Journal
ACS NANO
Volume 15, Issue 5, Pages 8306-8318Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c09217
Keywords
lattice engineering; layered double hydroxide nanosheet; defect structure; stacking number; energy functionality
Categories
Funding
- National Research Foundation of Korea (NRF) - Korea government (MSIP) [NRF-2020R1A2C3008671]
- Korea government (MSIT) [NRF-2017R1A5A1015365]
- Technology Innovation Program - Alchemist Project - Ministry of Trade, Industry & Energy (MOTIE, Korea) [20012315]
- MOST
- POSTECH
- Korea Evaluation Institute of Industrial Technology (KEIT) [20012315] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [4199990514159, 4199990213848] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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By adjusting the elastic deformation and chemical interactions of nanosheets, the defect structure and porosity of layered double hydroxides can be effectively controlled to enhance material performance. Nanohybrids with a small stacking number and rich in defects exhibit excellent performance as oxygen evolution electrocatalysts and supercapacitor electrodes with high specific capacitance.
An effective lattice engineering method to simultaneously control the defect structure and the porosity of layered double hydroxides (LDHs) was developed by adjusting the elastic deformation and chemical interactions of the nanosheets during the restocking process. The enlargement of the intercalant size and the lowering of the charge density were effective in increasing the content of oxygen vacancies and enhancing the porosity of the stacked nanosheets via layer thinning. The defect-rich Co-Al-LDH-NO3- nanohybrid with a small stacking number exhibited excellent performance as an oxygen evolution electrocatalyst and supercapacitor electrode with a large specific capacitance of similar to 2230 F g(-1) at 1 A g(-1), which is the largest capacitance of carbon-free LDH-based electrodes reported to date. Combined with the results of density functional theory calculations, the observed excellent correlations between the overpotential/capacitance and the defect content/stacking number highlight the importance of defect/stacking structures in optimizing the energy functionalities. This was attributed to enhanced orbital interactions with water/hydroxide at an increased number of defect sites. The present cost-effective lattice engineering process can therefore provide an economically feasible methodology to explore high-performance electrocatalyst/electrode materials.
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