Abstract
Developing efficient and stable electrocatalysts for the acidic oxygen evolution reaction (OER) is vital for advancing proton exchange membrane water electrolysis (PEMWE) technologies. Here, we report a flux synthesis of nitrogen-doped Ti–Ru rutile-type solid-solution oxides (M-TiRu4) using molten NaNO3 as the flux medium. The flux medium promotes the low-temperature conversion of TiN to rutile TiO2, while in situ-formed RuO2 nanoparticles facilitate lattice templating and couple with interfacial ion migration, enabling the formation of homogeneous solid solutions with abundant lattice heterogeneity. Simultaneously, nitrogen atoms are stably incorporated into the lattice of solid solutions, inducing bandgap narrowing, which enhances electronic conductivity. The developed M-TiRu4 catalyst exhibits exceptional acidic OER performance, delivering a low overpotential of 194 mV at 10 mA cm−2, superior durability over 600 h, and a Ru mass activity 7.8 times that of commercial RuO2. At the device level, M-TiRu4 enables PEMWE operation at 1.64 V @ 2 A cm−2 and maintains stable performance at 500 mA cm−2 for 200 h with a minimal degradation rate of 20 µV h−1. This work demonstrates a robust approach for designing high-performance, durable acidic OER catalysts via synergistic lattice and electronic structure engineering, paving the way for next-generation water-splitting technologies.
| Original language | English |
|---|---|
| Article number | e202514922 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 64 |
| Issue number | 49 |
| DOIs | |
| State | Published - Dec 1 2025 |
Funding
This article is based on work supported as part of the Atomic-C2E project by the US Department of Energy, Office of Science, under award number DE-SC-0024716. Use of the NSLS-II (NIST beamline 6-BM) was supported by the Department of Energy Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory (BNL) under contract no. DE-SC0012704. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 using NERSC award BES-ERCAP0032102. The authors also wish to express their appreciation to the Institute for Energy and Environment (IEE), Institute for a Secure and Sustainable Environment (ISSE) and Center for Materials Processing (CMP) from University of Tennessee Knoxville. This article is based on work supported as part of the Atomic‐C2E project by the US Department of Energy, Office of Science, under award number DE‐SC‐0024716. Use of the NSLS‐II (NIST beamline 6‐BM) was supported by the Department of Energy Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory (BNL) under contract no. DE‐SC0012704. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231 using NERSC award BES‐ERCAP0032102. The authors also wish to express their appreciation to the Institute for Energy and Environment (IEE), Institute for a Secure and Sustainable Environment (ISSE) and Center for Materials Processing (CMP) from University of Tennessee Knoxville.
Keywords
- Acidic oxygen evolution reaction
- Lattice engineering
- Molten salt synthesis
- Nitrogen doping
- Solid solution