Protein trap-engineered metal-organic frameworks for advanced enzyme encapsulation and mimicking

Immobilizing enzymes within metal-organic frameworks(MOFs)enables enzymes to against extreme environments.However,these MOF shells are just like armors,protective but heavy,which shield the enzymes from threats while locking them in the cage.The exploitation of immobilization strategy and intrinsic property of MOFs themselves is of great significance.Here,we proposed a functional protein trap strategy for efficient enzyme encapsulation.The ferrocenedicarboxylic acid(Fc)was used to induce the formation of defect-rich Co-based MOFs(CoBDC-Fc).As result,the engineered protein trap can not only improve the enzyme loading but also accelerate catalytic efficiency.Specifically,the atomically dispersed Fc sites serve as cocatalysts/cofactors and even change the conformation of enzymes in the construed microenvironment.Furthermore,the obtained CoBDC-Fc/enzyme exhibits excellent recyclability and tolerance to inhospitable conditions.Benefited by these,the CoBDC-Fc/enzyme/antigen composites were further prepared for cascade enzyme-linked immunosorbent assay of prostate-specific antigen with satisfactory sensitivity.

Exceptionally efficient deep blue anthracene-based luminogens:design,synthesis,photophysical,and electroluminescent mechanisms

Achieving high-efficiency deep blue emitter with CIE_(y)<0.06(CIE,Commission Internationale de L’Eclairage)and external quantum efficiency(EQE)>10%has been a long-standing challenge for traditional fluorescent materials in organic light-emitting diodes(OLEDs).Here,we report the rational design and synthesis of two new deep blue luminogens:4-(10-(4’-(9 H-carbazol-9-yl)-2,5-dimethyl-[1,1’-biphe nyl]-4-yl)anthracen-9-yl)benzonitrile(2 M-ph-pCzAnBzt)and 4-(10-(4-(9 H-carbazol-9-yl)-2,5-dimethyl phenyl)anthracen-9-yl)benzonitrile(2 M-pCzAnBzt).In particular,2 M-ph-pCzAnBzt produces saturated deep blue emissions in a non-doped electroluminescent device with an exceptionally high EQE of 10.44% and CIE_(x,y)(0.151,0.057).The unprecedented electroluminescent efficiency is attributed to the combined effects of higher-order reversed intersystem crossing and triplet-triplet up-conversion,which are supported by analysis of theoretical calculation,triplet sensitization experiments,as well as nanosecond transient absorption spectroscopy.This research offers a new approach to resolve the shortage of high efficiency deep blue fluorescent emitters.

Modulating Room Temperature Phosphorescence by Oxidation of Thianthrene to Achieve Pure Organic Single-Molecule White-Light Emission

In order to develop pure organic single-molecule white-light emitters(SMWLE),the oxidation of thianthrene(TA)was performed on sulfur atoms at different degrees to tune room temperature phosphorescence(RTP)emission.With increasing degrees of oxidation from 1OTA,2OTA,3OTA,to 4OTA,monomeric and aggregative RTP emission was gradually suppressed,due to the gradual disappearance of lone pair electrons on sulfur atoms.Among these compounds,monomers and aggregates of 1OTA demonstrated a better intensity match between fluorescence and RTP.

Thermally Activated Delayed Fluorescence of Aggregates Induced by Strongπ–πInteractions and Reversible Dual-Responsive Luminescence Switching

A reversible dual-responsive luminescent material was introduced by our group to show the simultaneous color and lifetime switching in response to external stimuli.Pristine crystalline powder of(E)-2-(benzo[d]thiazol-2-yl)-3-(pyren-1-yl)acrylonitrile(Py-BZTCN)shows the orderedπ–πstacking with only near-monomer-normal orange-yellow fluorescence,but it exhibits red emission with thermally activated delayed fluorescence(TADF)after grinding,which can be reversibly recovered by heating or fuming treatment.Grinding disturbs the orderedπ–πstacking of pristine powder,leading to the formation of small aggregates with compressed distance and increased overlap ofπ–πstacking between adjacent molecules.The cause of switching was verified by single-crystal X-ray diffraction experiments of two corresponding crystals.This strongπ–πinteraction effectively promotes the excited-state energy splitting and substantially decreases the singlet–triplet energy gap(ΔEST)of aggregates,resulting in the red TADF emission of aggregates through reverse intersystem crossing.This finding proposes a new route to realizing the TADF emission of aggregates through strong intermolecular interactions based on non-TADF monomer,thereby enabling a novel high-contrast dualresponsive luminescence switching.