Photoelectrochemical Reduction of Carbon Dioxide to Methanol through a Highly Efficient Enzyme Cascade

Kuk, Su Keun; Singh, Raushan Kumar; Nam, Dong Heon; Singh, Ranjitha; Lee, Jung-Kul; Park, Chan Beum

doi:10.1002/anie.201611379

Cited by 253 publications

(172 citation statements)

References 68 publications

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“…Combining the realms of photo-/electrocatalysis with biocatalysis, two benchmark contributions in the field for the reduction of CO 2 to methanol were reported by Ji et al 44 and Kuk et al 53 . Both systems combined three dehydrogenases in a cascade reaction to achieve methanol formation.…”

Section: Review Articlementioning

confidence: 99%

“…Compared with a solution-based system, the methanol yield increased substantially from 35 to > 90% by creation of this nanofibre-microcapsule reaction concept. Alternatively, Kuk et al 53 developed a system where photoanodes and -cathodes were linked to an NADH regeneration cycle with a formate dehydrogenase, a formaldehyde dehydrogenase and an alcohol dehydrogenase for this bioreduction cascade (Fig. 4).…”

Section: Review Articlementioning

confidence: 99%

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Opportunities and challenges for combining chemo- and biocatalysis

et al. 2018

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N ature has evolved highly efficient systems in the form of cascade reactions, which assemble the metabolic networks that support life (growth and survival). The basic principle of cascade reactions is also frequently used in biocatalysis, using enzymes in isolation, as well as in combination with chemocatalysts (see Fig. 1 and Box 1 for definition of terms) [1][2][3][4][5][6][7] . As there is no need for purification and isolation of intermediates, operating time, production costs and waste are reduced, and concomitantly, overall yields are improved. In addition, the problem of unstable or difficult to handle intermediates can be overcome, and reactivity as well as selectivity can be enhanced by avoiding unfavourable reaction equilibria through the cooperative effects of multiple catalysts 8 . Starting in the 1980s, the early examples of the combination of chemo-and biocatalysts were reported by the van Bekkum group, who pioneered the development of a process to make the sugar substitute d-mannitol from readily available d-glucose through the combination of a heterogeneous metal-catalysed hydrogenation and an enzyme-catalysed isomerization 9 . The first broadly applied technology for the combination of enzyme and metalcatalysts, which was the research subject of many academic groups as well as industry, emerged in the 1990s from the Williams group 10,11 and aimed to achieve higher yields than classical kinetic resolution of racemates, thus overcoming the limitation of a maximum yield of 50% in the latter case. A prominent example of work that developed this theme is the combination of lipase-catalysed kinetic resolution via acylation of secondary alcohols with Pd-or Rh-catalysed racemization via reversible transfer hydrogenation to achieve a dynamic kinetic resolution (DKR) [12][13][14] . This example was facilitated in part because lipases are active and stable in organic solvents. Later, for instance, Turner's group combined a monoamine oxidase-catalysed imine formation with a chemical reduction 15 to achieve the 100% theoretical yield through a deracemization process. In addition to the combination of metalcatalysis with enzymes, organocatalysis, electrochemistry and light-induced reaction couples have since then been studied extensively, going far beyond the scope of a DKR.The challenges to combining chemo-and biocatalysis in cascades (see Box 1 for definitions and Table 1) can be daunting, not least the requirement for the chemical step to occur in the presence of water, the preferred solvent for enzymes 3 . This Review therefore highlights recent examples of the combination of chemo-and biocatalysts in aqueous multistep syntheses, and looks at how to overcome limitations by, for example, design of appropriate reaction conditions, protein engineering and advanced reactor concepts. Furthermore, trends such as the integration of transition metalcatalysis into microorganisms and the introduction of novel chemistry into engineered enzymes are discussed, and a critical assessment of the impact of this research ...

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Section: Review Articlementioning

confidence: 99%

Section: Review Articlementioning

confidence: 99%

Opportunities and challenges for combining chemo- and biocatalysis

et al. 2018

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“…However, an expensive nicotinamide cofactor (NADH) is generally required to achieve catalytic turnover in such a biocatalytic process, and the regeneration of NADH usually limits the entire reaction. To solve this problem, Park et al [165] designed an integrated enzyme-cascade (TPIEC) system using a Rh complex and three dehydrogenase (i.e., FDH, formaldehyde dehydrogenase (FaldDH), and alcohol dehydrogenase (ADH)), as depicted in Fig. 14b.…”

Section: Enzymatic Biocatalystsmentioning

confidence: 99%

Section: Figure 14mentioning

confidence: 99%

“…Although the reaction pathways and intermediates are still controversial, the Cu-based catalysts hold the promise for future development. The other candidate is enzymatic biocatalysts [162,165]. The enzymatic biocatalysts typically show high selectivity for products without side reactions; however, high cost and poor stability hinder their further practical application, which should be emphatically considered.…”

Section: Summary and Perspectivesmentioning

confidence: 99%

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Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

et al. 2018

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The energy crisis and global warming become severe issues. Solar-driven CO 2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical (PEC) process, which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO 2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO 2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO 2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO 2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway. Furthermore, diversiform novel PEC setups are also outlined. These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO 2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.

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