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Single-Crystal Nitrogen-Rich Two-Dimensional Mo5N6 Nanosheets for Efficient and Stable Seawater Splitting
ACS Nano ( IF 17.1 ) Pub Date : 2018-11-29 00:00:00 , DOI: 10.1021/acsnano.8b07841
Huanyu Jin 1 , Xin Liu 1 , Anthony Vasileff 1 , Yan Jiao 1 , Yongqiang Zhao 1 , Yao Zheng 1 , Shi-Zhang Qiao 1
Affiliation  

Transition metal nitrides (TMNs) have great potential for energy-related electrocatalysis because of their inherent electronic properties. However, incorporating nitrogen into a transition metal lattice is thermodynamically unfavorable, and therefore most of the developed TMNs are deficient in nitrogen. Consequently, these TMNs exhibit poor structural stability and unsatisfactory performance for electrocatalytic applications. In this work, we design and synthesize an atomically thin nitrogen-rich nanosheets, Mo5N6, with the help of a Ni-inducing growth method. The as-prepared single-crystal electrocatalyst with abundant metal–nitrogen electroactive sites displays outstanding activity for the hydrogen evolution reaction (HER) in a wide range of electrolytes (pH 0–14). Further, the two-dimensional Mo5N6 nanosheets exhibit high HER activity and stability in natural seawater that are superior to other TMNs and even the Pt benchmark. By combining synchrotron-based spectroscopy and the calculations of electron density of state, we find that the enhanced properties of these nitrogen-rich Mo5N6 nanosheets originates from its Pt-like electronic structure and the high valence state of its Mo atoms.

中文翻译:

单晶富氮二维Mo 5 N 6纳米片,用于高效稳定地分离海水

过渡金属氮化物(TMN)由于其固有的电子特性,在与能源有关的电催化方面具有巨大潜力。然而,将氮掺入过渡金属晶格在热力学上是不利的,因此大多数已开发的TMN缺乏氮。因此,这些TMN在电催化应用中显示出差的结构稳定性和不令人满意的性能。在这项工作中,我们设计并合成了原子薄的富氮纳米片Mo 5 N 6,借助诱导镍的生长方法。所制备的具有丰富的金属-氮电活性位的单晶电催化剂在各种电解质(pH值为0-14)中对氢释放反应(HER)表现出出色的活性。此外,二维Mo 5 N 6纳米片在天然海水中显示出较高的HER活性和稳定性,优于其他TMN甚至Pt基准。通过基于同步加速器的光谱学和电子态密度的计算,我们发现这些富氮的Mo 5 N 6纳米片的增强性能源自其Pt状电子结构和Mo原子的高价态。
更新日期:2018-11-29
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