Enhanced Selectivity of Photocatalytic CO₂ Reduction to Formate via Tailoring the Metal Site

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3000 - 3007

Published: Feb. 5, 2025

Language: Английский

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Giant Enhancement of Optical Nonlinearity by Manipulating Guest Molecular Stacking Modes in Metal–Organic Frameworks

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

The influence of guest stacking interactions in host-guest (H-G) MOF composites on third-order nonlinear optical (NLO) performance remains largely unknown. Herein, we propose for the first time a noncovalent aggregate confinement strategy synthesizing H-G with different modes. And [perylene2]n (α-Pe) and [perylene]n (β-Pe) were selected as guests confined into novel Ca-based {[Ca(TBAPy)(DMA)2]·3DMA·[N(CH3)2]·H2O}n (Ca-MOF-pts). NLO results showed that compared to β-Pe@Ca-MOF-pts, saturable absorption (SA) self-defocusing properties α-Pe@Ca-MOF-pts increased by 2.71-fold 3.82-fold, respectively. Interestingly, α/β-Pe@Ca-MOF-pts can be transformed α/β-Pe@Ca-MOF-flu (Ca-MOF-flu = {[Ca1.5(TBAPy)(H2O)2]·DMA·[N(CH3)2]·2H2O}n) through self-adaptive topological evolution, corresponding signal change from SA reverse (RSA). As expected, β-Pe@Ca-MOF-flu, RSA α-Pe@Ca-MOF-flu are improved 2.94-fold 4.07-fold, respectively, demonstrating importance Theoretical calculation transient spectra indicated enhancement was attributed large π-π overlap α-Pe, which promoted electron delocalization/transfer optimized cross-sectional ground state excited state. This study provides new developing excellent properties.

Language: Английский

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Magneto-electric integrated design strategy of NiCo@C composites for synergistic absorption and conversion in mid-high frequency microwaves

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 2205 - 2215

Published: Oct. 11, 2023

Language: Английский

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CO driven tunable syngas synthesis via CO2 photoreduction using a novel NiCo bimetallic metal-organic frameworks

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 283 - 290

Published: Jan. 7, 2025

Language: Английский

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Arrangement of Ordered D–A Components in a Metal‐Organic Framework for Cocatalyst‐Free Photocatalytic Hydrogen Evolution with Efficient Proton Conduction

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract The arrangement of donor–acceptor (D–A) components in order at a molecular level provides means to achieve efficient electron‐hole separation for promoting the activity photocatalysts. Herein, we report coordination assembly D–A molecules with desired staggered energy levels two isostructural metal‐organic frameworks (MOFs) 1 and 2 , which exhibit high photocatalytic hydrogen evolution without using any cocatalysts photosensitizers. modulation active metal sites MOFs leads an increase rates from 1260 3218 µmol h −1 g . A detailed mechanism study revealed that bond defined by assisted centers is key efficiently generating photogenerated charge carriers, has appropriate affinity proton reduce barrier evolution. Besides, enhanced transport kinetics based on arrayed free carboxyl groups hydrogen‐bonded network endows higher conductivity than thus usage rate reaction kinetics.

Language: Английский

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Arrangement of Ordered D–A Components in a Metal‐Organic Framework for Cocatalyst‐Free Photocatalytic Hydrogen Evolution with Efficient Proton Conduction

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract The arrangement of donor–acceptor (D–A) components in order at a molecular level provides means to achieve efficient electron‐hole separation for promoting the activity photocatalysts. Herein, we report coordination assembly D–A molecules with desired staggered energy levels two isostructural metal‐organic frameworks (MOFs) 1 and 2 , which exhibit high photocatalytic hydrogen evolution without using any cocatalysts photosensitizers. modulation active metal sites MOFs leads an increase rates from 1260 3218 µmol h −1 g . A detailed mechanism study revealed that bond defined by assisted centers is key efficiently generating photogenerated charge carriers, has appropriate affinity proton reduce barrier evolution. Besides, enhanced transport kinetics based on arrayed free carboxyl groups hydrogen‐bonded network endows higher conductivity than thus usage rate reaction kinetics.

Language: Английский

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Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic CO2 reduction

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 2410 - 2419

Published: Sept. 14, 2023

Language: Английский

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A Cu(I)-Based MOF with Nonlinear Optical Properties and a Favorable Optical Limit Threshold

Nanomaterials, Journal Year: 2025, Volume and Issue: 15(2), P. 145 - 145

Published: Jan. 20, 2025

The exploitation of high-performance third-order nonlinear optical (NLO) materials that have a favorable limit (OL) threshold is essential due to rise in the application ultra-intense lasers. In this study, Cu-based MOF (denoted as Cu-bpy) was synthesized, and its NLO OL properties were investigated using Z-scan technique with nanosecond laser pulse excitation set at 532 nm. Cu-bpy exhibits typical rate reverse saturable absorption (RSA) coefficient 100 cm GW−1 0.75 J cm−2 (at concentration 1.6 mg mL−1), which lower than most been reported on so far. addition, DFT calculation performed agreement our experimental results. Furthermore, mechanism illustrated one-photon (1PA). These results investigate relationship between structure Cu-bpy, provide an theoretical basis for use limiting applications.

Language: Английский

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Zirconium-Based Metal–Organic Frameworks for Photocatalytic CO₂ Reduction

Precision Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: May 5, 2025

Language: Английский

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Transformation of SBUs and Synergy of MOF Host–Guest in Single Crystalline State: Ingenious Strategies for Modulating Third‐Order NLO Signals

Small, Journal Year: 2023, Volume and Issue: 20(4)

Published: Sept. 15, 2023

Abstract Central metal exchange can innovatively open the cavity of metal‐organic frameworks (MOFs) by alternating framework topology. Here, single‐crystal‐to‐single‐crystal (SC‐SC) transformation is reported from a Co‐based MOF {[Co 1.25 (HL) 0.5 (Pz‐NH 2 ) 0.25 ( µ 3 ‐O) ‐OH) (H O)]·0.125 Co·0.125 L·10.25H O} n (Co‐MOF, L = 5,5'‐(1 H ‐2,3,5‐triazole‐1,4‐diyl)diisophthalic acid) into two novel materials, {[Cu 1.75 0.75 0.125 O) 0.375 ]•3CH CN} (Cu‐MOF) and {[Zn 0.625 ]•4CH (Zn‐MOF), through exchanging Co 2+ in Cu or Zn , respectively. The free 4− Co‐MOF channels fuse with skeleton during Co→Cu Co→Zn processes, leading to expansion channel space secondary building units (SBUs) form an adjustable skeleton. nonlinear optical response results show that MOFs generated central exhibit different saturable absorption self‐focusing effect. In addition, loading polypyrrole (PPy) not only improve stability but also further optimize behavior. This work suggests SC‐SC introduction polymer molecules tune response, which provides new perspective for future study materials.

Language: Английский

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