Efficient selective electroreduction of carbon dioxide into energy-dense carbonaceous fuel products is highly desirable to mitigate environmental and energy-related problems. However, there is still a need to design an electrocatalyst with high selectivity and stability towards the CO₂ reduction reaction (CRR). Here, we present the promising performance of single-atom-Ni-decorated, nitrogen-doped carbon layers (SA-Ni@NC) as an efficient electrocatalyst for CRR. In this catalyst the Ni atoms are atomically dispersed and most have three-fold coordination with the N atoms in the carbon layers. Theoretical calculations show that the Ni-N3-C site can act as a highly active site for the reduction of CO₂ owing to the low energy barrier for the formation of *COOH intermediates. As a consequence, SA-Ni@NC exhibits a high Faradaic efficiency (up to 86.2%) for the production of CO at a potential of −0.6 V versus the reversible hydrogen electrode. Moreover, this simple method can also be used to produce a range of single-atom catalysts (such as SA-Co@NC). In view of the large family of zeolite imidazolate frameworks, we anticipate that our strategy will be extended to a variety of single-atom-decorated, nitrogen-doped carbon layers with a broad range of applications in energy conversion systems.

为了减轻环境和与能源有关的问题，非常需要将二氧化碳有效地选择性电还原为能量密集的含碳燃料产品。然而，仍然需要设计对CO ₂还原反应（CRR）具有高选择性和稳定性的电催化剂。在这里，我们提出了单原子镍修饰的氮掺杂碳层（SA-Ni @ NC）作为CRR的有效电催化剂的有前途的性能。在该催化剂中，Ni原子是原子分散的，并且大多数与碳层中的N原子具有三重配位。理论计算表明，Ni-N3-C位点可作为还原CO ₂的高活性位点由于形成* COOH中间体的能垒低。结果，相对于可逆氢电极，SA-Ni @ NC在-0.6 V的电势下产生高的法拉第效率（高达86.2％）。而且，这种简单的方法也可以用于生产一系列单原子催化剂（例如SA-Co @ NC）。鉴于存在大量的咪唑沸石骨架，我们预计我们的策略将扩展到各种单原子修饰的氮掺杂碳层，在能量转换系统中具有广泛的应用。