Low cost, highly selective and efficient electrocatalysts for CO₂ reduction reaction (CO2RR) is crucial for lowering the global carbon footprint and mitigating energy shortages. Here, we first report a highly selective and efficient electrocatalyst for CO₂RR to CO using a surface-regulated Ni nanoparticles supported on N-doped CMK-3 (N,O-Ni/CMK3). Compared with most Ni metal catalysts previously reported with severe competitive hydrogen evolution during the CO2RR, the N,O-Ni/CMK3 catalyst presents a superior CO faradaic efficiency of about 97%, a high CO partial current density (13.01 mA cm⁻¹) and turnover frequency (4.25 s⁻¹). The comprehensive characterization provides evidence that the N,O co-regulated Ni acts as the active center. Taking advantage of the N, O co-regulated chemical environment, N,O-Ni/CMK3 also displays a decent stability at negative potentials. Our work paves a novel approach for developing transition metal catalysts for CO2RR with enhanced activity and selectivity via regulating surface chemical environment.

用于 CO ₂还原反应 (CO2RR) 的低成本、高选择性和高效电催化剂对于降低全球碳足迹和缓解能源短缺至关重要。在这里，我们首先报告了一种使用在N掺杂 CMK-3 (N,O-Ni/CMK3)上负载的表面调节 Ni 纳米粒子将CO ₂ RR 转化为 CO 的高选择性和高效电催化剂。与之前报道的大多数在 CO2RR 过程中具有严重竞争性析氢的 Ni 金属催化剂相比，N,O-Ni/CMK3 催化剂具有约 97% 的优越 CO 法拉第效率、高 CO 分流密度 (13.01 mA cm ^-1 )和周转频率（4.25 s ^-1）。综合表征提供了证据表明 N,O 共调节的 Ni 作为活性中心。利用 N, O 共同调节的化学环境，N,O-Ni/CMK3 在负电位下也表现出不错的稳定性。我们的工作为通过调节表面化学环境开发具有增强活性和选择性的 CO2RR 过渡金属催化剂铺平了道路。