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Electron Delocalization of Au Nanoclusters Triggered by Fe Single Atoms Boosts Alkaline Overall Water Splitting
ACS Applied Materials & Interfaces ( IF 9.5 ) Pub Date : 2023-02-15 , DOI: 10.1021/acsami.2c21390
Yuanqing Sun 1 , Jiaqing Luo 1 , Manxue Zhang 1 , Jun Li 2 , Jingkun Yu 3 , Siyu Lu 3 , Weiyu Song 1 , Yuechang Wei 1 , Zhenxing Li 1 , Jian Liu 1, 4
Affiliation  

The rational design and in-depth understanding of the structure–activity relationship (SAR) of hydrogen and oxygen evolution reaction (HER and OER) bifunctional electrocatalysts are vital to decreasing the energy consumption of hydrogen production by electrochemical water splitting. Herein, we report an inducing electron delocalization method where Fe single atoms as inducers are used to regulate the electron structure of Au nanoclusters by the M–Nx–C substrate to acquire satisfactory intrinsic HER activity. Meanwhile, Fe single atoms also serve as efficient OER active sites to construct bifunctional electrocatalysts. On account of the strong synergistic effect between Au nanoclusters and Fe single atoms, the hybrid catalyst Au-Fe1NC/NF performs an outstanding alkaline HER and OER activity. Only 35.6 mV, 246 mV, and 1.52 V are needed to reach 10 mA cm–2 for alkaline HER, OER, and two-electrode electrolytic cells, respectively. In addition, the bifunctional electrocatalysts also display excellent electrochemical stability. DFT calculations demonstrate that the strong synergistic effect can enhance the O–H bond activation ability of Au nanoclusters and upshift the d-band center of the Fe single atom to promote alkaline electrocatalytic water splitting. The strong synergistic effect is proven to arise from the electron delocalization of Au nanoclusters triggered by Fe single atoms.

中文翻译:

由 Fe 单原子触发的 Au 纳米团簇的电子离域促进碱性整体水分解

合理设计和深入了解析氢反应(HER 和 OER)双功能电催化剂的构效关系(SAR)对于降低电化学水分解制氢的能耗至关重要。在此,我们报告了一种诱导电子离域方法,其中使用 Fe 单原子作为诱导剂,通过 M–N x –C底物调节 Au 纳米团簇的电子结构,以获得令人满意的固有 HER 活性。同时,Fe单原子也可作为高效的OER活性位点构建双功能电催化剂。由于Au纳米团簇与Fe单原子之间的强协同作用,杂化催化剂Au-Fe 1NC/NF 具有出色的碱性 HER 和 OER 活性。对于碱性 HER、OER 和双电极电解电池,分别仅需要 35.6 mV、246 mV 和 1.52 V 即可达到 10 mA cm –2 。此外,双功能电催化剂还表现出优异的电化学稳定性。DFT计算表明,强协同效应可以增强Au纳米团簇的O-H键活化能力,并使Fe单原子的d带中心上移,从而促进碱性电催化水分解。强大的协同效应被证明是由铁单原子触发的金纳米团簇的电子离域引起的。
更新日期:2023-02-15
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