期刊
NANO LETTERS
卷 22, 期 6, 页码 2236-2243出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c04220
关键词
artificial photosynthesis; surface polarity; nanowire; photoelectrode; GaN
类别
资金
- HydroGEN Advanced Water Splitting Materials Consortium, Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office [DE-EE0008086]
- U.S. Army Research Office Award [W911NF2110337]
- U.S. Department of Energy [DE-AC52-07NA27344]
- National Science Foundation Graduate Research Fellowship [1841052]
- U.S. Department of Defense (DOD) [W911NF2110337] Funding Source: U.S. Department of Defense (DOD)
- Division Of Graduate Education
- Direct For Education and Human Resources [1841052] Funding Source: National Science Foundation
Tuning the surface structure of gallium nitride (GaN) photoelectrodes is an effective approach to address challenges in artificial photosynthesis. Nonpolar surfaces of GaN exhibit significant photoelectrochemical activity, while polar c-plane surfaces show little to no activity. Density functional theory calculations provide insight into the atomic origin of this difference.
Tuning the surface structure of the photoelectrode provides one of the most effective ways to address the critical challenges in artificial photosynthesis, such as efficiency, stability, and product selectivity, for which gallium nitride (GaN) nanowires have shown great promise. In the GaN wurtzite crystal structure, polar, semipolar, and nonpolar planes coexist and exhibit very different structural, electronic, and chemical properties. Here, through a comprehensive study of the photoelectrochemical performance of GaN photocathodes in the form of films and nanowires with controlled surface polarities we show that significant photoelectrochemical activity can be observed when the nonpolar surfaces are exposed in the electrolyte, whereas little or no activity is measured from the GaN polar c-plane surfaces. The atomic origin of this fundamental difference is further revealed through density functional theory calculations. This study provides guideline on crystal facet engineering of metal-nitride photo(electro)catalysts for a broad range of artificial photosynthesis chemical reactions.
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