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New strategies in metal oxide nanowire based gas sensors

  • Autores: Feng Shao
  • Directores de la Tesis: Francisco Hernández Ramírez (dir. tes.), Albert Cornet i Calveras (dir. tes.), Nuria López (dir. tes.)
  • Lectura: En la Universitat de Barcelona ( España ) en 2014
  • Idioma: inglés
  • Tribunal Calificador de la Tesis: Alejandro Pérez Rodríguez (presid.), Juan Daniel Prades García (secret.), Neyvis Almora Barrios (voc.), Teresa Andreu Arbella (voc.), Damián Monllor Satoca (voc.)
  • Materias:
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  • Resumen
    • This thesis presents the results of applying new strategies to understand the mechanism and explore the sensing performance of metal oxide (MOX) nanowire based gas sensors by testing individual nanowire gas sensors, running density functional theory (DFT) calculations, using new materials, applying ex-situ analysis and temperature-pulsed operation mode. These MOX nanowires include SnO2, CuO decorated SnO2, CuO and ZnO, electrically contacted either individually or in bundles. With SnO2-NH3 as a model system, DFT calculations were made to draw the pictures of surface-gas interactions, which were combined with empirical modeling of individual nanowire sensors to determine the sensing mechanism of this system. The surface reaction routine that involves non lattice oxygen was found to responsible for the sensing effect. As an interfering substance to NH3 sensing, H2O was also studied in this approach. At the new material front, CuO decorated SnO2 nanowire showed significantly increased sensitivity toward H2S while keeping other gases, e.g., CO and NH3 low, offering good selectivity to this gas. Ex-situ analysis has shown that sulfurization and desulfurization reactions happened on CuO, confirming the charge transport channel depletion model proposed for this material. The less common p-type CuO was obtained with the facile thermal oxidation method. NH3, H2S and NO2 sensing have all indicated the key role of surface adsorbed oxygen species in its gas sensing. Due to its intrinsic property, the ZnO nanowires assembled onto micro hot plate (?HP) substrates by dielectrophoretic (DEP) alignment showed relative NH3 selectivity from CO. When operated in temperature-pulsed mode, sensitivity enhancement was seen at the low temperature end. Such effect was ascribed to the fast regulation of surface oxygen, H2O and NO2 in the pulsed mode. The current dissertation is organized as follows: Chapter 1 introduces the general background of the MOX gas sensors and the basic idea of computational chemistry. Chapter 2 gives a brief introduction to density functional theory, which is the major theoretical tool in this work. Chapter 3 describes the experimental and theoretical techniques that have been applied. Chapter 4 deals with the NH3/H2O sensing of SnO2 nanowire, DFT calculations and empirical modeling. The sensing mechanism of NH3 by SnO2 and the interfering principle of H2O were unveiled. Chapter 5 reports the H2S sensing of SnO2 and CuO decorated SnO2 nanowires and the study of the corresponding mechanisms. Chapter 6 explores the NH3, H2S and NO2 sensing properties of the individual CuO nanowire. The importance of surface oxygen species in gas sensing was demonstrated. Chapter 7 is about the DEP deposition of ZnO nanowires onto the ?HP sensing substrate and the NH3 sensing in isothermal and temperature-pulsed mode. Chapter 8 reviews the present work, highlighting the main achievements and proposes future directions.


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