期刊
SCIENCE
卷 352, 期 6284, 页码 448-450出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aaf2091
关键词
-
资金
- Laboratory Directed Research and Development Program seed project
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences
- U.S. Department of Energy [DE-AC36-08-GO28308]
- National Renewable Energy Laboratory
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0010334]
- U.S. Department of Energy, Office of Science [DE-SC0012518]
- U.S. Department of Energy (DOE) [DE-SC0012518, DE-SC0010334] Funding Source: U.S. Department of Energy (DOE)
The splitting of dinitrogen (N-2) and reduction to ammonia (NH3) is a kinetically complex and energetically challenging multistep reaction. In the Haber-Bosch process, N-2 reduction is accomplished at high temperature and pressure, whereas N-2 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 N-2 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 N-2 reduction. The CdS: MoFe protein biohybrids provide a photochemical model for achieving light-driven N-2 reduction to NH3.
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