The rational synthesis of earth-abundant materials with excellent electrocatalytic performances plays a critical role in electrochemical CO₂ reduction (ECR) to obtain value-added chemical products or fuels. Here we demonstrate a defective graphene (DG) as such an electrocatalyst candidate via a nitrogen removal method. The graphene with a large amount of topological defects offered abundant catalytically active sites, high electronic conductivity and strong adsorption of CO₂. Attributed to these features, the DG exhibited significantly higher electrocatalytic CO₂ reduction performances with an excellent faradaic efficiency of ∼84% at −0.6 V vs. reversible hydrogen electrode and a larger current density, compared to pristine graphene, nitrogen-doped graphene and edge-rich graphene. This work suggests a promising method for further designing efficient metal-free electrocatalysts for CO₂ reduction.

合理合成具有优异电催化性能的富地球材料在电化学CO ₂还原（ECR）以获得增值的化学产品或燃料中起着至关重要的作用。在这里，我们通过脱氮方法论证了一种有缺陷的石墨烯（DG）作为这种电催化剂的候选者。具有大量拓扑缺陷的石墨烯具有丰富的催化活性位，高电子电导率和对CO _2的强吸附性。由于这些特征，DG表现出明显更高的电催化CO ₂与原始石墨烯，氮掺杂石墨烯和富边石墨烯相比，在可逆氢电极下，在-0.6 V时具有约84％的极佳法拉第效率和更大的电流密度，具有良好的还原性能。这项工作为进一步设计用于CO ₂还原的高效无金属电催化剂提出了一种有前途的方法。