Unveiling the Aluminum Doping Effects of In‐Situ Transmogrified Dual‐LDH Heterostructure and Its Fermi‐Level Alignment to Water Splitting Potentials

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Nandapriya Manivelan, Junji Piao, Jaekook Kim, Seunghwa Lee, Youngji Kim, Vaiyapuri Soundharrajan, Min‐Kyu Son, Amir Humayun, Masoud Darvish Ganji, Hyunseok Ko, Kandasamy Prabakar
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引用次数: 0

Abstract

The layered double hydroxide (LDH) captivates the starlight of electrochemical water‐splitting applications due to its stacked layers and larger surface area. A novel approach is reported to integrate CoFe‐LDH/NiAl‐LDH heterostructure through a single‐step in situ transmogrification, harnessing the benefits of LDH. The in situ Raman spectroscopy reveals that aluminum (Al) doping promotes the formation of high‐valent CoIII/IV‐O active species concentration in LDH, whereas without Al dopants, the catalyst predominantly exhibit NiII/III‐O species and underperform the catalytic activity. The projected density of states is very close to the Fermi level positions in Al‐doped samples which significantly enhance the electron transfer processes. The Mott–Schottky studies confirm that both Al40 CoFe30 and Al60 CoFe20 catalysts are p‐type semiconductors, exhibiting a distinct redox behaviors under applied bias. At positive bias, Al60 CoFe20 undergoes downward band bending (accumulation), and align the Fermi‐level near the water oxidation potential, which promotes the oxygen evolution reaction (OER). The negative bias causes upward band bending (deep depletion) in the Al40 CoFe30, and shifts the Fermi‐level near the water reduction potential, and hence facilitates hydrogen evolution reaction (HER). Overall, this study highlights the importance of manipulating Fermi‐level alignment in LDH catalysts through strategic metal doping to achieve targeted water‐splitting reactions.
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来源期刊
Advanced Energy Materials
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.
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