Computational Screening of Bimetallic Catalysts: Application to Ammonia Decomposition

2021 ◽  
Author(s):  
Hongbo Wu ◽  
Chang Liu ◽  
Wei Guo
Keyword(s):  
Bimetallic Catalysts ◽  
Ammonia Decomposition ◽  
Computational Screening

scholarly journals Material Discovery and High Throughput Exploration of Ru Based Catalysts for Low Temperature Ammonia Decomposition

Materials ◽  
2020 ◽  
Vol 13 (8) ◽  
pp. 1869 ◽  
Author(s):  
Katherine McCullough ◽  
Pei-Hua Chiang ◽  
Juan D. Jimenez ◽  
Jochen A. Lauterbach
Keyword(s):  
Low Temperature ◽  
High Throughput ◽  
Bimetallic Catalysts ◽  
Active Sites ◽  
Operating Conditions ◽  
Ammonia Decomposition ◽  
Turnover Frequency ◽  
Surface Sites ◽  
Equivalent Number ◽  
Apparent Activation Energies

High throughput experimentation has the capability to generate massive, multidimensional datasets, allowing for the discovery of novel catalytic materials. Here, we show the synthesis and catalytic screening of over 100 unique Ru-Metal-K based bimetallic catalysts for low temperature ammonia decomposition, with a Ru loading between 1–3 wt% Ru and a fixed K loading of 12 wt% K, supported on γ-Al2O3. Bimetallic catalysts containing Sc, Sr, Hf, Y, Mg, Zr, Ta, or Ca in addition to Ru were found to have excellent ammonia decomposition activity when compared to state-of-the-art catalysts in literature. Furthermore, the Ru content could be reduced to 1 wt% Ru, a factor of four decrease, with the addition of Sr, Y, Zr, or Hf, where these secondary metals have not been previously explored for ammonia decomposition. The bimetallic interactions between Ru and the secondary metal, specifically RuSrK and RuFeK, were investigated in detail to elucidate the reaction kinetics and surface properties of both high and low performing catalysts. The RuSrK catalyst had a turnover frequency of 1.78 s−1, while RuFeK had a turnover frequency of only 0.28 s−1 under identical operating conditions. Based on their apparent activation energies and number of surface sites, the RuSrK had a factor of two lower activation energy than the RuFeK, while also possessing an equivalent number of surface sites, which suggests that the Sr promotes ammonia decomposition in the presence of Ru by modifying the active sites of Ru.

MCM-41 supported Co Mo bimetallic catalysts for enhanced hydrogen production by ammonia decomposition

2012 ◽  
Vol 207-208 ◽  
pp. 103-108 ◽  
Author(s):  
Xuezhi Duan ◽  
Gang Qian ◽  
Xinggui Zhou ◽  
De Chen ◽  
Weikang Yuan
Keyword(s):  
Hydrogen Production ◽  
Bimetallic Catalysts ◽  
Ammonia Decomposition ◽  
Mcm 41

Using first principles to predict bimetallic catalysts for the ammonia decomposition reaction

2010 ◽  
Vol 2 (6) ◽  
pp. 484-489 ◽  
Author(s):  
Danielle A. Hansgen ◽  
Dionisios G. Vlachos ◽  
Jingguang G. Chen
Keyword(s):  
First Principles ◽  
Bimetallic Catalysts ◽  
Decomposition Reaction ◽  
Ammonia Decomposition

Structure and composition of metal particles in Pt-Sn/Al2O3 bimetallic catalysts

1990 ◽  
Vol 48 (4) ◽  
pp. 278-279
Author(s):  
A. Sachdev ◽  
J. Schwank
Keyword(s):  
Bimetallic Catalysts ◽  
Bimetallic Catalyst ◽  
Size Structure ◽  
High Surface ◽  
High Surface Area ◽  
Metal Particles ◽  
Alloy Formation ◽  
Particle Size Range ◽  
Oxide Supports ◽  
Petroleum Fractions

Platinum - tin bimetallic catalysts have been primarily utilized in the chemical industry in the catalytic reforming of petroleum fractions. In this process the naphtha feedstock is converted to hydrocarbons with higher octane numbers and high anti-knock qualities. Most of these catalysts contain small metal particles or crystallites supported on high surface area insulating oxide supports. The determination of the structure and composition of these particles is crucial to the understanding of the catalytic behavior. In a bimetallic catalyst it is important to know how the two metals are distributed within the particle size range and in what way the addition of a second metal affects the size, structure and composition of the metal particles. An added complication in the Pt-Sn system is the possibility of alloy formation between the two elements for all atomic ratios.

Tuning the Redox Activity of Metal−Organic Frameworks for Enhanced, Selective O2 Binding

2019 ◽  
Author(s):  
Andrew Rosen ◽  
M. Rasel Mian ◽  
Timur Islamoglu ◽  
Haoyuan Chen ◽  
Omar Farha ◽  
...  
Keyword(s):  
Density Functional ◽  
Metal Organic Frameworks ◽  
Redox Activity ◽  
Screening Methods ◽  
Bridging Ligands ◽  
Metal Centers ◽  
Computational Screening ◽  
Open Metal Sites ◽  
Metal Organic ◽  
Unsaturated Metal Sites

<p>Metal−organic frameworks (MOFs) with coordinatively unsaturated metal sites are appealing as adsorbent materials due to their tunable functionality and ability to selectively bind small molecules. Through the use of computational screening methods based on periodic density functional theory, we investigate O<sub>2</sub> and N<sub>2</sub> adsorption at the coordinatively unsaturated metal sites of several MOF families. A variety of design handles are identified that can be used to modify the redox activity of the metal centers, including changing the functionalization of the linkers (replacing oxido donors with sulfido donors), anion exchange of bridging ligands (considering μ-Br<sup>-</sup>, μ-Cl<sup>-</sup>, μ-F<sup>-</sup>, μ-SH<sup>-</sup>, or μ-OH<sup>-</sup> groups), and altering the formal oxidation state of the metal. As a result, we show that it is possible to tune the O<sub>2</sub> affinity at the open metal sites of MOFs for applications involving the strong and/or selective binding of O<sub>2</sub>. In contrast with O<sub>2</sub> adsorption, N<sub>2</sub> adsorption at open metal sites is predicted to be relatively weak across the MOF dataset, with the exception of MOFs containing synthetically elusive V<sup>2+</sup> open metal sites. As one example from the screening study, we predict that exchanging the μ-Cl<sup>-</sup> ligands of M<sub>2</sub>Cl<sub>2</sub>(BBTA) (H<sub>2</sub>BBTA = 1<i>H</i>,5<i>H</i>-benzo(1,2-d:4,5-d′)bistriazole) with μ-OH<sup>-</sup> groups would significantly enhance the strength of O<sub>2</sub> adsorption at the open metal sites without a corresponding increase in the N<sub>2</sub> affinity. Experimental investigation of Co<sub>2</sub>Cl<sub>2</sub>(BBTA) and Co<sub>2</sub>(OH)<sub>2</sub>(BBTA) confirms that the former exhibits only weak physisorption, whereas the latter is capable of chemisorbing O<sub>2</sub> at room temperature. The chemisorption behavior is attributed to the greater electron-donating character of the μ-OH<sup>-</sup><sub> </sub>ligands and the presence of H-bonding interactions between the μ-OH<sup>-</sup> bridging ligands and the O<sub>2</sub> adsorbate.</p>

Efficient Prediction of Structural and Electronic Properties of Hybrid 2D Materials Using DFT and Machine Learning

2018 ◽  
Author(s):  
Sherif Tawfik ◽  
Olexandr Isayev ◽  
Catherine Stampfl ◽  
Joseph Shapter ◽  
David Winkler ◽  
...  
Keyword(s):  
Machine Learning ◽  
Band Gap ◽  
Density Functional ◽  
2D Materials ◽  
Van Der Waals ◽  
Building Blocks ◽  
Machine Learning Techniques ◽  
Interlayer Distance ◽  
Computational Screening ◽  
Wide Range

Materials constructed from different van der Waals two-dimensional (2D) heterostructures offer a wide range of benefits, but these systems have been little studied because of their experimental and computational complextiy, and because of the very large number of possible combinations of 2D building blocks. The simulation of the interface between two different 2D materials is computationally challenging due to the lattice mismatch problem, which sometimes necessitates the creation of very large simulation cells for performing density-functional theory (DFT) calculations. Here we use a combination of DFT, linear regression and machine learning techniques in order to rapidly determine the interlayer distance between two different 2D heterostructures that are stacked in a bilayer heterostructure, as well as the band gap of the bilayer. Our work provides an excellent proof of concept by quickly and accurately predicting a structural property (the interlayer distance) and an electronic property (the band gap) for a large number of hybrid 2D materials. This work paves the way for rapid computational screening of the vast parameter space of van der Waals heterostructures to identify new hybrid materials with useful and interesting properties.

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