Matrix Manipulation of Directly-Synthesized PbS Quantum Dot Inks Enabled by Coordination Engineering

The direct-synthesis of conductive PbS quantum dot (QD) ink is facile, scalable, and low-cost, boosting the future commercialization of optoelectronics based on colloidal QDs. However, manipulating the QD matrix structures still is a challenge, which limits the corresponding QD solar cell performance. Here, for the first time a coordination-engineering strategy to finely adjust the matrix thickness around the QDs is presented, in which halogen salts are introduced into the reaction to convert the excessive insulating lead iodide into soluble iodoplumbate species. As a result, the obtained QD film exhibits shrunk insulating shells, leading to higher charge carrier transport and superior surface passivation compared to the control devices. A significantly improved power-conversion efficiency from 10.52% to 12.12% can be achieved after the matrix engineering. Therefore, the work shows high significance in promoting the practical application of directly synthesized PbS QD inks in large-area low-cost optoelectronic devices.     

Water vapor volatilization and oxidation induced surface cracking of environmental barrier coating systems: A numerical approach

A numerical model is developed for surface crack propagation in brittle ceramic coatings, aiming at the intrinsic failure of rare-earth silicate environmental barrier coating systems (EBCs) under combustion conditions in advanced gas turbines. The main features of progressive degradation of EBCs in such conditions are captured, including selective silica vaporization in the top coat due to exposure to water vapor, diffusion path-dependent bond coat oxidation, as well as crack propagation during cyclic thermal loading. In light of these features, user-defined subroutines are implemented in finite element analysis, where surface crack growth is simulated by node separation. Numerical results are validated by existing experimental data, in terms of monosilicate layer thickening, thermal oxide growth, and fracture behaviors. The experimentally observed quasi-linear oxidation in the early stage is also elucidated. Furthermore, it is suggested that surface crack undergoes rapid propagation in the late stage of extended thermal cycling in water vapor and leads to catastrophic failure, driven by both thermal mismatch and oxide growth stresses. The latter is identified as the dominant mechanism of penetration. Based on detailed analyses of failure mechanisms, the optimization strategy of EBCs composition is proposed, balancing the trade-off between mechanical compliance and erosion resistance.     

Nitrate Additives Coordinated with Crown Ether Stabilize Lithium Metal Anodes in Carbonate Electrolyte

Lithium metal anodes (LMAs) are promising for next-generation batteries but have poor compatibility with the widely used carbonate-based electrolytes, which is a major reason for their severe dendrite growth and low Coulombic efficiency (CE). A nitrate additive to the electrolyte is an effective solution, but its low solubility in carbonates is a problem that can be solved using a crown ether, as reported. A rubidium nitrate additive coordinated with 18-crown-6 crown ether stabilizes the LMA in a carbonate electrolyte. The coordination promotes the dissolution of NO₃⁻ ions and helps form a dense solid electrolyte interface that is Li₃N-rich which guides uniform Li deposition. In addition, the Rb (18-crown-6)⁺ complexes are adsorbed on the dendrite tips, shielding them from Li deposition on the dendrite tips. A high CE of 97.1% is achieved with a capacity of 1 mAh cm⁻² in a half cell, much higher than when using the additive-free electrolyte (92.2%). Such an additive is very compatible with a nickel-rich ternary cathode at a high voltage, and the assembled full battery with a cathode material loading up to 10 mg cm⁻² shows an average CE of 99.8% over 200 cycles, indicating a potential for practical use.     

Bioinspired Supramolecular Slippery Organogels for Controlling Pathogen Spread by Respiratory Droplets

Surface-deposited pathogens are sources for the spread of infectious diseases. Protecting public facilities with a replaceable or recyclable antifouling coating is a promising approach to control pathogen transmission. However, most antifouling coatings are less effective in preventing pathogen-contained respiratory droplets because these tiny droplets are difficult to repel, and the deposited pathogens can remain viable from hours to days. Inspired by mucus, an antimicrobial supramolecular organogel for the control of microdroplet-mediated pathogen spread is developed. The developed organogel coating harvests a couple of unique features including localized molecular control-release, readily damage healing, and persistent fouling-release properties, which are preferential for antifouling coating. Microdroplets deposited on the organogel surfaces will be spontaneously wrapped with a thin liquid layer, and will therefore be disinfected rapidly due to a mechanism of spatially enhanced release of bactericidal molecules. Furthermore, the persistent fouling-release and damage-healing properties will significantly extend the life-span of the coating, making it promising for diverse applications.     

一种关于旅行商问题适用范围的优化方法

针对旅行商问题适用范围存在的局限性,结合实际的仓库拣货作业优化实例开展研究.考虑仓库内各货位点之间的相对位置关系以及拣货员可能行走的路线,设计出关于拣货员行走路线的分类算法;提出虚拟点的概念来解决旅行商问题求解时起点、终点不一致的问题;利用虚拟点,根据任务单要求找出拣货员所有的最优位置访问顺序;比较每一种情况,得到拣货员的最优路径,以实现缩短拣货总时间、减少人力和物力的总目标,较好地提高拣货效率.     

Effects of four multi-compound freezing medium on the quality of red drum (Sciaenops ocellatus) during frozen storage

Taking air freezing (AF) as the reference, the effects of four types of multi-compound freezing medium for cryogenic liquid quick-freezing (immersion freezing, IF) on the freezing rate, quality and myofibrillar protein (MP) denaturation of red drum (Sciaenops ocellatus) fillets during frozen storage (−18°C) from days 0 to 90 were studied. Samples were gathered on days 0, 15, 30, 45, 60 and 90 for analysis. The results showed that IF groups (IF-1: 20% ethanol, 30% propylene glycol, 10% sodium chloride aqueous solution; IF-2: 20% ethanol, 20% propylene glycol, 10% glycerol, 10% sodium chloride aqueous solution; IF-3: 20% ethanol, 20% propylene glycol, 10% polyethylene glycol, 10% sodium chloride aqueous solution; IF-4: 20% ethanol, 20% propylene glycol, 5% glycerol, 5% polyethylene glycol, 10% sodium chloride aqueous solution) significantly shortened the time to cross the formation zone of maximum ice crystals while the freezing rate was 6.13 times higher than the AF group after adding 30% propylene glycol as the freezing medium. Furthermore, compared with the AF group, the IF groups significantly reduced losses in the water-holding capacity, the myofibrillar fragmentation index, microstructure damage, texture characteristics, drip loss and water migration (P < 0.05). In addition, the MP of IF groups had higher maximum transition temperatures (T_max1 and T_max2), total sulfhydryl content, Ca²⁺-ATPase activity and relative α-helix content compared with the AF group. In conclusion, IF could significantly increase the freezing rate of red drum fillets, and slow down quality deterioration and denaturation of MP during frozen storage for 90 days (−18°C). In particular, IF-2 (20% ethanol, 20% propylene glycol, 10% glycerol, 10% sodium chloride aqueous solution) was found to be more suitable for the immersion freezing of marine fish among the four multi-compound freezing medium.     

Surface Reconstruction Engineering with Synergistic Effect of Mixed-Salt Passivation Treatment toward Efficient and Stable Perovskite Solar Cells

Surface passivation treatment is a widely used strategy to resolve trap-mediated nonradiative recombination toward high-efficiency metal-halide perovskite photovoltaics. However, a lack of passivation with mixture treatment has been investigated, as well as an in-depth understanding of its passivation mechanism. Here, a systematic study on a mixed-salt passivation strategy of formamidinium bromide (FABr) coupled with different F-substituted alkyl lengths of ammonium iodide is demonstrated. It is obtained better device performance with decreasing chain length of the F-substituted alkyl ammonium iodide in the presence of FABr. Moreover, they unraveled a synergistic passivation mechanism of the mixed-salt treatment through surface reconstruction engineering, where FABr dominates the reformation of the perovskite surface via reacting with the excess PbI₂. Meanwhile, ammonium iodide passivates the perovskite grain boundaries both on the surface and top perovskite bulk through penetration. This synergistic passivation engineer results in a high-quality perovskite surface with fewer defects and suppressed ion migration, leading to a champion efficiency of 23.5% with mixed-salt treatment. In addition, the introduction of the moisture resisted F-substituted groups presents a more hydrophobic perovskite surface, thus enabling the decorated devices with excellent long-term stability under a high humid atmosphere as well as operational conditions.     

Oxidation State Modulation of Bismuth for Efficient Electrocatalytic Nitrogen Reduction to Ammonia

Electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy for ammonia (NH₃) production under ambient conditions. However, it is severely impeded by the challenging activation of the NN bond and the competing hydrogen evolution reaction (HER), which makes it crucial to design electrocatalysts rationally for efficient NRR. Herein, the rational design of bismuth (Bi) nanoparticles with different oxidation states embedded in carbon nanosheets (Bi@C) as efficient NRR electrocatalysts is reported. The NRR performance of Bi@C improves with the increase of Bi⁰/Bi³⁺ atomic ratios, indicating that the oxidation state of Bi plays a significant role in electrochemical ammonia synthesis. As a result, the Bi@C nanosheets annealed at 900  ° C with the optimal oxidation state of Bi demonstrate the best NRR performance with a high NH₃ yield rate and remarkable Faradaic efficiency of 15.10  ± 0.43% at − 0.4 V versus RHE. Density functional theory calculations reveal that the effective modulation of the oxidation state of Bi can tune the p-filling of active Bi sites and strengthen adsorption of *NNH, which boost the potential-determining step and facilitate the electrocatalytic NRR under ambient conditions. This work may offer valuable insights into the rational material design by modulating oxidation states for efficient electrocatalysis.     

Magnetic porous nano-carbon catalysts supported silver nanoparticles derived from chitin and their application in catalytic reduction reactions

The exploitation of recycled carbonaceous catalysts from renewable biomass resources such as chitin is a crucial issue for the development of the sustainable society. In this article, the chitin-based N and O doped carbon microspheres (ChC) were fabricated by a simple dissolution, sol–gel transformation, and the carbonization methods. Subsequently, the novel magnetic Ag-Fe₃O₄@chitin-based carbon microspheres catalyst (MChC) was successfully constructed through the in situ redox reaction. The as-prepared MChC possessed rich micropores with high-surface area, and a narrow size distribution (50–120 μm). The Ag-Fe₃O₄ nanoparticles were immobilized through the interaction with C, N, and O atoms in the pores of MChC. The reduction of 4-nitrophenol was applied to evaluate the catalytic activity of MChC. 4-Nitrophenol (4-NP) could be fully reduced to 4-aminophenol (4-AP) in 5 min with the catalyst MChC-45. Moreover, MChC could be collected in solution with an external magnet in 8 s and remained relatively high-catalytic activity after 10 cycle times. This work provided novel ideas for the fabrication of doped carbon material from biomass and promoted its utilization in nanocatalytic applications.