Panchromatic ternary polymer dots
(Pdots) consisting of two conjugated
polymers (PFBT and PFODTBT) based on fluorene and benzothiadiazole
groups, and one small molecular acceptor (ITIC) have been prepared
and assessed for photocatalytic hydrogen production with the assistance
of a Pt cocatalyst. Femtosecond transient absorption spectroscopic
studies of the ternary Pdots have revealed both energy and charge
transfer processes that occur on the time scale of sub-picosecond
between the different components. They result in photogenerated electrons
being located mainly at ITIC, which acts as both electron and energy
acceptor. Results from cryo-transmission electron microscopy suggest
that ITIC forms crystalline phases in the ternary Pdots, facilitating
electron transfer from ITIC to the Pt cocatalyst and promoting the
final photocatalytic reaction yield. Enhanced light absorption, efficient
charge separation, and the ideal morphology of the ternary Pdots have
rendered an external quantum efficiency up to 7% at 600 nm. Moreover,
the system has shown a high stability over 120 h without obvious degradation
of the photocatalysts.
A small organic molecule
2,1,3-benzothiadiazole-4, 7-dicarbonitrile
(BTDN) is assessed for electrocatalytic hydrogen evolution on glassy
carbon electrode and shows a hydrogen production Faradaic efficiency
of 82% in the presence of salicylic acid. The key catalytic intermediates
of reduced species BTDN
–•
and protonated
intermediates are characterized or hypothesized by using various spectroscopic
methods and density functional theory (DFT)-based calculations. With
the experimental and theoretical results, a catalytic mechanism of
BTDN for electrocatalytic H
2
evolution is proposed.
This review provides the guidelines and knowledge gained so far on current strategies used to prepare, optimize and investigate polymer nanoparticles for fuel production, highlighting the future directions of polymer nano-photocatalyst development.
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