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D-Band Center Optimization of Edge-Rich Ultrathin RuZn Nanosheets With Moiré Superlattices for pH-Universal Hydrogen Evolution Reaction
Small ( IF 13.0 ) Pub Date : 2023-06-06 , DOI: 10.1002/smll.202303440
Rui Yu 1 , Xi Cao 1 , Qingqing Chen 1 , Wenjiang Li 1 , Aijian Huang 2, 3 , Xianwen Wei 1, 4 , Junjie Mao 1
Affiliation  

Electrocatalytic hydrogen evolution reaction (HER) is a promising way to produce pure and clean hydrogen. However, the preparation of efficient and economical catalysts for pH-universal HER remains a challenging but rewarding task. Herein, ultrathin RuZn nanosheets (NSs) with moiré superlattices and abundant edges are synthesized. The RuZn NSs with unique structure exhibit superb HER performance with overpotentials of 11, 13, and 29 mV to achieve 10 mA cm−2 in 1 M KOH, 1 M PBS, and 0.5 M H2SO4, respectively, which is substantially lower than those of Ru NSs and RuZn NSs without moiré superlattices. Density functional theory investigations reveal that the charge transfer from Zn to Ru will lead the appropriate downshift of the d-band center of surface Ru atoms, thus accelerating hydrogen desorption from the Ru sites, lowering the dissociation energy barrier of water and greatly improving the HER performance. This work provides an effective design scheme for high-performance HER electrocatalysts over a wide pH range, and propose a general route to prepare Ru-based bimetallic nanosheets with moiré superlattices.

中文翻译:

具有莫尔超晶格的富边缘超薄 RuZn 纳米片的 D 波段中心优化,用于 pH 通用析氢反应

电催化析氢反应(HER)是生产纯净氢气的一种有前景的方法。然而,制备高效且经济的 pH 通用 HER 催化剂仍然是一项具有挑战性但有益的任务。在此,合成了具有莫尔超晶格和丰富边缘的超薄 RuZn 纳米片(NS)。具有独特结构的RuZn NSs表现出优异的HER性能,过电势分别为11、13和29 mV,在1 M KOH、1 M PBS和0.5 MH 2 SO 4中分别达到10 mA cm -2,远低于没有莫尔超晶格的 Ru NS 和 RuZn NS 的结果。密度泛函理论研究表明,从Zn到Ru的电荷转移会导致表面Ru原子的d带中心适当下移,从而加速氢从Ru位点的解吸,降低了水的解离能垒,大大提高了HER表现。这项工作为宽pH范围内的高性能HER电催化剂提供了有效的设计方案,并提出了制备具有莫尔超晶格的Ru基双金属纳米片的一般路线。
更新日期:2023-06-06
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