Cohesive energy discrepancy drives the fabrication of multimetallic atomically dispersed materials for hydrogen evolution reaction.

Atomically dispersed single atom (SA) and atomic cluster (AC) metallic materials attract tremendous attentions in various fields. Expanding monometallic SA and AC to multimetallic SA/AC composites opens vast scientific and technological potentials yet exponentially increasing the synthesis difficulty. Here, we present a general energy-selective-clustering methodology to build the largest reported library of carbon supported bi-/multi-metallic SA/AC materials. The discrepancy in cohesive energy results into selective metal clustering thereby driving the symbiosis of multimetallic SA or/and AC. The library includes 23 bimetallic SA/AC composites, and expanded compositional space of 17 trimetallic, quinary-metallic, septenary-metallic SA/AC composites. We chose bimetallic M1SAM2AC to demonstrate the electrocatalysis utility. Unique decoupled active sites and inter-site synergy lead to 8/47 mV overpotential at 10 mA cm-2 for alkaline/acidic hydrogen evolution and over 1000 h durability in water electrolyzer. Moreover, delicate modulations towards composition and configuration yield high-performance catalysts for multiple electrocatalysis systems. Our work broadens the family of atomically dispersed materials from monometallic to multimetallic and provides a platform to explore the complex composition induced unconventional effects.

Routes to Bidirectional Cathodes for Reversible Aprotic Alkali Metal-CO2 Batteries.

Aprotic alkali metal-CO2 batteries (AAMCBs) have garnered significant interest owing to fixing CO2 and providing large energy storage capacity. The practical implementation of AAMCBs is constrained by the sluggish kinetics of the CO2 reduction reaction (CO2RR) and the CO2 evolution reaction (CO2ER). Because the CO2ER and CO2RR take place on the cathode, which connects the internal catalyst with the external environment. Building a bidirectional cathode with excellent CO2ER and CO2RR kinetics by optimizing the cathode's internal catalyst and environment has attracted most of the attention to improving the electrochemical performance of AAMCBs. However, there remains a lack of comprehensive understanding. This review aims to give a route to bidirectional cathodes for reversible AAMCBs, by systematically discussing engineering strategies of both the internal catalyst (atomic, nanoscopic, and macroscopic levels) and the external environment (photo, photo-thermal, and force field). The CO2ER and CO2RR mechanisms and the "engineering strategies from internal catalyst to the external environment-cathode properties-CO2RR and CO2ER kinetics and mechanisms-batteries performance" relationship are elucidated by combining computational and experimental approaches. This review establishes a fundamental understanding for designing bidirectional cathodes and gives a route for developing reversible AAMCBs and similar metal-gas battery systems.

A temperature compensated fiber probe for highly sensitive detection in virus gene biosensing.

This research presents an innovative reflective fiber optic probe structure, mutinously designed to detect H7N9 avian influenza virus gene precisely. This innovative structure skillfully combines multimode fiber (MMF) with a thin-diameter seven-core photonic crystal fiber (SCF-PCF), forming a semi-open Fabry-Pérot (FPI) cavity. This structure has demonstrated exceptional sensitivity in light intensity-refractive index (RI) response through rigorous theoretical and experimental validation. The development of a quasi-distributed parallel sensor array, which provides temperature compensation during measurements, has achieved a remarkable RI response sensitivity of up to 532.7 dB/RIU. The probe-type fiber optic sensitive unit, expertly functionalized with streptavidin, offers high specificity in detecting H7N9 avian influenza virus gene, with an impressively low detection limit of 10-2 pM. The development of this biosensor marks a significant development in biological detection, offering a practical engineering solution for achieving high sensitivity and specificity in light-intensity-modulated biosensing. Its potential for wide-ranging applications in various fields is now well-established.

Multi-stage 3D-printed guide for precise restoration of severely inclined teeth based on target restorative space guidance: a case report.

In clinical dentistry, addressing unique conditions such as tilted, elongated, and torsion teeth during preparation can be effectively managed through digital tooth morphology design. The production of a multi-stage 3D-printed guide offered a more efficient and accurate solution. This article presented a case of significant inclination, elongation, and torsion in the maxillary and mandibular canines that were successfully treated using crown restoration modification. A crown preparation guide was fabricated based on the final form design of the restoration using the target restorative space analysis technique to ensure precise tooth preparation. A tooth preparation guide was also designed and utilized further to enhance accuracy and efficiency during complex tooth preparation. The combined application of these multi-stage guides demonstrated promising clinical prospects.

Correlating the crystal structure and facet of indium oxides with their activities for CO2 electroreduction.

Constructing structure-function relationships is critical for the rational design and development of efficient catalysts for CO2 electroreduction reaction (CO2RR). In2O3 is well-known for its specific ability to produce formic acid. However, how the crystal phase and surface affect the CO2RR activity is still unclear, making it difficult to further improve the intrinsic activity and screen for the most active structure. In this work, cubic and hexagonal In2O3 with different stable surfaces ((111) and (110) for cubic, (120) and (104) for hexagonal) are investigated for CO2RR. Theoretical results demonstrate that the adsorption of reactants on cubic In2O3 is stronger than that on hexagonal In2O3, with the cubic (111) surface being the most active for CO2RR. In experiments, synthesized cubic In2O3 nanosheets with predominantly exposed (111) surfaces exhibited a high HCOO- Faradaic efficiency (87.5%) and HCOO- current density (-16.7 mA cm-2) at -0.9 V vs RHE. In addition, an aqueous Zn-CO2 battery based on a cubic In2O3 cathode was assembled. Our work correlates the phases and surfaces with the CO2RR activity, and provides a fundamental understanding of the structure-function relationship of In2O3, thereby contributing to further improvements in its CO2RR activity. Moreover, the results provide a principle for the directional preparation of materials with optimal phases and surfaces for efficient electrocatalysis.

In Situ Symbiosis of Cerium Oxide Nanophase for Enhancing the Oxygen Electrocatalysis Performance of Single-Atom Fe─N─C Catalyst with Prolonged Stability for Zinc-Air Batteries.

The Fenton reaction, induced by the H2O2 formed during the oxygen reduction reaction (ORR) process leads to significant dissolution of Fe, resulting in unsatisfactory stability of the iron-nitrogen-doped carbon catalysts (Fe-NC). In this study, a strategy is proposed to improve the ORR catalytic activity while eliminating the effect of H2O2 by introducing CeO2 nanoparticles. Transmission electron microscopy and subsequent characterizations reveal that CeO2 nanoparticles are uniformly distributed on the carbon substrate, with atomically dispersed Fe single-atom catalysts (SACs) adjacent to them. CeO2@Fe-NC achieves a half-wave potential of 0.89 V and a limiting current density of 6.2 mA cm-2, which significantly outperforms Fe-NC and commercial Pt/C. CeO2@Fe-NC also shows a half-wave potential loss of only 1% after 10 000 CV cycles, which is better than that of Fe-NC (7%). Further, H2O2 elimination experiments show that the introduction of CeO2 significantly accelerate the decomposition of H2O2. In situ Raman spectroscopy results suggest that CeO2@Fe-NC significantly facilitates the formation of ORR intermediates compared with Fe-NC. The Zn-air batteries utilizing CeO2@Fe-NC cathodes exhibit satisfactory peak power density and open-circuit voltage. Furthermore, theoretical calculations show that the introduction of CeO2 enhances the ORR activity of Fe-NC SAC. This study provides insights for optimizing SAC-based electrocatalysts with high activity and stability.

Achieving Uniform Li Deposition and Suppressed Electrolyte Flammability in Li-Metal Batteries via Designing Localized High-Concentration Electrolytes.

The increasing need for energy storage devices with high energy density has led to significant interest in Li-metal batteries (LMBs). However, the use of commercial electrolytes in LMBs is problematic due to their flammability, inadequate performance at low temperatures, and tendency to promote the growth of lithium dendrites and other flaws. This study introduces a localized high-concentration electrolyte (LHCE) that addresses these issues by employing non-flammable electrolyte components and incorporating carefully designed additives to enhance flame retardancy and low-temperature performance. By incorporating additives to optimize the electrolyte, it is possible to attain inorganic-dominated solid electrolyte interphases on both the cathode and anode. This achievement results in a uniform deposition of lithium, as well as the suppression of electrolyte decomposition and cathode deterioration. Consequently, this LHCE achieve over 300 stable cycles for both LiNi0.9Mn0.05Co0.05O2||Li cells and LiCoO2||Li cells, as well as 50 cycles for LiNi0.8Mn0.1Co0.1O2 (NCM811||Li) pouch cells. Furthermore, NCM811||Li cells maintain 84% discharge capacity at -20 °C, in comparison to the capacity at room temperature. The utilization of this electrolyte presents novel perspectives for the safe implementation of LMBs.

High-Pressure-Field Induced Synthesis of Ultrafine-Sized High-Entropy Compounds with Excellent Sodium-Ion Storage.

Emerging high entropy compounds (HECs) have attracted huge attention in electrochemical energy-related applications. The features of ultrafine size and carbon incorporation show great potential to boost the ion-storage kinetics of HECs. However, they are rarely reported because high-temperature calcination tends to result in larger crystallites, phase separation, and carbon reduction. Herein, using the NaCl self-assembly template method, by introducing a high-pressure field in the calcination process, the atom diffusion and phase separation are inhibited for the general formation of HECs, and the HEC aggregation is inhibited for obtaining ultrafine size. The general preparation of ultrafine-sized (<10 nm) HECs (nitrides, oxides, sulfides, and phosphates) anchored on porous carbon composites is realized. They are demonstrated by combining advanced characterization technologies with theoretical computations. Ultrafine-sized high entropy sulfides-MnFeCoCuSnMo/porous carbon (HES-MnFeCoCuSnMo/PC) as representative anodes exhibit excellent sodium-ion storage kinetics and capacities (a high rating capacity of 278 mAh g-1 at 10 A g-1 for full cell and a high cycling capacity of 281 mAh g-1 at 20 A g-1 after 6000 cycles for half cell) due to the combining advantages of high entropy effect, ultrafine size, and PC incorporation. Our work provides a new opportunity for designing and fabricating ultrafine-sized HECs.

Revolutionizing cancer treatment: enhancing CAR-T cell therapy with CRISPR/Cas9 gene editing technology.

CAR-T cell therapy, a novel immunotherapy, has made significant breakthroughs in clinical practice, particularly in treating B-cell-associated leukemia and lymphoma. However, it still faces challenges such as poor persistence, limited proliferation capacity, high manufacturing costs, and suboptimal efficacy. CRISPR/Cas system, an efficient and simple method for precise gene editing, offers new possibilities for optimizing CAR-T cells. It can increase the function of CAR-T cells and reduce manufacturing costs. The combination of CRISPR/Cas9 technology and CAR-T cell therapy may promote the development of this therapy and provide more effective and personalized treatment for cancer patients. Meanwhile, the safety issues surrounding the application of this technology in CAR-T cells require further research and evaluation. Future research should focus on improving the accuracy and safety of CRISPR/Cas9 technology to facilitate the better development and application of CAR-T cell therapy. This review focuses on the application of CRISPR/Cas9 technology in CAR-T cell therapy, including eliminating the inhibitory effect of immune checkpoints, enhancing the ability of CAR-T cells to resist exhaustion, assisting in the construction of universal CAR-T cells, reducing the manufacturing costs of CAR-T cells, and the security problems faced. The objective is to show the revolutionary role of CRISPR/Cas9 technology in CAR-T cell therapy for researchers.

Bioresponsive nanocomplex integrating cancer-associated fibroblast deactivation and immunogenic chemotherapy for rebuilding immune-excluded tumors.

Cancer-associated fibroblasts (CAFs) play a crucial role in creating an immunosuppressive environment and remodeling the extracellular matrix within tumors, leading to chemotherapy resistance and limited immune cell infiltration. To address these challenges, integrating CAFs deactivation into immunogenic chemotherapy may represent a promising approach to the reversal of immune-excluded tumor. We developed a tumor-targeted nanomedicine called the glutathione-responsive nanocomplex (GNC). The GNC co-loaded dasatinib, a CAF inhibitor, and paclitaxel, a chemotherapeutic agent, to deactivate CAFs and enhance the effects of immunogenic chemotherapy. Due to the modification with hyaluronic acid, the GNC preferentially accumulated in the tumor periphery and responsively released cargos, mitigating the tumor stroma as well as overcoming chemoresistance. Moreover, GNC treatment exhibited remarkable immunostimulatory efficacy, including CD8+ T cell expansion and PD-L1 downregulation, facilitating immune checkpoint blockade therapy. In summary, the integration of CAF deactivation and immunogenic chemotherapy using the GNC nanoplatform holds promise for rebuilding immune-excluded tumors.

Stabilization of LiCoO2 Cathodes in High Voltage Lithium Metal Batteries Through 2-(Trifluoromethyl)Benzamide (2-TFMBA) Electrolyte Additives.

Increasing the charging cutoff voltage of LiCoO2 to 4.6 V is significant for enhancing battery density. However, the practical application of Li‖LiCoO2 batteries with a 4.6 V cutoff voltage faces significant impediments due to the detrimental changes under high voltage. This study presents a novel bifunctional electrolyte additive, 2-(trifluoromethyl)benzamide (2-TFMBA), which is employed to establish a stable and dense cathode-electrolyte interface (CEI). Characterization results reveal that an optimized CEI is achieved through the synergistic effects of the amide groups and trifluoromethyl groups within 2-TFMBA. The resulting CEI not only enhances the structural stability of LiCoO2 but also serves as a high-speed lithium-ion conduction channel, which expedites the insertion and extraction of lithium ions. The Li‖LiCoO2 batteries with 0.5 wt% 2-TFMBA achieves an 84.7% capacity retention rate after enduring 300 cycles at a current rate of 1 C, under a cut-off voltage of 4.6 V. This study provides valuable strategic insights into the stabilization of cathode materials in high-voltage batteries.

Ultrasound-Assisted Preparation and Performance Regulation of Electrocatalytic Materials.

With the advancement of scientific research, the introduction of external physical methods not only adds extra freedom to the design of electro-catalytical processes for green technologies but also effectively improves the reactivity of materials. Physical methods can adjust the intrinsic activity of materials and modulate the local environment at the solid-liquid interface. In particular, this approach holds great promise in the field of electrocatalysis. Among them, the ultrasonic waves have shown reasonable control over the preparation of materials and the electrocatalytic process. However, the research on coupling ultrasonic waves and electrocatalysis is still early. The understanding of their mechanisms needs to be more comprehensive and deep enough. Firstly, this article extensively discusses the adhibition of the ultrasonic-assisted preparation of metal-based catalysts and their catalytic performance as electrocatalysts. The obtained metal-based catalysts exhibit improved electrocatalytic performances due to their high surface area and more exposed active sites. Additionally, this article also points out some urgent unresolved issues in the synthesis of materials using ultrasonic waves and the regulation of electrocatalytic performance. Lastly, the challenges and opportunities in this field are discussed, providing new insights for improving the catalytic performance of transition metal-based electrocatalysts.

In situ Implanting 3D Carbon Network Reinforced Zinc Composite by Powder Metallurgy for Highly Reversible Zn-based Battery Anodes.

Aqueous Zn-based batteries have emerged as compelling candidates for grid-scale energy storage, owing to their intrinsic safety, remarkable theoretical energy density and cost-effectiveness. Nonetheless, the dendrite formation, side reactions, and corrosion on anode have overshadowed their practical applications. Herein, we present an in situ grown carbon network reinforcing Zn matrix anode prepared by powder metallurgy. This carbon network provides an uninterrupted internal electron transport pathway and optimize the surface electric field distribution, thereby enabling highly reversible Zn deposition. Consequently, symmetrical cells demonstrate impressive stability, running for over 880 h with a low voltage hysteresis (≈32 mV). Furthermore, this Zn matrix composite anode exhibits enhanced performance in both the aqueous Zn-ion and the Zn-air batteries. Notably, Zn//MnO2 cells display superior rate capabilities, while Zn-air batteries deliver high power density and impressive Zn utilization rate (84.9 %). This work provides a new idea of powder metallurgy method for modified Zn anodes, showcasing potential for large-scale production.

Synthesis of Hierarchical CF@Fe3O4 Fibers Decorated with MoS2 Layers Forming Core-Sheath Microstructure toward Tunable and Efficient Electromagnetic Wave Absorption.

Hierarchical structural design has been verified as a feasible strategy to fabricate effective electromagnetic wave (EMW) absorbers, so we designed hierarchical core-sheath composites with magnetic particles and dielectric layers. In this work, a hierarchical structure of carbon fiber (CF)@Fe3O4@MoS2 (CPDF7-M) was prepared by introducing Fe3O4 and depositing MoS2 layers on the surface of fibers. Due to the synergistic effects from the CF@Fe3O4 increasing the conductive and magnetic loss and the outer MoS2 layers improving the impedance matching, the optimal reflection loss (RL) value was -63.1 dB at 2.7 mm and the effective absorption bandwidth (EAB) was 9.1 GHz covering the X and Ku band. Moreover, the EAB values were adjusted with a specific MoS2 loading at different thicknesses, which provided the necessary reference for the construction of efficient and flexible absorbers in the EMW absorption fields.

Room-Temperature Salt Template Synthesis of Nitrogen-Doped 3D Porous Carbon for Fast Metal-Ion Storage.

The water-soluble salt-template technique holds great promise for fabricating 3D porous materials. However, an equipment-free and pore-size controllable synthetic approach employing salt-template precursors at room temperature has remained unexplored. Herein, we introduce a green room-temperature antisolvent precipitation strategy for creating salt-template self-assembly precursors to universally produce 3D porous materials with controllable pore size. Through a combination of theoretical simulations and advanced characterization techniques, we unveil the antisolvent precipitation mechanism and provide guidelines for selecting raw materials and controlling the size of precipitated salt. Following the calcination and washing steps, we achieve large-scale and universal production of 3D porous materials and the recycling of the salt templates and antisolvents. The optimized nitrogen-doped 3D porous carbon (N-3DPC) materials demonstrate distinctive structural benefits, facilitating a high capacity for potassium-ion storage along with exceptional reversibility. This is further supported by in situ electrochemical impedance spectra, in situ Raman spectroscopy, and theoretical calculations. The anode shows a high rate capacity of 181 mAh g-1 at 4 A g-1 in the full cell. This study addresses the knowledge gap concerning the room-temperature synthesis of salt-template self-assembly precursors for the large-scale production of porous materials, thereby expanding their potential applications for electrochemical energy conversion and storage.

Recent research progresses of Sn/Bi/In-based electrocatalysts for electroreduction CO2 to formate.

Carbon dioxide electroreduction reaction (CO2RR) can take full advantage of sustainable power to reduce the continuously increasing carbon emissions. Recycling CO2 to produce formic acid or formate is a technologically and economically viable route to accomplish CO2 cyclic utilization. Developing efficient and cost-effective electrocatalysts with high selectivity towards formate is prioritized for the industrialized applications of CO2RR electrolysis. From the previous explored CO2RR catalysts, Sn, Bi and In based materials have drawn increasing attentions due to the high selectivity towards formate. However, there are still confronted with several challenges for the practical applications of these materials. Therefore, a rational design of the catalysts for formate is urgently needed for the target of industrialized applications. Herein, we comprehensively summarized the recent development in the advanced electrocatalysts for the CO2RR to formate. Firstly, the reaction mechanism of CO2RR is introduced. Then the preparation and design strategies of the highly active electrocatalysts are presented. Especially the innovative design mechanism in engineering materials for promoting catalytic performance, and the efforts on mechanistic exploration using in situ (ex situ) characterization techniques are reviewed. Subsequently, some perspectives and expectations are proposed about current challenges and future potentials in CO2RR research.

Reconstructed Bismuth Oxide through in situ Carbonation by Carbonate-containing Electrolyte for Highly Active Electrocatalytic CO2 Reduction to Formate.

The catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil the actual reaction mechanism during the CO2 electroreduction reaction (CO2 RR). However, currently the impact of the electrolyte microenvironment in which the electrolyte is in contact with the catalyst is overlooked and might induce a chemical evolution, thus confusing the reconstruction process and mechanism. In this work, the carbonate adsorption properties of metal oxides were investigated, and the mechanism of how the electrolyte carbonate affect the chemical evolution of catalysts were discussed. Notably, Bi2 O3 with weak carbonate adsorption underwent a chemical reconstruction to form the Bi2 O2 CO3 /Bi2 O3 heterostructure. Furthermore, in situ and ex situ characterizations unveiled the formation mechanism of the heterostructure. The in situ formed Bi2 O2 CO3 /Bi2 O3 heterostructure with strong electron interaction served as the highly active structure for CO2 RR, achieving a formate Faradaic efficiency of 98.1 % at -0.8 Vvs RHE . Theoretical calculations demonstrate that the significantly tuned p-orbit electrons of the Bi sites in Bi2 O2 CO3 /Bi2 O3 optimized the adsorption of the intermediate and lowered the energy barrier for the formation of *OCHO. This work elucidates the mechanism of electrolyte microenvironment for affecting catalyst reconstruction, which contributes to the understanding of reconstruction process and clarification of the actual catalytic structure.