TY  - JOUR
AU  - Xia, Lu
AU  - Gomes, Bruna Ferreira
AU  - Jiang, Wulyu
AU  - Escalera-López, Daniel
AU  - Wang, Yang
AU  - Hu, Yang
AU  - Faid, Alaa Y.
AU  - Wang, Kaiwen
AU  - Chen, Tengyu
AU  - Zhao, Kaiqi
AU  - Zhang, Xu
AU  - Zhou, Yingtang
AU  - Ram, Ranit
AU  - Polesso, Barbara
AU  - Guha, Anku
AU  - Su, Jiaqi
AU  - Lobo, Carlos
AU  - Haumann, Michael
AU  - Spatschek, Robert
AU  - Sunde, Svein
AU  - Gan, Lin
AU  - Huang, Ming
AU  - Zhou, Xiaoyuan
AU  - Roth, Christina
AU  - Lehnert, Werner
AU  - Cherevko, Serhiy
AU  - Gan, Liyong
AU  - Garcia de Arquer, F. Pelayo
AU  - Shviro, Meital
TI  - Operando-informed precatalyst programming towards reliable high-current-density electrolysis
JO  - Nature materials
VL  - 24
IS  - 5
SN  - 1476-1122
CY  - Basingstoke
PB  - Nature Publishing Group
M1  - PUBDB-2025-00929
SP  - 753 - 761
PY  - 2025
N1  - Publisher's Bespoke License
AB  - 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<sub>x</sub>Fe<sub>1−x</sub>S<sub>2</sub> model system, this leads to a threefold improvement in durability after programmed activation, with a cell degradation rate of 0.12 mV h<sup>−1</sup> over 550 h (standard operation: 0.29 mV h<sup>−1</sup>, constrained to 200 h), in an anion exchange membrane water electrolyser operating at 1 A cm<sup>−2</sup>. This work bridges predictive modelling and experimental design, improving the electrocatalyst reliability for industrial water electrolysis and beyond at high current densities.
LB  - PUB:(DE-HGF)16
C6  - pmid:40021826
UR  - <Go to ISI:>//WOS:001434078500001
DO  - DOI:10.1038/s41563-025-02128-7
UR  - https://bib-pubdb1.desy.de/record/624847
ER  -