Artificial Metalloproteins with Dinuclear Iron-Hydroxido Centers.
Artificial Metalloproteins with Dinuclear Iron-Hydroxido Centers.
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DOI：
10.1021/jacs.0c12564
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发表时间：
2021-02-10
影响因子：
15
通讯作者：
Borovik AS
中科院分区：
文献类型：
--
作者：
Miller KR;Biswas S;Jasniewski A;Follmer AH;Biswas A;Albert T;Sabuncu S;Bominaar EL;Hendrich MP;Moënne-Loccoz P;Borovik AS
双核铁中心与桥接羟基或氧化配体形成各种金属蛋白内的活性位点。这些位点的一个关键特征是蛋白质控制Fe中心周围结构的能力，这导致对功能至关重要的吸能状态。为了模拟这种受控环境，已经使用生物素-链霉亲和素（Sav）技术对人工蛋白质进行了工程化，其中来自相邻亚基的Fe复合物可以组装形成[Fe III-（μ-OH）-Fe III]核心。通过设计酪氨酸侧链的突变以协调Fe中心，通过Fe络合物在亚基内的位点特异性定位来促进组装过程。一个重要的结果是，Sav宿主可以调节Fe → Fe分离，已知这对天然金属蛋白的功能很重要。从X射线衍射方法的光谱和结构研究显示，不寻常的长Fe Fe分离的变化小于0.3后，额外的桥接配体的结合。由蛋白质宿主对二-Fe核心施加的结构约束是独特的，并且在工程化人工金属蛋白内产生具有吸能状态的活性位点的实例。
Dinuclear iron centers with a bridging hydroxido or oxido ligand form active sites within a variety of metalloproteins. A key feature of these sites is the ability of the protein to control the structures around the Fe centers, which leads to entatic states that are essential for function. To simulate this controlled environment, artificial proteins have been engineered using biotin-streptavidin (Sav) technology in which Fe complexes from adjacent subunits can assemble to form [FeIII-(μ-OH)-FeIII] cores. The assembly process is promoted by the site-specific localization of the Fe complexes within a subunit through the designed mutation of a tyrosinate side chain to coordinate the Fe centers. An important outcome is that the Sav host can regulate the Fe⋯Fe separation, which is known to be important for function in natural metalloproteins. Spectroscopic and structural studies from X-ray diffraction methods revealed uncommonly long Fe⋯Fe separations that change by less than 0.3 Å upon the binding of additional bridging ligands. The structural constraints imposed by the protein host on the di-Fe cores are unique and create examples of active sites having entatic states within engineered artificial metalloproteins.
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高分辨率扩展的X射线吸收精细结构分析为甲烷单加氧酶的Q中间体中较长的Fe···Fe距离提供了证据。
影响因子：
15
作者：
Cutsail GE 3rd;Banerjee R;Zhou A;Que L Jr;Lipscomb JD;DeBeer S
通讯作者：
DeBeer S
影响因子：
2.9
作者：
Calhoun, JR;Nastri, F;DeGrado, WF
通讯作者：
DeGrado, WF
DOI：
10.1073/pnas.86.7.2190
发表时间：
1989-04-01
影响因子：
11.1
作者：
HENDRICKSON, WA;PAHLER, A;PHIZACKERLEY, RP
通讯作者：
PHIZACKERLEY, RP
影响因子：
4.6
作者：
Alam, MA;Nethaji, M;Ray, M
通讯作者：
Ray, M
影响因子：
62.1
作者：
Jasniewski AJ;Que L Jr
通讯作者：
Que L Jr