Search

Chemical self‐recharging zinc ion batteries (ZIBs), which are capable of auto‐recharging in ambient air, are promising in self‐powered battery systems. Nevertheless, the exclusive reliance on chemical energy from oxygen for ZIBs charging often would bring some obstacles in charging efficiency. Herein, we develop photo‐assisted chemical self‐recharging aqueous ZIBs with a heterojunction of MoS2/SnO2 cathode, which are favorable to enhancing both the charging and discharging efficiency as well as the chemical self‐charging capabilities under illumination. The photo‐assisted process promotes the electron transfer from MoS2/SnO2 to oxygen, accelerating the occurrence of the oxidation reaction during chemical self‐charging. Furthermore, the electrons within the MoS2/SnO2 cathode exhibit a low transfer impedance under illumination, which is beneficial to reducing the migration barrier of Zn2+ within the cathode and thereby facilitating the uniform inserting of Zn2+ into MoS2/SnO2 cathode during discharging. This photo‐assisted chemical self‐recharging mechanism enables ZIBs to attain a maximum self‐charging potential of 0.95 V within 3 hours, a considerable self‐charging capacity of 202.5 mAh g−1 and excellent cycling performance in a self‐charging mode. This work not only provides a route for optimizing chemical self‐charging energy storage, but also broadens the potential application of aqueous ZIBs. [ABSTRACT FROM AUTHOR]

Advanced multiple resonance thermally activated delayed fluorescence (MR‐TADF) emitters with high efficiency and color purity have emerged as a research focus in the development of ultra‐high‐definition displays. Herein, we disclose an approach to modulate the charge‐transfer excited states of MR emitters via intramolecular covalent bond locking. This strategy can promote the evolution of strong intramolecular charge‐transfer (ICT) states into weak ICT states, ultimately narrowing the full‐width at half‐maximum (FWHM) of emitters. To modulate the ICT intensity, two octagonal rings are introduced to yield molecule m‐DCzDAz‐BNCz. Compounds m‐CzDAz‐BNCz and m‐DCzDAz‐BNCz exhibit bright light‐green and green fluorescence in toluene, with emission maxima of 504 and 513 nm, and FWHMs of 28 and 34 nm, respectively. Sensitized organic light‐emitting diodes (OLEDs) employing emitters m‐CzDAz‐BNCz and m‐DCzDAz‐BNCz exhibit green emission with peaks of 508 and 520 nm, Commission Internationale de L'Eclairage (CIE) coordinates of (0.12, 0.65) and (0.19, 0.69), and maximum external quantum efficiencies (EQEs) of 30.2 % and 32.6 %, respectively. [ABSTRACT FROM AUTHOR]

The lack of stable solid‐state electrolytes (SSEs) with high‐ionic conductivity and the rational design of electrode/electrolyte interfaces remains challenging for solid‐state lithium batteries. Here, for the first time, a high‐performance solid‐state lithium‐oxygen (Li−O2) battery is developed based on the Li‐ion‐conducted hydrogen‐bonded organic framework (LHOF) electrolyte and the HOF‐DAT@CNT composite cathode. Benefiting from the abundant dynamic hydrogen bonding network in the backbone of LHOF‐DAT SSEs, fast Li+ ion transport (2.2×10−4 S cm−1), a high Li+ transference number (0.88), and a wide electrochemical window of 5.05 V are achieved. Symmetric batteries constructed with LHOF‐DAT SSEs exhibit a stably cycled duration of over 1400 h with uniform deposition, which mainly stems from the jumping sites that promote a uniformly high rate of Li+ flux and the hydrogen‐bonding network structure that can relieve the structural changes during Li+ transport. LHOF‐DAT SSEs‐based Li−O2 batteries exhibit high specific capacity (10335 mAh g−1), and stable cycling life up to 150 cycles. Moreover, the solid‐state lithium metal battery with LHOF‐DAT SSEs endow good rate capability (129.6 mAh g−1 at 0.5 C), long‐term discharge/charge stability (210 cycles). The design of LHOF‐DAT SSEs opens an avenue for the development of novel SSEs‐based solid‐state lithium batteries. [ABSTRACT FROM AUTHOR]

Liquid organic hydrogen carriers (LOHCs) are attractive platform molecules that play an important role in hydrogen energy storage and utilization. The multi‐step hydrogenation of toluene (TOL) to methylcyclohexane (MCH) has been widely studied in the LOCHs systems, due to their relatively low toxicity and reasonable hydrogen storage capacity. Noble metal catalysts such as Ru has exhibited good performance in multi‐step hydrogenation reactions, while the application is still hindered by their high cost and low specific activity. Therefore, the primary challenge lies in the development of noble metal catalysts with both robust activity and efficient atomic utilization. In this study, a series of Ru species ranging from single atoms, fully exposed clusters to nanoparticles were fabricated to investigate their structural evolution in the TOL multi‐step hydrogenation reaction. The fully exposed and atomically dispersed Ru clusters, composed of an average of 3 Ru atoms, exhibit superior catalytic performance and recycle ability in TOL multi‐step hydrogenation. Moreover, it delivers a high turnover frequency of 9850.3 h−1 under the relatively mild reaction (100 °C, 1.5 MPa), compared with those of single atoms and nanoparticles, and shows a notable advantage over catalysts reported in previous studies. From density functional theory (DFT) calculations, the overall barrier of the TOL multi‐step hydrogenation reaction over the fully exposed Ru clusters is significantly lower than that of single atoms and nanoparticles, resulting in its higher activity. The present work provides an efficient strategy to regulate the reaction pathway of multi‐step complicated catalytic reactions by designing fully exposed metal cluster catalysts. [ABSTRACT FROM AUTHOR]

The development of deep‐blue organic light‐emitting diodes (OLEDs) featuring high efficiency and narrowband emission is of great importance for ultrahigh‐definition displays with wide color gamut. Herein, based on the nitrogen‐embedding strategy for modifying the short range charge transfer excited state energies of multi‐resonance (MR) thermally activated delayed fluorescence (TADF) emitters, we introduce one or two nitrogen atoms into the central benzene ring of a versatile boron‐embedded 1,3‐bis(carbazol‐9‐yl)benzene skeleton. This approach resulted in the stabilization of the highest occupied molecular orbital energy levels and the formation of intramolecular hydrogen bonds, and thus systematic hypsochromic shifts and narrowing spectra. In toluene solution, two heterocyclic‐based MR‐TADF molecules, Py‐BN and Pm‐BN, exhibit deep‐blue emissions with high photoluminescence quantum yields of 93 % and 94 %, and narrow full width at half maximum of 14 and 13 nm, respectively. A deep‐blue hyperfluorescent OLED based on Py‐BN exhibited a maximum external quantum efficiency of 27.7 % and desired color purity with Commission Internationale de L'Eclairage (CIE) coordinates of (0.150, 0.052). These results demonstrate the significant potential for the development of deep blue narrowband MR‐TADF emitters. [ABSTRACT FROM AUTHOR]

Therapeutic peptides are a major class of pharmaceutical drugs owing to their target‐binding specificity as well as their versatility in inhibiting aberrant protein‐protein interactions associated with human pathologies. Within the realm of amyloid diseases, the use of peptides and peptidomimetics tailor‐designed to overcome amyloidogenesis has been an active research endeavor since the late 90s. In more recent years, incorporating nanoparticles for enhancing the biocirculation and delivery of peptide drugs has emerged as a frontier in nanomedicine, and nanoparticles have further demonstrated a potency against amyloid aggregation and cellular inflammation to rival strategies employing small molecules, peptides, and antibodies. Despite these efforts, however, a fundamental understanding of the chemistry, characteristics and function of peptido‐nanocomposites is lacking, and a systematic analysis of such strategy for combating a range of amyloid pathogeneses is missing. Here we review the history, principles and evolving chemistry of constructing peptido‐nanocomposites from bottom up and discuss their future application against amyloid diseases that debilitate a significant portion of the global population. [ABSTRACT FROM AUTHOR]

Multi‐resonance thermally activated delayed fluorescence (MR‐TADF) emitters with narrow emission spectra have garnered significant attention in future organic light‐emitting diode (OLED) displays. However, current C=O/N‐embedded MR‐TADF systems still lack satisfactory performance in terms of electroluminescence bandwidths and external quantum efficiencies (EQEs). In this study, a C=O/N‐embedded green MR‐TADF emitter, featuring two acridone units incorporated in a sterically protected 11‐ring fused core skeleton, is successfully synthesized through finely controlling the reaction selectivity. The superior combination of multiple intramolecular fusion and steric wrapping strategies in the design of the emitter not only imparts an extremely narrow emission spectrum and a high fluorescence quantum yield to the emitter but also mitigates aggregation‐induced spectral broadening and fluorescence quenching. Therefore, the emitter exhibits leading green OLED performance among C=O/N‐based MR‐TADF systems, achieving an EQE of up to 37.2 %, a full width at half maximum of merely 0.11 eV (24 nm), and a Commission Internationale de l′Éclairage coordinate of (0.20, 0.73). This study marks a significant advance in the realization of ideal C=O/N‐based MR‐TADF emitters and holds profound implications for the design and synthesis of other MR‐TADF systems. [ABSTRACT FROM AUTHOR]

Bone metastasis is a type of metastatic tumors that involves the spreads of malignant tumor cells into skeleton, and its diagnosis and treatment remain a big challenge due to the unique tumor microenvironment. We herein develop osteoclast and tumor cell dual‐targeting biomimetic semiconducting polymer nanocomposites (SPFeNOC) for amplified theranostics of bone metastasis. SPFeNOC contain semiconducting polymer and iron oxide (Fe3O4) nanoparticles inside core and surface camouflaged hybrid membrane of cancer cells and osteoclasts. The hybrid membrane camouflage enables their targeting to both metastatic tumor cells and osteoclasts in bone metastasis through homologous targeting mechanism, thus achieving an enhanced nanoparticle accumulation in tumors. The semiconducting polymer mediates near‐infrared (NIR) fluorescence imaging and sonodynamic therapy (SDT), and Fe3O4 nanoparticles are used for magnetic resonance (MR) imaging and chemodynamic therapy (CDT). Because both cancer cells and osteoclasts are killed synchronously via the combinational action of SDT and CDT, the vicious cycle in bone metastasis is broken to realize high antitumor efficacy. Therefore, 4T1 breast cancer‐based bone metastasis can be effectively detected and cured by using SPFeNOC as dual‐targeting theranostic nanoagents. This study provides an unusual biomimetic nanoplatform that simultaneously targets osteoclasts and cancer cells for amplified theranostics of bone metastasis. [ABSTRACT FROM AUTHOR]

Anion‐coordination‐driven assembly (ACDA) has proven to be a very effective strategy for the construction of polyhedral structures. Here we demonstrate that variation of the "angle" of the backbone of C3‐symmetric tris‐bis(urea) ligands, from triphenylamine to triphenylphosphine oxide, results in the change of the final construct from an A4L4 tetrahedron to a higher‐nuclearity, A6L6 trigonal antiprism (A=anion, herein PO43−; L=ligand). Most interestingly, this assembly features a huge hollow internal space that is divided into three compartments: one central cavity and two large outer pockets. This multi‐cavity character enables the binding of different guests, namely monosaccharides or polyethylene glycol molecules (PEG600, PEG1000 and PEG2000), respectively. The results prove that anion coordination by multiple hydrogen bonds may provide both sufficient strength and flexibility, thus making possible the formation of complicated structures with adaptive guest binding ability. [ABSTRACT FROM AUTHOR]

Advanced multiple resonance induced thermally activated delayed fluorescence (MR‐TADF) emitters have emerged as a privileged motif for applications in organic light‐emitting diodes (OLEDs), because they furnish highly tunable TADF characteristics and high color purity emission. Herein, based on the unique nitrogen‐atom embedding molecular engineering (NEME) strategy, a series of compounds BN‐TP‐Nx (x=1, 2, 3, 4) have been customized. The nitrogen‐atom anchored at different position of triphenylene hexagonal lattice entails varying degrees of perturbation to the electronic structure. The newly‐constructed emitters have demonstrated the precise regulation of emission maxima of MR‐TADF emitters to meet the actual industrial demand, and further enormously enriched the MR‐TADF molecular reservoir. The BN‐TP‐N3‐based OLED exhibits ultrapure green emission, with peak of 524 nm, full‐width at half‐maximum (FWHM) of 33 nm, Commission Internationale de L'Eclairage (CIE) coordinates of (0.23, 0.71), and maximum external quantum efficiency (EQE) of 37.3 %. [ABSTRACT FROM AUTHOR]