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The crystallization and growth of perovskite crystals are two crucial factors influencing the performance of perovskite solar cells (PSCs). Moreover, iodoplumbate complexes such as PbI 2 , PbI 3 - , and PbI 4 2- in perovskite precursor solution dictate both the quality of perovskite crystals and the optoelectrical performance of PSCs. Here, we propose an iodoplumbate-coordination strategy that employs pentafluorophenylsulfonyl chloride (PTFC) as an additive to tailor the crystal quality. This strategy directly affects the thermodynamics and kinetics of perovskite crystal formation by regulating hydrogen bonds or coordination bonds with Pb 2+ or I - ions. Subsequently, the synergistic effect of the PTFC and FA + complex was beneficial for intermediate-to-perovskite phase transition, improving the crystalline quality and reducing the defect density in the perovskite film to suppress nonradiative recombination loss. Consequently, the treated PSCs achieved a power conversion efficiency (PCE) of 24.61%, demonstrating enhanced long-term stability under both light and thermal stress. The developed device retained 92.53% of its initial PCE after 1200 h of continuous illumination and 88.6% of its initial PCE after 600 h of 85 °C thermal stability tests, respectively, both conducted in N 2 atmospheres.

Cyclic voltammetry pretreatment of Pt-based electrocatalysts has been proven to be a normal activation process on achieving the optimal alkaline hydrogen evolution performance. Until now, the congruent relationship between the microstructural evolution and performance improvement during this process has rarely been reported. Herein, when the in situ transmission electron microscopy and in situ Raman analyses are employed, a self-reconstruction process from crystalline NiS into amorphous nickel hydroxide hydrate [Ni(OH) 2- x ·H 2 O, where x ≈ 0.3] on the surface of platinum-nickel nanowires has first been captured, which is the critical water dissociation active site to offer a sufficient proton supply. Furthermore, such a surficial reconstruction triggers an increase in the current density from -2.3 to -38.8 mA/cm 2 (at -70 mV), which is nearly 17 times. These observations point to the fact that it is essential to consider the fundamental mechanisms of hydrogen evolution on the active sites when the process is scaled up.

Pulp and periapical diseases can lead to the cessation of tooth development, resulting in compromised tooth structure and functions. Despite numerous efforts to induce pulp regeneration, effective strategies are still lacking. Growth factors (GFs) hold considerable promise in pulp regeneration due to their diverse cellular regulatory properties. However, the limited half-lives and susceptibility to degradation of exogenous GFs necessitate the administration of supra-physiological doses, leading to undesirable side effects. In this research, a heparin-functionalized bioactive glass (CaO-P 2 O 5 -SiO 2 -Heparin, abbreviated as PSC-Heparin) with strong bioactivity and a stable neutral pH is developed as a promising candidate to addressing challenges in pulp regeneration. Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis reveal the successful synthesis of PSC-Heparin. Scanning electron microscopy and X-ray diffraction show the hydroxyapatite formation can be observed on the surface of PSC-Heparin after soaking in simulated body fluid for 12 h. PSC-Heparin is capable of harvesting various endogenous GFs and sustainably releasing them over an extended duration by the enzyme-linked immunosorbent assay. Cytological experiments show that developed PSC-Heparin can facilitate the adhesion, migration, proliferation, and odontogenic differentiation of stem cells from apical papillae. Notably, the histological analysis of subcutaneous implantation in nude mice demonstrates PSC-Heparin is capable of promoting the odontoblast-like layers and pulp-dentin complex formation without the addition of exogenous GFs, which is vital for clinical applications. This work highlights an effective strategy of harvesting endogenous GFs and avoiding the involvement of exogenous GFs to achieve pulp-dentin complex regeneration, which may open a new horizon for regenerative endodontic therapy.

Osteoarthritis (OA) progression is highly associated with chondrocyte mitochondrial dysfunction and disorders of catabolism and anabolism of the extracellular matrix (ECM) in the articular cartilage. The mitochondrial unfolded protein response (UPR mt ), which is an integral component of the mitochondrial quality control (MQC) system, is essential for maintaining chondrocyte homeostasis. We successfully validated the pivotal role of activating transcription factor 5 (ATF5) in upregulating the UPR mt , mitigating IL-1β-induced inflammation and mitochondrial dysfunction, and promoting balanced metabolism in articular cartilage ECM, proving its potential as a promising therapeutic target for OA. Modified mRNAs (modRNAs) have emerged as novel and efficient gene delivery vectors for nucleic acid therapeutic approaches. In this study, we combined Atf5-modRNA (modAtf5) with engineered exosomes derived from bone mesenchymal stem cells (Ex modAtf5 ) to exert cytoprotective effects on chondrocytes in articular cartilage via Atf5. However, the rapid localized metabolization of Ex modAtf5 limits its application. PLGA-PEG-PLGA (Gel), an injectable thermosensitive hydrogel, was used as a carrier of Ex modAtf5 (Gel@Ex modAtf5 ) to achieve a sustained release of Ex modAtf5 . In vitro and in vivo , the use of Gel@Ex modAtf5 was shown to be a highly effective strategy for OA treatment. The in vivo therapeutic effect of Gel@Ex modAtf5 was evidenced by the preservation of the intact cartilage surface, low OARSI scores, fewer osteophytes, and mild subchondral bone sclerosis and cystic degeneration. Consequently, the combination of Ex modAtf5 and PLGA-PEG-PLGA could significantly enhance the therapeutic efficacy and prolong the exosome release. In addition, the mitochondrial protease ClpP enhanced chondrocyte autophagy by modulating the mTOR/Ulk1 pathway. As a result of our research, Gel@Ex modAtf5 can be considered to be effective at alleviating the progression of OA.

Porous carbons have shown their potential in sodium-ion batteries (SIBs), but the undesirable initial Coulombic efficiency (ICE) and rate capability hinder their practical application. Herein, learning from nature, we report an efficient method for fabricating a carbon framework (CK) with delicate porous structural regulation by biomimetic mineralization-assisted self-activation. The abundant pores and defects of the CK anode can improve the ICE and rate performance of SIBs in ether-based electrolytes, whereas they are confined in carbonate ester-based electrolytes. Notably, ether-based electrolytes enable CK anode to possess excellent ICE (82.9%) and high-rate capability (111.2 mAh g -1 at 50 A g -1 ). Even after 5500 cycles at a large current density of 10 A g -1 , the capacity retention can still be maintained at 73.1%. More importantly, the full cell consisting of the CK anode and Na 3 V 2 (PO 4 ) 3 cathode delivers a high energy density of 204.4 Wh kg -1 , with a power density of 2828.2 W kg -1 . Such outstanding performance of the CK anode is attributed to (1) hierarchical pores, oxygen doping, and defects that pave the way for the transportation and storage of Na + , further enhancing ICE; (2) a high-proportion NaF-based solid-electrolyte-interphase (SEI) layer that facilitates Na + storage kinetics in ether-based electrolytes; and (3) ether-based electrolytes that determine Na + storage kinetics further to dominate the performance of SIBs. These results provide compelling evidence for the promising potential of our synthetic strategy in the development of carbon-based materials and ether-based electrolytes for electrochemical energy storage.

In the field of sustainable chemistry, it is still a significant challenge to realize efficient light-powered space-confined catalysis and propulsion due to the limited solar absorption efficiency and the low mass and heat transfer efficiency. Here, novel semiconductor TiO 2 nanorockets with asymmetric, hollow, mesoporous, and double-layer structures are successfully constructed through a facile interfacial superassembly strategy. The high concentration of defects and unique topological features improve light scattering and reduce the distance for charge migration and directed charge separation, resulting in enhanced light harvesting in the confined nanospace and resulting in enhanced catalysis and self-propulsion. The movement velocity of double-layered nanorockets can reach up to 10.5 μm s -1 under visible light, which is approximately 57 and 119% higher than that of asymmetric single-layered TiO 2 and isotropic hollow TiO 2 nanospheres, respectively. In addition, the double-layered nanorockets improve the degradation rate of the common pollutant methylene blue under sustainable visible light with a 247% rise of first-order rate constant compared to isotropic hollow TiO 2 nanospheres. Furthermore, FEA simulations reveal and confirm the double-layered confined-space enhanced catalysis and self-propulsion mechanism.

Lactic acid (LA) is an important downstream product of glycolysis in living cells and is abundant in our body fluids, which are strongly associated with diseases. The development of enzyme-free LA sensors with high sensitivity and low consumption remains a challenge. 2D metal-organic frameworks (MOFs) are considered to be promising electrochemical sensing materials and have attracted much attention in recent years. Compared to monometallic MOFs, the construction of bimetallic MOFs (BMOFs) can obtain a larger specific surface area, thereby increasing the exposed active site. 3D petal-like Ni x Co y MOF films on nickel foams (Ni x Co y BMOF@Ni foams) are successfully prepared by combining atomic layer deposition-assisted technology and hydrothermal strategy. The established Ni x Co y BMOF@Ni foams demonstrate noticeable LA sensing activity, and the study is carried out on behalf of the Ni 1 Co 5 BMOF@Ni foam, which has a sensitivity of up to 9030 μA mM -1 cm -2 with a linear range of 0.01-2.2 mM and the detection limit is as low as 0.16 μM. Additionally, the composite has excellent stability and repeatability for the detection of LA under a natural air environment with high accuracy and reliability. Density functional theory calculation is applied to study the reaction process between composites and LA, and the result suggests that the active site in the NiCo BMOF film favors the adsorption of LA relative to the active site of monometallic MOF film, resulting in improved performance. The developed composite has a great potential for the application of noninvasive LA biosensors.

Organic dye-based agents with near-infrared (NIR)-II absorption have great potential for cancer theranostics because of the deeper tissue penetration and good biocompatibility. However, proper design is required to develop NIR-II-absorbing dyes with good optical properties. We proposed to construct chalcogen atom-modulated croconaine for NIR-II light-triggered photothermal theranostics. By introducing different chalcogen atoms (O, S, Se, or Te) into the structure of croconaine, the light absorption of croconaine can be precisely regulated from the NIR-I to the NIR-II range due to the heavy-atom effect. Especially, Te-substituted croconaine (CRTe) and its nanoformulations exhibit superior NIR-II responsiveness, a high photothermal conversion efficiency (70.6%), and good photostability. With their favorable tumor accumulation, CRTe-NPs from tumor regions can be visualized by NIR-II optoacoustic systems with high resolution and high contrast; meanwhile, their superior photothermal performance also contributes to efficient cell killing and tumor elimination upon 1064 nm laser irradiation. Therefore, this work provides an efficient strategy for the molecular design of NIR-II organic photothermal agents.

With the rapid development of information technology, the encrypted storage of information is becoming increasingly important for human life. The luminescent materials with a color-changed response under physical or chemical stimuli are crucial for information coding and anticounterfeiting. However, traditional fluorescent materials usually face problems such as a lack of tunable fluorescence, insufficient surface-adaptive adhesion, and strict synthesis conditions, hindering their practical applications. Herein, a series of luminescent lanthanide hybrid organogels (Ln-MOGs) were rapidly synthesized using a simple method at room temperature through the coordination between lanthanide ions and 2,6-pyridinedicarboxylic acid and 5-aminoisophthalic acid. And the multicolor fluorescent inks were also prepared based on the Ln-MOG and hyaluronic acid, with the advantages of being easy to write, color-adjustable, and water-responsive discoloration, which has been applied to paper-based anticounterfeiting technology. Inspired by the responsiveness of the fluorescent inks to water, we designed a logic system that can realize single-input logic operations (NOT and PASS1) and double-input logic operations (NAND, AND, OR, NOR, XOR). The encryption of a binary code can be actualized utilizing different luminescent response modes based on the logic circuit system. By adjusting the energy sensitization and luminescence mechanism of lanthanide ions in the gel structure, the information reading and writing ability of the fluorescent inks were verified, which has great potential in the field of multicolor pattern anticounterfeiting and information encryption.

Much progress has been made toward the development of wearable flexible strain sensors with high sensing performance to monitor human motion, but continuous function in harsh aqueous environments remains a significant challenge. A promising strategy has been the design of sensors with highly durable superhydrophobicity and maintenance of unique sensing properties. Herein, an extremely durable superhydrophobic strain sensor with an ultrawide sensing range was simply fabricated by directly brushing conductive carbon black nanoparticles (CBNPs) onto an elastic silicone rubber sheet (SS) with poly(dimethylsiloxane) (PDMS) coatings (i.e., SS/PDMS-CBNPs sensors). First, this method avoided the use of toxic solvents and a conventional prestretching treatment. Second, considering the easily destroyed rough structures and surface chemistry for conventional superhydrophobic sensors during practical applications, the prepared SS/PDMS-CBNP sensors showed excellent mechanical durability of both superhydrophobicity and sensing as examined by harsh abrasion (300 cycles), stretching (up to 200%), and ultrasonication (40 min) treatments. Third, the prepared superhydrophobic strain sensor exhibited high sensitivity (gauge factor of 101.75), high stretchability (0.015-460%), low hysteresis (83 ms), and long-term stability (10000 cycles). Fourth, the high biocompatibility of the SS/PDMS-CBNP sensor was demonstrated by rabbit skin irritation tests. Finally, the remarkable water-repellent and sensing properties of the SS/PDMS-CBNP sensor allowed its application to monitor a swimmer's real-time situation and send distress signals when needed.

Intelligent DNA nanomachines are powerful and versatile molecular tools for bioimaging and biodiagnostic applications; however, they are generally constrained by complicated synthetic processes and poor reaction efficiencies. In this study, we developed a simple and efficient molecular machine by coupling a self-powered rolling motor with a lipidic nanoflare (termed RMNF), enabling high-contrast, robust, and rapid probing of cancer-associated microRNA (miRNA) in serum and living cells. The lipidic nanoflare is a cholesterol-based lipidic micelle decorated with hairpin-shaped tracks that can be facilely synthesized by stirring in buffered solution, whereas the 3D rolling motor (3D RM) is a rigidified tetrahedral DNA scaffold equipped with four single-stranded "legs" each silenced by a locking strand. Once exposed to the target miRNA, the 3D RM can be activated, followed by self-powered precession based on catalyzed hairpin assembly (CHA) and lighting up of the lipidic nanoflare. Notably, the multivalent 3D RM that moves using four DNA legs, which allows the motor to continuously and acceleratedly interreact with DNA tracks rather than dissociate from the surface of the nanoflare, yielded a limit of detection (LOD) of 500 fM at 37 °C within 1.5 h. Through the nick-hidden and rigidified structure design, RMNF exhibits high biostability and a low false-positive signal under complex physiological settings. The final application of RMNF for miRNA detection in clinical samples and living cells demonstrates its considerable potential for biomedical imaging and clinical diagnosis.

Room-temperature phosphorescent (RTP) liquid crystal materials have garnered considerable attention because of their significant applications in organic light emitting diodes, polarized light emitting materials, and so forth. How to efficiently synthesize pure organic RTP liquid crystals and regulate their performance is of great significance. In this article, we propose a simple and feasible method to synthesize RTP liquid crystals and manipulate their properties through copolymerization. We constructed RTP liquid crystal copolymers by copolymerizing a phosphorescent monomer bearing biphenyl mesogen with a phosphorescent monomer bearing a dibenzofuran chromophore. All the synthesized copolymers show a liquid crystal property because of the introduction of biphenyl mesogen. Meanwhile, by changing the composition of copolymers, it is possible to regulate their RTP performance, including luminescence color and lifetime. As the content of the PMDFM0C component in copolymers increases, the phosphorescence lifetime gradually increases. For poly(MDFM0C(0.46)- co -MBi18C(0.54)), the phosphorescence lifetime can reach 463.0 ms. Moreover, the phosphorescence color of the PMDFM0C component in copolymers changes with the copolymer composition, which can induce variable room-temperature phosphorescence. In addition, when oriented, liquid crystal copolymer films can emit linearly polarized fluorescence and linearly polarized phosphorescence. The linearly polarized phosphorescence dichroic ratio and polarization ratio values of the oriented poly(MDFM0C(0.46)- co -MBi18C(0.54)) film are 3.33 and 0.50, respectively.

Magnesium-ion batteries (MIBs) have great potential in large-scale energy storage field with high capacity, excellent safety, and low cost. However, the strong solvation effect of Mg 2+ will lead to the formation of solvated ions in electrolytes with larger size and sluggish diffusion/reaction kinetics. Here, the concept of interfacial catalytic bond breaking is first introduced into the cathode design of MIBs by hybriding MoS 2 quantum dots with VS 4 (VS 4 @MQDs) as the cathode. The "in situ dynamic catalysis and re-equilibration" effects can catalyze the Cl-Mg bond breaking and trigger single Mg 2+ insertion/extraction chemistries, which can significantly accelerate the diffusion and reaction kinetics, as verified by the decreased diffusion energy barriers (0.26 eV for Mg 2+ vs 2.47 eV for MgCl + ) and fast diffusion coefficient. Benefitting from these dynamic catalysis effects, the constructed VS 4 @MQD-based MIBs deliver a high discharge capacity of ∼120 mA h g -1 at 200 mA g -1 and a long-term cyclic stability of 1000 cycles at 1 A g -1 . The improved performance and detailed characterizations well prove that the active ions in MIBs change from MgCl + /Mg 2 Cl 3+ to Mg 2+ with fast kinetics.

In wireless communication systems, a multibeam can be used to increase the number of spatial channels by space-division multiplexing. Furthermore, the multimode is used to enhance the channel capacity by mode-division multiplexing. However, few of the previously reported methods cannot achieve independent controls of orbital angular momentum (OAM) states by transmissive metasurfaces in both space-division and mode-division multiplexing simultaneously. To expand the wireless communication channel, a multilayer transmissive digital coding metasurface with a single emitting source is demonstrated for quad-OAM beam generation with a dual mode. By changing the geometry of the cross dipole for a unit cell, the polarization-dependent 3-bit phase responses are obtained to flexibly manipulate the multi-OAM beams with different modes in preset directions simultaneously. Two types of metasurfaces are designed and fabricated to realize four OAM beams with two topological charges in different directions by encoding the phase sequence in x - and y -directions, which is validated by both theoretical analyses and experimental results. This scheme of transmissive digital coding metasurface provides a simple way to the multiplexing, multichannel, and multiplatform communication and imaging systems.

Polyurethane (PU) is a widely used polymer material that will age under prolonged exposure to ultraviolet (UV) light, shortening the service life. Several methods have been used to prepare the anti-UV PU, including adding nonreactive anti-UV additives, functional fillers, and biological antioxidant molecules. However, the nonreactive anti-UV additives may migrate during long-term use, the functional fillers may damage the mechanical properties and seriously reduce the light transmittance of the sample, and the biological antioxidant molecules will inevitably color the sample. To solve these problems, in this work, a benzotriazole UV absorber (Chiguard R-455) was introduced into the PU molecular chains by in situ polymerization to prepare the nonmigrating intrinsic anti-UV PU sample with high performance and colorless transparency. The anti-UV PU samples exhibit light transmittance of over 88% in the visible range and superior mechanical properties with tensile strength higher than 65 MPa and elongation at break higher than 900%. After 24 h UV irradiation (200 W, 365 nm), the tensile strength and elongation at break of pure PU sample are significantly reduced to only 8.9 and 15.8% of the original one, respectively. On the contrary, the addition of Chiguard R-455 will endow the PU sample with excellent anti-UV performance. After 24 h UV irradiation, the tensile strength (67.2 ± 1.6 MPa) and elongation at break (917.4 ± 30.0%) of PU-0.5% (the content of Chiguard R-455 is only 0.5 wt %) have changed little compared with the sample without irradiation (67.4 ± 3.5 MPa and 919.4 ± 26.5%). Additionally, the anti-UV mechanism of the PU sample is systematically studied. This work provides a feasible method for preparing colorless, transparent, high-performance, nonmigrating intrinsic UV-shielding PU samples, which can be used as a UV light-shielding material in various fields with visible and aesthetic requirements, such as protection fields and wearable products.

Transarterial radioembolization (TARE) is a local radionuclide therapy and is successfully used in hepatocellular carcinoma (HCC) treatment. Radioactive microspheres have been widely studied for TARE. Preparation of ideal radioactive microspheres is significant for clinical research and patient treatment. In this study, we have designed a novel multifunctional microsphere, i.e., polydopamine (PDA)-coated 177 Lu-radiolabeled silica microspheres (MS) denoted as 177 Lu-MS@PDA, which can be used for TARE and photothermal therapy (PTT). The radiostability of 177 Lu-MS@PDA was significantly improved by coating 177 Lu-MS with PDA. In addition, the coating of PDA makes microspheres have excellent photothermal performance. MicroSPECT/CT images showed that 177 Lu-MS@PDA was accurately embolized and remained in the tumor during the observation time. At the time, it also showed that 177 Lu-MS@PDA was very stable in vivo. Furthermore, the anti-tumor results demonstrated that TARE combined with PTT of 177 Lu-MS@PDA can significantly inhibit tumor growth without obvious side effects. 177 Lu-MS@PDA holds great potential as a promising radioactive microsphere for HCC.

Ever-evolving advancements in films have fueled many of the developments in the field of electrochemical sensors. For biosensor application platforms, the fabrication of metal-organic framework (MOF) films on microscopically structured substrates is of tremendous importance. However, fabrication of MOF film-based electrodes always exhibits unsatisfactory performance, and the mechanisms of the fabrication and sensing application of the corresponding composites also need to be explored. Here, we report the fabrication of conformal MIL-53 (Fe) films on carbonized natural seaweed with the assistance of an oxide nanomembrane and a potential-dependent electrochemical dopamine (DA) sensor. The geometry and structure of the composite can be conveniently tuned by the experimental parameters, while the sensing performance is significantly influenced by the applied potential. The obtained sensor demonstrates ultrahigh sensitivity, a wide linear range, a low limit of detection, and a good distinction between DA and ascorbic acid at an optimized potential of 0.3 V. The underneath mechanism is investigated in detail with the help of theoretical calculations. This work bridges the natural material and MOF films and is promising for future biosensing applications.

Integration of extended gate field-effect transistors (EGFET) and photoelectrochemical (PEC) measurement to construct highly sensitive sensors is an innovative research field that was proven feasible by our previous work. However, it remains a challenge on how to adjust the interaction between the extended gate and the analyte and study its influence on EGFET-based PEC sensors. Herein, a new sensing strategy was proposed by a mutual electrostatic interaction. Three-dimensional TiO 2 and g-C 3 N 4 core-shell heterojunction on flexible carbon cloth (TCN) was designed as the extended sensing gate. Tetracycline (TC) was also used as a model analyte, and it contains electron-donating groups (-NH 2 and -OH) with negative charge. The designed TCN-extended sensing gate was negatively charged in the dark by introducing carbon vacancies with oxygen doping in the g-C 3 N 4 shell, while it was positively charged under illustration due to the aggregation of photogenerated holes on the surface. Therefore, a light-activated PEC sensing platform for the sensitive and selective determination of tetracycline (TC) was demonstrated. Such a PEC sensor exhibited wide linear ranges within 100 pM to 1 μM and 1-100 μM with a low detection limit of 0.42 pM. Furthermore, the sensing platform possessed excellent selectivity, good reproducibility, and stability. The proposed sensing strategy in this work can expand the paradigm for developing a light-regulated FET-based PEC sensor by mutual electrostatic interaction, and we believe that this work will offer a new perspective for the design of interface interaction in PEC devices.

The regeneration of harmful activated sludge into an energy source is an important strategy for municipal sludge treatment and recycling. Herein, SiO 2 -modified N,S auto-doped porous carbon (NSC@SiO 2 ) with high conductivity (70 S m -1 ) is successfully obtained through a simple calcination method of the activated sludge from wastewater treatment. Further, P-doped NSC@SiO 2 (NSPC@SiO 2 ) is designed to achieve a higher surface area (891 m 2 g -1 vs 624 m 2 g -1 ), a larger pore volume (0.87 cm 3 g -1 vs 0.08 cm 3 g -1 ), and more carbon defects. Due to its special structure, NSPC@SiO 2 is used as a sulfur host of lithium-sulfur batteries. The results of polysulfide adsorption experiments, S 2p X-ray photoelectron spectra (XPS), Li 2 S nucleation experiments, polysulfide symmetric cells, measurement of the galvanostatic intermittent titration (GITT), polarization voltage difference, lithium-ion diffusion rate, and Tafel slope verified that NSPC@SiO 2 greatly improved the adsorption capacity of polysulfides, lowered the barrier to Li 2 S formation and the internal resistances of cells, and accelerated Li + ion diffusion and the reaction kinetics of polysulfide conversion, resulting in the excellent performance of polysulfide capture and superior rate performance and cyclic stability. By comparing NSPC@SiO 2 with NSC@SiO 2 , a higher initial capacity (1377 mAh g -1 vs 1150 mAh g -1 at 0.1C), better rate capacity (912 mAh g -1 vs 719 mAh g -1 at 2C), and low capacity decay (0.094% per cycle within 200 cycles) are obtained. Our work provides direction for the treatment, disposal, and resource utilization of activated sludge.

Conductive hydrogel-based ionic skins have attracted immense attention due to their great application prospects in wearable electronic devices. However, simultaneously achieving a combination of a single hydrogel system and excellent comprehensive performance (i.e., mechanical durability, electrical sensitivity, broad-spectrum antibacterial activity, and biocompatibility) remains a challenge. Thus, a novel poly(ionic liquid) hydrogel consisting of poly(acrylamide- co -lauryl methacrylate- co -methyl-uracil-imidazolium chloride- co -2-acryloylamino-2-methyl-1-propane sulfonic acid) (AAm-LMA-MUI-AMPS) was prepared by a micellar copolymerization method. Herein, MUI serves as a supramolecular crosslinker and conductive and bacteriostatic components. Owing to the multiple supramolecular crosslinks and hydrophobic association in the network, the hydrogel exhibits excellent mechanical properties (624 kPa of breaking stress and 1243 kPa of compression stress), skin-like modulus (46.2 kPa), stretchability (1803%), and mechanical durability (200 cycles under 500% strain can be completely recovered). Moreover, with the coordinated combination of each monomer, the hydrogel exhibits the unique advantage of high conductivity (up to 59.34 mS/cm). Hence, the hydrogel was further assembled as an ionic skin sensor, which exhibited a gauge factor (GF) of 10.74 and 7.27 with and without LiCl over a broad strain range (1-1000%), respectively. Furthermore, the hydrogel sensor could monitor human movement in different strain ranges, including body movement and vocal cord vibration. In addition, the antibacterial activity and biocompatibility of the hydrogel sensor were investigated. These findings present a new strategy for the design of new-generation wearable devices with multiple functions.

The long-standing misuse of antibiotics has accelerated the emergence of drug-resistant bacteria, which gives rise to an urgent public health threat. Antibacterial photodynamic therapy (aPDT), as a burgeoning and promising antibacterial strategy, plays an essential role in avoiding the evolution of drug-resistant microbes. However, it is hard for conventional photosensitizers to achieve satisfactory antibacterial efficacy because of the complex bacterial infectious microenvironment (BIME). Herein, a cascade BIME-triggered near-infrared cyanine ( HA-CY ) nanoplatform has been developed via conjugating cyanine units to biocompatible hyaluronic acid (HA) for enhanced aPDT efficacy. The HA-CY nanoparticles can be dissociated under the overexpressed hyaluronidase in BIME to release a cyanine photosensitizer. Meanwhile, cyanine can be protonated under acidic BIME, where protonated cyanine can efficiently adhere to the surface of a negatively charged bacterial membrane and increase singlet oxygen production due to intramolecular charge transfer (ICT). Experiments in the cellular level and animal model proved that the BIME-triggered activation of aPDT could remarkably boost aPDT efficacy. Overall, this BIME-triggered HA-CY nanoplatform presents great promise for overcoming the dilemma of drug-resistant microbes.

Early detection of metallic corrosion is one considerable method to reduce imperceptible disasters nowadays. Fluorescent coatings with high sensitivity and long lifetimes for use in the early detection of metallic corrosion are in high demand, but they are presently difficult to prepare. Inspired by the chameleon's skin, which is capable of switching its color in different atmospheres sensitively and reversibly, we proposed herein a facile and universal all-in-one strategy of combining the fluorescent sensitivity and dynamic hydrogen bonds in a hydrogel to develop a reusable corrosion detection tape to cover metal surfaces. The fluorescent hydrogel tape was constructed using free radical copolymerization of monomers [hydroxyethyl methylacrylate (HEMA) and tetraphenylethene derivatives (TPEPy)]. Due to the aggregation-induced emission (AIE) behavior of TPEPy, the poly(HEMA- co -TPEPy) hydrogel is capable of monitoring the traces of corrosion via the release of ferric ions with a concentration as low as 10 -5 M. Moreover, due to the dynamic hydrogen bonds of hydroxyethyl groups in hydrogel networks, the fluorescent hydrogel tape exhibited good adhesion and well reusability for over 10 applications to effectively warn against early corrosion of stainless steel. This non-destructive and reversible method of early corrosion detection can provide valuable signals when maintenance is needed before the metal suffers serious damage.

Spinel-type manganese oxide is considered as a typical cobalt-free high-voltage cathode material for lithium-ion battery applications because of its low cost, non-toxicity, and easy preparation. Nevertheless, severe capacity fading during charge and discharge limits its commercialization. Therefore, understanding the electrochemical properties and its modification mechanism of spinel-type manganese oxide for a lithium-ion battery is of great research interest. Herein, we presented a theoretical study regarding the discharge process of LiMn 2 O 4 and LiNi 0.5 Mn 1.5 O 4 using first-principles calculations based on density functional theory. We found that the discharge process is accompanied by an increase in unit cell volume and lattice distortion. Moreover, 25% Ni-substitution increases the average calculated voltage of LiMn 2 O 4 from 3.83 to 4.61 V, which is very close to the experimental value. The electronic structure is further discussed to understand the mechanism of voltage increase. In addition, the Ni element also reduces the Li-ion diffusion barrier by 0.06 eV, which helps to improve the intrinsic rate performance of LiMn 2 O 4 . Our research can provide insight into how Ni-substitution influences the voltage and diffusion barrier of LiMn 2 O 4 and pave the way for other spinel-type manganese oxide electrode applications.

The low specific capacity and Mg non-affinity of graphite limit the energy density of ion rechargeable batteries. Here, we first identify that the monolayer C 12-3-3 in sp 2 - sp can achieve high specific capacities of 1181 mAh/g for Li and 739 mAh/g for Mg, higher than those of most previous anodes. The Li storage reaction is an "adsorption-conversion-intercalation mechanism", while the Mg storage reaction is an "adsorption mechanism". The 2D carbon material of C 3 carbon hybridization with high Li/Mg affinity is an appropriate anode material for Li-ion batteries and Mg-ion batteries via the first-principles simulations. The monolayer C 12-3-3 can achieve high specific capacities of 1181 mAh/g for Li and 739 mAh/g for Mg, higher than those of most previous anodes. The Li storage reaction is an "adsorption-conversion-intercalation mechanism", while the Mg storage reaction is an "adsorption mechanism". The 2D carbon material of C 12-3-3 displays fast diffusion kinetics with low diffusion barriers of 0.41 eV for Li and 0.21 eV for Mg. As a new carbon-based anode material, the monolayer C 12-3-3 will promote the practical application of batteries with high-capacity and high-rate performance.

Long-term neuroinflammation is a major barrier to neurological recovery after cerebral ischemia-reperfusion injury (CIRI). Here, a thermosensitive injectable supramolecular hybrid hydrogel is developed to sustainably deliver exosomes derived from interleukin-1β-stimulated bone marrow stromal cells (BMSCs) (βExos) with improved exosome production and anti-inflammatory capacity for neuroinflammation inhibition and neurological recovery. The supramolecular hydrogel displays self-healing and injectable features, along with high biocompatibility and tissue-like softness. The βExos effectively reduce the lipopolysaccharide-induced inflammatory responses in the immortalized mouse microglia (BV2) cell line, and the in situ formed hydrogel improves the exosome retention in the ischemic core area. More remarkably, in the middle cerebral artery occlusion in vivo model, glial scar formation and neuronal loss are significantly reduced by regulating neuroinflammation using the released βExos. Therefore, the combination of interleukin-1β-stimulated exosomes with injectable supramolecular hydrogel provides an appealing strategy for treating central nervous system diseases.

As one of the most promising candidates, ubiquitous cycling degradation seriously affects the accuracy of carbon nanotube (CNT)-based sensors, and the reason for which is still unclear. Herein, the cycling degradation mechanism of CNT-based strain sensors has been detected by comparatively investigating the difference between the sensing behavior of CNT- and silver nanowire (Ag-NW)-based sensors, from which the microcrack-disconnection and unfolding-tunneling effects have been clarified as the sensing mechanism for Ag-NWs and CNT-based strain sensors, respectively. Furthermore, sliding and unfolding behaviors resulting from the weak interaction between CNTs have been proven to cause degradation. Correspondingly, a creative magnetically induced patterning method is proposed by utilizing magnetic nanoparticles as obstacles to prevent the CNTs from relative sliding. Benefiting from the advantageous factor, the performance deficiency of the CNT-based sensor has been overcome, and the sensitivity was significantly improved up to 5.2 times with accurate human activity detection. The competitive sensing performance of the CNTs demonstrates the reference value of the deficiency mechanism and solution scheme obtained in this study.

Hydrogen isotope storage materials are of great significance for controlled nuclear fusion, which is promising to provide unlimited clean and dense energy. Conventional storage materials of micrometer-sized polycrystalline ZrCo alloys prepared by the smelting method suffer from slow kinetics, pulverization, disproportionation, and poor cycling stability. Here, we synthesize a honeycomb-structured ZrCo composed of highly crystalline submicrometer ZrCo units using electrospray deposition and magnesiothermic reduction. Compared with conventional ones, honeycomb ZrCo does not require activation and exhibits more than 1 order of magnitude increase in kinetic property. Owing to low defects and low stress, the anti-disproportionation ability and cycling stability of honeycomb ZrCo are also obviously higher than those of conventional ZrCo. Moreover, the interfacial stress (due to hydrogenation/dehydrogenation) as a function of particle radius is established, quantitatively elucidating that small-sized ZrCo reduces stress and pulverization. This study points out a direction for the structural design of ZrCo alloy with high-performance hydrogen isotope storage.

Two-dimensional semiconducting transition-metal dichalcogenides (TMDCs) have attracted extensive attention as building blocks of miniaturized electronic and optical devices. However, as the characteristics of TMDC devices are predominately determined by their device structures, the function of TMDC devices is fixed once fabricated, leaving the reconfigurable active device and circuit a challenge. Here, we have demonstrated the current rectification switching in TMDC vertical diodes using a liquid metal (EGaIn) top electrode with a reconfigurable contact area. The rectification switching is closely related to the ultrathin gallium oxide layer on the surface of EGaIn. Under the small contact, with the existence of gallium oxide, photocurrent dominates the electrical transport showing a negative rectification, while as the contact increases, the broken gallium oxide leads to rectification switching to the positive bias direction. Such rectification switching applies to thin TMDC flakes down to 3 nm, benefitting from the soft electrical contact between the TMDC and the EGaIn electrode. Our work shows the new possibility of actively reconfigurable TMDC vertical diodes enabled by the liquid metal electrode and will promote promising applications of flexible and tunable TMDC-based nanoelectronic devices.

Zr-oxide secondary building units construct metal-organic framework (MOF) materials with excellent gas adsorption properties and high mechanical, thermal, and chemical stability. These attributes have led Zr-oxide MOFs to be well-recognized for a wide range of applications, including gas storage and separation, catalysis, as well as healthcare domain. Here, we report structure search methods within the Cambridge Structural Database (CSD) to create a curated subset of 102 Zr-oxide MOFs synthesized to date, bringing a unique record for all researchers working in this area. For the identified structures, we manually corrected the proton topology of hydroxyl and water molecules on the Zr-oxide nodes and characterized their textural properties, Brunauer-Emmett-Teller (BET) area, and topology. Importantly, we performed systematic periodic density functional theory (DFT) calculations comparing 25 different combinations of basis sets and functionals to calculate framework partial atomic charges for use in gas adsorption simulations. Through experimental verification of CO 2 adsorption in selected Zr-oxide MOFs, we demonstrate the sensitivity of CO 2 adsorption predictions at the Henry's regime to the choice of the DFT method for partial charge calculations. We characterized Zr-MOFs for their CO 2 adsorption performance via high-throughput grand canonical Monte Carlo (GCMC) simulations and revealed how the chemistry of the Zr-oxide node could have a significant impact on CO 2 uptake predictions. We found that the maximum CO 2 uptake is obtained for structures with the heat of adsorption values >25 kJ/mol and the largest cavity diameters of ca. 6-7 Å. Finally, we introduced augmented reality (AR) visualizations as a means to bring adsorption phenomena alive in porous adsorbents and to dynamically explore gas adsorption sites in MOFs.

Rapid and precise serum cytokine quantification provides immense clinical significance in monitoring the immune status of patients in rapidly evolving infectious/inflammatory disorders, examplified by the ongoing severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pandemic. However, real-time information on predictive cytokine biomarkers to guide targetable immune pathways in pathogenic inflammation is critically lacking, because of the insufficient detection range and detection limit in current label-free cytokine immunoassays. In this work, we report a highly sensitive localized surface plasmon resonance imaging (LSPRi) immunoassay for label-free Interleukin 6 (IL-6) detection utilizing rationally designed peptide aptamers as the capture interface. Benefiting from its characteristically smaller dimension and direct functionalization on the sensing surface via Au-S bonding, the peptide-aptamer-based LSPRi immunoassay achieved enhanced label-free serum IL-6 detection with a record-breaking limit of detection down to 4.6 pg/mL, and a wide dynamic range of ∼6 orders of magnitude (values from 4.6 to 1 × 10 6 pg/mL were observed). The immunoassay was validated in vitro for label-free analysis of SARS-CoV-2 induced inflammation, and further applied in rapid quantification of serum IL-6 profiles in COVID-19 patients. Our peptide aptamer LSPRi immunoassay demonstrates great potency in label-free cytokine detection with unprecedented sensing capability to provide accurate and timely interpretation of the inflammatory status and disease progression, and determination of prognosis.

Two chiral molecules 1 and 2 were designed and synthesized with a pyrene moiety directly linked to a chiral cholesterol moiety and connected through a methylene spacer, respectively. Influence of the spacer on their stimuli-responsive luminescence, chirality, and self-assembly behaviors was systematically investigated. Molecules 1 and 2 had similar aggregation-induced emission enhancement (AIEE) in solution, because of carrying the same fluorescence moiety. Both molecules displayed mechanochromism (MC) property but with different color contrast, whereas only 2 showed mechanoluminescence (ML) activity. When doping in liquid crystal molecule 5CB, both molecules induced the formation of chiral nematic liquid crystals (N*-LCs) with strong circularly polarized luminescence (CPL). Molecule 2 induced single handedness signal, irrespective of doping ratios, while 1 -doped N*-LCs showed an inversion of CPL signal from negative to positive upon the increase of doping ratios. Molecules 1 and 2 also self-assembled into different coassemblies with 5CB. Their distinct behaviors were attributed to the influence of the methylene spacer, which caused different molecular conformation and steric bulkiness; accordingly, it changed intermolecular interactions and molecular packing of the two molecules and led to diverse chirality and luminescence. This work provided important model molecules to better understand the molecular structure-property relationship and guide the design of novel functional molecules.

Photothermal conversion is a directly, sustainable, and green path to use solar energy and the one of the most important keys is the photothermal conversion material. How to obtain the durable and effective material for photothermal conversion with low cost and facile preparation is still a great challenge. In this work, the carbon nanotubes (CNTs) are grown on the carbon fibers (CFs) via the catalysis of trapped Fe and Co. The absorption of the as-prepared CFs/CNTs illustrate the enhancement from the visible light to the near-infrared light range. The photothermal conversion characterization shows the grown CNTs promoting the higher surface temperature and the highest temperature reaches to about 325 °C under 10 sun irradiations. The water evaporation on the CFs/CNTs is measured 1.40 ± 0.03 kg·cm -2 ·h -1 under 1 sun irradiation and the water evaporation rate is also found depending on the irradiation density. The photothermal conversion applications and the water evaporation under natural irradiation also reveal the suitable candidate of the CFs/CNTs for photothermal conversion application. This work provides a facile path to obtain effective carbon-based materials for photothermal application.

Monitoring conductivity changes of discontinuous palladium (Pd) nanostructures upon hydrogenation is becoming one of the most promising approaches toward hydrogen sensing. Development of sensors in this type has long been impeded due to strong ubiquitous interfacial adhesion which could distinctly restrict Pd expansion so as to hinder the closing of a nanogap. Herein, graphene underlayers were applied in the fabrication of nanogap-based hydrogen sensors to promote the lateral expansion of a Pd nanowire upon hydrogenation by reducing the adhesion between the metal and the substrate. In order to clarify details as well as mechanisms underlaid of graphene-enhanced Pd expansion, nanowire samples with serial lengths (6-48 μm) and gaps (0-260 nm in width) were controllably prepared on single-layer graphene (SLG), double-layer graphene (DLG), and quadruple-layer graphene (QLG, DLG × 2) via the combination of electron beam lithography (EBL) and electron beam deposition (EBD) technology. Response features and intrinsic analysis in physical sense of the graphene-based discontinuous Pd circuits upon hydrogen were established, in light of which the effects of underlayers on Pd expansion and on nanogap closing process were investigated. Such graphene-promoted expansion was demonstrated through the achievement of the closure of a large gap threshold ( G t ) up to 260 nm as well as the systematical investigation of its influence on the sensing performance.

Solar-driven photoreduction of CO 2 into valuable fuels offers a sustainable technology to relieve the energy crisis as well as the greenhouse effect. Yet the exploration of highly efficient, selective, stable, and environmental benign photocatalysts for CO 2 reduction remains a major issue and challenge. The interfacial engineering of heterojunction photocatalysts could be a valid approach to boost the efficiency of the catalytic process. Herein, we propose a novel covalent organic framework/metal organic framework (COF/MOF) heterojunction photocatalyst, using olefin (C═C) linked covalent organic framework (TTCOF) and NH 2 -UiO-66 (Zr) (NUZ) as representative building blocks, for enhanced CO 2 reduction to CO. The optimized TTCOF/NUZ exhibited a superior CO yield (6.56 μmol g -1 h -1 ) in gas-solid system when irradiated by visible light and only with H 2 O (g) as weak reductant, and it was 4.4 and 5 times higher than pristine TTCOF and NUZ, respectively. The photogenerated electrons transfer route was proposed to follow the typical step-scheme (S-scheme), which was affirmed by XPS, in situ XPS and EPR characterizations. The boosting CO 2 photoreduction activity could be credited to the special charge carrier separation in S-scheme heterojunction, which can accelerate photogenerated electrons transportation and improve the redox ability at the interface. This work paves the way for the design and preparation of novel COF/MOF S-scheme heterostructure photocatalysts for CO 2 reduction.

A cost-effective and highly efficient electrolyte with a wide electrochemical window, high reversibility of Mg plating/stripping, non-/low-corrosivity, good compatibility with cathode materials, and tolerance of trace water and impurity is crucial for the commercialization of rechargeable magnesium batteries. In this work, a novel boron-centered non-nucleophilic electrolyte that meets all the above requirements is prepared via a facile and economic approach from the raw materials B(TFE) 3 /MgCl 2 /CrCl 3 /Mg (BMCM). The as-prepared BMCM electrolyte is mainly composed of tetracoordinated anions [B(TFE) 4 ] - and solvated cations [Mg 2 (μ-Cl) 2 (DME) 4 ] 2+ . The BMCM electrolyte demonstrates attractive electrochemical performance, with a low overpotential (∼139 mV), a high Coulombic efficiency (∼97%), a high anodic stability (∼3.5 V vs Mg/Mg 2+ ), and a long-term (more than 500 h) cycling stability. Moreover, BMCM shows good compatibility with the CuS cathode material. The CuS|BMCM|Mg full cell delivers a discharge specific capacity of 231 mAh g -1 (at 56 mA g -1 ), which can retain ∼88% even after 100 cycles. Importantly, the BMCM electrolyte is cost-effective and tolerant of trace impurity and water, which has great potential to be commercialized. This work is expected to promote the development of practical rechargeable magnesium batteries.

Carbon dioxide (CO 2 ) sensing using an optical technique is of great importance in the environment and industrial emission monitoring. However, limited by the poor specific adsorption of gas molecules as well as insufficient coupling efficiency, there is still a long way to go toward realizing a highly sensitive optical CO 2 gas sensor. Herein, by combining the advantages of a whispering-gallery-mode microcavity and a metal-organic framework (MOF) film, a porous functional microcavity (PF-MC) was fabricated with the assistance of the atomic layer deposition technique and was applied to CO 2 sensing. In this functional composite, the rolled-up microcavity provides the ability to tune the propagation of light waves and the electromagnetic coupling with the surroundings via an evanescent field, while the nanoporous MOF film contributes to the specific adsorption of CO 2 . The composite demonstrates a high sensitivity of 188 nm RIU -1 (7.4 pm/% with respect to the CO 2 concentration) and a low detection limit of ∼5.85 × 10 -5 RIU. Furthermore, the PF-MC exhibits great selectivity to CO 2 and outstanding reproducibility, which is promising for the next-generation optical gas sensing devices.

The modulation of electronic behavior of metal-based catalysts is vital to optimize their catalytic performance. Herein, metal-organic frameworks (MOFs) are pyrolyzed to afford a series of different-structured Cu-carbon composites and Cu@N-doped carbon composites. Then a series of CO-resistant catalysts, namely, Co or Ni nanoparticles supported by the Cu-based composites, are synthesized for the hydrogen generation from aqueous NH 3 BH 3 . Their catalytic activities are boosted under light irradiation and regulated by the compositions and the fine structures of doped N species with pyridine, pyrrole, and graphitic configurations in the composite supports. Particularly, the optimized Co-based catalyst with the highest graphitic N content exhibits a high activity, achieving a total turnover frequency (TOF) value of 210 min -1 , which is higher than all the reported unprecious catalysts. Further investigations verify that the light-driven synergistic electron effect of plasmonic Cu-based composites and Co nanoparticles accounts for the high-performance hydrogen generation.

Directional water transport that occurs in natural insects and plants is important to both organisms and advanced science and technology. Despite the many studies conducted to facilitate directional liquid transport by constructing double-layered hydrophilic/hydrophobic materials, it remains difficult to achieve continuous water transport and reduce liquid wastage due to the hydrophilic regions. Herein, a directional water transport fabric (DWTF) was fabricated using a simple single-side coating method based on entirely hydrophobic materials. With coating thicknesses of 13-29 μm, the fabric could guide the continuous water motion from the coated to the uncoated side and can be utilized as a "liquid diode". In addition, the DWTF exhibited a water wastage reduction during the transport process, benefiting from the intrinsic hydrophobic properties of the material. Moreover, a plausible mechanism of water transport is proposed to explain the water droplet transfer in the bilayered hydrophobic materials. Consequently, the resulting DWTF exhibited an excellent accumulative one-way transport capability (AOTC) of 965.7% and a desirable overall moisture management capability (OMMC) of 0.92. This work provides an avenue for fabricating smart fluid delivery materials to various applications such as flexible microfluidics, wound dressing, oil-water separation processes, and engineered desiccant materials.

The earth-abundant iron and nitrogen doped carbon (Fe-N-C) catalyst has great potential to substitute noble metal catalysts for oxygen reduction reaction (ORR) in H 2 -O 2 proton exchange membrane fuel cells (PEMFCs). Herein, we report the preparation of Fe-N 4 moiety doped carbon nanotubes (CNTs) by ball milling and two-step pyrolysis with dual metal-organic frameworks (MOFs) as the precursor. This catalyst shows high ORR catalytic performance and stability. Different from traditional inorganic iron sources, the MOF structure can effectively prevent the iron metal from aggregating during pyrolysis. In PEMFC, the catalyst shows high current density (0.39 A/cm 2 at 0.7 V) and power density (850 mW/cm 2 ). Such a method brings inspiration for the reasonable design of FeNC catalysts with high catalytic activity for H 2 -O 2 PEMFCs.

Acute ischemic stroke has become the major cause of mortality and disability worldwide. Following ischemic stroke, the reperfusion injury is mainly mediated by the burst of reactive oxygen and nitrogen species (RONS). Therefore, blocking the excessive production or removing RONS holds great promise as a potential therapeutic strategy. Herein, we developed a Co-doped Fe 3 O 4 nanozyme that is capable of scavenging H 2 O 2 , O 2 •- , • NO, and ONOO- in vitro and in vivo and provides neuroprotection against ischemic stroke. In vitro experiments showed that pre-incubation with the Co-Fe 3 O 4 nanozyme could prevent neurotoxicity and neuroinflammation induced by H 2 O 2 or lipopolysaccharide, respectively, in HT22 cells. After intravenous administration, the Co-Fe 3 O 4 nanozyme showed no signs of toxicity in peripheral organs of C57BL/6J mice, even after prolonged delivery for 4 weeks. In permanent photothrombotic stroke model and transient middle cerebral artery occlusion stroke model, the Co-Fe 3 O 4 nanozyme specifically accumulated in the infarct rim at 72 h post-stroke and was endocytosed by neurons, astrocytes, microglia, and endothelial cells. Importantly, the Co-Fe 3 O 4 nanozyme delivery reduced the infarct volume in both stroke models. The observation that the Co-Fe 3 O 4 nanozyme was efficacious in two well-characterized ischemic stroke models provides strong evidence that it represents a powerful tool for targeting oxidative and nitrosative stress in the ischemic brain.

Monitoring hypoxia-related changes in subcellular organelles would provide deeper insights into hypoxia-related metabolic pathways, further helping us to recognize various diseases on subcellular level. However, there is still a lack of real-time, in situ , and controllable means for biosensing in subcellular organelles under hypoxic conditions. Herein, we report a reductase and light programmatical gated nanodevice via integrating light-responsive DNA probes into a hypoxia-responsive metal-organic framework for spatiotemporally controlled imaging of biomolecules in subcellular organelles under hypoxic conditions. A small-molecule-decorated strategy was applied to endow the nanodevice with the ability to target subcellular organelles. Dynamic changes of mitochondrial adenosine triphosphate under hypoxic conditions were chosen as a model physiological process. The assay was validated in living cells and tumor tissue slices obtained from mice models. Due to the highly integrated, easily accessible, and available for living cells and tissues, we envision that the concept and methodology can be further extended to monitor biomolecules in other subcellular organelles under hypoxic conditions with a spatiotemporal controllable approach.

Aristolochic acid (AA) has been reported to cause a series of health problems, including aristolochic acid nephropathy and liver cancer. However, AA-containing herbs are highly safe in combination with berberine (Ber)-containing herbs in traditional medicine, suggesting the possible neutralizing effect of Ber on the toxicity of AA. In the present study, in vivo systematic toxicological experiments performed in zebrafish and mice showed that the supramolecule self-assembly formed by Ber and AA significantly reduced the toxicity of AA and attenuated AA-induced acute kidney injury. Ber and AA can self-assemble into linear heterogenous supramolecules (A-B) via electrostatic attraction and π-π stacking, with the hydrophobic groups outside and the hydrophilic groups inside during the drug combination practice. This self-assembly strategy may block the toxic site of AA and hinder its metabolism. Meanwhile, A-B linear supramolecules did not disrupt the homeostasis of gut microflora as AA did. RNA-sequence analysis, immunostaining, and western blot of the mice kidney also showed that A-B supramolecules almost abolished the acute nephrotoxicity of AA in the activation of the immune system and tumorigenesis-related pathways.

Selective hydrogenation of alkynes plays a pivotal role in the field of chemical production but still suffers from restrained catalytic activity and low alkene selectivity. Herein, a dynamic modification strategy was utilized by preferentially attaching diethylenetriamine (DETA) to the surface of the support to modify the Pd catalyst. The DETA-modified Pd catalyst demonstrates unprecedented reactivity (14,412 h -1 ) and selectivity as high as 94% for the semihydrogenation of 2-methyl-3-butyn-2-ol at 35 °C, presenting a 36-fold higher reactivity than the Lindlar catalyst. Moreover, the yield exceeds 98.2% at full conversion under no solvent and organic adsorbate conditions, indicating the potential applications for industrial production. Systematic studies reveal that flexible DETA serves in a reversible "breathing pattern" for the molecular discrimination by constructing dynamic metal-support interaction (DMSI), enabling selective exclusion of alkenes from the Pd surface. DETA is competent to dynamically adjust the adsorption behaviors of reactants and effectively boost the intrinsic activity of the modified catalyst. Impressively, the DETA-modified Pd catalyst exhibits exceptional stability even after being recycled 20 times. This work sheds light on a novel and applicable method for the rational design of heterogeneous catalysts via DMSI.

Graphite has become a critical material because of its essential role in the lithium-ion battery (LIB) industry. However, the synthesis of graphite requires an energy-intensive thermal treatment. Also, when used in sodium-ion and potassium-ion batteries (SIBs and PIBs), the graphite anode shows poor capacities and cycling stability, which hinders the development of next-generation battery technologies. Finding suitable anode materials for commercial alkali metal-ion batteries is not only urgent for the energy storage industry, but is also important for economic and sustainable development. In this work, we use fly ash carbon (FAC), a residue of crude oil combustion, as an anode material for alkali metal-ion batteries. The FAC anodes show relatively high capacities and excellent cycling stability. The charge storage mechanism of FAC anode is shown to be intercalation coupled with redox reactions of oxygen functional groups. This work shows that FAC is a promising scalable anode material for alkali metal-ion batteries.

An electrochemical N 2 reduction reaction (NRR), as an environmentally benign method to produce NH 3 , is a suitable alternative to substitute the energy-intensive Haber-Bosch technology. Unfortunately, to date, it is obstructed by the lack of efficient electrocatalysts. Here, a CoS 2 /MoS 2 nanocomposite with CoS 2 nanoparticles decorated on MoS 2 nanosheets is fabricated and adapted as a catalyst for the NRR. As unveiled by experimental and theoretical results, the strong interaction between CoS 2 and MoS 2 modulates interfacial charge distribution with electrons transferring from CoS 2 to MoS 2 . Consequently, a local electrophilic region is formed near the CoS 2 side, which enables effective N 2 absorption. On the other hand, the nucleophilic area formed near the MoS 2 side is in favor of breaking stable N≡N, the potential-determining step (*N 2 → *N 2 H) which brings about a much decreased energy barrier than that on pure MoS 2 . As a result, this catalyst exhibits an excellent NRR performance, NH 3 yield and Faradaic efficiency of 54.7 μg·h -1 ·mg -1 and 20.8%, respectively, far better than most MoS 2 -based catalysts.

The conversion of asphalt into hexagon-like porous carbon (HPC) with a micro-mesoporous structure is realized by the coupling of template-directing and chemical activation methodologies. The specific surface area of HPC can reach up to 1356 m 2 g -1 even at such a low-proportioned dosage of activator (0.5-fold) and is also larger than those of template-directed carbon and activation-derived carbon, as it benefited from the coupling merits of template-directing and chemical activation. Excellent capacitive-energy-storage behavior with respect to rate capability, capacitance retention, and durability are delivered by HPC//HPC symmetric supercapacitors assembled with aqueous and organic electrolytes. This great compatibility for different kinds of electrolytes and electrode properties is owed to the robust hexagon-like microarchitecture feature associated with hierarchical pore structure, which not only hinders the stacking between each other but also provides a buffer function for the volume variation and sufficient active sites for the storage of electrolyte ions. The drastic temperature variation has almost no influence on the diffusion and transfer rate of electrolyte ions, further evidencing the advanced feature of the hierarchical pore structure. Additionally, HPC//Li 4 Ti 5 O 12 LIC assembled with the Li-based electrolyte also presents a superior Ragone performance. The coexistence of micro- and mesopores for the HPC makes it an attractive electrode material for various capacitive-energy-storage devices. This work provides a promising way to realize the plasticity of pore channels and mass production of high capacitive storage ability of electrode material via the combination of template-directing and chemical activation strategies.

Despite recent advances in bioinspired underwater adhesives, achieving tough, fast, and stable adhesion in aqueous environments is still challenging. Here, an underwater super-tape with semi-interpenetrating polymer networks (SIPNs) and a water-repelling liquid surface is synthesized. In the SIPN, the linear chains easily diffuse to adapt to the adherends, and the cross-linked chains provide the super-tape with high dimensional stability. Meanwhile, both the linear and cross-linked chains bear many catechol groups, which can not only vigorously interact with the adherends but also form numerous hydrogen bonds serving as sacrificial bonds in the SIPN. Thus, the super-tape shows both high interfacial adhesion and cohesive energy. Moreover, the super-tape is covered with a water-repelling liquid surface by spraying it with traces of a hydrophobic solvent. It is demonstrated that the hydrophobic solvent absorbed on the surface of the super-tape can remove water between the tape and adherends, enabling their intimate contact to form a strong interaction. As such, the super-tape shows excellent instant adhesion property under water, and the adhesive strength and toughness increase with time and reach their maximum values at around 5 h. The maximum debonding energy of the super-tape reaches 3933 J m -2 , which is much higher than those of existing double-sided tapes.

Photothermal therapy is a new type of tumor therapy with great potential. An ideal photothermal therapy agent should have high photothermal conversion effect, low biological toxicity, and degradability. The development of novel photothermal therapy agents with these properties is of great demand. In this study, we synthesized boron quantum dots (BQDs) with an ultrasmall hydrodynamic diameter. Both in vitro and in vivo studies show that the as-synthesized BQDs have good biological safety, high photoacoustic imaging performance, and photothermal conversion ability, which can be used for photoacoustic imaging-guided photothermal agents for tumor treatment. Our investigations confirm that the BQDs hold great promise in tumor theranostic applications.

Due to the dynamic nature of networks and high mobility of molecular chains, self-healing elastomers are usually confronted with the trade-off between self-healing efficiency and mechanical properties. Herein, a self-healing ionomer with both high mechanical performance and high self-healing efficiency has been successfully developed by grafting bromobutyl rubber (BIIR) with pyridine-based derivatives. Interestingly, the substituents on the pyridine ring can be used to regulate the interaction forces of ionic clusters and molecular dynamics. The electron-donating effect of the substituents facilitates stable π-π stacking between pyridyl ions, inducing the formation of regular and large ion aggregates, thereby improving the mechanical strength of the ionomer. Meanwhile, the plasticizing effect of the substituents reduces the activation energy and relaxation temperature of the ionic aggregates, thus endowing the ionomer with a high self-healing efficiency. As a result, the ionomer shows tensile strength as high as 8.1 ± 0.3 MPa under room temperature and self-healing efficiency of 100 ± 3% at 60 °C. Therefore, this strategy can be easily extended to other halogen-containing polymers, leading to a novel class of self-healing ionomers that hold great promise in diverse applications.