Colloidal Synthesis of Carbon Dot-ZnSe Nanoplatelet Van der Waals Heterostructures for Boosting Photocatalytic Generation of Methanol-Storable Hydrogen.
Dechao ChenRohan J HudsonCheng TangQiang SunJeffery R HarmerMiaomiao LiuMehri GhasemiXiaomin WenZixuan LiuWei PengXuecheng YanBruce CowieYongsheng GaoColin L RastonAijun DuTrevor A SmithQin LiPublished in: Small (Weinheim an der Bergstrasse, Germany) (2024)
Methanol is not only a promising liquid hydrogen carrier but also an important feedstock chemical for chemical synthesis. Catalyst design is vital for enabling the reactions to occur under ambient conditions. This study reports a new class of van der Waals heterojunction photocatalyst, which is synthesized by hot-injection method, whereby carbon dots (CDs) are grown in situ on ZnSe nanoplatelets (NPLs), i.e., metal chalcogenide quantum wells. The resultant organic-inorganic hybrid nanoparticles, CD-NPLs, are able to perform methanol dehydrogenation through CH splitting. The heterostructure has enabled light-induced charge transfer from the CDs into the NPLs occurring on a sub-nanosecond timescale, with charges remaining separated across the CD-NPLs heterostructure for longer than 500 ns. This resulted in significantly heightened H 2 production rate of 107 µmole·g -1 ·h -1 and enhanced photocurrent density up to 34 µA cm -2 at 1 V bias potential. EPR and NMR analyses confirmed the occurrence of α-CH splitting and CC coupling. The novel CD-based organic-inorganic semiconductor heterojunction is poised to enable the discovery of a host of new nano-hybrid photocatalysts with full tunability in the band structure, charge transfer, and divergent surface chemistry for guiding photoredox pathways and accelerating reaction rates.
Keyphrases
- visible light
- quantum dots
- room temperature
- water soluble
- carbon dioxide
- nk cells
- magnetic resonance
- air pollution
- small molecule
- high resolution
- ionic liquid
- emergency department
- molecular dynamics
- high throughput
- energy transfer
- human health
- mass spectrometry
- dengue virus
- plant growth
- aedes aegypti
- oxide nanoparticles