Tunable metal hydroxide–organic frameworks for catalysing oxygen evolution

The oxygen evolution reaction is central to making chemicals and energy carriers using electrons. Combining the great tunability of enzymatic systems with known oxide-based catalysts can create breakthrough opportunities to achieve both high activity and stability. Here we report a series of metal h...

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Vydáno v:Nature materials Ročník 21; číslo 6; s. 673 - 680
Hlavní autoři: Yuan, Shuai, Peng, Jiayu, Cai, Bin, Huang, Zhehao, Garcia-Esparza, Angel T., Sokaras, Dimosthenis, Zhang, Yirui, Giordano, Livia, Akkiraju, Karthik, Zhu, Yun Guang, Hübner, René, Zou, Xiaodong, Román-Leshkov, Yuriy, Shao-Horn, Yang
Médium: Journal Article
Jazyk:angličtina
Vydáno: London Nature Publishing Group UK 01.06.2022
Nature Publishing Group
Springer Nature - Nature Publishing Group
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Biomaterials
Catalytic activity
Cations
Chemical engineering
Chemistry
Chemistry and Materials Science
Condensed Matter Physics
Density functional theory
Electrolytes
Electrons
Evolution
Hydroxides
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Iron
Laboratories
Ligands
MATERIALS SCIENCE
Metal hydroxides
Metal oxides
Metals
Nanotechnology
Nickel
Optical and Electronic Materials
Oxygen
Oxygen evolution reactions
Porous materials
Stability
Substitution reactions
Transition metals
ISSN:1476-1122, 1476-4660, 1476-4660
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Shrnutí:The oxygen evolution reaction is central to making chemicals and energy carriers using electrons. Combining the great tunability of enzymatic systems with known oxide-based catalysts can create breakthrough opportunities to achieve both high activity and stability. Here we report a series of metal hydroxide–organic frameworks (MHOFs) synthesized by transforming layered hydroxides into two-dimensional sheets crosslinked using aromatic carboxylate linkers. MHOFs act as a tunable catalytic platform for the oxygen evolution reaction, where the π–π interactions between adjacent stacked linkers dictate stability, while the nature of transition metals in the hydroxides modulates catalytic activity. Substituting Ni-based MHOFs with acidic cations or electron-withdrawing linkers enhances oxygen evolution reaction activity by over three orders of magnitude per metal site, with Fe substitution achieving a mass activity of 80 A  g catalyst − 1 at 0.3 V overpotential for 20 h. Density functional theory calculations correlate the enhanced oxygen evolution reaction activity with the MHOF-based modulation of Ni redox and the optimized binding of oxygenated intermediates. The oxygen evolution reaction is central to making chemicals and energy carriers using electrons. Metal hydroxide–organic frameworks are shown to act as a tunable catalytic platform for oxygen evolution, with π–π interactions dictating stability and transition metals modulating activity.
Bibliografie:ObjectType-Article-1
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USDOE Office of Science (SC), Basic Energy Sciences (BES)
AC02-76SF00515
ISSN:1476-1122
1476-4660
1476-4660
DOI:10.1038/s41563-022-01199-0