Development
of special organic materials that are able to absorb
light energy in the second near-infrared window (NIR-II) is significantly
important for treating deep-tissue-buried diseases or supplying power
to implantable electronic devices. Herein, a narrow bandgap donor–acceptor
(D-A) conjugated polymer with thiophene-fused benzodifurandione-based
oligo(p-phenylenevinylene) (TBDOPV) as acceptor part and 2,2′-bithiophene
(DT) as donor part was developed and exploited as a photothermal conversion
material with high extinction coefficient and robust photostability
in the NIR-II window. According to transient absorption analysis results,
the photothermal conversion ability of this polymer is attributed
to the fast internal conversion (IC) process. The high photothermal
conversion efficiency makes this polymer a promising NIR-II adsorbing
antenna to remotely actuate thermo-dependent devices, e.g., high-performance
photothermal–electrical and photothermal–mechanical
converters.
Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Pt nanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of ∼65 ps, 5.0 mL of assembled CdSe/CdS QDs/cocatalysts solution produces 94 ± 1.5 mL (4183 ± 67 μmol) of molecular H in 8 h, giving rise to an internal quantum yield of ∼65% in the first 30 min and a total turnover number of >1.64 × 10 per Pt nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of the interparticle ET process, which is the key step for advanced H photosynthesis.
The installation of heterojunctions on the surfaces of carbon nanotubes (CNTs) is an effective method for promoting the charge separation processes needed for CNT-based electronics and optoelectronics applications. Conjugated polymers are proven state-of-the-art candidates for modifying the surfaces of CNTs. However, all previous attempts to incorporate conjugated polymers to CNTs resulted in unordered interfaces. Herein we show that well-defined chains of regioregular poly(3-hexylthiophene) (P3HT) were successfully grown from the surfaces of multiwalled CNTs (MWNTs) using surface-initiated Kumada catalyst-transfer polycondensation. The polymerization was found to proceed in a controlled manner as chains of tunable lengths were prepared through variation of the initial monomer-to-initiator ratio. Moreover, it was determined that large-diameter MWNTs afforded highly ordered P3HT aggregates, which exhibited a markedly bathochromically shifted optical absorption due to a high grafting density induced planarization of the polymer chains. Using ultrafast spectroscopy, the heterojunctions formed between the MWNTs and P3HT were shown to effectively overcome the binding energy of excitons, leading to photoinduced electron transfer from P3HT to MWNTs. Finally, when used as prototype devices, the individual MWNT-g-P3HT core-shell structures exhibited excellent photoresponses under a low illumination density.
The light absorber, protecting layer, and active site have been integrated into an ultra-small nanocrystal through a site-and spatial-selective cation exchange reaction. Owing to the excellent electronic communication between CdSe and catalytic active sites, the protection of the ZnS shell, and the spatial delocalization of electron-hole pairs, the well-designed multifunctional CdSe/Zn 1Àx Fe x S QDs exhibit highly efficient and ultra-stable performance toward photocatalytic H 2 evolution.
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