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000624847 1001_ $$0P:(DE-H253)PIP1101088$$aXia, Lu$$b0
000624847 245__ $$aOperando-informed precatalyst programming towards reliable high-current-density electrolysis
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000624847 520__ $$aElectrocatalysts support crucial industrial processes and emerging decarbonization technologies, but their design is hindered by structural and compositional changes during operation, especially at application-relevant current densities. Here we use operando X-ray spectroscopy and modelling to track, and eventually direct, the reconstruction of iron sulfides and oxides for the oxygen evolution reaction. We show that inappropriate activation protocols lead to uncontrollable Fe oxidation and irreversible catalyst degradation, compromising stability and reliability and precluding predictive design. Based on these, we develop activation programming strategies that, considering the thermodynamics and kinetics of surface reconstruction, offer control over precatalyst oxidation. This enables reliable predictions and the design of active and stable electrocatalysts. In a Ni$_x$Fe$_{1−x}$S$_2$ model system, this leads to a threefold improvement in durability after programmed activation, with a cell degradation rate of 0.12 mV h$^ {−1}$ over 550 h (standard operation: 0.29 mV h$^{−1}$, constrained to 200 h), in an anion exchange membrane water electrolyser operating at 1 A cm$^{−2}$. This work bridges predictive modelling and experimental design, improving the electrocatalyst reliability for industrial water electrolysis and beyond at high current densities.
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000624847 7001_ $$0P:(DE-HGF)0$$aGomes, Bruna Ferreira$$b1
000624847 7001_ $$0P:(DE-H253)PIP1101087$$aJiang, Wulyu$$b2
000624847 7001_ $$00000-0002-2001-9775$$aEscalera-López, Daniel$$b3
000624847 7001_ $$0P:(DE-HGF)0$$aWang, Yang$$b4
000624847 7001_ $$0P:(DE-HGF)0$$aHu, Yang$$b5
000624847 7001_ $$0P:(DE-HGF)0$$aFaid, Alaa Y.$$b6
000624847 7001_ $$0P:(DE-H253)PIP1111698$$aWang, Kaiwen$$b7
000624847 7001_ $$0P:(DE-H253)PIP1111697$$aChen, Tengyu$$b8
000624847 7001_ $$0P:(DE-HGF)0$$aZhao, Kaiqi$$b9
000624847 7001_ $$0P:(DE-HGF)0$$aZhang, Xu$$b10
000624847 7001_ $$0P:(DE-HGF)0$$aZhou, Yingtang$$b11
000624847 7001_ $$0P:(DE-H253)PIP1105202$$aRam, Ranit$$b12
000624847 7001_ $$0P:(DE-HGF)0$$aPolesso, Barbara$$b13
000624847 7001_ $$0P:(DE-HGF)0$$aGuha, Anku$$b14
000624847 7001_ $$0P:(DE-HGF)0$$aSu, Jiaqi$$b15
000624847 7001_ $$0P:(DE-H253)PIP1092317$$aLobo, Carlos$$b16
000624847 7001_ $$0P:(DE-H253)PIP1024252$$aHaumann, Michael$$b17
000624847 7001_ $$0P:(DE-HGF)0$$aSpatschek, Robert$$b18
000624847 7001_ $$0P:(DE-HGF)0$$aSunde, Svein$$b19
000624847 7001_ $$0P:(DE-HGF)0$$aGan, Lin$$b20
000624847 7001_ $$0P:(DE-HGF)0$$aHuang, Ming$$b21
000624847 7001_ $$0P:(DE-HGF)0$$aZhou, Xiaoyuan$$b22
000624847 7001_ $$0P:(DE-H253)PIP1008104$$aRoth, Christina$$b23
000624847 7001_ $$0P:(DE-H253)PIP1096034$$aLehnert, Werner$$b24
000624847 7001_ $$0P:(DE-H253)PIP1086067$$aCherevko, Serhiy$$b25
000624847 7001_ $$0P:(DE-HGF)0$$aGan, Liyong$$b26
000624847 7001_ $$0P:(DE-H253)PIP1105188$$aGarcia de Arquer, F. Pelayo$$b27$$eCorresponding author
000624847 7001_ $$0P:(DE-H253)PIP1096036$$aShviro, Meital$$b28$$eCorresponding author
000624847 773__ $$0PERI:(DE-600)2088679-2$$a10.1038/s41563-025-02128-7$$gVol. 24, no. 5, p. 753 - 761$$n5$$p753 - 761$$tNature materials$$v24$$x1476-1122$$y2025
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