Exploration of non-noble-metal-based catalysts with high catalytic activity and selectivity is significant for driving innovation in green chemistry and technology. Herein, we report a facile synthesis of two-dimensional (2D) NiCo-MOF bimetallic nanosheets, which exhibited excellent catalytic performance, in terms of high conversion rate (99.9%), high selectivity (98.0–99.9%), rapid reduction kinetics (1–10 min) and mild reaction conditions (room temperature), for the catalytic hydrogenation of various nitroarenes and aldehyde compounds. These excellent catalytic performances were distinctly superior to those of other catalysts, and they can stem from the unique structure of the 2D NiCo-MOF bimetallic catalyst. The bimetallic system could effectively enhance the reaction selectivity with considerable reactivity, and the maximized utilization of the dispersed catalytic sites in the 2D MOF-based single-atom catalytic system could efficiently enhance the overall catalytic activity. Thus, the co-action of the synergistic effect of the bimetallic system and the maximal utilization of the catalytic sites endowed the 2D bimetallic MOF catalytic system with rapid, efficient, and highly selective catalysis under extremely gentle conditions. The reaction mechanism of the hydrogenation was investigated by density functional theory calculations and X-ray photoelectron spectroscopy. Our study provides an appealing strategy for constructing highly efficient and selective catalysts and demonstrates the significance of 2D ultrathin MOF nanosheets in the catalysis field.

中文翻译：

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超薄 2D NiCo-MOF 双金属纳米片作为硝基芳烃化学选择性加氢的单原子催化剂


探索具有高催化活性和选择性的非贵金属基催化剂对于推动绿色化学和技术的创新具有重要意义。在此，我们报道了二维 （2D） NiCo-MOF 双金属纳米片的简单合成，它在高转化率 （99.9%）、高选择性 （98.0-99.9%）、快速还原动力学 （1-10 分钟） 和温和的反应条件（室温）方面表现出优异的催化性能，用于各种硝基芳烃和醛类化合物的催化加氢。这些优异的催化性能明显优于其他催化剂，它们可以源于 2D NiCo-MOF 双金属催化剂的独特结构。双金属体系可以有效地提高反应选择性，具有相当大的反应活性，并且最大限度地利用二维 MOF 基单原子催化体系中分散的催化位点可以有效地提高整体催化活性。因此，双金属体系的协同效应和催化位点的最大利用的协同作用赋予了二维双金属 MOF 催化体系在极其温和的条件下具有快速、高效和高选择性的催化作用。通过密度泛函理论计算和 X 射线光电子能谱研究了氢化反应机理。我们的研究为构建高效和选择性催化剂提供了一种有吸引力的策略，并证明了二维超薄 MOF 纳米片在催化领域的重要性。