Crystalline‐Amorphous Interface‐Triggered Electron Redistribution on Copper(II) Sulfide@Metal (Ni, Co, and Fe) Oxyhydroxides for Ultra‐Efficient Overall Water/Seawater Splitting

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2024-12-02 DOI:10.1002/aenm.202403657

Peng Gu, Yidong Song, Yihe Fan, Xin Meng, Jin Liu, Guofeng Wang, Zhouguanwei Li, Heyuan Sun, Ziyu Zhao, Jinlong Zou

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引用次数: 0

Abstract

Rearranging the electronic orbitals of metal sites through interface engineering is the breakthrough for achieving high efficiencies in hydrogen/oxygen evolution reactions (HER/OER) on bimetallic catalysts. Here, via a multistep liquid‐phase synthesis strategy, the crystalline‐amorphous (c‐a) interface is built by coating amorphous oxyhydroxide layer on the surface of crystallized copper(II) sulfide (CuS@MOOH, M = iron (Fe), cobalt (Co) and nickel (Ni)) with an internal cavity. For HER, c‐a interface facilitates the electron filling of the 3d orbitals of Cu, thereby enhancing the coordination between Cu sites (Cu2+/Cu+) and *H and reducing the energy barrier for *H adsorption. For OER, c‐a interface triggers electronic rearrangement in the 3d orbitals of M sites, prompting electron transition from the t2g orbitals to the eg orbitals to achieve a half‐filled state, optimizing the oxygen‐intermediates adsorption on M sites (M3+/M4+). Among CuS@MOOH, the as‐marked CuS@CoOOH‐6 exhibits the best activities with ultra‐low overpotentials of 62 mV (HER) and 136 mV (OER). Only 1.52 V is sufficient to power the electrolyzer with CuS@CoOOH‐6‐based cathode/anode, maintaining a ultra‐stable efficiency (96.9 %) over 72 h. Notably, CuS@CoOOH‐6 also exhibits impressive activity/durability for natural seawater electrolysis. This study enhances understanding of the properties and electronic structure of the c‐a interface for water splitting.

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来源期刊

Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS

CiteScore

41.90

自引率

4.00%

发文量

889

审稿时长

1.4 months

期刊介绍： Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.