1. Manipulating Photoconduction in Supramolecular Networks for Solar-Driven Nitrate Conversion to Ammonia and Oxygen.
- Author
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Hong F, Su X, Fang Y, He X, and Shan B
- Abstract
For photoelectrodes to be used in practical catalytic applications, challenges exist in achieving the efficient production and transport of photogenerated charge-separated states. Analogous concepts in traditional inorganic photoelectrodes can be applied to their organic-polymer counterparts with improved charge-separation efficiencies. In this work, we develop photoconductive organic networks to form a high-performance photoelectrode for NO
3 - reduction to NH3 . In the integrated network, interfaces between the organic electron-donating photoconductor and electron-accepting catalyst can generate charge carriers efficiently upon illumination, leading to enhanced charge separation for photoelectrocatalysis. The photoelectrode network is capable of converting NO3 - to NH3 at an external quantum efficiency of 13%. By coupling with a BiVO4 photoanode in tandem, the system reduces NO3 - to NH3 and oxidizes H2 O to O2 simultaneously at Faradaic efficiencies of 95-98% with sustained photocurrents and production yields. Investigation of the photoconductive network by steady-state/time-resolved spectroscopies reveals the efficient generation and transport of free charge carriers in the photoelectrode, providing a basis for high photoelectrocatalytic performances.- Published
- 2024
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