Energy & Environmental Materials最新文献

Seawater electrolysis has attracted considerable attention in hydrogen production. However, the chloride ions (Cl⁻) in seawater can corrode metal sites and decrease the lifespans of the oxygen evolution reaction (OER). Herein, we report a reversed-active sites strategy, converting Cl⁻-affinitive metal sites to Cl⁻-repellent oxygen sites, for OER in alkaline seawater electrolysis. First, ex/in situ experiments confirm the effectiveness of such a strategy using typical perovskites following the adsorbate evolution mechanism (AEM) or lattice oxygen-mediated mechanism (LOM). Furthermore, the origins of the superior activity and durability of as-prepared La_0.3SrCo_0.5Fe_0.5O_x (La0.3) can be ascribed to higher participation of lattice oxygen in OER, rapid bulk oxygen diffusion, and excellent OH⁻ adsorption kinetics. Hence, an alkaline seawater electrolytic cell with La0.3 as the anode produces 10 mA cm⁻² at just 1.57 V and maintains near-constant activity over 150 hours. This work introduces novel concepts for the production of superactive and steady electrocatalysts for the electrolysis of seawater.

Owing to its excellent eco-friendliness and facile water elution properties, aluminum-based lithium adsorbents have attracted a surge of interest for selectively extracting Li⁺ from Salt Lake brines, which account for more than 60% of the global lithium resources. However, structural collapse, facile deactivation during desorption process, and ultra-low actual adsorption capacity limit its further large-scale application, particularly in low-grade sulfate-type brines. Herein, considering its advantages, limitations, and structural features, the structural collapse of the aluminum-based lithium adsorbent was effectively suppressed by the in situ intercalation of VO₃⁻ and V₂O₇⁴⁻ into the interlayer of [LiAl₂(OH)₆]⁺. Evidently, the initial adsorption capacity and $��{\alpha }_{\mathrm{Mg}}^{\mathrm{Li}}�$ of as-configured adsorbents powder are 14.96 mg g⁻¹ and 192.42 in real sulfate-type West Taijinar Salt Lake brines following NaCl salts removal with 800 mg L⁻¹ Li⁺ and 9.56 g L⁻¹ SO₄²⁻. Furthermore, the initial and retained adsorption capacities of these novel adsorbents granulate in brines after 100 adsorption/desorption cycles are 26.68 and 10.36 mg g⁻¹, respectively, which are almost 10 times higher than those of industrially utilized products. Based on experiments and density functional theory calculations, the process and mechanism of anion intercalation control were preliminarily elucidated. Furthermore, research findings indicate that intercalated anions can influence not only interlayer interactions but also the backbone strength of LDH-type adsorbents. This work significantly overcomes the major utilization challenges of aluminum-based lithium adsorbents, thereby enabling the high-efficiency and stable extraction of Li⁺ from low-grade brines, including sulfate-type brines.

Traditional nanofiltration membranes face challenges such as membrane fouling and difficulties in achieving precise separation of small organic molecules. A promising solution to these issues is the preparation of thin-film nanocomposite membranes. In this study, Cu and Ag bimetals were incorporated into covalent organic frameworks to fabricate thin-film nanocomposite membranes. The hydrophilic monomer 1,3,5-tris(4-aminophenyl) benzene of covalent organic frameworks was introduced as a water phase monomer during interfacial polymerization to enhance the organic–inorganic compatibility. The incorporated covalent organic frameworks within the thin-film nanocomposite membrane loosened the selective layer, resulting in an enhanced permeability of 24.6 LMH bar⁻¹. The membrane exhibited a rejection rate over 99.0% for Congo Red, Xylene Brilliant Cyanine G, and Reactive Blue, while exhibiting relatively low rejection rates of MgCl₂ and NaCl. Moreover, the outstanding catalytic capability of the incorporated bimetals led to a 4-nitrophenol conversion rate of 84.38%, enabling simultaneous conversion and separation. The integration of covalent organic frameworks and bimetals also imparted robust antibacterial properties, significantly enhancing operational stability. In conclusion, the covalent organic framework-Cu/Ag-based thin-film nanocomposite membrane demonstrated superior catalytic and separation capabilities, presenting a promising alternative for advanced filtration applications.

With the growing global energy demand and the pressing need for a clean energy transition, supercapacitors (SCs) have demonstrated significant application potential in electric vehicles, wearable electronics, and renewable energy storage systems owing to their rapid charge–discharge capability, exceptional power density, and prolonged cycle life. The improvement of their overall performance fundamentally depends on the synergistic design of electrode materials and electrolyte systems, as well as the precise regulation of the electrode-electrolyte interface. This review focuses on the key components of supercapacitors, systematically reviewing the design strategies of high-performance electrode materials, outlining recent advances in novel electrolyte systems, and comprehensively discussing the critical roles of interfacial reinforcement and optimization in enhancing device energy density, power performance, and cycling stability. Furthermore, interfacial engineering strategies and innovations in device architecture are proposed to address interfacial degradation in flexible SCs under mechanical stress. Finally, key future research directions are highlighted, including the development of high-voltage and wide-temperature-range electrolyte systems and the integrated advancement of multiscale in situ characterization techniques and theoretical modeling. This review aims to provide theoretical guidance and innovative strategies for material design, contributing toward the realization of next-generation supercapacitors with enhanced energy density and reliability.

Unlike conventional electrochromic devices, Zinc anode-based electrochromic devices (ZECDs) ensure excellent charge balance between the electrochromic layer and Zn anode during the coloring/bleaching by reversible metal deposition/stripping on the Zn anode. Meanwhile, the inherent potential difference between the metal anode and the electrochromic layer can drive the spontaneous coloration/bleaching of ZECDs, featuring energy retrieval functionality. This review discusses the working mechanisms, performance indexes of ZECDs, and the impact of material selection on ZECD performance. Furthermore, we comprehensively summarize the latest research progress of ZECDs in energy storage, smart windows, and multicolor displays. We argue that using high-transparency zinc mesh, additive manufacturing processes, and self-healing electrochromic materials can significantly advance the commercialization of large-area ZECDs. Finally, “electrode-free” device structures, renewable or replaceable electrolytes, and strategies to suppress zinc dendrites are prospected to overcome cost-effectiveness and lifespan issues of ZECDs. This review aims at enabling more efficient and advanced ZECDs for multifunctional applications.

The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure–activity relationships. However, synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity. We herein propose a topological confinement pre-anchoring strategy via pre-anchoring spatially resolved Zn/Fe dual-metal sources in a structurally engineered metal–organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single-atom catalysts. Extended X-ray absorption fine structure measurements and X-ray absorption near-edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single-atom catalysts. The ultrahigh surface area, hierarchical pore, and synergistic effect between Zn/Fe can greatly favor the exposure of the active site, mass transport, and improvement of intrinsic activity. Consequently, the ZnFe bimetallic single-atom catalyst demonstrates superior oxygen reduction reaction performance, achieving a half-wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm⁻² at 0.85 V versus RHE in 0.1 m KOH electrolyte. These metrics not only surpass those of commercial Pt/C, but also rival the highest-performing catalysts reported to date. The Zn-air battery built with ZnFe bimetallic single-atom catalyst exhibits high power density (278.5 mW cm⁻²) and specific discharging capacities (657 mAh g⁻¹). This work provides a new design pathway for constructing atomically dispersed multi-metal electrocatalysts for high-performance energy-related applications.

While the instantaneous power of triboelectric nanogenerators (TENGs) has significantly increased, the average power remains unsatisfactory. Achieving a continuous and stable output remains a significant challenge. Herein, a self-excited vibration TENG inspired by woodpeckers is proposed. This structure converts gravitational potential energy into the continuous vibration of a cantilever beam. A dynamic simulation model of the system is established, and the influence of different structural parameters on the motion characteristics and electrical performance is discussed. Meanwhile, the experimental results indicate that the accelerated motion (approximate free-fall motion) is transformed into approximately uniform velocity motion. For a 3 cm² TENG, the instantaneous power density reaches 2.03 W m⁻², and the average power is 127% higher than that of the conventional cantilever beam mode. The proposed self-excited vibration mechanism is a promising approach for enhancing the average power and operational duration of TENGs. It shows great potential in fluid energy harvesting.

Magnesium batteries are attracting growing interest as next-generation energy storage technology due to their high safety, cost-effectiveness, and resource abundance. However, their development remains limited by sluggish Mg²⁺ transport kinetics at the electrode/electrolyte interface. Herein, we propose an electrolyte design strategy that modulates the Mg²⁺ solvation structure by introducing tetrahydrofuran (THF) as a co-solvent into a borate-based electrolyte, Mg[B(hfip)₄] (MBF) in dimethoxyethane (DME). THF, selected from a series of linear and cyclic ethers, has a comparable dielectric constant and donor number to DME, but its cyclic structure introduces steric hindrance that induces competitive coordination with Mg²⁺. This competition weakens Mg²⁺ − solvent interactions, yielding a more labile solvation structure and enhanced desolvation kinetics. As a result, Mg||Mg cells employing the optimized MBF/1D1T electrolyte (DME: THF = 1:1, v:v) exhibit a significantly reduced Mg plating/stripping overpotential of 120 mV at 10 mA cm⁻², compared with 316 mV at 8 mA cm⁻² with MBF/DME, along with exceptional cycling stability exceeding 1200 h. Furthermore, representative sulfide cathodes such as CuS and VS₄ demonstrate faster activation and improved high-rate performance in the presence of MBF/1D1T.

Zinc oxide (ZnO) films, as representative piezoelectric semiconductors, have garnered considerable interest in ultrasonic testing. Current research challenges include maintaining the consistency of continuous c-axis orientation and determining the fundamental link between the electrical structure and piezoelectric response. Accordingly, we have proposed ZnO films incorporated with an orientation-inducing layer (OIL), utilizing orientation induction and rapid deposition technology to regulate the growth structure of the ZnO films. Furthermore, the influence of the competitive mechanism between the film growth and lateral diffusion on the film's growth structure has been investigated. Piezoelectric force microscopy (PFM) analysis demonstrated the regulation and enhancement of ZnO piezoelectric polarization by the OIL. The enhancement mechanism of OIL on film performance was revealed via experimental examination of the film structure, morphology, crystallization orientation, oxygen vacancies, carrier concentration, band structure, and density of states based on density functional theory (DFT). Benefiting from the superior electromechanical response of the ZnO OIL sensor, characterized by fast response recovery times of 2.4 ms/7.7 ms and a sensitivity of 1.09 V/N, the device has successfully demonstrated practical applications in both motion pressure detection and bolt axial force measurement. These findings provide new insights into the ultrasonic detection for aerospace applications of ZnO OIL piezoelectric devices and demonstrate significant potential for health monitoring in connection systems.

Renewable electricity-driven production of value-added sulfur and H₂ via electrocatalytic H₂S decomposition represents a sustainable route to conventional thermocatalysis. Both the electrocatalyst and electrolyte solution strongly impact the H₂S decomposition performance. Despite significant progress in developing sophisticated electrocatalysts, a well-designed electrolyte solution in conjunction with industrial catalysts is an attractive strategy to advance the industrialization process of electrocatalytic H₂S decomposition, but remains unexplored. Here, for the first time, we design a solid–liquid–gas three-phase indirect electrolysis system based on a kind of CS₂-N electrolyte solution and Ni-Mo₂C that can efficiently enable H₂S decomposition into valuable H₂ and sulfur. Specifically, the solid-phase Ni-Mo₂C as a heterogeneous redox mediator presents excellent electrocatalytic efficiency for the H₂S removal efficiency of up to 99%, and the formation of liquid-phase sulfur product (CS₂-N electrolyte solution dissolves sulfur, yield up to 95%) with the generation of gas-phase H₂ product (~1.32 mL min⁻¹), resulting in an interesting three-phase indirect electrolysis system. Remarkably, it enables the scale-up production (~6 g in a batch experiment) of sulfur with continuous operation for 120 h without attenuation. This work may inaugurate a new electrocatalytic H₂S decomposition avenue to explore porous metal materials and electrolyte systems in simultaneous production of value-added sulfur and H₂.