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homogeneous, and heterogeneous catalysis [4]. With the pressing need for defossilization of power generation and the chemical value chain, homogeneous catalysis will play a major role in re-defining the energy-chemistry nexus [5]. 6.2 State of the art and scientific challenges Most current technologies using homogeneous catalysts are centralized processes that use fossil- derived feedstocks (oil, natural gas, and coal), generally via CO as an intermediate. In fact, among the many transformations that organometallic catalysts enable in the petrochemical value chain, carbonylation reactions, i.e. the introduction of carbon monoxide (CO), are the most prominent. This reaction class comprises bulk chemical production of acetic acid (5 Mt/y), production of large volume commodities (hydroformylation or oxo-process, 10 Mt/y), as well as pharmaceutical products (e.g. anti-inflammatory agents such as ibuprofen and naproxen). To achieve defossilization of the chemical industry, these current industrial processes must be adapted or overhauled to consume renewable energy and feedstocks, e.g. CO2 with green H2 or CO derived from the co-electrolysis of CO2 and water. This “harvest” of fossil-free electricity with renewable feedstocks to produce chemical products is referred to as Power-to-X. Recently, molecular catalysts have demonstrated great success in this area, catalyzing the direct transfor- mation of simple raw materials, such as CO2, N2, H2O, and H2, to chemicals currently produced from energy-intensive, multistep petrochemical processes (Figure 6.1). They include the first ex- amples of reductive functionalization of CO2 to methylamines (featuring a N-CH3 linkage) and other organic molecules used as solvents, reagents and agrochemicals [6, 7]. Furthermore, some of these transformations were conducted under ambient pressure and low temperature (<100 ◦C), thanks to the high reactivity and unprecedented kinetic control of homogeneous catalysts [8]. The potential of homogeneous catalysts to open novel reaction pathways is perhaps best illustrated in considering the direct conversion of CO2 to formaldehyde. While reduction of CO2 to formaldehyde using heterogeneous catalysts currently requires CO2 hydrogenation to methanol and subsequent oxidation at >250 ◦C, it has been shown that it can be achieved directly from CO2/H2 mixtures using organometallic catalysts [9, 10]. Research efforts to fully explore the potential of homoge- neous catalysts and to integrate them in realistic settings are thus highly desirable to validate the economic viability of such strategies. On the atomic scale, the performance of homogeneous catalysts is determined by embedding the metal center in a defined organic molecule, the so-called ligand, allowing for systematic variation of the electronic structure and geometric architecture of the active species and providing a unique methodological basis for rational catalyst design and optimization. This modularity has proven extremely powerful in the petrochemical industry, and it should be exploited in the context of new energy inputs, feedstocks, and building blocks. Already, this emerging strategy has led to significant 61PDF Image | sustainable production of fuels and chemicals
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