Latest ArticlesThe structural principles of traditional Chinese mortise-and-tenon joints have inspired breakthroughs in supramolecular engineering. Nevertheless, substantial challenges remain in constructing nanoscale supramolecular architectures with precisely controlled giant dimensions. Herein, we report a precision-guided synthetic strategy for constructing giant 2D and 3D supramolecular architectures with rhomboidal motifs, which was achieved through a dovetail joint strategy. Initial assembly of bis-mortise ligand L1 with dovetail tenon ligand L2 in the presence of Cd2+ ions yielded the fundamental bis-rhombic supramolecule R1. Subsequent structural elaboration of the dovetail tenon motif enabled the development of multitopic ligands L3 and L4, which facilitated the construction of expanded architectures of the giant bis-propeller supramolecule R2 and tris-propeller supramolecule R3. The synthesized supramolecules R1–R3 were fully characterized multidimensional NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), traveling wave ion mobility mass spectrometry (TWIM-MS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). This work develops an innovative dovetail-joint assembly strategy for constructing rigid giant supramolecular architectures, establishing a new paradigm for precision engineering of complex 3D molecular systems.
In recent years, AgBiS2 nanocrystals (NCs) have emerged as a research hotspot in the field of solar cells due to their excellent optoelectronic properties and environmentally friendly characteristics. Although the theoretical power conversion efficiency (PCE) of AgBiS2 NC solar cells can reach up to 26%, the current best device only achieved a PCE of 10.84%. Such an enormous efficiency gap is primarily caused by the complex surface defects, severe carrier recombination, and undesirable energy-level mismatches. Therefore, this review comprehensively summarizes recent advancements in AgBiS2 NCs, including their crystal structures, optoelectronic properties, synthesis methods, ligand engineering, and device optimization. By fine-tuning synthesis conditions (e.g., temperature, precursor ratios) and employing ligand exchange strategies (solid-state/liquid-state), significant improvements in material performance have been realized. Furthermore, device structure optimization (e.g., transport layer selection, interface modification) and energy-level alignment engineering have further enhanced efficiency. Despite decent stabilities of AgBiS2 NCs, several challenges such as large-area uniformity and long-term device durability remain unraveled, which may be the major obstacles for their further commercialization. Future advancements in defect control, the development of novel ligands, and encapsulation technologies are expected to expand the applications of AgBiS2 NCs in flexible electronics, aerospace, and wearable devices.
PEGylation, the controlled covalent conjugation of polyethylene glycol to therapeutics, enhances therapeutic efficacy through optimized pharmacokinetics. However, to date no high-molecular-weight PEGylated small-molecule prodrugs have received regulatory approval. This technological gap can be partially attributed to the exponential proliferation of metabolic intermediates resulting from multi-payload conjugation strategies, which introduces unprecedented analytical complexities in metabolite profiling and pharmacokinetic characterization. To address this challenge, we developed a liquid chromatography-triple-quadrupole/time-of-flight mass spectrometry platform for PEG20k-(irinotecan)3, a Phase Ⅲ clinical candidate. Our methodology employs payload stoichiometry-based chromatographic resolution for clustering isomeric PEG species. Complementarily, diagnostic product ions at m/z 699.83, 569.27, and 587.28 enable systematic differentiation between double-loaded, single-loaded, and released irinotecan payload. This approach successfully identifies eight metabolic clusters spanning from PEG-conjugates, cleaved PEG segments, and released small-molecule species. Its demonstrated capacity to deconvolute complex metabolic profiles—through payload-stoichiometry based chromatographic resolution coupled with diagnostic ion analysis—positions this workflow as an attractive tool for accelerating the development of PEGylated small-molecule therapeutics.
Sustainable development for our life is important task, which is driven by key materials and technologies. In this roadmap, we discuss three main aspects in addressing environmental questions, green chemical processes and energy challenges. They are included, such as gas treatment and separation, wastewater treatment, waste gas treatment, solid waste treatment, lithium extraction, hydrogen production, water splitting, CO2 reduction, photocatalytic clean technologies, plastic degradation, fuel cells, lithium batteries, sodium batteries, aqueous batteries, solid state batteries, metal air batteries and supercapacitors. Their status, challenges, progress and future perspectives are also discussed. We hope that this paper can give clear views on sustainable development in materials and technologies.
This research explores the influence of crystallinity on gas chromatographic (GC) separation using covalent organic frameworks (COFs) as stationary phases. Three COF materials (CTF-DCBs) with varying crystallinity were synthesized and characterized. CTF-DCB-1, with superior crystallinity, demonstrated high-selectivity GC separation of benzene isomers as well as styrene/phenylacetylene mixtures, while CTF-DCB-2 and CTF-DCB-3 exhibited lower crystallinity and worse separation performance. Thermodynamic and kinetic tests showed that CTF-DCB-1 had the worst thermodynamic adsorption but low diffusion mass transfer resistance, which resulted in the best separation. Therefore, optimizing the crystallinity of COFs is necessary for balancing the kinetic diffusion and thermodynamic interactions towards the analytes, achieving high-performance GC stationary phases.
Regulation of apoptosis represents a key parameter in all living organisms. In this paper, an input-induced logic-gated modular nanocalculator is designed to regulate cancer cell apoptosis by programmatically combining and connecting logic gate modules with different functions. Via rational design of the various logic gate modules of the nanocalculator, different apoptosis related operations including cancer cell targeting, apoptosis induction, and apoptosis monitoring could be performed. Importantly, each of these logic gate modules could independently perform apoptosis related YES logic operations when ran separately. After combining each YES logic gate module into a logic circuit and connecting it to the GO scaffold to construct a logic-gated nanocalculator, the input-induced logic-gated modular nanocalculator could selectively enter cancer cells and control the drug release to logically apoptosis (output), by performing AND logic gate operations when inputs (nucleolin and H+) were included at the same time. Moreover, evidence suggests that these efficient logical calculations proceed in cancer cell apoptosis regulation without the general limiations of lithography in nanotechnology. As such, this work provides a new vision for the construction of a logic-gated modular nanocalculator with logical calculation proficiency potentially useful in cancer therapy and the regulation of life.
Magnesium hydride (MgH2) demonstrates immense potential as a solid-state hydrogen storage material, while its commercial utilization is impeded by the elevated operating temperature and sluggish reaction kinetics. Herein, a MOF derived multi-phase FeNi3-S catalyst was specially designed for efficient hydrogen storage in MgH2. Experiments confirmed that the incorporation of FeNi3-S into MgH2 significantly lowered the desorption temperature and accelerated the kinetics of hydrogen desorption and reabsorption. The initial dehydrogenation temperature of the MgH2 + 10 wt% FeNi3-S composite was 202 °C, which was 123 °C lower than that of pure MgH2. At 325 °C, the MgH2 + 10 wt% FeNi3-S composite released 6.57 wt% H2 (fully dehydrogenated) within 1000 s. Remarkably, MgH2 + 10 wt% FeNi3-S composite initiated rehydrogenation at room temperature and rapidly absorbed 2.49 wt% H2 within 30 min at 100 °C. Moreover, 6.3 wt% H2 was still retained after 20 cycles at 300 °C, demonstrating the superior cycling performance of the MgH2 + 10 wt% FeNi3-S composite. The activation energy fitting calculations further evidenced the addition of FeNi3-S enhanced the de/resorption kinetics of MgH2 (Ea = 98.6 kJ/mol and 43.3 kJ/mol, respectively). Through phase and microstructural analysis, it was determined that the exceptional hydrogen storage performance of the composite was attributed to the in-situ formation of Mg/Mg2Ni + Fe/MgS and MgH2/Mg2NiH4 + Fe/MgS hydrogen storage systems. Further mechanistic analysis revealed that Mg2Ni/Mg2NiH4 served as “hydrogen pump” and Fe/MgS served as “hydrogen diffusion channel”, thus accelerating the dissociation and recombination of hydrogen molecules. In conclusion, this work offers insight into catalysts combining transition metal alloys and transition metal sulfide for exerting muti-phase synergistic effect on boosting the dehydrogenation/hydrogenation reactions of MgH2, which can also inspire future pioneering work on designing and fabricating high efficient catalysts in other energy storage related areas.
The rate-limited activation of NN triple bonds with high bond energies has been a bottleneck in photoctalytic nitrogen fixation. Here, polymeric carbon nitride with frustrated Lewis pairs (FLPs) was constructed by inserting electron-deficient magnesium into g-C3N4 (CN). The synergistic interactions between Mg and amino groups in CN led to a 7.2 fold increase in the photoreactivity of nitrogen (N2) fixation by carbon nitride.
Photocatalytic fuel cells provide promising opportunities for sustainable wastewater treatment and energy conversion. However, their applications are challenged by the sluggish oxygen reducton reaction (ORR) kinetics at cathodes owning to the low O2 solubility and diffusion rate. Herein, we proposed a photo-biocatalytic fuel cell (PBFC) with a novel hybrid biocathode based on artificially engineered algal cells coated by ZIF-8 confined carbon dots/bilirubin oxidase (ZIF-8/CDs/BOD@algae). Microalgae absorbed CO2 and provided O2 in situ for BOD catalysts. Due to effective absorption of O2 by imidazole and confinement of hydrophobic porous ZIF-8, oxygen diffusion has been accelerated in MOF/enzyme systems. Importantly, the introduction of CDs alleviated the poor conductivity of ZIF-8 and improved the electron transfer rate of BOD. Thus, the biocathode exhibited a high current density of 1767 µA/cm2, a 2.26-fold increase compared with that of CDs/BOD/algae biocathode. Also, it displayed enduring operational stability for up to 60 h since the firmly wrapped ZIF-8 shells could encapsulate proteins and protect algae from the external stimulation. When coupled with Mo: BiVO4 photoanodes, the PBFC exhibited a remarkable power output of 131.8 µW/cm2 using tetracycline hydrochloride (TCH) as a fuel and an increased degradation rate of TCH. Therefore, this work not only establishs an effective confinement strategy for enzyme to enrich oxygen, but also unveils new possibilities for modified microalgal cells aiding photoelectrocatalytic systems to recover energy from wastewater treatment.
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