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@ARTICLE{Xia:624847,
author = {Xia, Lu and Gomes, Bruna Ferreira and Jiang, Wulyu and
Escalera-López, Daniel and Wang, Yang and Hu, Yang and
Faid, Alaa Y. and Wang, Kaiwen and Chen, Tengyu and Zhao,
Kaiqi and Zhang, Xu and Zhou, Yingtang and Ram, Ranit and
Polesso, Barbara and Guha, Anku and Su, Jiaqi and Lobo,
Carlos and Haumann, Michael and Spatschek, Robert and Sunde,
Svein and Gan, Lin and Huang, Ming and Zhou, Xiaoyuan and
Roth, Christina and Lehnert, Werner and Cherevko, Serhiy and
Gan, Liyong and Garcia de Arquer, F. Pelayo and Shviro,
Meital},
title = {{O}perando-informed precatalyst programming towards
reliable high-current-density electrolysis},
journal = {Nature materials},
volume = {24},
number = {5},
issn = {1476-1122},
address = {Basingstoke},
publisher = {Nature Publishing Group},
reportid = {PUBDB-2025-00929},
pages = {753 - 761},
year = {2025},
note = {Publisher's Bespoke License},
abstract = {Electrocatalysts support crucial industrial processes and
emerging decarbonization technologies, but their design is
hindered by structural and compositional changes during
operation, especially at application-relevant current
densities. Here we use operando X-ray spectroscopy and
modelling to track, and eventually direct, the
reconstruction of iron sulfides and oxides for the oxygen
evolution reaction. We show that inappropriate activation
protocols lead to uncontrollable Fe oxidation and
irreversible catalyst degradation, compromising stability
and reliability and precluding predictive design. Based on
these, we develop activation programming strategies that,
considering the thermodynamics and kinetics of surface
reconstruction, offer control over precatalyst oxidation.
This enables reliable predictions and the design of active
and stable electrocatalysts. In a Ni$_x$Fe$_{1−x}$S$_2$
model system, this leads to a threefold improvement in
durability after programmed activation, with a cell
degradation rate of 0.12 mV h$^ {−1}$ over 550 h
(standard operation: 0.29 mV h$^{−1}$, constrained to
200 h), in an anion exchange membrane water electrolyser
operating at 1 A cm$^{−2}$. This work bridges
predictive modelling and experimental design, improving the
electrocatalyst reliability for industrial water
electrolysis and beyond at high current densities.},
cin = {FS DOOR-User},
ddc = {610},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20221247
(I-20221247) / JUNIOR LEADER - Junior Leader la Caixa
Postdoctoral Fellowship Programme: Shaping the new
generation of leaders in research (847648) / NASCENT -
Nanoscale Advance of CO2 Electroreduction (101077243)},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20221247 /
G:(EU-Grant)847648 / G:(EU-Grant)101077243},
experiment = {EXP:(DE-H253)P-P64-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:40021826},
UT = {WOS:001434078500001},
doi = {10.1038/s41563-025-02128-7},
url = {https://bib-pubdb1.desy.de/record/624847},
}