Ultrahigh Loading Research Articles

Hydrophobic modified poly(l‐glutamic acid) graft copolymer micelles with ultrahigh drug loading capacity for anticancer drug delivery

AbstractSelf‐assembled polymeric nanoparticle (NP) drug carriers are capable of encapsulated and controlled delivery, facilitating improvements in the therapeutic efficiency of drugs. Here we report a series of poly(l‐glutamic acid)‐g‐methoxy poly(ethylene glycol)/4‐phenylbutyl ester (PLG‐g‐mPEG/PB) copolymers, which were synthesized by esterification of 4‐phenylbutanol (PB) and PLG‐g‐mPEG in different feed ratios. The copolymers obtained form into nano‐sized micelles in aqueous solution by a self‐assembly process, with lower critical micelle concentration value for higher PB ratio in the copolymers. Variable temperature infrared spectroscopy and circular dichroism were used to prove the breaking of intermolecular hydrogen bonds after PB modification. Podophyllotoxin (PPT), an effective anticancer agent, was incorporated into the inner core of the micelle system by physical entrapment through hydrophobic interaction between the drug and the PB‐modified copolymers. Both the drug loading content and the loading efficiency increased with PB content in the PLG‐g‐mPEG/PB copolymers and reached an ultrahigh value of 28.2 wt% and 94%, respectively. The PPT‐encapsulated micelles (PPT‐NPs) were stable at pH 7.4 but dissociated and released 80% of loaded PPT in a weak acidic environment (pH 5.0). The in vitro proliferation of non‐small‐cell lung cancer cells (A549) was significantly inhibited by PPT‐NPs in a cytotoxicity assay. These results demonstrate that hydrophobic modification is an efficient route for tuning the self‐assembly behaviour and drug encapsulation of PLG‐g‐mPEG copolymers, and our PLG‐g‐mPEG/PB will serve as a promising carrier for hydrophobic anticancer drug delivery. © 2021 Society of Industrial Chemistry.

Self-Delivery Janus-Prodrug for Precise Immuno-Chemotherapy of Colitis-Associated Colorectal Cancer.

Aromatized thioketal (ATK) linked the immunoregulatory molecule (budesonide, Bud) and the cytotoxic molecule (gemcitabine, Gem) to construct a ROS-activated Janus-prodrug, termed as BAG. Benefiting from the hydrogen bonding, π-π stacking, and other intermolecular interactions, BAG could self-assemble into nanoaggregates (BAG NA) with a well-defined spherical shape and uniform size distribution. Compared to the carrier-based drug delivery system, BAG NA have ultrahigh drug loading content and ROS concentration-dependent drug release. Colitis-associated colorectal cancer (CAC) is a typical disease in which chronic inflammation transforms into tumors. BAG NA can be internalized by colon cancer C26 cells and then triggered by excessive intracellular ROS to release nearly 100% of the drugs. Based on this, BAG NA showed a stronger pro-apoptotic effect than free Bud combined with free Gem. What is gratifying is that orally administered BAG NA can precisely accumulate in the diseased colon tissues of CAC mice induced by AOM/DSS and simultaneously release Bud and Gem. Bud can regulate the tumor immune microenvironment to restore and enhance the cytotoxicity of Gem. Therefore, BAG NA maximizes the synergistic therapeutic effect through co-delivery of Bud and Gem. This work provided a cutting-edge method for constructing self-delivery Janus-prodrug based on ATK and confirmed its potential application in inflammation-related carcinogenesis.

A New Turbomachine for Clean and Sustainable Hydrocarbon Cracking

Abstract Decarbonizing highly energy-intensive industrial processes is imperative if nations are to comply with anthropogenic greenhouse gas emissions targets by 2050. This is a significant challenge for high-temperature industrial processes, such as hydrocarbon cracking, and there have been limited developments thus far. The novel concept presented in this study aims to replace the radiant section of a hydrocarbon cracking plant with a novel turboreactor. This is one of the first major and potentially successful attempts at decarbonizing the petrochemical industry. Rather than using heat from the combustion of natural gas, the novel turboreactor can be driven by an electric motor powered by renewable electricity. Switching the fundamental energy transfer mechanism from surface heat exchange to mechanical energy transfer significantly increases the exergy efficiency of the process. Theoretical analysis and numerical simulations show that the ultrahigh aerodynamic loading rotor is able to impart substantial mechanical energy into the feedstock without excess temperature difference and metal temperature magnitude. A complex shockwave system then transforms the kinetic energy into internal energy over an extremely short distance. The version of the turboreactor developed and presented in this study uses a single rotor row, in which a multistage environment is achieved regeneratively by guiding the flow through a toroidal-shaped vaneless space. This configuration leads to a reduction in reactor volume by more than two orders of magnitude compared with a conventional furnace. A significantly lower wall surface temperature, supersonic gas velocities, and a shorter primary gas path enable a controlled reduction in the residence time for chemical reactions, which optimizes the yield. For the same reasons, the conditions for coke deposition on the turboreactor surfaces are unfavorable, leading to an increase in plant availability. This study demonstrates that the mechanical work input into the feedstock can be dissipated through an intense turbulent mixing process, which maintains an ideal and controlled pressure level for cracking.

Unveiling low-tortuous effect on electrochemical performance toward ultrathick LiFePO4 electrode with 100 mg cm−2 area loading

Thickening electrodes can significantly increase the energy density and reduce the cost of batteries. However, the electrochemical performance of thick electrodes is limited by the kinetics of lithium-ion transport, resulting in severe polarization and poor electrochemical performance. Here, we investigate the electrochemical behavior of low-tortuous thick electrodes constructed by freeze-drying method. It is shown that low tortuosity can accelerate the transport of lithium-ions and mainly reduce the concentration polarization, leading to improved rate capability. Due to the fast lithium-ions transport kinetics, the electrochemical performance of low tortuous thick electrode is not dominantly determined by concentration polarization until a thickness of 125 μm, much higher than a thickness of 46 μm for the high tortuosity electrode. Thick electrodes with low tortuosity possess a stable cathode electrolyte interface, leading to superior cyclability. Area capacities of low tortuous thick electrodes increase linearly with active material loadings, indicating the independence of specific capacity and electrode thickness. Even at an ultrahigh area loading of 99.56 mg cm −2 , this low-tortuous thick electrode delivers an area capacity of 14.8 mAh cm −2 . This work reveals the electrochemical behavior of low tortuous thick electrode, providing guidance for applicable thick electrodes in high-performance lithium batteries. The low-tortuous thick electrode with straight lithium-ion transport channels is prepared by freezing drying strategy. Low-tortuous electrodes can not only accelerate lithium-ion transport kinetics and reduce the concentration polarization, but also possess a stable cathode electrolyte interface, enabling superior rate capability and cyclability. The rate determining step of the low-tortuous electrode changes to concentration polarization at bigger critical thickness. • The low tortuous LiFePO 4 thick electrode was prepared by the freeze-drying route. • Low tortuous electrode structure is beneficial for the transport of lithium-ions. • Low tortuous LiFePO 4 electrode shows superior rate capability and cyclability.

(Rose Bengal)/(Eosin Yellow)-Gold-Polypyrrole Hybrids: A Design for Dual Photo-Active Nano-System with Ultra-High Loading Capacity.

PurposeEnhancement of the photodynamic/photothermal efficiency of two water-soluble dyes, rose bengal (RB) and eosin yellow (EY), via conjugation to a polymeric nano-system gold-polypyrrole nanoparticle (AuPpy NPs).MethodologyA multi-step synthesis method and an in situ one-pot synthesis method were used. Loading percentage, particle size, zeta potential, morphology, UV-Vis-NIR spectrophotometry and in vitro photothermal activity were measured. Then, both hybrid nanocomposites were examined for their cytotoxicity and photocytotoxicity on HepG2 cell line as a model for cancer cells.ResultsDyes loaded in the traditional multi-step method did not exceed 9% w/w, while in the one-pot synthesis method they reached ~67% w/w and ~75% w/w for EY-AuPpy NPs and RB-AuPpy NPs, respectively. UV-Vis-NIR spectrophotometry showed that both nano-systems exhibited intense absorption in the NIR region. The mean size of the nanoparticles was ~31.5 nm (RB-AuPpy NPs) and ~33.6 nm (EY-AuPpy NPs) with zeta potential values of −26.5 mV and −33 mV, respectively. TEM imaging revealed the morphology of both hybrids, showing ultra-nano spherical-shaped gold cores in the case of RB-AuPpy NPs, and different shapes of larger gold cores in the case of EY-AuPpy NPs, both embedded in the polymer film. Conjugation to AuPpy was found to significantly reduce the dark cytotoxicity of both RB and EY, preserving the photocytotoxicity of EY and enhancing the photocytotoxicity of RB.ConclusionGold-polypyrrole nanoparticles represent an effective delivery system to improve the photodynamic and photothermal properties of RB and EY. The in situ one-pot synthesis method provided a means to greatly increase the loading capacity of AuPpy NPs. While both hybrid nanocomposites exhibited greatly diminished dark cytotoxicity, RB-AuPpy NPs showed significantly enhanced photocytotoxicity compared to the free dyes. This pattern enables the safe use of both dyes in high concentrations with sustained action, reducing dose frequency and side effects.

Amphiphilic small molecular mates match hydrophobic drugs to form nanoassemblies based on drug-mate strategy

Nanomedicine has made great progress in the targeted therapy of cancer. Here, we established a novel drug-mate strategy by studying the formulation of nanodrugs at the molecular level. In the drug-mate combination, the drug is a hydrophobic drug that is poorly soluble in water, and the mate is an amphiphilic small molecule (SMA) that has both hydrophilic and lipophilic properties. We proposed that the hydrophobic drug could co-assemble with a suitable SMA on a nanoscale without additive agents. The proof-of-concept methodology and results were presented to support our hypothesis. We selected five hydrophobic drugs and more than ten amphiphilic small molecules to construct a library. Through molecular dynamic simulation and quantum chemistry computation, we speculated that the formation of nanoassemblies was related to the binding energy of the drug-mate, and the drug-mate interaction must overcome drug-drug interaction. Furthermore, the obtained SF/VECOONa nanoassemblieswas selected as a model, which had an ultra-high drug loading content (46%), improved pharmacokinetics, increased bioavailability, and enhanced therapeutic efficacy. In summary, the drug-mate strategy is an essential resource to design exact SMA for many hydrophobic drugs and provides a reference for the design of a carrier-free drug delivery system.

Multifunctional cation-vacancy-rich ZnCo2O4 polysulfide-blocking layer for ultrahigh-loading Li-S battery

The major hurdle in Li-S battery commercialization is the severe shuttle effect and sluggish reaction kinetics of polysulfide conversion during charge-discharge cycling. Herein, to overcome these barriers, we designed and synthesized Zn defective Zn/Co oxide (ZDZCO) nanosheets, a cation-vacancy-rich bimetallic oxide for the construction of a multifunctional polysulfide-blocking layer. Both theoretical and experimental studies have comprehensively demonstrated that the ZDZCO shows robust binding capability towards polysulfides and a high catalytic ability for fast polysulfide conversion. Through a facile coating process, the multifunctional ZDZCO polysulfide-blocking layer is incorporated on a commercial polypropylene separator, forming a composite separator. The resultant separator facilitates an ultrahigh sulfur loading of 21.06 mg cm -2 and an areal capacity as high as 24.25 mAh cm -2 . This study illuminates a promising and practical strategy to construct high-performance Li-S batteries with high sulfur loading. A multifunctional cation-vacancy-rich ZnCo 2 O 4 modified separator has been developed to create a strong affinity to polysulfides and rapid catalytic conversion between the polysulfides for the achievement of ultrahigh areal loading and high-performance Li-S batteries. • Cation-vacancy-rich bimetallic oxide constructs a novel multifunctional polysulfide-blocking layer. • Cation vacancies boost catalytic performance of the multifunctional polysulfide-blocking layer. • The Li-S battery achieves an ultrahigh loading of 21.06 mg cm -2 and prolonged lifespan of 60 cycles.

Hydrazided hyaluronan/cisplatin/indocyanine green coordination nanoprodrug for photodynamic chemotherapy in liver cancer

It is still a huge challenge for concurrent highly efficient loading of chemotherapeutic agent and photosensitizer into single nanocarrier via stimuli-responsive linkages due to their different physicochemical properties and pharmacokinetics. Herein, based on the discovery of unique cisplatin-hydrazide and cisplatin-indocyanine green (ICG) coordination reactions, a multifunctional coordination nanoprodrug, cisplatin/ICG co-loaded hydrazided hyaluronan/bovine serum albumin (HBCI) nanoparticles, was developed by a desolvation-dual coordination process. The nanoprodrug exhibited ultrahigh drug loading efficiency and glutathione/NIR light dual-responsive drug release behavior. In vitro cellular studies demonstrated efficient internalization and apoptosis-inducing ability of the nanoprodrug in HepG2 cells. In vivo results confirmed the efficacious tumor accumulation and biosafety of HBCI nanoprodrug and synergistic effect of HBCI-based combined photodynamic chemotherapy on inhibiting tumor growth. Overall, this work not only provides a novel dual coordination approach for highly efficient loading of cisplatin and ICG but also verifies the therapeutic potential of HBCI nanoprodrug in combating hepatocellular carcinoma.

Operational load enhancement for an anaerobic membrane bioreactor through ethanol fermentation pretreatment of food waste

Anaerobic digestion (AD) of food waste (FW) tends to result in the accumulation of volatile fatty acids (VFA), especially a large quantity of propionic acid that is inevitably produced. Propionic acid has a significant inhibitory effect on AD at a concentration far lower than acetic acid. Therefore, anaerobic digestion cannot be operated at an excessively high load. We proposed an AD system that used a considerable amount of starch-rich food waste for ethanol fermentation as a pretreatment and reported that it improved methane concentration in biogas with a low propionic acid accumulation even under high-load operation. This study examined whether ethanol fermentation pretreatment (EP) of food waste can contribute to high-load operation on AD using an anaerobic membrane bioreactor (AnMBR). This involved a sequential bath experiment using FW that was saccharized before fermentation to ethanol. The results are compared with those for FW without pretreatment. The organic loading rate (OLR) was stepwise increased to 43.5 g COD/L/d by increasing the feed OLR, the hydraulic retention time (HRT) was six days and methane content was 71%–74%, which is thrice the capability of the control series and the highest load in the reports of medium temperature AD of FW. Furthermore, the primary methanogens were tolerant to ammonia inhibition. Correspondingly, the ammonium produced improved the buffering capacity of AD at high load. Functional archaeal and bacterial communities in the two reactors were examined. The abundance of hydrogenotrophic methanogens in AnMBR are determined to highlight the impact of the EP for FW disposal through 16S rRNA sequence analysis. Because there were multiple methanogens that use hydrogen, the higher decomposition of the substrate was attributable to the maintenance of a lower hydrogen partial pressure. It contributed to create a virtuous cycle with the EP. This study demonstrates the performance of the EP during high loading and long-term AD operation using an AnMBR; moreover, ultra-high load is achieved by changing the metabolic pathway.

Improving the Durability of Lithium-Metal Anode via In situ Constructed Multilayer SEI.

In this work, a novel multilayer solid electrolyte interphase (SEI) is demonstrated to prolong the durability of a lithium-metal anode. It is in situ generated via reducing lithium bis(oxalate) borate (LiBOB) and fluoroethylene carbonate (FEC) in the electrolyte containing them as additives. The as-obtained SEI could be roughly divided into three layers: the polycarbonates surface membrane, LiF-rich middle layer, and B-containing polymer bottom film corresponding to their sequentially reductive potentials of 0.8, 1.55, and 1.8 V vs Li+/Li, respectively. This special structure prolongs the durability of lithium-metal anode since the elastic bottom layer could buffer the influence of volumetric variation and the LiF-rich middle layer could suppress Li dendrite growth and electrolyte permeation. Benefiting from the protection of this multilayer SEI, LiNi0.88Co0.09Al0.03O2/Li batteries with ultrahigh cathode loading of ∼4.5 mAh cm-2 stably operate for 200 cycles with the accumulated capacity of 750 mAh cm-2 and the coulombic efficiency of 99.78%. This approach provides a simple and efficient strategy to hover lithium-metal anode.

Efficient Electronic Modulation of g-C 3 N 4 Photocatalyst by Implanting Atomically Dispersed Ag 1 -N 3 for Extremely High Hydrogen Evolution Rates

Efficient Electronic Modulation of g-C ₃ N ₄ Photocatalyst by Implanting Atomically Dispersed Ag ₁ -N ₃ for Extremely High Hydrogen Evolution Rates

A (110) Facet-Dominated Vanadium Dioxide Enabling Bidirectional Electrocatalysis for Lithium-Sulfur Batteries.

Catalysis is an effective way to improve the performance of lithium-sulfur (Li-S) batteries by enhancing the reaction kinetics of polysulfides. However, the bidirectional catalysis for discharging and charging processes in Li-S battery is still challenging. Herein, a (110) facet-dominated VO2 is prepared through the thermal-induced partial decomposition of (NH4)2V4O9 (NVO), forming a (110)VO2@NVO hybrid with the bidirectional catalysis ability. This (110) facet-dominated VO2 shows the ability to break the S-S bond to guide the Li2S deposition in the reduction process and reduce the delithiation barrier of Li2S to promote the oxidation process. The above hybrid is loaded on carbon nanofiber (CNF) to build an interlayer, where the 3D CNF and the conductive NVO ensure the fast electron transfer. The assembled battery with the above interlayer exhibits a high capacity of 1038 mAh g-1 after 300 cycles at 0.1 C (capacity retention: 70%). At a high rate of 5 C, a high capacity of 521 mAh g-1 after 1000 cycles is reached. Even under an ultrahigh sulfur loading of 10.3 mg cm-2 and a low electrolyte/sulfur ratio of 4 μL mgS-1, stable cycling performance with a high capacity of >3 mAh cm-2 is also achieved.

The Influences of Grain Refiner, Inclusion Level, and Filter Grade on the Filtration Performance of Aluminum Melt

The addition of grain refiner particles in the aluminum melt is known to reduce the filtration efficiency of ceramic foam filter (CFF). In the present work, a systematic study on the influence of the addition level of Al-Ti-B master alloys and the inclusion level on the filtration performance of aluminum melt has been investigated by pilot-scale filtration tests using 50 PPi and 80 PPi filters. The inclusion level of the melt has been measured using both LiMCA and PoDFA. For 80 PPi CFF, the N20 inclusion (diameter larger than 20 μm) value in the post-filtrated melt does not increase when an ultra-high level of inclusions is introduced in the form of chips. For the melts with a low level of grain refiners (~ 0.5 kg/ton), the filtration performance of CFF is not affected by grain refiners, regardless of inclusion load. An addition of 2.0 kg/ton grain refiners reduces the filtration performance for melts with a high inclusion level, where post-filtration inclusions with the size of 15-20 µm were significantly increased. It is found, however, for the melts with an ultra-high inclusion load, the filtration performance of 80 PPi CFF is not affected by the grain refiner addition up to 2.0 kg/ton. The interactions between inclusions and grain refiner particles and the filtration mechanism have been studied by characterizing the spent filter and measuring the pressure drop during the filtration process. It is revealed that the strong adherence between oxide film with grain refiner particles dominates the grain refiner influence on the filtration performance of CFF. During the filtration process, oxide films have strong influences on the capturing of other inclusions such as oxide particles and TiB2 particles by the filter. A mechanism based on the interactions between oxide films and grain refiner particles is proposed to explain the CFF performance under the influence of grain refiner.

Aqueous Protein-Polymer Bioconjugation via Photoinduced RAFT Polymerization Using High Loading Heterogeneous Catalyst.

Light-driven polymerization, such as photoinduced electron/energy transfer-reversible addition-fragmentation chain transfer (PET-RAFT) polymerization, enables biological benign conditions and versatile functional polymer structure design, which is readily used in protein-polymer bioconjugates. However, conventional metalloporphyrinic homogeneous catalysts for PET-RAFT polymerization suffer from limited aqueous solubility and tedious purification. Here we demonstrate the design of PET-RAFT photocatalyst from the reticular assembled Zr-porphyrinic metal-organic frameworks (MOFs), along with a biomacromolecule-based chain transfer agent, as efficient bioconjugation tools in water. Our methodology offers manufacturing advantages on bioconjugates under mild conditions such that MTT (3-[4,5-dimethylthiazol-2-yl]-2,5 diphenyl tetrazolium bromide) and cytotoxicity assays have shown the preservation of the protein integrity, bioactivity, and high cell viability after PET-RAFT polymerization. We find that the fast kinetics are benefiting from the ultrahigh loading of metalloporphyrins in MOF-525-Zn. This heterogeneous catalyst also allows us to maintain living characteristics to incorporate myriads of monomers into block copolymers. Other advantages like easy postreaction purification, reusability, and high oxygen tolerance even in an open system are demonstrated. This study provides a tool of highly efficient heterogeneous photocatalysts for polymer-protein bioconjugation in aqueous media and paves the road for biological applications.

Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol

Cobalt species as active sites for photocatalytic reduction of CO2 to valuable products such as methanol have received increasing attention, however, it remains a huge challenge to achieve the high activity. Herein, a pyrolysis-induced-vaporization strategy was successfully employed to fabricate Co/g-C3N4 single-atom catalysts (Co/g-C3N4 SACs) with surface Co atom loading up to 24.6 wt%. Systematic investigation of Co/g-C3N4 SACs formation process disclosed that concentrated-H2SO4 exfoliation of g-C3N4 nanosheets (g-C3N4 NSs) as the substrate followed by a two-step calcination process is essential to achieve ultrahigh metal loading. It was found that the ultrahigh-density of Co single-atom sites were anchored on the g-C3N4 substrate surface and coordinated with two nitrogen and one carbon atoms (Co-N2C). These single dispersed Co-N2C sites on the g-C3N4 surface were found to act not only as electron gathering centers but also as the sites of CO2 adsorption and activation, subsequently, boosting the photocatalytic methanol generation during light irradiation. As a result, the methanol formation rate at 4 h (941.9 μmol g−1) over Co/g-C3N4-0.2 SAC with 24.6 wt% surface Co loading was 13.4 and 2.2 times higher than those of g-C3N4 (17.7 μmol g−1) and aggregated CoOx/g-C3N4-0.2 (423.9 μmol g−1), respectively. Simultaneously, H2 (18.9 μmol g−1 h−1), CO (2.9 μmol g−1 h−1), CH4 (3.4 μmol g−1 h−1), C2H4 (1.1 μmol g−1 h−1), C3H6 (1.4 μmol g−1 h−1), and CH3OCH3 (3.3 μmol g−1 h−1) products were detected over Co/g-C3N4-0.2 SAC. Besides, the photocatalytic activity of the Co/g-C3N4-0.2 SAC for the reduction of CO2 to methanol was stable within 12-cycle experiments (~48 h). This work paves a strategy to boost the photoreduction CO2 activity via loading ultrahigh surface density single atomically dispersed cobalt active sites.

Three-dimensional hierarchical porous lignin-derived carbon/WO3 for high-performance solid-state planar micro-supercapacitor

The development of advanced energy storage systems, such as rechargeable batteries and supercapacitors (SCs), is one of the great challenges related to energy demand with the rapid development of world economy. Herein, a three-dimensional hierarchical porous lignin-derived carbon/WO3 (HPC/WO3) was prepared by carbonization and solvothermal process. This electrode material for supercapacitor can be operated at a wide voltage window range of −0.4 V to 1.0 V. More importantly, 3HPC/WO3 with ultrahigh mass loading (~3.56 mg cm−2) has excellent specific capacitance of 432 F g−1 at 0.5 A g−1 and cycling stability of 86.6% after 10,000 cycles at 10 A g−1. The as-assembled asymmetrical supercapacitor shows an energy density of 34.2 W h kg−1 at a power density of 237 W kg−1 and energy density of 16 W h kg−1 at a power density is 14,300 W kg−1. A solid-state planar micro-supercapacitor (MSC) was fabricated using HPC/WO3 nanocomposites. Moreover, the calculated specific capacity of MSC was 20 mF cm−2 in polyvinyl alcohol–sulfuric acid gel electrolyte. Overall, through the reasonable design of HPC/WO3 nanocomposite materials and the efficient assembly of MSCs, the performance of the device was greatly improved, thus providing a clear strategy for the development of energy storage devices.

A Cyanine-Mediated Self-Assembly System for the Construction of a Two-in-One Nanodrug.

The combination of gene therapy and chemotherapy provides a We developed a simple and versatile approach to prepare a series of two-in-one nanodrugs through direct self-assembly of cyanine-labeled single-stranded DNA (Cys-DNA) and different types of drug molecules. Molecular dynamics simulation showed that the Cys introduced into the DNA could enhance the noncovalent interaction between Cys-DNA and drug molecules. More drug molecules were incorporated into Cys-DNA, tending to spontaneously form hybrid Cys-DNA/drug nanosphere. Such nanospheres serve as both carriers and cargoes, excluding the extra use of nontherapeutic excipients and showing ultrahigh drug loading capacity. Following this approach, an antisense oligonucleotides/doxorubicin nanodrug model was constructed, demonstrating the significant synergistic anti-tumor therapeutic effect. As a proof of the concept, our study establishes a simple and reproducible two-in-one nucleic acid-based drug formulation.

Ultrahigh-Capacity and Scalable Architected Battery Electrodes via Tortuosity Modulation.

A thick electrode with high areal capacity is a straightforward approach to maximize the energy density of batteries, but the development of thick electrodes suffers from both fabrication challenges and electron/ion transport limitations. In this work, a low-tortuosity LiFePO4 (LFP) electrode with ultrahigh loadings of active materials and a highly efficient transport network was constructed by a facile and scalable templated phase inversion method. The instant solidification of polymers during phase inversion enables the fabrication of ultrathick yet robust electrodes. The open and aligned microchannels with interconnected porous walls provide direct and short ion transport pathways, while the encapsulation of active materials in the carbon framework offers a continuous pathway for electron transport. Benefiting from the structural advantages, the ultrathick bilayer LiFePO4 electrodes (up to 1.2 mm) demonstrate marked improvements in rate performance and cycling stability under high areal loadings (up to 100 mg cm-2). Simulation and operando structural characterization also reveal fast transport kinetics. Combined with the scalable fabrication, our proposed strategy presents an effective alternative for designing practical high energy/power density electrodes at low cost.

Cyclic Ether-Water Hybrid Electrolyte-Guided Dendrite-Free Lamellar Zinc Deposition by Tuning the Solvation Structure for High-Performance Aqueous Zinc-Ion Batteries.

The serious zinc dendrites and poor cyclability at high cathode loading owing to the strong solvation effect of traditional aqueous electrolytes are the main bottlenecks to the development of aqueous rechargeable zinc-ion batteries (ARZIBs). Here, we design an ether-water hybrid zinc-ion electrolyte with bifunctional roles of not only unplugging the dendrites bottleneck at the Zn anode but also extending the cycle life at high cathode loading. A cyclic ether (1,4-dioxane (DX)) is incorporated into traditional ZnSO4-based electrolytes to finely tune the solvation sheath of Zn2+. DX is found to guide the deposition orientation of zinc along the (002) plane, leading to not a dendritic structure but distinctively dense lamellar deposition due to the stronger affinity of the cyclic DX molecules toward Zn(002) than that of water, which is proven by density functional theory calculations. The cycling lifespan of the Zn anode extends up to over 600 h at 5.0 mA cm-2 and maintains extremely high Coulombic efficiency of 99.8%, thereby further enabling the Zn-MnO2 full cells to stably cycle at an ultrahigh mass loading of 9.4 mg cm-2, paving the way to their practical applications. This work also provides a novel electrolyte regulating solution for other aqueous multivalent metal-ion batteries.

A Cyanine‐Mediated Self‐Assembly System for the Construction of a Two‐in‐One Nanodrug

AbstractThe combination of gene therapy and chemotherapy provides a We developed a simple and versatile approach to prepare a series of two‐in‐one nanodrugs through direct self‐assembly of cyanine‐labeled single‐stranded DNA (Cys‐DNA) and different types of drug molecules. Molecular dynamics simulation showed that the Cys introduced into the DNA could enhance the noncovalent interaction between Cys‐DNA and drug molecules. More drug molecules were incorporated into Cys‐DNA, tending to spontaneously form hybrid Cys‐DNA/drug nanosphere. Such nanospheres serve as both carriers and cargoes, excluding the extra use of nontherapeutic excipients and showing ultrahigh drug loading capacity. Following this approach, an antisense oligonucleotides/doxorubicin nanodrug model was constructed, demonstrating the significant synergistic anti‐tumor therapeutic effect. As a proof of the concept, our study establishes a simple and reproducible two‐in‐one nucleic acid‐based drug formulation.