Efficiently converting CO2 into value-added chemicals remains a significant challenge due to its inert nature. Here, we present the rational design of Pd/NiCo2O4 hybrid nanocatalysts with diverse morphologies for highly efficient CO2 hydrogenation to formate. The synergistic combination of Pd and NiCo2O4 offers improved catalytic activity towards formate production. Remarkably, the observation of a morphology-dependent Pd-NiCo2O4 interaction, linked to the presence of oxygen vacancies in NiCo2O4, significantly contributes to our understanding of catalytic activity. The rose-like Pd/NiCo2O4 catalyst achieves an impressive formate yield (85.3 molformate moltotalPd−1 h−1) due to its low oxygen vacancy concentration and subsequent generation of less positively-charged Pd species, emphasizing the crucial role of oxygen vacancies in hybrid nanocatalyst performance. These findings were further validated through density functional theory calculations, providing valuable insights into the design and optimization of nanocatalysts for CO2 hydrogenation. This contributes to the development of efficient and sustainable processes for CO2 utilization in the production of formate and other valuable chemicals.

中文翻译：

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Pd/NiCo2O4杂化纳米催化剂的抗缺陷工程增强CO2加氢生成甲酸盐


由于其惰性，有效地将二氧化碳转化为增值化学品仍然是一个重大挑战。在这里，我们提出了具有多种形貌的 Pd/NiCo2O4 杂化纳米催化剂的合理设计，用于高效 CO2 加氢生成甲酸盐。 Pd 和 NiCo2O4 的协同组合提高了甲酸生产的催化活性。值得注意的是，观察到与 NiCo2O4 中氧空位的存在相关的形态依赖性 Pd-NiCo2O4 相互作用，极大地有助于我们理解催化活性。玫瑰状的 Pd/NiCo2O4 催化剂由于其低氧空位浓度和随后产生的带正电荷较少的 Pd 物质，实现了令人印象深刻的甲酸盐产率（85.3 molformate moltotalPd−1 h−1），强调了氧空位在杂化中的关键作用纳米催化剂性能。这些发现通过密度泛函理论计算得到进一步验证，为二氧化碳加氢纳米催化剂的设计和优化提供了宝贵的见解。这有助于在甲酸盐和其他有价值的化学品生产中开发高效且可持续的二氧化碳利用工艺。