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Although the multiple-component (MC) blend strategy has been frequently used as a very effective way to improve the performance of organic solar cells (OSCs), there is a strong need to understand the fundamental working mechanism and material selection rule for achieving optimal MC-OSCs. Here we present the ‘dilution effect’ as the mechanism for MC-OSCs, where two highly miscible components are molecularly intermixed. Contrary to the aggregation-induced non-radiative decay, the dilution effect enables higher luminescence quantum efficiencies and open-circuit voltages (VOC) in MC-OSCs via suppressed electron–vibration coupling. The continuously broadened bandgap together with reduced electron–vibration coupling also explains the composition-dependent VOC in ternary blends well. Moreover, we show that electrons can transfer between different acceptors, depending on the energy offset between them, which contributes to the largely unperturbed charge transport and high fill factors in MC-OSCs. The discovery of the dilution effect enables the demonstration of a high power conversion efficiency of 18.31% in an MC-OSC.A strategy based on molecular intermixing of two highly miscible components enables the demonstration of high efficiency multiple-component organic solar cells.

It has been a challenging topic and perpetual task to design and synthesize covalent macrocycles with characteristic self-assembling behaviors and excellent host-guest properties in supramolecular chemistry. Herein, we present a family of macrocyclic diphenylamine[n]arenes ( DPA[n]s , n = 3–7) consisting of methyldiphenylamine units through a facile one-pot synthesis strategy. Unlike many other reported macrocyclic arenes, the resultant non-planar DPA[n]s feature intrinsic π-π stacking interactions, interesting self-assembling behaviors and ethene/ethyne capture properties. Specifically, strong multiple intermolecular edge-to-face aromatic interactions in DPA[3] have been systematically investigated both in solid and solution states. The intriguing findings on the intermolecular edge-to-face stacking interaction mode in the macrocycle would further highlight the importance of noncovalent π-π interaction in supramolecular self-assembly. This study will also shed light on the macrocyclic and supramolecular chemistry and, we expect, will provide a direction for design and synthesis of covalent macrocycles in this area. The design of covalent macrocycles which show characteristic self-assembly behaviour and host-guest properties is challenging. Here, the authors demonstrate the synthesis of diphenylamine[n]arenes through a one-pot synthesis and demonstrate the π-π pi stacking of the non-planar rings as well as ethane/ethyne host-guest interactions.

Sophisticated mechanically interlocked molecules (MIMs) with interesting structures, properties and applications have attracted great interest in the field of supramolecular chemistry. We herein report a highly efficient self-assembly of heterometallic triangular necklace 1 containing Cu and Pt metals with strong antibacterial activity. Single-crystal X-ray analysis shows that the finely arranged triangular necklace 1 has two racemic enantiomers in its solid state with intriguing packing motif. The superior antibacterial activity of necklace 1 against both standard and clinically drug-resistant pathogens implies that the presence of Cu(I) center and platinum(II) significantly enhance the bacterium-binding/damaging activity, which is mainly attributed to the highly positively charged nature, the possible synergistic effect of heterometals in the necklace, and the improved stability in culture media. This work clearly discloses the structure-property relationships that the existence of two different metal centers not only facilitates successful construction of heterometallic triangular necklace but also endows it with superior nuclease properties and antibacterial activities. Precise assembly of heterometallic complexes is a challenge. Here, the authors design a heterometallic triangular necklace through a highly efficient threading-and-ring-closing approach driven by metal-ligand coordination, which shows strong bacterium-binding and cell wall/plasma membrane-disrupting capacity for killing bacterial cells.

Triangulene, also known as Clar’s hydrocarbon, has been sought after by chemists for more than 70 years but with limited success. Herein, we report an oxidative dehydrogenation method to synthesize two kinetically blocked [3]triangulene derivatives TRI-1 (reported) and TRI-2 (newly synthesized), in which the three most reactive sites are substituted by bulky mesityl groups and electron-withdrawing 2,4,6-trichlorophenyl groups, and meanwhile, three vertices of triangulene are substituted by tert-butyl groups. Interestingly, the dihydro-triangulene core possesses two isomers well characterized by UV-vis, NMR spectroscopy, and X-ray crystallographic analysis, which is interestingly substituent-dependent. The newly synthesized TRI-2 is isolated in crystalline form, and X-ray crystallographic analysis reveals that the aryl substituents are nearly perpendicular to the triangulene plane and thus cause little perturbation of the electronic properties of the triangulene. Notably, 2,4,6-trichlorophenyl-substituted TRI-2 exhibits enhanced stability compared to the reported mesityl-substituted TRI-1, e.g., TRI-2 is stable for months in a crystalline state under a nitrogen atmosphere, and TRI-2 in a solution state is also more persistent than TRI-1 (half-life for TRI-1 ≈ 18 h vs. TRI-2 ≈ 132 h). This achievement will facilitate the design and synthesis of stable triangulene dimers and oligomers with higher spin multiplicity.

Interpenetration is a phenomenon frequently encountered in self-assembled Pd 2 L 4 -type coordination cages, while the mechanism of the interpenetration process remains unclear. Here we show the synthesis and solvent-mediated interconversion of highly soluble phenoxazine-based monomeric cage 1 and corresponding interlocked dimer 2 . We succeed in the isolation and single-crystal structure analysis of both 1 and 2 with the same guest anion by changing the solvents utilized in self-assembly. The monomeric-to-dimeric cage conversion occurs by heating in weakly coordinating solvents, while dimeric-to-monomeric cage conversion takes place through a disassembly and reassembly process in strongly coordinating solvents at low concentration or by the addition/removal of competing ligand. The interconversion may be driven by the distinct thermodynamic stabilities of 1 and 2 in different solvents. Additionally, Cl – anions template the interpenetration of 1 because of the strong chloride binding affinity of 2 which could serve as an anion-binding catalyst for the C–Cl bond cleavage. While Pd 2 L 4 -type coordination cages tend to form interlocked dimers, isolation and characterization of both the cage and its interlocked dimer is very challenging. Herein, the authors report the synthesis and solvent-mediated interconversion of highly soluble phenoxazine-based monomeric cage and corresponding interlocked dimer.

Organic diradicaloids usually display an open-shell singlet ground state with significant singlet diradical character ( y 0 ) which endow them with intriguing physiochemical properties and wide applications. In this study, we present the design of an open-shell nitrogen-centered diradicaloid which can reversibly respond to multiple stimuli and display the tunable diradical character and chemo-physical properties. 1a was successfully synthesized through a simple and high-yielding two-step synthetic strategy. Both experimental and calculated results indicated that 1a displayed an open-shell singlet ground state with small singlet-triplet energy gap (Δ E S−T  = −2.311 kcal mol − 1 ) and a modest diradical character ( y 0  = 0.60). Interestingly, 1a was demonstrated to undergo reversible Lewis acid-base reaction to form acid-base adducts, which was proven to effectively tune the ground-state electronic structures of 1a as well as its diradical character and spin density distributions. Based on this, we succeeded in devising a photoresponsive system based on 1a and a commercially available photoacid merocyanine (MEH). We believe that our studies including the molecular design methodology and the stimuli-responsive organic diradicaloid system will open up a new way to develop organic diradicaloids with tunable properties and even intelligent-responsive diradicaloid-based materials. The electronic structures and open-shell diradical character of organic diradicaloids endow them with potentially useful optical, electronic and magnetic properties. Here, an open-shell nitrogen-centered diradicaloid is reported and shown to readily react with Lewis and Brønsted acids to form acid-base adducts, allowing for tuning of ground-state electronic structure, diradical character and spin density distribution.

With the popularity of the Internet, computer technology has been applied to college education, especially English teaching. Through the network platform (hereinafter referred to as NP), college students can compete in English, including listening, speaking, reading and writing. Through Promoting Learning by Competition (hereinafter referred to as PLBC), students can show their learning knowledge through skill competition, which will better integrate situational teaching and practical teaching. Through the NP, we can gather students from all over the country to participate in the competition, which has solved the basic problem of the number of participants for colleges and universities. By PLBCs, colleges and universities can cultivate practical professionals, which can increase the practicability of students’ English ability. Through blended English teaching model (hereinafter referred to as BETM), colleges and universities can form a teaching system of “teaching, learning, practice and competition”, which will strengthen students’ practical ability and learning efficiency. First of all, this paper analyzes the importance of PLBC. Then, this paper demonstrates the advantages of BETM. Finally, some suggestions are put forward.

Camrelizumab is a novel programmed cell death protein 1 (PD-1) inhibitor developed in China that exhibits good efficacy in several advanced cancer types, including non-small cell lung cancer (NSCLC); however, its utility as a neoadjuvant regimen in NSCLC remains unclear. Thus, the present study aimed to explore the efficacy and safety of neoadjuvant camrelizumab plus chemotherapy in patients with locally advanced NSCLC. A total of 56 patients with stage IIIA/IIIB resectable NSCLC were analyzed in the present prospective observational study. Amongst the cohort, 31 patients underwent neoadjuvant camrelizumab (200 mg every 2 weeks) plus paclitaxel and carboplatin (PC) chemotherapy, while another 25 cases underwent neoadjuvant PC chemotherapy alone. The pathological response, disease-free survival (DFS) time, overall survival (OS) time and adverse events (AEs) were analyzed. The complete pathological response (25.8 vs. 8.3%; P=0.159) and major pathological response (MPR) (61.3 vs. 37.5%; P=0.080) rates were higher in the camrelizumab plus PC group compared with the findings in the PC group, although the results were not statistically significant. DFS time was significantly prolonged in the camrelizumab plus PC group compared with that in the PC group (P=0.030); however, there was no difference in OS time between these two groups (P=0.251). Following adjustment by multivariate analysis, the camrelizumab plus PC regimen versus the PC regimen alone was independently associated with higher MPR [odds ratio, 5.216; 95% confidence interval (CI), 1.178-23.086; P=0.030], and favorable DFS [hazard ratio (HR), 0.055; 95% CI, 0.007-0.442; P=0.006] and OS (HR, 0.025; 95% CI, 0.002-0.416; P=0.010) times. The most common AEs of the neoadjuvant camrelizumab plus PC regimen were alopecia (51.6%), nausea and vomiting (45.2%), anemia (41.9%) and fatigue (41.9%), the majority of which occurred in patients with grade 1-2 disease. The present results indicated that neoadjuvant camrelizumab plus PC chemotherapy exhibited a superior pathological response and survival profile to PC chemotherapy alone, and was well tolerated in patients with locally advanced NSCLC.

In this study, the design and synthesis of two novel diazapentacene‐based macrocycles ( M3 and M4 ) is reported via a one‐pot Yamamoto coupling reaction. These macrocycles are constructed by π‐extension of a dihydrophenazine core, maintaining its excellent redox activity while offering enlarged cavities and enhanced electron‐donating properties. As a result, M3 and M4 exhibit strong electron‐rich characteristics and well‐defined cavities, enabling their use as efficient iodine adsorbents to mitigate photo‐thermal‐induced iodine loss and perovskite degradation in solar cells. The macrocycles demonstrate dual‐mode iodine capture: physical adsorption through cavity confinement and chemical adsorption via charge‐transfer interactions, both of which show excellent reversibility. Addressing the critical issue of operational instability in perovskite solar cells (PSCs), caused by iodine escape and Pb⁰ defect formation, these macrocycles effectively trap volatile iodine species and suppress defect generation. Notably, PSCs incorporating macrocycle M4 achieve a high efficiency of 26.13% and outstanding operational stability, retaining ≈95.85% of their initial efficiency after 1000 h of maximum power point (MPP) tracking at 85  °C under the International Summit on Organic Photovoltaic Stability‐Light‐Soaking Test at 65/85 °C (ISOS‐L‐2) protocol.

Interpenetration is a phenomenon frequently encountered in self-assembled Pd L -type coordination cages, while the mechanism of the interpenetration process remains unclear. Here we show the synthesis and solvent-mediated interconversion of highly soluble phenoxazine-based monomeric cage 1 and corresponding interlocked dimer 2. We succeed in the isolation and single-crystal structure analysis of both 1 and 2 with the same guest anion by changing the solvents utilized in self-assembly. The monomeric-to-dimeric cage conversion occurs by heating in weakly coordinating solvents, while dimeric-to-monomeric cage conversion takes place through a disassembly and reassembly process in strongly coordinating solvents at low concentration or by the addition/removal of competing ligand. The interconversion may be driven by the distinct thermodynamic stabilities of 1 and 2 in different solvents. Additionally, Cl anions template the interpenetration of 1 because of the strong chloride binding affinity of 2 which could serve as an anion-binding catalyst for the C-Cl bond cleavage.