A Porphyrin/Graphene Framework: A Highly Efficient and Robust Electrocatalyst for Carbon Dioxide Reduction,Advanced Energy Materials

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A Porphyrin/Graphene Framework: A Highly Efficient and Robust Electrocatalyst for Carbon Dioxide Reduction
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-07-15 , DOI: 10.1002/aenm.201801280
Jaecheol Choi ₁ , Pawel Wagner ₁ , Rouhollah Jalili _{1,

2} , Jeonghun Kim ₃ , Douglas R. MacFarlane ₄ , Gordon G. Wallace ₁ , David L. Officer ₁

Affiliation

Developing immobilized molecular complexes, which demonstrate high product efficiencies at low overpotential in the electrochemical reduction of CO₂ in aqueous media, is essential for the practical production of reduction products. In this work, a simple and facile self‐assembly method is demonstrated by electrostatic interaction and π–π stacking for the fabrication of a porphyrin/graphene framework (FePGF) composed of Fe(III) tetraphenyltrimethylammonium porphyrin and reduced liquid crystalline graphene oxide that can be utilized for the electrocatalytic reduction of CO₂ to CO on a glassy carbon electrode in aqueous electrolyte. The FePGF results in an outstanding robust catalytic performance for the production of CO with 97.0% faradaic efficiency at an overpotential of 480 mV and superior long‐term stability relative to other heterogeneous molecular complexes of over 24 h (cathodic energy efficiency: 58.1%). In addition, a high surface area carbon fiber paper is used as a substrate for FePGF catalyst, resulting in enhanced current density of 1.68 mA cm⁻² with 98.7% CO faradaic efficiency at an overpotential of 430 mV for 10 h, corresponding to a turnover frequency of 2.9 s⁻¹ and 104 400 turnover number. Furthermore, FePGF/CFP has one of the highest cathodic energy efficiencies (60.9%) reported for immobilized metal complex catalysts.

中文翻译：

卟啉/石墨烯骨架：一种高效且坚固的二氧化碳还原电催化剂

开发固定化的分子配合物，对于在还原介质的实际生产中必不可少的，所述固定化的分子配合物在电化学还原水性介质中的CO _2时，在低过电势下显示出高的产品效率。在这项工作中，通过静电相互作用和π-π堆叠展示了一种简单而便捷的自组装方法，该方法用于制造由铁（III）四苯基三甲基铵卟啉和可还原的液晶氧化石墨烯组成的卟啉/石墨烯骨架（FePGF）。用于电催化还原CO ₂在水性电解质中的玻璃碳电极上还原成CO。FePGF在480 mV的超电势下具有97.0％的法拉第效率，相对于24小时以上的其他非均质分子络合物，具有出色的鲁棒催化性能，可产生97.0％的法拉第效率，且长期稳定性更高（阴极能效：58.1％）。此外，高表面积碳纤维纸用作FePGF催化剂的底物，在430 mV的超电势下保持10 h产生的电流密度为1.68 mA cm ^-2，具有98.7％的CO法拉第效率，对应于周转率2.9 s ^-1的频率和104400的周转次数。此外，FePGF / CFP具有固定化金属络合物催化剂的最高阴极能效（60.9％）之一。

更新日期：2018-07-15

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