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双原子催化剂以其独特的性质已成为催化领域新的研究前沿，双原子金属间的协同作用有望提高反应性能和理解复杂的催化反应过程。然而，现有研究主要集中于单原子催化剂与双原子催化剂性能的比较，如何精准控制金属原子间距离和双原子构型进而优化催化性能仍然是一个挑战。 近日，中国科学院大连化物所林坚研究员、福州大学林森教授和皇家墨尔本理工大学马天翼教授合作，以氮掺杂碳锚定的Ni和Fe双原子催化剂为研究对象，构筑出孤立的NiFe双原子、氮桥联的NiFe双原子、以及NiFe直接成键三种构型，研究NiFe原子间相互作用对电催化CO2还原性能的影响。
研究发现，三种构型催化剂上NiFe均以原子对形式高度分散，Ni和Fe原子间距离分别为~6.1 Å（NiFe-isolate），~2.7 Å（NiFe-N bridge）和~2.1 Å（NiFe-bonding）。其中，氮桥联的NiFe双原子中Ni向Fe转移更多电子，优化了Fe中心电子分布，表现出合适的金属间相互作用。与孤立的NiFe双原子、Ni-Fe直接成键双原子相比，氮桥联的NiN4和FeN4双原子催化剂提高了CO2电还原性能。 此外，DFT理论计算也表明当Ni和Fe具有合适距离时，即氮桥联的NiFe位点具有明显的协同作用，能够调节*COOH中间体具有合适的吸附强度，而且可以促进*CO脱附，加快了CO2电还原为CO过程。 最终，具有合适金属原子间距离的氮桥联NiFe双原子催化剂在CO2电催化还原反应中表现出高的电流密度、法拉第效率和良好的稳定性。该工作不仅揭示了双原子间距离效应，而且为调控双原子间相互作用以增强催化性能提供新思路。 论文信息 Tuning the Inter-Metal Interaction between Ni and Fe Atoms in Dual-Atom Catalysts to Boost CO2 Electroreduction Dr. Yang Chen, Jia Zhao, Xiaoli Pan, Prof Lin Li, Zhounan Yu, Prof. Xiaodong Wang, Prof. Tianyi Ma, Sen Lin, Prof. Jian Lin 文章的第一作者是中国科学院大连化物所的博士后陈洋和福州大学博士生赵佳。 Angewandte Chemie International Edition DOI: 10.1002/anie.202411543
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