Gadolinium-Mediated Oxygen Affinity Induced Efficient Covalorization of CH<sub>4</sub> and N<sub>2</sub>O in an Ir–Gd<sub>2</sub>O<sub>3</sub> Single-Atom Catalyst
Yunshuo Wu, Haiqiang Wang, Feng‐Shou Xiao, Zhongbiao Wu
Abstract
Valorization of nitrous oxide (N 2 O) and methane (CH 4 ) for chemicals has garnered growing interest for mitigating their climate impact. Dry reforming of methane (DRM) with industrial N 2 O exhaust offers a promising route. However, the DRM reaction often requires rigorous temperatures (>650 °C) accompanied by overoxidation, hindering CO and H 2 formation due to weak oxygen binding on catalysts. Here, we report a Gd 2 O 3 -supported iridium single-atom catalyst (SAC), with an effective Ir 1 –Gd 2 O 3 synergy. At only 450 °C, it exhibits high N 2 O (99.3%) and CH 4 (48.2%) conversion and syngas yields (138.3 mol of CO kg cat –1 h –1 and 184.9 mol of H 2 kg cat –1 h –1 ) and a H 2 /CO ratio of 1.34, over 100 h. Mechanism studies revealed that Gd 2 O 3 enabled controlled oxygen release for CO production, while Ir single atoms facilitated CH 4 activation and H 2 formation. This work presents a low-temperature, sustainable strategy for greenhouse gas utilization and highlights the potential of Gd 2 O 3 -based single-atom catalysts in heterogeneous catalysis.