Lithium Metal-Gas Reactions.

Markowitz, Meyer M.; Boryta, Daniel A.

doi:10.1021/je60015a047

Cited by 57 publications

(66 citation statements)

References 10 publications

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“…Consequently, Li is no longer obstructed by the SEI layer, leading to enhanced nitridation, as evidenced by increased NH 3 production with increasing temperatures (Figure a). The abrupt increase in NH 3 above 180 °C agrees well with previous TGA data regarding Li under an N 2 atmosphere, and is reasonable given the melting point of metallic Li (180.5 °C) . However, additional side reactions likely occur between residual PC and unprotected Li after SEI decomposition at elevated temperatures (>100 °C), resulting in the formation of more Li 2 CO 3 .…”

Section: Methodssupporting

confidence: 55%

Electrochemical Synthesis of Ammonia from Water and Nitrogen: A Lithium‐Mediated Approach Using Lithium‐Ion Conducting Glass Ceramics

et al. 2017

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Lithium-mediated reduction of dinitrogen is ap romising methodt oe vade electron-stealing hydrogen evolution, ac ritical challenge which limits faradaic efficiency (FE) and thus hinders the success of traditional protic-solvent-based ammonia electro-synthesis. Av iable implementation of the lithium-mediated pathway using lithium-ion conducting glass ceramics involves i) lithium deposition, ii)nitridation,a nd iii)ammonia formation. Ammonia was successfully synthesized from molecular nitrogen and water,y ielding am aximum FE of 52.3 %. Witha n ammonia synthesis rate comparable to previously reported approaches, the fairly high FE demonstrates the possibility of using this nitrogen fixation strategya sasubstitute for firmly established, yet exceedingly complicated and expensivet echnology,a nd in so doing represents an ext-generation energy storagesystem.The Haber-Bosch process is aw ell-established ammonia (NH 3 ) synthesis technology that converts more than 120 million tons of N 2 into NH 3 annually. [1,2] However,this process is exceedingly energy intensiveo wing to harsh operating conditions, and exhibits extensive carbon emission. [1] Therefore, the development of more environmentally benign alternatives is crucial.Electrochemical synthesisi sa na ttractive candidatef or N 2 fixation ase nergy consumption, if optimized (i.e. with low overvoltage and high faradaic efficiency), could potentially be reduced as compared to the Haber-Bosch process while avoiding CO 2 emission. [3,4] If the required electricity for the process is supplied from renewable sources, this approach offers a meanstostore excess renewable energy in agreen energy carrier with an energy density comparable to fossil fuels. [5] True sustainability,h owever,w ill only be realized if the electrons required for the N 2 reduction originate from water rather than H 2 .Over the last three decades, such electrochemical processes have been developed, with state-of-the art technologiess ummarized in Ta ble S1 in the Supporting Information. [6][7][8][9][10][11][12][13][14][15][16] Unfortunately,t he faradaic efficiencies (FEs) in most cases were unbearably low (< 5%)a st he competing hydrogen evolution from water or ap rotonw as preferred over the intended N 2 reduction, which was particularly sluggish owing to the strong triple bond of N 2 (941 kJ mol À1 ). [3,17,18] Innovative strategies are thus indispensable to overcome such obstacles and achieve excellent selectivity in the N 2 reduction.One promisingw ay is to employ Li as amediator in the electro-synthesis. In contact with N 2 ,m etallicL i, on accounto fi ts strong reducing power,c auses dissociation to form lithium nitride (Li 3 N) even under ambient conditions. Thus-formed Li 3 N is ah igh-energyi ntermediate for NH 3 synthesis that is readily transformed into NH 3 upon reaction with protons or water. [17] This so-called "Li-mediated pathway" was firstly applied to synthesizing NH 3 in studies by Ts unetoe tal.,w hich reported an impressively high maximum FE of 59 %a t5 0atm of N 2 (1 atm = 0....

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Section: Methodssupporting

confidence: 55%

Electrochemical Synthesis of Ammonia from Water and Nitrogen: A Lithium‐Mediated Approach Using Lithium‐Ion Conducting Glass Ceramics

et al. 2017

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“…Ar þ -ion sputtering allows to obtain depth profiles and to change the surface composition. The high reactivity of lithium, mentioned above, makes it also possible to change the surface composition by scratching the foil under specific atmosphere [22].…”

Section: Surface Preparationmentioning

confidence: 99%

Challenges for lithium species identification in complementary Auger and X-ray photoelectron spectroscopy

Hoffmann

Zier

Oswald

et al. 2015

Journal of Power Sources

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“…These observations are not in accordance with those of Markowitz and Boryta. [7] They stated that reaction 1 would be the first and the faster one when the metallic lithium is exposed to air. Work is in progress to understand our observation and compare it to results obtained in the past.…”

Section: à3mentioning

confidence: 99%

“…Sputter-evaporation is one of the techniques of choice for plating substrates by physical methods. [6] The deposition of Lithium on any substrate currently faces two major issues: Li diffusion into the substrate and Li reactivity with air according to the following chemical reactions: [7] 6 Li ðsÞ þ N 2ðgÞ ! 2Li 3 (2) Lithium coatings on various substrates have numerous applications: Boron neutron capture therapy, neutron activation analysis, super-conducting tokamak etc.…”

Section: Introductionmentioning

confidence: 99%

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Analyses of Thick Lithium Coatings Deposited by Sputter‐Evaporation and Exposed to Air

Rigaux

Lafort

Bodart

et al. 2009

Plasma Processes & Polymers

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Lithium coatings on various substrates have numerous applications: Boron neutron capture therapy, neutron activation analysis, super‐conducting tokamak etc. Traditionally these coatings are produced by well‐known techniques such as electrochemistry and evaporation. In this work, we investigated a new method based on sputter‐evaporation, which enables thick coatings (>10 µm) to be built on various substrates within a short timeframe. In order to minimize the process time, evaporation techniques can be used but the coating quality suffers. Moreover, it is well known that the use of DC magnetron sputtering results in the deposition of good quality coatings (smoothness, density, adhesion); however, the deposition rate is low. The rationale of this work is to combine these two techniques, yielding a sputter‐evaporation process that possesses the advantages of each separate technique. Li is placed in a stainless steel crucible (cathode), and heated by the plasma generated by a magnetron discharge. The Li temperature is measured by a thermocouple welded onto the cathode and measured at different plasma power densities. The deposition rate of lithium is measured using a quartz balance and by profilometry, at several temperatures (from 0 to 580 °C). Li samples were depth‐profiled with the resonant nuclear reaction 7Li(p,γ)7. In addition to the concentration, certain characteristics like the density and the chemical reactivity of layers, are also important. Thus we have studied the evolution of the density with time, estimated by weight and profilometry measurements, and the change in morphology, by cross‐sectional scanning electron microscopy (SEM), of samples exposed to air at room temperature. The evolution of the film compounds have also been determined by X‐ray powder diffraction. These physical properties have been investigated for various bias substrates during deposition.

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Lithium Metal-Gas Reactions.

Cited by 57 publications

References 10 publications

Electrochemical Synthesis of Ammonia from Water and Nitrogen: A Lithium‐Mediated Approach Using Lithium‐Ion Conducting Glass Ceramics

Electrochemical Synthesis of Ammonia from Water and Nitrogen: A Lithium‐Mediated Approach Using Lithium‐Ion Conducting Glass Ceramics

Challenges for lithium species identification in complementary Auger and X-ray photoelectron spectroscopy

Analyses of Thick Lithium Coatings Deposited by Sputter‐Evaporation and Exposed to Air

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