Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5

Huang, Dan; Ma, Tianyu; Brown, Dennis E.; Lapidus, Saul H.; Ren, Yang; Gao, Jianrong

doi:10.1021/acs.chemmater.0c04913

Title: Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe_11.5Si_1.5

Abstract

Here, ferromagnetic transitions, the magnetocaloric effect, and the atomic-scale microstructure in an annealed bulk material of LaFe_11.5Si_1.5 were investigated using magnetic measurements, Mössbauer spectroscopy, high-resolution X-ray diffraction analysis, and high-resolution transmission electron microscopy. The results provide evidence of the coexistence of two ferromagnetic phases with different Curie temperatures. The phase with a Curie temperature of 216 K corresponds to a Si-rich phase of a NaZn₁₃-type structure with a small lattice volume, whereas the phase with a Curie temperature of 185 K corresponds to a Si-poor phase of a NaZn₁₃-type structure with a large lattice volume. This phase coexistence is observed on a nanometer scale and it can account for inverse thermal hysteresis of the ferromagnetic transition in the Si-rich phase during warming. Furthermore, the phase coexistence helps the bulk material achieve a refrigeration capacity of 170 J kg^-1 due to a combination of the magnetocaloric effect in each phase. It is determined that the magnetocaloric effect in the Si-rich and the Si-poor phase brings about a maximum of the total entropy change of -3.55 and -6.80 and J kg^-1 K^-1 at respective Curie temperatures, respectively. Fundamentally, the phase coexistence indicates coloring of Si atoms in the lattice of a NaZn₁₃-typemore »« less

Authors:

Huang, Dan ^[1]; Ma, Tianyu ^[2]; Brown, Dennis E. ^[3];

^[4]; Ren, Yang ^[4];

^[5]

Northeastern Univ., (China)
Xi'an Jiaotong Univ., (China)
Northern Illinois Univ., DeKalb, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Northeastern Univ., Shenyang (China)

Publication Date:: Mon Apr 05 00:00:00 EDT 2021

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Ministry of Science and Technology (MOST) (China); China Scholarship Council

OSTI Identifier:: 1870429

Grant/Contract Number:: AC02-06CH11357; 51831003; 50671024; 2012CB619405

Resource Type:: Accepted Manuscript

Journal Name:: Chemistry of Materials

Additional Journal Information:: Journal Volume: 33; Journal Issue: 8; Journal ID: ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; grain; lattices, magnetic properties; phase separation; phase transitions

Citation Formats


                    Huang, Dan, Ma, Tianyu, Brown, Dennis E., Lapidus, Saul H., Ren, Yang, and Gao, Jianrong. Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5.  United States: N. p., 2021. 
Web.  doi:10.1021/acs.chemmater.0c04913.

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                    Huang, Dan, Ma, Tianyu, Brown, Dennis E., Lapidus, Saul H., Ren, Yang, & Gao, Jianrong. Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5.  United States.  https://doi.org/10.1021/acs.chemmater.0c04913

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                    Huang, Dan, Ma, Tianyu, Brown, Dennis E., Lapidus, Saul H., Ren, Yang, and Gao, Jianrong. Mon .  
"Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5".  United States.  https://doi.org/10.1021/acs.chemmater.0c04913.  https://www.osti.gov/servlets/purl/1870429.

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@article{osti_1870429,

  title        = {Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5},

  author       = {Huang, Dan and Ma, Tianyu and Brown, Dennis E. and Lapidus, Saul H. and Ren, Yang and Gao, Jianrong},

  abstractNote = {Here, ferromagnetic transitions, the magnetocaloric effect, and the atomic-scale microstructure in an annealed bulk material of LaFe11.5Si1.5 were investigated using magnetic measurements, Mössbauer spectroscopy, high-resolution X-ray diffraction analysis, and high-resolution transmission electron microscopy. The results provide evidence of the coexistence of two ferromagnetic phases with different Curie temperatures. The phase with a Curie temperature of 216 K corresponds to a Si-rich phase of a NaZn13-type structure with a small lattice volume, whereas the phase with a Curie temperature of 185 K corresponds to a Si-poor phase of a NaZn13-type structure with a large lattice volume. This phase coexistence is observed on a nanometer scale and it can account for inverse thermal hysteresis of the ferromagnetic transition in the Si-rich phase during warming. Furthermore, the phase coexistence helps the bulk material achieve a refrigeration capacity of 170 J kg-1 due to a combination of the magnetocaloric effect in each phase. It is determined that the magnetocaloric effect in the Si-rich and the Si-poor phase brings about a maximum of the total entropy change of -3.55 and -6.80 and J kg-1 K-1 at respective Curie temperatures, respectively. Fundamentally, the phase coexistence indicates coloring of Si atoms in the lattice of a NaZn13-type structure and can be attributed to nanoscale phase separation of a disordered precursor during annealing of the bulk material. The nanoscale phase separation may occur in other magnetocaloric materials, thus allowing for improvement of their refrigeration capacity.},

  doi          = {10.1021/acs.chemmater.0c04913},

  journal      = {Chemistry of Materials},

  number       = 8,

  volume       = 33,

  place        = {United States},

  year         = {Mon Apr 05 00:00:00 EDT 2021},

  month        = {Mon Apr 05 00:00:00 EDT 2021}

}

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Title: Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe11.5Si1.5

Abstract

Citation Formats

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Stability and Magnetocaloric Properties of Sintered La(Fe, Mn, Si)$_{13}$H$_{z}$ Alloys journal, October 2011

Influence of electronic and metallographic structures on hydrogen redistribution in La(Fe,Si)13-based magnetocaloric compounds journal, May 2019

Zero thermal expansion in NaZn 13 -type La(Fe,Si) 13 compounds journal, January 2015

Application of the exchange-striction model for the calculation of the FeRh alloys magnetic properties journal, May 2019

Magnetocaloric effect of LaFe11.35Co0.6Si1.05 alloy journal, May 2017

Phase separation-induced nanoscale heterogeneity in Gd5Si1.5Ge2.5 journal, September 2020

Exploring La(Fe,Si)13-based magnetic refrigerants towards application journal, September 2012

Formation mechanisms of NaZn13-type phase in giant magnetocaloric La–Fe–Si compounds during rapid solidification and annealing journal, October 2015

Itinerant-electron metamagnetic transition and large magnetocaloric effects in La ( Fe x Si 1 − x ) 13 compounds and their hydrides journal, March 2003

Structure and magnetic transition of LaFe 13 x Si x compounds journal, October 2003

Low-temperature large reversible “table-like” magnetocaloric effect in HoNi0.9Cu0.1Al compound journal, January 2015

Broadening of temperature working range in magnetocaloric La(Fe,Co,Si)13- based multicomposite journal, November 2017

The effect of the thermal decomposition reaction on the mechanical and magnetocaloric properties of La(Fe,Si,Co)13 journal, June 2012

Anomalous behavior of thermal expansion of α-Fe impurities in the La(Fe,Co,Si)13- based alloys modified by Mn or selected lanthanides (Ce, Pr, Ho) journal, February 2019

Giant Negative Thermal Expansion in NaZn 13 -Type La(Fe, Si, Co) 13 Compounds journal, July 2013

Mössbauer spectroscopic evaluation of chemical and electronic distributions in La(Fe0.81Si0.19)13 journal, March 2004

Recent developments in magnetocaloric materials journal, May 2005

Itinerant electron metamagnetic transition in La(FexSi1−x)13 intermetallic compounds journal, April 1999

Table-like magnetocaloric effect and enhanced refrigerant capacity of HPS La(Fe,Si)13-based composites by Ce–Co grain boundary diffusion journal, February 2020

La(Fe,Si)13-based magnetic refrigerants obtained by novel processing routes journal, September 2008

Effect of α-Fe impurities on the field dependence of magnetocaloric response in LaFe11.5Si1.5 journal, October 2015

EXPGUI , a graphical user interface for GSAS journal, April 2001

Structure and magnetic entropy change of melt-spun LaFe11.57Si1.43 ribbons journal, February 2005

Determination of the Antimony Valence State in Eu 10 Mn 6 Sb 13 journal, January 2004

Magnetic entropy change in Fe-based compound LaFe10.6Si2.4 journal, November 2000

Influence of negative lattice expansion and metamagnetic transition on magnetic entropy change in the compound LaFe11.4Si1.6 journal, June 2001

Large magnetic entropy change and low hysteresis loss in the Nd- and Co-doped La(Fe,Si)13 compounds journal, April 2008

Pyrochlores. IV. Crystallographic and Mössbauer studies of A 2 FeSbO 7 pyrochlores journal, December 1968

The correlation of the magnetic properties and the magnetocaloric effect in (Gd1−xErx)NiAl alloys journal, November 1998

Itinerant-electron metamagnetic transition and large magnetovolume effects in La ( Fe x Si 1 − x ) 13 compounds journal, November 2001

Magneto-elastic coupling in La(Fe, Mn, Si) 13 H y within the Bean-Rodbell model journal, May 2016

Magnetocaloric effect in NaZn13-type La1−xPrxFe11.44Si1.56 melt-spun ribbons journal, May 2010

Large entropy change, adiabatic temperature change, and small hysteresis in La(Fe,Mn)11.6Si1.4 strip-cast flakes journal, March 2015

First-order magnetic phase transition in LaFe 11.7 Si 1.3 studied using Mössbauer spectroscopy journal, June 2004

PHASE RELATIONS AND MICROSTRUCTURE OF La - Fe - Si ALLOYS UNDER DIFFERENT SOLIDIFICATION CONDITIONS journal, December 2011

Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5 journal, November 2019

Table-like magnetocaloric effect in Gd 56 Ni 15 Al 27 Zr 2 alloy and its field independence feature journal, September 2015

La(Fe,Co,Si)13 bulk alloys and ribbons with high temperature magnetocaloric effect journal, May 2010

An Application of the “Coloring Problem”: Structure−Composition−Bonding Relationships in the Magnetocaloric Materials LaFe 13 - x Si x journal, January 2008

Direct observation of paramagnetic spin fluctuations in LaFe 13−x Si x journal, December 2019

Systematic study of the microstructure, entropy change and adiabatic temperature change in optimized La–Fe–Si alloys journal, May 2011

Optimization of La(Fe,Co) 13− x Si x based compounds for magnetic refrigeration journal, May 2007

Study of the critical behaviour of the magnetization and electrical resistivity in cubic La(Fe, Si)13 compounds journal, April 1983

Structural and magnetic properties of magnetocaloric LaFe13–xSix compounds synthesized by high energy ball-milling journal, December 2010

Recent Progress in Exploring Magnetocaloric Materials journal, December 2009

Great magnetic entropy change in La(Fe, M ) 13 ( M =Si, Al) with Co doping journal, July 2000

Memory effect and inverse thermal hysteresis in La0.87Mn0.98Fe0.02Ox journal, May 2007

Phase equilibria in the Fe–La–Si ternary system journal, January 2012

Title: Nanoscale Phase Separation and Large Refrigerant Capacity in Magnetocaloric Material LaFe_11.5Si_1.5

Reversible solid-state hydrogen-pump driven by magnetostructural transformation in the prototype system La(Fe,Si) ₁₃ H _y
journal, October 2012

Multiple Metamagnetic Transitions in the Magnetic Refrigerant $La (Fe, Si)_{13} H_{x}$
journal, October 2008

Magnetic Relaxation and Asymmetric Quadrupole Doublets in the Mössbauer Effect
journal, January 1965

Enhancement of Refrigeration Capacity and Table-Like Magnetocaloric Effect in LaFe 10.7Co 0.8Si 1.5/ La 0.6Pr 0.4Fe 10.7Co 0.8Si 1.5 Composite
journal, October 2015

The dynamics of spontaneous hydrogen segregation in LaFe ₁₃₋ _x Si _x H _y
journal, May 2014

Strain-driven inverse thermal hysteresis behaviour in half-doped manganites
journal, May 2008

Site dependent hardening of the lanthanum metal lattice by hydrogen absorption
journal, March 2011

Large magnetocaloric effect in La(FexSi1−x)13 itinerant-electron metamagnetic compounds
journal, August 2002

Microstructure and magnetic properties of as-quenched cubic and tetragonal La(Fe1−xSix)13 compounds
journal, November 2013

Exotic hysteresis of ferrimagnetic transition in Laves compound TbCo ₂
journal, December 2019

Stability and Magnetocaloric Properties of Sintered La(Fe, Mn, Si)$_{13}$H$_{z}$ Alloys
journal, October 2011

Influence of electronic and metallographic structures on hydrogen redistribution in La(Fe,Si)13-based magnetocaloric compounds
journal, May 2019

Zero thermal expansion in NaZn ₁₃ -type La(Fe,Si) ₁₃ compounds
journal, January 2015

Application of the exchange-striction model for the calculation of the FeRh alloys magnetic properties
journal, May 2019

Magnetocaloric effect of LaFe11.35Co0.6Si1.05 alloy
journal, May 2017

Phase separation-induced nanoscale heterogeneity in Gd5Si1.5Ge2.5
journal, September 2020

Exploring La(Fe,Si)13-based magnetic refrigerants towards application
journal, September 2012

Formation mechanisms of NaZn13-type phase in giant magnetocaloric La–Fe–Si compounds during rapid solidification and annealing
journal, October 2015

Itinerant-electron metamagnetic transition and large magnetocaloric effects in $La ({Fe}_{x} {Si}_{1 - x})_{13}$ compounds and their hydrides
journal, March 2003

Structure and magnetic transition of LaFe _{13 x} Si _x compounds
journal, October 2003

Low-temperature large reversible “table-like” magnetocaloric effect in HoNi0.9Cu0.1Al compound
journal, January 2015

Broadening of temperature working range in magnetocaloric La(Fe,Co,Si)13- based multicomposite
journal, November 2017

The effect of the thermal decomposition reaction on the mechanical and magnetocaloric properties of La(Fe,Si,Co)13
journal, June 2012

Anomalous behavior of thermal expansion of α-Fe impurities in the La(Fe,Co,Si)13- based alloys modified by Mn or selected lanthanides (Ce, Pr, Ho)
journal, February 2019

Giant Negative Thermal Expansion in NaZn ₁₃ -Type La(Fe, Si, Co) ₁₃ Compounds
journal, July 2013

Mössbauer spectroscopic evaluation of chemical and electronic distributions in La(Fe0.81Si0.19)13
journal, March 2004

Recent developments in magnetocaloric materials
journal, May 2005

Itinerant electron metamagnetic transition in La(FexSi1−x)13 intermetallic compounds
journal, April 1999

Table-like magnetocaloric effect and enhanced refrigerant capacity of HPS La(Fe,Si)13-based composites by Ce–Co grain boundary diffusion
journal, February 2020

La(Fe,Si)13-based magnetic refrigerants obtained by novel processing routes
journal, September 2008

Effect of α-Fe impurities on the field dependence of magnetocaloric response in LaFe11.5Si1.5
journal, October 2015

EXPGUI , a graphical user interface for GSAS
journal, April 2001

Structure and magnetic entropy change of melt-spun LaFe11.57Si1.43 ribbons
journal, February 2005

Determination of the Antimony Valence State in Eu ₁₀ Mn ₆ Sb ₁₃
journal, January 2004

Magnetic entropy change in Fe-based compound LaFe10.6Si2.4
journal, November 2000

Influence of negative lattice expansion and metamagnetic transition on magnetic entropy change in the compound LaFe11.4Si1.6
journal, June 2001

Large magnetic entropy change and low hysteresis loss in the Nd- and Co-doped La(Fe,Si)13 compounds
journal, April 2008

Pyrochlores. IV. Crystallographic and Mössbauer studies of A ₂ FeSbO ₇ pyrochlores
journal, December 1968

The correlation of the magnetic properties and the magnetocaloric effect in (Gd1−xErx)NiAl alloys
journal, November 1998

Itinerant-electron metamagnetic transition and large magnetovolume effects in $La ({Fe}_{x} {Si}_{1 - x})_{13}$ compounds
journal, November 2001

Magneto-elastic coupling in La(Fe, Mn, Si) ₁₃ H _y within the Bean-Rodbell model
journal, May 2016

Magnetocaloric effect in NaZn13-type La1−xPrxFe11.44Si1.56 melt-spun ribbons
journal, May 2010

Large entropy change, adiabatic temperature change, and small hysteresis in La(Fe,Mn)11.6Si1.4 strip-cast flakes
journal, March 2015

First-order magnetic phase transition in ${LaFe}_{11.7} {Si}_{1.3}$ studied using Mössbauer spectroscopy
journal, June 2004

PHASE RELATIONS AND MICROSTRUCTURE OF La - Fe - Si ALLOYS UNDER DIFFERENT SOLIDIFICATION CONDITIONS
journal, December 2011

Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5
journal, November 2019

Table-like magnetocaloric effect in Gd ₅₆ Ni ₁₅ Al ₂₇ Zr ₂ alloy and its field independence feature
journal, September 2015

La(Fe,Co,Si)13 bulk alloys and ribbons with high temperature magnetocaloric effect
journal, May 2010

An Application of the “Coloring Problem”: Structure−Composition−Bonding Relationships in the Magnetocaloric Materials LaFe ₁₃ _- _x Si _x
journal, January 2008

Direct observation of paramagnetic spin fluctuations in LaFe _13−x Si _x
journal, December 2019

Systematic study of the microstructure, entropy change and adiabatic temperature change in optimized La–Fe–Si alloys
journal, May 2011

Optimization of La(Fe,Co) _{13− x} Si _x based compounds for magnetic refrigeration
journal, May 2007

Study of the critical behaviour of the magnetization and electrical resistivity in cubic La(Fe, Si)13 compounds
journal, April 1983

Structural and magnetic properties of magnetocaloric LaFe13–xSix compounds synthesized by high energy ball-milling
journal, December 2010

Recent Progress in Exploring Magnetocaloric Materials
journal, December 2009

Great magnetic entropy change in La(Fe, M ) ₁₃ ( M =Si, Al) with Co doping
journal, July 2000

Memory effect and inverse thermal hysteresis in La0.87Mn0.98Fe0.02Ox
journal, May 2007

Phase equilibria in the Fe–La–Si ternary system
journal, January 2012