Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation
Abstract
Abstract Ni‐based hydroxides are promising electrocatalysts for biomass oxidation reactions, supplanting the oxygen evolution reaction (OER) due to lower overpotentials while producing value‐added chemicals. The identification and subsequent engineering of their catalytically active sites are essential to facilitate these anodic reactions. Herein, the proportional relationship between catalysts’ deprotonation propensity and Faradic efficiency of 5‐hydroxymethylfurfural (5‐HMF)‐to‐2,5 furandicarboxylic acid (FDCA, FE FDCA ) is revealed by thorough density functional theory (DFT) simulations and atomic‐scale characterizations, including in situ synchrotron diffraction and spectroscopy methods. The deprotonation capability of ultrathin layer‐double hydroxides (UT‐LDHs) is regulated by tuning the covalency of metal (M)‐oxygen (O) motifs through defect site engineering and selection of M 3+ co‐chemistry. NiMn UT‐LDHs show an ultrahigh FE FDCA of 99% at 1.37 V versus reversible hydrogen electrode (RHE) and retain a high FE FDCA of 92.7% in the OER‐operating window at 1.52 V, about 2× that of NiFe UT‐LDHs (49.5%) at 1.52 V. Ni–O and Mn–O motifs function as dual active sites for HMF electrooxidation, where the continuous deprotonation of Mn–OH sites plays a dominant role in achieving high selectivity while suppressing OER at high potentials. The results showcase a universal concept of modulating competing anodic reactions in aqueous biomass electrolysis by electronically engineering themore »
- Authors:
-
[1]
- School of Chemical Engineering University of New South Wales Sydney NSW 2052 Australia
- Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA
- School of Chemical Engineering The University of Adelaide Adelaide SA 5005 Australia
- Department of Chemistry Chemical Engineering Division Technical University Berlin 10623 Berlin Germany
- US Army DEVCOM Chemical Biological Center Aberdeen Proving Grounds MD 21010 USA
- X‐Ray Science Division Argonne National Laboratory Argonne IL 60439 USA
- Australian Synchrotron Australian Nuclear Science and Technology Organisation Clayton VIC 3168 Australia
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 2067633
- Alternate Identifier(s):
- OSTI ID: 2067635
- Grant/Contract Number:
- DE‐AC02‐06CH11357
- Resource Type:
- Published Article
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Name: Advanced Materials Journal Volume: 35 Journal Issue: 48; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Yang, Yuwei, Lie, William Hadinata, Unocic, Raymond R., Yuwono, Jodie A., Klingenhof, Malte, Merzdorf, Thomas, Buchheister, Paul Wolfgang, Kroschel, Matthias, Walker, Anne, Gallington, Leighanne C., Thomsen, Lars, Kumar, Priyank V., Strasser, Peter, Scott, Jason A., and Bedford, Nicholas M. Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation. Germany: N. p., 2023.
Web. doi:10.1002/adma.202305573.
Yang, Yuwei, Lie, William Hadinata, Unocic, Raymond R., Yuwono, Jodie A., Klingenhof, Malte, Merzdorf, Thomas, Buchheister, Paul Wolfgang, Kroschel, Matthias, Walker, Anne, Gallington, Leighanne C., Thomsen, Lars, Kumar, Priyank V., Strasser, Peter, Scott, Jason A., & Bedford, Nicholas M. Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation. Germany. https://doi.org/10.1002/adma.202305573
Yang, Yuwei, Lie, William Hadinata, Unocic, Raymond R., Yuwono, Jodie A., Klingenhof, Malte, Merzdorf, Thomas, Buchheister, Paul Wolfgang, Kroschel, Matthias, Walker, Anne, Gallington, Leighanne C., Thomsen, Lars, Kumar, Priyank V., Strasser, Peter, Scott, Jason A., and Bedford, Nicholas M. Thu .
"Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation". Germany. https://doi.org/10.1002/adma.202305573.
@article{osti_2067633,
title = {Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation},
author = {Yang, Yuwei and Lie, William Hadinata and Unocic, Raymond R. and Yuwono, Jodie A. and Klingenhof, Malte and Merzdorf, Thomas and Buchheister, Paul Wolfgang and Kroschel, Matthias and Walker, Anne and Gallington, Leighanne C. and Thomsen, Lars and Kumar, Priyank V. and Strasser, Peter and Scott, Jason A. and Bedford, Nicholas M.},
abstractNote = {Abstract Ni‐based hydroxides are promising electrocatalysts for biomass oxidation reactions, supplanting the oxygen evolution reaction (OER) due to lower overpotentials while producing value‐added chemicals. The identification and subsequent engineering of their catalytically active sites are essential to facilitate these anodic reactions. Herein, the proportional relationship between catalysts’ deprotonation propensity and Faradic efficiency of 5‐hydroxymethylfurfural (5‐HMF)‐to‐2,5 furandicarboxylic acid (FDCA, FE FDCA ) is revealed by thorough density functional theory (DFT) simulations and atomic‐scale characterizations, including in situ synchrotron diffraction and spectroscopy methods. The deprotonation capability of ultrathin layer‐double hydroxides (UT‐LDHs) is regulated by tuning the covalency of metal (M)‐oxygen (O) motifs through defect site engineering and selection of M 3+ co‐chemistry. NiMn UT‐LDHs show an ultrahigh FE FDCA of 99% at 1.37 V versus reversible hydrogen electrode (RHE) and retain a high FE FDCA of 92.7% in the OER‐operating window at 1.52 V, about 2× that of NiFe UT‐LDHs (49.5%) at 1.52 V. Ni–O and Mn–O motifs function as dual active sites for HMF electrooxidation, where the continuous deprotonation of Mn–OH sites plays a dominant role in achieving high selectivity while suppressing OER at high potentials. The results showcase a universal concept of modulating competing anodic reactions in aqueous biomass electrolysis by electronically engineering the deprotonation behavior of metal hydroxides, anticipated to be translatable across various biomass substrates.},
doi = {10.1002/adma.202305573},
journal = {Advanced Materials},
number = 48,
volume = 35,
place = {Germany},
year = {Thu Oct 12 00:00:00 EDT 2023},
month = {Thu Oct 12 00:00:00 EDT 2023}
}
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