Latest ArticlesModulating the exposed facets of metal-organic frameworks (MOFs) is an effective strategy to enhance the synergistic effects between adsorption and photocatalytic reduction of U(Ⅵ). Herein, we successfully synthesized four morphologically distinct types of NH2-MIL-125(Ti), offering insights into the impact of facet engineering on the combined adsorption and photoreduction of U(Ⅵ). An elevated exposure ratio of the {001} facet endows NH2-MIL-125(Ti) with a larger surface area, enhanced light absorption, and efficient separation of photogenerated charge carriers. Among the four photocatalysts (W, D, S and T), T with a high proportion of {001} facets, demonstrated outstanding adsorption-photocatalytic synergy, achieving over 97% of U(Ⅵ) within 20 min of visible light irradiation across a broad concentrations and pH range, without requiring a hole-trapping agent. The uranium extraction mechanism involves U(Ⅵ) coordination and chelation with active sites during adsorption, followed by reduction to U(Ⅳ) via photogenerated electrons during photocatalysis. This study highlights the use of facet engineering to enhance adsorption and photocatalytic efficiency in MOF-based photocatalysts.
Water electrolysis for practical applications faces challenges such as slow kinetics of catalysts in oxygen evolution reaction (OER). These can be effectively improved by facilitating the migration of oxygen intermediates at the material's interface. In this work, we employed carbon dots to modify a heterophase Ir-based oxide catalyst (h-IrO2@CDs) to improve their acidic OER performance. Experimental and theoretical studies reveal that CDs enhances oxygen intermediate migration between rutile and 1T phases, enabling a synergistic oxidation pathway. The small amount addition of CDs reduces energy barriers in the rate-determining step and mitigates excessive oxidation, which significantly boost catalytic activity and stability of IrO2@CDs. The optimal h-IrO2@CDs-3 catalyst achieves a low overpotential (161 mV) for 10 mA/cm2 OER current and remains stable for > 762 h at 10 mA/cm2. The low cost and easy synthesis make CDs highly promising for enhancing overall performance in catalytic fields.
Proton-conducting materials are essential for energy and electronic technologies. Polyoxometalates (POMs), as molecularly well-defined metal oxide nanoclusters with high proton conductivity, are promising candidates for such applications. However, their intrinsic crystalline brittleness poses significant challenges for practical device processing. In this work, we present a strategy to incorporate POM nanoclusters into supramolecular ionic networks (SINs). By using synergistic electrostatic and hydrogen bonding interactions, we uniformly disperse POM nanoclusters into zwitterionic liquids, forming an ionic network structure. The resulting POM-based SIN electrolytes exhibit semi-solid flexibility and high proton conductivity of 2.0 × 10-3 S/cm. Notably, these electrolytes demonstrate strong adhesion with activated carbon electrodes, resulting in flexible supercapacitors with a stable electrolyte-electrode interface that retains 90% capacitance after 14,000 charge-discharge cycles and 10,000 bending cycles. This study provides a promising approach for developing nanocluster-based soft electrolyte materials for flexible devices.
Lithium-ion batteries (LIBs) are essential energy storage devices widely used in portable electronics, transportation, and various other applications. However, current anode materials, with their low intercalation potentials and poor rate performance, struggle to balance energy density, power density, and safety, particularly under extreme conditions. In this work, we report a self-regulating micro-channel network that forms a three-dimensional (3D) composite electrode architecture without binders and conductive additives, offering a promising anode solution for fast-charging LIBs. Benefiting from the robust 3D architecture with abundant Li+ active sites and superior electronic conductivity, the niobium tungsten oxide@carbon nanotube (NWO/CNT) composite electrode demonstrates a high reversible capacity (246.6 mAh/g at 0.2 C), excellent rate capability (117.1 mAh/g at 60 C), and long-term durability (73.0% capacity retention after 10,000 cycles). Additionally, a thick electrode with high mass loading (10 mg/cm2) shows remarkable high-rate performance, retaining 51.7% capacity at 20 C. Notably, when paired with LiFePO4 (LFP) cathodes, the NWO@CNT//LFP@CNT full batteries exhibit impressive high-power capability (2.8 kW/kg), high energy density (394.2 Wh/kg), and exceptional cycle stability (82% capacity retention after 6000 cycles). Most importantly, this composite electrode architecture also enables the fabrication of a planar, miniaturized, all-solid-state lithium-ion battery with fast-charging capabilities.
Ruthenium, possessing a comparable metal-hydrogen bond energy to Pt, has emerged as a promising electrocatalyst for the hydrogen oxidation reaction (HOR), but its practical applications are hindered by susceptibility to deactivation or dissolution under operating conditions of fuel cells. Herein, graphene-encapsulated Ru nanoparticles (Ru@NG) was employed as the HOR catalyst for high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs). The graphene shells on the Ru can block effectively the surface adsorption of phosphoric acid in electrolyte and CO in anode fuel, but does not affect H2 free access to Ru sites, thus increase the activity expression and stability of catalysts under the high temperature, strong acid, and oxidation conditions of the HT-PEMFCs. With Ru@NG as the anode catalyst, the fuel cell delivers a peak power density of 760 mW/cm2 with pure H2, and additionally, it shows better tolerance to CO that the performance is 1.5 times that of the Pt/C catalysts with H2 fuel containing 1% CO. This work provides an alternative strategy to design the electrocatalysts for HT-PEMFCs.
Ferroelastics have attracted considerable interest because of their promising uses in areas such as energy conversion, sensing technologies, and beyond. However, exploring ferroelastics with high-temperature dielectric switching and photoluminescence remains a challenge. Here, we have synthesized two ferroelastics (DMTP)PbBr3 (DMTP = N,N-dimethyl-1,2,3,6-tetrahydropyridine) and (DMTP)PbI3 under the guidance of halogen substitution strategy. (DMTP)PbI3 experiences the dielectric switching at 371 K, and upon halogen substitution, the strengthened intermolecular interactions lead to (DMTP)PbBr3 undergoing a similar switching at around 390 K. Additionally, two compounds both emit orange light under ultraviolet illumination. (DMTP)PbI3 has the photoluminescence quantum yield of 2.68%, while (DMTP)PbBr3, due to the increased distortion of the inorganic part after halogen substitution, achieves the higher quantum yield of 12%. This work offers meaningful perspectives on exploring the search for ferroelectrics with photoluminescence and high-temperature dielectric switching, and also demonstrates the rationality of the halogen substitution strategy.
Alkali metal-ion batteries, such as lithium-ion and sodium-ion batteries, have been widely recognized by both academia and industry for their high energy density, long cycle life, low self-discharge rate, and environmental friendliness. Theoretical calculations are crucial in elucidating the energy storage mechanism of alkali metal-ion batteries and in designing the next generation of high-performance energy storage systems. This article reviews the application of theoretical calculations in alkali metal-ion batteries. These calculations are instrumental for experimental researchers in understanding the microscopic design of electrode materials, optimizing various interfaces and electrolyte structures, and clarifying ion and electron transport behaviors as well as electrochemical reaction mechanisms. Specifically, researchers typically calculate the reduction reactions, charge state changes, and structural changes of cathode materials to predict their electrochemical reactivity and optimize their performance and stability. Calculations and simulations of alkali metal batteries focus on ion transport dynamics within the electrolyte, including energy level distribution, solvation structure, and molecular dynamics simulations. Analyzing oxidation reactions, ion diffusion, and volume changes in various alkali metal-ion battery anode materials enables the screening and design of new anode materials with superior electrochemical properties. This review also discusses the challenges of applying theoretical calculations in alkali metal-ion batteries and provides an outlook for future research. Critical insights are offered for advancing research paradigms that integrate theoretical and experimental approaches in the development of energy storage electrode materials.
Chirality, a fundamental property of biological systems, is widely present at the molecular, cellular, and tissue levels. Current studies have shown that chiral inorganic nanomaterials, have good chiral optical activity as well as high enantioselectivity. When interacting with biological systems, the enantioselective behavior of chiral inorganic nanomaterials towards biomolecules can distinguish between different isomers of biomarkers, which, combined with the excellent optical activity of chiral inorganic nanomaterials, allows for the rapid and sensitive detection of biomarkers. Moreover, chiral inorganic nanomaterials exhibit stronger internalization and retention capabilities in cells, and by specifically targeting specific biomarkers can regulate cellular activity and catalyze related reactions, thereby achieving synergistic treatment of various diseases. In addition, chiral inorganic nanomaterials also have good biocompatibility and do not cause cell damage in living organisms. Moreover, chiral inorganic nanomaterials have programmable surfaces that can be tailored to suit specific biological functions. Due to the important role of chiral inorganic nanomaterials in the biomedical field, this paper summarizes and discusses the synthesis and biomedical applications of chiral inorganic nanomaterials. It further looks forward to its future development prospects to provide a reference for promoting relevant research on chiral inorganic nanomaterials in biomedical fields.
The application of commercial hard carbon (HC) materials in sodium-ion batteries (SIBs) is limited by their inferior rate capability (<5.0 A/g) and low tap density (<1.0 g/cm3). Alloying-type bismuth (Bi) offers a high theoretical volumetric capacity of 3800 mAh/cm3 and superb rate capability but suffers from large volume expansion (~244%) and undesirable structural pulverization. Herein, a hectogram-scale Bi-inlaid carbon skeleton (GC-Bi) composite was synthesized through a facile precipitation-carbonization method using low-cost industrial-grade chemical reagents. The as-prepared GC-Bi composite features a unique particle-nested-bulk architecture, achieving a high tap-density of 3.33 g/cm3, which is approximately 4.16 times greater than that of commercial HC. Besides, the carbon sheath enhances the electronic conductivity and accommodates the substantial volume swelling of the embedded Bi particles, contributing to the formation of a thin and stable solid electrolyte interface on the electrode. Consequently, the GC-Bi anode achieves a high volumetric capacity (1123 mAh/cm3), impressive rate capability (207.8 mAh/g at 80 A/g), together with long cyclability retaining 96.5% of its capacity after 5000 cycles in a Na//GC-Bi half-cell and 78% after 800 cycles in a GC-Bi//Na3V2(PO4)3 full-cell.
Reversible modulation of the transmittance in electrochromic devices (ECDs) holds tremendous potential for energy-saving windows. The choice of electrolyte significantly influences the optical modulation, coloring response speed, coloring efficiency, and cycling stability of electrochromic devices. Moreover, traditional electrolytes are prone to instability under extreme temperature conditions, leading to device failure and severely limiting the widespread application of smart electrochromic windows. This study introduces LiCl water-in-salt electrolyte (WiSE) into tungsten oxide-based ECDs. LiCl WiSE exhibits wide-temperature tolerance and excellent ion conductivity. Therefore, the constructed tungsten oxide ECD demonstrates large optical modulation (76.2%@700 nm), fast response time (tc = 2.0 s, tb = 1.8 s), and high cycling stability (95.8% retention after 1000 cycles). Especially, it operates efficiently over a wide temperature range of -30~80 ℃. This research provides a new approach for electrolyte selection in the fabrication of high-performance, wide-temperature-tolerant ECDs.
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