Determination of the “NiOOH” charge and discharge mechanisms at ideal activity

Merrill, Matthew; Worsley, Marcus; Wittstock, Arne; Biener, Juergen; Stadermann, Michael

doi:10.1016/j.jelechem.2014.01.022

Title: Determination of the “NiOOH” charge and discharge mechanisms at ideal activity

Abstract

Here, optimization of electrodeposition conditions produced Ni(OH)₂ deposits chargeable up to 1.84 ± 0.02 e^– per Ni on and the resulting nickel oxide/hydroxide active material could subsequently deliver 1.58 ± 0.02 e^– per Ni ion (462 mA h/g) over a potential range <0.2 V. The ability of the “NiOOH” active material to deliver an approximately ideal charge and discharge facilitated a coulometric and thermodynamic analysis through which the charge/discharge mechanisms were determined from known enthalpies of formation. The (dis)charge states were confirmed with in situ Raman spectroscopy. The mechanisms were additionally evaluated with respect to pH and potential dependence, charge quantities, hysteresis, and fluoride ion partial inhibition of the charge mechanism. The results indicate that the “NiOOH” (dis)charges as a solid-state system with mechanisms consistent with known nickel and oxygen redox reactions. A defect chemistry mechanism known for the LiNiO₂ system also occurs for “NiOOH” to cause both high activity and hysteresis. Similar to other cation insertion nickel oxides, the activity of the “NiOOH” mechanism is predominantly due to oxygen redox activity and does not involve the Ni4⁺ oxidation state. The “NiOOH” was produced from cathodic electrodeposition of Ni(OH)₂ from nickel nitrate solutions onto highly oriented pyrolytic graphite at idealmore »« less

Authors:

Merrill, Matthew ^[1]; Worsley, Marcus ^[1]; Wittstock, Arne ^[1]; Biener, Juergen ^[1]; Stadermann, Michael ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Chemical Sciences Div.

Publication Date:: Fri Jan 24 00:00:00 EST 2014

Research Org.:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1305895

Report Number(s):: LLNL-JRNL-539131
Journal ID: ISSN 1572-6657

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Electroanalytical Chemistry

Additional Journal Information:: Journal Volume: 717-718; Journal Issue: C; Journal ID: ISSN 1572-6657

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 30 DIRECT ENERGY CONVERSION; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; NiOOH; Ni(OH)2; nickel electrode; nickel oxy-hydroxide; active oxygen

Citation Formats


                    Merrill, Matthew, Worsley, Marcus, Wittstock, Arne, Biener, Juergen, and Stadermann, Michael. Determination of the “NiOOH” charge and discharge mechanisms at ideal activity.  United States: N. p., 2014. 
Web.  doi:10.1016/j.jelechem.2014.01.022.

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                    Merrill, Matthew, Worsley, Marcus, Wittstock, Arne, Biener, Juergen, & Stadermann, Michael. Determination of the “NiOOH” charge and discharge mechanisms at ideal activity.  United States.  https://doi.org/10.1016/j.jelechem.2014.01.022

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                    Merrill, Matthew, Worsley, Marcus, Wittstock, Arne, Biener, Juergen, and Stadermann, Michael. Fri .  
"Determination of the “NiOOH” charge and discharge mechanisms at ideal activity".  United States.  https://doi.org/10.1016/j.jelechem.2014.01.022.  https://www.osti.gov/servlets/purl/1305895.

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@article{osti_1305895,

  title        = {Determination of the “NiOOH” charge and discharge mechanisms at ideal activity},

  author       = {Merrill, Matthew and Worsley, Marcus and Wittstock, Arne and Biener, Juergen and Stadermann, Michael},

  abstractNote = {Here, optimization of electrodeposition conditions produced Ni(OH)2 deposits chargeable up to 1.84 ± 0.02 e– per Ni on and the resulting nickel oxide/hydroxide active material could subsequently deliver 1.58 ± 0.02 e– per Ni ion (462 mA h/g) over a potential range <0.2 V. The ability of the “NiOOH” active material to deliver an approximately ideal charge and discharge facilitated a coulometric and thermodynamic analysis through which the charge/discharge mechanisms were determined from known enthalpies of formation. The (dis)charge states were confirmed with in situ Raman spectroscopy. The mechanisms were additionally evaluated with respect to pH and potential dependence, charge quantities, hysteresis, and fluoride ion partial inhibition of the charge mechanism. The results indicate that the “NiOOH” (dis)charges as a solid-state system with mechanisms consistent with known nickel and oxygen redox reactions. A defect chemistry mechanism known for the LiNiO2 system also occurs for “NiOOH” to cause both high activity and hysteresis. Similar to other cation insertion nickel oxides, the activity of the “NiOOH” mechanism is predominantly due to oxygen redox activity and does not involve the Ni4+ oxidation state. The “NiOOH” was produced from cathodic electrodeposition of Ni(OH)2 from nickel nitrate solutions onto highly oriented pyrolytic graphite at ideal electrodeposition current efficiencies and the deposition mechanism was also characterized.},

  doi          = {10.1016/j.jelechem.2014.01.022},

  journal      = {Journal of Electroanalytical Chemistry},

  number       = C,

  volume       = 717-718,

  place        = {United States},

  year         = {Fri Jan 24 00:00:00 EST 2014},

  month        = {Fri Jan 24 00:00:00 EST 2014}

}

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A detailed investigation has been carried out of the structure and electrochemical activity of electrodeposited Ni-Fe films for the oxygen evolution reaction (OER) in alkaline electrolytes. Ni-Fe films with a bulk and surface composition of 40% Fe exhibit OER activities that are roughly 2 orders of magnitude higher than that of a freshly deposited Ni film and about 3 orders of magnitude higher than that of an Fe film. The freshly deposited Ni film increases in activity by as much as 20-fold during exposure to the electrolyte (KOH); however, all films containing Fe are stable as deposited. The oxidation ofmore »« less
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https://doi.org/10.1021/ja405351s

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Electrochemical Dehydrogenation Pathways of Amines to Nitriles on NiOOH

Journal Article Bender, Michael T. ; Choi, Kyoung-Shin - JACS Au

Nitriles are highly important synthetic intermediates with applications in a wide variety of organic reactions including production of pharmaceuticals, fine chemicals, and agricultural chemicals. Thus, developing effective green routes to oxidize amines to nitriles is of great interest. One promising method to achieve the oxidation of primary amines to nitriles is through electrochemical oxidation on NiOOH electrodes. This reaction has long been thought to occur through an indirect mechanism consisting of a series of potential independent hydrogen atom transfer steps to catalytic Ni³⁺ sites in NiOOH, which reduces NiOOH to Ni(OH)₂. The role of the applied potential in this mechanismmore »« less
https://doi.org/10.1021/jacsau.2c00150

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Title: Determination of the “NiOOH” charge and discharge mechanisms at ideal activity

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Citation Formats

Environmentally Friendly Nickel-Zinc Battery for High Rate Application with Higher Specific Energy journal, August 2009

Electrochemical and Spectroscopic Evidence on the Participation of Quadrivalent Nickel in the Nickel Hydroxide Redox Reaction journal, January 1989

Characterization of Redox States of Nickel Hydroxide Film Electrodes by In Situ Surface Raman Spectroscopy journal, January 1988

In situ extended x‐ray absorption fine structure spectroscopy of thin‐film nickel hydroxide electrodes journal, February 1991

Dynamic EXAFS study of discharging nickel hydroxide electrode with non-integer Ni valency journal, July 2001

X-Ray Absorption Fine Structure Spectra and the Oxidation State of Nickel in Some of Its Oxycompounds journal, January 1994

In Situ X-Ray Absorption Near-Edge Structure Evidence for Quadrivalent Nickel in Nickel Battery Electrodes journal, January 1996

In situ X-ray absorption fine structure and optical reflectance studies of electrodeposited nickel hydrous oxide films in alkaline electrolytes journal, November 1997

Quantitative Interpretation of K-Edge NEXAFS Data for Various Nickel Hydroxides and the Charged Nickel Electrode journal, November 1997

Electronic State of Nickel in Barium Nickel Oxide, BaNiO 3 journal, April 1998

Non-cooperative Jahn-Teller effect in LiNiO2: An EXAFS study journal, April 1995

Ab initio study of lithium intercalation in metal oxides and metal dichalcogenides journal, July 1997

Electronic structure of Li-doped NiO journal, January 1992

Various aspects of LiNiO 2 chemistry: A review journal, January 2005

X-ray photoelectron spectroscopic chemical state quantification of mixed nickel metal, oxide and hydroxide systems journal, April 2009

New interpretations of XPS spectra of nickel metal and oxides journal, May 2006

Voltammetric and XPS investigations of nickel hydroxide electrochemically dispersed on gold surface electrodes journal, February 1999

Dissolution and passivation of nickel. An X-ray photoelectron spectroscopic study journal, January 1977

Electronic Structure of Lithium Nickel Oxides by Electron Energy Loss Spectroscopy journal, June 2005

Changes in Chemical Bondings by Li Deintercalation in LiMO 2 (M=Cr, V, Co and Ni) journal, April 1999

Changes in electronic structure by Li ion deintercalation in LiNiO2 from nickel L-edge and O K-edge XANES journal, July 2001

White lines and d -band occupancy for the 3 d transition-metal oxides and lithium transition-metal oxides journal, June 2004

Character of Holes in Li x Ni 1 − x O and Their Magnetic Behavior journal, January 1989

Orbital Frustration at the Origin of the Magnetic Behavior in LiNiO 2 journal, April 2001

Surface properties of LiCoO2, LiNiO2 and LiNi1−xCoxO2 journal, March 2007

Charge disproportionation and Jahn-Teller distortion in LiNiO 2 and NaNiO 2 : A density functional theory study journal, August 2011

The mechanism of electrodeposition and operation of Ni(OH)2 layers journal, July 1996

Nickel hydroxide electrodeposition from nickel nitrate solutions: mechanistic studies journal, February 2001

The Effect of Current and Nickel Nitrate Concentration on the Deposition of Nickel Hydroxide Films journal, April 1995

First principles reaction modeling of the electrochemical interface: Consideration and calculation of a tunable surface potential from atomic and electronic structure journal, April 2006

Effect of Ions on the Structure of Water: Structure Making and Breaking journal, March 2009

Effects of Deposition Potential and Anneal Temperature on the Hexagonal Nanoporous Nickel Hydroxide Films journal, July 2007

Electrochemical precipitation of nickel hydroxide journal, November 2002

Efficient electrochromic nickel oxide thin films by electrodeposition journal, January 2010

Synthesis and Electrochemical Investigations of Ni[sub 1−x]O Thin Films and Ni[sub 1−x]O on Three-Dimensional Carbon Substrates for Electrochemical Capacitors journal, January 2005

Metal Oxide Catalysts for the Evolution of O 2 from H 2 O journal, March 2008

Three-dimensional bicontinuous ultrafast-charge and -discharge bulk battery electrodes journal, March 2011

Ni(OH) 2 Nanoplates Grown on Graphene as Advanced Electrochemical Pseudocapacitor Materials journal, June 2010

In Situ Raman Studies on Cathodically Deposited Nickel Hydroxide Films and Electroless Ni−P Electrodes in 1 M KOH Solution journal, February 1998

Spatial resolution of redox processes within nickel oxide films on gold using real-time surface-enhanced Raman spectroscopy journal, May 1989

X-ray diffraction and micro-Raman spectroscopy analysis of new nickel hydroxide obtained by electrodialysis journal, April 2000

In Situ Laser Raman Spectroscopic Study of Anodic Corrosion Films on Nickel and Cobalt journal, January 1984

In situ Raman Spectroscopy Study of the Nickel Oxyhydroxide Electrode (NOE) System journal, January 1990

Review of the structure and the electrochemistry of nickel hydroxides and oxy-hydroxides journal, January 1982

Angle-resolved infrared spectroelectrochemistry. 1. An in situ study of thin-film nickel oxide electrodes journal, January 1989

Extended x-ray absorption fine structure investigations of nickel hydroxides journal, January 1990

Electrochemical and In Situ Raman Spectroscopic Characterization of Nickel Hydroxide Electrodes journal, January 1997

Structural models for nickel electrode active mass journal, March 1988

Electrochemical behaviour of the β(II)-Ni(OH)2/β(III)-NiOOH redox couple upon potentiodynamic cycling conditions journal, July 2006

In Situ Raman Study of Nickel Oxide and Gold-Supported Nickel Oxide Catalysts for the Electrochemical Evolution of Oxygen journal, April 2012

Photoelectrochemistry of Nickel Hydroxide Thin Films journal, January 1989

Redox behavior of the nickel oxide electrode system: quartz crystal microbalance studies journal, January 1997

Osmotic Coefficients and Mean Activity Coefficients of Uni‐univalent Electrolytes in Water at 25°C journal, October 1972

Proton Intercalation Hysteresis in Charging and Discharging Nickel Hydroxide Electrodes journal, August 1999

In situ time-resolved x-ray absorption near edge structure study of the nickel oxide electrode journal, August 1989

Methods for investigation of ionic reactions in aqueous solutions with half-times as short as 10 –9 sec. Application to neutralization and hydrolysis reactions journal, January 1954

Cyclic voltammetric studies of the effects of time and temperature on the capacitance of electrochemically deposited nickel hydroxide journal, January 2001

Preparation of hexagonal nanoporous nickel hydroxide film and its application for electrochemical capacitor journal, May 2007

A Study of the Preparation of NiO[sub x] Electrode via Electrochemical Route for Supercapacitor Applications and Their Charge Storage Mechanism journal, January 2002

Synthesis of porous NiO nanocrystals with controllable surface area and their application as supercapacitor electrodes journal, September 2010

Metal Oxide and Hydroxide–Based Aqueous Supercapacitors: From Charge Storage Mechanisms and Functional Electrode Engineering to Need‐Tailored Devices journal, February 2019

NiFe-Based (Oxy)hydroxide Catalysts for Oxygen Evolution Reaction in Non-Acidic Electrolytes journal, July 2016

Oxygen Isotope Labeling Experiments Reveal Different Reaction Sites for the Oxygen Evolution Reaction on Nickel and Nickel Iron Oxides journal, June 2019

Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations journal, July 2019

Oxygen Isotope Labeling Experiments Reveal Different Reaction Sites for the Oxygen Evolution Reaction on Nickel and Nickel Iron Oxides journal, July 2019

Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations journal, July 2019

Ternary Ni-Co-Fe oxyhydroxide oxygen evolution catalysts: Intrinsic activity trends, electrical conductivity, and electronic band structure journal, April 2019

Spectroelectrochemical study of water oxidation on nickel and iron oxyhydroxide electrocatalysts journal, November 2019

Monitoring compositional changes in Ni(OH) 2 electrocatalysts employed in the oxygen evolution reaction journal, January 2019

A nanostructured nickel/carbon matrix as an efficient oxygen evolution reaction electrocatalyst for rechargeable zinc–air batteries journal, January 2019

Influence of iron doping on tetravalent nickel content in catalytic oxygen evolving films journal, January 2017

Characterization of NiFe oxyhydroxide electrocatalysts by integrated electronic structure calculations and spectroelectrochemistry journal, March 2017

Nickel-iron catalysts for electrochemical water oxidation – redox synergism investigated by in situ X-ray spectroscopy with millisecond time resolution text, January 2018

Environmentally Friendly Nickel-Zinc Battery for High Rate Application with Higher Specific Energy
journal, August 2009

Electrochemical and Spectroscopic Evidence on the Participation of Quadrivalent Nickel in the Nickel Hydroxide Redox Reaction
journal, January 1989

Characterization of Redox States of Nickel Hydroxide Film Electrodes by In Situ Surface Raman Spectroscopy
journal, January 1988

In situ extended x‐ray absorption fine structure spectroscopy of thin‐film nickel hydroxide electrodes
journal, February 1991

Dynamic EXAFS study of discharging nickel hydroxide electrode with non-integer Ni valency
journal, July 2001

X-Ray Absorption Fine Structure Spectra and the Oxidation State of Nickel in Some of Its Oxycompounds
journal, January 1994

In Situ X-Ray Absorption Near-Edge Structure Evidence for Quadrivalent Nickel in Nickel Battery Electrodes
journal, January 1996

In situ X-ray absorption fine structure and optical reflectance studies of electrodeposited nickel hydrous oxide films in alkaline electrolytes
journal, November 1997

Quantitative Interpretation of K-Edge NEXAFS Data for Various Nickel Hydroxides and the Charged Nickel Electrode
journal, November 1997

Electronic State of Nickel in Barium Nickel Oxide, BaNiO ₃
journal, April 1998

Non-cooperative Jahn-Teller effect in LiNiO2: An EXAFS study
journal, April 1995

Ab initio study of lithium intercalation in metal oxides and metal dichalcogenides
journal, July 1997

Electronic structure of Li-doped NiO
journal, January 1992

Various aspects of LiNiO ₂ chemistry: A review
journal, January 2005

X-ray photoelectron spectroscopic chemical state quantification of mixed nickel metal, oxide and hydroxide systems
journal, April 2009

New interpretations of XPS spectra of nickel metal and oxides
journal, May 2006

Voltammetric and XPS investigations of nickel hydroxide electrochemically dispersed on gold surface electrodes
journal, February 1999

Dissolution and passivation of nickel. An X-ray photoelectron spectroscopic study
journal, January 1977

Electronic Structure of Lithium Nickel Oxides by Electron Energy Loss Spectroscopy
journal, June 2005

Changes in Chemical Bondings by Li Deintercalation in LiMO ₂ (M=Cr, V, Co and Ni)
journal, April 1999

Changes in electronic structure by Li ion deintercalation in LiNiO2 from nickel L-edge and O K-edge XANES
journal, July 2001

White lines and $d$ -band occupancy for the $3 d$ transition-metal oxides and lithium transition-metal oxides
journal, June 2004

Character of Holes in ${Li}_{x} {Ni}_{1 - x} O$ and Their Magnetic Behavior
journal, January 1989

Orbital Frustration at the Origin of the Magnetic Behavior in ${LiNiO}_{2}$
journal, April 2001

Surface properties of LiCoO2, LiNiO2 and LiNi1−xCoxO2
journal, March 2007

Charge disproportionation and Jahn-Teller distortion in LiNiO $_{2}$ and NaNiO $_{2}$ : A density functional theory study
journal, August 2011

The mechanism of electrodeposition and operation of Ni(OH)2 layers
journal, July 1996

Nickel hydroxide electrodeposition from nickel nitrate solutions: mechanistic studies
journal, February 2001

The Effect of Current and Nickel Nitrate Concentration on the Deposition of Nickel Hydroxide Films
journal, April 1995

First principles reaction modeling of the electrochemical interface: Consideration and calculation of a tunable surface potential from atomic and electronic structure
journal, April 2006

Effect of Ions on the Structure of Water: Structure Making and Breaking
journal, March 2009

Effects of Deposition Potential and Anneal Temperature on the Hexagonal Nanoporous Nickel Hydroxide Films
journal, July 2007

Electrochemical precipitation of nickel hydroxide
journal, November 2002

Efficient electrochromic nickel oxide thin films by electrodeposition
journal, January 2010

Synthesis and Electrochemical Investigations of Ni[sub 1−x]O Thin Films and Ni[sub 1−x]O on Three-Dimensional Carbon Substrates for Electrochemical Capacitors
journal, January 2005

Metal Oxide Catalysts for the Evolution of O ₂ from H ₂ O
journal, March 2008

Three-dimensional bicontinuous ultrafast-charge and -discharge bulk battery electrodes
journal, March 2011

Ni(OH) ₂ Nanoplates Grown on Graphene as Advanced Electrochemical Pseudocapacitor Materials
journal, June 2010

In Situ Raman Studies on Cathodically Deposited Nickel Hydroxide Films and Electroless Ni−P Electrodes in 1 M KOH Solution
journal, February 1998

Spatial resolution of redox processes within nickel oxide films on gold using real-time surface-enhanced Raman spectroscopy
journal, May 1989

X-ray diffraction and micro-Raman spectroscopy analysis of new nickel hydroxide obtained by electrodialysis
journal, April 2000

In Situ Laser Raman Spectroscopic Study of Anodic Corrosion Films on Nickel and Cobalt
journal, January 1984

In situ Raman Spectroscopy Study of the Nickel Oxyhydroxide Electrode (NOE) System
journal, January 1990

Review of the structure and the electrochemistry of nickel hydroxides and oxy-hydroxides
journal, January 1982

Angle-resolved infrared spectroelectrochemistry. 1. An in situ study of thin-film nickel oxide electrodes
journal, January 1989

Extended x-ray absorption fine structure investigations of nickel hydroxides
journal, January 1990

Electrochemical and In Situ Raman Spectroscopic Characterization of Nickel Hydroxide Electrodes
journal, January 1997

Structural models for nickel electrode active mass
journal, March 1988

Electrochemical behaviour of the β(II)-Ni(OH)2/β(III)-NiOOH redox couple upon potentiodynamic cycling conditions
journal, July 2006

In Situ Raman Study of Nickel Oxide and Gold-Supported Nickel Oxide Catalysts for the Electrochemical Evolution of Oxygen
journal, April 2012

Photoelectrochemistry of Nickel Hydroxide Thin Films
journal, January 1989

Redox behavior of the nickel oxide electrode system: quartz crystal microbalance studies
journal, January 1997

Osmotic Coefficients and Mean Activity Coefficients of Uni‐univalent Electrolytes in Water at 25°C
journal, October 1972

Proton Intercalation Hysteresis in Charging and Discharging Nickel Hydroxide Electrodes
journal, August 1999

In situ time-resolved x-ray absorption near edge structure study of the nickel oxide electrode
journal, August 1989

Methods for investigation of ionic reactions in aqueous solutions with half-times as short as 10 ^–9 sec. Application to neutralization and hydrolysis reactions
journal, January 1954

Cyclic voltammetric studies of the effects of time and temperature on the capacitance of electrochemically deposited nickel hydroxide
journal, January 2001

Preparation of hexagonal nanoporous nickel hydroxide film and its application for electrochemical capacitor
journal, May 2007

A Study of the Preparation of NiO[sub x] Electrode via Electrochemical Route for Supercapacitor Applications and Their Charge Storage Mechanism
journal, January 2002

Synthesis of porous NiO nanocrystals with controllable surface area and their application as supercapacitor electrodes
journal, September 2010

Metal Oxide and Hydroxide–Based Aqueous Supercapacitors: From Charge Storage Mechanisms and Functional Electrode Engineering to Need‐Tailored Devices
journal, February 2019

NiFe-Based (Oxy)hydroxide Catalysts for Oxygen Evolution Reaction in Non-Acidic Electrolytes
journal, July 2016

Oxygen Isotope Labeling Experiments Reveal Different Reaction Sites for the Oxygen Evolution Reaction on Nickel and Nickel Iron Oxides
journal, June 2019

Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations
journal, July 2019

Oxygen Isotope Labeling Experiments Reveal Different Reaction Sites for the Oxygen Evolution Reaction on Nickel and Nickel Iron Oxides
journal, July 2019

Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations
journal, July 2019

Ternary Ni-Co-Fe oxyhydroxide oxygen evolution catalysts: Intrinsic activity trends, electrical conductivity, and electronic band structure
journal, April 2019

Spectroelectrochemical study of water oxidation on nickel and iron oxyhydroxide electrocatalysts
journal, November 2019

Monitoring compositional changes in Ni(OH) ₂ electrocatalysts employed in the oxygen evolution reaction
journal, January 2019

A nanostructured nickel/carbon matrix as an efficient oxygen evolution reaction electrocatalyst for rechargeable zinc–air batteries
journal, January 2019

Influence of iron doping on tetravalent nickel content in catalytic oxygen evolving films
journal, January 2017

Characterization of NiFe oxyhydroxide electrocatalysts by integrated electronic structure calculations and spectroelectrochemistry
journal, March 2017

Nickel-iron catalysts for electrochemical water oxidation – redox synergism investigated by in situ X-ray spectroscopy with millisecond time resolution
text, January 2018