Most of phosphors undergo thermal quenching (TQ) at high temperature, due to thermal-activated non-radiative transitions. TQ effects lead to significant reduced luminous efficiency of phosphors at high operation temperature, hindering their application in high power phosphor-converted white light-emitting diodes (WLED). Here, we report a zero-dimensional metal halide perovskite: Cs2ZrCl6:Sb3+, exhibiting robust anti-TQ red emission up to 500 K, comparable to the mainstream anti-TQ phosphors (e.g. K2SiF6:Mn4+). The hetero-valent doping of Sb3+ induces structure defects of host and thus compensate the non-radiative emission loss through thermal accelerated energy transfer from defects to emitter at high temperature. We assembled the red anti-TQ phosphor into a white light-emitting diode (WLED) device, achieving stable output light intensity and chromaticity up to 2000 mA.
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Open Access
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The transition to sustainable energy systems necessitates efficient hydrogen production via water electrolysis, with anion-exchange membrane water electrolyzers (AEMWEs) emerging as a cost-effective alternative by combining the merits of alkaline water electrolyzers (AWEs) and proton-exchange membrane water electrolyzers (PEMWEs). However, challenges persist in membrane stability, oxygen evolution reaction (OER) kinetics, and mass transport efficiency. This review highlights the pivotal role of transition metal-based layered double hydroxides (LDHs) as high-performance, non-precious OER catalysts for AEMWEs, emphasizing their tunable electronic structures, abundant active sites, and alkaline stability. We systematically outline LDHs synthesis strategies (top-down/bottom-up approaches, and self-supporting LDHs engineering on the conductive substrates), and AEMWE component design, including membrane-electrode assembly optimization and ionomer-free architectures. Standardized evaluation protocols-short-circuit inspection, impedance spectroscopy, and durability assessment are detailed to benchmark performance. Moreover, recent advances in LDHs modification (cation/anion doping, heterojunction design, three-dimensional (3D) electrode structuring) are discussed for alkaline-fed systems, alongside emerging applications in seawater and pure-water electrolysis. By correlating material innovations with device-level metrics, this work provides a roadmap to address scalability challenges, offering perspectives on advancing AEMWEs for sustainable, large-scale hydrogen production.
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The development of sustainable hydrogen production technologies is critical to addressing the global energy crisis and environmental challenges. Among water electrolysis systems, anion-exchange membrane water electrolyzers (AEMWEs) have gained attention for their ability to combine cost-effectiveness with high efficiency. However, AEMWEs face challenges such as sluggish oxygen evolution reaction (OER) catalysts with low conductivity and density of active sites, especially with the feed stock of pure water. In this study, a tri-metal Prussian blue analogue (PBA) was synthesized at room temperature and employed as an efficient OER pre-catalyst. Electrochemical activation of this as-prepared material in the alkaline solution generates highly active and conductive crystalline-amorphous metal (oxy)hydroxides as the true catalytic sites, which exhibited exceptional OER performance with the overpotential of 251 mV at 10 mA·cm–2 and stable operation for 500 h in the alkaline solution. When applied as anode in AEMWEs, it delivered 1 A·cm–2 at 1.72 and 2.20 V with the feedstock of alkaline solution (1 M KOH) and pure water, respectively, demonstrating its large application prospect in AEMWE.
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Herein, we fabricate a well-patterned semiconductor ripple structure via confined Couette flow of a quantum dot solution between two glass slides. This method is broadly applicable to diverse colloidal quantum dots, including environmentally friendly CuInxGa1−xS2, InP, and ZnSe nanocrystals. The resulting ripple structure demonstrates strong linear dichroism and polarization capabilities for lasers across a broad wavelength range (445–635 nm). Our work offers a convenient, solution-processable strategy for fabricating semiconductor-based polarizer films.
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The development of efficient and stable visible-light-driven hydrogen (H2) generation photocatalysts plays a crucial role in sustainable energy conversion. In this study, we constructed an all-solid Z-scheme heterostructure by integrating carbon quantum dots (CQDs) as a photogenerated carrier transfer bridge between ZnIn2S4 and CeO2. The unique structure of ZnIn2S4/CQDs/CeO2 facilitates the efficient separation and transfer of photogenerated electron-hole pairs, while the CQDs act as a solid-state electron mediator, enhancing interfacial charge transfer and suppressing recombination. Under visible-light irradiation (λ ≥ 420 nm), when the concentration of ZnIn2S4 is 40%, the hydrogen generation rate of ZnIn2S4/CQDs/CeO2-2 reaches 7.7 mmol·g−1·h−1, which is 12.8 times higher than that of unmodified ZnIn2S4 (0.6 mmol·g−1·h−1) and significantly greater than that of ZnIn2S4/CeO2 (4.2 mmol·g−1·h−1). Furthermore, the all-solid Z-scheme configuration ensures excellent stability, as demonstrated by prolonged cycling tests. We investigated CQDs as a bridge to facilitate the vector transfer of photogenerated electrons from ZnIn2S4 to CeO2 through density functional theory calculations. Additionally, X-ray photoelectron spectroscopy results confirmed the Z-scheme mechanism of photogenerated carrier transfer within the ZnIn2S4/CQDs/CeO2 heterojunction. This study not only demonstrates an effective approach for promoting charge transfer in nanocomposites using CQDs but also provides a new strategy for developing efficient hydrogen evolution photocatalysts without the involvement of precious metals.
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The electrochemical oxygen reduction reaction (ORR) is pivotal in energy conversion via a 4e− ORR pathway and green hydrogen peroxide production via 2e− ORR pathway. Transition metal single atom catalysts (TM SACs) have attracted intense attention in recent years for ORR due to their high activity and near maximum metal atom utilization. The future development of TM SACs for ORR requires improved understanding of reaction pathways, since currently the true origin of activity remains contentious owing to the lack of qualitative/quantitative information about active sites. Knowledge-guided design is imperative for the optimization of TM SACs performance in terms of activity and selectivity. This review focuses on the latest progress in the design of TM SACs for ORR, placing particular attention on efforts to elucidate reaction mechanisms. Experimental evidence based on in-situ/operando characterization measurements, along with theoretical predictions, are summarized to deepen understanding of the structure-performance relationships at both atomic and molecular level. Finally, some perspectives are offered relating to the fundamental science needed for TM SACs to find practical application in energy storage and conversion devices. We hope this review will inspire the development of new synthetic routes towards high-performance ORR electrocatalysts for the energy sector.
Hydrogen energy, a new type of clean and efficient energy, has assumed precedence in decarbonizing and building a sustainable carbon-neutral economy. Recently, hydrogen production from water splitting has seen considerable advancements owing to its advantages such as zero carbon emissions, safety, and high product purity. To overcome the large energy barrier and high cost of water splitting, numerous efficient electrocatalysts have been designed and reported. However, various difficulties in promoting the industrialization of electrocatalytic water splitting remain. Further, as high-performance electrocatalysts that satisfy industrial requirements are urgently needed, a better understanding of water-splitting systems is required. In this paper, the latest progress in water electrolysis is reviewed, and experimental evidence from in situ/operando spectroscopic surveys and computational analyses is summarized to present a mechanistic understanding of hydrogen and oxygen evolution reactions. Furthermore, some promising strategies, including alloying, morphological engineering, interface construction, defect engineering, and strain engineering for designing and synthesizing electrocatalysts are highlighted. We believe that this review will provide a knowledge-guided design in fundamental science and further inspire technical engineering developments for constructing efficient electrocatalysts for water splitting.
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The rational design of metal single-atom catalysts (SACs) for electrochemical nitrogen reduction reaction (NRR) is challenging. Two-dimensional metal–organic frameworks (2DMOFs) is a unique class of promising SACs. Up to now, the roles of individual metals, coordination atoms, and their synergy effect on the electroanalytic performance remain unclear. Therefore, in this work, a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations. For a specific metal, a proper metal-intermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities. The hybridization interaction strength can be quantitatively described with the p−/d- band center energy difference (Δd-p), which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance. The maximum free energy change (ΔGmax) and Δd-p have a volcanic relationship with OsC4(Se)4 located at the apex of the volcanic curve, showing the best NRR performance. The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and positions. This work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs.
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Developing highly active and robust oxygen evolution reaction (OER) electrocatalysts is still a critical challenge for water electrolyzers and metal–air batteries. Realizing the dynamic evolution of the intermediate and charge transfer during OER and developing a clear OER mechanism is crucial to design high-performance OER catalysts. Recently in Nature, Xue and colleagues revealed a new OER mechanism, coupled oxygen evolution mechanism (COM), which involves a switchable metal and oxygen redox under light irradiation in nickel oxyhydroxide-based materials. This newly developed mechanism requires a reversible geometric conversion between octahedron (NiO6) and square planar (NiO4) to achieve electronic states with both “metal redox” and “oxygen redox” during OER. The asymmetric structure endows NR-NiOOH with a nonoverlapping region between the dz2 orbitals and a1g* bands, which facilitate the geometric conversion and enact the COM pathway. As a result, NR-NiOOH exhibited better OER activity and stability than the traditional NiOOH.
Water splitting is important to the conversion and storage of renewable energy, but slow kinetics of the oxygen evolution reaction (OER) greatly limits its utility. Here, under visible light illumination, the p-n WO3/SnSe2 (WS) heterojunction significantly activates OER catalysis of CoFe-layered double hydroxide (CF)/carbon nanotubes (CNTs). Specifically, the catalyst achieves an overpotential of 224 mV at 10 mA cm−2 and a small Tafel slope of 47 mV dec−1, superior to RuO2 and most previously reported transition metal-based OER catalysts. The p-n WS heterojunction shows strong light absorption to produce photogenerated carriers. The photogenerated holes are trapped by CF to suppresses the charge recombination and facilitate charge transfer, which accelerates OER kinetics and boost the activity for the OER. This work highlights the possibility of using heterojunctions to activate OER catalysis and advances the design of energy-efficient catalysts for water oxidation systems using solar energy.
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