A Nanoconfined Four-Enzyme Cascade Simultaneously Driven by Electrical and Chemical Energy, with Built-in Rapid, Confocal Recycling of NADP(H) and ATP.
A Nanoconfined Four-Enzyme Cascade Simultaneously Driven by Electrical and Chemical Energy, with Built-in Rapid, Confocal Recycling of NADP(H) and ATP.
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DOI：
10.1021/acscatal.2c00999
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发表时间：
2022-08-05
期刊：
影响因子：
12.9
通讯作者：
Armstrong, Fraser A.
中科院分区：
文献类型：
--
作者：
Megarity, Clare F.;Weald, Thomas R. I.;Heath, Rachel S.;Turner, Nicholas J.;Armstrong, Fraser A.
关键词：
羧酸还原酶 (CAR) 的实验证明了通电纳米限制对于促进具有多个可交换辅因子的酶级联的研究和执行的重要性，CAR 是一种在单个催化循环中需要 NADPH 和 ATP 的酶。通过同时传递电能和化学能来驱动和监测将四种酶装入并捕获在氧化铟锡 (ITO) 电极的随机纳米孔中，将肉桂酸转化为肉桂醛。电能由铁氧还蛋白 NADP+ 还原酶转换，该还原酶与 ITO 进行快速、直接的电子交换并再生 NADP(H)。磷酸烯醇丙酮酸（一种包含在本体溶液中的燃料）提供的化学能由腺苷酸激酶和丙酮酸激酶共同转导，有效地将 AMP 产物转化回下一个循环所需的 ATP。使用双激酶系统可以剖析回收过程，以评估在稳态前和稳态催化过程中 AMP 去除和 ATP 供应的单独作用。
The importance of energized nanoconfinement for facilitating the study and execution of enzyme cascades that feature multiple exchangeable cofactors is demonstrated by experiments with carboxylic acid reductase (CAR), an enzyme that requires both NADPH and ATP during a single catalytic cycle. Conversion of cinnamic acid to cinnamaldehyde by a package of four enzymes loaded into and trapped in the random nanopores of an indium tin oxide (ITO) electrode is driven and monitored through the simultaneous delivery of electrical and chemical energy. The electrical energy is transduced by ferredoxin NADP+ reductase, which undergoes rapid, direct electron exchange with ITO and regenerates NADP(H). The chemical energy provided by phosphoenolpyruvate, a fuel contained in the bulk solution, is cotransduced by adenylate kinase and pyruvate kinase, which efficiently convert the AMP product back into ATP that is required for the next cycle. The use of the two-kinase system allows the recycling process to be dissected to evaluate the separate roles of AMP removal and ATP supply during presteady-state and steady-state catalysis.
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DOI：
10.1021/acs.jpclett.1c01517
发表时间：
2021-07-08
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Herold RA;Reinbold R;Megarity CF;Abboud MI;Schofield CJ;Armstrong FA
通讯作者：
Armstrong FA
影响因子：
4.1
作者：
Gahloth, Deepankar;Aleku, Godwin A.;Leys, David
通讯作者：
Leys, David
影响因子：
3.5
作者：
Banin, U.;Waiskopf, N.;Brudvig, G. W.
通讯作者：
Brudvig, G. W.
影响因子：
16.6
作者：
Kim, Yang Hee;Campbell, Elliot;Banta, Scott
通讯作者：
Banta, Scott
影响因子：
16.6
作者：
Elani, Yuval;Law, Robert V.;Ces, Oscar
通讯作者：
Ces, Oscar