Impact of Strain-Induced Changes in Defect Chemistry on Catalytic Activity of Nd₂NiO_4+δ Electrodes

It is well known that defect chemistry plays a vital role in determining the electronic structure, ionic conductivity, and catalytic activity of metal oxides, as demonstrated in perovskite-based oxides to achieve desired functionalities. In this work, we explored the possibility of tuning the defect chemistry and hydrogen oxidation reaction (HOR) activity of Nd2NiO4+δ model thin films by controlling the lattice strain. Highly textured Nd2NiO4+δ thin films with different strain states were prepared on (110)- and (100)-oriented single-crystal yttrium-stabilized zirconium (YSZ) substrates using pulsed laser deposition. Electrochemical impedance spectroscopy results indicated that the NNO(100) film on the YSZ(110) substrate with larger tensile strain in the a–b plane and compressive strain along the c axis exhibited higher HOR activity than the NNO(110) film on the YSZ(100) substrate at 500–600 °C. The enhancement in HOR activity is attributed to the strain-induced difference in the oxygen defect concentration, as confirmed by high-resolution X-ray diffraction analysis. We believe that the correlation among the strain state, defect chemistry, and catalytic properties is helpful for rational design of more efficient electrode materials.