铁钴基催化剂的构筑及其在锌-空气电池中的应用

    锌-空气电池（Zinc-air batteries, ZABs）因具有出色的理论容量，较高的安全性以及廉价的工艺成本等优势，在新一代的能源储存领域受到了较大的关注。然而，ZABs 的输出功率受限于氧还原反应（Oxygen Reduction Reaction, ORR ） 速率， 其快速充电能力则取决于析氧反应（ Oxygen Evolution Reaction, OER）活性，因此，制备一种高效、稳定的双功能催化剂是ZABs 广泛应用的关键。为了满足高功率密度和快速充电ZABs 的需求，本研究从活性位点设计和催化剂载体构筑两个方面出发，利用理论计算及原位拉曼测试，深入地研究了铁钴基催化剂的反应机理，确定了ORR 和OER 的活性位点；同时，通过碳载体的优化，成功地将两种高效的催化活性位点整合到一种催化剂中，制备出性能卓越且稳定的铁钴基双功能催化剂，实现了高功率密度和快速充电ZABs 的应用。论文的主要研究内容和结果如下：
    在生物质玉米须多孔碳载体上，我们精确调控催化剂从铁纳米颗粒到铁单原子，用于提高ORR 和OER 性能。其中，分级多孔结构和中空管状形貌具有暴露更多活性位点、提高电子传输速率和促进反应物质传递的优势，是ORR 和OER 活性提升的关键因素。而且，铁单原子的高负载量（4.3 wt.%）和超高的N掺杂量（10 wt.%）也可以弥补传统Fe-N-C 催化剂在OER 方面性能的不足，从而增强本征的OER 性能。将制备的催化剂组装为柔性ZABs 的空气电极时，其表现出101 mW cm^-2 的高峰值功率密度，放电-充电的电压差为0.73 V，循环寿命超过44 小时，展现出巨大的潜力。通过简单的水热法，成功地在碳布上合成了碳酸钴（CoCO3）和氢氧氧铁（FeOOH）复合催化剂（CoCO₃@FeOOH/CC）。通过原位电化学活化的方法，使CoFe₂O₄/CoFeOOH 催化剂（R-CoCO₃@FeOOH/CC）在OER 电流密度为50 和500 mA cm^-2 时的过电位显著降低，分别为190 和238 mV。通过原位拉曼光谱分析和显微镜观察，高性能的OER 活性位点为CoOOH和FeOOH。基于R-CoCO3@FeOOH/CC 较高的OER 性能，其自支撑的ZABs在5 mA cm^-2 持续运行下的电压仅为1.74 V。这些发现为高性能的铁钴基OER 催化剂的设计和应用提供了宝贵的参考。
    最终，我们构建了准超疏水催化剂，其中CoFe 纳米颗粒（CoFe NP）和CoFe 单原子（CoFe SA）分别负载在沸石咪唑酯骨架（ZIF）衍生碳和中空碳管上（CoFe NP@SA）。其中，CoFe SA 对ORR 具有很高的活性，同时原位拉曼光谱也证明了CoFe NP 通过电化学重构过程转变为CoOOH 和FeOOH，提升了OER 活性。此外，催化剂的疏水-亲空气表面可以排斥水分子，以创建丰富的固-液-气三相反应界面，并暴露活性位点，从而促进反应分子/离子在界面之间的扩散和氧气吸附。因此，CoFe NP@SA 催化剂表现出极低的ORR/OER 电位差为0.6 V。当其组装为ZABs 时，在50 mA cm^-2的高电流密度下，展示出2.09 V 的低电位差，并且在1200 小时内具有良好的稳定性。这一方法为实现高功率密度和快速充电的ZABs 铺平了道路。

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