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Processing of materials in the form of ceramics normally involves several steps including calcination at a relatively low temperature for synthesis of the end-product powder and sintering at a high temperature for densification. The work we have been developing introduces a novel approach enabling synthesis plus sintering of materials in a single running experiment by using electric fields, ending with dense ceramics that display grains noticeably finer than in conventional processing. This new paradigm is fully illustrated with experiments conducted on amorphous CaCu3Ti4O12 precursor powder, shown to experience, on heating, crystallization through intermediate phases, followed by chemical reaction leading to synthesis of the end-product powder, plus densification depending on field adjustment. The processing time and furnace temperature are considerably reduced, demonstrating that enhanced synthesis and sintering rates applied under field input. Similar results found in Bi2/3Cu3Ti4O12 are also shown. The different factors that may contribute to this unique scenario, including Joule heating, defect generation, and reduction of free energy for nuclei formation promoted by the applied field, are briefly discussed. Overall, the findings we bring here are exclusive as they show an exploitable way that allows rapid processing of materials with good control over particle and grain coarsening.


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Ultrafast synthesis and sintering of materials in a single running experiment approach by using electric fields

Show Author's information Lílian M. JESUSa,#Ronaldo S. SILVAbJean-Claude M’ PEKOa( )
São Carlos Institute of Physics, University of São Paulo (USP), P.O. Box: 369, CEP: 13560-970 São Carlos, SP, Brazil
Group of Advanced Ceramic Materials, Department of Physics, Federal University of Sergipe (UFS), CEP: 49100-000 São Cristóvão, SE, Brazil

# Present address: Department of Physics, Federal University of São Carlos (UFSCar), 13560-905 São Carlos, SP, Brazil.

Abstract

Processing of materials in the form of ceramics normally involves several steps including calcination at a relatively low temperature for synthesis of the end-product powder and sintering at a high temperature for densification. The work we have been developing introduces a novel approach enabling synthesis plus sintering of materials in a single running experiment by using electric fields, ending with dense ceramics that display grains noticeably finer than in conventional processing. This new paradigm is fully illustrated with experiments conducted on amorphous CaCu3Ti4O12 precursor powder, shown to experience, on heating, crystallization through intermediate phases, followed by chemical reaction leading to synthesis of the end-product powder, plus densification depending on field adjustment. The processing time and furnace temperature are considerably reduced, demonstrating that enhanced synthesis and sintering rates applied under field input. Similar results found in Bi2/3Cu3Ti4O12 are also shown. The different factors that may contribute to this unique scenario, including Joule heating, defect generation, and reduction of free energy for nuclei formation promoted by the applied field, are briefly discussed. Overall, the findings we bring here are exclusive as they show an exploitable way that allows rapid processing of materials with good control over particle and grain coarsening.

Keywords:

field-assisted processing, synthesis, sintering, microstructure, dielectric response
Received: 16 October 2018 Revised: 21 December 2018 Accepted: 26 December 2018 Published: 13 June 2019 Issue date: June 2019
References(54)
[1]
Y-M Chiang, DP Birnie III, WD Kingery. Physical Ceramics: Principles for Ceramic Science and Engineering. John Wiley & Sons, Inc., 1997.
[2]
S Polarz, A Roy, M Lehmann, et al. Structure-property-function relationships in nanoscale oxide sensors: A case study based on zinc oxide. Adv Funct Mater 2007, 17: 1385-1391.
[3]
K Wang, F-Z Yao, W Jo, et al. Temperature-insensitive (K,Na)NbO3-based lead-free piezoactuator ceramics. Adv Funct Mater 2013, 23: 4079-4086.
[4]
LS MacAry, ML Kahn, C Estournès, et al. Size effect on properties of varistors made from zinc oxide nanoparticles through low temperature spark plasma sintering. Adv Funct Mater 2009, 19: 1775-1783.
[5]
I-W Chen, X-H Wang. Sintering dense nanocrystalline ceramics without final-stage grain growth. Nature 2000, 404: 168-171.
[6]
CP Cameron, R Raj. Grain-growth transition during sintering of colloidally prepared alumina powder compacts. J Am Ceram Soc 1988, 71: 1031-1035.
[7]
G-D Zhan, JD Kuntz, JL Wan, et al. Single-wall carbon nanotubes as attractive toughening agents in alumina-based nanocomposites. Nat Mater 2003, 2: 38-42.
[8]
R Raj, M Cologna, JSC Francis. Influence of externally imposed and internally generated electrical fields on grain growth, diffusional creep, sintering and related phenomena in ceramics. J Am Ceram Soc 2011, 94: 1941-1965.
[9]
K Lu. Sintering of nanoceramics. Int Mater Rev 2008, 53: 21-38.
[10]
XL He, F Ye, HJ Zhang, et al. Study on microstructure and thermal conductivity of spark plasma sintering AlN ceramics. Mater Des 2010, 31: 4110-4115.
[11]
KA Nekouee, RA Khosroshahi. Preparation and characterization of β-SiAlON/TiN nanocomposites sintered by spark plasma sintering and pressureless sintering. Mater Des 2016, 112: 419-428.
[12]
GA Samara. Pressure and temperature dependences of the dielectric properties of the perovskites BaTiO3 and SrTiO3. Phys Rev 1966, 151: 378-386.
[13]
M Malinowski, K Łukaszewicz, S Åsbrink. The influence of high hydrostatic pressure on lattice parameters of a single crystal of BaTiO3. J Appl Cryst 1986, 19: 7-9.
[14]
Cologna M, Rashkova B, Raj R. Flash sintering of nanograin zirconia in <5 s at 850°C. J Am Ceram Soc 2010, 93: 3556-3559.10.1111/j.1551-2916.2010.04089.x
[15]
J-C M’Peko, JSC Francis, R Raj. Impedance spectroscopy and dielectric properties of flash versus conventionally sintered yttria-doped zirconia electroceramics viewed at the microstructural level. J Am Ceram Soc 2013, 96: 3760-3767.
[16]
ALG Prette, M Cologna, VM Sglavo, et al. Flash-sintering of Co2MnO4 spinel for solid oxide fuel cell applications. J Power Sources 2011, 196: 2061-2065.
[17]
M Cologna, JSC Francis, R Raj. Field assisted and flash sintering of alumina and its relationship to conductivity and MgO-doping. J Eur Ceram Soc 2011, 31: 2827-2837.
[18]
R Muccillo, ENS Muccillo, M Kleitz. Densification and enhancement of the grain boundary conductivity of gadolinium-doped barium cerate by ultra fast flash grain welding. J Eur Ceram Soc 2012, 32: 2311-2316.
[19]
XM Hao, YJ Liu, ZH Wang, et al. A novel sintering method to obtain fully dense gadolinia doped ceria by applying a direct current. J Power Sources 2012, 210: 86-91.
[20]
J-C M’Peko, JSC Francis, R Raj. Field-assisted sintering of undoped BaTiO3: Microstructure evolution and dielectric permittivity. J Eur Ceram Soc 2014, 34: 3655-3660.
[21]
SK Jha, R Raj. The effect of electric field on sintering and electrical conductivity of titania. J Am Ceram Soc 2014, 97: 527-534.
[22]
LM Jesus, RS Silva, R Raj, et al. Electric field-assisted flash sintering of CaCu3Ti4O12: Microstructure characteristics and dielectric properties. J Alloys Compd 2016, 682: 753-758.
[23]
X Su, G Bai, J Zhang, et al. Preparation and flash sintering of MgTiO3 nanopowders obtained by the polyacrylamide gel method. Appl Surf Sci 2018, 442: 12-19.
[24]
MA Subramanian, D Li, N Duan, et al. High dielectric constant in ACu3Ti4O12 and ACu3Ti3FeO12 phases. J Solid State Chem 2000, 151: 323-325.
[25]
J Li, MA Subramanian, HD Rosenfeld, et al. Clues to the giant dielectric constant of CaCu3Ti4O12 in the defect structure of “SrCu3Ti4O12”. Chem Mater 2004, 16: 5223-5225.
[26]
DC Sinclair, TB Adams, FD Morrison, et al. CaCu3Ti4O12: One-step internal barrier layer capacitor. Appl Phys Lett 2002, 80: 2153-2155.
[27]
Adams TB, Sinclair DC, West AR. Giant barrier layer capacitance effects in CaCu3Ti4O12 ceramics. Adv Mater 2002, 14: 1321-1323.10.1002/1521-4095(20020916)14:18<1321::AID-ADMA1321>3.0.CO;2-P
[28]
S-Y Chung, I-D Kim, S-JL Kang. Strong nonlinear current-voltage behaviour in perovskite-derivative calcium copper titanate. Nat Mater 2004, 3: 774-778.
[29]
R Schmidt, MC Stennett, NC Hyatt, et al. Effects of sintering temperature on the internal barrier layer capacitor (IBLC) structure in CaCu3Ti4O12 (CCTO) ceramics. J Eur Ceram Soc 2012, 32: 3313-3323.
[30]
R Löhnert, R Schmidt, J Töpfer. Effect of sintering conditions on microstructure and dielectric properties of CaCu3Ti4O12 (CCTO) ceramics. J Electroceram 2015, 34: 241-248.
[31]
MP Pechini. U.S. Patent No. 3,330.697. 1967.
[32]
LM Jesus, JCA Santos, DV Sampaio, et al. Polymeric synthesis and conventional versus laser sintering of CaCu3Ti4O12 electroceramics: (Micro)structures, phase development and dielectric properties. J Alloys Compd 2016, 654: 482-490.
[33]
ASTM E1382-97. Standard Test Methods for Determining Average Grain Size Using Semiautomatic and Automatic Image Analysis. ASTM International, West Conshohocken, PA, 1997.
[34]
MF García-Sánchez, J-C M’Peko, AR Ruiz-Salvador, et al. An elementary picture of dielectric spectroscopy in solids: Physical basis. J Chem Educ 2003, 80: 1062-1073.
[35]
B Bochu, MN Deschizeaux, JC Joubert, et al. Synthèse et caractérisation d'une série de titanates pérowskites isotypes de [CaCu3](Mn4)O12. J Solid State Chem 1979, 29: 291-298.
[36]
LM Jesus, RS Silva, R Raj, et al. Electric field-assisted ultrafast synthesis of nanopowders: A novel and cost-efficient approach. RSC Adv 2016, 6: 107208-107213.
[37]
JJ Liu, YC Sui, C-G Duan, et al. CaCu3Ti4O12: Low-temperature synthesis by pyrolysis of an organic solution. Chem Mater 2006, 18: 3878-3882.
[38]
JJ Liu, RW Smith, W-N Mei. Synthesis of the giant dielectric constant material CaCu3Ti4O12 by wet-chemistry methods. Chem Mater 2007, 19: 6020-6024.
[39]
R Raj. Joule heating during flash-sintering. J Eur Ceram Soc 2012, 32: 2293-2301.
[40]
RI Todd, E Zapata-Solvas, RS Bonilla, et al. Electrical characteristics of flash sintering: Thermal runaway of Joule heating. J Eur Ceram Soc 2015, 35: 1865-1877.
[41]
YY Zhang, J-I Jung, J Luo. Thermal runaway, flash sintering and asymmetrical microstructural development of ZnO and ZnO-Bi2O3 under direct currents. Acta Mater 2015, 94: 87-100.
[42]
YX Du, AJ Stevenson, D Vernat, et al. Estimating Joule heating and ionic conductivity during flash sintering of 8YSZ. J Eur Ceram Soc 2016, 36: 749-759.
[43]
H Charalambous, SK Jha, RT Lay, et al. Investigation of temperature approximation methods during flash sintering of ZnO. Ceram Int 2018, 44: 6162-6169.
[44]
H Charalambous, SK Jha, XL Phuah, et al. In situ measurement of temperature and reduction of rutile titania using energy dispersive X-ray diffraction. J Eur Ceram Soc 2018, 38: 5503-5511.
[45]
M Yu, S Grasso, R McKinnon, et al. Review of flash sintering: Materials, mechanisms and modelling. Adv Appl Ceram 2017, 116: 24-60.
[46]
Y Gao, FZ Liu, DG Liu, et al. Electrical-field induced nonlinear conductive behavior in dense zirconia ceramic. J Mater Sci Technol 2017, 33: 897-900.
[47]
DG Liu, YJ Cao, JL Liu, et al. Effect of oxygen partial pressure on temperature for onset of flash sintering 3YSZ. J Eur Ceram Soc 2018, 38: 817-820.
[48]
XH Su, G Bai, YJ Jia, et al. Flash sintering of lead zirconate titanate (PZT) ceramics: Influence of electrical field and current limit on densification and grain growth. J Eur Ceram Soc 2018, 38: 3489-3497.
[49]
JSC Francis, R Raj. Influence of the field and the current limit on flash sintering at isothermal furnace temperatures. J Am Ceram Soc 2013, 96: 2754-2758.
[50]
W Liu, KM Liang, YK Zheng, et al. The effect of an electric field on the phase separation of glasses. J Phys D: Appl Phys 1997, 30: 3366-3370.
[51]
KS Naik, VM Sglavo, R Raj. Flash sintering as a nucleation phenomenon and a model thereof. J Eur Ceram Soc 2014, 34: 4063-4067.
[52]
SIR Costa, M Li, JR Frade, et al. Modulus spectroscopy of CaCu3Ti4O12 ceramics: Clues to the internal barrier layer capacitance mechanism. RSC Adv 2013, 3: 7030-7036.
[53]
LM Jesus, LB Barbosa, DR Ardila, et al. Effect of conventional and laser sintering on the (micro)structural and dielectric properties of Bi2/3Cu3Ti4O12 synthesized through a polymeric precursor route. J Alloys Compd 2018, 735: 2384-2394.
[54]
LM Jesus. Conventional, laser and electric field-assisted processing of ACu3Ti4O12 (A = Ca, Bi2/3) electroceramics: (Micro)structure and (di)electrical properties. Ph.D. Thesis. São Carlos Institute of Physics, University of São Paulo (USP), Brazil, 2016.
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Publication history

Received: 16 October 2018
Revised: 21 December 2018
Accepted: 26 December 2018
Published: 13 June 2019
Issue date: June 2019

Copyright

© The author(s) 2019

Acknowledgements

This work was partly supported by the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - Brasil (CAPES) - Finance Code 001, through Grant Nos. BEX 3276/14-7 and BEX 9291/13-0. J.-C. M’Peko devised the work. L. M. Jesus and R. S. Silva were responsible for chemical synthesis. L. M. Jesus conducted the field-assisted processing experiments, plus material characterization (XRD, SEM, and dielectric measurements) under J.-C. M’Peko’s supervision. J.-C. M’Peko wrote the first draft of the manuscript, and all present authors participated in manuscript revision, followed by submission approval. L. M. Jesus and J.-C. M’Peko are profoundly grateful to Prof. R. Raj (at CU Boulder, USA) for introduction to flash sintering experiments and for allowing collection of some data presented here. S. K. Jha and J.-M. Lebrun are also thanked for assistance in some of the conducted flash experiments, as well as B. E. Francisco for help with some of the XRD measurements carried out.

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