基于Mn（II）的HOF单晶到单晶转化为MOF增强的光电催化析氧反应

IF 4.1 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2025-06-13 DOI:10.1016/j.jphotochem.2025.116569

Ting-Ting Wu, Xi-Rui Guo, Zi-Yue Hu, Shi-Yun He, Heng-Bo Wang, Ye-Tong Lei, Jiu-Fu Lu, Bo Liu

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引用次数: 0

摘要

从水中获取氢能对可持续经济增长和环境友好型发展至关重要。然而，电解过程中析氧反应（OER）的高能量势垒仍然是一个严峻的挑战。在此，我们报道了一个Mn（II）基氢键有机骨架（HOF） {[Mn(H2O)2(4- pdca)2]·2H2O} (SNUT-28)，它经历了溶剂诱导的单晶到单晶（SC-SC）转变，形成金属有机骨架（MOF） {[Mn2(H2O)4(4- pdca)2]·5H2O}n （SNUT-29）。SNUT-28具有灵活的氢键网络，能够实现均匀的电极分布和增强的光电流密度（2.0 V vs RHE时为2.43 mA∙cm−2）。相比之下，具有共价Mn-O配位的SNUT-29具有较低的电荷转移电阻（Rct = 266.4 Ω）和优越的光子灵敏度。这项研究为设计高效光电催化OER的hof到mof转换提供了见解。

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Single-crystal-to-single-crystal transformation of Mn(II)-based HOF to MOF for enhanced photoelectrocatalytic oxygen evolution reaction

Harvesting hydrogen energy from water is pivotal for sustainable economic growth and environmentally friendly development. However, the high energy barrier of the oxygen evolution reaction (OER) in water electrolysis remains a critical challenge. Herein, we report a Mn(II)-based hydrogen-bonded organic framework (HOF), {[Mn(H₂O)₂(4-PDCA)₂]·2H₂O} (SNUT-28), which undergoes solvent-induced single-crystal-to-single-crystal (SC-SC) transformation to form a metal–organic framework (MOF), {[Mn₂(H₂O)₄(4-PDCA)₂]·5H₂O}_n (SNUT-29). SNUT-28 exhibits a flexible hydrogen-bonded network, enabling uniform electrode distribution and enhanced photocurrent density (2.43 mA∙cm⁻² at 2.0 V vs RHE). In contrast, SNUT-29, with covalent Mn-O coordination, demonstrates reduced charge transfer resistance (Rct = 266.4 Ω) and superior photonic sensitivity. This study provides insights into designing HOF-to-MOF transformations for efficient photoelectrocatalytic OER.

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来源期刊

Journal of Photochemistry and Photobiology A-chemistry 化学-物理化学

CiteScore

7.90

自引率

7.00%

发文量

580

审稿时长

48 days

期刊介绍： JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.