单原子铁锚定富石墨氮多孔碳氧还原电催化剂及锌-空气电池
Single Atomic Fe anchored Porous Carbon with Rich Graphitic Nitrogen as Electrocatalysts for Oxygen Reduction Reaction and Zn-Air Batteries
摘要：
锌空气电池（ZAB）因其高的理论能量密度而成为新一代的储能装置，其性能依赖于阴极催化剂的氧还原反应（ORR）性能。单原子铁锚定氮掺杂碳（Fe-N-C）由于最大限度地利用了铁原子而成为一种很有前途的ORR电催化剂。然而，获得高速率和稳定的Fe-N-C仍然具有挑战性。提出了一种制备Fe-N-C催化剂（PC-Fe-50）的新方法，该催化剂的氧还原性能优于商业铂催化剂和酞菁铁（FePc）。当与商品OER催化剂（RuO 2）混合用作ZAB的空气阴极时，获得了809 W h kg-1的高能量密度和128 mW cm-2的高功率密度，以及稳定的循环充电性能。通过密度泛函理论计算，我们发现碳中大量的N掺杂（7.47at%）对具有两种最常见构型（FeN 4C 10，记为D1; FeN 4C 12，记为D2）的FeNx结构起着重要作用.调整了ORR中间体在Fe中心上的结合能。通过比较可能的结构和FePc分子的活性，我们发现PC-Fe-50催化剂中真正的活性中心可能是相邻N原子结合的D2，而不是文献报道的Fe-N-C催化剂中广泛认可的活性结构D1。
英文摘要：
Zn-air battery (ZAB) has distinguished itself as new generation of energy storage device due to the high theoretical energy density and its performance relies on the oxygen reduction reaction (ORR) performance of the cathode catalysts. Single atomic Fe anchored N-doped carbon (Fe-N-C) has emerged as a promising ORR electrocatalyst because of the maximum utilization of Fe atoms. However, to obtain high-rate and stable Fe-N-C remains challenging. A novel and facile approach to fabricate Fe-N-C catalyst (PC-Fe-50) with outstanding ORR performance superior to commercial platinum catalyst and iron phthalocyanine (FePc), is proposed here. When mixed with commercial OER catalyst (RuO2) and employed as the air cathode in ZAB, a high energy density of 809 W h kg-1, high power density of 128 mW cm-2, and stable cycling rechargeable performance are obtained. By means of density functional theory calculations, we revealed that the abundant N dopants (7.47 at%) in carbon play significant roles on FeNx moieties with two most common configurations (FeN4C10, denoted as D1; FeN4C12, denoted as D2). The binding energies of ORR intermediates on Fe center are adjusted. By comparing the activity of possible structures and FePc molecule, we find the realistic active sites in PC-Fe-50 catalyst may be the D2 combining the adjacent N atoms, instead of D1, the widely recognized active structure in reported Fe-N-C catalysts.
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