Developing efficient and stable catalysts for electrochemical CO₂ reduction reaction (CO₂RR) in a wide potential window is highly desirable for achieving carbon neutrality, but remains greatly challenging. Herein, we demonstrate a facile synthetic strategy to synthesize transition metal nickel-nitrogen-carbon (Ni-N-C) catalyst where nickel nanoparticles have been in-situ encapsulated into N-doped carbon nanotubes (Ni@NCNT) for CO₂RR. Strikingly, the as-prepared Ni@NCNT catalyst shows a high CO Faradaic efficiency (>90%) in a wide potential range of −0.65 to −1.0 V versus reversible hydrogen electrode (vs. RHE), a large current density of 16.3 mA cm⁻² at −0.8 V vs. RHE and robust durability after a continuous electroreduction of 18 h. Density functional theory calculations suggest that compared to pure Ni (111) and Ni nanoparticles-free solid N-doped carbon nanorods (NCNR), Ni@NCNT can more effectively suppress H₂ evolution and stabilize ∗COOH intermediates without influencing ∗CO desorption, thus, giving rise to high activity and desirable selectivity toward CO₂RR.

为实现碳中和非常需要开发用于电化学 CO ₂还原反应 (CO ₂ RR) 的高效且稳定的催化剂，但仍具有很大的挑战性。在此，我们展示了一种简便的合成策略来合成过渡金属镍-氮-碳 (Ni-NC) 催化剂，其中镍纳米颗粒已被原位封装到用于 CO ₂ RR 的N 掺杂碳纳米管 (Ni@NCNT) 中。引人注目的是，与可逆氢电极相比，所制备的 Ni@NCNT 催化剂在 -0.65 至 -1.0 V 的宽电位范围内显示出高 CO 法拉第效率（>90%），电流密度为 16.3 mA cm ^-2 at -0.8 V vs. 连续电还原 18 小时后的 RHE 和坚固耐用性。密度泛函理论计算表明，与纯 Ni (111) 和不含 Ni 纳米颗粒的固体 N 掺杂碳纳米棒 (NCNR) 相比，Ni@NCNT 可以更有效地抑制 H ₂析出并稳定 ∗COOH 中间体而不影响 ∗CO 解吸，因此，产生高活性和对 CO ₂ RR 的理想选择性。