Universal molecular-confined synthesis of interconnected porous metal oxides-N-C frameworks for electrocatalytic water splitting

You, Bo; Zhang, Yadong; Yin, Peiqun; Jiang, De-en; Sun, Yujie

doi:10.1016/j.nanoen.2018.04.009

Title: Universal molecular-confined synthesis of interconnected porous metal oxides-N-C frameworks for electrocatalytic water splitting

Journal Article · Wed Apr 04 00:00:00 EDT 2018 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2018.04.009· OSTI ID:1543574

You, Bo ^[1]; Zhang, Yadong ^[2]; Yin, Peiqun ^[1]; Jiang, De-en ^[2]; Sun, Yujie ^[3]

University of Science and Technology of China, Hefei (China)
University of California, Riverside, CA (United States)
Utah State University, Logan, UT (United States)

The rational synthesis of high performance electrocatalysts at low cost for water splitting (hydrogen and oxygen evolution reaction, HER and OER) is highly desirable but remains a key challenge. Herein, we report a versatile molecular-confining route to construct strongly coupled metal oxides-N-C frameworks with interconnected configuration. By simply chelating various transition metal ions with ethylenediaminetetraacetic acid disodium salt (EDTA) in agarose hydrogel and subsequent carbonization, the high specific surface area porous N-C frameworks with strongly coupled metal oxides (e.g., manganese, iron, cobalt, nickel and their mixed oxides) can be prepared as advanced nonprecious water splitting electrocatalysts. For instance, the resulting Co₃O₄-N-C frameworks with the high surface area of 153 m² g^-1, and the moderate nitrogen content of 1.23%, require an overpotential of 324 mV to afford a current density of 10 mA cm^-2 in 0.1 M KOH for OER, superior to commercial RuO₂ catalysts. Density functional theory (DFT) calculations reveal that the strong coupling between N-C and Co₃O₄ tunes the local electronic structure of Co for high-valence active sites and assures optimal adsorption energies of OER intermediates. Moreover, Co₂P-N-C electrocatalysts derived from Co₃O₄-N-C also exhibit excellent HER performance under 1.0 M KOH with a low overpotential of 139 mV to reach 10 mA cm^-2, a small Tafel slope of 45 mV dec^-1 and impressive stability, underscoring the versatility of our synthetic strategy.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Riverside, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); Utah State University; National Science Foundation (NSF); University of California, Riverside

Grant/Contract Number:: AC02-05CH11231; CHE-1653978; AC02–05CH11231

OSTI ID:: 1543574

Alternate ID(s):: OSTI ID: 1496460

Journal Information:: Nano Energy, Vol. 48, Issue C; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 55 works

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Title: Universal molecular-confined synthesis of interconnected porous metal oxides-N-C frameworks for electrocatalytic water splitting

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