Prosiding Seminar Nasional Teknologi Energi Nuklir 2016 ISSN: 2355-7524 Batam, 4-5 Agustus 2016

STUDY ON ROLE OF NUCLEAR FOR CO2 CONVERSION IN PETROCHEMICAL INDUSTRY

Djati H Salimy1, Ign. Djoko Irianto1 1) Center for Technology and Safety (PTKRN) National Nuclear Energy Agency of Indonesia (BATAN) Puspiptek Area Serpong Tangerang Selatan 15310 Indonesia Email: [email protected]

ABSTRACT STUDY ON ROLE OF NUCLEAR HYDROGEN COGENERATION FOR CO2 CONVERSION IN PETROCHEMICAL INDUSTRY. Study on the process of nuclear hydrogen cogeneration for the conversion of CO2 in the petrochemical industry has conducted. The purpose of the study was role of nuclear hydrogen cogeneration to support the conversion of CO2 in the petrochemical industry. The method used is literature study based on the results of existing research. The results showed that nuclear hydrogen cogeneration process capable of providing large quantities of hydrogen needed as an important raw material in the petrochemical industry. Cogeneration system is also capable of providing nuclear heat energy that can be used to execute the process of CO2 conversion. Conventionally, the needs of hydrogen as raw material for the petrochemical industry are supplied with process steam reforming of natural gas, while the needs of heat energy derived from natural gas combustion. Replacement of conventional technology of steam reforming of natural gas and thermal energy sources of natural gas combustion to CO2 conversion with nuclear hydrogen cogeneration system, capable of suppressing the rate of depletion of fossil fuel natural gas that has implications for the reduction of CO2 emission rate significantly.

Keywords: cogeneration system, CO2 conversion, CO2 emission

ABSTRAK STUDI PERAN KOGENERASI HIDROGEN NUKLIR UNTUK KONVERSI CO2 PADA INDUSTRI PETROKIMIA. Telah dilakukan studi proses kogenerasi hidrogen dengan energi nuklir untuk proses konversi CO2 pada industri petrokimia. Tujuan studi adalah untuk memahami peran kogenerasi hidrogen nuklir untuk mendukung proses konversi CO2 pada industri petrokimia. Metode yang digunakan adalah studi pustaka berdasarkan hasil penelitian yang sudah ada. Hasil kajian menunjukkan bahwa proses kogenerasi hidrogen nuklir mampu menyediakan hidrogen dalam jumlah besar yang diperlukan sebagai bahan baku penting dalam industri petrokimia. Sistem kogenerasi juga mampu menyediakan energi panas nuklir yang dapat digunakan untuk menjalankan proses konversi CO2. Secara konvensional, kebutuhan hidrogen sebagai bahan baku industri petrokimia dipasok dengan proses steam reforming gas alam, sedang kebutuhan energi panas diperoleh dari pembakaran gas alam. Penggantian teknologi konvensional steam reforming gas alam dan sumber energi panas pembakaran gas alam untuk konversi CO2 dengan sistem kogenerasi hidrogen nuklir, mampu menekan laju pengurasan bahan bakar fosil gas alam yang berimplikasi pada pengurangan laju emisi CO2 yang cukup signifikan.

Kata kunci: sistem kogenerasi, konversi CO2, emisi CO2

INTRODUCTION

Increased of CO2 content in the atmosphere, due to the burning of fossil fuels and deforestation, cause environmental damage due to the effects of global warming caused by greenhouse gases. It encourages research activities around the world to capture and utilize the CO2. One way to reduce CO2 emissions is to convert it into products that have value added. Beside, CO2 can be considered as an abundant and renewable raw material for various products of the petrochemical industry and synthetic fuels. CO2 has an advantage over other C1 toxic materials such as monoxide and phosgene [1]. Research for the conversion of CO2 into chemical products or synthetic fuels is one of the areas of active scientific research. The production of synthetic fuels from CO2 could significantly affect the mitigation of global CO2 emissions due to the volume of CO2 that is utilized quite large [2]. To

89 Study on Role of Nuclear Hydrogen Cogeneration For CO2.... ISSN: 2355-7524 Djati H Salimy dkk produce petrochemicals by conversion of CO2 needs utilization of hydrogen. Massive system is needed to supply hydrogen. electrolysis is one mature technology to produce hydrogen. Some studies indicate that big scale water electrolysis is an interesting and important alternative, especially when there are excess electricities near the petrochemical complexes [3]. Water splitting by utilizing high temperature nuclear reactor is also interesting technology to supply hydrogen for CO2 conversion [4]. One of the applications of R & D in high-temperature nuclear reactor that is promising for industrial applications in the future is nuclear cogeneration process of hydrogen production by thermochemical process which uses water as main raw material [4]. Principally, this process is a process of thermochemical decomposition of water to produce hydrogen and which occurs at high temperatures. Heat energy of nuclear reactor coming out from high-temperature nuclear reactors can serve as heat energy source to run the process. Among the nuclear thermochemical process, a process with iodine-sulfur cycle is the most advanced. The process that was originally developed by General Atomics in America in the 1970s, later adopted and developed by several countries such as Japan, Germany, China, France, and South Korea. Japan is targeting couple HTTR with thermochemical processes of iodine-sulfur cycle can be realized by the end of the decade in 2010 [5]. South Korea is also adopting this process in the early 2000s, targeting the demonstration plant scale operation in 2026 [6]. National Nuclear Energy Agency (BATAN) as a R&D institute in the field of nuclear technology, currently develop nuclear energy system based on the high temperature gas cooled reactor (HTGR) named RGTT200K. Energy conversion system of RGTT200K is designed in a cogeneration configuration for electricity production and or for process heat for industrial purposes. To support the design of cogeneration system, some R&D of cogeneration system has been done. The assessments of nuclear process heat application, such as hydrogen production (steam reforming of LNG, water splitting), coal gasification, etc. are also continually in progress. Trend of R&D in developed countries, related to application of nuclear hydrogen cogeneration to convert CO2 to valuable product also must be anticipated. Nuclear hydrogen cogeneration can become the important key technology in the future to convert CO2 into alternative fuels and valuable chemicals. From the system, hydrogen production will become an important chemical feedstock, while the availability of high-temperature thermal energy can be a source of heat energy required for the process of CO2 conversion [7]. Utilization of high temperature nuclear reactors as a source of heat energy can save the burning of fossil fuels significantly, which implies a decrease in the rate of CO2 emissions. While the use of CO2 as a raw material to be attractive alternatives to reduce the concentration of CO2 in atmosphere. In this study, the analysis is limited to nuclear hydrogen cogeneration for conversion of CO2 into urea and methanol that are an important product in petrochemical industry. Beside, both products are also the product that consume hydrogen and CO2 in large quantity. In terms of thermal energy consumption, both products also require large amounts of heat energy. The purpose of the study was to understand the role of nuclear hydrogen cogeneration to support the conversion of CO2 in the petrochemical industry particularlyin converting CO2 into methanol and urea. The results are expected become important input to the stakeholders in formulating policies of nuclear energy development in Indonesia, particularly the development of the use of high-temperature nuclear reactor in the future.

NUCLEAR COGENERATION FOR CO2 CONVERSION Nuclear Hydrogen Cogeneration Cogeneration, also known as combined heat and power (CHP), is a very efficient; clean; and reliable approach to generate power and thermal energy from a single fuel source [8]. Typically, cogeneration plants recover percentage of the “” that is otherwise discarded from conventional power generation. The recovered waste heat is effectively utilized in other thermal energy applications. Current nuclear power plants have low thermal efficiencies generally in the range of 30 to 35% compared to other steam cycle energy conversion systems. Countries embarking on nuclear power should consider co-generation and the use of waste heat from a NPP to increase energy utilization and overall efficiency.

90 Prosiding Seminar Nasional Teknologi Energi Nuklir 2016 ISSN: 2355-7524 Batam, 4-5 Agustus 2016

In a number of countries, co-generation and heat production using nuclear reactors is already an effective way to meet different types of energy needs. Currently, there are 79 reactors operating in cogeneration mode and the potential for applying this technology more widely appears promising [9,10]. Heat applications cover a wide range of specific temperature requirements starting from low temperatures i.e., just above room temperature for applications such as hot water and steam for agro-industry, district heating, and sea water desalination; reaching more than 1000° Celsius for process steam and heat applications i.e., for chemical industry and high-pressure injection steam, enhanced oil recovery, oil shale and oil sand processing, oil refinery, refinement of coal and lignite, and water splitting for the production of hydrogen. With the rapid increase in energy demand (for both electricity and heat), concern over global warming could pave the way for nuclear energy to exert a major positive impact on energy security and climate change. Fgure 1 shows the typical nuclear cogeneration system, using HTGR as energi source.

Figure 1. HTGR Cogeneration for electricity, hydrogen, and desalination [11]

The R & D of hydrogen production from water with a thermochemical process was developed very intensively in the developed countries. One promising process is the process of water splitting thermochemical iodine-sulfur cycle. The process that was originally developed by General Atomics in America in the 1970s, then adopted and developed by several countries such as Japan, Germany, China, France, and South Korea. In the early 1990s Japan began to conduct an intensive study of the thermochemical iodine-sulfur cycle, and successfully did the continuous operation laboratory scale in 1994, in spite of the thermal efficiency of less than 20%, very far from the desired thermal efficiency (51%) [5]. In the late 1990s Japan build a demonstration plant adjacent to the reactor HTTR with the target coupling them at the end of 2010 decade. Figure 2 shows the HTGR utilization for hydrogen production with the process of thermochemical IS.

Figure 2. HTGR for hydrogen cogeneration, thermochemical IS process [11] CO2 Conversion

The issue of global warming induced by CO2 emissions has become a global issue that is increasingly important in the world. It can be a major cause of climate change and the negative impact on human life. One of the indicators used in analyzing the issue of global warming is the increase of greenhouse gases, especially CO2, as a result of human activities. So far, efforts have been started to reduce the impact of global warming, such as reforestation, energy saving, the use of new and renewable energy, and utilization of engineering and technology. One of the technologies used is carbon capture and storage technology named CCS (Carbon Capture and Storage).

91 Study on Role of Nuclear Hydrogen Cogeneration For CO2.... ISSN: 2355-7524 Djati H Salimy dkk

Figure 3. Capture and separation of CO2 [12]

CCS is most commonly defined as the capture of CO2 from an industrial or power- sector point source combined with its transport and its storage in stable geological formations [12]. CCS is seen as one of the possible technologies in the portfolio of mitigation options that can contribute to cost-effective emission reductions. In theory, CCS facilitates the continued use of fossil fuels while reducing atmospheric CO2 emissions. Beside that, carbon capture and utilisation (CCU) has also been suggested as a partial alternative to divert some carbon dioxide from the transport and storage route. While carbon dioxide is considered to be a thermodynamically and chemically stable molecule under standard conditions, it can react with other chemical feedstocks given sufficient energy or using a catalyst to produce value added commodity chemicals [13] and fuels [14].

In principle the CCS is technology to capture and separate CO2 from other gases, and then transported to another place to be stored in the stable geological disposal [12,15] . While, in the CCU technology, captured CO2 will be used as raw materials for industries. In this way, beside the advantages of a decreasing the rate of CO2 emissions, also obtained added value of CO2 as raw materials. Some industries that use CO2 as the raw material become the target of this program.

Figure 3 shows the principle of capture and separation of CO2 from various industrial processes producing CO2. Figure 4 demonstrates the potential use of CO2 as raw material for industrial processes [16].

Figure 4. Potential application of CO2 Utilization [16]

Couple of Nuclear Hydrogen Cogeneration and CO2 Conversion High temperature gas-cooled reactors (HTGR), one of nuclear reactors jfyufthat operate at high temperatures open up opportunities not only the utilization of thermal energy for electricity generation, but it can be operated in the mode of cogeneration to generate both electricity and process heat. The technology of nuclear hydrogen cogeneration not only offers the availability of hydrogen as an important raw material of the petrochemical industry, but also provides enables the availability of thermal energy in the form of process heat, process steam and electricity which needed as the energy source of the petrochemical industry. In this study, discussion is limited to coupling of nuclear hydrogen cogeneration to support the conversion of CO2 into urea and methanol. Urea and methanol are petrochemical products that require raw materials of hydrogen and CO2 in relatively large quantities. As a final product, urea will play an important role as an agricultural fertilizer to

92 Prosiding Seminar Nasional Teknologi Energi Nuklir 2016 ISSN: 2355-7524 Batam, 4-5 Agustus 2016 increase agricultural productivity due to the limited agricultural land and the increasing food needs. While methanol is a potential alternative fuels as a source for a .

Figure 5. Couple of nuclear hydrogen cogeneration with CO2 conversion to urea [7]

Figure 5 shows the coupling of nuclear cogeneration for the conversion of CO2 into urea, which is the result of previous studies [7]. In conventional processes, the technology of steam reforming of natural gas is used as a technology to produce hydrogen as a feedstock to produce ammonia at ammonia unit. The needed CO2 in urea synthesis unit supplied from the product of side reactions that occur in the process of steam reforming of natural gas. In the process, by applying nuclear hydrogen cogeneration, natural gas steam reforming function is replaced by a nuclear process of water splitting to produce hydrogen needed for ammonia plant [7,17]. While CO2 requirements for urea synthesis supplied from CO2 emissions coal power plant. In this system, HTGR nuclear reactor is utilized as back bonne of utility plant that will supply the energy needs in the form of process heat, process steam and electricity.

Figure 6 shows nuclear hydrogen cogeneration coupling for the conversion of CO2 into methanol [18]. In conventional processes, the technology of steam reforming of natural gas is used as a technology to produce synthesis gas (a mixture of hydrogen and CO), then with a specific catalyst, hydrogen and CO is reacted to form methanol. In the process, by applying nuclear hydrogen cogeneration, the function of natural gas steam reforming is replaced by a nuclear process of water splitting to produce hydrogen needed at the ammonia plant. Unlike the process of steam reforming of natural gas, the nuclear water splitting is not generating CO or CO2. Instead needs CO2 and CO in methanol synthesis unit is supplied by CO2 emissions of coal power plant. In this system, HTGR nuclear reactor is utilized as back bonne for utility plant that will supply the energy needs in the form of process heat, process steam and electricity.

Figure 6. Couple of nuclear hydrogen cogeneration with CO2 conversion to methanol [18] DISCUSSION The use of nuclear energy has mostly concentrated on producing electricity. Another established but much smaller application has been as a power source for ships: submarines, icebreakers and even merchant ships. Non-electricity applications based on direct use of heat generated in the fission process of water cooled nuclear reactors could include process heat for various low temperature industrial applications, desalination and district heating. A modern unit with a generating capacity of 1,800 MWe could also produce 1,000 MW of heat for district heating [10]. In this case the electrical output would fall by about 200 MW, but the total efficiency would increase from less than 40% to almost 60%. This in turn would cut CO2 emissions by 2 million tons a year if the use of the waste heat from the nuclear plant avoided the need to burn an equivalent amount of natural gas and coal. The system is economically

93 Study on Role of Nuclear Hydrogen Cogeneration For CO2.... ISSN: 2355-7524 Djati H Salimy dkk viable only if the distance between the production and use of the heat is not too great; it should be less than 100 km. The efficiency of electricity production can be increased by using higher temperature, this also expands the range of possible applications for process heat. Industrial processes which need process heat at high temperatures include wood pulp manufacture (around 400°C); desulphurization of heavy oil in petroleum refining (around 500°C); production of syngas, styrene, ethylene and hydrogen via steam reforming, Copper-Chlorine (around 550°C) or Iodine-Sulphur thermochemical processes (around 800°C); and the manufacture of iron, cement and glass (around 1,000°C) [19]. In nuclear terms such temperatures can only be achieved by the various Generation IV reactors, which also introduce entirely new operating principles and safety features [20]. The creation of entirely new applications for nuclear power, such as process heat and hydrogen, is one of the main objectives in the development of Generation IV technologies [19, 21]. However, not every type of Generation IV reactor will be suitable. For processes requiring temperatures in the range 500–900°C, the gas-cooled HTR (High Temperature Reactor) and VHTR (Very High Temperature Reactor) have the clearest potential in the near future. The high-temperature Pebble Bed Reactor (PBR) is especially designed for cogeneration. HTRs could extend the use of nuclear fission beyond electricity production, replacing fossil fuels in supplying heat to petrochemical plants, steel plants and paper mills, and producing energy carriers such as hydrogen [11]. A nuclear reactor capable of producing both electricity and high-temperature heat would open up additional industrial applications. These include the possibility of producing hydrogen in industrial quantities and very efficiently, based on high temperature electrolysis or thermal decomposition of water. HTGRs are under development for use in the process industries, and may become available within a decade. They operate at peak temperature of 700 – 850oC and have thermal output in the range of 250 – 600 MWt. China and Japan have built test reactors. In China, the construction of an HTR-PM (High Temperature Reactor-Pebble Bed Module) reactor started in December 2012. The HTR-PM power plant has two reactors and the plant is expected to be in operation by the end of 2017 [22].

From the point of CO2 conversion, recovery and utilization of CO2 is a technology known since the second half of 1800’s [13]: three major processes were developed between 1869 and 1922, namely the synthesis of salicylic acid from phenol–salts (Na and K) and CO2 discovered in 1869, the Solvay process for the synthesis of NaHCO3–Na2CO3 developed in 1882, and the conversion of ammonia and CO2 into urea achieved in 1922. In all such applications, CO2 recovered from other industrial processes (synthesis of ammonia or carbonated rocks decomposition for the production of CaO) was used. Such processes are thermal reactions occurring in a mild range of temperature, not exceeding 200oC.

The efficient utilization of CO2 has attracted considerable attention from fundamental research to industrial application in recent years [23,24]. The efficient utilization of (renewable) CO2 will not only help to alleviate greenhouse effect, but also to obtain useful chemicals [1]. Heterogeneous catalysis, electrocatalysis and are presently the three predominant chemical methods for converting CO2 into some useful chemicals, such as methanol, formic acid and formaldehyde, etc. [25,26]. Methanol is one synthetic alternative fuel that is targeted by researcher in the world as one of important product from CO2 conversion. China is the country holding the highest number of patents for CO2 conversion to methanol issued between 2008 and 2013 [27,28].

This CO2-to-fuel integrating the heat from nuclear plant technology could lead towards the sustainable development in the long term since cement industries, pulp and paper industries, as well as steel industries are the boundless sources of CO2 [28]. Until now, CO2 to fuel has been usually considered coupled to renewable sources such as wind power. In France 14% of electrical power is produced by renewable energy but also around 78% is provided by nuclear reactors [4]. Nuclear power is also a low CO2 footprint energy source, which can be used massively for CO2 to fuel processes [3]. As stated before, nuclear hydrogen cogeneration by means of nuclear water splitting of iodine sulfur cycle is the most developed technology of high temperature nuclear reactor application. This technology is interesting from the point of hydrogen and thermal energy output from the system. Hydrogen will be used as important feedstocks of petrochemical, while thermal energy from HTGR (in the form of heat, steam or electricity) is absolutely

94 Prosiding Seminar Nasional Teknologi Energi Nuklir 2016 ISSN: 2355-7524 Batam, 4-5 Agustus 2016 needed to run the process. As nuclear hydrogen cogeneration do not utilize carbon source as raw material, the system need CO2 source from the other system. Fossil power plant, cement industries, or the other industry that emit CO2 in a huge quantity can be used as CO2 source. By utilizing technology of CCS and or CCU, CO2can be captured and separated from the other gases, and use them as material of carbon source for petrochemical. Some studies indicated the important of nuclear hydrogen cogeneration as the key technology for CO2 conversion in the future. Study in US, indicated the role of nuclear hydrogen cogeneration in conversion CO2 emission from cement plant to produce synthetic fuel [29]. The other similar studies also have been doing in around the world such as nuclear hydrogen cogeneration for CO2 conversion to: ammonia and urea production [7, 17], methanol [18, 30], synthetic fuels [3, 9, 29, and 31].

In principle, the technology of high temperature nuclear reactors applications, CO2 conversion, and cogeneration aims to reduce the rate of CO2 emissions. If all three of these technologies are combined in one system, it is expected to become the key technology to support sustainable development. As an illustration, previous studies on nuclear hydrogen cogeneration to convert CO2 into urea indicate that [7]: HTGR of 2x600 MW thermal power can be converted into process heat for hydrogen production, process steam and electricity for low temperature chemical processes (less than 400oC). Urea production, with a capacity of 1725 tons per day, requiring 596357 tons of CO2 per year can be supplied from the coal power plant with a capacity of 90 MWe. Utilization of HTGR as heat sources can save natural gas amounted to 21.25 million MMBTU per year, which is equivalent to a decrease in the rate of CO2 emissions by 1.24 million tons per year. In addition, the system still generates electricity to be connected to a grid of 230 MWe (140 MWe from HTGR and 90 MWe from coal power plant), with a total potential emissions savings of 1.84 million tons per year.

CONCLUSSION Study on role of nuclear hydrogen cogeneration for CO2 conversion in petrochemical industry is already performed. From the study, it can be understood that the nuclear hydrogen cogeneration technology has the ability of providing hydrogen in large quantities as a petrochemical raw materials, and supplying process heat for the processes. From this it can be concluded that in the future this technology can be relied upon as a key technology replaces the conventional technology based on fossil fuel of natural gas. This replacement of conventional technology with nuclear hydrogen cogeneration system, capable of suppressing the rate of depletion of fossil fuel natural gas that has implications for the reduction of CO2 emission rate significantly.

ACKNOWLEDGMENT The author appreciate to Center for Nuclear Energy System Assessment for the financing support through in-house budget of 2015. Special thanks to Dr. Syaiful Bakhri who have been willing to read and correct to improve this paper

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