Non-photochromic solar energy storage in carbon nitride surpassing blue radicals for hydrogen production

Potassium poly(heptazine imide) (KPHI) exhibiting the dual functionality of photon absorption and photoelectron storage for solar energy conversion is a new class of ionic two-dimensional (2D) carbon nitrides. Rather than forming blue radicals upon storing photoelectrons in the yellow crystalline KP...

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Published inJournal of materials chemistry. A, Materials for energy and sustainability Vol. 10; no. 14; pp. 7728 - 7738
Main Authors Wu, Pei-Shan, Lin, Tzu-Jen, Hou, Sheng-Shu, Chen, Chih-Chia, Tsai, Dai-Ling, Huang, Kuan-Hsiang, Wu, Jih-Jen
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 05.04.2022
Subjects
Carbon
Carbon nitride
Crystal structure
Crystallinity
Density functional theory
Energy conversion
Energy storage
Hydrogen evolution
Hydrogen production
Molecular structure
Photocatalysis
Photochromism
Photoelectrons
Photon absorption
Potassium
Radicals
Solar energy
Solar energy conversion
Storage capacity
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Summary:Potassium poly(heptazine imide) (KPHI) exhibiting the dual functionality of photon absorption and photoelectron storage for solar energy conversion is a new class of ionic two-dimensional (2D) carbon nitrides. Rather than forming blue radicals upon storing photoelectrons in the yellow crystalline KPHIs, here non-photochromic solar energy storage in the in-plane short-range-ordered KPHI is reported, which demonstrates superior photocatalytic and dark photocatalytic activities for hydrogen evolution. Density functional theory calculations confirm that the electron storage capacity of the short-range-ordered KPHI is higher than that of the crystalline one. Moreover, the molecular structure remains unchanged after electrons are stored, resulting in non-photochromic solar energy storage in short-range-ordered KPHI. In crystalline KPHI, the stored photoelectrons drive the change of potassium ion locations to form a blue radical. This work demonstrates that the photophysical properties of light-storing carbon nitrides are tunable by modifying the microstructure of KPHIs towards efficient solar energy storage and conversion.
ISSN:2050-7488
2050-7496
DOI:10.1039/D1TA10091B