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DOI	10.1073/pnas.2014086118
	Tailoring electrocatalytic activity of in situ crafted perovskite oxide nanocrystals via size and dopant control
	Harn Y.-W.; Liang S.; Liu S.; Yan Y.; Wang Z.; Jiang J.; Zhang J.; Li Q.; He Y.; Li Z.; Zhu L.; Cheng H.-P.; Lin Z.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:25
英文摘要	Perovskite oxides (ABO3) have been widely recognized as a class of promising noble-metal–free electrocatalysts due to their unique compositional flexibility and structural stability. Surprisingly, investigation into their size-dependent electrocatalytic properties, in particular barium titanate (BaTiO3), has been comparatively few and limited in scope. Herein, we report the scrutiny of size- and dopant-dependent oxygen reduction reaction (ORR) activities of an array of judiciously designed pristine BaTiO3 and doped BaTiO3 (i.e., La- and Co-doped) nanoparticles (NPs). Specifically, a robust nanoreactor strategy, based on amphiphilic star-like diblock copolymers, is employed to synthesize a set of hydrophobic polymer-ligated uniform BaTiO3 NPs of different sizes (≤20 nm) and controlled compositions. Quite intriguingly, the ORR activities are found to progressively decrease with the increasing size of BaTiO3 NPs. Notably, La- and Co-doped BaTiO3 NPs display markedly improved ORR performance over the pristine counterpart. This can be attributed to the reduced limiting barrier imposed by the formation of -OOH species during ORR due to enhanced adsorption energy of intermediates and the possibly increased conductivity as a result of change in the electronic states as revealed by our density functional theory–based first-principles calculations. Going beyond BaTiO3 NPs, a variety of other ABO3 NPs with tunable sizes and compositions may be readily accessible by exploiting our amphiphilic star-like diblock copolymer nanoreactor strategy. They could in turn provide a unique platform for both fundamental and practical studies on a suite of physical properties (dielectric, piezoelectric, electrostrictive, catalytic, etc.) contingent upon their dimensions and compositions. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Star-like diblock copolymer \| perovskite nanocrystals \| oxygen reduction reaction \| density functional theory
语种	英语
scopus关键词	copolymer; perovskite nanocrystal; adsorption; Article; catalysis; chemical composition; chemical structure; conductance; controlled study; density functional theory; energy conversion; hydrophobicity; particle size; reduction (chemistry); synthesis
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238514
作者单位	School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States; Department of Physics, University of Florida, Gainesville, FL 32611, United States; Quantum Theory Project, University of Florida, Gainesville, FL 32611, United States; Department of Macromolecular Science and Engineering, Case Western Reserve University, Cleveland, OH 44106, United States; Center for Molecular Magnetic Quantum Materials, University of Florida, Gainesville, FL 32611, United States
推荐引用方式 GB/T 7714	Harn Y.-W.,Liang S.,Liu S.,et al. Tailoring electrocatalytic activity of in situ crafted perovskite oxide nanocrystals via size and dopant control[J],2021,118(25).
APA	Harn Y.-W..,Liang S..,Liu S..,Yan Y..,Wang Z..,...&Lin Z..(2021).Tailoring electrocatalytic activity of in situ crafted perovskite oxide nanocrystals via size and dopant control.Proceedings of the National Academy of Sciences of the United States of America,118(25).
MLA	Harn Y.-W.,et al."Tailoring electrocatalytic activity of in situ crafted perovskite oxide nanocrystals via size and dopant control".Proceedings of the National Academy of Sciences of the United States of America 118.25(2021).