Electrochemical CO₂ reduction driven by intermittent renewable energy sources is usually limited by output voltage fluctuation caused by their spatial and temporal discontinuities of those renewable energy sources. The development of high-performance catalysts with large current density and high selectivity for the target products in a wide operating potential window is of great importance for utilizing intermittent renewable electricity for CO₂ reduction. Herein, we report a two-dimensional (2D) Ni phthalocyanine polymer (NiPcP) that displays superior catalytic activity and high selectivity for CO₂-to-CO conversion with a Faradaic efficiency (FE_CO) over 98% in a wide operating potential window from –0.15 to –0.60 V and a maximum current density of 236 mA cm^–2 at –0.6 V. At an overpotential of 0.39 V, NiPcP delivers a nearly 100% FE of CO production, a large CO current density of 197 mA cm^–2 and an impressive TOF of 23148 h^–1. Experimental and theoretical results disclose that the inherent electronic structure of Ni units, conjugated nature and hydrophobicity of NiPcP promote the CO₂RR to CO production and restrain the competitive hydrogen evolution reaction, thereby enhancing the catalytic activity and selectivity for CO₂-to-CO conversion. This work emphasizes the importance of modulating the structure and hydrophobicity of nanostructured catalysts for enhancing CO₂RR performance.

间歇性可再生能源驱动的电化学CO ₂还原通常受限于由这些可再生能源的空间和时间不连续性引起的输出电压波动。开发具有大电流密度和高选择性的目标催化剂，在宽的工作潜力范围内的高性能催化剂，对于利用间歇性可再生电力减少CO ₂至关重要。在本文中，我们报道了二维（2D）的Ni酞菁聚合物（NiPcP），其显示优异的催化活性高，用于CO选择性₂ -to-CO转化用法拉第效率（FE _CO）在–0.15至–0.60 V的宽工作电势范围内，且–0.6 V时的最大电流密度为236 mA cm ^–2时，超过98％。在0.39 V的过电势下，NiPcP可产生近100％的CO产生FE ，CO电流密度大，为197 mA cm ^–2，TOF为23148 h ^–1。实验和理论结果表明，Ni单元的固有电子结构，NiPcP的共轭性质和疏水性可促进CO ₂ RR生成CO并抑制竞争性氢释放反应，从而增强对CO ₂的催化活性和选择性。-CO转换。这项工作强调了调节纳米结构催化剂的结构和疏水性以增强CO ₂ RR性能的重要性。