Utilizing full-spectrum sunlight for ammonia decomposition to hydrogen over GaN nanowires-supported Ru nanoparticles on silicon

• Published in: Nature communications Vol. 15; no. 1; pp. 7393 - 11
• Main Authors: Li, Jinglin, Sheng, Bowen, Chen, Yiqing, Yang, Jiajia, Wang, Ping, Li, Yixin, Yu, Tianqi, Pan, Hu, Qiu, Liang, Li, Ying, Song, Jun, Zhu, Lei, Wang, Xinqiang, Huang, Zhen, Zhou, Baowen
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 27-08-2024; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/146; 147/137; 639/638/675; 639/638/77/890; Ammonia; Aqueous solutions; Batch reactors; Current carriers; Decomposition; Decomposition reactions; Density functional theory; Energy charge; Gallium; Gallium nitrides; Humanities and Social Sciences; Hydrogen production; Illumination; multidisciplinary; Nanoparticles; Nanotechnology; Nanowires; Reaction mechanisms; Ruthenium; Science; Science (multidisciplinary); Silicon; Sunlight
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-51810-y

Photo-thermal-coupling ammonia decomposition presents a promising strategy for utilizing the full-spectrum to address the H
2
storage and transportation issues. Herein, we exhibit a photo-thermal-catalytic architecture by assembling gallium nitride nanowires-supported ruthenium nanoparticles on a silicon for extracting hydrogen from ammonia aqueous solution in a batch reactor with only sunlight input. The photoexcited charge carriers make a predomination contribution on H
2
activity with the assistance of the photothermal effect. Upon concentrated light illumination, the architecture significantly reduces the activation energy barrier from 1.08 to 0.22 eV. As a result, a high turnover number of 3,400,750 is reported during 400 h of continuous light illumination, and the H
2
activity per hour  is nearly 1000 times higher than that under the pure thermo-catalytic conditions. The reaction mechanism is extensively studied by coordinating experiments, spectroscopic characterizations, and density functional theory calculation. Outdoor tests validate the viability of such a multifunctional architecture for ammonia decomposition toward H
2
under natural sunlight.
The author report a Ru NPs/GaN NWs nanoarchitecture on Si for utilizing full spectrum to drive efficient and robust photothermal H
2
production from NH
3
with a high turnover number of >3,400,750 over 400 h.