ATP-uncoupled, six-electron photoreduction of hydrogen cyanide to methane by the molybdenum-iron protein

Journal of the American Chemical Society
Lauren E Roth, F Akif Tezcan

Abstract

A detailed study of the eight-electron/eight-proton catalytic reaction of nitrogenase has been hampered by the fact that electron and proton flow in this system is controlled by ATP-dependent protein-protein interactions. Recent studies have shown that it is possible to circumvent the dependence on ATP through the use of potent small-molecule reductants or light-driven electron injection, but success has been limited to two-electron reductions of hydrazine, acetylene, or protons. Here we show that a variant of the molybdenum-iron protein labeled with a Ru-photosensitizer can support the light-driven, six-electron catalytic reduction of hydrogen cyanide into methane and likely also ammonia. Our findings suggest that the efficiency of this light-driven system is limited by the initial one- or two-electron reduction of the catalytic cofactor (FeMoco) to enable substrate binding, but the subsequent electron-transfer steps into the FeMoco-bound substrate proceed efficiently.

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Citations

Jan 29, 2014·Journal of Inorganic Biochemistry·Sudharsan DwaraknathLionel Cheruzel
Nov 28, 2013·Chemical Reviews·Jay R Winkler, Harry B Gray
Sep 18, 2013·Journal of the American Chemical Society·Ngoc-Han TranLionel E Cheruzel
Sep 12, 2015·Journal of the American Chemical Society·Cedric P OwensF Akif Tezcan
Dec 9, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Daniel SippelOliver Einsle
Nov 26, 2015·Chemical Communications : Chem Comm·Yousoon LeeLeslie J Murray
Jun 27, 2020·Biotechnology and Applied Biochemistry·Emily H Edwards, Kara L Bren
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Jul 19, 2019·Photosynthesis Research·Dandan ZhengJiangyun Wang
Jan 31, 2020·Chemical Reviews·Hannah L Rutledge, F Akif Tezcan
Apr 3, 2020·Chemical Reviews·Casey Van StappenSerena DeBeer
May 28, 2020·Chemical Reviews·Kazuki Tanifuji, Yasuhiro Ohki
Jun 17, 2020·Chemical Reviews·Oliver Einsle, Douglas C Rees
Jul 30, 2021·Biotechnology Advances·Nan YangHao Song
May 31, 2019·Journal of the American Chemical Society·Hannah L RutledgeF Akif Tezcan
Jan 29, 2014·Chemical Reviews·Brian M HoffmanLance C Seefeldt
Dec 19, 2014·Journal of the American Chemical Society·F Akif TezcanDouglas C Rees
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Apr 2, 2015·Biochemistry·Karamatullah DanyalLance C Seefeldt

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