Enhancing photocatalytic CO2-to-CO conversion by iron complexes through 8-hydroxyquinoline ligand regulation

IF 4 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Structure Pub Date : 2025-03-11 DOI:10.1016/j.molstruc.2025.142039

Zhichao Xu , Xin Huang , Liyan Zhang , Duojun Cao , Dongdong Liu , Guozan Yuan

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Abstract

Metal complexes, with their well-defined molecular structures and design flexibility, offer an ideal platform for developing CO₂ reduction photocatalysts. While ligand modification is an effective strategy to enhance catalytic performance, it also presents several challenges. In this work, two 8-hydroxyquinoline-based organic ligands bearing different substituents were initially synthesized. Two ligands were subsequently employed in reactions with Fe(III) ion, respectively, generating two distinct molecular complexes, designated 1-Fe and 2-Fe. The binuclear structures of two complexes were unambiguously elucidated by single-crystal X-ray diffraction (SCXRD), and ESI-MS spectra. Under visible-light irradiation, both complexes demonstrated photocatalytic activity for CO₂ reduction to CO in aqueous solution. Notably, complex 1-Fe exhibited a marked improvement in both activity (TON_CO = 3106) and selectivity (Sel_CO = 81 %) compared to the 2-Fe catalyst (TON_CO = 1641, Sel_CO = 61 %). Furthermore, the superior CO₂ photoreduction performance of 1-Fe was comprehensively investigated by electrochemical tests, and photoinduced electron transfer dynamics, as well as in-situ attenuated total reflection infrared fourier transform spectroscopy (ATR-IFTS).

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来源期刊

Journal of Molecular Structure 化学-物理化学

CiteScore

7.10

自引率

15.80%

发文量

2384

审稿时长

45 days

期刊介绍： The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.