Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation

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.

doi:10.1002/adma.202305573

Title: Defect‐Promoted Ni‐Based Layer Double Hydroxides with Enhanced Deprotonation Capability for Efficient Biomass Electrooxidation

Journal Article · 11 October 2023 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202305573 · OSTI ID:2067633

Yang, Yuwei ^[1]; Lie, William Hadinata ^[1]; Unocic, Raymond R. ^[2]; Yuwono, Jodie A. ^[3]; Klingenhof, Malte ^[4]; Merzdorf, Thomas ^[4]; Buchheister, Paul Wolfgang ^[4]; Kroschel, Matthias ^[4]; Walker, Anne ^[5]; Gallington, Leighanne C. ^[6]; Thomsen, Lars ^[7]; Kumar, Priyank V. ^[1]; Strasser, Peter ^[4]; Scott, Jason A. ^[1];

^[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

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2067633

Alternate ID(s):: OSTI ID: 2566130; OSTI ID: 2067635

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 48 Vol. 35; ISSN 0935-9648

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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