Latest ArticlesInspired by biological ion channels, numerous artificial asymmetric ion channels have been synthesized to facilitate the fabrication of ionic circuits. Nevertheless, the creation of biomimetic asymmetric ion channels necessitates expensive scientific apparatus and intricate material processing procedures, which constrains its advancement within the realm of ionic devices. In this study, we have devised dynamic asymmetric ion channels with mechanical responsiveness by combining polymers of varying elastic modulus along the longitudinal axis of carbon nanotube fiber (CNTF). The ion rectification can be modulated via the disparate response of CNTF-based ion channels to mechanical stress. We have effectively employed these asymmetric ion channels with mechanical sensitivity in the design of a logic gate device, achieving logic operations such as “AND” and “OR”. The conception of these dynamic asymmetric ion channels with mechanical sensitivity offers a straightforward, cost-effective, and versatile approach for generating ion channels, highlighting their potential application in intricate, highly integrated ionic circuits.
Carbon materials have been used as the support for catalysts in the field of acetylene hydrochlorination, the influence of inevitable oxygen-containing moieties on the reaction is often ignored and the mechanism of the oxygen-doping structure remains ambiguous. Herein, we explored the effect of the oxygen-containing group (C–O–C) in the support on the activity of single-atom dispersed Cu catalysts. By immersing the Cu single-atom catalyst in an alkaline solution, the epoxy species on the carbon support was cleaved to obtain a pure ether species while the Cu site was modified to a more electron-deficient state. The turnover frequency value of Cu/O-FLP catalyst with epoxy groups was 1.6-fold higher than that of alkaline treated catalyst. Our result indicated that the epoxy groups could assist adjacent single-atom Cu sites to synergistically promote the adsorption and cleavage of the reactant hydrogen chloride toward form C–OH and Cu–Cl bonds, and reduce the reaction energy barrier. The presence of electron deficient Cu sites and ether species could induce competitive adsorption of the acetylene and hydrogen chloride, thereby reducing the activity of the catalyst. This study highlights the influence of surface oxygen species and the tunability of the support, providing the foundation for the fabrication of higher-activity Cu catalysts for acetylene hydrochlorination.
To promote the practices of perovskite photovoltaics, it requires to develop efficient perovskite solar cells (PVSCs) standing long-time operation under the adverse environments. Herein, we demonstrate that the tailor-made conjugated polymers as conductive adhesives stabilized the originally redox-reactive heterointerface between perovskite and metal oxide, facilitating the access of efficient and stable inverted PVSCs. It was revealed that bithiophene and phenyl alternating conjugated polymers with partial glycol chains atop of the metal oxide layer has resulted in effective organic-inorganic hybrid hole transporting bilayers, which allow maintaining efficient hole extraction and transport, meanwhile preventing halide migration to directly contact with the nickel oxide (NiOx) layer. As a result, the corresponding inverted PVSCs with the organic-inorganic hole transporting bilayers have achieved an excellent power conversion efficiency of 23.22%, outperforming 20.65% of bare NiOx-based devices. Moreover, the encapsulated PVSCs with organic-inorganic bilayers exhibited the excellent photostability with 91% of the initial efficiency after 1000-h one-sun equivalent illumination in ambient conditions. Overall, this work provides new insights into stabilizing the vulnerable heterointerface for perovskite solar cells.
Due to the heterogeneity of tumors, single phototherapy cannot completely ablate tumors and inhibit tumor metastasis. To overcome these, we formulated targeted and multifunctional polymersomes ABC@ICG-IMQ-LHRH (AIRL) that encapsulated Toll-like receptor (TLR) 7/8 agonist imiquimod (IMQ) and photosensitizer indocyanine green (ICG) in the hydrophobic layer as well as bubble-generator NH4HCO3 in the hydrophilic cavity to inhibit the growth of primary and distant tumors, and prevent tumor metastasis through synergistic photoimmunotherapy. The AIRL polymersomes exhibited uniform and stable size, and high drug encapsulation efficiency, acid/reduction/laser responsiveness, excellent photothermal conversion efficiency, effective reactive oxygen species generation, high tumor accumulation. AIRL could be effectively internalized by dendritic cells (DCs), achieve lysosome escape and enhance DCs maturation. The synergistic photoimmunotherapy via AIRL polymersomes remarkably promoted the differentiation and activation of T cells, elevated strong systemic immune response to eradicate primary tumors and inhibit the growth of distant tumors. Simultaneously, the endurable immunological memory prevented tumor metastasis, which provided a promising nanoplatform for the combination therapy of cancer.
Ulcerative colitis (UC) is a chronic inflammatory bowel disease characterized by persistent inflammation of the colon and disrupted intestinal function. Ramulus mori (Sangzhi) alkaloids (SZ-A), derived from twigs of mulberry, were approved by the National Medical Products Administration in 2020 for treating type 2 diabetes mellitus. Accumulated evidence has confirmed that SZ-A also alleviates non-alcoholic fatty liver disease and ameliorates inflammation, indicating its potential to address inflammation in UC. However, the treatment of UC faces challenges due to low drug delivery efficiency and short retention time. To overcome these challenges, an injectable and adherent in-situ thermo-sensitive hydrogel containing SZ-A was developed for rectal drug delivery, utilizing the thermo-sensitive polymers Poloxamer 407 and 188. The thermo-sensitive hydrogel system was designed with a moderate gelation temperature of 32 ± 0.5 ℃, a short gelation time of 64 s, a pH range of 7–10, high moisturizing capability exceeding 90%, and moderate mechanical strength of 4–5 s. In a rat model with UC, the in situ thermo-sensitive hydrogel significantly extended the retention time at the colonic site and enabled sustained release after rectal administration. Symptoms of UC were markedly reduced following rectal administration of SZ-A thermo-sensitive hydrogel. Furthermore, the release of inflammatory factors, such as interleukin-1β (IL-1β), IL-6, IL-18, tumor necrosis factor-α (TNF-α), and transforming growth factor-β1 (TGF-β1), significantly decreased in the SZ-A thermo-sensitive hydrogel group. The integrity of the colonic mucosal barrier was significantly enhanced following the application of SZ-A thermo-sensitive hydrogel. In conclusion, rectal administration of SZ-A in situ thermo-sensitive hydrogel effectively alleviated UC symptoms, inhibited the secretion of inflammatory factors, and promoted the repair of the colonic mucosal barrier. This approach holds promise as a potential treatment for UC.
Commercial V2O5-based catalysts have been successfully applied in NH3 selective catalytic reduction (NH3-SCR) of NOx from power stations, but their poor alkali-resistance restrains the wider application in nonelectrical industries. In this study, NOx reduction against alkali poisoning over V2O5/TiO2 is greatly improved via Ce(SO4)2 modification. It has been originally demonstrated that Ce4+–SO42− pair sites play crucial roles in improving NOx reduction against alkali poisoning over V2O5/TiO2 catalysts. The strong interaction between V species and Ce sites of Ce4+–SO42− pairs triggers the reaction between NH4+species and gaseous NO via Eley-Rideal (E-R) reaction pathway. After K-poisoning, the SO42− sites of Ce4+–SO42− pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway. This work demonstrates an effective strategy to enhance NOx reduction against alkali poisoning over catalysts via constructing Ce4+–SO42− pair sites, contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.
The detrimental "shuttle effect" of lithium polysulfides (LiPSs) together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur (Li-S) batteries from commercial success. Here, we first propose the implementability of layered rare-earth hydroxides (LREHs) in Li-S batteries to optimize electrochemical performance. In this work, a two-dimensional (2D) rare-earth-based composite constructed by the layered gadolinium hydroxy chloride [Gd2(OH)5(H2O)]Cl nanoplates (LGdH NPs) and graphene oxide (GO) was designed as a sulfur immobilizer for Li-S batteries. Combining the experimental results and density functional theory (DFT) calculations, it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling, but also acts as an effective catalyst to accelerate the liquid-solid conversion of polysulfides. The Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C, as well as excellent cycle stability with a decay rate of 0.087% over 500 cycles at 2 C. This study provided a deep understanding of the mechanism to suppress the "shuttle effect" by the LREHs, and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.
Copper phthalocyanine (CuPc) is adopted as an electrolyte additive to stabilize lithium anode for lithium-sulfur (Li-S) batteries. CuPc with a planar molecular structure and lithiophilic N-containing group, is likely to be adsorbed on the surface of Li anode to form a coating layer, which can restrict the direct contact between Li anode and solvents, and guide the uniform deposition of Li+ ions. The Li||Li symmetric cells demonstrate a stable cycle performance, and Li||Cu cells show high Coulombic efficiencies. In Li-S batteries, the formed stable solid-electrolyte interface (SEI) film containing copper sulfides can protect Li anode from the polysulfide corrosion and side reactions with the electrolyte, leading to the compact and smooth surface morphology of Li anode. Therefore, the Li-S batteries with CuPc additive deliver much higher capacity, better cycle performance and rate capability as compared to the one without CuPc additive.
Due to its high operational voltage and energy density, P2-type Na0.67Ni0.3Mn0.7O2 has become a leading cathode material for sodium-ion batteries (SIBs), which is an ideal option for large-scale energy storage. However, the practical application of P2-type Na0.67Ni0.3Mn0.7O2 is limited by the capacity constraints and unwanted phase transitions, presenting significant challenges to the widespread application of SIBs. To address these challenges and optimize the electrochemical properties of the P2 phase cathode material, this study proposes a Cu and Zn co-doped strategy to improve the electrochemical performance. The incorporation of Cu/Zn can stabilize the P2-phase structure against P2-O2 phase transitions, thus enhancing its electrochemical properties. The as-obtained P2-type Na0.67[Ni0.3Mn0.58Cu0.09Zn0.03]O2 cathode material shows an impressive cycling stability, maintaining 80% capacity retention after 1000 cycles at 2 C. The cyclic voltammetry (CV) tests show that the Cu2+/Cu3+ redox reaction is also involved in charge compensation during the charge/discharge process.
O3-type layered oxide cathodes have been widely investigated due to their high reversible capacities and sufficient Na+ reservoirs. However, such materials usually suffer from complex multistep phase transitions along with drastic volume changes, leading to the unsatisfied cycle performance. Herein, we report a Mg/Ti co-doped O3-type NaNi0.5Mn0.5O2, which can effectively suppress the complex multistep phase transition and realize a solid-solution reaction within a wide voltage range. It is confirmed that, the Mg/Ti co-doping is beneficial to enhance the structural stability and integrity by absorbing micro-strain and distortions. Thus, the as obtained sample delivers an outstanding cyclic performance (82.3% after 200 cycles at 1 C) in the voltage range of 2.0–4.0 V, and a high discharge capacity of 86.6 mAh/g after 100 cycles within the wide voltage range (2.0–4.5 V), which outperform the existing literatures. This co-doping strategy offers new insights into high performance O3-type cathode for sodium ion batteries.
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