High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb2Co2O7 with Large Cation Mixed Occupancy

Junye Yang; Jianhong Dai; Zhehong Liu; Runze Yu; Hajime Hojo; Zhiwei Hu; Tunwen Pi; Yunliang Soo; Changqing Jin; Masaki Azuma; Youwen Long

doi:10.1021/acs.inorgchem.7b01646

High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb₂Co₂O₇ with Large Cation Mixed Occupancy

Junye Yang, Jianhong Dai, Zhehong Liu, Runze Yu, Hajime Hojo, Zhiwei Hu, Tunwen Pi, Yunliang Soo, Changqing Jin, Masaki Azuma, Youwen Long

Research output: Contribution to journal › Article › peer-review

3 Citations (Scopus)

Abstract

The novel A₂B₂O₇-type compound Pb₂Co₂O₇ was synthesized at 8 GPa and 1673 K. Synchrotron X-ray diffraction shows a cubic pyrochlore structure with space group Fd3m. Rietveld structural analysis reveals a large cation mixed occupancy at both A and B sites by about 40%, the greatest value found in the pyrochlore family. In combination with the X-ray absorption spectroscopy results, the specific chemical composition and charge states are determined to be (Co_0.6Pb_0.4)³⁺₂(Pb_0.6Co_0.4)⁴⁺₂O₇, in which both the A-site Co³⁺ and the B-site Co⁴⁺ are low-spin. Due to the tetrahedral geometric frustration effects as well as the random Co⁴⁺ and Pb⁴⁺ distribution at the B site, spin glassy behavior is well observed following the conventional critical slowing down feature in Pb₂Co₂O₇.

Original language	English
Pages (from-to)	11676-11680
Number of pages	5
Journal	Inorganic chemistry
Volume	56
Issue number	19
DOIs	https://doi.org/10.1021/acs.inorgchem.7b01646
Publication status	Published - Oct 2 2017
Externally published	Yes

All Science Journal Classification (ASJC) codes

Physical and Theoretical Chemistry
Inorganic Chemistry

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10.1021/acs.inorgchem.7b01646

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High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb₂Co₂O₇ with Large Cation Mixed Occupancy. / Yang, Junye; Dai, Jianhong; Liu, Zhehong; Yu, Runze; Hojo, Hajime; Hu, Zhiwei; Pi, Tunwen; Soo, Yunliang; Jin, Changqing; Azuma, Masaki; Long, Youwen.

In: Inorganic chemistry, Vol. 56, No. 19, 02.10.2017, p. 11676-11680.

Research output: Contribution to journal › Article › peer-review

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title = "High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb2Co2O7 with Large Cation Mixed Occupancy",

abstract = "The novel A2B2O7-type compound Pb2Co2O7 was synthesized at 8 GPa and 1673 K. Synchrotron X-ray diffraction shows a cubic pyrochlore structure with space group Fd3m. Rietveld structural analysis reveals a large cation mixed occupancy at both A and B sites by about 40%, the greatest value found in the pyrochlore family. In combination with the X-ray absorption spectroscopy results, the specific chemical composition and charge states are determined to be (Co0.6Pb0.4)3+2(Pb0.6Co0.4)4+2O7, in which both the A-site Co3+ and the B-site Co4+ are low-spin. Due to the tetrahedral geometric frustration effects as well as the random Co4+ and Pb4+ distribution at the B site, spin glassy behavior is well observed following the conventional critical slowing down feature in Pb2Co2O7.",

author = "Junye Yang and Jianhong Dai and Zhehong Liu and Runze Yu and Hajime Hojo and Zhiwei Hu and Tunwen Pi and Yunliang Soo and Changqing Jin and Masaki Azuma and Youwen Long",

note = "Funding Information: The authors thank L. X. Li for structural determination and fruitful discussions. This work was supported by the 973 Project of the Ministry of Science and Technology of China (Grant No. 2014CB921500), the National Natural Science Foundation of China (Grant Nos. 11574378, 51772324, and 61404052), and the Chinese Academy of Sciences (Grant Nos. QYZDB-SSW-SLH013, XDB07030300, YZ201555, and GJHZ1773). M. Azuma was supported by Kanagawa Institute of Industrial Science and Technology. Y. Long was partially supported by World Research Hub Initiative, Institute of Innovative Research, Tokyo Institute of Technology and Collaborative Research Projects, Laboratory for Materials and Structures, Tokyo Institute of Technology. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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doi = "10.1021/acs.inorgchem.7b01646",

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T1 - High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb2Co2O7 with Large Cation Mixed Occupancy

AU - Yang, Junye

AU - Dai, Jianhong

AU - Liu, Zhehong

AU - Yu, Runze

AU - Hojo, Hajime

AU - Hu, Zhiwei

AU - Pi, Tunwen

AU - Soo, Yunliang

AU - Jin, Changqing

AU - Azuma, Masaki

AU - Long, Youwen

N1 - Funding Information: The authors thank L. X. Li for structural determination and fruitful discussions. This work was supported by the 973 Project of the Ministry of Science and Technology of China (Grant No. 2014CB921500), the National Natural Science Foundation of China (Grant Nos. 11574378, 51772324, and 61404052), and the Chinese Academy of Sciences (Grant Nos. QYZDB-SSW-SLH013, XDB07030300, YZ201555, and GJHZ1773). M. Azuma was supported by Kanagawa Institute of Industrial Science and Technology. Y. Long was partially supported by World Research Hub Initiative, Institute of Innovative Research, Tokyo Institute of Technology and Collaborative Research Projects, Laboratory for Materials and Structures, Tokyo Institute of Technology. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/10/2

Y1 - 2017/10/2

N2 - The novel A2B2O7-type compound Pb2Co2O7 was synthesized at 8 GPa and 1673 K. Synchrotron X-ray diffraction shows a cubic pyrochlore structure with space group Fd3m. Rietveld structural analysis reveals a large cation mixed occupancy at both A and B sites by about 40%, the greatest value found in the pyrochlore family. In combination with the X-ray absorption spectroscopy results, the specific chemical composition and charge states are determined to be (Co0.6Pb0.4)3+2(Pb0.6Co0.4)4+2O7, in which both the A-site Co3+ and the B-site Co4+ are low-spin. Due to the tetrahedral geometric frustration effects as well as the random Co4+ and Pb4+ distribution at the B site, spin glassy behavior is well observed following the conventional critical slowing down feature in Pb2Co2O7.

AB - The novel A2B2O7-type compound Pb2Co2O7 was synthesized at 8 GPa and 1673 K. Synchrotron X-ray diffraction shows a cubic pyrochlore structure with space group Fd3m. Rietveld structural analysis reveals a large cation mixed occupancy at both A and B sites by about 40%, the greatest value found in the pyrochlore family. In combination with the X-ray absorption spectroscopy results, the specific chemical composition and charge states are determined to be (Co0.6Pb0.4)3+2(Pb0.6Co0.4)4+2O7, in which both the A-site Co3+ and the B-site Co4+ are low-spin. Due to the tetrahedral geometric frustration effects as well as the random Co4+ and Pb4+ distribution at the B site, spin glassy behavior is well observed following the conventional critical slowing down feature in Pb2Co2O7.

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ER -

High-Pressure Synthesis of the Cobalt Pyrochlore Oxide Pb₂Co₂O₇ with Large Cation Mixed Occupancy

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