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Phase formation capability and compositional design of β-phase multiple rare-earth principal component disilicates.

ABSTRACT: A key strategy to design environmental barrier coatings focuses on doping multiple rare-earth principal components into β-type rare-earth disilicates (RE₂Si₂O₇) to achieve versatile property optimization. However, controlling the phase formation capability of (nRE_xi)₂Si₂O₇ remains a crucial challenge, due to the complex polymorphic phase competitions and evolutions led by different RE³⁺ combination. Herein, by fabricating twenty-one model (RE^I_0.25RE^II_0.25RE^III_0.25RE^IV_0.25)₂Si₂O₇ compounds, we find that their formation capability can be evaluated by the ability to accommodate configurational randomness of multiple RE³⁺ cations in β-type lattice while preventing the β-to-γ polymorphic transformation. The phase formation and stabilization are controlled by the average RE³⁺ radius and the deviations of different RE³⁺ combinations. Subsequently, based on high-throughput density-functional-theory calculations, we propose that the configurational entropy of mixing is a reliable descriptor to predict the phase formation of β-type (nRE_xi)₂Si₂O₇. The results may accelerate the design of (nRE_xi)₂Si₂O₇ materials with tailored compositions and controlled polymorphic phases.

SUBMITTER: Luo Y

PROVIDER: S-EPMC9992687 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

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Phase formation capability and compositional design of β-phase multiple rare-earth principal component disilicates.

Luo Yixiu Y Sun Luchao L Wang Jiemin J Du Tiefeng T Zhou Cui C Zhang Jie J Wang Jingyang J

Nature communications 20230308 1

A key strategy to design environmental barrier coatings focuses on doping multiple rare-earth principal components into β-type rare-earth disilicates (RE2Si2O7) to achieve versatile property optimization. However, controlling the phase formation capability of (nRExi)2Si2O7 remains a crucial challenge, due to the complex polymorphic phase competitions and evolutions led by different RE3+ combination. Herein, b ...[more]

PMID: 36882392

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Project description:The rational design of catalysts remains a challenging endeavor within the broader chemical community owing to the myriad variables that can affect key bond-forming events. Designing selective catalysts for any reaction requires an efficient strategy for discovering predictive structure-activity relationships. Herein, we describe the use of iterative supervised principal component analysis (ISPCA) in de novo catalyst design. The regioselective synthesis of 2,5-dimethyl-1,3,4-triphenyl-1H-pyrrole (C) via a Ti-catalyzed formal [2 + 2 +1] cycloaddition of phenylpropyne and azobenzene was targeted as a proof of principle. The initial reaction conditions led to an unselective mixture of all possible pyrrole regioisomers. ISPCA was conducted on a training set of catalysts, and their performance was regressed against the scores from the top three principal components. Component loadings from this PCA space and k-means clustering were used to inform the design of new test catalysts. The selectivity of a prospective test set was predicted in silico using the ISPCA model, and optimal candidates were synthesized and tested experimentally. This data-driven predictive-modeling workflow was iterated, and after only three generations the catalytic selectivity was improved from 0.5 (statistical mixture of products) to over 11 (>90% C) by incorporating 2,6-dimethyl-4-(pyrrolidin-1-yl)pyridine as a ligand. The origin of catalyst selectivity was probed by examining ISPCA variable loadings in combination with DFT modeling, revealing that ligand lability plays an important role in selectivity. A parallel catalyst search using multivariate linear regression (MLR), a popular approach in catalysis informatics, was also conducted in order to compare these strategies in a hypothetical catalyst scouting campaign. ISPCA appears to be more robust and predictive than MLR when sparse training sets are used that are representative of the data available during the early search for an optimal catalyst. The successful development of a highly selective catalyst without resorting to long, stochastic screening processes demonstrates the inherent power of ISPCA in de novo catalyst design and should motivate the general use of ISPCA in reaction development.

Dataset Information

Phase formation capability and compositional design of β-phase multiple rare-earth principal component disilicates.

Publications

Phase formation capability and compositional design of β-phase multiple rare-earth principal component disilicates.

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