Coherent Sub-Nanometer Interface between Crystalline and Amorphous Materials Boosts Electrochemical Synthesis of Hydrogen Peroxide.
Coherent Sub-Nanometer Interface between Crystalline and Amorphous Materials Boosts Electrochemical Synthesis of Hydrogen Peroxide.
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DOI：
10.1002/smll.202302380
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发表时间：
2023-06
期刊：
影响因子：
13.3
通讯作者：
Zhikang Bao;Zihao Yao;Chongzhi Zhu;Yikuan Liu;Shijie Zhang;Jinyan Zhao;Lei Ding;Zaixiang Xu-Zaixiang
中科院分区：
文献类型：
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作者：
Zhikang Bao;Zihao Yao;Chongzhi Zhu;Yikuan Liu;Shijie Zhang;Jinyan Zhao;Lei Ding;Zaixiang Xu-Zaixiang
由成分、形状或晶体结构可能不同的不同类型的组件构成的界面上出现了大量但在很大程度上未被探索的奇异现象和特性。晶体和非晶态材料之间的相干界面可能引起的独特性质仍然知之甚少，也缺乏制造这种界面的一般策略。结果表明，通过局部氧化可以构建由共格注册的晶态和非晶态材料组成的异质结构。作为概念验证研究，由晶态P3N5生成非晶态P3N5Ox可以在不中断共格界面上共价键的情况下合成由晶态P3N5和非晶态P3N5Ox组成的异质结构。异质结构是由非晶态P3N5Ox基质包裹的纳米级短程有序的P3N5结构域决定的，它同时具有界面上的快速电荷转移和双组分的催化协同效应。这种P3N5/P3N5Ox异质结对*OOH中间体具有最佳的吸附能，在0.4VRHE下选择性为96.68%，在-0.3VRHE下的产率为321.5 mmolh-1gCatalyst-1，表现出良好的电催化性能。目前的研究为晶体和非晶态材料之间形成的亚纳米相干界面的合成策略、化学结构和催化性能提供了新的见解。
There are enormous yet largely underexplored exotic phenomena and properties emerging from interfaces constructed by diverse types of components that may differ in composition, shape, or crystal structure. It remains poorly understood the unique properties a coherent interface between crystalline and amorphous materials may evoke, and there lacks a general strategy to fabricate such interfaces. It is demonstrated that by topotactic partial oxidation heterostructures composed of coherently registered crystalline and amorphous materials can be constructed. As a proof-of-concept study, heterostructures consisting of crystalline P3 N5 and amorphous P3 N5 Ox can be synthesized by creating amorphous P3 N5 Ox from crystalline P3 N5 without interrupting the covalent bonding across the coherent interface. The heterostructure is dictated by nanometer-sized short-range-ordered P3 N5 domains enclosed by amorphous P3 N5 Ox matrix, which entails simultaneously fast charge transfer across the interface and bicomponent synergistic effect in catalysis. Such a P3 N5 /P3 N5 Ox heterostructure attains an optimal adsorption energy for *OOH intermediates and exhibits superior electrocatalytic performance toward H2 O2 production by adopting a selectivity of 96.68% at 0.4 VRHE and a production rate of 321.5 mmol h-1 gcatalyst -1 at -0.3 VRHE . The current study provides new insights into the synthetic strategy, chemical structure, and catalytic property of a sub-nanometer coherent interface formed between crystalline and amorphous materials.