Influence of coordination number and ionic radius on metal ion preference and activity of lanthanide-dependent alcohol dehydrogenase: Insights from mutational studies and density functional theory

IF 5.4 2区医学 Q1 BIOPHYSICS

Colloids and Surfaces B: Biointerfaces Pub Date : 2025-02-25 DOI:10.1016/j.colsurfb.2025.114596

Lun Wang , Ke Liu , Zhongdi Song , Hainam Do , Lirong Yang , Jianping Wu , Ling Jiang , Haoran Yu

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引用次数: 0

Abstract

Lanthanide (Ln) elements form a cofactor complex with pyrroloquinoline quinone (PQQ) in bacterial alcohol dehydrogenases (Ln^3 +-ADH). The lanthanide elements did not support Ln³⁺-ADH activity equally, with only early lanthanides (La³⁺-Gd³⁺) promoting high enzyme activity. However, the early lanthanides did not promote the activity equally and the detailed mechanism of Ln³⁺-ADH exhibiting different activity in the presence of different light Lns remains obscure. To uncover the role of lanthanides in promoting Ln³⁺-ADH activity, we systemically characterized the activity of an Ln³⁺-ADH from Pseudomonas putida KT2440 (PedH) in the presence of various Ln³⁺ ions. In the results, enzyme activity displayed a bell-shaped trend along with the lanthanide series, with Nd³⁺ providing the highest activity. Active site mutation analysis revealed that modifying the number of coordinating ligands shifted the metal preference of the enzyme. DFT calculation revealed that the HOMO-LUMO gap, substrate interaction energy and metal ions binding distances were critical for the lanthanides in promoting enzyme activity. This work shed light on the critical role of metal ions in Ln³⁺-ADH catalysis, providing insights for future exploration and engineering of Ln-dependent proteins.

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来源期刊

Colloids and Surfaces B: Biointerfaces 生物-材料科学：生物材料

CiteScore

11.10

自引率

3.40%

发文量

730

审稿时长

42 days

期刊介绍： Colloids and Surfaces B: Biointerfaces is an international journal devoted to fundamental and applied research on colloid and interfacial phenomena in relation to systems of biological origin, having particular relevance to the medical, pharmaceutical, biotechnological, food and cosmetic fields. Submissions that: (1) deal solely with biological phenomena and do not describe the physico-chemical or colloid-chemical background and/or mechanism of the phenomena, and (2) deal solely with colloid/interfacial phenomena and do not have appropriate biological content or relevance, are outside the scope of the journal and will not be considered for publication. The journal publishes regular research papers, reviews, short communications and invited perspective articles, called BioInterface Perspectives. The BioInterface Perspective provide researchers the opportunity to review their own work, as well as provide insight into the work of others that inspired and influenced the author. Regular articles should have a maximum total length of 6,000 words. In addition, a (combined) maximum of 8 normal-sized figures and/or tables is allowed (so for instance 3 tables and 5 figures). For multiple-panel figures each set of two panels equates to one figure. Short communications should not exceed half of the above. It is required to give on the article cover page a short statistical summary of the article listing the total number of words and tables/figures.