Latest ArticlesAlthough lots of efforts have been devoted on new less hygroscopic dopants to address problems in hole transport materials (HTM), the long-time post-oxidation and the volatilization of 4-tert-butylpyridine (tBP) are still issues. A new doping mechanism for spiro-OMeTAD by disulfiram (TETD) is revealed in this work. Owing to its disulfide bond, TETD can be activated easily to produce reactive sulfur for the rapid oxidation of spiro-OMeTAD in the absence of oxygen with formation of [spiro-OMeTAD•]+[SC(S)N(C2H5)2]-. Thus, in this situation, the Li+ ion has the opportunity to coordinate tBP and fix each other in HTM film. DFT calculations suggest that the resulting favorable energy (with a ΔE of −1.29 eV) must come from the mutual interactions among Li+, TFSI−, and tBP, which is different from the well-known doping process that tBP would not participate in the doping reaction. As a result, the introduction of a new radical into the HTM greatly reduce device performance fluctuations due to the environmental dependence and inhibit tBP volatilizing for enhanced long-term stability.
Colon-targeted oral drug delivery systems are one of the most promising therapeutic strategies for alleviating and curing inflammatory bowel disease (IBD), but they still face challenges in successfully passing through the harsh gastrointestinal environment and intestinal mucus barrier. To overcome the gastrointestinal barriers for oral drug delivery mentioned above, a "spore-like" oral nanodrug delivery platform (Cur/COS/SC NPs) has been developed. Firstly, chitooligosaccharides (COS) are encapsulated on the surface of Curcumin nanoparticles (Cur NPs) to form carrier-free nanoparticles (Cur/COS NPs). Subsequently, inspired by the natural high resistance of spore coat (SC), SC is chosen as the "protective umbrella" to encapsulate Cur/COS NPs for precision targeted therapy of IBD. After oral administration, SC can effectively protect NPs through the rugged gastrointestinal environment and exhibit excellent intestinal mucus penetration characteristics. Moreover, the negatively-charged Cur/COS/SC NPs specifically target positively-charged inflamed colon via electrostatic interactions. It is demonstrated that Cur/COS/SC NPs can promote the expression of tight junction proteins, inhibit aberrant activation of the Toll-like receptor 4/myeloid differentiation primary response gene 88/nuclear factor-κB (TLR4/MyD88/NF-κB) signaling pathway, and downregulate the levels of pro-inflammatory factors, exhibiting excellent anti-inflammatory effects. Notably, it is found that Cur/COS/SC NPs can significantly increase the richness and diversity of gut microbiota, and restore the homeostasis of gut microbiota by inhibiting pathogenic bacteria and promoting probiotics. Hence, Cur/COS/SC NPs provide a safe, efficient, and feasible new strategy for IBD treatment.
Achieving seamless tiling through the self-assembly of organic species has long fascinated scientists for its potential applications across various fields. However, constructing periodic nanostructures with high-order tessellation remains challenging, particularly in achieving precise control at the supramolecular level. In this study, we present the successful creation of multiple seamless 2D tessellations on Au (111) surface using versatile hexagonal tiles derived from a singular molecular unit, namely 2,6,10-tribromotricycloquinazoline. Through scanning tunneling microscopy imaging, seven distinct 2D tessellations, ranging from regular to semiregular to k-uniform tilings, are unveiled at the molecular level. Density functional theory calculations provide a theoretical basis for the formation of these complex 2D tessellation, highlighting the important role of the variability of Br···Br/H contacts in facilitating complex seamless 2D tessellations on surface. This work opens avenues for exploring possibilities in constructing intricate tiling patterns with diverse applications.
Sluggish conversion reaction kinetics and spontaneous shuttle effect of lithium polysulfides (LiPSs) are deemed as the two big mountains that hinder the practical application of lithium-sulfur batteries (LSBs). Herein, dual-defect engineering strategy is implemented by introducing boron-doping and phosphorus-vacancy sites with MoP@NC composite as the precursor. Based on the experimental characterizations and theoretical calculations, B-MoP1-x@NC-based electrode presents low oxidation potential, high lithium diffusivity, small Tafel slope and strong adsorption capability for polysulfides, which is beneficial to enhance the adsorption capability for LiPSs, reduce the lithium diffusion energy barriers and Gibbs free energy for the conversion reactions of LiPSs. As demonstrated, the corresponding Li-S/B-MoP1-x@NC batteries can remain high reversible capacity of 753 mAh/g at 0.5 C after 300 cycles, and keep a stable capacity of 520 mAh/g at 0.5 C after 100 cycles even at the high-loading content of 5.1 mg/cm2. According to the results of in-situ UV–vis spectra, the satisfactory battery performance majorly originates from the existence of dual-defect characteristics in B-MoP1-x@NC catalyst, which effectively promotes the conversion reaction kinetics of LiPSs, and restrains the shuttle behavior of LiPSs. The key ideas of this work will enlighten the development of catalytic cathode materials for sulfur-based secondary batteries.
The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting. In this study, NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework (NiCo-MOF) as source of nickel and cobalt. Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO3. The prepared SrTiO3 loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting, achieving an apparent quantum yield of 11.9% at 350 ± 10 nm. Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni, reducing the free energy of H adsorption. The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability. This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.
Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants (ECs) from water, surpassing the limitations of traditional methods. Environmental functional materials (EFMs), particularly high-end oxidation systems using eco-friendly nanomaterials, show promise for absorbing and degrading ECs. This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological, physical, and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification. Through meticulous comparison, we unequivocally advocate for the imperative integration of environmentally benign nanomaterials, notably titanium-based variants, in forthcoming methodologies. Our in-depth exploration scrutinizes the catalytic efficacy, underlying mechanisms, and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts. Additionally, strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.
In the realm of drug discovery, recent advancements have paved the way for innovative approaches and methodologies. This comprehensive review encapsulates six distinct yet interrelated mini-reviews, each shedding light on novel strategies in drug development. (a) The resurgence of covalent drugs is highlighted, focusing on the targeted covalent inhibitors (TCIs) and their role in enhancing selectivity and affinity. (b) The potential of the quantum mechanics-based computational aid drug design (CADD) tool, Cov_DOX, is introduced for predicting protein-covalent ligand binding structures and affinities. (c) The scaffolding function of proteins is proposed as a new avenue for drug design, with a focus on modulating protein-protein interactions through small molecules and proteolysis targeting chimeras (PROTACs). (d) The concept of pro-PROTACs is explored as a promising strategy for cancer therapy, combining the principles of prodrugs and PROTACs to enhance specificity and reduce toxicity. (e) The design of prodrugs through carbon-carbon bond cleavage is discussed, offering a new perspective for the activation of drugs with limited modifiable functional groups. (f) The targeting of programmed cell death pathways in cancer therapies with small molecules is reviewed, emphasizing the induction of autophagy-dependent cell death, ferroptosis, and cuproptosis. These insights collectively contribute to a deeper understanding of the dynamic landscape of drug discovery.
The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology. Here, Candida rugosa lipase (CRL) was firstly adsorbed on the surface of magnetic zeolitic imidazolate framework-8 (ZIF-8) nanospheres, which was further encapsulated with a mesoporous SiO2 nano-membrane formed by tetraethyl orthosilicate (TEOS) polycondensation. Consequently, lipase could be firmly immobilized on carrier surface by physical binding rather than chemical binding, which did not damage the active conformation of enzyme. There were mesopores on the silica nano-membrane, which could improve the accessibility of enzyme and its apparent catalytic activity. Moreover, silica membrane encapsulation could also improve the stability of enzyme, suggesting an effective enzyme immobilization strategy. It showed that TEOS amount and the encapsulation time had significant effects on the thickness of silica membrane and the enzyme activity. The analysis in enzyme activity and protein secondary structure showed that lipase encapsulated in silica membrane retained the active conformation to the greatest extent. Compared with the adsorbed lipase, the encapsulated lipase increased its thermostability by 3 times and resistance to chemical denaturants by 7 times. The relative enzyme activity remained around 80% after 8 repetitions, while the adsorbed lipase only remained at 7.3%.
The extracellular vesicles show great potential as a noninvasive biomarker for the early detection of cancer. Hence, there is an urgent requirement to create biosensors that are time-saving, simple, and easily scalable in order to accomplish rapid, sensitive, and quantitative detection of extracellular vesicles. In this study, we present a self-propelled DNA walker powered by endonuclease Nt.BbvCI, which enables the development of a "signal on" sensing platform for the rapid and highly sensitive detection of extracellular vesicles. The DNA motor employed tracks made of streptavidin magnetic beads, which consisted of substrate strands labeled with fluorescein and motor strands locked by aptamers. The aptamer recognition of the target protein on extracellular vesicles unlocked the motor strand, initiating the DNA motor process. After replacing the optimal buffer solution containing the endonuclease Nt.BbvCI, the motor strands autonomously moved along the streptavidin magnetic beads track, continuously releasing fluorescent molecules and producing detectable fluorescence signals. Under optimal conditions, the detection range was from 2×104 particles/mL to 2×109 particles/mL, with a detection limit of 2.9×103 particles/mL, demonstrating excellent selectivity. This method has demonstrated good selectivity in different tumor-derived extracellular vesicles and performs well in complex biological samples. The ability to effectively analyze surface proteins of extracellular vesicles in a short period of time gives our DNA walker a tremendous potential for developing simple and cost-effective clinical diagnostic devices.
Dion–Jacobson (DJ) phase hybrid perovskites have been proven to improve the photovoltaic performance of the devices due to its unique structure. At present, some DJ hybrid perovskites have been reported and used for photodetection filed, but most of them are based on lead-bromide systems, which is not conducive to construct broadband photodetection devices due to the limitation of intrinsic absorption. Herein, we constructed a bilayered DJ hybrid perovskite (3AMPY)(EA)Pb2I7 (3AMPY2+ is 3-(aminomethyl)pyridinium, EA+ is ethylammonium) using an aromatic spacer, which exhibit large current on/off ratios of ~104 under 520 and 637 nm illumination. In particular, the single crystal device based on (3AMPY)(EA)Pb2I7 shows a distinguished detectivity of 7.4 × 1012 Jones and a high responsivity of 0.89 A/W under 637 nm illumination. Such finding not only enriches the quantities of DJ hybrid perovskites, but also provides useful assistance for constructing high-performance optoelectronic device in the future.
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