Generation of efficient
light-induced charge separation inside
the photocatalyst is an essential factor for a high catalytic efficiency.
The usual immobilization of metal or metal oxide particles on semiconductor
photocatalysts offers an uncontrolled assembly of active sites during
the reaction. The introduction of single metal atoms on photocatalysts
can lead to extremely high atomic utilization and precise active sites.
However, this approach is limited because of the lack of suitable
photosensitizers for single atom immobilization. Here, we have designed
photocatalytic carbon quantum dots with anchoring sites for single
cobalt atoms in a defined Co–N4 structure via facile
pyrolysis of vitamin B12. Carbon dots functioned as both light-harvesting
antenna and support for the cobalt atom with high atom loadings up
to 3.27 wt %. This new photocatalytic material demonstrated enhanced
visible light absorption, efficient charge separation, and reduced
electrochemical impedance, while single Co atoms acted as the active
site with strong oxidative ability. As a result, the photocatalysts
showed excellent visible light-promoted photocatalytic efficiency
with oxygen evolution rates up to 168 μmol h–1 g–1 via water oxidation, imine formation with
high conversion (∼90%) and selectivity (>99%), and complete
photodegradation of organic dyes.
A highly
efficient approach to C(sp3)–C(sp3) bond
construction via on-DNA photoredox catalysis between
on-DNA alkenes and N-aryl tertiary amines was developed.
The methodology demonstrated 55%–95% conversions without obvious
DNA damage, as seen by qPCR tests. Furthermore, various functional
groups, such as carboxylic acids, aldehydes, and aryl halides, that
can be used to create library diversities were shown to be tolerant
of the C–H activation conditions.
We report the first example of photo-induced carbocation-enhanced charge transport in triphenylmethane junctions using the scanning tunneling microscopy break junction (STM-BJ) technique.
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