气候变化领域集成服务门户(CCPortal): Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides

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DOI	10.1039/d0ee03701j
	Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides
	Zhuang Z.; Li Y.; Li Y.; Huang J.; Wei B.; Sun R.; Ren Y.; Ding J.; Zhu J.; Lang Z.; Moskaleva L.V.; He C.; Wang Y.; Wang Z.; Wang D.; Li Y.
发表日期	2021
ISSN	17545692
起始页码	1016
结束页码	1028
卷号	14 期号:2
英文摘要	Complexity in strongly correlated oxides such as perovskite strictly dominates their performance for oxygen reduction reaction (ORR). Precise control of the physical correlations among spin, charge, orbital, and lattice degrees of freedom in these oxides can exercise considerable enhancement of ORR activity, but has until now remained elusive. Here, we show that nonmagnetic hexavalent molybdenum (Mo6+) atomically dispersed within oxide lattice steers the intrinsic activity of catalytically active sites by entrapping extrinsic electrons at their 3d orbitals, without the occurrence of lattice symmetry breaking and magnetic perturbation. With double perovskite La2Co2+Mn4+O6 as a model catalyst, the atomic-scale electron trap generates additional high-spin, catalytically active Mn3+(t32ge1g) sites and highly conductive Co2+(e2g)-O-Mn3+(e1g) double exchange channels, leading to five-fold improvement in ORR activity. First-principles calculations reveal a substantial increase of the spin density on Mn sites caused by electron trapping, and unambiguously confirm a more exothermic reaction pathway as well as a lower barrier of the rate-limiting surface hydroxide regeneration on Mo1/La2CoMnO6. We can also extend this strategy with atomic precision easily to other four oxide catalysts and achieve large enhancement in their ORR activities as anticipated, indicating its broad utility. This work embodies the theories of condensed matter physics in rational design of ORR catalysts, and may inspire further development of the control of electron correlation in strongly correlated electron systems. © The Royal Society of Chemistry.
英文关键词	Calculations; Catalysts; Crystal lattices; Degrees of freedom (mechanics); Electrolytic reduction; Electron traps; Oxygen reduction reaction; Perovskite; Double perovskites; Electron trapping; First-principles calculation; Intrinsic activities; Magnetic perturbation; Perovskite oxides; Strongly correlated electron system; Surface hydroxide; Electrons; asymmetry; correlation; detection method; electron; molybdenum; oxidation; perovskite; reduction; symmetry
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190775
作者单位	Department of Chemistry, Tsinghua University, Beijing, China; Inst. of Appl. and Phys. Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, Bremen, Germany; College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, China; State Key Laboratory of Material Processing and Die and Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, China; International Iberian Nanotechnology Laboratory (INL), Braga, Portugal; State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China; State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, China; Center for Marine Materials Corrosion and Protection, College of Materials, Xiamen University, Xiamen, China; Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Phy...
推荐引用方式 GB/T 7714	Zhuang Z.,Li Y.,Li Y.,et al. Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides[J],2021,14(2).
APA	Zhuang Z..,Li Y..,Li Y..,Huang J..,Wei B..,...&Li Y..(2021).Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides.Energy & Environmental Science,14(2).
MLA	Zhuang Z.,et al."Atomically dispersed nonmagnetic electron traps improve oxygen reduction activity of perovskite oxides".Energy & Environmental Science 14.2(2021).