Intrinsic Defect-Rich Graphene Coupled Cobalt Phthalocyanine for Robust Electrochemical Reduction of Carbon Dioxide,ACS Applied Materials & Interfaces

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Intrinsic Defect-Rich Graphene Coupled Cobalt Phthalocyanine for Robust Electrochemical Reduction of Carbon Dioxide
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-05-19 , DOI: 10.1021/acsami.1c04344
Fengxia Liang ₁ , Jun Zhang ₁ , Zewei Hu ₁ , Chao Ma ₁ , Wenpeng Ni ₁ , Yan Zhang ₁ , Shiguo Zhang ₁

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Carbon-based matrix is known to exert a profound influence on the stability and activity of a supported molecular catalyst for electrochemical CO₂ reduction reaction (eCO₂RR), while regulating the interfacial π–π interaction by designing functional species on the carbon matrix has seldom been explored. Herein, promoted π electron transfer between a graphene substrate and cobalt phthalocyanine (CoPc) is achieved by introducing abundant intrinsic defects into graphene (DrGO), which not only generates more electrochemically active Co sites and leads to a positive shift of the Co²⁺/Co⁺ reduction potential but also enhances the CO₂ chemical adsorption. Consequently, as compared to the defect-free counterpart rGO-CoPc, DrGO-CoPc could yield CO with a Faradaic efficiency (FE_CO) higher than 85% in a wide potential range from −0.53 to −0.88 V, and the largest FE_CO and partial CO current density (J_CO) achieve 90.2% and 73.9 mA cm^–2, respectively. More importantly, both FE_CO and J_CO can be dramatically improved when conducting eCO₂RR in an ionic liquid-based electrolyte, for which FE_CO is higher than 90.0% in a wide potential range of 600 mV, with the peak J_CO of up to 113.6 mA cm^–2 in an H-type cell. The excellent eCO₂RR performance of DrGO-CoPc rates itself as one of the best immobilized molecular catalysts.

中文翻译：

富含本征缺陷的石墨烯偶联钴酞菁，用于二氧化碳的稳健电化学还原

众所周知，碳基基质对用于电化学 CO ₂还原反应 (eCO ₂ RR)的负载型分子催化剂的稳定性和活性产生深远的影响，同时通过设计碳基质上的功能物种来调节界面 π-π 相互作用具有很少被探索。在此，石墨烯基底和钴酞菁（CoPc）之间的 π 电子转移是通过将丰富的本征缺陷引入石墨烯（DrGO）来实现的，这不仅会产生更多的电化学活性 Co 位点，而且会导致 Co ²⁺ / Co ⁺还原潜力但也提高了 CO ₂化学吸附。因此，与无缺陷的对应物 rGO-CoPc 相比，DrGO-CoPc 可以在从 -0.53 到 -0.88 V 的广泛电位范围内产生法拉第效率（FE _CO）高于 85% 的_CO，以及最大的 FE _CO和部分 CO 电流密度 ( J _CO ) 分别达到 90.2% 和 73.9 mA cm ^–2。更重要的是，在基于离子液体的电解质中进行 eCO ₂ RR时，FE _CO和J _CO都可以得到显着改善，在600 mV 的宽电位范围内，FE _CO高于 90.0%，峰值J _CO为高达 113.6 mA cm ^–2在 H 型电池中。DrGO-CoPc出色的 eCO ₂ RR 性能使其成为最好的固定分子催化剂之一。

更新日期：2021-06-02

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