Scalable Defect Engineering of Pt3Te4Nanosheets Activates an Electro-Switchable and Termination-Dependent PtO2Skin for Low-Overpotential Hydrogen Evolution
Dadiani T. D’Olimpio G. Tamasauskaite-Tamasiunaite L. Zenone S. Kuo C.-N. Amati M. Milosz Z. Gregoratti L. Hrbek T. Rodríguez M.G. Istrate M.C. Lue C.S. Lobko Y. Ghica C. Norkus E. Zhang Y.-W. Cupolillo A. Boukhvalov D.W. Politano A.
11 February 2026American Chemical Society
ACS Applied Materials and Interfaces
2026#18Issue 58026 - 8038 pp.
Topological materials are promising electrocatalysts for the hydrogen evolution reaction (HER) because of their protected electronic states and exceptional carrier mobility. Among them, the topological metal Pt3Te4 (mitrofanovite) exhibits low Tafel slopes in the nanocrystals. Realizing this potential in scalable catalyst systems requires nanoscale texturing coupled with precise control of the surface chemistry under operating conditions. Herein, we demonstrate that hydrogen peroxide (H2O2)-assisted liquid-phase exfoliation (LPE) of bulk Pt3Te4 yields nanoporous nanosheets that retain their metallic character and are chemically preconditioned to develop a bias-controlled PtO2 skin that governs the catalytic activity. Crucially, spectromicroscopy resolves termination-selective oxidation: PtO2 forms exclusively on PtTe2-like terminations, whereas Pt2Te2 terminations remain metallic. Operando ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) in an electrochemical cell revealed the bias-dependent emergence of surface oxide phases in H2O2-treated nanosheets. The joint effect of the higher accessible site density imparted by nanoporosity and the emergence of a bias-controlled PtO2/PtTe2-terminated Pt3Te4 surface junction rationalizes the improved catalytic activity: the overpotential at 10 mA cm–2 decreases by ∼30% (from 113.1 to 78.7 mV), while the exchange current density more than triples (from 0.106 to 0.347 mA cm–2), all with an unchanged Tafel slope (∼53 mV dec–1) and sustained stability over 50 h in acid. By combining a single scalable top-down step with operando proof that the catalytically active oxide is switched on by bias rather than being a static passivation layer, this study establishes a precise interface-engineering principle for Pt3Te4 nanosheets and a practical path to efficient, scalable HER catalysts based on nanosheets of topological metals.
defect engineering , electroswitchable oxide skin , hydrogen evolution reaction , liquid-phase exfoliation , operando XPS , platinum telluride , scanning photoemission microscopy , termination-dependent catalysis
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Department of Physical and Chemical Sciences, University of L’Aquila, via Vetoio, L’Aquila (AQ), 67100, Italy
Department of Catalysis, Center for Physical Sciences and Technology, Sauletekio Ave. 3, Vilnius, LT-10257, Lithuania
Department of Applied Science and Technology, Polytechnic University of Turin, Corso Castelfidardo, 39, Turin, 10129, Italy
Academy of Innovative Semiconductor and Sustainable Manufacturing (AISSM), National Cheng Kung University, Tainan, 70101, Taiwan
Department of Physics, National Cheng Kung University, Tainan, 70101, Taiwan
Taiwan Consortium of Emergent Crystalline Materials (TCECM), National Science and Technology Council, Taipei, 10601, Taiwan
Elettra─Sincrotrone Trieste SCpA, AREA Science Park, Strada Statale 14 km 163.5, Trieste, 34149, Italy
Department of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University, V Holešovičkách 2, Prague, 18000, Czech Republic
National Institute of Materials Physics, Atomistilor 405A, Magurele, 077125, Romania
Institute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR), Singapore, 138632, Singapore
Department of Physics, University of Calabria, Via P. Bucci cubo 31/C, Cosenza, Rende, 87036, Italy
College of Science, Institute of Materials Physics and Chemistry, Nanjing Forestry University, Nanjing, 210037, China
Institute of Physics and Technology, Satbayev University, Ibragimov str. 11, Almaty, 050032, Kazakhstan
Department of Physical and Chemical Sciences
Department of Catalysis
Department of Applied Science and Technology
Academy of Innovative Semiconductor and Sustainable Manufacturing (AISSM)
Department of Physics
Taiwan Consortium of Emergent Crystalline Materials (TCECM)
Elettra─Sincrotrone Trieste SCpA
Department of Surface and Plasma Science
National Institute of Materials Physics
Institute of High Performance Computing (IHPC)
Department of Physics
College of Science
Institute of Physics and Technology
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