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Lattice Engineering to Simultaneously Control the Defect/Stacking Structures of Layered Double Hydroxide Nanosheets to Optimize Their Energy Functionalities
ACS Nano ( IF 15.8 ) Pub Date : 2021-04-16 , DOI: 10.1021/acsnano.0c09217 Najin Kim 1 , Tae-Ha Gu 1 , Dongyup Shin 2 , Xiaoyan Jin 3 , Hyeyoung Shin 4 , Min Gyu Kim 5 , Hyungjun Kim 2 , Seong-Ju Hwang 3
ACS Nano ( IF 15.8 ) Pub Date : 2021-04-16 , DOI: 10.1021/acsnano.0c09217 Najin Kim 1 , Tae-Ha Gu 1 , Dongyup Shin 2 , Xiaoyan Jin 3 , Hyeyoung Shin 4 , Min Gyu Kim 5 , Hyungjun Kim 2 , Seong-Ju Hwang 3
Affiliation
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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 restacking 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 ∼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.
中文翻译：
同时控制层状双氢氧化物纳米片的缺陷/堆积结构以优化其能量功能的晶格工程
通过调整纳米片在重新堆叠过程中的弹性变形和化学相互作用，开发了一种有效的晶格工程方法，可同时控制层状双氢氧化物（LDHs）的缺陷结构和孔隙率。嵌入剂尺寸的增加和电荷密度的降低有效地增加了氧空位的含量并通过层薄化提高了堆叠纳米片的孔隙率。富缺陷Co-Al系-LDH-NO 3 -纳米杂化物具有小的层叠数显示出优异的性能如析氧电和超级电容器电极用的~2230 F G大的比电容-1 1 A G -1，这是迄今为止报道的无碳LDH基电极的最大电容。结合密度泛函理论计算的结果，观察到的过电势/电容与缺陷含量/堆积数之间的极好的相关性突出了缺陷/堆积结构在优化能量功能方面的重要性。这归因于缺陷位置数量增加时与水/氢氧化物的轨道相互作用增强。因此，当前具有成本效益的晶格工程方法可以提供一种经济可行的方法来研究高性能的电催化剂/电极材料。
更新日期：2021-05-25
中文翻译：
同时控制层状双氢氧化物纳米片的缺陷/堆积结构以优化其能量功能的晶格工程
通过调整纳米片在重新堆叠过程中的弹性变形和化学相互作用，开发了一种有效的晶格工程方法，可同时控制层状双氢氧化物（LDHs）的缺陷结构和孔隙率。嵌入剂尺寸的增加和电荷密度的降低有效地增加了氧空位的含量并通过层薄化提高了堆叠纳米片的孔隙率。富缺陷Co-Al系-LDH-NO 3 -纳米杂化物具有小的层叠数显示出优异的性能如析氧电和超级电容器电极用的~2230 F G大的比电容-1 1 A G -1，这是迄今为止报道的无碳LDH基电极的最大电容。结合密度泛函理论计算的结果，观察到的过电势/电容与缺陷含量/堆积数之间的极好的相关性突出了缺陷/堆积结构在优化能量功能方面的重要性。这归因于缺陷位置数量增加时与水/氢氧化物的轨道相互作用增强。因此，当前具有成本效益的晶格工程方法可以提供一种经济可行的方法来研究高性能的电催化剂/电极材料。
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