Energy & Environmental Materials最新文献

Uniform deposition is a promising strategy to inhibit dendrite growth and corrosion of the Zn anode in cost-effective energy storage systems: aqueous Zn-ion batteries (AZIBs). Herein, we report a regulating Zn²⁺ ions dissolution/deposition method for achieving a highly reversible Zn anode. 11-mercaptoundecanoic acid (MUA) as ligands was utilized to protect the (002) plane, benefiting from the strong affinity between the thiol group and Zn, with MUA anchoring in the form of Zn-S-RCOOH, which contributes to a stable interface for uniform deposition/deposition. More importantly, the MUA bonds to the (002) plane tightly and acts as a “rivet,” strengthening the Zn–Zn bonds of the (002) plane and leading to the high exposure of the (002) plane during the plating and stripping process. The MUA@Zn anode with 50 μm ultrathin thickness exhibits excellent stability (over 4000 h) and low overpotential at high current density (0.1–23 mA cm⁻²) and capacity (0.1–23 mAh cm⁻²). In addition, it also delivers a capacity of 194.1 mAh g⁻¹ at 1 A g⁻¹ and capacity retention of 95% after 1000 cycles. Consequently, our work provides a facial yet interfacial engineering approach in realizing the enhancement of Zn anode stability, exhibiting significant potential for practical application in AZIBs.

Understanding and managing charge carrier recombination dynamics is crucial for optimizing the performance of metal halide perovskite optoelectronic devices. In this work, we introduce a machine learning-assisted intensity-modulated two-photon photoluminescence microscopy approach for quantitatively mapping recombination processes in MAPbBr₃ perovskite microcrystalline films at micrometer-scale resolution. To enhance model accuracy, a balanced classification sampling strategy was applied during the machine learning optimization stage. The trained regression chain model accurately predicts key physical parameters—exciton generation rate ($��G�$), initial trap concentration ($��N_{\mathrm{TR}}�$), and trap energy barrier ($��E_a�$)—across a 576-pixel spatial mapping. These parameters were then used to solve a system of coupled ordinary differential equations, yielding spatially resolved simulations of carrier populations and recombination behaviors at steady-state photoexcitation. The resulting maps reveal pronounced local variations in exciton, electron, hole, and trap populations, as well as photoluminescence and nonradiative losses. Correlation analysis identifies three distinct recombination regimes: 1) a trap-filling regime predominated by nonradiative recombination, 2) a crossover regime, and 3) a band-filling regime with significantly enhanced radiative efficiency. A critical trap density threshold (~10¹⁷ $��{\mathrm{cm}}^{�-�3�}�$) marks the transition between these regimes. This work demonstrates machine learning-assisted intensity-modulated two-photon photoluminescence microscopy as a powerful framework for diagnosing carrier dynamics and guiding defect passivation strategies in perovskite materials.

Promising aqueous zinc metal batteries (AZMBs) continue to face significant challenges regarding zinc anode reversibility due to detrimental reactions including hydrogen evolution and corrosion. Herein, the d-band center is used as an “intuitive descriptor” to compare the hydrogen evolution activity of zinc-based transition bimetallic oxides (ZTBOs) of fourth-period transition metal elements, and the advantages of ZnTi₃O₇ (ZTO) functional protective layer in inhibiting hydrogen evolution and extending the lifespan of the zinc anode are selectively identified. The ZTO exhibits a lower d-band energy level, which affects the adsorption of active H* and exhibits lower hydrogen evolution reaction activity. At the same time, the dense ZTO protective layer provides suitable ion channels to promote the uniform distribution of zinc flux and achieve uniform Zn deposition. Thus, cells with Zn@ZTO anodes exhibit over 6000 h of cycling stability (1 mA cm⁻²) and a high coulombic efficiency of 99.9% within 1200 cycles. Moreover, when paired with a V₆O₁₃ cathode, the assembled full cell exhibits excellent lifespan, retaining 86.9% of its capacity after 5000 cycles at 10 A g⁻¹. This work provides new strategies and insights for designing inorganic protective layers, addressing HER-related challenges, and advancing the practicality of AZMBs.

Photoswitchable catalysis provides a non-invasive strategy for dynamically controlling light-driven chemical energy conversion processes. The defining advantage of photoswitchable catalytic systems lies in their unique dual capacity: i) spatiotemporal precision in resolving reactive species generation through optical addressing; and ii) adaptive multifunctionality enabling on-demand switching between distinct active phases, thereby suppressing competing pathways and eliminating undesired side reactions. Current research paradigms remain predominantly anchored in molecular systems, whereas solid-state semiconductor architectures—with their inherent advantages in recyclability and thermal stability—suffer from critical deficiencies in excitation-selective reactivity modulation and interfacial charge transfer kinetics. Here we comment on a recent work, writing in National Science Review, reported spin–orbit coupling-mediated control over anti-Kasha photophysical pathways in semiconductors of carbonylated carbon nitride, enabling optically switchable catalytic dynamics. We further analyzed the profound implications of this work and presented a forward-looking outlook on the future development of the photoswitchable catalysis.

High-entropy ceramics have exhibited promising application prospects in aerospace, electronic devices, and extreme environment protection. Current powder sintering routes for preparing high-entropy ceramics are hindered by stringent powder requirements, reliance on long-term high-temperature and high-pressure synthesis, as well as compositional inhomogeneity and coarse grains. In this work, the low-temperature glass crystallization method was innovatively introduced into the preparation of high-entropy ceramics. Using garnet-structured rare-earth aluminates (RE₃Al₅O₁₂, RE is rare-earth elements) as a model system, a series of single-phase RE₃Al₅O₁₂ ceramics with entropy gradients were successfully synthesized through the glass crystallization method at a low temperature (1000 °C). Notably, the as-prepared (Eu_0.2Gd_0.2Y_0.2Yb_0.2Lu_0.2)₃Al₅O₁₂ (HEC) samples exhibited a low thermal conductivity of 3.58 W m⁻¹ K⁻¹ (at 300 K) and a high thermal expansion coefficient (TEC) of 10.85 × 10⁻⁶ K⁻¹, representing a 21% reduction in thermal conductivity and a 32% increase in TEC compared to reported Yb₃Al₅O₁₂ ceramics. The HEC samples also exhibited superior mechanical properties compared to most existing high-entropy ceramics, with a hardness of 22.08 GPa and a Young's modulus of 311.6 GPa. The exceptional comprehensive properties of the HEC samples make them a promising candidate material for thermal barrier coatings (TBCs) and high-temperature structural applications. This investigation confirms that high-entropy ceramics with outstanding properties can be successfully prepared using a glass crystallization method, providing a novel strategy for the low-temperature and pressureless controllable synthesis of single-phase high-entropy ceramics.

This study enhances quantum dot-sensitized solar cells (QDSSCs) with a photoanode containing gold and silver nanoparticles in a diamond-like carbon (DLC) matrix. The nanoparticles exhibit a synergistic effect, increasing the photoanode's response to visible light through localized surface plasmon resonance (LSPR). Simulations show that these nanoparticles improve charge transfer and cell efficiency by creating additional electron traps. DLC acts as a shield, protecting silver nanoparticles from corrosion, thus enhancing cell stability. The modified photoanode significantly increases the short-circuit current density compared to the standard photoanode, confirming the simulation results and demonstrating the potential for improved solar cell performance.

The emerging n-type Mg₃(Sb, Bi)₂-based materials have attracted considerable attention for their excellent thermoelectric performance. Whereas, practical thermoelectric device applications require materials that exhibit not only superior thermoelectric performance but also robust mechanical properties. This work systematically investigates the mechanical and thermoelectric properties of Mg_3.2-xCe_xSbBi_0.97Te_0.03. The x = 0.04 sample exhibits a Vickers hardness of up to 1012 MPa. The compressive and bending stress–strain curves show that minor doping can enhance the strength while maintaining high plasticity. The superior mechanical characteristics are attributed to dense dislocations and lattice distortions induced by Ce doping. Furthermore, the thermoelectric evaluation shows that the trivalent rare earth Ce element acts as a moderately efficient dopant, leading to increased carrier concentration to 4.55 × 10¹⁹ cm⁻³. However, both the electrical conductivity (σ) and Seebeck coefficient (S) gradually decrease with the increase of Ce doping, particularly at high doping levels (x = 0.04 and 0.06), leading to the slight decrease in power factor. Meanwhile, Ce doping introduces point defects, lattice distortions, and dislocations, thereby enhancing the phonon scattering and reducing the lattice thermal conductivity (к_L). As a result, an ultralow к_L of ~0.51 W m⁻¹ K⁻¹ and a peak zT of ~1.52 are achieved for the sample of x = 0.02. This work provides some insights into the synergistic enhancement of thermoelectric and mechanical properties in Mg₃(Sb, Bi)₂-based compounds, inspiring further exploration of their practical applications in thermoelectric devices.

High-entropy spinel oxides are promising anode materials for lithium-ion batteries owing to their unique crystal structures, which provide enhanced structural stability, multiple redox-active sites, and three-dimensional Li⁺ diffusion pathways. However, the intrinsic complexity and compositional diversity of high-entropy systems have limited a comprehensive understanding of the correlation between crystal structure, elemental composition, and rate performance, thereby impeding further optimization and practical application. In this study, a high-entropy spinel oxide (Fe_0.2Co_0.2Ni_0.2Cr_0.2Zn_0.2)₃O₄ (FCNCZO) is synthesized to investigate its electrochemical properties. The material delivers a high reversible capacity of 551 mAh g⁻¹ at 500 mA g⁻¹ after 110 cycles and maintains an excellent rate capability of 330 mAh g⁻¹ at a high current density of 2000 mA g⁻¹. Density functional theory calculations indicate that the synergistic interaction among multiple metal elements reduces the bandgap and broadens the d-band width. Moreover, the high-entropy effect promotes metal-oxygen orbital hybridization, facilitates charge redistribution, and significantly enhances rate capability. These findings provide new microscopic insights into the high-entropy effect and demonstrate its potential in designing next-generation high-entropy anode materials with superior rate performance for high-power lithium-ion batteries.

This study developed a symbiotic dual-confinement strategy integrating interstitial oxygen doping and carbon coating to enhance high-entropy alloys for high-current-density zinc-air batteries. Through the combination of theoretical cluster models with the experimental synthesis of MnFeCoNiCu@C high-entropy alloys, the synergistic suppression of demetalization and kinetic optimization was investigated. The dual-confined high-entropy alloys exhibited no significant attenuation for 1600 h in zinc-air batteries and resisted large current of 100 mA cm⁻² impacts, with density functional theory calculations confirming lower d-band centers and higher formation energies, correlating with enhanced durability and reaction kinetics. This approach simultaneously addresses atomic-scale metal dissolution and nanoscale mass transfer limitations, surpassing conventional coating strategies. The findings establish a framework for designing robust high-entropy alloys, advancing their application in high-demand electrocatalysis and energy conversion technologies.

In this study, lithium carbonate (Li₂CO₃) sourced from the Salar de Uyuni salt flat in Bolivia was used in the synthesis of cathode active material for Li-ion batteries. X-ray diffraction, atomic absorption spectrometry, and scanning electron microscopy analyses confirmed that the material had a high phase purity (99.59%, battery-grade) and a suitable morphology for active material synthesis, comparable to a similar commercially obtained material. Li[Ni_1/3Mn_1/3Co_1/3]O₂ (NMC111) was synthesized as a model system using Li₂CO₃ as the precursor and evaluated in full, large-format pouch cells along with three-electrode cells, using commercially relevant active material fractions and mass loadings for meaningful assessment of electrochemical performance. These cells exhibited capacities close to theoretical values and similar to that of commercially obtained NMC111, demonstrating the viability of the raw material. Operando X-ray diffraction analysis of aged pouch cells revealed that capacity loss was due to depletion of lithium inventory, without any disruption to the long-range cathode crystal structure or significant degradation in lithium kinetics. Postmortem analysis of the cycled electrodes further confirmed that transition metal dissolution and lithium trapping on the anode side were key contributors to the capacity fading observed in the pouch cells. This work demonstrates the potential of Salar de Uyuni's lithium resources for the production of cells relevant to practical applications.