Herein, we report for the first time the use of bipyridine-based hydrogel for selective and visible detection and absorption of Cd(2+). At low concentrations, hydrogelator 1 was applied for selective detection of Cd(2+) in vitro and in living cells with high sensitivity. In the absence of metal ions, 1 is nonfluorescent at 470 nm. Upon addition of metal ions, 1 selectively coordinates to Cd(2+), causing an 86-fold increase of fluorescence intensity at 470 nm via the chelation enhanced fluorescence (CHEF) effect, as revealed by first-principles simulations. At 1.5 wt% and pH 5.5, 1 self-assembles into nanofibers to form hydrogel Gel I. Since Cd(2+) could actively participate in the hydrogelation and promote the self-assembly, we also successfully applied Gel I for visible detection and absorption of Cd(2+). With these excellent properties, Gel I is expected to be explored as one type of versatile biomaterial for not only environmental monitoring but also for pollution treatment in the near future.
Achieving high charge recombination probability has been the major challenge for the practical utilization of molecule-based solar harvesting. Molecular switches were introduced to stabilize the charge separation state in donor-acceptor systems, but it is difficult to seamlessly incorporate the ON/OFF switching actions into the optoelectronic conversion cycle. Here we present a self-adaptive system in which the donor and acceptor are bridged by a switchable moiety that enables a complete charge separation repeatedly. Calculations are presented for a platinum(II) terpyridyl complex with an azobenzene bridge. The charge transfer induced by light extracts electrons from the azobenzene group, automatically triggering a trans → cis isomerization. The resulting conformation suppresses charge recombination. Energized charges are trapped in the acceptor, ready for charge collection by electrodes. The bridge then goes through inverse isomerization to restore the conjugation and conductance. This self-adaptive design provides a novel way to improve the performance of optoelectronic conversion and realize practical solar-harvesting applications in organic molecular systems.
A boron radical contact ion-pair MesB{4-(3,5-dimethylpyridinyl)}K(18-crown-6)(THF) (1K) has been isolated and characterized by electron paramagnetic resonance (EPR) spectroscopy, UV-vis absorption spectroscopy and single crystal X-ray diffraction. The geometry, bonding and spin density distribution are shown to be affected by the NK interaction. The unpaired electron resides mainly on the boron atom and falls between those of triarylboron radical anions and neutral boron radicals. The work provides a novel boron-centered radical intermediate, connecting anionic and neutral boryl radicals.
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