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oai:figshare.com:article/34037483 2026-10-01T01:04:58Z category_1 category_4 category_915 category_12 category_16 category_19 category_24 category_272 category_873 category_39 category_132 category_135 portal_63 item_type_6 month_year_10_2026

Atomic Scale Origin of the OER Activity–Stability Trade-Off in NiFe Layered Double Hydroxides: Lattice-Site Oxygen Triggers Fe Leaching Liancong Xu (25147292) Zhuoyang Xie (20648456) Jin Liu (12833) Xia Chen (299366) Linping Hu (23003391) Rui Wu (237891) Jiawei Liu (553742) Li Li (14993) Zidong Wei (1554397) Biophysics Biochemistry Physical Sciences not elsewhere classified Cell Biology Physiology Pharmacology Evolutionary Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Ecology Infectious Diseases Computational Biology assisted interfacial reconstruction octahedral coordination structure oer ), yet 4 </ sub provide theoretical guidance atomic scale origin site oxygen regeneration site oxygen coupling theoretical overpotential vacancy structure coupled structure vacancy suppression tetrahedral feo term stability substitution pathway representative non reconstructed double oer conditions metal catalyst induced deactivation h species findings elucidate determining barrier 29 v 05 ev NiFe layered double hydroxide (NiFe-LDH) is a representative non-precious-metal catalyst for the alkaline oxygen evolution reaction (OER), yet its long-term stability is compromised by Fe leaching under OER conditions. Herein, using density functional theory calculations and constant-potential ab initio molecular dynamics simulations, we provide an atomic-scale understanding linking high OER activity to the origin of Fe leaching. We reveal that the OER on the reconstructed active NiFeOOH phase preferentially follows an adsorbate-site/lattice-site oxygen coupling (ALOC) mechanism, achieving a theoretical overpotential as low as 0.29 V. Notably, the coupled structure that enables this high OER activity also drives the accumulation of oxygen vacancies. We identify the reconstructed double-oxygen-vacancy structure, formed through solvation-assisted interfacial reconstruction, as the precursor for Fe leaching. Subsequently, an OH^–-assisted coordination/substitution pathway at undercoordinated Fe sites progressively disturbs the octahedral coordination structure, leading to Fe leaching as a tetrahedral FeO₄H species with a rate-determining barrier of 1.05 eV. These findings elucidate how lattice-site-oxygen-involved OER catalysis inherently triggers Fe-leaching-induced deactivation and provide theoretical guidance for stabilizing NiFe-LDH through oxygen-vacancy suppression, lattice-site oxygen regeneration, and local coordination environment strengthening. 2026-09-30T00:00:00Z Text Journal contribution 10.1021/acs.jpcc.6c05263.s001 https://figshare.com/articles/journal_contribution/Atomic_Scale_Origin_of_the_OER_Activity_Stability_Trade-Off_in_NiFe_Layered_Double_Hydroxides_Lattice-Site_Oxygen_Triggers_Fe_Leaching/34037483 CC BY-NC 4.0