Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen
Study and use of metal-containing biological reagents often involves the need to manipulate the redox level. We report herein the synthesis of a heterogeneous catalyst system that allows the use of Hâ‚‚ as a reductant for the one-electron reduction of horseheart ferricytochrome c (cyt câ‚’â‚“), sper...
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American Chemical Society
1981
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Online Access: | https://doi.org/10.1021/ja00415a045 |
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ftcaltechauth:oai:authors.library.caltech.edu:rtksb-c0z29 2024-06-23T07:56:58+00:00 Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen Bookbinder, Dana C. Lewis, Nathan S. Wrighton, Mark S. 1981-12-16 https://doi.org/10.1021/ja00415a045 unknown American Chemical Society https://doi.org/10.1021/ja00415a045 oai:authors.library.caltech.edu:rtksb-c0z29 eprintid:120840 resolverid:CaltechAUTHORS:20230413-768760000.16 info:eu-repo/semantics/closedAccess Other Journal of the American Chemical Society, 103(25), 7656-7659, (1981-12-16) Colloid and Surface Chemistry Biochemistry General Chemistry Catalysis info:eu-repo/semantics/article 1981 ftcaltechauth https://doi.org/10.1021/ja00415a045 2024-06-12T03:19:13Z Study and use of metal-containing biological reagents often involves the need to manipulate the redox level. We report herein the synthesis of a heterogeneous catalyst system that allows the use of H₂ as a reductant for the one-electron reduction of horseheart ferricytochrome c (cyt cₒₓ), sperm whale myoglobin, and stellacyanin from the lacquer of Rhus vernicifera. Application of the principles illustrated by our catalyst in other systems is possible inasmuch as the reducing power of H₂ is sufficiently great that many biological systems are thermodynamically reducible with H₂. An advantage in using H₂ as a source of reducing power is that the oxidation product is H⺠which is acceptable since most biological systems are studied in buffered media. A heterogeneous catalyst is desirable to facilitate the separation of the catalyst from the product. © 1981 American Chemical Society. N.S.L. acknowledges support as a John and Fannie Hertz Fellow, 1977-1981. D.C.B. acknowledges partial support as an M.I.T. NPW Fellow, 1981. Partial support from the United States Department of Energy, Basic Energy Sciences, Division of Chemical Sciences, is acknowledged. We appreciate the generous assistance of Professor Edward I. Solomon and his research group and the use of their purified stellacyanin. Helpful discussions with Professors William H. Orme-Johnson, Alexander Klibanov, and George M. Whitesides are gratefully acknowledged. Article in Journal/Newspaper Sperm whale Caltech Authors (California Institute of Technology) Journal of the American Chemical Society 103 25 7656 7659 |
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Caltech Authors (California Institute of Technology) |
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topic |
Colloid and Surface Chemistry Biochemistry General Chemistry Catalysis |
spellingShingle |
Colloid and Surface Chemistry Biochemistry General Chemistry Catalysis Bookbinder, Dana C. Lewis, Nathan S. Wrighton, Mark S. Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
topic_facet |
Colloid and Surface Chemistry Biochemistry General Chemistry Catalysis |
description |
Study and use of metal-containing biological reagents often involves the need to manipulate the redox level. We report herein the synthesis of a heterogeneous catalyst system that allows the use of H₂ as a reductant for the one-electron reduction of horseheart ferricytochrome c (cyt cₒₓ), sperm whale myoglobin, and stellacyanin from the lacquer of Rhus vernicifera. Application of the principles illustrated by our catalyst in other systems is possible inasmuch as the reducing power of H₂ is sufficiently great that many biological systems are thermodynamically reducible with H₂. An advantage in using H₂ as a source of reducing power is that the oxidation product is H⺠which is acceptable since most biological systems are studied in buffered media. A heterogeneous catalyst is desirable to facilitate the separation of the catalyst from the product. © 1981 American Chemical Society. N.S.L. acknowledges support as a John and Fannie Hertz Fellow, 1977-1981. D.C.B. acknowledges partial support as an M.I.T. NPW Fellow, 1981. Partial support from the United States Department of Energy, Basic Energy Sciences, Division of Chemical Sciences, is acknowledged. We appreciate the generous assistance of Professor Edward I. Solomon and his research group and the use of their purified stellacyanin. Helpful discussions with Professors William H. Orme-Johnson, Alexander Klibanov, and George M. Whitesides are gratefully acknowledged. |
format |
Article in Journal/Newspaper |
author |
Bookbinder, Dana C. Lewis, Nathan S. Wrighton, Mark S. |
author_facet |
Bookbinder, Dana C. Lewis, Nathan S. Wrighton, Mark S. |
author_sort |
Bookbinder, Dana C. |
title |
Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
title_short |
Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
title_full |
Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
title_fullStr |
Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
title_full_unstemmed |
Heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
title_sort |
heterogeneous one-electron reduction of metal-containing biological molecules using molecular hydrogen as the reductant: synthesis and use of a surface-confined viologen redox mediator that equilibrates with hydrogen |
publisher |
American Chemical Society |
publishDate |
1981 |
url |
https://doi.org/10.1021/ja00415a045 |
genre |
Sperm whale |
genre_facet |
Sperm whale |
op_source |
Journal of the American Chemical Society, 103(25), 7656-7659, (1981-12-16) |
op_relation |
https://doi.org/10.1021/ja00415a045 oai:authors.library.caltech.edu:rtksb-c0z29 eprintid:120840 resolverid:CaltechAUTHORS:20230413-768760000.16 |
op_rights |
info:eu-repo/semantics/closedAccess Other |
op_doi |
https://doi.org/10.1021/ja00415a045 |
container_title |
Journal of the American Chemical Society |
container_volume |
103 |
container_issue |
25 |
container_start_page |
7656 |
op_container_end_page |
7659 |
_version_ |
1802650396576972800 |