A Self-Assembled Hetero-Structured Inverse-Spinel and Anti-Perovskite Nanocomposite for Ultrafast Water Oxidation.
A Self-Assembled Hetero-Structured Inverse-Spinel and Anti-Perovskite Nanocomposite for Ultrafast Water Oxidation.
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DOI：
10.1002/smll.202002089
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发表时间：
2020-06
期刊：
影响因子：
13.3
通讯作者：
Nana Ma;Gao Chen;Yanping Zhu;Hainan Sun;J. Dai;Hang Chu;R. Ran;Wei Zhou;R. Cai;Zongping Sh
中科院分区：
文献类型：
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作者：
Nana Ma;Gao Chen;Yanping Zhu;Hainan Sun;J. Dai;Hang Chu;R. Ran;Wei Zhou;R. Cai;Zongping Sh
尖晶石和钙钛矿具有独特的晶体结构，是电催化中最受欢迎的两种材料家族，然而，它们通常表现出较差的导电性，对电化学反应过程中的电荷转移过程产生负面影响。本文报道了一种高导电性的反尖晶石（Fe3 O4）和反钙钛矿（Ni3 FeN）异质结构纳米复合材料作为一种上级析氧电催化剂，其可以基于一锅法合成策略容易地制备。由于Ni/Fe 3d和N 2 p轨道间的强杂化，在析氧反应（OER）过程中，Ni 3 FeN3很容易转变为真实的活性物种NiFe（oxyOH），而Fe 3 O4组分具有较低的O-p带中心，结构稳定。结果，达到了高的表面反应性和体电子传输能力。通过在独立的碳纤维纸上直接生长Fe3 O4/Ni3 FeN异质结构并基于三电极配置进行测试，仅需要160 mV的过电位即可提供30 mA cm-2的OER电流密度。此外，在100小时的延长试验期内观察到可忽略的性能衰减。这一工作为合理设计新型电催化异质结构材料提供了理论依据。
Spinel and perovskite with distinctive crystal structures are two of the most popular material families in electrocatalysis, which, however, usually show poor conductivity, causing a negative effect on the charge transfer process during electrochemical reactions. Herein, a highly conductive inverse spinel (Fe3 O4 ) and anti-perovskite (Ni3 FeN) hetero-structured nanocomposite is reported as a superior oxygen evolution electrocatalyst, which can be facilely prepared based on a one-pot synthesis strategy. Thanks to the strong hybridization between Ni/Fe 3d and N 2p orbitals, the Ni3 FeN is easily transformed into NiFe (oxy)hydroxide as the real active species during the oxygen evolution reaction (OER) process, while the Fe3 O4 component with low O-p band center relative to Fermi level is structurally stable. As a result, both high surface reactivity and bulk electronic transport ability are reached. By directly growing Fe3 O4 /Ni3 FeN heterostructure on freestanding carbon fiber paper and testing based on the three-electrode configuration, it requires only 160 mV overpotential to deliver a current density of 30 mA cm-2 for OER. Also, negligible performance decay is observed within a prolonged test period of 100 h. This work sheds light on the rational design of novel heterostructure materials for electrocatalysis.