Paving the way to nanoionics: atomic origin of barriers for ionic transport through interfaces
The blocking of ion transport at interfaces strongly limits the performance of electrochemical nanodevices for energy applications. The barrier is believed to arise from space-charge regions generated by mobile ions by analogy to semiconductor junctions. Here we show that something different is at p...
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| Veröffentlicht in: | Scientific reports 2015-12, Vol.5 (1), p.17229-17229, Article 17229 |
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| creator | Frechero, M. A. Rocci, M. Sánchez-Santolino, G. Kumar, Amit Salafranca, J. Schmidt, Rainer Díaz-Guillén, M. R. Durá, O. J. Rivera-Calzada, A. Mishra, R. Jesse, Stephen Pantelides, S. T. Kalinin, Sergei V. Varela, M. Pennycook, S. J. Santamaria, J. Leon, C. |
| description | The blocking of ion transport at interfaces strongly limits the performance of electrochemical nanodevices for energy applications. The barrier is believed to arise from space-charge regions generated by mobile ions by analogy to semiconductor junctions. Here we show that something different is at play by studying ion transport in a bicrystal of yttria (9% mol) stabilized zirconia (YSZ), an emblematic oxide ion conductor. Aberration-corrected scanning transmission electron microscopy (STEM) provides structure and composition at atomic resolution, with the sensitivity to directly reveal the oxygen ion profile. We find that Y segregates to the grain boundary at Zr sites, together with a depletion of oxygen that is confined to a small length scale of around 0.5 nm. Contrary to the main thesis of the space-charge model, there exists no evidence of a long-range O vacancy depletion layer. Combining ion transport measurements across a single grain boundary by nanoscale electrochemical strain microscopy (ESM), broadband dielectric spectroscopy measurements and density functional calculations, we show that grain-boundary-induced electronic states act as acceptors, resulting in a negatively charged core. Besides the possible effect of the modified chemical bonding, this negative charge gives rise to an additional barrier for ion transport at the grain boundary. |
| doi_str_mv | 10.1038/srep17229 |
| format | Article |
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A. ; Rocci, M. ; Sánchez-Santolino, G. ; Kumar, Amit ; Salafranca, J. ; Schmidt, Rainer ; Díaz-Guillén, M. R. ; Durá, O. J. ; Rivera-Calzada, A. ; Mishra, R. ; Jesse, Stephen ; Pantelides, S. T. ; Kalinin, Sergei V. ; Varela, M. ; Pennycook, S. J. ; Santamaria, J. ; Leon, C.</creator><creatorcontrib>Frechero, M. A. ; Rocci, M. ; Sánchez-Santolino, G. ; Kumar, Amit ; Salafranca, J. ; Schmidt, Rainer ; Díaz-Guillén, M. R. ; Durá, O. J. ; Rivera-Calzada, A. ; Mishra, R. ; Jesse, Stephen ; Pantelides, S. T. ; Kalinin, Sergei V. ; Varela, M. ; Pennycook, S. J. ; Santamaria, J. ; Leon, C. ; Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)</creatorcontrib><description>The blocking of ion transport at interfaces strongly limits the performance of electrochemical nanodevices for energy applications. The barrier is believed to arise from space-charge regions generated by mobile ions by analogy to semiconductor junctions. 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A.</creatorcontrib><creatorcontrib>Rocci, M.</creatorcontrib><creatorcontrib>Sánchez-Santolino, G.</creatorcontrib><creatorcontrib>Kumar, Amit</creatorcontrib><creatorcontrib>Salafranca, J.</creatorcontrib><creatorcontrib>Schmidt, Rainer</creatorcontrib><creatorcontrib>Díaz-Guillén, M. R.</creatorcontrib><creatorcontrib>Durá, O. J.</creatorcontrib><creatorcontrib>Rivera-Calzada, A.</creatorcontrib><creatorcontrib>Mishra, R.</creatorcontrib><creatorcontrib>Jesse, Stephen</creatorcontrib><creatorcontrib>Pantelides, S. T.</creatorcontrib><creatorcontrib>Kalinin, Sergei V.</creatorcontrib><creatorcontrib>Varela, M.</creatorcontrib><creatorcontrib>Pennycook, S. J.</creatorcontrib><creatorcontrib>Santamaria, J.</creatorcontrib><creatorcontrib>Leon, C.</creatorcontrib><creatorcontrib>Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)</creatorcontrib><title>Paving the way to nanoionics: atomic origin of barriers for ionic transport through interfaces</title><title>Scientific reports</title><addtitle>Sci Rep</addtitle><addtitle>Sci Rep</addtitle><description>The blocking of ion transport at interfaces strongly limits the performance of electrochemical nanodevices for energy applications. The barrier is believed to arise from space-charge regions generated by mobile ions by analogy to semiconductor junctions. Here we show that something different is at play by studying ion transport in a bicrystal of yttria (9% mol) stabilized zirconia (YSZ), an emblematic oxide ion conductor. Aberration-corrected scanning transmission electron microscopy (STEM) provides structure and composition at atomic resolution, with the sensitivity to directly reveal the oxygen ion profile. We find that Y segregates to the grain boundary at Zr sites, together with a depletion of oxygen that is confined to a small length scale of around 0.5 nm. Contrary to the main thesis of the space-charge model, there exists no evidence of a long-range O vacancy depletion layer. Combining ion transport measurements across a single grain boundary by nanoscale electrochemical strain microscopy (ESM), broadband dielectric spectroscopy measurements and density functional calculations, we show that grain-boundary-induced electronic states act as acceptors, resulting in a negatively charged core. 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A.</au><au>Rocci, M.</au><au>Sánchez-Santolino, G.</au><au>Kumar, Amit</au><au>Salafranca, J.</au><au>Schmidt, Rainer</au><au>Díaz-Guillén, M. R.</au><au>Durá, O. J.</au><au>Rivera-Calzada, A.</au><au>Mishra, R.</au><au>Jesse, Stephen</au><au>Pantelides, S. T.</au><au>Kalinin, Sergei V.</au><au>Varela, M.</au><au>Pennycook, S. J.</au><au>Santamaria, J.</au><au>Leon, C.</au><aucorp>Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Paving the way to nanoionics: atomic origin of barriers for ionic transport through interfaces</atitle><jtitle>Scientific reports</jtitle><stitle>Sci Rep</stitle><addtitle>Sci Rep</addtitle><date>2015-12-17</date><risdate>2015</risdate><volume>5</volume><issue>1</issue><spage>17229</spage><epage>17229</epage><pages>17229-17229</pages><artnum>17229</artnum><issn>2045-2322</issn><eissn>2045-2322</eissn><abstract>The blocking of ion transport at interfaces strongly limits the performance of electrochemical nanodevices for energy applications. The barrier is believed to arise from space-charge regions generated by mobile ions by analogy to semiconductor junctions. Here we show that something different is at play by studying ion transport in a bicrystal of yttria (9% mol) stabilized zirconia (YSZ), an emblematic oxide ion conductor. Aberration-corrected scanning transmission electron microscopy (STEM) provides structure and composition at atomic resolution, with the sensitivity to directly reveal the oxygen ion profile. We find that Y segregates to the grain boundary at Zr sites, together with a depletion of oxygen that is confined to a small length scale of around 0.5 nm. Contrary to the main thesis of the space-charge model, there exists no evidence of a long-range O vacancy depletion layer. Combining ion transport measurements across a single grain boundary by nanoscale electrochemical strain microscopy (ESM), broadband dielectric spectroscopy measurements and density functional calculations, we show that grain-boundary-induced electronic states act as acceptors, resulting in a negatively charged core. Besides the possible effect of the modified chemical bonding, this negative charge gives rise to an additional barrier for ion transport at the grain boundary.</abstract><cop>London</cop><pub>Nature Publishing Group UK</pub><pmid>26673351</pmid><doi>10.1038/srep17229</doi><tpages>1</tpages><oa>free_for_read</oa></addata></record> |
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| subjects | 639/301/299/893 639/766/119/544 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY Electrochemistry Electron microscopy fuel cells Grain boundaries Humanities and Social Sciences Interfaces Ion transport Ions multidisciplinary Oxygen Oxygen depletion Science Spectroscopy surfaces, interfaces and thin films Transmission electron microscopy Zirconia |
| title | Paving the way to nanoionics: atomic origin of barriers for ionic transport through interfaces |
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