarcity is dened as a change in the availability of a resource over time [38]. The availability of a resource may depend upon other factors. For example, production of helium is tied to the production of natural gas. As natural gas becomes scarcer, the supply of helium may be less stable and the cost may increase. Similarly, iodine production in the U.S. is extracted from subsurface brines, often associated with oil production. As oil becomes scarcer, the supply of iodine may be affected. As discussed earlier, production of iodine worldwide is 18,000 ton per year. One sulfuriodine hydrogen production plant would require 56% of the current annual world production capacity of iodine. Steel and concrete, on the other hand, are relatively abundant, as is sulfuric acid. Global steel production in 1997 was 773 million tons. Worldwide production of cement totaled 1.25 billion tons in 1991 [14]. In 1995, 35.6 million tons of sulfuric acid was produced in the United States [41]. Construction and operation of the reference plant have a negligible effect on the supply of these resources.

3.

Sensitivity analysis

Due to differing assumptions in calculations, variability in data, and differences in reporting, uncertainty exists in the

calculation of emissions. In particular, the chemical industry is restrictive concerning information on certain production processes [29]. Therefore, specic data is lacking regarding key materials in the SI process, such as specic energy consumption and GHG emissions in the production of helium and iodine. Sensitivity analyses were performed to evaluate the effects of variability of data on the calculation of overall life cycle emissions. Since the AHTR and the hydrogen plants are currently in the conceptual stage, the types and quantities of materials have been estimated. Projects at the conceptual stage typically exhibit uncertainty in the range from 10 to 25% [18]. As seen in Table 2, variability in data for materials of construction has little effect on overall GHG emissions. Even when that data are adjusted upward by 50%, the total emissions are affected by only 1.6% (6.7% versus 5.1% of total). When the relatively small contribution to total emissions from these materials is considered, a large error in calculated values results in very small changes to the results of the LCA. The same is true for chemical inventory of the hydrogen plant, i.e., helium, iodine and sulfuric acid. Assumptions regarding plant life and capacity factor affect specic emissions and unit cost of a process. For example, General Atomics assumes a 60-year plant life, with a 90% availability factor, resulting in 54 effective-years of operation. For ISPRA Mark 9, the corresponding values are 30-years, 80%, and 24 effective-years. Uranium Information Center uses a 40year life and 80% capacity factor, resulting in 32 effective-years. This LCA uses a 30-year plant life and 90% availability factor. Since the SI process requires an AHTR, the shorter plant life is assumed to account for high-temperature corrosion, and fatigue due to thermal cycles in both the reactor and hydrogen plants. The 90% availability factor is based on actual experience in operating nuclear reactors gained over the past 40 years. The largest single contributor to greenhouse gas emissions from the nuclear fuel cycle is operations associated with mining, milling and enrichment of nuclear fuel. According to British Energy, about 37% of the total carbon footprint results from extraction, conversion, enrichment and fabrication of nuclear fuel [6]. The amount of emissions is proportional to the concentration of uranium present in the ore, as well as the method of enrichment. The remainder of the emissions results from nuclear plant operations; construction and decommissioning; fuel reprocessing; and construction and operation of radioactive waste facilities. For this LCA, the largest potential contributor to greenhouse gas emissions is the electrical power required to operate the nuclear and hydrogen plants process and auxiliary equipment. That power is assumed to originate from the power grid in the U.S., generating electricity from the combustion of coal, oil, natural gas, and about one-fth from nuclear and renewable sources. Emissions from that power alone are 7804 g CO2/kg H2. These emissions would be reduced by 99% if that energy could be supplied from nuclear power, either from a separate power plant or a hybrid nuclear plant. The use of a hybrid 1000 MW(th) nuclear plant could supply both 600 MW(th) nuclear heat to the SI thermochemical cycle and 100 MW(e) electrical power for nuclear plant operations and the SI process equipment. This would increase emissions due to construction of the turbine building and power

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Table 2 Greenhouse gas emissions for sulfuriodine cycle Component/material

Helium Sulfuric acid Iodine Water (high purity) Hydrogen plant construction [28] Steel Cement Aggregate Decommissioning Heat exchanger Subtotal hydrogen plant subsystem Nuclear plant Construction Steel Concrete Remainder Decommissioning Nuclear fuel Operating electrical Subtotal nuclear plant subsystem Total

Inventory
3.7 ton 100 ton 2120 ton 40 ton

Specic CO2 emissions (g CO2-eq/kg)

0.5 4.1E 6 2.0 82.18 (11,888) 0.4% of total [28]

Total GHG emissions (g CO2-eq/kg H2)

0.002 0.000526 0.33 82.18 45.77

3272 ton 10,242 ton (10% of construction) 800 ton

0.89

0.9 129.2 32.3 (36.7)

3675 ton 209,760 ton (5% of total) (10% of construction) 45 ton 100 MW(e)

4.15 24.2 1.3 2.6 2277.5 (1372.2) 60.6 (7804)

2277.5 (1372.18) 60.6 (7804) 2370.4 (9212) 2499.6 (9341.9)

Note: Values in parentheses for nuclear plant subsystem assume electrical power obtained from the U.S. grid. Other values assume power from hybrid nuclear plant or other nuclear source.

generation equipment by a factor of two. However, as demonstrated in this LCA, construction is a relatively small contributor to overall emissions. The reactor, however, would require 66% more nuclear fuel, increasing the GHG contribution to 2277.5 g CO2/kg H2. Both of these together would result in a total GWP of for the system of 2675 g CO2/kg H2. This is still a factor of 34 less than production of hydrogen by steam reforming of natural gas.

4.

Discussion of results

Results of various energy and life-cycle analyses show that nuclear-based processes for production of hydrogen result in signicantly lower usage of fossil fuels and lower greenhouse gas emissions than steam methane reforming, which is the predominant method of hydrogen production. Steam reforming of natural gas results in 900011,888 g CO2-eq/kg H2. Coal gasication produces 12,400 g CO2-eq/kg H2 [35,36]. On the other hand, high-temperature electrolysis of water using a very hightemperature gas-cooled nuclear reactor (VHTR) results in 2000 g CO2-eq/kg H2 [3]. Utgikar and Bradley estimate greenhouse gas emissions of 2515 g CO2-eq/kg H2 using Ispra Mark 9 process coupled with VHTR [2]. For each process, nuclear reactor construction and operation contribute 1250 g CO2-eg/kg H2. Wu et al. performed a life cycle assessment for generic thermochemical processes resulting in 2530 g CO2-eq/km, which includes end-use in hydrogen fuel-cell vehicles. Assuming 95 km/kg H2 results in w2700 g CO2-eq/kg H2. They conclude that hydrogen production in a central plant using a thermochemical process coupled with a nuclear heat source reduces total energy usage by 2126%, and reduces greenhouse gas emissions by 7480%.

For comparison, production of hydrogen from solar (photovoltaic), solar (thermal), wind and hydro-electric energy results in 2124, 800, 860, and 584 g CO2-eq/kg H2, respectively [44,45]. From a strict comparison of greenhouse gas emissions, these technologies appear competitive with nuclear-power based production methods. Further analysis of these renewable energy technologies is necessary to determine their overall competitiveness with respect to cost, spatial requirements, and other environmental impacts. Such analysis is beyond the scope of this study. The results of this LCA compare favorably with previous studies. The total global warming potential for the sulfur iodine cycle coupled with an advanced high-temperature reactor is 2500 g CO2-eq/kg H2, assuming electrical power to operate the reactor pumps and process equipment is supplied from a nuclear reactor. If that power is supplied from the grid in the U.S., the carbon footprint of this process is nominally only 20% better than the current method of hydrogen production, with emissions of 9477 g CO2-eq/kg H2.

5.

Conclusion

It is concluded that production of hydrogen from the sulfur iodine thermochemical cycle coupled with a nuclear reactor results in approximately one-fth to one-sixth the greenhouse gas emissions from steam reforming of natural gas. It is further shown that relatively little difference in greenhouse gas emissions exists between several hydrogen production processes using a nuclear reactor as the heat source. Life-cycle assessments should be performed which examine each process objectively, consistently, and equitably. Further work needs to be done to standardize life-cycle

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analyses for the various available nuclear options to enable valid comparisons. However, this environmental LCA provides only one input to the decision-making process. The decision to use a specic thermochemical cycle should be based on objective criteria, as well as technical feasibility and life-cycle environmental impacts. Other factors to be considered would include socio-economic impacts, resource usage and depletion, politics, and national strategy. Sensitivity analyses should be performed to determine which factors have the greatest effect on results. Ultimately, the results of a life-cycle analysis must be examined in the context of its stated purpose. If the intent of hydrogen generation is to replace hydrocarbon-based fuels in automobiles and enhance energy independence, then higher greenhouse gas emissions may be acceptable from the process. On the other hand, if reducing GHG emissions is the ultimate goal, various LCAs can be compared and the appropriate technology selected.

references

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