The development of high-performance electrocatalysts for CO₂ reduction reaction (CO2RR) is a prerequisite to enable CO₂-to-fuels electrolysis a feasible solution for reaching a carbon neutral cycle and producing value-added fuels. In this work, we report the design of a novel nanostructured electrocatalyst consisting of carbon nanotube/carbon nanosheet architecture with N and Fe doping (NFe-CNT/CNS) by a SiO₂-protected calcination strategy. The hierarchical structure of CNT/CNS affords abundant N-induced defects and Fe−N species as highly active sites and facilitates mass transportation, and carbon nanotube also offers a smooth route for charge transfer in the CO2RR process. These synergistic merits afford NFe-CNT/CNS with high performance for CO2RR in terms of a maximum FE of 69% at a low overpotential of 0.48 V, a small Tafel slope of 89 mV dec⁻¹, and enhanced stability for CO production in aqueous solution. The findings demonstrate that the integration of structural design and dopants optimization is effective to boost electrocatalytic activity of nanocarbons for CO₂ reduction.

研发用于CO ₂还原反应的高性能电催化剂（CO2RR）是使CO ₂燃料电解成为实现碳中和循环和生产增值燃料的可行解决方案的先决条件。在这项工作中，我们报告了一种新型的纳米结构电催化剂的设计，该催化剂由通过SiO ₂掺杂N和Fe的碳纳米管/碳纳米片结构（NFe-CNT / CNS）组成保护的煅烧策略。CNT / CNS的分层结构提供了大量的N诱导的缺陷和Fe-N物种作为高活性位点，并促进了质量迁移，并且碳纳米管还为CO2RR过程中的电荷转移提供了一条平滑的途径。这些协同优势使NFe-CNT / CNS具有出色的CO2RR性能，最大FE为69％，低过电势为0.48 V，Tafel斜率为89 mV dec ^-1小，并提高了在水溶液中生产CO的稳定性解决方案。这些发现表明，结构设计和掺杂剂优化的整合有效地提高了纳米碳对CO ₂还原的电催化活性。