Tunable metal hydroxide–organic frameworks for catalysing oxygen evolution

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

doi:10.1038/s41563-022-01199-0

Title: Tunable metal hydroxide–organic frameworks for catalysing oxygen evolution

Journal Article · 23 February 2022 · Nature Materials

DOI: https://doi.org/10.1038/s41563-022-01199-0 · OSTI ID:1867425

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^[4]; Garcia-Esparza, Angel T. ^[5]; Sokaras, Dimosthenis ^[5];

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^[2]; Akkiraju, Karthik ^[2]; Zhu, Yun Guang ^[2];

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Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Nanjing Univ. (China)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Shandong Univ., Jinan (China)
Stockholm Univ. (Sweden)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Hemholtz-Zentrum Dresden-Rossendorf (Germany)

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 80A $$g^{-1}_{catalyst}$$ 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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1867425

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 6 Vol. 21; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Tunable metal hydroxide–organic frameworks for catalysing oxygen evolution

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