期刊
ACS ENERGY LETTERS
卷 2, 期 2, 页码 445-453出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.6b00665
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资金
- National Science Foundation [CHE 1464938]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC-0001234]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1464938] Funding Source: National Science Foundation
The chemical literature often does not differentiate between photocatalytic (PC) and photosynthetic (PS) processes (including artificial photosynthesis) even though these reactions differ in their thermodynamics. Photocatalytic processes are thermodynamically downhill (Delta G < 0) and are merely accelerated by the catalyst, whereas photosynthetic processes are thermodynamically unfavorable (Delta G > 0) and require photochemical energy input to occur. Here we apply this differentiation to analyze the basic functions of PC and PS devices and to formulate design criteria for improved performance. As will be shown, the corresponding devices exhibit distinctly different sensitivities to their functional parameters. For example, under conditions of optimal light absorption, carrier lifetimes, and electrochemical rates, the performance of PCs is limited only by their surface area, while type 1 PS devices are limited by their carrier mobility and mass transport, and type 2 PS devices are limited by electrochemical charge-transfer selectivity. Strategies for the optimization of type 1 and 2 photosynthetic devices and photocatalysts are also discussed.
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