一种依赖铈的光酶

IF 12.9 1区生物学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Nature chemical biology Pub Date : 2024-10-22 DOI:10.1038/s41589-024-01767-2

Majda Bratovič

引用次数: 0

摘要

酶能有效催化多种反应，但要重新设计酶来加速自然界未知的反应却极具挑战性。镧系元素，尤其是铈络合物，以前曾被用于通过自由基进行的光催化转化。然而，这些自由基反应很少具有立体选择性。为了解决这个问题，Klein、Leiss-Maier 等人在计算设计的蛋白质支架中心添加了四个谷氨酸，从而开发出一种镧系元素结合酶。他们将这种酶称为 PhotoLanZyme 1.0（PLZ1.0），它能在氯化铈（III）和可见光的作用下催化 1,2-二醇的 C-C 键自由基裂解。为了提高光稳定性和金属结合动力学，研究小组通过突变镧系元素结合位点附近的色氨酸，并在蛋白质表面引入突变以减少非特异性铈结合，进一步改造了这种光敏酶。最终的变体PLZ1.4能以非对映选择性方式催化裂解多种芳香取代的二元醇，并能裂解芳香木质素模型化合物。研究小组利用 PLZ1.1 与 Lpp-OmpA 序列（以前曾用于人工金属酶的表面展示）的融合构建物，在大肠杆菌中建立了降解木质素模型化合物的全细胞生物催化系统。最后，他们利用假单胞菌 KT2440 的醇脱氢酶 PedH，证明了依赖镧系元素的天然酶在铈光氧化催化中的适用性，该酶需要氧化还原辅助因子吡咯喹啉醌（PQQ）和镧系元素离子进行反应。该酶是在没有 PQQ 的情况下表达和重组的。在氯化铈（III）和光的作用下，PedH 可以催化二元醇裂解。这项研究为设计能催化镧系元素介导的光氧化反应的人工酶开辟了新途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature chemical biology 生物-生化与分子生物学

CiteScore

23.90

自引率

1.40%

发文量

238

审稿时长

12 months

期刊介绍： Nature Chemical Biology stands as an esteemed international monthly journal, offering a prominent platform for the chemical biology community to showcase top-tier original research and commentary. Operating at the crossroads of chemistry, biology, and related disciplines, chemical biology utilizes scientific ideas and approaches to comprehend and manipulate biological systems with molecular precision. The journal embraces contributions from the growing community of chemical biologists, encompassing insights from chemists applying principles and tools to biological inquiries and biologists striving to comprehend and control molecular-level biological processes. We prioritize studies unveiling significant conceptual or practical advancements in areas where chemistry and biology intersect, emphasizing basic research, especially those reporting novel chemical or biological tools and offering profound molecular-level insights into underlying biological mechanisms. Nature Chemical Biology also welcomes manuscripts describing applied molecular studies at the chemistry-biology interface due to the broad utility of chemical biology approaches in manipulating or engineering biological systems. Irrespective of scientific focus, we actively seek submissions that creatively blend chemistry and biology, particularly those providing substantial conceptual or methodological breakthroughs with the potential to open innovative research avenues. The journal maintains a robust and impartial review process, emphasizing thorough chemical and biological characterization.

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