Mechanoenzymology: State of the Art and Challenges towards Highly Sustainable Biocatalysis

Abstract

Global awareness of the importance of developing environmentally friendlier and more sustainable methods for the synthesis of valuable chemical compounds has led to the design of novel synthetic strategies, involving bio‐ and organocatalysis as well as the application of novel efficient and ground‐breaking technologies such as present‐day solvent‐free mechanochemistry. In this regard, the evaluation of biocatalytic protocols mediated by the combination of mechanical activation and enzymatic catalysis has recently attracted the attention of the chemical community. Such mechanoenzymatic strategy represents an innovative and promising “green” approach in chemical synthesis that poses nevertheless new paradigms regarding the relative resilience of biomolecules to the mechanochemical stress and to the apparent high energy, at least in so‐called hot‐spots, during the milling process. Herein, relevant comments on the conceptualization of such mechanoenzymatic approach as a sustainable option in chemical synthesis, recent progress in the area, and associated challenges are discussed.

Mechanoenzymatic Reactions Involving Polymeric Substrates or Products

“…While several existing review articles discuss mechanoenzymatic reactions, [31][32][33][34][35] this minireview will focus specifically on those that involve polymeric substrates or products. Polymers are ubiquitous in society and central in a number of trending research areas such as peptide therapeutics, [36] the production of biofuels from lignocellulosic biomass, [37] and tackling the plastic pollution problem.…”

Lipase-Mediated Mechanoenzymatic Synthesis of Sugar Esters in Dissolved Unconventional and Neat Reaction Systems

“… 30 Kinetic resolution by mechanoenzymology was extensively studied as well, for many active pharmaceutical ingredients due to high enantioselectivity. 31 CALB was also applied in further mechanoenzymatic reactions, for example, acylation of primary amines, hydrolysis of amino esters, or ring-opening polymerization of ω-pentadecalactone. 32 Moreover, the use of organic solvents, volatile thus problematic in an eco-friendly context, 33 and extensive heat to reach the activation energy of certain chemical reactions can be reduced by using mechanochemistry.…”

Mechanoenzymatic reactions with whole cell transaminases: shaken, not stirred

“…This resulted in higher yields compared to constant milling and also benefits from decreased energy consumption. 18 In vitro reactions with enzymes typically involve the use of dilute aqueous conditions. Using mechanoenzymatic methods, it is typically possible to use high substrate concentrations, resulting in more facile reaction work-ups and greater efficiencies.…”