Sang-Cheol Shin, Iaan Cho, Sun Kyung Han, Jaewon Heo, Junhwi Han, Hotae Jeon, Jaehyun Lee, Min Kyung Cho, Daniel J. Preston, In Soo Kim, Bonggeun Shong, Won‐Kyu Lee
We present a strain-engineering strategy for oxygen-modified nickel telluride/nickel oxide heterostructures capable of enabling bifunctional alkaline water electrolysis with performance surpassing Pt and IrO x benchmarks. The heterostructures are synthesized via electrochemical Te dissolution and mild oxidation of mechanically exfoliated NiTe 2, followed by controlled strain induction through substrate buckling. Atomic-scale simulations and spectroscopic analyses indicate that Te-vacancy/O-substituted NiTe 2 domains promote oxygen-intermediate spillover between adjacent active sites, reducing OER overpotentials. In parallel, strained NiTe 2 domains facilitate hydrogen-intermediate transfer to NiO containing Ni vacancies, leading to accelerated HER kinetics and near-thermoneutral hydrogen adsorption. Strain modulation adjusts the electronic structure and increases active-site density, enabling stable operation at industrial-level current densities (>1 A cm –2 ). These findings illustrate how defect chemistry coupled with strain engineering can be utilized to develop high-performance, earth-abundant bifunctional electrocatalysts.