Jucai Yang

Developing efficient and thermally stable red phosphors is important for high‐performance phosphor‐converted white light‐emitting diodes. Herein, Eu ³⁺ ‐activated LiTaGeO ₅ phosphors were synthesized by a solid‐state reaction and systematically investigated through combined experimental and theoretical approaches. Rietveld refinement and first‐principles calculations suggest that Eu ³⁺ preferentially occupies the Li site, while electronic structure calculations reveal localized Eu 4 f states without substantially altering the host framework. Under 394 nm excitation, LiTaGeO ₅ :Eu ³⁺ exhibits intense red emission at 611 ( ⁵ D ₀ → ⁷ F ₂ ) together with pronounced deep‐red emission near 704 nm ( ⁵ D ₀ → ⁷ F ₄ ). The optimized LiTaGeO ₅ :0.033Eu ³⁺ phosphor shows a photoluminescence quantum yield of 51.06% and retains approximately 86% of its initial emission intensity at 423 K, and has a thermal‐quenching activation energy of about 0.52 eV. A NUV‐pumped WLED achieves a CRI of 91 and a CCT of 4500 K. Transmission imaging, fluorescent anti‐counterfeiting, infrared thermography, and COMSOL simulations further demonstrate its potential for solid‐state lighting and optical applications.

Doping provides an effective means to tailor the chemical properties of clusters and construct novel functional materials. However, the specific effects of rare-earth doping on the structural evolution and electronic properties of semiconductor clusters remain unclear. To address this, we systematically investigated the structures, growth patterns, electronic properties, and spectroscopic characteristics of Ge_n⁻ and LaGe_n^0/− clusters (n = 10–20) using the ABCluster global search method combined with the mPW2PLYP double-hybrid density functional. Notably, the global minimum (GM) structures of Ge_n⁻ (n = 12–20), confirmed based on calculated energies and measured photoelectron spectroscopy data, differ from previously reported structures. Starting from n = 12, the GM structure of the Ge_n⁻ cluster can be considered as formed by attaching an additional Ge_(n–9) or Ge_(n–10) subcluster to a capped tetragonal antiprism Ge₉ (or dicapped tetragonal antiprism Ge₁₀) subunit. The evolution pattern of LaGe_n (n = 10–19) clusters can be viewed as substitutional structures, in which a La atom substitutes one Ge atom in the Ge_(n+1)⁻ cluster. At n = 20, a cage-like structure is formed. For LaGe_n⁻ (n = 10–19), when n = 10–12 and 18, the structures are linked configurations, where the La atom connects two Ge subclusters. For the remaining clusters, although their global minimum structures tend toward linked configurations, they are fundamentally substitutional in nature. The GM structure of LaGe₂₀⁻ is an encapsulated configuration, with the La atom encapsulated at the center of the Ge cage. The average binding energies, relative stabilities, and HOMO–LUMO energy gaps of the clusters were evaluated. The photoelectron spectra of LaGe_n⁻ (n = 10–20) and the UV–vis absorption spectrum of the LaGe₂₀⁻ cluster were simulated. The results demonstrate that the LaGe₂₀⁻ superatom cluster with high Ih symmetry exhibits favorable optical properties, along with excellent chemical and thermodynamic stability, suggesting its potential as a promising building block for further exploration in optoelectronic-related applications.

The electrocatalytic reduction of CO₂ (CO₂RR) into value-added chemicals represents a promising strategy for achieving carbon-neutral energy conversion. However, it is fundamentally limited by sluggish reaction kinetics, insufficient product selectivity, and the competitive hydrogen evolution reaction (HER). Herein, density functional theory (DFT) calculations were employed to systematically investigate transition-metal single-atom catalysts anchored on boron and nitrogen co-doped graphene (TM@BNG), with the aim of elucidating the role of heteroatom-induced coordination engineering in modulating catalytic performance. The results demonstrate that B, N co-doping effectively tailors the electronic structure of the metal active sites, thereby optimizing the adsorption energetics of key intermediates and dictating the reaction pathways. Among the 27 candidates examined, Pd@BNG, Ag@BNG, Sc@BNG, Cu@BNG, Co@BNG, Cd@BNG, and Y@BNG exhibit superior catalytic activity and selectivity toward CO or HCOOH production, featuring low limiting potentials down to −0.06 V while simultaneously suppressing HER. Mechanistic analysis reveals that product selectivity is governed by the relative stabilization of *COOH and *HCOO intermediates during the initial proton-coupled electron transfer step. Furthermore, a physically interpretable descriptor (φ), derived from intrinsic electronic properties using machine-learning approaches, establishes a volcano-type correlation with the limiting potential and provides an effective activity-screening criterion within the investigated TM@BNG dataset. Collectively, these findings clarify the electronic-structure modulation of TM@BNG single-atom catalysts and provide a system-specific framework for screening related B/N-coordinated CO₂RR electrocatalysts.

The electrocatalytic reduction of CO₂ (CO2RR) into value-added chemicals represents a promising strategy for achieving carbon-neutral energy conversion. However, it is fundamentally limited by sluggish reaction kinetics, insufficient product selectivity, and the competitive hydrogen evolution reaction (HER). Herein, density functional theory (DFT) calculations were employed to systematically investigate transition-metal single-atom catalysts anchored on boron and nitrogen co-doped graphene (TM@BNG), with the aim of elucidating the role of heteroatom-induced coordination engineering in modulating catalytic performance. The results demonstrate that B, N co-doping effectively tailors the electronic structure of the metal active sites, thereby optimizing the adsorption energetics of key intermediates and dictating the reaction pathways. Among the 27 candidates examined, Pd@BNG, Ag@BNG, Sc@BNG, Cu@BNG, Co@BNG, Cd@BNG, and Y@BNG exhibit superior catalytic activity and selectivity toward CO or HCOOH production, featuring low limiting potentials down to −0.06 V while simultaneously suppressing HER. Mechanistic analysis reveals that product selectivity is governed by the relative stabilization of *COOH and *HCOO intermediates during the initial proton-coupled electron transfer step. Furthermore, a physically interpretable descriptor (φ), constructed via machine-learning approaches based on intrinsic electronic properties, establishes a volcano-type correlation with the limiting potential, thereby enabling quantitative prediction of catalytic activity. Collectively, these findings elucidate the electronic-structure modulation of single-atom catalysts and establish a generalizable framework for the rational design of high-performance CO₂RR electrocatalysts.

Silver metal‐doped silicon clusters possess properties that are crucial for advancing microelectronics, catalysis, and energy storage technologies. In the present study, the equilibrium geometry and the growth pattern of silver‐doped silicon anionic cluster AgSi _n ⁻ ( n = 3 – 20) were systematically studied using mPW2PLYP schemes in combination with the global search technique. The growth pattern of AgSi _n ⁻ clusters can be summarized as follows: For n = 3–10, the Ag atom is adsorbed on the surface of the pure Si _n structure; starting at n = 11, the configuration transitions to a substitutional type where an Ag atom replaces a Si atom in the pure Si _{n +1} structure. Simulated photoelectron spectroscopy (PES) and Raman spectra, which are employed for structural identification, are presented and compared with previously reported experimental PES. Besides that, the relative stabilities, HOMO–LUMO gaps, and natural population analysis were also performed. This study provides theoretical insights for the future discovery of novel functional cluster nanomaterials.