Achieving Photocatalytic Overall Nitrogen Fixation via an Enzymatic Pathway on a Distorted CoP4 Configuration.

Photocatalytic nitrogen (N2) fixation over semiconductors has always suffered from poor conversion efficiency owing to weak N2 adsorption and the difficulty of N≡N triple bond dissociation. Herein, a Co single-atom catalyst (SAC) model with a C-defect-evoked CoP4 distorted configuration was fabricated using a selective phosphidation strategy, wherein P-doping and C defects co-regulate the local electronic structure of Co sites. Comprehensive experiments and theoretical calculations revealed that the distorted CoP4 configuration caused a strong charge redistribution between the Co atoms and adjacent C atoms, minimizing their electronegativity difference.

Large Scale Synthesis of Red-Emitting Quantum Dots for Efficient and Stable Light-Emitting Diodes.

It is known that large-scale synthesis of emitters affords colloidal quantum dot (CQD) materials with a great opportunity toward the mass production of quantum dot light-emitting diodes (QLEDs) based commercial electronic products. Herein, an unprecedented example of scalable CQD (> 0.5 kilogram) is achieved by using a core/shell structure of CdZnSe/ZnSeS/CdZnS, in which CdZnSe, ZnSeS, and CdZnS alloys are used as the inner core, transition layer and outermost shell, respectively.

Upper Layer-Modulated Pseudo Planar Heterojunction with Metal Complex Acceptor for Efficient and Stable Organic Photovoltaics.

Modulating self-aggregation and charge transport in the upper acceptor layer of the pseudo planar heterojunction (PPHJ) is crucial for enhancing dielectric constant and suppressing trap density, leading to efficient and stable organic photovoltaics (OPVs). In this work, a metal complex acceptor (MCA), PtAC-Cl, is selectively incorporated into the upper host Y6 layer of PPHJ to regulate morphology and fill trap states. There exists a strong chemical interaction between PtAC-Cl and Y6, which can promote electron transfer.

Iron-Catalyzed Cross-Dehydrogenative Coupling of -Quinone Methides with Formamides: Activation of C(sp)-H Bonds.

A novel and straightforward method for the iron-catalyzed regioselective cross-dehydrogenative coupling of -quinone methides (-QMs) with formamides has been developed, facilitated by the activation of the C(sp)-H bonds of the formyl and alkenyl substituents via a radical strategy. This method does not require the preactivation of the substrates, and it can accommodate a wide range of -QMs and formamides under the optimized reaction conditions, resulting in the formation of the expected C-7 acetamides-functionalized -quinone methides with moderate to good yields. The control experiments revealed that the reaction follows the fundamental equation of second-order kinetics.

Fabrication of Ultrafine L1-FePt-Based Magnetic Patterns Enabled by Single-Step Nanoimprint-Assisted Block Copolymer Self-Assembly.

The bit islands in magnetic patterns play a crucial role in advancing magnetic recording density, but the trade-off issues between miniaturization and scalable production are still challenging. Here we present a two-in-one technique of nanoimprint lithography (NIL)-assisted self-assembly using a specially engineered FePt-containing block copolymer (BCP), offering a simple one-step fabrication for L1-FePt bit-patterned media with high throughput. This method combines top-down NIL with bottom-up self-assembly to precisely control the ultrafine magnetic bits in the nanoscale patterns.

Platinum(II) bis(arylacetylide) complexes bearing diarylamino-substituted bipyridine ligands for solution-processable phosphorescent OLED applications.

A comprehensive investigation has been carried out on a series of complexes of the type (N^N)Pt(-CC-Ar), where N^N represents diarylamino-substituted 2,2'-bipyridine (bpy) ligands and -CC-Ar refers to the substituted arylacetylide ligands. The introduction of trifluoromethyl and methoxy substituents to the phenylacetylide unit results in color tuning of the phosphorescence energy in these complexes. The bulky diarylamino substituents on the bipyridine ligand showed distinctive electronic properties, resulting in improved hole-transporting characteristics.

Over 18.2% efficiency of layer-by-layer all-polymer solar cells enabled by homoleptic iridium(III) carbene complex as solid additive.

The vertical phase distribution of active layers plays a vital role in balancing exciton dissociation and charge transport for achieving efficient polymer solar cells (PSCs). The layer-by-layer (LbL) PSCs are commonly prepared by using sequential spin-coating method from donor and acceptor solutions with distinct solvents and solvent additives. The enhanced exciton dissociation is expected in the LbL PSCs with efficient charge transport in the relatively neat donor or acceptor layers.

Work Function-Guided Electrocatalyst Design.

The development of high-performance electrocatalysts for energy conversion reactions is crucial for advancing global energy sustainability. The design of catalysts based on their electronic properties (e.g.

Water-Soluble Small Organic Fluorophores for Oncological Theragnostic Applications: Progress and Development.

Cancer is one of the major noncommunicable diseases, responsible for millions of deaths every year worldwide. Though various cancer detection and treatment modalities are available today, many deaths occur owing to its late-stage detection and metastatic nature. Noninvasive detection using luminescence-based imaging tools is considered one of the promising techniques owing to its low cost, high sensitivity, and brightness.

An All-In-One Integrating Strategy for Designing Platinum(II)-Based Supramolecular Polymers for Photocatalytic Hydrogen Evolution.

Organic polymer photocatalysts have achieved significant progress in photocatalytic hydrogen evolution, while developing the integrated organic polymers possessing the functions of photosensitizer, electron transfer mediator, and catalyst simultaneously is urgently needed and presents a great challenge. Considering that chalcogenoviologens are able to act as photosensitizers and electron-transfer mediators, a series of chalcogenoviologen-containing platinum(II)-based supramolecular polymers is designed, which exhibited strong visible light-absorbing ability and suitable bandgap for highly efficient photocatalytic hydrogen evolution without the use of a cocatalyst. The hydrogen evolution rate (HER) increases steadily with the decrease in an optical gap of the polymer.

Photoactivated Circularly Polarized Luminescent Organic Radicals in Doped Amorphous Polymer.

Luminescent organic radicals, especially those with photoactivated circularly polarized luminescence (CPL) features, hold great significance for cutting-edge optoelectronic applications, but their development still remains a challenge. In this study, we propose a novel strategy to achieve photoactivated CPL radicals by bonding two phosphine centers within an axial chiral system, yielding a compound of R/S-5,5-bis(diphenylphosphino)-4,4'-bibenzo[d][1,3]dioxole (R/S-BDP). The photoactivated R/S-BDP molecules in polymer matrix display a robust quantum yield of 19.

Large-Area Fabrication of Hexaazatrinaphthylene-Based 2D Metal-Organic Framework Films for Flexible Photodetectors and Optoelectronic Synapses.

2D conjugated metal-organic frameworks (c-MOFs) have emerged as promising materials for (opto)electronic applications due to their excellent charge transport properties originating from the unique layered-stacked structures with extended in-plane conjugation. The further advancement of MOF-based (opto)electronics necessitates the development of novel 2D c-MOF thin films with high quality. Cu-HHHATN (HHHATN: hexahydroxyl-hexaazatrinaphthylene) is a recently reported 2D c-MOF featuring high in-plane conjugation, strong interlayer π-π stacking, and multiple coordination sites, while the production of its thin-film form has not yet been reported.

Synthesis, Characterization, Cytotoxicity, Cellular Imaging, Molecular Docking, and ADMET Studies of Piperazine-Linked 1,8-Naphthalimide-Arylsulfonyl Derivatives.

To reduce the mortality and morbidity associated with cancer, new cancer theranostics are in high demand and are an emerging area of research. To achieve this goal, we report the synthesis and characterization of piperazine-linked 1,8-naphthalimide-arylsulfonyl derivatives (SA1-SA7). These compounds were synthesized in good yields following a two-step protocol and characterized using multiple analytical techniques.

Ruthenium-Catalyzed 1,6-Hydroalkylation of -Quinone Methides with Ketones via the Activation of C()-H Bonds.

A simple and efficient method for the ruthenium-catalyzed 1,6-hydroalkylation of -quinone methides (-QMs) with ketones via the activation of C()-H bonds has been disclosed. Without the need for preactivation of the substrates and oxidant, a broad range of -QMs and ketones are well tolerated, producing the expected 1,6-hydroalkylation products with moderate to good yields. Step-by-step control experiments and DFT calculation were conducted systematically to gain insights for the plausible reaction mechanism.

Two new red-emitting ternary europium(III) complexes with high photoluminescence quantum yields and exceptional performance in OLED devices.

Two new organo-europium complexes (OEuCs) [Eu(btfa)(Bathphen)] (OEuC-1) and [Eu(tta)(Bathphen)] (OEuC-2) where btfa and tta are the anions of 4,4,4-trifluoro-1-phenyl-1,3-butanedione and 2-thenoyltrifluoroacetone while Bathphen = Bathophenanthroline have been synthesized and characterized. Both complexes in the solid state exhibit strong red emissions with photoluminescence quantum yields (PLQYs) of 80% ± 10%. These complexes were tested as dopants in the emitting layer (EML) to fabricate red organic light emitting diodes (R-OLEDs).

The Novel Organic Emitters for High-Performance Narrow-Band Deep Blue OLEDs.

Narrow-band deep-blue organic light-emitting diodes (OLEDs) have played a key role in the field of high-quality full-color displays. However, because of the considerable challenges of inherent band gaps, unbalanced carrier injection and the lack of molecular structures, narrow-band deep-blue emitters develop slowly compared with red- and green-emitting materials. Encouragingly, with the continuous efforts of scientists in recent years, great progress has been made in the molecule design and material synthesis of highly efficient narrow-band deep-blue emitters.

Copper-Catalyzed Aerobic Oxidative/Decarboxylative Phosphorylation of Aryl Acrylic Acids with P(III)-Nucleophiles.

A copper-catalyzed aerobic oxidative/decarboxylative phosphorylation of aryl acrylic acids with P(III)-nucleophiles the Michaelis-Arbuzov rearrangement for the synthesis of β-ketophosphine oxides, β-ketophosphinates, and β-ketophosphonates is reported. The present reaction could be conducted effectively without the use of a ligand and a base. Various kinds of aryl acrylic acids and P(III)-nucleophiles are tolerated in the transformation, generating the desired β-keto-organophosphorus compounds as a valuable class of phosphorus-containing intermediates with good to excellent yields.

Efficient 1-(thiophen-2-yl)isoquinoline-based ionic iridophosphors with bulky counterions for solution-processed deep-red electroluminescence.

A pair of high-efficiency deep-red emissive ionic iridophosphors (Ira and Irb) showing high photoluminescence quantum yields (PLQYs) are rationally designed by using 1-(thiophen-2-yl)isoquinoline as the cyclometalating ligand. Two bulky tetraarylborate anions (tetraphenylborate and tetrakis(3,5-bis(trifluoromethyl)phenyl)borate) are selected to improve their PLQYs in both solution and aggregated states, which enables efficient electroluminescence a solution-processed approach. The variation of the tetraarylborate anions also aims to tune the photophysical properties of these deep-red emissive iridophosphors.

A Cobalt-Based Metal-Organic Framework Nanosheet as the Electrode for High-Performance Asymmetric Supercapacitor.

Inspired by the significant advantages of the bottom-up synthesis whose structures and functionalities can be customized by the selection of molecular components, a 2D metal-organic framework (MOF) nanosheet Co-BTB-LB has been synthesized by a liquid-liquid interface-assisted method. The as-prepared Co-BTB-LB is identified by scanning electron microscopy/energy dispersive spectroscopy (SEM/EDX) and X-ray photoelectron spectroscopy (XPS), and the sheet-like structure is verified by scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and atomic force microscopy (AFM). Co-BTB-LB electrode exhibits an excellent capacity of 4969.

Efficient Red Organic Light Emitting Diodes of Nona Coordinate Europium Tris(β-Diketonato) Complexes Bearing 4'-Phenyl-2,2':6',2''-Terpyridine.

Two novel nona-coordinated Eu(III) complexes [Eu(btfa) (Ph-TerPyr)] (Eu-1) and [Eu(NTA) (Ph-TerPyr)] (Eu-2) have been synthesized and characterized. The structure of the complexes was elucidated by density functional theory (DFT) methods. The experimental photophysical properties of the complexes were investigated and complemented with theoretical calculations.

Integrating Asymmetric O-B-N Unit in Multi-Resonance Thermally Activated Delayed Fluorescence Emitters towards High-Performance Deep-Blue Organic Light-Emitting Diodes.

Developing deep-blue thermally activated delayed fluorescence (TADF) emitters with both high efficiency and color purity remains a formidable challenge. Here, we proposed a design strategy by integrating asymmetric oxygen-boron-nitrogen (O-B-N) multi-resonance (MR) unit into traditional N-B-N MR molecules to form a rigid and extended O-B-N-B-N MR π-skeleton. Three deep-blue MR-TADF emitters of OBN, NBN and ODBN featuring asymmetric O-B-N, symmetric N-B-N and extended O-B-N-B-N MR units were synthesized through the regioselective one-shot electrophilic C-H borylation at different positions of the same precursor.

One-Pot Synthesis of Acetylacetonate-Based Isomeric Phosphorescent Cyclometalated Iridium(III) Complexes via Random Cyclometalation: A Strategy for Excited-State Manipulation.

The excited-state manipulation of the phosphorescent iridium(III) complexes plays a vital role in their photofunctional applications. The development of the molecular design strategy promotes the creative findings of novel iridium(III) complexes. The current molecular design strategies for iridium(III) complexes mainly depend on the selective cyclometalation of the ligands with the iridium(III) ion, which is governed by the steric hindrance of the ligand during the cyclometalation.

Non-covalent interactions (NCIs) in π-conjugated functional materials: advances and perspectives.

The design and development of functional materials with real-life applications are highly demanding. Understanding and controlling inter- and intra-molecular interactions provide opportunities to design new materials. A judicious manipulation of the molecular structure significantly alters such interactions and can boost selected properties and functions of the material.

Constructing 2D Sandwich-like MOF/MXene Heterostructures for Durable and Fast Aqueous Zinc-Ion Batteries.

Two-dimensional metal-organic frameworks (2D MOFs) can be used as the cathodes for high-performance zinc-ion battery due to their large one-dimensional channels. However, the conventionally poor electrical conductivity and low structural stability hinder their advances. Herein, we report an alternately stacked MOF/MX heterostructure, exhibiting the 2D sandwich-like structure with abundant active sites, improved electrical conductivity and exceptional structural stability.