Light‐driven catalysis with engineered enzymes and biomimetic systems

Abstract

Efforts to drive catalytic reactions with light, inspired by natural processes like photosynthesis, have a long history and have seen significant recent growth. Successfully engineering systems using biomolecular and bioinspired catalysts to carry out light‐driven chemical reactions capitalizes on advantages offered from the fields of biocatalysis and photocatalysis. In particular, driving reactions under mild conditions and in water, in which enzymes are operative, using sunlight as a renewable energy source yield environmentally friendly systems. Furthermore, using enzymes and bioinspired systems can take advantage of the high efficiency and specificity of biocatalysts. There are many challenges to overcome to fully capitalize on the potential of light‐driven biocatalysis. In this mini‐review, we discuss examples of enzymes and engineered biomolecular catalysts that are activated via electron transfer from a photosensitizer in a photocatalytic system. We place an emphasis on selected forefront chemical reactions of high interest, including CH oxidation, proton reduction, water oxidation, CO2 reduction, and N2 reduction.

A biohybrid strategy for enabling photoredox catalysis with low-energy light

“…33 Nanoparticles or small molecules were covalently attached to enzymes, and electron transfer between them has been demonstrated. [34][35][36][37][38][39][40][41][42][43] However, the stringent distance dependence requirements and nonspecific reactivity of electron transfer create additional synthetic and operational challenges. [44][45][46][47] Energy transfer, which occurs over longer distances, was introduced by conjugating together transition-metal photocatalysts with different excitation energies, which expanded their absorption window.…”

Accelerated Reaction Engineering of Photo(bio)catalytic Reactions through Parallelization with an Open‐Source Photoreactor

“…Placed at the intersection of photochemistry and biocatalysis, the topic of photobiocatalysis gained interest in the synthetic community in the recent years [1–4] . Photobiocatalysis has the potential of combining the synthetic advantages of biocatalytic transformations, such as their high degree of selectivity and their sustainable nature, [5–7] with the promise of novel reactivities that may be unlocked by using photons as reagents.…”

Light-Driven CO2 Reduction by Co-Cytochrome b562

“…One possible path is through artificial photosynthesis, where light is utilized as the energy source to drive production of carbon-free or carbon-neutral fuels, mirroring the role of the enzyme RuBisCO in fixing CO 2 . In that vein, promising approaches interfacing photosensitizers and/or materials with molecular catalysts, enzymes, and microorganisms have been developed (Woo, 2017;Luan and Lu, 2018;Edwards and Bren, 2020;Ma et al, 2020).…”