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

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

Journal Article · Thu Sep 21 00:00:00 EDT 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]

Univ. of New South Wales, Sydney, NSW (Australia)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Adelaide, SA (Australia)
Technical Univ. of Berlin (Germany)
US Dept. of Homeland Security (DHS), Aberdeen Proving Ground, MD (United States). DEVCOM Chemical Biological Center
Argonne National Laboratory (ANL), Argonne, IL (United States)
Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, VIC (Australia). Australian Synchrotron

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, FEFDCA) 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 M³⁺ 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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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2067633

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

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

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
Ni-based layered double hydroxide
biomass electrooxidation
defective engineering
electron transfer processes
metal-oxygen covalency
proton transfer processes
structural evolution

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

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