Surface and Defect Engineering Coupling of Charge Shuttle and Redox Site in Cs₃Bi₂Br₉/g-C₃N₄ for Efficient Photocatalytic C(sp³)–H Bond Activation

ACS Materials Letters, Год журнала: 2025, Номер unknown, С. 610 - 619

Опубликована: Янв. 16, 2025

Solar-driven organic synthesis using halide perovskites (HPs) has garnered much attention, but their unsatisfactory conversion efficiency limits further applications. Addressing charge dynamics and redox site issues is a straightforward approach to improving performance. Herein, we report the synergistic separation active modulation in lead-free Cs3Bi2Br9 HP N-vacancy reticular g-C3N4 nanosheet for selective C(sp3)–H bond activation. This regulation exhibits strong interfacial interaction, enabling effective transfer with more sites. Theoretical calculations experimental characterizations detailed enhanced reduced energy barriers surface photoredox reactions. When applied toluene oxidation under simulated solar light, optimized photocatalyst achieves total rate of 6865.3 μmol g–1 h–1 an outstanding benzaldehyde selectivity over 92%, outperforming most reported HP-based photocatalysts. work offers universal strategy developing efficient photocatalysts solar-to-chemical conversion.

Язык: Английский

---

Defects of Metal Halide Perovskites in Photocatalytic Energy Conversion: Friend or Foe?

Advanced Science, Год журнала: 2024, Номер 11(29)

Опубликована: Июнь 3, 2024

Abstract Photocatalytic solar‐to‐fuel conversion over metal halide perovskites (MHPs) has recently attracted much attention, while the roles of defects in MHPs are still under debate. Specifically, mainstream viewpoint is that detrimental to photocatalytic performance, some recent studies show certain types contribute photoactivity enhancement. However, a systematic summary why it contradictory and how affect performance lacking. In this review, innovative MHP photocatalysts highlighted. First, origins elaborated, followed by clarifying benefits including optical absorption, charge dynamics, surface reaction. Afterward, progress on defect‐related photocatalysis, i.e., CO 2 reduction, H generation, pollutant degradation, organic synthesis systematically discussed critically appraised, putting emphasis their beneficial effects. With offering peculiar sets merits demerits, personal opinion ongoing challenges concluded outlining potentially promising opportunities for engineering photocatalysts. This critical review anticipated offer better understanding spur inspiration designing efficient

Язык: Английский

---

Precisely Modulating Oxygen Vacancies Via Heterovalent Ions Substitution in Spinel‐Structured Phosphor for Versatile Applications

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 7, 2025

Abstract Rare‐earth ions doped phosphors have attracted great research interests owing to their versatile applications in optoelectronic fields. The often created atom vacancies because of the heterovalent substitution and different ion radii. However, how previously modulate defect concentration position phosphor is still a challenge significantly important for facilitating optical applications. Herein, accurate modulation oxygen spinel‐like ZnGa 2 O 4 demonstrated via Eu 3+ doping advanced temperature sensing information encryption experimental results first‐principle calculations confirmed that more introduced into lattice can lead generation high as well much deeper wider deficient states its electronic bandgap, which therefore endow potential afterglow emission. distinct luminescence quenching between at temperatures verified outstanding intensity ratio modeled performance with maximum relative sensitivity ( S r ) value 5.96% K −1 (@360 K) :0.02Eu sample. Moreover, by virtue fantastic thermal‐induced luminescence, dynamic optimal anti‐counterfeiting over :Eu been also achieved.

Язык: Английский

---

Strain Relaxation via Lattice Matching Effect for Highly Efficiency Stable Perovskite Solar Cells

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 14, 2025

Abstract The residual strain and crystallographic defects in perovskite films pose significant challenges to improving the efficiency stability of solar cells (PSCs). To address these issues, 3,5‐difluorobenzenesulfonamide (DBF) is introduced as a powerful additive. spacing functional groups DBF molecules precisely comparable bond lengths angles lattice, structural feature originating from geometric compatibility between its benzene ring substituents [PbI 6 ] octahedral framework structure. This atomic‐scale matching effectively minimizes lattice mismatch, enabling release passivate film. spontaneous interaction PbI 2 slows down crystal growth, film quality. size‐matching effect with strong interactions F···MA⁺ (FA⁺) hydrogen bonds ─S═O (─NH )···Pb ⁺ coordination defects. As result, DBF‐modified PSCs achieve champion 25.18%. More importantly, devices demonstrate excellent environmental stability, retaining 97.71% their initial power conversion (PCE) after 1600 h an atmospheric environment (25 °C, 20% RH) without encapsulation. study provides simple effective strategy enhance photovoltaics.

Язык: Английский

---

Phase Transition in Halide Double Perovskites for Solar‐To‐Chemical Energy Conversion

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 6, 2025

Abstract Halide double perovskites have recently garnered significant interest in solar energy conversion applications owing to their non‐toxic and high absorption properties. However, unanticipated structural distortion within these materials can compromise performance, suppressing the is essential remains challenging. Here, it reported that using phenylethylamine triggering disorder‐order phase transition largely increase ordering extent of octahedra perovskite Cs 2 AgBiBr 6 , which suppress self‐trapped exciton defect enable rapid charge separation, leading exceptional photo‐physics/chemistry properties with over sixfold photoactivity enhancement photocatalytic C−H bond activation compared less ordered structures. This work provides an effective strategy solve challenging problem disorder phenomenon halide for boosting solar‐to‐chemical conversion.

Язык: Английский

---

Tailoring the Microstructure of B‐Cation Octahedra in Halide Double Perovskites for Efficient Selective CO₂‐to‐CO Photoreduction

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 12, 2025

Abstract Solar‐driven CO 2 photoreduction using halide perovskites (HPs) has recently garnered significant attention; however, the conversion efficiency remains suboptimal for practical applications. Here, Cs AgBiBr 6 double as a model photocatalyst, interplay between coordination of octahedral B‐cation sites and photocatalytic performance are reported. The results reveal that modulating microstructure octahedra in enables orbital rehybridization, resulting an upshifted d‐band center reduced effective masses, thereby improving adsorption strength intermediates, lowering reaction energy barriers, promoting charge separation. Experimentally, it is demonstrated tailored achieves selective toward without sacrificial agents, yielding generation rate 23.73 µmol g −1 h with ≈100% selectivity, 13‐fold higher than pristine outperforms most reported HP‐based photocatalysts. This work highlights modulation HPs strategy efficient solar‐to‐fuel conversion.

Язык: Английский

---

A closer look at the interface of Cs3Bi2Br9 lead free perovskite in photocatalytic process

Journal of Physics and Chemistry of Solids, Год журнала: 2024, Номер unknown, С. 112534 - 112534

Опубликована: Дек. 1, 2024

Язык: Английский

---