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Ligand and Anion Co-Leaching Induced Complete Reconstruction of Polyoxomolybdate-Organic Complex Oxygen-Evolving Pre-Catalysts

机译:配体和阴离子共浸诱导诱导聚氧钼钼 - 有机复合氧化前催化剂的完全重建

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摘要

The coordination compounds in the oxygen evolution reaction (OER) have been researched extensively. However, their poor durability (mostly 100 h) and controversial reconstruction mechanism restrict their practical applications. Herein, a new-type polyoxomolybdate-organic complex (POMo) via wet-chemistry synthesis with fixed coordination between metal centers (Ni2+ and [Mo8O26](4-)) and 2-Methylimidazole ligand is introduced. After introducing iron, a series of Fe-doped Ni-POMo with porous and amorphous structures are fabricated. These features accelerate the diffusion-leaching processes of ligands and anions, resulting in rapid and complete phase reconstruction during alkaline OER. As a result, nickel-iron (oxy)hydroxides with rich vacancies and poly-/low-crystalline features are in situ generated through dissolution-redeposition, and serve as the OER-active species. The optimized Fe0.052Ni-POMo array pre-catalyst has excellent activity and sustains ultrastable catalysis for 545 h. The complete reconstruction of POMo enables high catalytic durability (230 h) and stable active phase under realistic conditions (30 wt% KOH, 60.9 degrees C). Accordingly, the completely reconstructed catalysts with unique structures and ultrastable catalysis have the potential to be applied in industry.
机译:已经广泛地研究了氧进化反应(OER)中的配位化合物。然而,它们耐久性差(大多是百分比)和有争议的重建机制限制了其实际应用。这里,引入了通过湿化学合成的新型聚氧钼酰胺 - 有机络合物(POMO),所述湿化学合成具有金属中心(Ni2 +和[MO8O26](4-))和2-甲基咪唑配体之间的固定配位。在引入铁后,制造了一系列具有多孔和非晶结构的Fe掺杂的Ni-Pomo。这些特征加速了配体和阴离子的扩散浸出过程,导致碱性oer期间快速完整的相位重建。结果,具有丰富空位和聚/低晶体特征的镍 - 铁(氧)氢氧化物通过溶解 - 再沉积原位原位产生,并用作oer活性物种。优化的Fe0.052Ni-Pomo阵列预催化剂具有优异的活性,并且可持续545小时的可升温催化。 POMO的完全重建使得能够在现实条件下具有高催化耐久性(230小时)和稳定的活性相(30wt%KOH,60.9℃)。因此,具有独特结构和无限催化的完全重建的催化剂具有适用于工业的可能性。

著录项

  • 来源
    《Advanced Functional Materials》 |2021年第31期|2101792.1-2101792.9|共9页
  • 作者单位

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China;

    Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China|Adv Energy Sci & Technol Guangdong Lab Foshan Xianhu Lab Foshan 528200 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    complete reconstruction; in situ Raman; multi-component co-leaching; polyoxomolybdate-organic complexes; ultrastable oxygen evolution;

    机译:完全重建;原位拉曼;多组分共浸液;聚氧键钼酸盐 - 有机络合物;无借氧氧气进化;

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