Abstract
Coenzyme B12-dependent glycerol dehydratase (GDHt) catalyzes the dehydration reaction of glycerol in the presence of adenosylcobalamin to yield 3-hydroxypropanal (3-HPA), which can be converted biologically to versatile platform chemicals such as 1,3-propanediol and 3-hydroxypropionic acid. Owing to the increased demand for biofuels, developing biological processes based on glycerol, which is a byproduct of biodiesel production, has attracted considerable attention recently. In this review, we will provide updates on the current understanding of the catalytic mechanism and structure of coenzyme B12-dependent GDHt, and then summarize the results of engineering attempts, with perspectives on future directions in its engineering.
Highlights
Glycerol dehydratase are categorized on the basis of their reliance on coenzyme B12 (adenosylcobalamin (AdoCbl): coenzyme B12-independent glycerol dehydratase (GDHt) and coenzyme B12-dependent GDHt (Yamanishi et al, 2002; Liao et al, 2003a; O’Brien et al, 2004)
Coenzyme B12-dependent GDHts are relatively resistant to aerobic conditions (Jiang et al, 2016), and have been utilized for bioconversion of glycerol (Liu et al, 2016)
The dehydration reaction catalyzed by coenzyme B12-dependent GDHt has been reported as the rate-limiting step for the bioconversion of glycerol into 1,3-PD or 3-HP (Ahrens et al, 1998; Yuanyuan et al, 2004)
Summary
Glycerol dehydratase (GDHt; EC 4.2.1.30) catalyzes the dehydration reaction of glycerol yielding 3-hydroxypropanal (3-HPA) that can be biologically converted into 1,3-propanediol (1,3-PD) or 3-hydroxypropionic acid (3-HP) by expressing 1,3-propanediol dehydrogenase or aldehyde dehydrogenase, respectively, in microorganisms (Pawelkiewicz, 1965; Schneider et al, 1970; Stroinski et al, 1974; Toraya, 2000a; Huang et al, 2002; Liu et al, 2016; Park et al, 2017). 1,3-PD is used as a monomer for synthesizing polyethers, polyurethanes, and polyesters (Koutinas et al, 2014; Garlapati et al, 2016; Liu et al, 2016). 3-HP is a versatile platform chemical that can be converted into acrylic acid, acrylonitrile, and malonic acid (Valdehuesa et al, 2013; Chen and Liu, 2016; Kalantari et al, 2017). The crystal structures of the coenzyme B12-dependent GDHt from Klebsiella pneumoniae (KpGDHt) in the presence or absence of a substrate have been reported (Yamanishi et al, 2002; Liao et al, 2003a).
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