Amidst the global energy crisis and escalating CO₂ levels, developing efficient catalysts for converting CO₂ into sustainable energy sources is paramount. Here, we focus on Pd-M (M = Ni, Cu, Fe, In) bimetallic catalysts supported on hollow dodecahedron nickel cobalt oxide (h-NCO) for low-temperature CO₂ hydrogenation to formate. The catalytic evaluation of Pd_xM_y/h-NCO samples emphasized formate production, demonstrating significant enhancement from heteronuclear interactions between Pd and secondary metal species. Notably, Pd₈Ni₂/h-NCO achieved the highest formate production rate (187.07 mol_formate mol_Pd⁻¹h⁻¹) at relatively low temperatures (333 K). Experimental and density functional theory calculations unveiled that heteronuclear interactions induced charge polarization, reducing the reaction energy and facilitating CO₂ hydrogenation to formate. Additionally, the unique hollow dodecahedron NCO structure offered a substantial surface area and facilitated the effective dispersion of metal species, contributing to the enhanced catalytic performance. This work highlights the significance of heteronuclear interactions in bimetallic catalysts for CO₂ conversion, offering insights for catalyst system advancement.

中文翻译：

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Pd-M（M = Ni、Cu、Fe、In）双金属与空心十二面体镍钴氧化物的异核相互作用，用于增强低温 CO2 加氢制甲酸盐


在全球能源危机和 CO₂ 水平不断上升的情况下，开发将 CO₂ 转化为可持续能源的高效催化剂至关重要。在这里，我们重点介绍了负载在空心十二面体镍钴氧化物 （h-NCO） 上的 Pd-M（M = Ni、Cu、Fe、In）双金属催化剂，用于低温 CO₂ 加氢制甲酸盐。Pd_xM_y/h-NCO 样品的催化评价强调甲酸盐的产生，表明 Pd 和次生金属物种之间的异核相互作用显着增强。值得注意的是，Pd₈Ni₂/h-NCO 在相对较低的温度 （333 K） 下实现了最高的甲酸盐生成速率 （187.07 mol_甲酸盐 mol ^{Pd-1 h-1}）。实验和密度泛函理论计算揭示了异核相互作用诱导电荷极化，降低了反应能并促进了 CO₂ 加氢生成甲酸盐。此外，独特的空心十二面体 NCO 结构提供了相当大的表面积，并促进了金属种类的有效分散，有助于提高催化性能。这项工作强调了双金属催化剂中异核相互作用对 CO₂ 转化的重要性，为催化剂系统的发展提供了见解。