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At least 397 records · Page 22

Intermetallic Nanocatalysts from Heterobimetallic Group 10–14 Pyridine-2-thiolate Precursors

Intermetallic compounds are atomically ordered inorganic materials containing two or more transition metals and main-group elements in unique crystal structures. Intermetallics based on group 10 and group 14 metals have shown enhanced activity, selectivity, and durability in comparison to simple metals and alloys in many catalytic reactions. While high-temperature solid-state methods to prepare intermetallic compounds exist, softer synthetic methods can provide key advantages, such as enabling the preparation of metastable phases or of smaller particles with increased surface areas for catalysis. In this work, we study a generalized family of heterobimetallic precursors to binary intermetallics, each containing a group 10 metal and a group 14 tetrel bonded together and supported by pincer-like pyridine-2-thiolate ligands. Upon thermal decomposition, these heterobimetallic complexes form 10–14 binary intermetallic nanocrystals. Experiments and density functional theory (DFT) computations help in better understanding the reactivity of these precursors toward the synthesis of specific intermetallic binary phases. Using Pd 2 Sn as an example, we demonstrate that nanoparticles made in this way can act as uniquely selective catalysts for the reduction of nitroarenes to azoxyarenes, which highlights the utility of the intermetallics made by our method. Employing heterobimetallic pincer complexes as precursors toward binary nanocrystals and other metal-rich intermetallics provides opportunities to explore the fundamental chemistry and applications of these materials.

10-14 intermetallics↗

Catalytic Tandem CO 2 –Ethane Reactions and Hydroformylation for C3 Oxygenate Production

The strategy of tandem hydroformylation reaction for C3 oxygenate production from CO 2 and ethane represents an opportunity of simultaneously upgrading greenhouse gas CO 2 and the large-reserved shale gas into value-added liquid products. One of the challenges is how to tune and achieve the appropriate ethylene/CO/H 2 ratios for the downstream hydroformylation. Herein, the desired ethylene/CO/H 2 ratios were analyzed and identified by considering different combinations of main and side-reactions of CO 2 and ethane, based on which the PtSn 3 /γ-Al 2 O 3 catalyst was identified as promising to enable the catalytic tandem hydroformylation reaction. Further, the combined studies of reactor evaluation, in situ and ex situ characterization and theoretical calculations revealed that the Pt cluster/SnO x interfacial structures dominated the simultaneous dehydrogenation and dry reforming of ethane, thereby allowing the co-formation of ethylene, CO and H 2 that were subsequently converted to C3 oxygenates in the tandem hydroformylation reactor. The current work not only demonstrates the design principles of suitable catalysts for the tandem-reactor strategy, but also highlights the utilization of CO 2 and shale gas to produce value-added oxygenate products.

03 NATURAL GAS↗

Investigation of catalytic reduction and filter techniques for simultaneous measurements of NO, NO2, and HNO3 in the stratosphere

A concept for measuring stratospheric NOy-species is presented which utilizes the catalytic reduction of NO2 and HNO3 over heated metal catalysts and the chemisorption of HNO3 on Nylon. Using the Max Planck Institute for Aeronomy (MPAE) chemiluminescent balloon-borne sonde, stratospheric NO and NO2 profiles have been measured since 1983. NO is detected by chemiluminescence produced in reaction with O3 while NO2 needs first to be converted to NO over a heated stainless steel catalyst. To improve this technique for simultaneously measuring HNO3, the catalytic reduction of NO2 and HNO3 over several metal catalysts and the chemisorption of NO2 and HNO3 on Nylon have been investigated in laboratory tests. The results of these tests under simulated stratospheric conditions are presented in detail in this paper. They demonstrate that the simultaneous measurement of NO, NO2 and HNO3 is indeed possible with the combination of stainless steel or Au as a catalyst and a nylon filter.

Wendt, J.↗

Mesoflow: An Open-Source Reacting Flow Solver for Catalysis at Mesoscale

We present the capabilities and software performance metrics of our open-source continuum solver for catalysis, Mesoflow, developed specifically for modeling transport and chemistry at the mesoscale. Our solver utilizes Cartesian block-structured adaptive mesh refinement to resolve complex catalyst surface morphologies directly obtained from X-ray tomography data. An immersed boundary based formulation enables rapid representation of complex geometries prevalent in most mesoporous catalyst interfaces. The solver is developed on top of open-source performance portable library, AMReX, providing parallel execution capabilities on current and upcoming high-performance-computing (HPC) architectures. Our flexible software framework enables integration of complex chemical mechanisms at heterogenous interfaces and time-split algorithms for circumventing highly disparate reaction and flow time-scales. Our current studies indicate a ten-fold performance gain by using graphics-processing-units (GPUs) compared to a single processor for representative problem sizes (2 million cell mesh). We will also present a brief introduction on how to build and use this software for application problems pertaining to catalytic upgrading and gas transport within porous catalyst particles.

adaptive meshing↗

Study of Sabatier Catalyst Performance for a Mars ISRU Propellant Production Plant

NASA is currently developing technologies for use in the field of in-situ resource utilization (ISRU). One of the technologies being advanced is the Sabatier, or methanation, reactor which converts carbon dioxide and hydrogen into methane gas and water at high temperatures. This paper discusses the catalyst life and performance issues for these reactors that would be expected on Mars and describes the test methods employed and observed results. The various catalysts were tested in their capacity for the continuous production of methane gas via the Sabatier reaction and the possible effects of launch vibration loads, exposure to liquid water, particulate contamination, and chemical contamination to the overall observed reaction efficacy of the catalysts evaluated.

Franco, Carolina↗

Study of Sabatier Catalyst Performance for a Mars ISRU Propellant Production Plant

NASA is currently developing technologies for use in the field of in-situ resource utilization (ISRU). One of the technologies being advanced is the Sabatier, or methanation, reactor which converts carbon dioxide and hydrogen into methane gas and water at high temperatures. This paper discusses the catalyst life and performance issues for these reactors that would be expected on Mars and describes the test methods employed and observed results. The various catalysts were tested in their capacity for the continuous production of methane gas via the Sabatier reaction and the possible effects of launch vibration loads, exposure to liquid water, particulate contamination, and chemical contamination to the overall observed reaction efficacy of the catalysts evaluated.

Franco, Carolina↗

Optimizing the Heisenberg Vortex Tube for Hydrogen Cooling (Final Technical Report)

Hydrogen utilization at Plug Power sites ranges between 70-93% with the remainder vented and lost to the atmosphere. The goal of this project was to improve hydrogen utilization at Plug Power fulfillment centers via the patented Heisenberg vortex tube (HVT). The HVT combines conventional counterflow vortex tubes with para-orthohydrogen conversion catalyst to allow the cooling of hydrogen flows with no moving parts or external energy inputs. In year 1 of this project the HVT was evaluated to improve hydrogen utilization via the following concepts: 1) increasing liquid hydrogen pump volumetric efficiency by 20% through vapor separation and subcooling of the liquid, 2) reducing liquid hydrogen storage tank boil-off losses by 20% through thermal vapor shielding (TVS), and 3) increase isentropic efficiency of supercritical hydrogen expansion at 40-50 K, from 31% to over 40%. The TVS concept was selected as the most favorable application for further development. While the conceptual analysis was underway, the cryocatalysis hydrogen experiment facility (CHEF) was retrofitted with a new cryocooler, higher pressure condenser tanks, and in-situ fiber-optic Raman probes for ortho-parahydrogen composition analysis at the inlets and outlets of the HVT. To our knowledge this is the first in-situ implementation of cryogenic Raman probes for ortho-parahydrogen analysis. Subsequent testing of catalyzed and non-catalyzed HVT identified a low flow rate, high-conversion efficacy regime well suited for TVS development. Computational fluid dynamics (CFD), Reduced order modeling (ROM), and quantum Monte Carlo atomistic simulations were applied to optimize the design of the HVT implemented for TVS. The simulations and analysis identified a ruthenium-based catalyst as the most optimal for high conversion with little pressure losses and was matched to experimental measurements. These results indicated the design could achieve the 20% boil-off reduction target. An HVT field-trial was designed and constructed by Plug Power and implemented at a customer site. However, budget limitations reduced the amount of catalyst that could be applied to the HVT. With the reduced amount of catalyst, CFD analysis estimated about 3% reduction in boil-off. A similar amount of boil-off reduction was observed during preliminary measurements during tank commissioning. However, the results have a large margin for error and were operated at relatively low tank temperatures when the HVT has the lowest potential for improvement. This project demonstrated the use of para-orthohydrogen catalysis for reducing liquid hydrogen tank boil-off losses. The field trial system is anticipated to provide long-term experimental measurements on tank operational performance that will allow Plug Power to instrument additional tanks in the future. Recommendations for future work include the development of higher activity, lower cost para-orthohydrogen conversion catalyst for use in the HVT. Tank process optimizations could maximize the efficacy of the HVT and further improve hydrogen utilization.

08 HYDROGEN↗

From Powder to Power: Tailored Pre-Milling Strategy that Optimizes Microstructure for Efficient Hydrogen Evolution

The hydrogen evolution reaction (HER) plays a critical role in enabling large-scale electrolytic hydrogen production and advancing future technologies and fuel production. Among non-precious metals, NiMo-based catalysts are particularly attractive due to their capability to promote both water dissociation and hydrogen adsorption in alkaline media. However, conventional NiMo catalysts often suffer from incomplete alloying, particle aggregation, weak metal–support interactions, and surface oxidation, which significantly limit active site utilization, electronic conductivity, and long-term stability. Herein, we report a scalable, solid-state, two-step ball milling strategy for constructing an efficient NiMo/C catalyst for the HER. Pre-milling the metal precursors prior to carbon incorporation promotes efficient solid-state activation, leading to the formation of uniformly alloyed, ultrafine, and defect-rich Ni–Mo nanoparticles with robust metal–carbon interfacial anchoring. Benefiting from this integrated structural design, the optimized NiMo/C catalyst exhibits low overpotentials and Tafel slopes, reduced charge-transfer resistance, and excellent durability under alkaline conditions. Comprehensive structural and surface analysis reveal that the enhanced HER performance can be attributed to the synergistic interplay of homogeneous Ni–Mo alloying, uniform nanoparticle dispersion on a defect-rich carbon scaffold, enhanced accessibility of catalytically active sites, and optimized electronic coupling that stabilizes the catalyst surface. This work highlights the two-step solid-state ball milling strategy as a simple, robust, and scalable route for the preparation of effective and durable non-precious metal HER electrocatalysts, offering practical insights toward large-scale and inexpensive hydrogen production.

Yang, Xiaoxuan [Oak Ridge National Laboratory (ORN↗

A high-performance and durable direct NH 3 tubular protonic ceramic fuel cell integrated with an internal catalyst layer

Nickel-based cermet anode-supported protonic ceramic fuel cells (PCFCs) show great potential for direct utilization of ammonia. However, the insufficient activity of anode and the deterioration of anode activity/durability caused by the undesired interaction between nickel and ammonia greatly limit the application. Here, we report tubular PCFCs embedded with a catalytic iron layer. Such cells show peak power densities of 1.507 W cm -2 and 1.078 W cm -2 at 700 °C when using H 2 and NH 3 as fuel, respectively, which are the highest tubular PCFC performance so far ever reported. In addition, the stability of cells with the catalyst layer has been dramatically enhanced when compared with that of cells without the catalyst layer. As a result, the enhancement of activity and durability is attributed to the catalytic activity of iron for ammonia decomposition, through which the direct contact between nickel and ammonia has been minimized and the anode structure has therefore been protected.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Antimicrobial Properties of Corn Stover Lignin Fractions Derived from Catalytic Transfer Hydrogenolysis in Supercritical Ethanol with a Ru/C Catalyst

Converting lignin to value-added products at high yields provides an avenue for making ethanol biorefineries more profitable while reducing the carbon footprint of products generally derived from petroleum. In this study, corn stover lignin was depolymerized by catalytic transfer hydrogenolysis (CTH) in supercritical ethanol with a Ru/C catalyst. The lignin-derived bio-oil was then sequentially extracted utilizing hexane, petroleum ether, chloroform, and ethyl acetate as solvents in order of less polar to polar, and the subsequent bio-oils were characterized using GPC, GC/MS, and HSQC NMR. In this work, results show that the monomers in the bio-oil fractions contained primarily alkylated phenols, hydrogenated hydroxycinnamic acid derivatives, syringol and guaiacol-type lignins created from reductive cleavages of ether linkages, which were sequentially extracted into groups depending on the solvent polarity. The antimicrobial properties of the bio-oils were screened against Gram-positive (Bacillus subtilis, Lactobacillus amylovorus, and Staphylococcus epidermidis) and Gram-negative (Escherichia coli) bacteria and yeast (Saccharomyces cerevisiae) by examining microbial growth inhibition. Results show that CTH-derived bio-oils inhibited all tested organisms at concentrations less than 3 mg/mL. Total monomer concentration and the presence of specific monomers (i.e., syringyl propane) showed correlations to antimicrobial activity, likely due to cell death or membrane damage. This study provides insights into using sequential extraction to fractionate lignin-derived compounds and correlations between the properties of the extracted compounds and their antimicrobial activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Data-Driven Discovery of Bimetallic Nanoparticles Catalysts for the Hydrogenolysis of Polyethylene

Supported platinum nanoparticles are known to convert polyolefins to high-quality liquid hydrocarbons with hydrogen under relatively mild conditions. However, no systematic study has been undertaken using bimetallic catalysts for polyethylene upcycling. Specifically, a total of 98 monometallic and bimetallic combinations (Ag, Cr, Co, Cu, Fe, Ga, In, Mn, Ni, Pd, Pt, Rh, Ru, Zr) on alumina were synthesized utilizing surface organometallic chemistry (SOMC) technique via robotic platform. These were investigated at a small scale (10 mg of catalyst and 50 mg of polyethylene) for their activity for the hydrogenolysis of polyethylene in a high-throughput batch reactor. Combinations of Ni and Co were selected as candidates with high activity toward conversion into paraffin oils. Reaction conditions were optimized with Ni/Co/Al 2 O 3 catalyst at a larger scale (300 mg catalyst and 3 g polyethylene) to obtain a high yield (93.1%) of paraffin wax with desired properties (M n = 380 Da) and low polydispersity (Đ = 1.2). Ni/Co/Al 2 O 3 was compared against Co/Ni/Al 2 O 3 to understand the role of the deposition sequence. When Co is deposited before Ni, a layer of cobalt aluminate is formed upon reduction, stabilizing the deposition of 5 nm metallic Ni particles. When nickel is deposited before Co, particles are larger (average >20 nm) and more oxidized (Ni δ+ in NiAl 2 O 4 ), decreasing the availability of the catalytically active metallic Ni. In conclusion, the difference in electronic environments was also described by DFT calculations, which revealed that smaller 3D clusters of Ni are preferred on CoAl2O4 over the 3D clusters on NiAl 2 O 4 and that these smaller clusters are more reducible, as confirmed experimentally.

Polymer↗

Determining Proton Transport in Pseudo Catalyst Layers Using Hydrogen Pump DC and AC Techniques

Optimizing electrode morphology with a more uniform ionomer distribution is key to reducing ohmic losses and increasing electrocatalyst utilization in polymer electrolyte fuel cells (PEFCs). Inherent ionomer conductivity, volume fraction and tortuosity determine effective ionic conductivity. We use hydrogen pump (HP) method to measure effective ionic conductivity of a pseudo catalyst layer (PCL) comprised of Vulcan XC-72 carbon black and 3M 825 EW ionomer with ionomer to carbon (I/C) ratios of 0.6, 1 and 1.4 and relative humidity (RH) range of 50 to 120%. These direct current (DC) experiments are then compared with electrochemical impedance spectroscopy (EIS). Both DC and EIS methods show good agreement, indicating that EIS can be used as an alternative to DC method in HP experiment. Ionic conductivity for PCL with I/C of 1 and 1.4 was found to be about one order of magnitude higher than I/C of 0.6 for most of the RH range. At 90% RH tortuosities for I/C = 1 and 1.4 were close to 1, whereas tortuosity for I/C = 0.6 was 3. With decrease in relative humidity tortuosities increased linearly and at 50% relative humidity a PCL with I/C = 0.6 had the highest tortuosity of 6.1.

25 ENERGY STORAGE↗

Single Metal Atom Catalysts Prepared by Diluted Atomic Layer Deposition

The scalable and facile preparation of single-atom catalysts remains a critical challenge. Here, in this study, we introduce diluted atomic layer deposition (DALD), a unique approach for synthesizing supported metal catalysts with precisely tunable loadings. Unlike conventional metal deposition by ALD which uses pure metal precursors, DALD employs a diluted precursor mixture, combining organometallic precursors with the corresponding free ligand in controlled ratios. The method enables precise control over metal loadings, allowing the synthesis of structures ranging from nanoparticles to isolated single atoms, as exemplified by Ir, Rh, and Pt on high-surface-area γ-Al 2 O 3 . With its inherent simplicity and exceptional efficiency in metal precursor utilization, DALD represents a highly scalable strategy, unlocking opportunities for integrating single-atom catalysts into industrial processes.

36 MATERIALS SCIENCE↗

Pd-Ru pair on Pt surface for promoting hydrogen oxidation and evolution in alkaline media

Hydrogen oxidation reaction in alkaline media is critical for alkaline fuel cells and electrochemical ammonia compressors. The slow hydrogen oxidation reaction in alkaline electrolytes requires large amounts of scarce and expensive platinum catalysts. While transition metal decoration can enhance Pt catalysts’ activity, it often reduces the electrochemical active surface area, limiting the improvement in Pt mass activity. Here, we enhance Pt catalysts’ activity without losing surface-active sites by using a Pd-Ru pair. Utilizing a mildly catalytic thermal pyrolysis approach, Pd-Ru pairs are decorated on Pt, confirmed by extended X-ray absorption fine structure and high-angle annular dark-field scanning transmission electron microscopy. Density functional theory and ab-initio molecular dynamics simulations indicate preferred Pd and Ru dopant adsorption. The Pd-Ru decorated Pt catalyst exhibits a mass-based exchange current density of 1557 ± 85 A g –1 metal for hydrogen oxidation reaction, demonstrating superior performance in an ammonia compressor.

25 ENERGY STORAGE↗

Non-bonding interaction of dual atom catalysts for enhanced oxygen reduction reaction

Here, we demonstrate the design of graphene-supported dual atom catalysts (DACs) for the four-electron oxygen reduction reaction (ORR), by utilizing the non-bonding interaction of counterpart metals (M) that synergistically tune the electronic properties and catalytic activity of the Fe active site in FeMN 6 -DAC and FeMN 8 -DAC systems, where M stands for Fe, Co, Ni, Cu, and Zn. More specifically, for Fe-M distances below 15Å, the non-bonding interaction is significant, making the system act as the DAC. We predicted that FeNiN 6 -DAC and FeNiN 8 -DAC exhibit a low ORR overpotential (η ORR ) of 0.28 V and 0.47 V, respectively, which are at the summits of volcano plots. This low η ORR originates from the high Bader charge transfer coupled with high spin density at the Fe site in both the FeNiN 6 -DAC and FeNiN 8 -DAC systems, which weakens the adsorption of OH* intermediate while enhancing its desorption to H 2 O. Guided by these density functional theory (DFT) computational results, we synthesized FeCoN 8 -DAC and FeNiN 8 -DAC along with N-doped graphene and confirmed their structures with scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption near-edge structure (XANES), extended X-ray absorption fine structure (EXAFS), and electron spin resonance (ESR). We verify experimentally the catalytic activities and find that FeNiN 8 -DAC has the low experimental overpotential of 0.39 V with a Tafel slope of 47 mVdec -1 . Based on these results, we propose a DFT-guided strategy to tune the charge transfer and spin population of the active site toward designing DACs for electrochemical ORR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structure Sensitive Reaction Kinetics of Chiral Molecules on Intrinsically Chiral Surfaces

Enantiospecific heterogeneous catalysis utilizes chiral surfaces to resolve enantiomers via structure sensitive surface chemistry. The catalyst design challenge is the identification of chiral surface structures that maximize enantiospecificity. Herein, we develop data driven models for the enantiospecificity of tartaric acid reactions on chiral Cu(hkl) R&S surfaces. Measurements of enantiospecific rate constants were obtained by using curved Cu(hkl) R&S surfaces that enable kinetic measurements on hundreds of chiral surface orientations. One model uses feature vectors derived from generalized coordination numbers to capture the local structure around Cu atoms exposed by the Cu(hkl) R&S surfaces. The second model introduces the use of chiral cubic harmonic functions to capture the symmetry constraints of the face-centered cubic Cu structure. The model using 58 generalized coordination numbers has a fitting error similar to that of the model using only 5 cubic harmonic functions. The two models predict maxima in the enantiospecificity on surfaces with very similar surface orientations. The models developed in this work are applicable for any enantiospecific reaction happening on any chiral material with a cubic lattice structure, opening the way to understanding the surface structure sensitivity of the enantiospecific reaction kinetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stability of heterogeneous single-atom catalysts: a scaling law mapping thermodynamics to kinetics

Heterogeneous single-atom catalysts (SACs) hold the promise of combining high catalytic performance with maximum utilization of often precious metals. We extend the current thermodynamic view of SAC stability in terms of the binding energy (E bind ) of single-metal atoms on a support to a kinetic (transport) one by considering the activation barrier for metal atom diffusion. A rapid computational screening approach allows predicting diffusion barriers for metal–support pairs based on E bind of a metal atom to the support and the cohesive energy of the bulk metal (E c ). Metal–support combinations relevant to contemporary catalysis are explored by density functional theory. Assisted by machine-learning methods, we find that the diffusion activation barrier correlates with (E bind ) 2 /E c in the physical descriptor space. This diffusion scaling-law provides a simple model for screening thermodynamics to kinetics of metal adatom on a support.

36 MATERIALS SCIENCE↗

Electrocatalytic water oxidation performance in an extended porous organic framework with a covalent alliance of distinct Ru sites

The rational synthesis of durable, earth-abundant efficient electrocatalysts for the oxygen evolution reaction (OER) from water is one of the most important routes for storing renewable energy and minimizing fossil fuel combustion. The prime hurdles for effectively utilizing commercial RuO 2 as (OER) electrocatalysts are its very low stability, catalyst deactivation, and high cost. In this work, we explored a Ru-integrated porous organic polymer (Ru@Bpy-POP) by a facile one-pot Friedel–Crafts alkylation strategy between redox-active (Ru(demob) 3 Cl 2 ) and a carbazole unit, which is composed of unique features including an extended framework unit, isolated active sites, and tunable electrode kinetics. Ru@Bpy-POP can serve as a bridge between a Metal–Organic Framework (MOF) and POP-based catalytic systems with a balanced combination of covalent bonds (structural stability) and open metal sites (single site catalysis). Ru@Bpy-POP, deposited on a three-dimensional nickel foam electrode support, exhibits a promising electrocatalytic OER activity with an ultra-low ruthenium loading compared to a benchmark RuO 2 catalyst, providing an overpotential of about 270 mV to reach 10 mA cm –2 in an alkaline medium. Moreover, a high current density of 248 mA cm –2 was achieved for the Ru@Bpy-POP catalyst at only 1.6 V (vs. RHE), which is much higher than 91 mA cm –2 for commercial RuO 2 . The robust, albeit highly conjugated, POP framework not only triggered facile electro-kinetics but also suppressed aggregation and metallic corrosion during electrolysis. In particular, the benefits of covalent integration of distinct Ru sites into the framework can modulate intermediate adsorption and charge density, which contributes to its exceptional OER activity. All of the critical steps involved in OER are complemented by Density Functional Theory (DFT) calculations, which suggest that electrocatalytic water oxidation proceeds from a closed-shell configuration to open-shell electronic configurations with high-spin states. Finally, these open-shell configurations are more stable than their closed-shell counterparts by 1 eV, improving the overall catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗