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嵌入在镍钴层状双氢氧化物中的原子分散银原子促进析氧反应。

Atomically Dispersed Silver Atoms Embedded in NiCo Layer Double Hydroxide Boost Oxygen Evolution Reaction.

作者信息

He Wenjun, Zhang Rui, Liu Hui, Hao Qiuyan, Li Ying, Zheng Xuerong, Liu Caichi, Zhang Jun, Xin Huolin L

机构信息

Key Laboratory of Special Functional Materials for Ecological Environment and Information (Ministry of Education), Hebei University of Technology, Tianjin, 300130, China.

Department of Physics and Astronomy, University of California, Irvine, CA, 92697, USA.

出版信息

Small. 2023 Aug;19(34):e2301610. doi: 10.1002/smll.202301610. Epub 2023 Apr 24.

Abstract

Bimetallic layered double hydroxides (LDHs) are promising catalysts for anodic oxygen evolution reaction (OER) in alkaline media. Despite good stability, NiCo LDH displays an unsatisfactory OER activity relative to the most robust NiFe LDH and CoFe LDH. Herein, a novel NiCo LDH electrocatalyst modified with single-atom silver grown on carbon cloth (Ag -NiCo LDH/CC) that exhibits exceptional OER activity and stability in 1.0 m KOH is reported. The Ag -NiCo LDH/CC catalyst only requires a low overpotential of 192 mV to reach a current density of 10 mA cm , obviously boosting the OER activity of NiCo LDH/CC (410 mV@10 mA cm ). Inspiringly, Ag -NiCo LDH/CC can maintain its high activity for up to 500 h at a large current density of 100 mA cm , exceeding most single-atom OER catalysts. In situ Raman spectroscopy studies uncover that the in situ formed NiCoOOH during OER is the real active species. Hard X-ray absorption spectrum (XAS) and density functional theory (DFT) calculations validate that single-atom Ag occupying Ni site increases the chemical valence of Ni elements, and then weakens the adsorption of oxygen-contained intermediates on Ni sites, fundamentally accounting for the enhanced OER performance.

摘要

双金属层状双氢氧化物(LDHs)是碱性介质中阳极析氧反应(OER)很有前景的催化剂。尽管稳定性良好,但相对于最强大的NiFe LDH和CoFe LDH,NiCo LDH的OER活性并不理想。在此,报道了一种在碳布上生长有单原子银修饰的新型NiCo LDH电催化剂(Ag-NiCo LDH/CC),其在1.0 m KOH中表现出优异的OER活性和稳定性。Ag-NiCo LDH/CC催化剂仅需192 mV的低过电位就能达到10 mA cm的电流密度,明显提高了NiCo LDH/CC的OER活性(410 mV@10 mA cm)。令人鼓舞的是,Ag-NiCo LDH/CC在100 mA cm的大电流密度下可保持其高活性长达500小时,超过了大多数单原子OER催化剂。原位拉曼光谱研究发现,OER过程中原位形成的NiCoOOH是真正的活性物种。硬X射线吸收光谱(XAS)和密度泛函理论(DFT)计算证实,占据Ni位点的单原子Ag增加了Ni元素的化学价,进而减弱了含氧中间体在Ni位点上的吸附,从根本上解释了OER性能的增强。

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