Abstract
The partial oxidation of methane (POM) is an attractive route for syngas production. However, Ni‐based catalysts often suffer from deactivation due to carbon deposition, metal sintering, and unstable metal–support interactions. In this study, the influence of zirconia (ZrO
2
) source and selected oxide promoters on the performance of Ni/ZrO
2
catalysts in POM was investigated. A series of 5 wt.% Ni catalysts were prepared using ZrO
2
supports from five commercial sources with different crystalline phases and textural properties. The best‐performing support was further modified by co‐impregnation with 10 wt.% Al
2
O
3
, TiO
2
, and Y
2
O
3
. The catalysts were characterized using physicochemical techniques and evaluated in a fixed‐bed reactor at 600°C under CH
4
/O
2
= 2.0 (GHSV = 14,400 mL·g
−1
·h
−1
). Raman spectroscopy and transmission electron microscopy were used to examine carbon deposition on spent catalysts. The results showed that the crystalline phase and textural properties of ZrO
2
influenced the catalytic performance. Among the unpromoted catalysts, Ni supported on DK‐type monoclinic ZrO
2
exhibited the highest CH
4
conversion (52.2%) and H
2
yield (51.4%), which was associated with improved Ni accessibility and moderate metal–support interactions. The introduction of oxide promoters further enhanced the activity, with Y‐promoted Ni/ZrO
2
achieving the highest performance (60% CH
4
conversion and 58.2% H
2
yield). XPS and H
2
‐TPR analyses suggested an increased contribution of interfacial Ni–O–Zr species together with enhanced reducibility for the Y‐promoted catalyst. These results indicate that both the ZrO
2
source and promoter type influence the balance between Ni dispersion, reducibility, and catalytic performance in POM.