Photo- and Electrocatalytic Dual-Layer Cathode Facilitating Zn Peroxide Chemistry in Near-Neutral Zn–Air Batteries

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 26, 2025

Rechargeable zinc-air batteries (ZABs) using near-neutral aqueous electrolytes are gaining significant attention due to their high energy density, low cost, safety, and the excellent reversibility of zinc (Zn) anode in mild electrolytes. However, sluggish O2/ZnO2 conversion carbon-based cathodes these leads a large voltage hysteresis (>600 mV) between charge discharge. Metal- or metal oxide-based electrocatalysts rarely used reduce overpotentials this because presence may trigger undesirable H2O-participated oxygen reduction/evolution reactions, disrupting pH balance electrolyte. Here, we propose dual-layer catalytic cathode comprising an outer photocatalyst layer (exposed air) gold (Au) nanoparticles (NPs) decorated tungsten oxide (Au@WO3) loaded on carbon paper, inner electrocatalyst electrolyte) based nanotube (CNT). The hydrophobic CNT not only provides numerous active sites ample accommodation for but also prevents electrolyte from contacting layer. Under light, effectively separates photogenerated electron–hole pairs, which then transferred layer, reducing overpotential electrochemical conversion. As result, ZAB demonstrates stability at 0.1 mA cm–2; with very small (<150 mV), significantly improving efficiency.

Language: Английский

---

High Entropy Oxide-Polyoxometalate Sub-1 nm Hetero-Nanowires as Cathode Catalysts in Li–O₂ Batteries

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 28, 2025

It is desirable for lithium-oxygen batteries (LOBs) to fabricate the cathode catalysts with high catalytic activity and stability. High entropy oxide (HEO) sub-1 nm nanowires (SNWs) nearly 100% active site exposure intrinsic stability are doubtless one of best candidates. Herein, under a mild solvothermal condition, by incorporating phosphomolybdic acid (PMA) into multimetal reaction system, series HEO-PMA SNWs successfully prepared, where variety metal oxides adjustable from mono component six components. When these as applied LOBs, capacity cycling LOBs steadily improved species increasing stepwise, indicating that modulation effect plays an important role in enhancing battery performance. Additionally, considering difference various oxides, performance further optimized keeping number elements constant just adjusting kind oxide. Particularly, BiCuFeCeWPtOx-PMA based delivers (11206 mA h g-1) excellent 213 cycles, making it promising electrocatalyst candidate LOBs.

Language: Английский

---

High‐Entropy Materials: from Bulk to Sub‐nano

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract High‐entropy materials (HEMs), characterized by their unique compositions involving multiple principal elements and inherent configurational disorder, have emerged as a focal point of material science research since introduction, owing to exceptional structural stability superior performance. The distinctive features HEMs, including the high‐entropy effect, lattice distortion, sluggish diffusion, cocktail enabled wide‐ranging applications in fields such energy storage, catalysis, electronic devices, beyond. This review systematically documents evolution HEMs synthesis, from traditional melting‐based methods for bulk production recent breakthroughs addressing limitations elemental immiscibility, ultimately enabling precise multi‐path synthesis nano‐ sub‐nano materials. It comprehensively examines controllable strategies across various dimensional scales, principles composition‐structure design, regulation multidimensional morphologies, multifunctional properties materials' multi‐component characteristics. Furthermore, this work prospectively explores emerging that could drive future development with particular emphasis on potential synergies between high‐throughput experimentation, data‐driven approaches, chiral factors, entropy‐driven strategies, advanced high‐resolution characterization techniques.

Language: Английский

---

Active‐Site‐Switching in Medium‐Entropy Metal Sulfides for Wide‐Temperature High‐Power Zn‐Air Pouch Cells

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Abstract Quasi‐solid‐state Zn‐air pouch cells (QZPCs) promise a high energy‐to‐cost ratio while ensuring inherent safety. However, addressing the challenges associated with exploring superior energy‐wise cathode catalysts along their activity origin, and super‐ionic electrolytes remains fundamental task. Herein, realistic high‐performance QZPCs are contrived, underpinned by robust NiVFeCo medium‐entropy metal sulfides (MESs) bifunctional air record‐low potential polarization of 0.523 V, paired sodium polyacrylate‐ionic liquid hydrogel exhibiting exceptional conductivity (234 mS cm −1 ) water retention (93.8% at 7 days) room temperature as conductor electrolyte. Through combined studies in situ Raman, ex X‐ray absorption fine structure analysis, theoretic calculations, an intriguing adaptive active‐sites‐switching mechanism MESs during discharging/charging processes is unveiled, revealing dynamic role transition Co Ni active sites reversible oxygen electrocatalysis. Consequently, persistent low super ion‐conductive electrolyte endorse excellent rate performance from 1 to 100 mA −2 temperature. Moreover, impressively cell‐level energy density 105 Wh kg cell ultra‐long cycle lifespan 4000 cycles 5 −30 °C achieved.

Language: Английский

---

High-entropy spinel oxides as efficient ORR catalysts towards enhanced kinetics for zinc-air batteries

Journal of Energy Storage, Journal Year: 2025, Volume and Issue: 123, P. 116784 - 116784

Published: April 25, 2025

Language: Английский

---

Laser Irradiated Noble Metal‐Free High Entropy Oxide 2‐D Sheets for Highly Efficient Anion Exchange Membrane Water Electrolyzers

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 25, 2025

Abstract High entropy oxides (HEOs) have recently emerged as excellent alternative catalysts that can potentially replace noble metal such RuO 2 and IrO for water splitting applications. However, existing methods of synthesizing these are often tedious. In this work, a straightforward method is proposed using ultra‐fast laser irradiation to synthesize heavily wrinkled metal‐free (CoCuFeMnNi) 3 O 4 HEO 2‐D sheets on nickel foam oxygen evolution reaction (OER) performance. These facilitate the OER at low overpotential only 245 mV achieve 10 mA cm −2 stable after 100 h testing. This performance outmatches majority reported HEA catalysts. As an anode in anion exchange electrolyzer (AEMWE), remarkably high current density 1.722 A achieved 2.0 V with negligible catalyst deterioration despite 70 result outranks other state‐of‐the‐art AEMWE today. work proves synthesis enables efficient catalysts, pioneer interconnected irradiation. Crucially, noble‐metal free HEOs highly durable industrial devices.

Language: Английский

---

Dual Z-scheme heterostructured polyoxometalate/activated carbon/TiO2 ternary composite for efficient photocatalytic N2 fixation

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 354, P. 129536 - 129536

Published: Sept. 4, 2024

Language: Английский

---

Entropy Engineering of 2D Materials

Advanced Science, Journal Year: 2024, Volume and Issue: 11(46)

Published: Oct. 23, 2024

Abstract Entropy, a measure of disorder or uncertainty in the thermodynamics system, has been widely used to confer desirable functions alloys and ceramics. The incorporation three more principal elements into single sublattice increases entropy medium high levels, imparting these materials mélange advanced mechanical catalytic properties. In particular, when scaling down dimensionality crystals from bulk 2D space, interplay between stabilization quantum confinement offers enticing opportunities for exploring new fundamental science applications, since structural ordering, phase stability, local electronic states distorted get significantly reshaped. During last few years, large family high‐entropy is rapidly expanding host MXenes, hydrotalcites, chalcogenides, metal‐organic frameworks (MOFs), many other uncharted members. Here, recent advances this dynamic field are reviewed, elucidating influence on properties underlying elementary mechanisms materials. their structure‐property relationships resulting theoretical predictions experimental findings discussed. Furthermore, an outlook key challenges such emerging also provided.

Language: Английский

---

Electrocatalytic oxidation of methane to low-carbon alcohol via stable Ni+/Ni0 interface

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 563, P. 114234 - 114234

Published: May 23, 2024

Language: Английский

---

Electrochemical Biosensor Based on Dual-Ligand Functionalized Lanthanide-Encapsulated Polyoxometalate Conductive Polymer Film for Detecting Broad-Spectrum Tumor Marker MicroRNA-155

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(46), P. 22149 - 22161

Published: Nov. 1, 2024

In this work, a dual-ligand functionalized lanthanide-encapsulated selenotungstate [H2N(CH3)2]16Na2H10[Ho6(H2O)10(HPACA)4W10O28(Ac)2][SeW9O33]6 · 60H2O (1, HPACA = 2-pyrazinecarboxylic acid, HAc acetic acid) was successfully acquired by simultaneously incorporating rigid and flexible Ac– ligands to one reaction system. Interestingly, the polyanion [Ho6(H2O)10(HPACA)4W10O28(Ac)2][SeW9O33]628– of 1 is composed six trivacant Keggin-type [B-α-SeW9O33]8– units interconnected through an organic–inorganic hybrid bimetallic [Ho6(H2O)10(HPACA)4W10O28(Ac)2]20+ cluster. Moreover, 1@PNMPy film (PNMPy poly(N-methylpyrrole)) prepared electrochemical polymerization strategy. The doping significantly narrows bandgap in film, which enables exhibit remarkable conductivity rapid electron transfer capability. Then, film-modified glassy carbon electrode used construct 1@PNMPy-based biosensor (ECBS), achieves sensitive detection (a low limit 0.108 fM wide concentration range 10–8–10–15 M) for broad-spectrum tumor marker microRNA-155. Also, ECBS has good specific recognition performance microRNA-155 variety interfering media. research not only contributes deeper understanding synthetic chemistry multicomponent polyoxometalate (POM)-based materials but also can further expand innovative applications POM-based devices.

Language: Английский

---