Novel mixed polyanions lithium-ion battery cathode materials predicted by high-throughput ab initio computations

Hautier, Geoffroy; Jain, Anubhav; Chen, Hailong; Moore, Christopher; Ong, Shyue Ping; Ceder, Gerbrand

doi:10.1039/c1jm12216a

Cited by 210 publications

(207 citation statements)

References 36 publications

(43 reference statements)

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“…Several novel compounds were identified and subsequently synthesized and tested, including a monoclinic form of LiMnBO 3 , 64 layered Li 9 V 3 (P 2 O 7 ) 3 (PO 4 ) 2 , 65 Cr-doped LiVO 2 , 66 and a new class of Li 3 MPO 4 CO 3 (M ¼ transition metal) materials, which are unconventional in that they mix two different polyanion groups (phosphate and carbonate). 67 Building upon the "Materials Project" infrastructure, 68 the Joint Center for Energy Storage (JCESR) launched a highthroughput computational search for multivalent ion intercalation compounds as well as novel electrolyte formulations. Multivalent intercalation cathodes can exhibit very high energy density compared to their Li-ion counterparts, creating the materials innovation challenge of identifying host structures with sufficient ionic mobility.…”

Section: Energy Conversion: Thermoelectricsmentioning

confidence: 99%

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Green

Choi

Hattrick‐Simpers

et al. 2017

Applied Physics Reviews

246

173

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The Materials Genome Initiative, a national effort to introduce new materials into the market faster and at lower cost, has made significant progress in computational simulation and modeling of materials. To build on this progress, a large amount of experimental data for validating these models, and informing more sophisticated ones, will be required. High-throughput experimentation generates large volumes of experimental data using combinatorial materials synthesis and rapid measurement techniques, making it an ideal experimental complement to bring the Materials Genome Initiative vision to fruition. This paper reviews the state-of-the-art results, opportunities, and challenges in high-throughput experimentation for materials design. A major conclusion is that an effort to deploy a federated network of high-throughput experimental (synthesis and characterization) tools, which are integrated with a modern materials data infrastructure, is needed.

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Section: Energy Conversion: Thermoelectricsmentioning

confidence: 99%

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Green

Choi

Hattrick‐Simpers

et al. 2017

Applied Physics Reviews

246

173

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“…[1][2][3][4][5][6][7][8] Reaction energies are also critical to the ab initio study of the thermodynamic stability of known materials [9][10][11][12][13][14] or the prediction of novel phases. [15][16][17][18][19][20][21][22][23][24][25][26][27] Indeed, it is a compound's energy relative to the energy from combinations of other phases, which determines its stability.…”

Section: Introductionmentioning

confidence: 99%

“…These phase diagrams are useful when studying the phase stability of known but also predicted compounds. Several recent studies relied on such phase diagrams to investigate the stability of new proposed phosphates-based compounds for lithium-ion batteries, [20][21][22] new predicted ternary oxides, 18 new iron borides 17 or new intermetallics. 16,26 Zero K phase diagrams based on GGA computations for all compounds in the ICSD are also available online through the Materials Project.…”

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confidence: 99%

Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability

et al. 2012

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The evaluation of reaction energies between solids using density functional theory (DFT) is of practical importance in many technological fields and paramount in the study of the phase stability of known and predicted compounds. In this work, we present a comparison between reaction energies provided by experiments and computed by DFT in the generalized gradient approximation (GGA), using a Hubbard U parameter for some transition metal elements (GGA+U). We use a data set of 135 reactions involving the formation of ternary oxides from binary oxides in a broad range of chemistries and crystal structures. We find that the computational errors can be modeled by a normal distribution with a mean close to zero and a standard deviation of 24 meV/atom. The significantly smaller error compared to the more commonly reported errors in the formation energies from the elements is related to the larger cancellation of errors in energies when reactions involve chemically similar compounds. This result is of importance for phase diagram computations for which the relevant reaction energies are often not from the elements but from chemically close phases (e.g., ternary oxides vs binary oxides). In addition, we discuss the distribution of computational errors among chemistries and show that the use of a Hubbard U parameter is critical to the accuracy of reaction energies involving transition metals even when no major change in formal oxidation state is occurring.

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“…The aforementioned theoretical prediction and experimental investigations 13,[28][29][30] reveal clearly that Na 3 MnCO 3 PO 4 has a potential to be a high capacity cathode material for NIBs. Therefore, in this study, we have investigated factors, other than the electronic conductivity, that can affect the electrochemical properties of Na 3 MnCO 3 PO 4 as the cathode material for NIBs.…”

mentioning

confidence: 99%

“…In this context, Na 3 MnCO 3 PO 4 has been predicted via ab initio calculations 28,29 to be capable of delivering two electron transfer redox reactions per formula and thus has a high theoretical capacity (i.e., 191 mAh/g of Na 3 MnCO 3 PO 4 ). The earlier experiments, however, were only able to obtain a low specific capacity of 125 mAh/g, i.e., ∼65% of the theoretical.13 Recently, our group has shown that high specific capacities, reaching as high as 92% of the theoretical, can be achieved when aided by the addition of 53 wt% (60 vol%) carbon black (CB) which provides a continuous CB network interacting with almost all Na 3 MnCO 3 PO 4 particles in the cathode and allow them to participate in electrochemical reactions. …”

mentioning

confidence: 99%

Roles of Processing, Structural Defects and Ionic Conductivity in the Electrochemical Performance of Na₃MnCO₃PO₄Cathode Material

Wang¹,

Sawicki²,

Kaduk

et al. 2015

J. Electrochem. Soc.

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Na 3 MnCO 3 PO 4 with a potential to deliver two-electron transfer reactions per formula via Mn 2+ /Mn 3+ and Mn 3+ /Mn 4+ redox reactions and a high theoretical capacity (191 mAh/g) can play an important role in Na-ion batteries. This study investigates the dependence of the electrochemical performance of Na 3 MnCO 3 PO 4 -based sodium-ion batteries on processing, structural defects and ionic conductivity. Na 3 MnCO 3 PO 4 has been synthesized via hydrothermal process under various conditions with and without subsequent high-energy ball milling. Particle sizes, structural defects and ionic conductivity have been studied as a function of processing conditions. It is found that Na 3 MnCO 3 PO 4 nanoparticles (20 nm in diameter) can be produced from hydrothermal synthesis, but the reaction time is critical in obtaining nanoparticles. Nanoparticles exhibit a higher ionic conductivity than agglomerated particles. Further, structural defects also have a strong influence on ionic conductivity which, in turn, affects the charge/discharge capacities of the Na 3 MnCO 3 PO 4 -based sodium-ion batteries. These results provide guidelines for rational design and synthesis of high capacity Na 3 MnCO 3 PO 4 for Na-ion batteries in the near future. High power and high energy density rechargeable batteries with long cycle life and low cost are in urgent demand for electric vehicles and large-scale energy storage devices. [1][2][3][4] In light of these emerging demands, interest in Na-ion batteries (NIBs) has increased recently because of the abundance and low cost of Na metal. Although NIBs have the cost advantage over Li-ion batteries (LIBs), it is generally agreed that the gravimetric and volumetric energy densities of NIBs cannot compete with that of LIBs because of two intrinsic shortcomings. First, Li has a higher ionization potential than Na.15 Second, Li + ions are smaller and lighter than Na + ions. 15 One way to mitigate these intrinsic deficiencies is to search for high capacity anodes and cathodes. In this context, Na 3 MnCO 3 PO 4 has been predicted via ab initio calculations 28,29 to be capable of delivering two electron transfer redox reactions per formula and thus has a high theoretical capacity (i.e., 191 mAh/g of Na 3 MnCO 3 PO 4 ). The earlier experiments, however, were only able to obtain a low specific capacity of 125 mAh/g, i.e., ∼65% of the theoretical.13 Recently, our group has shown that high specific capacities, reaching as high as 92% of the theoretical, can be achieved when aided by the addition of 53 wt% (60 vol%) carbon black (CB) which provides a continuous CB network interacting with almost all Na 3 MnCO 3 PO 4 particles in the cathode and allow them to participate in electrochemical reactions. 30The aforementioned theoretical prediction and experimental investigations 13,[28][29][30] reveal clearly that Na 3 MnCO 3 PO 4 has a potential to be a high capacity cathode material for NIBs. Therefore, in this study, we have investigated factors, other than the electronic conductivity, that can affect t...

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Novel mixed polyanions lithium-ion battery cathode materials predicted by high-throughput ab initio computations

Cited by 210 publications

References 36 publications

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability

Roles of Processing, Structural Defects and Ionic Conductivity in the Electrochemical Performance of Na₃MnCO₃PO₄Cathode Material

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Novel mixed polyanions lithium-ion battery cathode materials predicted by high-throughput ab initio computations

Cited by 210 publications

References 36 publications

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies

Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability

Roles of Processing, Structural Defects and Ionic Conductivity in the Electrochemical Performance of Na3MnCO3PO4Cathode Material

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Roles of Processing, Structural Defects and Ionic Conductivity in the Electrochemical Performance of Na₃MnCO₃PO₄Cathode Material