Reversing the thermal induced sintering phenomenon and forming high temperature stable fine dispersed metallic centers with unique structural and electronic properties is one of the ever-lasting targets of heterogeneous catalysis. Here we report that the dispersion of metallic Ni particles into under-coordinated two-dimensional Ni clusters over γ-Mo₂N is a thermodynamically favorable process based on the AIMD simulation. A Ni-4nm/γ-Mo₂N model catalyst is synthesized and used to further study the reverse sintering effect by the combination of multiple in-situ characterization methods, including in-situ quick XANES and EXAFS, ambient pressure XPS and environmental SE/STEM etc. The under-coordinated two-dimensional layered Ni clusters on molybdenum nitride support generated from the Ni-4nm/γ-Mo₂N has been demonstrated to be a thermally stable catalyst in 50 h stability test in CO₂ hydrogenation, and exhibits a remarkable catalytic selectivity reverse compared with traditional Ni particles-based catalyst, leading to a chemo-specific CO₂ hydrogenation to CO.

逆转热致烧结现象并形成具有独特结构和电子性能的高温稳定的细分散金属中心是多相催化永恒的目标之一。在这里，我们报道了基于 AIMD 模拟，金属 Ni 颗粒在 γ-Mo ₂ N 上分散到欠配位的二维 Ni 团簇中是一个热力学有利的过程。合成了Ni-4nm/γ-Mo ₂ N模型催化剂，并结合多种原位表征方法（包括原位快速XANES和EXAFS、常压XPS和环境SE/）进一步研究了反向烧结效应。 STEM等。由Ni-4nm/γ-Mo ₂ N生成的氮化钼载体上的欠配位二维层状Ni簇在CO ₂加氢50小时稳定性测试中被证明是一种热稳定催化剂，并表现出与传统的基于镍颗粒的催化剂相比，具有显着的催化选择性逆转，导致化学特异性的CO ₂加氢为CO。