Chemical passivation is an effective approach to suppress the grain surface dominated charge recombination in perovskite solar cells (PSCs). However, the passivation effect is usually labile on perovskite crystal surface since most passivating agents are weakly anchored. Here, the use of a bidentate molecule, 2‐mercaptopyridine (2‐MP), to increase anchoring strength for improving the passivation efficacy and stability synchronously is demonstrated. Compared to monodentate counterparts of pyridine and p‐toluenethiol, 2‐MP passivation on CH3NH3PbI3 film results in twofold improvement of photoluminescence lifetime and remarkably enhanced tolerance to chlorobenzene washing and vacuum heating, which improve the power conversion efficiency of n–i–p planar structured PSCs from 18.35% to 20.28%, with open‐circuit voltage approaching 1.18 V. Moreover, the CH3NH3PbI3 films passivated with 2‐MP exhibit unprecedented humid‐stability that they can be exposed to saturated humidity for at least 5 h, mainly due to the passivation induced surface deactivation, which renders the unencapsulated devices retaining 93% of the initial efficiency after 60 days aging in air with relative humidity of 60–70%.
High-fidelity
mapping of amyloid-β (Aβ) plaques is
critical for the early detection of Alzheimer’s disease. However,
in vivo probing of Aβ plaques by commercially available thioflavin
derivatives (ThT or ThS) has proven to be extremely limited, as evident
by the restriction of enrichment quenching effect, low signal-to-noise
(S/N) ratio, and poor blood–brain
barrier (BBB) penetrability. Herein, we demonstrate a rational design
strategy of near-infrared (NIR) aggregation-induced emission (AIE)-active
probes for Aβ plaques, through introducing a lipophilic π-conjugated
thiophene-bridge for extension to NIR wavelength range with enhancement
of BBB penetrability, and tuning the substituted position of the sulfonate
group for guaranteeing specific hydrophilicity to maintain the fluorescence-off state before binding to Aβ deposition. Probe QM-FN-SO3 has settled well the AIE dilemma between the lipophilic requirement
for longer emission and aggregation behavior from water to protein
fibrillogenesis, thus making a breakthrough in high-fidelity feedback
on in vivo detection of Aβ plaques with remarkable binding affinity,
and serving as an efficient alternative to the commercial probe ThT
or ThS.
Particle-stabilized W/O/W emulsion gels were fabricated using a two-step procedure: ( i) a W/O emulsion was formed containing saccharose (for osmotic stress balance) and gelatin (as a gelling agent) in the aqueous phase and polyglycerol polyricinoleate (a lipophilic surfactant) in the oil phase; ( ii) this W/O emulsion was then homogenized with another water phase (W) containing wheat gliadin nanoparticles (hydrophilic emulsifier). The gliadin nanoparticles in the external aqueous phase aggregated at pH 5.5, which led to the formation of particle-stabilized W/O/W emulsion gels with good stability to phase separation. These emulsion gels were then used to coencapsulate a hydrophilic bioactive (epigallocatechin-3-gallate, EGCG) in the internal aqueous phase (encapsulation efficiency = 65.5%) and a hydrophobic bioactive (quercetin) in the oil phase (encapsulation efficiency = 97.2%). The emulsion gels improved EGCG chemical stability and quercetin solubility under simulated gastrointestinal conditions, which led to a 2- and 4-fold increase in their effective bioaccessibility, respectively.
Development of fluorescent probes for on-site sensing and long-term tracking of specific biomarkers is particularly desirable for the early detection of diseases. However, available small-molecule probes tend to facilely diffuse across the cell membrane or remain at the activation site but always suffer from the aggregation-caused quenching (ACQ) effect. Here we report an enzyme-activatable aggregationinduced emission (AIE) probe QM-bgal, which is composed of a hydrophilic b-galactosidase (b-gal)triggered galactose moiety and a hydrophobic AIE-active fluorophore QM-OH. The probe is virtually non-emissive in aqueous media, but when activated by b-gal, specific enzymatic turnover would liberate hydrophobic AIE luminogen (AIEgen) QM-OH, and then highly fluorescent nanoaggregates are in situ generated as a result of the AIE process, allowing for on-site sensing of endogenous b-gal activity in living cells. Notably, taking advantage of the improved intracellular retention of nanoaggregates, we further exemplify QM-bgal for long-term ($12 h) visualization of b-gal-overexpressing ovarian cancer cells with high fidelity, which is essential for biomedicine and diagnostics. Thus, this enzyme-activatable AIE probe not only is a potent tool for elucidating the roles of b-gal in biological systems, but also offers an enzyme-regulated liberation strategy to exploit multifunctional probes for preclinical applications.Scheme 1 Schematic illustration of an enzyme-regulated liberation strategy for on-site sensing and long-term tracking.Scheme 2 Enzyme-activatable probes for b-gal activity sensing.This journal is
In vivo fluorescent monitoring of physiological processes with high‐fidelity is essential in disease diagnosis and biological research, but faces extreme challenges due to aggregation‐caused quenching (ACQ) and short‐wavelength fluorescence. The development of high‐performance and long‐wavelength aggregation‐induced emission (AIE) fluorophores is in high demand for precise optical bioimaging. The chromophore quinoline‐malononitrile (QM) has recently emerged as a new class of AIE building block that possesses several notable features, such as red to near‐infrared (NIR) emission, high brightness, marked photostability, and good biocompatibility. In this minireview, we summarize some recent advances of our established AIE building block of QM, focusing on the AIE mechanism, regulation of emission wavelength and morphology, the facile scale‐up and fast preparation for AIE nanoparticles, as well as potential biomedical imaging applications.
Chemiluminescence (CL)-based technologies have revolutionized in vivo monitoring of biomolecules.H owever, significant technical hurdles have limited the achievement of trigger-controlled, bright, and enriched CL signal. Herein, ad ual-lock strategy uses sequence-dependent triggers for bright optical imaging with real-time fluorescent signal and ultra-sensitive CL signal. These probes can obtain an analytetriggered accumulation of stable pre-chemiluminophore with aggregation-induced emission (AIE), and then the pre-chemiluminophore exhibits ar apid photooxidation process (1,2dioxetane generation) by TICT-based free-radical addition, therebya chieving an enrichment and bright CL signal. The dual-locks trategy expands the in vivo toolbox for highly accurate analysis and has for the first time allowed access to accurately sense and trace biomolecules with high-resolution, dual-mode of chemo-fluoro-luminescence,a nd three-dimensional (3D) imaging in living animals.
The strategy of molecularly precise self-assembly of theranostic nanoprobes within a single-molecular framework is used to avoid batch-to-batch variability, and concurrently achieving real-time tracking of the in vivo behaviour of prodrugs for the first time.
Fluorescence-based technologies have revolutionized in vivo monitoring of biomolecules. However, significant technical hurdles in both probe chemistry and complex cellular environments have limited the accuracy of quantifying these biomolecules. Herein, we report a generalizable engineering strategy for dual-emission anti-Kasha-active fluorophores, which combine an integrated fluorescein with chromene (IFC) building block with donor-π-acceptor structural modification. These fluorophores exhibit an invariant near-infrared Kasha emission from the S 1 state, while their anti-Kasha emission from the S 2 state at around 520 nm can be finely regulated via a spirolactone open/closed switch. We introduce bio-recognition moieties to IFC structures, and demonstrate ratiometric quantification of cysteine and glutathione in living cells and animals, using the ratio (S 2 /S 1) with the S 1 emission as a reliable internal reference signal. This de novo strategy of tuning anti-Kasha-active properties expands the in vivo ratiometric quantification toolbox for highly accurate analysis in both basic life science research and clinical applications.
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