Photothermal and Photochemical Nanostructured Catalyst Engineering Towards Efficient Solar Fuel Production
Author | : Jia Jia |
Publisher | : |
Total Pages | : |
Release | : 2017 |
ISBN-10 | : OCLC:1333980814 |
ISBN-13 | : |
Rating | : 4/5 (14 Downloads) |
Download or read book Photothermal and Photochemical Nanostructured Catalyst Engineering Towards Efficient Solar Fuel Production written by Jia Jia and published by . This book was released on 2017 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: With global energy demand rising alongside the advancement of climate change, the conversion of greenhouse gas carbon dioxide into value-added chemicals and fuels is attracting increasing attention. The crux for the successful development of this promising technology is the exploration and discovery of highly active, selective, and stable catalyst materials. Herein we demonstrate that the reverse water gas shift (RWGS) reaction can be driven by Nb2O5 nanorod-supported Pd nanocrystals, without external heating, using visible and near infrared (NIR) light. By measuring the dependence of the RWGS reaction rates on the intensity and spectral power distribution of filtered light incident on the nanostructured Pd@Nb2O5 catalyst, we determine the RWGS reaction to be initiated by heat generated from thermalized charge carriers in the Pd nanocrystals that are excited by inter-band and intra-band absorption of visible and NIR light. We also demonstrate that the catalytic activity and selectivity of CO2 reduction to CO and CH4 products can be systematically tailored, by varying the size of the Pd nanocrystals, to acheive champion turnover frequencies (0.61 sâ 1) and efficient conversion of solar energy to stored chemical energy. The remarkable control over the catalytic performance of Pd@Nb2O5 stems from a combination of photothermal, electronic, and size effects. The insight gleaned from this detailed experimental-theoretical study provides a blueprint for how to tailor the performance metrics of earth-abundant, low-cost metal-metal oxide (M@M'Ox) analogues. Finally, we report a lattice strain and defect controlled strategy that enables the high-performance of low-cost photocatalystic materials. Lattice compressed ultrafine nonstoichiometric indium oxide dots, In2O3-x(OH)y, grown on the surface of niobium pentoxide nanorods were fabricated; the optimized hybrid structure exhibits 44-fold increase in efficiency compared with pristine In2O3-x(OH)y, along with extremely long-term operational stability, potentially originating from the increased number of active oxygen vacancies, prolonged excited-state lifetimes, and enhanced photo-generated carrier energies.