Solvent/pH-directed synthesis of Mn coordination polymers for enhanced photoelectrocatalytic water splitting

IF 4.1 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2025-06-18 DOI:10.1016/j.jphotochem.2025.116586

Meng-Qi Tuo, Jia-Xin Fan, De-Cong Qiao, Di Ma, Wan-Lin Zhao, Zi-Yue Hu, Bo Liu, Jiu-Fu Lu

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引用次数: 0

Abstract

As global energy demands escalate, hydrogen energy has emerged as a pivotal clean energy source. However, developing high-performance, low-cost catalysts for the oxygen evolution reaction (OER) remains a critical challenge. Herein, the controlled assembly of ligand 4-CPCA with manganese chloride through pH modulation and solvent regulation yields three distinct coordination architectures: a zero-dimensional Mn(II) monomer {Mn(H₂O)₂[H(4-CPCA)]₂}·2H₂O (SNUT-18), a one-dimensional chain (1D) [Mn(H₂O)₃(4-CPCA)]ₙ (SNUT-33), and a two-dimensional bilayer (2D) [Mn(H₂O)₂(4-CPCA)·H₂O]ₙ (SNUT-34). (4-CPCA = 1-(4-carboxyphenyl)-4-oxo-1,4-dihydropyridazine-3-carboxylic acid.; DMA = dimethylacetamide). Structural characterization confirmed the crystal structure, while solid-state UV–vis diffuse reflectance spectroscopy (UV–Vis DRS) and Mott-Schottky (M-S) analysis identified their n-type semiconductor behavior. Electrocatalytic evaluation revealed that SNUT-18, SNUT-33, and SNUT-34 exhibited significantly reduced overpotentials, lower Tafel slopes, and decreased electrochemical impedance Under simulated solar irradiation (300 W Xe lamp). This work highlights the critical role of structural dimensionality in optimizing photoelectrocatalytic OER activity.

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溶剂/ ph定向合成用于增强光电催化水分解的Mn配位聚合物

随着全球能源需求的不断增长，氢能已成为一种关键的清洁能源。然而，开发高性能、低成本的析氧反应催化剂仍然是一个关键的挑战。在这里，通过pH调节和溶剂调节，配体4-CPCA与氯化锰的控制组装产生了三种不同的配位结构：零维Mn（II）单体{Mn（H₂O）₂[H(4-CPCA)]₂}·2H₂O (SNUT-18)，一维链（1D） [Mn（H₂O）₃（4-CPCA）]和二维双层（2D） [Mn（H₂O）₂（4-CPCA）·H₂O] （SNUT-34）。(4-CPCA = 1-（4-羧基苯基）-4-氧-1,4-二氢吡啶-3-羧酸；二甲基乙酰胺)。结构表征证实了晶体结构，而固态UV-vis漫反射光谱（UV-vis DRS）和莫特-肖特基（M-S）分析证实了它们的n型半导体行为。电催化评价表明，在模拟太阳照射（300 W氙灯）下，SNUT-18、SNUT-33和SNUT-34的过电位显著降低，Tafel斜率降低，电化学阻抗降低。这项工作强调了结构维度在优化光电催化OER活性中的关键作用。

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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.