Defect-Rich Ni3FeN Nanocrystals Anchored on N-Doped Graphene for Enhanced Electrocatalytic Oxygen Evolution
Defect-Rich Ni3FeN Nanocrystals Anchored on N-Doped Graphene for Enhanced Electrocatalytic Oxygen Evolution
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锚定在氮掺杂石墨烯上的富含缺陷的 Ni3FeN 纳米晶体用于增强电催化析氧
DOI：
10.1002/adfm.201706018
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发表时间：
2018
影响因子：
19
通讯作者：
Bao Jianchun
中科院分区：
文献类型：
--
作者：
Zhao Shulin;Li Meng;Han Min;Xu Dongdong;Yang Jing;Lin Yue;Shi Nai En;Lu Yanan;Yang Rui;Liu Bitao;Dai Zhihui;Bao Jianchun
金属氮化物纳米结构由于其独特的光学、电学和催化性能，在光电子、清洁能源和催化领域有着广泛的应用。尽管已经取得了很大的进展，合成的缺陷丰富（DR）的氮化镓纳米晶体或相关的纳米杂化物仍然是一个挑战，其电催化析氧反应（OER）的应用还没有得到充分的研究。本文中，通过控制退火气氛，通过NiFe层状双氢氧化物/氧化石墨烯前体的程序升温退火和氮化处理来制备DR-Ni 3FeN纳米晶体和N掺杂石墨烯（N-G）纳米杂化物（DR-Ni 3FeN/N-G）。在纳米杂化材料中，DR-Ni 3FeN纳米晶锚定在N-G上，除了约10%的层错外，主要表现为孪晶缺陷。这种纳米杂化物可以有效地催化OER在碱性介质中具有小的过电位（0.25 V），以达到10 mA cm-2的电流密度和高的周转频率（0.46 s-1），上级他们的同行（几乎无缺陷的Ni 3FeN/N-G），商业IrO 2，和国家的最先进的OER催化剂报道。除了上级活性外，它们还表现出比它们的同行更好的耐久性。微观结构、光谱和电化学分析表明，DR-Ni 3FeN/ N-G纳米杂化材料的OER性能的提高主要源于Ni 3FeN活性相中丰富的孪晶缺陷以及DR-Ni 3FeN与N-G之间的强相互作用。
Owing to their unique optical, electronic and catalytic properties, metal nitrides nanostructures are widely used in optoelectronics, clean energy, and catalysis fields. Despite great progress has been achieved, synthesis of defect-rich (DR) bimetallic nitride nanocrystals or related nanohybrids remains a challenge, and their electrocatalytic application for oxygen evolution reaction (OER) has not been fully studied. Herein, the DR-Ni3FeN nanocrystals and N-doped graphene (N-G) nanohybrids (DR-Ni3FeN/N-G) are fabricated through temperature-programmed annealing and nitridation treatment of NiFe-layered double hydroxides/graphene oxide precursors by controlling annealing atmosphere. In the nanohybrids, the DR-Ni3FeN nanocrystals are anchored on N-G, and mainly show twin crystal defects besides ~10% of stacking faults. Such nanohybrids can efficiently catalyze OER in alkaline media with a small overpotential (0.25 V) to attain the current density of 10 mA cm-2 and a high turnover frequency (0.46 s-1), superior to their counterparts (the nearly defect-free Ni3FeN/N-G), commercial IrO2, and the-state-of-art reported OER catalysts. Except for the superior activity, they show better durability than their counterparts yet. As revealed by microstructural, spectroscopic and electrochemical analyses, the enhanced OER performance of DR-Ni3FeN/ N-G nanohybrids originates from the abundant twin crystal defects in Ni3FeN active phase and the strong interplay between DR-Ni3FeN and N-G.