Bulletin of the American Physical Society
APS March Meeting 2022
Volume 67, Number 3
Monday–Friday, March 14–18, 2022; Chicago
Session K47: Computational Design and Discovery of Novel Materials IVFocus Recordings Available
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Sponsoring Units: DCOMP DMP Chair: Christie Chiu, Princeton University Room: McCormick Place W-470B |
Tuesday, March 15, 2022 3:00PM - 3:12PM |
K47.00001: Guided design of alloys, strengthened via precipitation Nikolai A Zarkevich Using theoretical and computational guidance, we are designing stronger middle and high-entropy alloys and superalloys for the airspace applications. We focus on improving mechanical properties of materials at cryogenic and elevated temperatures. Here we discuss basic science and fundamental theory that are being used for guided design of next-generation alloys. As examples, we consider the medium-entropy NiCoCr alloy and precipitated superalloys with a local phase transformation strengthening. |
Tuesday, March 15, 2022 3:12PM - 3:24PM |
K47.00002: Towards Accurate and Efficient Predictions of Martensitic Transition Temperatures for Shape Memory Alloys from First Principles Zhigang Wu, Hessam Malmir, John Lawson Recent rapid progresses in physics theory and computational power have made it possible to predict the martensitic transition temperatures (MTTs) in shape memory alloys (SMAs) from first principles. In particular, rigorous while time-consuming thermodynamic integration has been employed to compute the anharmonic phonon free energies, which play a crucial role in determining martensitic phase transitions in SMAs. However, this approach has only been applied to simple binaries, and its accuracy is unsatisfying for certain SMAs such as the most commonly used NiTi. In this work, we report on several new developments to our method that bring first-principles theory and experiment much closer into agreement including the MTT of NiTi, and that improve the computational efficiency significantly. We have applied our refined approach to investigate the Ni0.5Ti0.5-xHfx and PdxNi0.5-xTi0.5 ternaries, and the predicted MTT for each composition is within 100K compared with experiment. We will address various techniques to overcome the difficulty encountered in studying ternaries. Our theoretical approach is expected to be a broadly applicable and predictive theory for designing complex SMAs with desirable properties. |
Tuesday, March 15, 2022 3:24PM - 3:36PM |
K47.00003: Electronic analysis of sigma phase destabilization in a family of compositionally complex ferritic stainless steel substitutes. Anna Soper, Savanah Diaz, Holly Frank, Jonas Kaufman, Adam Shaw, Kevin Laws, Lori Bassman, Aurora Pribram-Jones Stainless steels are used extensively in industry due to a combination of desirable material properties, such as corrosion resistance and strength. However, ferritic stainless steels form a brittle sigma phase at moderately high processing temperatures, which limits their utility. Recent experimental results from our group found that small amounts of Al in the presence of Mn suppress the formation of the Fe-Cr sigma phase, leaving the desired ductile, body centered cubic phase. This first principles work uses the Crystal Orbital Hamilton Population method to explore the hypothesis that Al destabilizes sigma geometry by changing the electron distribution among the crystal's molecular orbitals. In order to create representative structures for this analysis, we combine a generalized cluster expansion with Monte Carlo simulations to determine the preferential placement of atomic species on each of the five symmetrically distinct lattice sites of the sigma crystal structure. Because the sigma phase is too complex for its energy to be cluster expanded using conventional automated fitting procedures, we implement an iterative method to efficiently select fitting structures that span the composition space of the alloy system. Beyond creating a model to assess the mechanisms for sigma phase destabilization in Fe-Cr-Mn-Al structures, this work pushes the limits on the size and complexity of metallic systems that have been modeled using cluster expansions. |
Tuesday, March 15, 2022 3:36PM - 3:48PM |
K47.00004: Role of alloying on tunability of martensitic phase transformation in multi-principal element alloys Prashant Singh, Sezer Picak, Aayush Sharma, YI Chumlyakov, Raymundo Arroyave, Ibrahim Karaman, Duane D Johnson Multi-principal element alloys (MPEAs) are an intriguing class of materials where structure and property relations can be controlled via chemical disorder. Employing density-functional theory, we tuned free energies between f.c.c. and h.c.p. phases using disorder in Fe-Mn-Co-Cr based MPEAs to show that free-energy difference and stacking-fault energy directly correlates with martensitic phase transformation and chemical short-range order. The prediction of possible martensitic transformation at specific Fe composition, i.e., x=40at.% in FexMn80-xCo10Cr10, offers an understanding of electronic level physics driving transformation-induced plasticity. This also establishes the relevance of theory-guided design for the next-generation alloys with superior structure-property correlation and provides unique insights for controlling phase transformation in technologically relevant alloys. |
Tuesday, March 15, 2022 3:48PM - 4:00PM |
K47.00005: Mechanisms of CO2and H2O co-adsorption in pyrazine-linked hybrid ultramicroporous materials Saif Ullah, Kui Tan, Timo Thonhauser Sorption-based carbon-separation applications using porous materials are often severely limited by the inevitable presence of water, thus greatly affecting their performance. An entirely unexpected breakthrough has been achieved with ultramicroporous materials. There are very few materials that can perform well in the presence of water and the MFSIX-3 series (M=Ti or Si) is leading this class of materials and has become the new benchmark for CO2 capture. Despite this exciting development, the mechanisms by which MFSIX-3 is capable to retain its excellent performance in the presence of water remain unknown. Herein, we combine in situ infrared spectroscopy with ab initio calculations to provide insights into the co-adsorption of H2O and CO2 in prototypal pyrazine-linked HUMs. An in-depth study of binding sites and sorption mechanisms reveal the following: (i) conclusive experimental evidence that both CO2 and H2O molecules occupy the same pore; (ii) synergistic sorbate-sorbent interactions that enable co-adsorption in such a narrow ultramicropore; and (iii) the beneficial effects induced by higher humidity. Our results provide bottom-up design principlesto custom-design their pore size/chemistry and allow for new carbon capture benchmarks, even in the presence of humidity. |
Tuesday, March 15, 2022 4:00PM - 4:12PM |
K47.00006: Tuning molecular adsorption in metal-organic frameworks through coadsorption and temperature-dependent diffusion barriers Timo Thonhauser, Saif Ullah, Eric Chapman, Kui Tan We report a novel strategy to increase the gas adsorption selectivity of metal organic frameworks (MOFs) by coadsorbing other molecules. Specifically, we find that addition of tightly bound NH3 molecules in MOF-74 dramatically alters its adsorption behavior of C2H2 and C2H4. Combining in situ infrared spectroscopy and ab initio calculations, we find that—as a result of coadsorbed NH3 molecules attaching to the open metal sites—C2H2 binds more strongly and diffuses much faster than C2H4. Most remarkably, C2H4 is now almost completely excluded from entering the MOF once C2H2 has been loaded. This finding suggests a new route to tune the adsorption behavior of MOFs through harnessing the interactions among coadsorbed guests. Furthermore, in the same MOF, we report a temperature-induced variation in a capping-layer gate-opening mechanism through a combination of in situ infared experiments and ab initio simulations of the capping layer. An atypical acceleration and increase in the loading of adsorbed molecules upon raising the temperature above room temperature is observed. This finding shows the discovery of novel temperature-dependent kinetics that goes beyond standard kinetics and suggest a new avenue for tailoring selective adsorption by thermally tuning the surface barrier. |
Tuesday, March 15, 2022 4:12PM - 4:24PM |
K47.00007: Impact of defects and charge doping on O2 binding in the metal-organic framework Fe2(bdp)3 from first principles Alex Smith, Kaitlyn Engler, Kennedy McCone, Lena Funke, Jeffrey Long, Jeffrey B Neaton Fe2(bdp)3 (bdp = benzene-1,4-dipyrazolate) is a metal-organic framework with delocalized electrons along iron-pyrazolate chains whose conductivity and electronic structure are greatly affected by electron doping via alkali metals including Li, Na, and K. Its tunability makes it a candidate material for O2 separations, but outstanding questions regarding the influence of defect anions in place of the bdp ligand and regarding the localization of charge upon doping the material hinder an understanding of how O2 binding can be tuned to yield ideal O2 separations performance. We perform first principles density functional theory calculations on MxFe2(bdp)3 with M = {Li, Na, K} with and without linker defects to study structural, electronic, and magnetic changes due to charge doping and defects. We study the impact of these changes on O2 binding energies with an aim toward understanding which material properties affect O2 binding the most. Our calculations are compared with results from experimental NMR and binding enthalpy studies of the material to facilitate an understanding of O2 binding in the material upon doping and in the presence of defects. |
Tuesday, March 15, 2022 4:24PM - 4:36PM |
K47.00008: Defect Termination in the UiO-66 Family of Metal–Organic Frameworks: The Role of Water and Modulator Haardik Pandey, Kui Tan, Timo Thonhauser The emergence of superior water stable Zr-based metal-organic framework UiO-66 represents a breakthrough in MOF chemistry for practical applications. However, ever since the structure was first reported in 2008 (J. Am. Chem. Soc. 2008, 130, 13850), it has often been observed that a notable concentration of defects are present in UiO-66 samples. The defect concentration can be well controlled during synthesis, leading to highly tunable properties for this structure. However, there has been a long-standing debate regarding the nature of the compensating species present at the defective sites. Here, we present unambiguous evidence that the missing-linker defect sites in an ambient environment are compensated with both carboxylate and water (bound through intermolecular H-bonding), which is further supported by ab initio calculations. In contrast to the prevailing assumption that the monocarboxylate groups (COO−) of the modulators form bidentate bonding with two Zr4+ sites, COO− is found to coordinate to an open Zr4+ site in a unidentate mode. The neighboring Zr4+ site is terminated by a coordinating H2O molecule, which helps to stabilize the COO− group. This finding provides a new understanding of defect termination in UiO-66, and sheds light on the origin of its catalytic activity. |
Tuesday, March 15, 2022 4:36PM - 5:12PM |
K47.00009: Data-driven materials discovery for the solar production of hydrogen Invited Speaker: Ismaila Dabo
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Tuesday, March 15, 2022 5:12PM - 5:24PM |
K47.00010: AI-driven study of carbon-dioxide activation on semiconductor oxides. Aliaksei Mazheika, Yanggang Wang, Rosendo Valero, Francesc Viñes, Francesc Illas, Luca M Ghiringhelli, Sergey V Levchenko, Matthias Scheffler We have developed a strategy for a rational design of catalytic materials using subgroup discovery (SGD) – an artificial-intelligence method that identifies statistically exceptional subgroups in a dataset. With that, we identify features of catalyst materials (“catalysts’ genes”) that correlate with mechanisms promoting or hindering the activation of carbon dioxide (CO2), towards a chemical conversion of CO2 to fuels or other useful chemicals. Our training set consists of high-throughput first-principles calculations of CO2 adsorption on the surfaces of a broad family of oxides. We demonstrate that the decrease of OCO-angle, previously proposed as the indicator of activation, is insufficient to account for the good catalytic performance of experimentally characterized oxides. Instead, SGD analysis shows that these surfaces consistently exhibit combinations of “genes” resulting in a strong elongation of a C-O bond due to binding of one O atom in CO2 molecule to a surface cation. The same combinations of “genes” also minimize the OCO-angle, but under the constraint that the Sabatier principle is satisfied. Based on these findings, we propose a set of new promising oxide-based catalyst materials for CO2 conversion, and a recipe to find more. – A. Mazheika et.al. ArXiv:1912.06515. |
Tuesday, March 15, 2022 5:24PM - 5:36PM |
K47.00011: Electrochemical Potential of the Metal Organic Framework MIL-101(Fe) as Cathode Material in Li-Ion Batteries Bernardo Barbiellini, Fatemeh Keshavarz, Marius Kadek, Arun Bansil We discuss the characteristic factors that determine the electrochemical potentials in a metal-organic framework (MOF) used as cathode for Li-ion batteries via density functional theory-based simulations. Our focus is on MIL-101(Fe) cathode material. Our study gives insight into the role of local atomic environment and structural deformations in generating electrochemical potential. |
Tuesday, March 15, 2022 5:36PM - 5:48PM |
K47.00012: Computational Design and Validation of Polymer Membranes with high CO2 Permeability Hsianghan Hsu, Ronaldo Giro, Akihiro Kishimoto, Lisa Hamada, Seiji Takeda, Mathias B Steiner Membranes made of polymer are being developed and applied to carbon dioxide (CO2) separation in carbon capture at industrial scale. Computational discovery of new membrane materials relies on data collection and machine learning algorithms for automatically creating new monomers in the process. The physical performance validation of generated monomer candidates within the actual membrane, however, is complicated, time consuming and computationally expensive. In this contribution, we have selected CO2-Permeability and Cohesive Energy Density (CED) as figures-of-merit in our AI inverse molecular design workflow. We compute CED according to group contribution based Fedors-type cohesive energy and the molar volume from SMILES representations. Within the generated results, two representative monomers with similar structures but with different polarities were selected for physical validation. Specifically, we have performed Constant Pressure Drop Molecular Dynamics simulations of separation performance for membranes made of the two monomers, leading to high permeability results. our approach could be extended from homopolymer to copolymer membrane discovery to cover a broader range of materials applications.
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