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Electroreduction of Carbon Dioxide Driven by the Intrinsic Defects in the Carbon Plane of a Single Fe–N4 Site
Advanced Materials ( IF 27.4 ) Pub Date : 2020-11-26 , DOI: 10.1002/adma.202003238 Wenpeng Ni 1 , Zhixiao Liu 1 , Yan Zhang 1 , Chao Ma 1 , Huiqiu Deng 2 , Shiguo Zhang 1 , Shuangyin Wang 3
Advanced Materials ( IF 27.4 ) Pub Date : 2020-11-26 , DOI: 10.1002/adma.202003238 Wenpeng Ni 1 , Zhixiao Liu 1 , Yan Zhang 1 , Chao Ma 1 , Huiqiu Deng 2 , Shiguo Zhang 1 , Shuangyin Wang 3
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Manipulating the in‐plane defects of metal–nitrogen–carbon catalysts to regulate the electroreduction reaction of CO2 (CO2RR) remains a challenging task. Here, it is demonstrated that the activity of the intrinsic carbon defects can be dramatically improved through coupling with single‐atom Fe–N4 sites. The resulting catalyst delivers a maximum CO Faradaic efficiency of 90% and a CO partial current density of 33 mA cm−2 in 0.1 m KHCO3. The remarkable enhancements are maintained in concentrated electrolyte, endowing a rechargeable Zn–CO2 battery with a high CO selectivity of 86.5% at 5 mA cm−2. Further analysis suggests that the intrinsic defect is the active sites for CO2RR, instead of the Fe–N4 center. Density functional theory calculations reveal that the Fe–N4 coupled intrinsic defect exhibits a reduced energy barrier for CO2RR and suppresses the hydrogen evolution activity. The high intrinsic activity, coupled with fast electron‐transfer capability and abundant exposed active sites, induces excellent electrocatalytic performance.
中文翻译：
Fe-N4单点碳平面中固有缺陷驱动的二氧化碳的电还原
操纵金属-氮-碳催化剂的面内缺陷来调节CO 2（CO 2 RR）的电还原反应仍然是一项艰巨的任务。在此证明，通过与单原子Fe–N 4位点偶联，可以显着提高固有碳缺陷的活性。生成的催化剂在0.1 m KHCO 3中提供90％的最大CO法拉第效率和33 mA cm -2的CO分流密度。浓缩电解液中的显着增强得以保持，使可充电Zn-CO 2电池具有较高的5 mA cm -2时的CO选择性为86.5％。进一步的分析表明，固有缺陷是CO 2 RR的活性位点，而不是Fe–N 4中心。密度泛函理论计算表明，Fe–N 4耦合的固有缺陷对CO 2 RR的能垒降低，并抑制了析氢活性。高固有活性，再加上快速的电子转移能力和丰富的暴露活性位点，可诱导出色的电催化性能。
更新日期：2021-01-04
中文翻译：
Fe-N4单点碳平面中固有缺陷驱动的二氧化碳的电还原
操纵金属-氮-碳催化剂的面内缺陷来调节CO 2（CO 2 RR）的电还原反应仍然是一项艰巨的任务。在此证明，通过与单原子Fe–N 4位点偶联，可以显着提高固有碳缺陷的活性。生成的催化剂在0.1 m KHCO 3中提供90％的最大CO法拉第效率和33 mA cm -2的CO分流密度。浓缩电解液中的显着增强得以保持，使可充电Zn-CO 2电池具有较高的5 mA cm -2时的CO选择性为86.5％。进一步的分析表明，固有缺陷是CO 2 RR的活性位点，而不是Fe–N 4中心。密度泛函理论计算表明，Fe–N 4耦合的固有缺陷对CO 2 RR的能垒降低，并抑制了析氢活性。高固有活性，再加上快速的电子转移能力和丰富的暴露活性位点，可诱导出色的电催化性能。
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