Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid
Top Cited Papers
- 22 April 2016
- journal article
- other
- Published by American Association for the Advancement of Science (AAAS) in Science
- Vol. 352 (6284), 448-450
- https://doi.org/10.1126/science.aaf2091
Abstract
The splitting of dinitrogen (N2) and reduction to ammonia (NH3) is a kinetically complex and energetically challenging multistep reaction. In the Haber-Bosch process, N2 reduction is accomplished at high temperature and pressure, whereas N2 fixation by the enzyme nitrogenase occurs under ambient conditions using chemical energy from adenosine 5′-triphosphate (ATP) hydrolysis. We show that cadmium sulfide (CdS) nanocrystals can be used to photosensitize the nitrogenase molybdenum-iron (MoFe) protein, where light harvesting replaces ATP hydrolysis to drive the enzymatic reduction of N2 into NH3. The turnover rate was 75 per minute, 63% of the ATP-coupled reaction rate for the nitrogenase complex under optimal conditions. Inhibitors of nitrogenase (i.e., acetylene, carbon monoxide, and dihydrogen) suppressed N2 reduction. The CdS:MoFe protein biohybrids provide a photochemical model for achieving light-driven N2 reduction to NH3.Keywords
Funding Information
- U.S. Department of Energy, Office of Science (DE-SC0012518)
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