A biospecies-derived genomic DNA hybrid gel electrolyte for electrochemical energy storage.

Intrinsic impediments, namely weak mechanical strength, low ionic conductivity, low electrochemical performance, and stability have largely inhibited beyond practical applications of hydrogels in electronic devices and remains as a significant challenge in the scientific world. Here, we report a biospecies-derived genomic DNA hybrid gel electrolyte with many synergistic effects, including robust mechanical properties (mechanical strength and elongation of 6.98 MPa and 997.42%, respectively) and ion migration channels, which consequently demonstrated high ionic conductivity (73.27 mS/cm) and superior electrochemical stability (1.64 V). Notably, when applied to a supercapacitor the hybrid gel-based devices exhibit a specific capacitance of 425 F/g. Furthermore, it maintained rapid charging/discharging with a capacitance retention rate of 93.8% after ∼200,000 cycles while exhibiting a maximum energy density of 35.07 Wh/kg and a maximum power density of 193.9 kW/kg. This represents the best value among the current supercapacitors and can be immediately applied to minicars, solar cells, and LED lightning. The widespread use of DNA gel electrolytes will revolutionize human efforts to industrialize high-performance green energy.

Three-dimensional atrous inception module for crowd behavior classification.

Recent advances in deep learning have led to a surge in computer vision research, including the recognition and classification of human behavior in video data. However, most studies have focused on recognizing individual behaviors, whereas recognizing crowd behavior remains a complex problem because of the large number of interactions and similar behaviors among individuals or crowds in video surveillance systems. To solve this problem, we propose a three-dimensional atrous inception module (3D-AIM) network, which is a crowd behavior classification model that uses atrous convolution to explore interactions between individuals or crowds. The 3D-AIM network is a 3D convolutional neural network that can use receptive fields of various sizes to effectively identify specific features that determine crowd behavior. To further improve the accuracy of the 3D-AIM network, we introduced a new loss function called the separation loss function. This loss function focuses the 3D-AIM network more on the features that distinguish one type of crowd behavior from another, thereby enabling a more precise classification. Finally, we demonstrate that the proposed model outperforms existing human behavior classification models in terms of accurately classifying crowd behaviors. These results suggest that the 3D-AIM network with a separation loss function can be valuable for understanding complex crowd behavior in video surveillance systems.

Surfactant-Free, Size-Controllable, and Scalable Green Synthesis of ZIF-8 Particles with Narrow Size Distribution by Tuning Key Reaction Parameters in Water Solvent.

The chemical/physical properties and reliable performance of nanoporous materials are strongly influenced by the particle size and corresponding distribution. Among many types of MOFs, ZIF-8, is still widely used and many studies have been conducted to control the particle size and uniformity of ZIF-8 using surfactants and organic solvents. However, the use of surfactants and organic solvents process is expensive and may cause environmental pollution. For the first time, in this paper, a surfactant-free, size-controllable, and scalable green synthesis method of ZIF-8 particles is reported using four reaction parameters (temperature, concentration, pouring time, and reactant ratio) that affect the formation of nuclei and growth of ZIF-8 crystals. The as-synthesized ZIF-8 nanoparticles show great uniformity and controllable particle sizes in the wide range of 147-915 nm. In addition, a 2 L large-scale synthesis of ZIF-8 with narrow size distribution is developed by finely tuned particle size in water without any additives. To demonstrate the efficient utilization of nanopores according to the particle size and size distribution, an adsorption test is conducted on the ZIF-8 nanoparticles. This study will support the synthesis of size-controlled ZIF-8 with narrow size distribution and their composites for achieving high performance in the emerging applications.

Multiporous ZIF-8 carbon/cellulose composite beads: Highly efficient and scalable adsorbents for water treatment.

Metal-organic framework (MOF) particles are one of the most promising adsorbents for removing organic contaminants from wastewater. However, powder-type MOF particles face challenges in terms of utilization and recovery. In this study, a novel bead-type adsorbent was prepared using activated carbon based on the zeolitic imidazolate framework-8 (AC-ZIF-8) and a regenerated cellulose hydrogel for dye removal. AC-ZIF-8 particles with a large surface area were obtained by carbonization and chemical activation with KOH. The AC-ZIF-8 powders were efficiently immobilized in hydrophilic cellulose hydrogel beads via cellulose dissolution/regeneration. The prepared AC-ZIF-8/cellulose hydrogel (AC-ZIF-8/CH) composite beads exhibit a large specific surface area of 1412.8 m2/g and an excellent maximum adsorption capacity of 565.13 mg/g for Rhodamine B (RhB). Moreover, the AC-ZIF-8/CH beads were effective over a wide range of pH, temperatures and for different types of dyes. These composite beads also offer economic benefits through desorption of dyes for recycling. The AC-ZIF-8/CH beads can be produced in substantial amounts and used as fillers in a fixed-bed column system, which can purify the continuous inflow of dye solutions. These findings suggest that our simple approach for preparing high-performance adsorbent beads will broaden the application of dye adsorbents, oil-water separation, and catalysts.

The role of the North Atlantic Ocean on the increase in East Asia's spring extreme hot day occurrences across the early 2000s.

The occurrence frequency of East Asia's extreme hot day in boreal spring has increased since 1979. Using observational data and a Linear baroclinic model experiment, our study suggests that the occurrence of hot day is mainly due to anomalous high pressure over East Asia associated with a horizontal stationary wave train originating from a positive phase of the North Atlantic Tripole (NAT) sea surface temperature (SST) in spring. The effect of a positive phase of the NAT SST is evident in the 2000s, apparently associated with the linear trend of the North Atlantic SST like a positive phase of the NAT SST. Before 2000s, in contrast, SST forcing in the Indian Ocean and eastern tropical Pacific, which is associated with a negative phase of the NAT SST, may contribute to induce the East Asian hot days through atmospheric teleconnections. This implies that the relationship between a positive phase of the NAT SST and the occurrence of hot days in East Asia has been changed during the 2000s.

Arctic/North Atlantic atmospheric variability causes Severe PM10 events in South Korea.

Severe PM10 (particulate matter with a diameter of <10 µm) events in South Korea are known to be caused by stable atmospheric circulation conditions related to high-pressure anomalies in the upper troposphere. However, research on why these atmospheric circulation patterns occur is unknown. In this study, we propose new large-scale teleconnection pathways that cause severe PM10 events during the midwinter in South Korea. This study investigated instances of extremely high (EH)-PM10 in South Korea during mid-winter and examined the corresponding atmospheric teleconnection patterns to identify the factors contributing to EH-PM10 events. K-means clustering analysis revealed that EH-PM10 instances were associated with two large-scale teleconnection patterns. Cluster 1 exhibited a wave train pattern originating in the North Atlantic that developed from Eurasia to the Korean Peninsula. Cluster 2 was associated with a wave-like teleconnection pattern from the Barents-Kara Sea to the Korean Peninsula. The Rossby waves, triggered by the North Atlantic and the Arctic, propagated and weakened the surface pressure system. This led to a high-pressure anomaly over the Korean Peninsula, reducing atmospheric ventilation and causing a rapid increase in PM10 concentration within a few days. Furthermore, an experiment involving a linear baroclinic model established that atmospheric forcing in upstream regions has the potential to induce large-scale atmospheric teleconnection patterns, resulting in EH-PM10 cases in South Korea. These findings emphasize the ventilation effect and transport of PM10 concentrations modulated by two large-scale teleconnection patterns originating from the Arctic and North Atlantic, leading to EH-PM10 events in South Korea. Understanding this combined phenomenon may assist in the implementation of emission reduction measures based on the results of short-term forecasts of severe PM10 events.

Metal-organic framework-based high-performance column chip for micro gas chromatography: hybrid function for simultaneous preconcentration and separation of volatile organic compounds.

Numerous attempts have been made to replace commercial bulky gas chromatography (GC) systems with compact GC systems for monitoring volatile organic compounds in indoor air. However, recently developed compact GC systems are still too bulky in terms of user convenience, portability, and on-site analysis. Hence, an advanced miniaturization of compact GC systems is needed. Importantly, the small and high-performance gas pretreatment chip devices should be developed for compact GC systems. This paper reports the development of a metal-organic framework (MOF)-coated hybrid micro gas chromatography column chip (hybrid GC chip) capable of preconcentration and separation on harmful volatile organic compounds at low-concentration in one single chip device. The hybrid GC chip, 2 cm × 2 cm in size, was fabricated using a microelectromechanical systems process. The synthesized MOF-5 particles were coated on the inner wall of the fabricated hybrid GC chip and acted as an adsorbent and a stationary phase. The developed hybrid GC chip afforded high preconcentration factors with 1033-1237 and high separation resolutions with 3.8-13.3. The developed column showed good performance as a gas preconcentrator and separation column, and is the first device to perform both roles in one single chip device.

AI-driven robotic chemist for autonomous synthesis of organic molecules.

The automation of organic compound synthesis is pivotal for expediting the development of such compounds. In addition, enhancing development efficiency can be achieved by incorporating autonomous functions alongside automation. To achieve this, we developed an autonomous synthesis robot that harnesses the power of artificial intelligence (AI) and robotic technology to establish optimal synthetic recipes. Given a target molecule, our AI initially plans synthetic pathways and defines reaction conditions. It then iteratively refines these plans using feedback from the experimental robot, gradually optimizing the recipe. The system performance was validated by successfully determining synthetic recipes for three organic compounds, yielding that conversion rates that outperform existing references. Notably, this autonomous system is designed around batch reactors, making it accessible and valuable to chemists in standard laboratory settings, thereby streamlining research endeavors.

Spontaneous generation of singlet oxygen on microemulsion-derived manganese oxides with rich oxygen vacancies for efficient aerobic oxidation.

Developing innovative catalysts for efficiently activating O2 into singlet oxygen (1O2) is a cutting-edge field with the potential to revolutionize green chemical synthesis. Despite its potential, practical implementation remains a significant challenge. In this study, we design a series of nitrogen (N)-doped manganese oxides (Ny-MnO2, where y represents the molar amount of the N precursor used) nanocatalysts using compartmentalized-microemulsion crystallization followed by post-calcination. These nanocatalysts demonstrate the remarkable ability to directly produce 1O2 at room temperature without the external fields. By strategically incorporating defect engineering and interstitial N, the concentration of surface oxygen atoms (Os) in the vicinity of oxygen vacancy (Ov) reaches 51.1% for the N55-MnO2 nanocatalyst. This feature allows the nanocatalyst to expose a substantial number of Ov and interstitial N sites on the surface of N55-MnO2, facilitating effective chemisorption and activation of O2. Verified through electron paramagnetic resonance spectroscopy and reactive oxygen species trapping experiments, the spontaneous generation of 1O2, even in the absence of light, underscores its crucial role in aerobic oxidation. Density functional theory calculations reveal that an increased Ov content and N doping significantly reduce the adsorption energy, thereby promoting chemisorption and excitation of O2. Consequently, the optimized N55-MnO2 nanocatalyst enables room-temperature aerobic oxidation of alcohols with a yield surpassing 99%, representing a 6.7-fold activity enhancement compared to ε-MnO2 without N-doping. Furthermore, N55-MnO2 demonstrates exceptional recyclability for the aerobic oxidative conversion of benzyl alcohol over ten cycles. This study introduces an approach to spontaneously activate O2 for the green synthesis of fine chemicals.

Multiscale Porous Carbon Materials by In Situ Growth of Metal-Organic Framework in the Micro-Channel of Delignified Wood for High-Performance Water Purification.

Porous carbon materials are suitable as highly efficient adsorbents for the treatment of organic pollutants in wastewater. In this study, we developed multiscale porous and heteroatom (O, N)-doped activated carbon aerogels (CAs) based on mesoporous zeolitic imidazolate framework-8 (ZIF-8) nanocrystals and wood using 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidation, in situ synthesis, and carbonization/activation. The surface carboxyl groups in a TEMPO-oxidized wood (TW) can provide considerably large nucleation sites for ZIF-8. Consequently, ZIF-8, with excellent porosity, was successfully loaded into the TW via in situ growth to enhance the specific surface area and enable heteroatom doping. Thereafter, the ZIF-8-loaded TW was subjected to a direct carbonization/activation process, and the obtained activated CA, denoted as ZIF-8/TW-CA, exhibited a highly interconnected porous structure containing multiscale (micro, meso, and macro) pores. Additionally, the resultant ZIF-8/TW-CA exhibited a low density, high specific surface area, and excellent organic dye adsorption capacity of 56.0 mg cm-3, 785.8 m2 g-1, and 169.4 mg g-1, respectively. Given its sustainable, scalable, and low-cost wood platform, the proposed high-performance CA is expected to enable the substantial expansion of strategies for environmental protection, energy storage, and catalysis.

ProLonged Liposomal Delivery of TLR7/8 Agonist for Enhanced Cancer Vaccine.

Despite numerous studies on cancer treatment, cancer remains a challenging disease to cure, even after decades of research. In recent years, the cancer vaccine has emerged as a promising approach for cancer treatment, offering few unexpected side effects compared to existing therapies. However, the cancer vaccine faces obstacles to commercialization due to its low efficacy. Particularly, the Toll-like receptor (TLR) adjuvant system, specifically the TLR 7/8 agonist, has shown potential for activating Th1 immunity, which stimulates both innate and adaptive immune responses through T cells. In this study, we developed ProLNG-S, a cholesterol-conjugated form of resiquimod (R848), to enhance immune efficacy by stimulating the immune system and reducing toxicity. ProLNG-S was formulated as ProLNG-001, a positively charged liposome, and co-administered with ovalbumin (OVA) protein in the B16-OVA model. ProLNG-001 effectively targeted secondary lymphoid organs, resulting in a robust systemic anti-tumor immune response and tumor-specific T cell activation. Consequently, ProLNG-001 demonstrated potential for preventing tumor progression and improving survival compared to AS01 by enhancing anti-tumor immunity.

Spectral correction of light emitting diodes enables accurate hydration ratio calculation using narrowband diffuse reflectance spectroscopy.

Significance: Light emitting diodes (LEDs) are commonly utilized for tissue spectroscopy due to their small size, low cost, and simplicity. However, LEDs are often approximated as single-wavelength devices despite having relatively broad spectral bandwidths. When paired with photodiodes, the wavelength information of detected light cannot be resolved. This can result in errors during chromophore concentration calculations. These errors are particularly apparent when analyzing water and fat in the 900 to 1000 nm window where the spectral bandwidth of LEDs can encompass much of the analysis region, resulting in intense crosstalk. Aim: We utilize and present a spectral correction (SC) algorithm to correct for the spectral bandwidth of LEDs. We show the efficacy using a narrowband technique of spectrally broad and overlapping LEDs. Approach: Narrowband diffuse reflectance spectroscopy (nb-DRS), a technique capable of quantifying the hydration ratio (RH2O) of turbid media, was utilized. nb-DRS typically requires a broadband light source and spectrometer. We reduce the hardware to just five LEDs and a photodiode detector, relying on SC to compensate for spectral crosstalk. The effectiveness of our SC approach was tested in simulations as well as in an emulsion phantom and limited selection of human tissue. Results: In simulations, we show that calculated RH2O errors increased with the spectral bandwidth of LEDs but could be corrected using SC. Likewise, in emulsions, we found an average error of 8.7% (maximum error 14%) if SC was not used. By contrast, applying SC reduced the average error to 2.2% (maximum error of 6.4%). We show that despite utilizing multiple, spectrally broad, and overlapping LEDs, SC was still able to restore the performance of our narrowband method, making it comparable to a much larger full broadband system.

Composite polymer electrolytes with ionic liquid grafted-Laponite for dendrite-free all-solid-state lithium metal batteries.

Composite polymer electrolytes (CPEs) with high ionic conductivity and favorable electrolyte/electrode interfacial compatibility are promising alternatives to liquid electrolytes. However, severe parasitic reactions in the Li/electrolyte interface and the air-unstable inorganic fillers have hindered their industrial applications. Herein, surface-edge opposite charged Laponite (LAP) multilayer particles with high air stability were grafted with imidazole ionic liquid (IL-TFSI) to enhance the thermal, mechanical, and electrochemical performances of polyethylene oxide (PEO)-based CPEs. The electrostatic repulsion between multilayers of LAP-IL-TFSI enables them to be easily penetrated by PEO segments, resulting in a pronounced amorphous region in the PEO matrix. Therefore, the CPE-0.2LAP-IL-TFSI exhibits a high ionic conductivity of 1.5 × 10-3 S cm-1 and a high lithium-ion transference number of 0.53. Moreover, LAP-IL-TFSI ameliorates the chemistry of the solid electrolyte interphase, significantly suppressing the growth of lithium dendrites and extending the cycling life of symmetric Li cells to over 1000 h. As a result, the LiFePO4||CPE-0.2LAP-IL-TFSI||Li cell delivers an outstanding capacity retention of 80% after 500 cycles at 2C at 60 °C. CPE-LAP-IL-TFSI also shows good compatibility with high-voltage LiNi0.8Co0.1Mn0.1O2 cathodes.

Open-Mouthed Hollow Carbons: Systematic Studies as Cobalt- and Nitrogen-Doped Carbon Electrocatalysts for Oxygen Reduction Reaction.

Although hollow carbon structures have been extensively studied in recent years, their interior surfaces are not fully utilized due to the lack of fluent porous channels in the closed shell walls. This study presents a tailored design of open-mouthed particles hollow cobalt/nitrogen-doped carbon with mesoporous shells (OMH-Co/NC), which exhibits sufficient accessibility and electroactivity on both the inner and outer surfaces. By leveraging the self-conglobation effect of metal sulfate in methanol, a raspberry-structured Zn/Co-ZIF (R-Zn/Co-ZIF) precursor is obtained, which is further carbonized to fabricate the OMH-Co/NC. In-depth electrochemical investigations demonstrate that the introduction of open pores can enhance mass transfer and improve the utilization of the inner active sites. Benefiting from its unique structure, the resulting OMH-Co/NC exhibits exceptional electrocatalytic oxygen reduction performance, achieving a half-wave potential of 0.865 V and demonstrating excellent durability.

Hydrophobic, Sustainable, High-Barrier Regenerated Cellulose Film via a Simple One-Step Silylation Reaction.

With the increasing importance of environmental protection, high-performance biopolymer films have received considerable attention as effective alternatives to petroleum-based polymer films. In this study, we developed hydrophobic regenerated cellulose (RC) films with good barrier properties through a simple gas-solid reaction via the chemical vapor deposition of alkyltrichlorosilane. RC films were employed to construct a biodegradable, free-standing substrate matrix, and methyltrichlorosilane (MTS) was used as a hydrophobic coating material to control the wettability and improve the barrier properties of the final films. MTS readily coupled with hydroxyl groups on the RC surface through a condensation reaction. We demonstrated that the MTS-modified RC (MTS/RC) films were optically transparent, mechanically strong, and hydrophobic. In particular, the obtained MTS/RC films exhibited a low oxygen transmission rate of 3 cm3/m2 per day and a low water vapor transmission rate of 41 g/m2 per day, which are superior to those of other hydrophobic biopolymer films.