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Nano Research

Article Title

Phase boundary engineering of metal-organic-framework-derived carbonaceous nickel selenides for sodium-ion batteries

Authors

Shiyao Lu, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China Department of Chemistry, City University of Hong Kong, Hong Kong 999077, Hong Kong, China
Hu Wu, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China
Jingwei Hou, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK School of Chemical Engineering, University of Queensland, St Lucia, QLD 4072, Australia
Limin Liu, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China
Jiao Li, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China
Chris J. Harris, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK
Cheng-Yen Lao, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK
Yuzheng Guo, School of Electrical Engineering and Automation, Wuhan University, Wuhan 430072, China
Kai Xi, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK Cambridge Graphene Centre, Department of Engineering, University of Cambridge, Cambridge CB3 0FA, UK
Shujiang Ding, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China
Guoxin Gao, Xi’an Key Laboratory of Sustainable Energy Materials Chemistry, MOE Key Laboratory for Nonequilibrium Synthesis and Modulation of Condensed Matter, State Key Laboratory of Electrical Insulation and Power Equipment, School of Chemistry, Xi’an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power, Xi’an Jiaotong University, Xi’an 710049, China
Anthony K. Cheetham, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK Materials Research Laboratory, University of California, Santa Barbara, CA 93106, USA
R. Vasant Kumar, Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK

Keywords

metal organic frameworks, phase boundary, carbon nanotube, metal selenides, sodium ion batteries

Abstract

Sodium-ion batteries (SIBs) are promising power sources due to the low cost and abundance of battery-grade sodium resources, while practical SIBs suffer from intrinsically sluggish diffusion kinetics and severe volume changes of electrode materials. Metalorganic framework (MOFs) derived carbonaceous metal compound offer promising applications in electrode materials due to their tailorable composition, nanostructure, chemical and physical properties. Here, we fabricated hierarchical MOF-derived carbonaceous nickel selenides with bi-phase composition for enhanced sodium storage capability. As MOF formation time increases, the pyrolyzed and selenized products gradually transform from a single-phase Ni3Se4 into bi-phase NiSex then single-phase NiSe2, with concomitant morphological evolution from solid spheres into hierarchical urchin-like yolk-shell structures. As SIBs anodes, bi-phase NiSex@C/CNT-10h (10 h of hydrothermal synthesis time) exhibits a high specific capacity of 387.1 mAh/g at 0.1 A/g, long cycling stability of 306.3 mAh/g at a moderately high current density of 1 A/g after 2,000 cycles. Computational simulation further proves the lattice mismatch at the phase boundary facilitates more interstitial space for sodium storage. Our understanding of the phase boundary engineering of transformed MOFs and their morphological evolution is conducive to fabricate novel composites/hybrids for applications in batteries, catalysis, sensors, and environmental remediation.

Graphical Abstract

Publisher

Tsinghua University Press

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