Martínez-Moñino Ana Belén, Zapata-Pérez Rubén, García-Saura Antonio Ginés, Gil-Ortiz Fernando, Pérez-Gilabert Manuela, Sánchez-Ferrer Álvaro
Department of Biochemistry and Molecular Biology-A, Faculty of Biology, Regional Campus of International Excellence "Campus Mare Nostrum", University of Murcia, Campus Espinardo, E-30100 MURCIA, Spain.
Murcia Biomedical Research Institute (IMIB), Murcia, Spain.
PLoS One. 2017 Apr 7;12(4):e0174759. doi: 10.1371/journal.pone.0174759. eCollection 2017.
NAD+ has emerged as a crucial element in both bioenergetic and signaling pathways since it acts as a key regulator of cellular and organismal homeostasis. Among the enzymes involved in its recycling, nicotinamide mononucleotide (NMN) deamidase is one of the key players in the bacterial pyridine nucleotide cycle, where it catalyzes the conversion of NMN into nicotinic acid mononucleotide (NaMN), which is later converted to NAD+ in the Preiss-Handler pathway. The biochemical characteristics of bacterial NMN deamidases have been poorly studied, although they have been investigated in some firmicutes, gamma-proteobacteria and actinobacteria. In this study, we present the first characterization of an NMN deamidase from an alphaproteobacterium, Agrobacterium tumefaciens (AtCinA). The enzyme was active over a broad pH range, with an optimum at pH 7.5. Moreover, the enzyme was quite stable at neutral pH, maintaining 55% of its activity after 14 days. Surprisingly, AtCinA showed the highest optimal (80°C) and melting (85°C) temperatures described for an NMN deamidase. The above described characteristics, together with its high catalytic efficiency, make AtCinA a promising biocatalyst for the production of pure NaMN. In addition, six mutants (C32A, S48A, Y58F, Y58A, T105A and R145A) were designed to study their involvement in substrate binding, and two (S31A and K63A) to determine their contribution to the catalysis. However, only four mutants (C32A, S48A Y58F and T105A) showed activity, although with reduced catalytic efficiency. These results, combined with a thermal and structural analysis, reinforce the Ser/Lys catalytic dyad mechanism as the most plausible among those proposed.
烟酰胺腺嘌呤二核苷酸(NAD+)已成为生物能量和信号通路中的关键元素,因为它是细胞和机体稳态的关键调节因子。在参与其循环利用的酶中,烟酰胺单核苷酸(NMN)脱酰胺酶是细菌吡啶核苷酸循环的关键参与者之一,它催化NMN转化为烟酸单核苷酸(NaMN),随后在普赖斯-汉德勒途径中转化为NAD+。尽管已经在一些厚壁菌门、γ-变形菌门和放线菌门中对细菌NMN脱酰胺酶进行了研究,但对其生化特性的研究仍很少。在本研究中,我们首次对来自α-变形菌门的根癌土壤杆菌(AtCinA)的NMN脱酰胺酶进行了表征。该酶在较宽的pH范围内具有活性,最适pH为7.5。此外,该酶在中性pH下相当稳定,14天后仍保持其活性的55%。令人惊讶的是,AtCinA显示出报道的NMN脱酰胺酶中最高的最适温度(80°C)和熔点温度(85°C)。上述特性,连同其高催化效率,使AtCinA成为生产纯NaMN的有前途的生物催化剂。此外,设计了六个突变体(C32A、S48A、Y58F、Y58A、T105A和R145A)来研究它们在底物结合中的作用,以及两个突变体(S31A和K63A)来确定它们对催化的贡献。然而,只有四个突变体(C32A、S48A、Y58F和T105A)显示出活性,尽管催化效率有所降低。这些结果,结合热分析和结构分析,强化了丝氨酸/赖氨酸催化二元机制是所提出的机制中最合理的这一观点。