[en] In this study, we propose a straightforward method for x determination in sub-stoichiometric
nickel oxide (Ni1−xO) films prepared by ultrasonic spray pyrolysis on fluor-tin oxide (FTO)
substrates by varying the post-deposition thermal treatment. The Ni3+ concentration, the flat
band potential (Φfb) and the open circuit potential (Voc) were determined by electrochemical
impedance analysis in aqueous media and correlated to the transmission of Ni1−xO films.
An x-ray photoelectron spectroscopy study was also performed to quantify the amount of
Ni3+ in the films and compare it with the one determined by electrochemical analysis. The
electrochromic behavior of the Ni1−xO films in non-aqueous electrolyte was investigated as
well.
With increasing Ni3+ concentration the films became more brownish and more conductive,
both Voc and Φfb values increased. Calibration curves of transmission at 550 nm or open
circuit potential versus carrier concentration were plotted and allowed the prediction of x in an
unknown Ni1−xO sample. The Ni1−xO films characterized by the highest Ni3+ concentration
have a darker colored state but lower transmission modulation, due to their reduced specific
surface and increased crystallinity.
Disciplines :
Physics
Author, co-author :
Manceriu, Laura ; Université de Liège > Département de chimie (sciences) > LCIS - GreenMAT
Colson, Pierre ; Université de Liège > Département de chimie (sciences) > LCIS - GreenMAT
Maho, Anthony ; Université de Liège > Département de chimie (sciences) > LCIS - GreenMAT
Eppe, Gauthier ; Université de Liège > Département de chimie (sciences) > Chimie analytique inorganique
Nguyen, Ngoc Duy ; Université de Liège > Département de physique > Physique des solides, interfaces et nanostructures
Labrugere, Christine; CNRS, Université de Bordeaux, PLACAMAT UMS 3626, F-33600 Pessac, France
Rougier, Aline; CNRS, Université de Bordeaux, ICMCB, UPR 9048, F-33600 Pessac, France
Cloots, Rudi ; Université de Liège > Département de chimie (sciences) > LCIS - GreenMAT
Henrist, Catherine ; Université de Liège > Département de chimie (sciences) > LCIS - GreenMAT
Language :
English
Title :
Straightforward prediction of the Ni1−xO layers stoichiometry by using optical and electrochemical measurements
Mihelcic M, Šurca Vuk A, Jerman I, Orel B, Švegl F, Moulki H, Faure C, Campet G and Rougier A 2014 Comparison of electrochromic properties of Ni1-xO in lithium and lithium-free aprotic electrolytes: from Ni1-xO pigment coatings to flexible electrochromic devices Sol. Energy Mater. Sol. Cells 120 116-30
Denayer J et al 2014 Surfactant-assisted ultrasonic spray pyrolysis of nickel oxide and lithium-doped nickel oxide thin films, toward electrochromic applications Appl. Surf. Sci. 321 61-9
Hod I, Tachan Z, Shalom M and Zaban A 2013 Characterization and control of the electronic properties of a NiO based dye sensitized photocathode Phys. Chem. Chem. Phys. 15 6339-43
Lin Y-C, Chen Y-T and Yao P-C 2013 Effect of post-heat-treated NiOx overlayer on performance of nanocrystalline TiO2 thin films for dye-sensitized solar cells J. Power Sources 240 705-12
Ozdemir S, Osburn T B and Gole J L 2011 Nanostructure modified gas sensor detection matrix for NO transient conversion of NO to NO2 J. Electrochem. Soc. 158 J201-7
Zhang J, Zeng D, Zhu Q, Wu J, Huang Q and Xie C 2016 Effect of nickel vacancies on the room-temperature NO2 sensing properties of mesoporous NiO nanosheets J. Phys. Chem. C 120 3936-45
Long H, Fang G, Huang H, Mo X, Xia W, Dong B, Meng X and Zhao X 2009 Ultraviolet electroluminescence from ZnO/NiO-based heterojunction light-emitting diodes Appl. Phys. Lett. 95 013509
Tyagi M, Tomar M and Gupta V 2013 Postdeposition annealing of NiOx thin films: a transition from n-type to p-type conductivity for short wave length optoelectronic devices J. Mater. Res. 28 723-32
Andrzej S 2012 Defect complexes and defect clusters in Mn1-δO, Co1-δO and Ni1-δO oxides diagrams of the concentrations of point defects Int. J. Chem. 4 2-25
Sockel H G and Schmalzried H 1968 Coulometric titration in transition metal oxides Ber. Bunsenges. Phys. Chem. 72 745-54
Lunkenheimer P, Loidl A, Otterman C R and Bange K 1951 Correlated barrier hoping in NiO films Phys. Rev. B 44 5927-30
Chen T F, Wang A J, Shang B Y, Wu Z L, Li Y L and Wang Y S 2015 Property modulation of NiO films grown by radio frequency magnetron sputtering J. Alloys Compd. 643 167-73
Nandy S, Saha B and Mitra M K 2007 Effect of oxygen partial pressure on the electrical and optical properties of highly (2 0 0) oriented p-type Ni1-xO films by DC sputtering J. Mater. Sci. 42 5766-72
Wen R-T, Granqvist C G and Niklasson G A 2015 Anodic electrochromism for energy-efficient windows: cation/anion-based surface processes and effects of crystal facets in nickel oxide thin films Adv. Funct. Mater. 25 3359-70
Da Rocha M and Rougier A 2016 Electrochromism of non-stoichiometric NiO thin film: as single layer and in full device Appl. Phys. A 122 1-7
Wu C-C and Yang C-F 2015 Effect of annealing temperature on the characteristics of the modified spray deposited Li-doped NiO films and their applications in transparent heterojunction diode Sol. Energy Mater. Sol. Cells 132 492-8
Chan X H, Jennings J R, Hossain M A, Yu K K Z and Wang Q 2011 Characteristics of p-NiO thin films prepared by spray pyrolysis and their application in CdS-sensitized photocathodes J. Electrochem. Soc. 158 H733-40
Kim D S and Lee H C 2012 Nickel vacancy behavior in the electrical conductance of nonstoichiometric nickel oxide film J. Appl. Phys. 112 034504
Yang J-L, Lai Y-S and Chen J S 2005 Effect of heat treatment on the properties of non-stoichiometric p-type nickel oxide films deposited by reactive sputtering Thin Solid Films 488 242-6
Bouessay I, Rougier A, Poizot P, Moscovici J, Michalowicz A and Tarascon J-M 2005 Electrochromic degradation in nickel oxide thin film: a self-discharge and dissolution phenomenon Electrochim. Acta 50 3737-45
Rubin M, Wen S-J, Richardson T, Kerr J, von Rottkay K and Slack J 1998 Electrochromic lithium nickel oxide by pulsed laser deposition and sputtering Sol. Energy Mater. Sol. Cells 54 59-66
Thimsen E, Martinson A B F, Elam J W and Pellin M J 2012 Energy levels, electronic properties and rectification in ultrathin p-NiO films synthesized by atomic layer deposition J. Phys. Chem. C 12 16830-40
Nakaoka K, Ueyama J and Ogura K 2004 Semiconductor and electrochromic properties of electrochemically deposited nickel oxide films J. Electroanal. Chem. 571 93-9
An W-J, Thimsen E and Biswas P 2010 Aerosol-chemical vapor deposition method for synthesis of nanostructured metal oxide thin films with controlled morphology J. Phys. Chem. Lett. 1 249-53
Nalage S R, Chougule M A, Sen S, Joshi P B and Patil V B 2012 Sol-gel synthesis of nickel oxide thin films and their characterization Thin Solid Films 520 4835-40
Usha K S, Sivakumar R, Sanjeeviraja C, Sathe V, Ganesan V and Wang T Y 2016 Improved electrochromic performance of a radio frequency magnetron sputtered NiO thin film with high optical switching speed RSC Adv. 6 79668-80
Qing Y, Yang C, Yu Z, Zhang Z, Hu Q and Liu C 2016 Large-area fabrication of superhydrophobic zinc surface with reversible wettability switching and anticorrosion J. Electrochem. Soc. 163 D385-91
Antony J, Nutting J, Baer D R, Meyer D, Sharma A and Qiang Y 2006 Size-dependent specific surface area of nanoporous film assembled by core-shell iron nanoclusters J. Nanomat. 2006 1-4
Newman R and Chrenko R M 1959 Optical properties of nickel oxide Phys. Rev. 114 1507-13
Ramesham R 1998 Determination of flat-band potential for boron-doped diamond electrode in 0.5 m NaCl by ac-impedance spectroscopy Thin Solid Films 322 158-66
Choi S C, Koumoto K and Yanagida H 1986 Electrical conduction and effective mass of a hole in single-crystal NiO J. Mater. Sci. 21 1947-50
Natu G, Hasin P, Huang Z, Ji Z, He M and Wu Y 2012 Valence band-edge engineering of nickel oxide nanoparticles via cobalt doping for application in p-type dye-sensitized solar cells ACS Appl. Mater. Interfaces 4 5922-9
Sørensen O T 1981 Nonstoichiometric oxides Thermodynamics and Defect Structure of Nonstoichiometric Oxides (New York: Academic) ch 1 pp 2-56
Preda I, Gutierrez A, Abbate M, Yubero F, Mendez J, Alvarez L and Soriano L 2008 Interface effects in the Ni 2p x-ray photoelectron spectra of NiO thin films grown on oxide substrates Phys. Rev. B 77 075411 1-7
Chen Y, Sun Y, Dai X, Zhang B, Ye Z, Wang M and Wu H 2015 Tunable electrical properties of NiO thin films and p-type thin-film transistors Thin Solid Films 592 195-9
Reddy A M, Reddy A S, Lee K and Reddy P S 2011 Effect of oxygen partial pressure on the structural, electrical and optical properties of sputtered NiO films Ceram. Int. 37 2837-43
Chen Z, Xiao A, Chen Y, Zuo C, Zhou S and Li L 2013 Highly porous nickel oxide thin films prepared by a hydrothermal synthesis method for electrochromic application J. Phys. Chem. Solids 74 1522-6