Ever since humans have existed, they have impacted the earth in many different ways (Redman, 1999). Currently, important impacts are associated with the excessive use of non-renewable fossil fuels such as coal, oil and natural gas. Most fossil fuels are used for electricity generation, heating and mobility (eia, 2011), and as feedstock in the chemical industry (IEA et al., 2013). Moreover, the use of fossil fuels is associated with carbon dioxide emissions (CO2) (IEA, 2014; Leimk¨uhler, 2010). Emitting CO2 into the atmosphere leads to global warming and disrupts the natural carbon cycle (Stocker et al., 2013). To close the disrupted carbon cycle, CO2 can be captured and re-utilized, thereby mitigating global warming and saving fossil resources (Styring et al., 2014).CO2 can be captured from current anthropogenic CO2 sources or directly from the atmosphere. Captured CO2 can then be utilized as valuable physical product “as such”or as alternative carbon feedstock for fuels, chemicals and materials. The general concept of CO2 Capture and Utilization (CCU) can be considered established: already today, CO2 is captured and utilized in processes in the chemical industry (Aresta et al., 2014). However, the scope of CO2 utilization is limited. Despite the existing industrial implementations as well as continuous progress and current efforts in CCU research, most CCU technologies are still in early stages of development. Besides the limited technological readiness, CCU is intrinsically challenging since both capture and utilization of CCU typically require substantial amounts of energy (Sakakura et al., 2007). If the provision of energy relies on fossil resources, indirect CO2 emissions are caused. Therefore, the intuitively expected environmental benefits from using CO2 are not given by default (Peters et al., 2011b). In fact, it cannot be ruled out that a tediously accomplished CCU process is finally environmentally less sustainable than a conventional fossil-based route. Therefore, it is desirable to know whether a specific CCU process is environmentally favorable. For this purpose, a reliable environmental assessment of CCU is required.As indicators for the environmental performance of CCU, a large variety of approaches are proposed ranging from qualitative design principles (Anastas andWarner, 1998) and metrics for ‘green’ chemistry (Constable et al., 2002) to CCU-specific ad-hoc criteria (Peters et al., 2011b; M¨uller and Arlt, 2014). These approaches are rather intended to guide the development towards ‘sustainable’ CCU processes than to systematically quantify the actual environmental impacts. In contrast to these approaches, Life-Cycle Assessment (LCA) is a systematic and standardized methodology to analyze the actual environmental impacts of products and processes (ISO 14040, 2009). Although LCA is frequently advocated for the environmental assessment of CCU (Aresta and Dibenedetto, 2007b; Peters et al., 2011b; Quadrelli et al., 2011), it is not yet standard practice (Sch¨affner et al., 2014). The reasons for this are the complexity of LCA as well as the limited data availability of many CCU processes at early design stages (Quadrelli et al., 2011). In this context, this thesis pursues two major goals: First, the thesis enables and supports the reliable environmental assessment for CCU processes using LCA. To overcome the complexity of LCA and to enable LCA novices to apply LCA to CCU, a jargon-free introduction is presented for LCA in the context of CCU. Furthermore, a framework for LCA of CCU is derived to avoid severe pitfalls in LCA of CCU. A case study for CO2-based polymers illustrates the application of LCA as well as the size and origin of environmental benefits of CCU. The second goal of this thesis is to provide an LCA-based approach to support the design of environmentally beneficial CCU processes at early stages. In summary, the thesis is intended to facilitate the utilization of LCA for CCU from early design stages to industrial implementation.

Ever since humans have existed, they have impacted the earth in many different ways (Redman, 1999). Currently, important impacts are associated with the excessive use of non-renewable fossil fuels such as coal, oil and natural gas. Most fossil fuels are used for electricity generation, heating and mobility (eia, 2011), and as feedstock in the chemical industry (IEA et al., 2013). Moreover, the use of fossil fuels is associated with carbon dioxide emissions (CO2) (IEA, 2014; Leimk¨uhler, 2010). Emitting CO2 into the atmosphere leads to global warming and disrupts the natural carbon cycle (Stocker et al., 2013). To close the disrupted carbon cycle, CO2 can be captured and re-utilized, thereby mitigating global warming and saving fossil resources (Styring et al., 2014).CO2 can be captured from current anthropogenic CO2 sources or directly from the atmosphere. Captured CO2 can then be utilized as valuable physical product “as such”or as alternative carbon feedstock for fuels, chemicals and materials. The general concept of CO2 Capture and Utilization (CCU) can be considered established: already today, CO2 is captured and utilized in processes in the chemical industry (Aresta et al., 2014). However, the scope of CO2 utilization is limited. Despite the existing industrial implementations as well as continuous progress and current efforts in CCU research, most CCU technologies are still in early stages of development. Besides the limited technological readiness, CCU is intrinsically challenging since both capture and utilization of CCU typically require substantial amounts of energy (Sakakura et al., 2007). If the provision of energy relies on fossil resources, indirect CO2 emissions are caused. Therefore, the intuitively expected environmental benefits from using CO2 are not given by default (Peters et al., 2011b). In fact, it cannot be ruled out that a tediously accomplished CCU process is finally environmentally less sustainable than a conventional fossil-based route. Therefore, it is desirable to know whether a specific CCU process is environmentally favorable. For this purpose, a reliable environmental assessment of CCU is required.As indicators for the environmental performance of CCU, a large variety of approaches are proposed ranging from qualitative design principles (Anastas andWarner, 1998) and metrics for ‘green’ chemistry (Constable et al., 2002) to CCU-specific ad-hoc criteria (Peters et al., 2011b; M¨uller and Arlt, 2014). These approaches are rather intended to guide the development towards ‘sustainable’ CCU processes than to systematically quantify the actual environmental impacts. In contrast to these approaches, Life-Cycle Assessment (LCA) is a systematic and standardized methodology to analyze the actual environmental impacts of products and processes (ISO 14040, 2009). Although LCA is frequently advocated for the environmental assessment of CCU (Aresta and Dibenedetto, 2007b; Peters et al., 2011b; Quadrelli et al., 2011), it is not yet standard practice (Sch¨affner et al., 2014). The reasons for this are the complexity of LCA as well as the limited data availability of many CCU processes at early design stages (Quadrelli et al., 2011). In this context, this thesis pursues two major goals: First, the thesis enables and supports the reliable environmental assessment for CCU processes using LCA. To overcome the complexity of LCA and to enable LCA novices to apply LCA to CCU, a jargon-free introduction is presented for LCA in the context of CCU. Furthermore, a framework for LCA of CCU is derived to avoid severe pitfalls in LCA of CCU. A case study for CO2-based polymers illustrates the application of LCA as well as the size and origin of environmental benefits of CCU. The second goal of this thesis is to provide an LCA-based approach to support the design of environmentally beneficial CCU processes at early stages. In summary, the thesis is intended to facilitate the utilization of LCA for CCU from early design stages to industrial implementation.

Ever since humans have existed, they have impacted the earth in many different ways (Redman, 1999). Currently, important impacts are associated with the excessive use of non-renewable fossil fuels such as coal, oil and natural gas. Most fossil fuels are used for electricity generation, heating and mobility (eia, 2011), and as feedstock in the chemical industry (IEA et al., 2013). Moreover, the use of fossil fuels is associated with carbon dioxide emissions (CO2) (IEA, 2014; Leimk¨uhler, 2010). Emitting CO2 into the atmosphere leads to global warming and disrupts the natural carbon cycle (Stocker et al., 2013). To close the disrupted carbon cycle, CO2 can be captured and re-utilized, thereby mitigating global warming and saving fossil resources (Styring et al., 2014).CO2 can be captured from current anthropogenic CO2 sources or directly from the atmosphere. Captured CO2 can then be utilized as valuable physical product “as such”or as alternative carbon feedstock for fuels, chemicals and materials. The general concept of CO2 Capture and Utilization (CCU) can be considered established: already today, CO2 is captured and utilized in processes in the chemical industry (Aresta et al., 2014). However, the scope of CO2 utilization is limited. Despite the existing industrial implementations as well as continuous progress and current efforts in CCU research, most CCU technologies are still in early stages of development. Besides the limited technological readiness, CCU is intrinsically challenging since both capture and utilization of CCU typically require substantial amounts of energy (Sakakura et al., 2007). If the provision of energy relies on fossil resources, indirect CO2 emissions are caused. Therefore, the intuitively expected environmental benefits from using CO2 are not given by default (Peters et al., 2011b). In fact, it cannot be ruled out that a tediously accomplished CCU process is finally environmentally less sustainable than a conventional fossil-based route. Therefore, it is desirable to know whether a specific CCU process is environmentally favorable. For this purpose, a reliable environmental assessment of CCU is required.As indicators for the environmental performance of CCU, a large variety of approaches are proposed ranging from qualitative design principles (Anastas andWarner, 1998) and metrics for ‘green’ chemistry (Constable et al., 2002) to CCU-specific ad-hoc criteria (Peters et al., 2011b; M¨uller and Arlt, 2014). These approaches are rather intended to guide the development towards ‘sustainable’ CCU processes than to systematically quantify the actual environmental impacts. In contrast to these approaches, Life-Cycle Assessment (LCA) is a systematic and standardized methodology to analyze the actual environmental impacts of products and processes (ISO 14040, 2009). Although LCA is frequently advocated for the environmental assessment of CCU (Aresta and Dibenedetto, 2007b; Peters et al., 2011b; Quadrelli et al., 2011), it is not yet standard practice (Sch¨affner et al., 2014). The reasons for this are the complexity of LCA as well as the limited data availability of many CCU processes at early design stages (Quadrelli et al., 2011). In this context, this thesis pursues two major goals: First, the thesis enables and supports the reliable environmental assessment for CCU processes using LCA. To overcome the complexity of LCA and to enable LCA novices to apply LCA to CCU, a jargon-free introduction is presented for LCA in the context of CCU. Furthermore, a framework for LCA of CCU is derived to avoid severe pitfalls in LCA of CCU. A case study for CO2-based polymers illustrates the application of LCA as well as the size and origin of environmental benefits of CCU. The second goal of this thesis is to provide an LCA-based approach to support the design of environmentally beneficial CCU processes at early stages. In summary, the thesis is intended to facilitate the utilization of LCA for CCU from early design stages to industrial implementation.