A bound iron porphyrin is redox active in hybrid bacterial reaction centers modified to possess a four-helix bundle domain
A bound iron porphyrin is redox active in hybrid bacterial reaction centers modified to possess a four-helix bundle domain
复制标题
结合的铁卟啉在修饰为具有四螺旋束结构域的杂合细菌反应中心中具有氧化还原活性
DOI：
10.1007/s43630-021-00142-7
复制
发表时间：
2022
影响因子：
3.1
通讯作者：
Williams, J. C.
中科院分区：
文献类型：
--
作者：
Allen, J. P.;Chamberlain, K. D.;Olson, T. L.;Williams, J. C.
本文报道了一种新型氧化还原活性辅助因子杂化反应中心的设计。反应中心执行光合作用的初级光化学，即光诱导电子从细菌叶绿素二聚体转移到一系列电子受体。杂化配合物是由人工的四螺旋束与反应中心的m亚基融合而成的。尽管进行了较大的修饰，但光谱显示纯化后的杂化反应中心聚集成活性配合物，保留了特征辅因子吸收峰，并且能够光诱导电荷分离。四螺旋束可以结合铁原卟啉在还原和氧化状态。铁原卟啉结合到杂化反应中心后，光激发产生一个新的导数信号，其最大波长为402 nm，最小波长为429 nm。这种信号的振幅随着光照持续时间的延长而增加，并在黑暗中持续存在。当铁原卟啉加入到没有四螺旋束结构域的反应中心时，或者当不氧化还原的锌原卟啉结合时，没有观察到信号。结果与新的氧化还原反应产生的信号一致，即电子从铁原卟啉转移到氧化的细菌叶绿素二聚体。这些结果证明了将卟啉结合到杂化反应中心以获得新的光驱动功能的可行性。图形抽象
In this paper we report the design of hybrid reaction centers with a novel redox-active cofactor. Reaction centers perform the primary photochemistry of photosynthesis, namely the light-induced transfer of an electron from the bacteriochlorophyll dimer to a series of electron acceptors. Hybrid complexes were created by the fusion of an artificial four-helix bundle to the M-subunit of the reaction center. Despite the large modification, optical spectra show that the purified hybrid reaction centers assemble as active complexes that retain the characteristic cofactor absorption peaks and are capable of light-induced charge separation. The four-helix bundle could bind iron-protoporphyrin in either a reduced and oxidized state. After binding iron-protoporphyrin to the hybrid reaction centers, light excitation results in a new derivative signal with a maximum at 402 nm and minimum at 429 nm. This signal increases in amplitude with longer light durations and persists in the dark. No signal is observed when iron-protoporphyrin is added to reaction centers without the four-helix bundle domain or when a redox-inactive zinc-protoporphyrin is bound. The results are consistent with the signal arising from a new redox reaction, electron transfer from the iron-protoporphyrin to the oxidized bacteriochlorophyll dimer. These outcomes demonstrate the feasibility of binding porphyrins to the hybrid reaction centers to gain new light-driven functions.Graphical abstract
登录
查看更多内容
影响因子：
2.3
作者：
Chino, Marco;Maglio, Ornella;Nastri, Flavia;Pavone, Vincenzo;DeGrado, William F.;Lombardi, Angela
通讯作者：
Lombardi, Angela
DOI：
10.1016/j.bbabio.2015.09.008
发表时间：
2016-05
期刊：
Biochimica et biophysica acta
影响因子：
--
作者：
Fry BA;Solomon LA;Leslie Dutton P;Moser CC
通讯作者：
Moser CC
影响因子：
5.6
作者：
Calhoun, JR;Kono, H;Saven, JG
通讯作者：
Saven, JG
影响因子：
18.9
作者：
Joann C. Williams;James P. Allen
通讯作者：
James P. Allen
能够还原球形红细菌修饰反应中心的细菌叶绿素二聚体的结合锰氧化物
影响因子：
3.7
作者：
E. Espiritu, K. Chamberlain
通讯作者：
E. Espiritu, K. Chamberlain