2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO2 Electrocatalysis at Low Overpotentials,Advanced Materials

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2D Copper Tetrahydroxyquinone Conductive Metal–Organic Framework for Selective CO2 Electrocatalysis at Low Overpotentials
Advanced Materials ( IF 27.4 ) Pub Date : 2021-02-01 , DOI: 10.1002/adma.202004393
Leily Majidi ₁ , Alireza Ahmadiparidari ₁ , Nannan Shan ₂ , Saurabh N. Misal ₁ , Khagesh Kumar ₃ , Zhehao Huang ₄ , Sina Rastegar ₁ , Zahra Hemmat ₁ , Xiaodong Zou ₄ , Peter Zapol ₂ , Jordi Cabana ₃ , Larry A. Curtiss ₂ , Amin Salehi‐Khojin ₁

Affiliation

Metal–organic frameworks (MOFs) are promising materials for electrocatalysis; however, lack of electrical conductivity in the majority of existing MOFs limits their effective utilization in the field. Herein, an excellent catalytic activity of a 2D copper (Cu)‐based conductive MOF, copper tetrahydroxyquinone (CuTHQ), is reported for aqueous CO₂ reduction reaction (CO₂RR) at low overpotentials. It is revealed that CuTHQ nanoflakes (NFs) with an average lateral size of 140 nm exhibit a negligible overpotential of 16 mV for the activation of this reaction, a high current density of ≈173 mA cm⁻² at −0.45 V versus RHE, an average Faradaic efficiency (F.E.) of ≈91% toward CO production, and a remarkable turnover frequency as high as ≈20.82 s⁻¹. In the low overpotential range, the obtained CO formation current density is more than 35 and 25 times higher compared to state‐of‐the‐art MOF and MOF‐derived catalysts, respectively. The operando Cu K‐edge X‐ray absorption near edge spectroscopy and density functional theory calculations reveal the existence of reduced Cu (Cu⁺) during CO₂RR which reversibly returns to Cu²⁺ after the reaction. The outstanding CO₂ catalytic functionality of conductive MOFs (c‐MOFs) can open a way toward high‐energy‐density electrochemical systems.

中文翻译：

低过电势下选择性CO2电催化的二维铜四羟基醌导电金属-有机骨架

金属有机框架（MOF）是用于电催化的有前途的材料。但是，大多数现有MOF中缺乏导电性限制了它们在现场的有效利用。在此，据报道，在低超电势下，水性CO ₂还原反应（CO ₂ RR）具有二维铜（Cu）基导电MOF优异的催化活性，即四羟基醌铜（CuTHQ）。据透露，铜 THQ纳米薄片（NFS），用140的平均横向尺寸纳米表现出可忽略的超电势16毫伏的用于该反应的≈173毫安cm的高电流密度的激活^-2在相对于RHE为-0.45 V时，CO产生的平均法拉第效率（FE）约为91％，显着的周转频率高达≈20.82s ^-1。在低超电势范围内，获得的CO形成电流密度分别比最先进的MOF和MOF衍生的催化剂高35倍和25倍。接近边缘光谱的操作性K K边缘X射线吸收和密度泛函理论计算揭示了CO ₂ RR过程中还原的Cu（Cu ⁺）的存在，反应后可逆地还原为Cu ²⁺。导电MOF（c-MOF）出色的CO ₂催化功能可以为通向高能量密度电化学系统开辟道路。

更新日期：2021-03-09

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