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by Ni/Fe-containing carbon monoxide dehydrogenase [4]. Furthermore, responsive protein matrices have evolved over billions of years to optimize essential energy conversion processes, such as energy and electron transfers by porphyrin-type cofactors in photosynthetic conversion and respiration. 7.2.1 Bioinspired catalytic systems The metallocofactor active sites of enzymes provide researchers with key chemistry lessons regarding chemical conversion under ambient conditions. However, such metal active sites generally do not work alone. Biology has carefully engineered responsive protein matrices to control metallocofactor properties, subtly enhancing substrate reactivity by tuning matrix dynamics and energy barriers. Electron and proton delivery pathways are tuned to couple catalytic processes to the energetic constraints imposed by the environment. The clear role of protein matrices in biological systems contrasts sharply with the standard chemists’ approach: here, the chemical properties of cofactors are tuned, while modification of the matrix is largely ignored. In recent years, the research com- munity has made great progress in the understanding of metalloenzyme mechanisms, but many important research questions remain unanswered. In particular, the atomic level functioning of many biological systems is not deeply understood, nor is it known how to apply these insights in the context of hierarchical biological and engineered architectures. Rationally designed catalysts could be used in isolation or as modules in artificial photosynthesis of type (i). 7.2.2 Bioengineered and biohybrid systems Photosynthetic microorganisms can be opti- mized by metabolic engineering and trans- formed into microbial cell factories to produce highly diverse compounds from abundant chem- ical starting materials, such as H2O, CO2, N2, and O2, and sunlight (Figure 7.1A). Technolo- gies employing certain photosynthetic microor- ganisms, such as algae and cyanobacteria, are already quite developed. Several industrial pro- cesses exist, such as Ecoduna, Algaenergy, Al- gosource in Europe and Euglena Co. Ltd. in Japan. These explicit biological systems have been engineered to host novel synthetic pro- duction pathways and enzymes. While most of the available prototypes still have low solar- to-chemicals conversion efficiencies and will re- Figure 7.1: Comparison of type (ii) (Genetically engineered photosynthetic microbial cell factories, panel A) and type (iii) (biohybrid systems, panel B) artificial photosynthesis. Both in- volve microbes and are optimized to produce target chemicals in bioreactors. The inorganic photosensitizer stage in (B) is a com- plex photoelectrochemical nanostructure matching time, length and energy scales to overcome recombination losses in the four- electron water oxidation process (figure courtesy of P. Kallio, Turku Synthetic Biology team). 70PDF Image | sustainable production of fuels and chemicals
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