TY - JOUR
T1 - A biohybrid strategy for enabling photoredox catalysis with low-energy light
AU - Cesana, Paul T.
AU - Li, Beryl X.
AU - Shepard, Samuel G.
AU - Ting, Stephen I.
AU - Hart, Stephanie M.
AU - Olson, Courtney M.
AU - Martinez Alvarado, Jesus I.
AU - Son, Minjung
AU - Steiman, Talia J.
AU - Castellano, Felix N.
AU - Doyle, Abigail Gutmann
AU - MacMillan, David W.C.
AU - Schlau-Cohen, Gabriela S.
N1 - Funding Information:
This work was supported as part of BioLEC , an Energy Frontier Research Center funded by the U.S. Department of Energy , Office of Science under award # DE-SC0019370. The authors acknowledge Antonius Koller of the Koch Institute for Integrative Cancer Research at MIT for the intact MS measurements.
Funding Information:
This work was supported as part of BioLEC, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science under award # DE-SC0019370. The authors acknowledge Antonius Koller of the Koch Institute for Integrative Cancer Research at MIT for the intact MS measurements. Conceptualization: P.T.C. B.X.L. C.M.O. M.S. T.J.S. F.N.C. A.G.D. D.W.C.M. and G.S.S-C.; resources: P.T.C. C.M.O. S.M.H. M.S. and T.J.S.; investigation: P.T.C. S.M.H. S.G.S. B.X.L. S.I.T. and J.I.M.A.; writing?original draft: P.T.C. B.X.L. and G.S.S-C.; writing?review and editing: P.T.C. B.X.L. S.I.T. S.G.S. J.I.M.A. F.N.C. A.G.D. D.W.C.M. and G.S.S-C.; funding acquisition: F.N.C. A.G.D. D.W.C.M. and G.S.S-C.; supervision: F.N.C. A.G.D. D.W.C.M. and G.S.S-C. The authors declare no competing interests.
Publisher Copyright:
© 2021 Elsevier Inc.
PY - 2022/1/13
Y1 - 2022/1/13
N2 - Natural systems drive the high-energy reactions of photosynthesis with efficient and broadband energy capture. Transition-metal photocatalysts similarly convert light into chemical reactivity, and yet suffer from light-limited operation and require blue-to-UV excitation. In photosynthesis, both light capture and reactivity have been optimized by separation into distinct sites. Inspired by this modular architecture, we synthesized a biohybrid photocatalyst by covalent attachment of the photosynthetic light-harvesting protein R-phycoerythrin (RPE) to the transition-metal photocatalyst tris(2,2′-bipyridine)ruthenium(II) ([Ru(bpy)3]2+). Spectroscopic investigation found that absorbed photoenergy was efficiently funneled from RPE to [Ru(bpy)3]2+. The utility of the biohybrid photocatalyst was demonstrated via an increase in yields for a thiol-ene coupling reaction and a cysteinyl-desulfurization reaction, including recovered reactivity at red wavelengths where [Ru(bpy)3]2+ alone does not absorb.
AB - Natural systems drive the high-energy reactions of photosynthesis with efficient and broadband energy capture. Transition-metal photocatalysts similarly convert light into chemical reactivity, and yet suffer from light-limited operation and require blue-to-UV excitation. In photosynthesis, both light capture and reactivity have been optimized by separation into distinct sites. Inspired by this modular architecture, we synthesized a biohybrid photocatalyst by covalent attachment of the photosynthetic light-harvesting protein R-phycoerythrin (RPE) to the transition-metal photocatalyst tris(2,2′-bipyridine)ruthenium(II) ([Ru(bpy)3]2+). Spectroscopic investigation found that absorbed photoenergy was efficiently funneled from RPE to [Ru(bpy)3]2+. The utility of the biohybrid photocatalyst was demonstrated via an increase in yields for a thiol-ene coupling reaction and a cysteinyl-desulfurization reaction, including recovered reactivity at red wavelengths where [Ru(bpy)3]2+ alone does not absorb.
KW - SDG12: Responsible consumption and production
KW - SDG7: Affordable and clean energy
KW - biohybrid
KW - energy transfer
KW - photoredox catalysis
KW - photosynthetic light harvesting
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U2 - 10.1016/j.chempr.2021.10.010
DO - 10.1016/j.chempr.2021.10.010
M3 - Article
AN - SCOPUS:85122634134
SN - 2451-9308
VL - 8
SP - 174
EP - 185
JO - Chem
JF - Chem
IS - 1
ER -