دورية أكاديمية
A photoactive semisynthetic metalloenzyme exhibits complete selectivity for CO 2 reduction in water.
العنوان: | A photoactive semisynthetic metalloenzyme exhibits complete selectivity for CO |
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المؤلفون: | Schneider CR; Ohio State Biochemistry Program, The Ohio State University, Columbus, OH 43210, USA. shafaat.1@osu.edu., Manesis AC, Stevenson MJ, Shafaat HS |
المصدر: | Chemical communications (Cambridge, England) [Chem Commun (Camb)] 2018 May 03; Vol. 54 (37), pp. 4681-4684. |
نوع المنشور: | Journal Article |
اللغة: | English |
بيانات الدورية: | Publisher: Royal Society of Chemistry Country of Publication: England NLM ID: 9610838 Publication Model: Print Cited Medium: Internet ISSN: 1364-548X (Electronic) Linking ISSN: 13597345 NLM ISO Abbreviation: Chem Commun (Camb) Subsets: PubMed not MEDLINE |
أسماء مطبوعة: | Original Publication: Cambridge : Royal Society of Chemistry |
مستخلص: | A series of artificial metalloenzymes containing a ruthenium chromophore and [NiII(cyclam)]2+, both incorporated site-selectively, have been constructed within an azurin protein scaffold. These light-driven, semisynthetic enzymes do not evolve hydrogen, thus displaying complete selectivity for CO2 reduction to CO. Electrostatic effects rather than direct excited-state electron transfer dominate the ruthenium photophysics, suggesting that intramolecular electron transfer from photogenerated RuI to [NiII(cyclam)]2+ represents the first step in catalysis. Stern-Volmer analyses rationalize the observation that ascorbate is the only sacrificial electron donor that supports turnover. Collectively, these results highlight the important interplay of elements that must be considered when developing and characterizing molecular catalysts. |
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معلومات مُعتمدة: | T32 GM008512 United States GM NIGMS NIH HHS |
تواريخ الأحداث: | Date Created: 20180421 Date Completed: 20180507 Latest Revision: 20240324 |
رمز التحديث: | 20240324 |
مُعرف محوري في PubMed: | PMC5934327 |
DOI: | 10.1039/c8cc01297k |
PMID: | 29675518 |
قاعدة البيانات: | MEDLINE |
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