% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@ARTICLE{Yang:596487,
author = {Yang, Yuwei and Lie, William Hadinata and Unocic, Raymond R
and Yuwono, Jodie A and Klingenhof, Malte and Merzdorf,
Thomas and Buchheister, Paul 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},
title = {{D}efect‐{P}romoted {N}i‐{B}ased {L}ayer {D}ouble
{H}ydroxides with {E}nhanced {D}eprotonation {C}apability
for {E}fficient {B}iomass {E}lectrooxidation},
journal = {Advanced materials},
volume = {tbd},
issn = {0935-9648},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {PUBDB-2023-06162},
pages = {2305573},
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.},
cin = {DOOR ; HAS-User},
ddc = {660},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3)},
pid = {G:(DE-HGF)POF4-6G3},
experiment = {EXP:(DE-H253)P-P21.1-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {37734330},
UT = {WOS:001084218100001},
doi = {10.1002/adma.202305573},
url = {https://bib-pubdb1.desy.de/record/596487},
}