ABSTRACT The efficient CO 2 ‐to‐propane conversion represents a critical pathway for greenhouse gas valorization and clean energy production, constrained by challenges including inefficient CO 2 activation, imprecise C─C coupling regulation, and insufficient catalyst stability. Here, ZrZnO X ‐based metal oxide catalysts from binary to penta‐component were synthesized via solution combustion. Characterization reveals Al 3+ incorporation plays a decisive structure‐directing role. Al 3+ suppresses segregated ZnGa 2 O 4 formation and promotes In 3+ /Ga 3+ substitution into ZrO 2 ‐derived fluorite‐related lattice, forming compositionally homogeneous ZrZnInGaAlO X high‐entropy oxide with uniform elemental distribution, enriched oxygen vacancies, and redistributed electronic environments. Coupled with H‐SSZ‐13 zeolite, the stabilized oxide enabled direct CO 2 hydrogenation to propane (33.67% conversion, 76.35% selectivity at 380°C). Post‐reaction characterization revealed partial In segregation into In 2 O 3 domains while the multicomponent matrix retained generally homogeneous elemental distribution on the microscale, indicating mild structural reconstruction rather than catastrophic collapse. These results demonstrate Al 3+ ’s essential role in stabilizing high‐entropy oxide architectures and improving catalytic activity and durability in tandem CO 2 hydrogenation, providing an effective materials design strategy for CO 2 conversion into value‐added hydrocarbons.
Zhao et al. (Fri,) studied this question.