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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

A versatile elevated-pressure reactor combined with an ultrahigh vacuum surface setup for efficient testing of model and powder catalysts under clean gas-phase conditions

A small-volume reaction cell for catalytic or photocatalytic testing of solid materials at pressures up to 1000 Torr has been coupled to a surface-science setup used for standard sample preparation and characterization under ultrahigh vacuum (UHV). The reactor and sample holder designs allow easy sample transfer from/to the UHV chamber, and investigation of both planar and small amounts of powder catalysts under the same conditions. The sample is heated with an infrared laser beam and its temperature is measured with a compact pyrometer. Combined in a regulation loop, this system ensures fast and accurate temperature control as well as clean heating. The reaction products are automatically sampled and analyzed by mass spectrometry and/or gas chromatography (GC). Unlike previous systems, our GC apparatus does not use a recirculation loop and allows working in clean conditions at pressures as low as 1 Torr while detecting partial pressures smaller than 10{sup −4} Torr. The efficiency and versatility of the reactor are demonstrated in the study of two catalytic systems: butadiene hydrogenation on Pd(100) and CO oxidation over an AuRh/TiO{sub 2} powder catalyst.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Design of Dilute Palladium–Indium Alloy Catalysts for the Selective Hydrogenation of CO 2 to Methanol

Adding small amounts of a more reactive dopant metal to a more selective host metal is a well-known strategy for promoting the catalytic reactivity of the latter without sacrificing its selectivity. While substantial attention has been given to coinage metal hosts for activating individual C–H or O–H bonds, less attention has been given to more exotic metals, such as indium, which is highly selective in the complex hydrogenation of CO 2 to methanol. Herein, we describe the synthesis and properties of Pd–In alloys containing Pd in various states of aggregation (isolated atom, small clusters, and extended clusters) assessed through various characterization methods. These materials exhibit unique catalytic behaviors, with Pd promoting both the reaction rate and methanol selectivity in all cases, though its efficacy is highest when Pd is present in small clusters. Here, the inefficiency of high Pd loadings is due in part to losses in Pd accessibility, while the importance of aggregated vs isolated Pd is theorized to result from accelerated H 2 activation. Methods used to synthesize more conventional dilute-limit and single-atom alloy catalysts can, therefore, be extended to non-coinage metal hosts to promote and control more complex chemistries, though the roles of ensemble size may greatly differ.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Atomic Ordering-Induced Ensemble Variation in Alloys Governs Electrocatalyst On/Off States

The catalytic behavior of a material is influenced by ensembles—the geometric configuration of atoms. Traditional approaches, mainly utilizing solid-solution alloys in electrocatalysis, have often overlooked the challenges posed by concurrent changes in the electronic structure (i.e. d-band center) when the composition is altered. Here, this study introduces a methodology that distinctly separates the geometric effects (i.e. ensembles) from the electronic structure. We compare the reactivity of compositionally identical, but structurally different Pd 3 Bi ordered intermetallic and solid-solution alloys. Remarkably, we find that Pd 3 Bi intermetallics display nearly no reactivity for the methanol oxidation (MOR), while their solid-solution counterparts have significant reactivity. This highlights a unique case where materials with identical chemical compositions demonstrate drastically different catalytic behavior underscoring the critical importance of ensembles in electrocatalysis. Specifically, Pd 3 Bi intermetallics form smaller ensembles (average coordination number: 4.5 ± 1.6) with almost no measurable MOR activity at room temperature, in contrast to the solid-solution Pd 3 Bi that exhibit larger ensembles (average coordination number: 6.8 ± 0.9) and considerable MOR reactivity (0.5 mA cm −2 Pd ). An ordered Pd 3 Bi alloy, with an intermediate ensemble size (average coordination number: 5.3 ± 1.2), displays moderate MOR activity (0.1 mA cm −2 Pd ), further confirming the direct correlation between ensemble size and catalytic activity. Notably, all Pd 3 Bi alloys maintain similar electronic structures, because the chemical composition of the alloys is fixed, indicating that the differences in reactivity are predominantly from changes to the ensemble size. Our findings offer an approach for precisely controlling catalytic activity through manipulating the geometric configuration of the atoms within an alloy, paving the way for more efficient catalyst design.

alloys↗
DOE OSTI2023

Nucleation-mediated reshaping of facetted metallic nanocrystals: Breakdown of the classical free energy picture

Shape stability is key to avoiding degradation of performance for metallic nanocrystals synthesized with facetted non-equilibrium shapes to optimize properties for catalysis, plasmonics, and so on. Reshaping of facetted nanocrystals is controlled by the surface diffusion-mediated nucleation and growth of new outer layers of atoms. Here, Kinetic Monte Carlo (KMC) simulation of a realistic stochastic atomistic-level model is applied to precisely track the reshaping of Pd octahedra and nanocubes. Unexpectedly, separate constrained equilibrium Monte Carlo analysis of the free energy profile during reshaping reveals a fundamental failure of the classical nucleation theory (CNT) prediction for the reshaping barrier and rate. Why? Nucleation barriers can be relatively low for these processes, so the system is not locally equilibrated before crossing the barrier, as assumed in CNT. This claim is supported by an analysis of a first-passage problem for reshaping within a master equation framework for the model that reasonably captures the behavior in KMC simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Understanding Behavior of Self-Regenerative Catalysts by Transmission Electron Microscopy

First promoted by Daihatsu Motor Co. as an intelligent catalyst [1], the self-regenerative catalyst is an automotive catalyst in which the precious metal (e.g. Pt, Pd, Rh) supposedly dissolves into a carefully chosen perovskite oxide support upon oxidation, and re-disperses as metallic particles upon reduction; cyclical redox conditions that are already present in gasoline engine exhaust due to the fuel injection control system. This is counter to the behavior of metal particles on most supports, that irreversibly coarsen during redox cycling. Though the mechanistics of such a system are of great interest to the catalyst community, the authors of the original report (and subsequent studies) utilized only bulk characterization techniques (e.g. EXAFS, XANES) to analyze the average structure, and thus they did not satisfactorily probe the local environment of the metal particles and/or ions

electron microscopy↗
DOE OSTI2018

Confined Ultrathin Pd-Ce Nanowires with Outstanding Moisture and SO 2 Tolerance in Methane Combustion

Here, an efficient strategy (enhanced metal oxide interaction and core–shell confinement to inhibit the sintering of noble metal) is presented confined ultrathin Pd-CeO x nanowire (2.4 nm) catalysts for methane combustion, which enable CH 4 total oxidation at a low temperature of 350 °C, much lower than that of a commercial Pd/Al 2 O 3 catalyst (425 °C). Importantly, unexpected stability was observed even under harsh conditions (800 °C, water vapor, and SO 2 ), owing to the confinement and shielding effect of the porous silica shell together with the promotion of CeO 2 . Pd-CeO x solid solution nanowires (Pd-Ce NW) as cores and porous silica as shells (Pd-CeNW@SiO 2 ) were rationally prepared by a facile and direct self-assembly strategy for the first time. Finally, this strategy is expected to inspire more active and stable catalysts for use under severe conditions (vehicle emissions control, reforming, and water–gas shift reaction).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Kinetics of the functionalization of mesoporous silica nanoparticles: Implications on surface group distributions, adsorption and catalysis

The post-synthesis functionalization (grafting) kinetics of mesoporous silica nanoparticles (MSN) with organotrimethoxysilanes (R-TMS) is studied via solution 1 H NMR spectroscopy. The process involves a rapid adsorption/ desorption pre-equilibrium followed by reaction of R-TMS with surface silanols. Grafting rates are affected by the functional group in R-TMS. For example, the grafting rate of aminopropyl-trimethoxysilane (AP-TMS) is one order of magnitude higher than other R-TMS. High concentrations of AP-TMS result in substrate-inhibition kinetics, likely due to steric and mobility constraints for reactant alignment at high coverage. The higher rates of AP-TMS grafting indicate a catalytic effect of amine groups. This effect depends on the amine’s basicity and can be used to control the grafting rates and degree of condensation of other R-TMS. Adjusting the rate of mercaptopropyl-trimethoxysilane (MP-TMS) grafting using amines gives MP-MSN materials of varying adsorptive and catalytic activities, illustrated by Pd scavenging experiments and use of Pd@MP-MSN as catalysts for a Suzuki-Miyaura cross-coupling reaction.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Identifying the Atomic-Level Effects of Metal Composition on the Structure and Catalytic Activity of Peptide-Templated Materials

Bioinspired approaches for the formation of metallic nanomaterials have been extensively employed for a diverse range of applications including diagnostics and catalysis. These materials can often be used under sustainable conditions; however, it is challenging to control the material size, morphology, and composition simultaneously. Here we have employed the R5 peptide, which forms a 3D scaffold to direct the size and linear shape of bimetallic PdAu nanomaterials for catalysis. The materials were prepared at varying Pd:Au ratios to probe optimal compositions to achieve maximal catalytic efficiency. These materials were extensively characterized at the atomic level using transmission electron microscopy, extended X-ray absorption fine structure spectroscopy, and atomic pair distribution function analysis derived from high-energy X-ray diffraction patterns to provide highly resolved structural information. The results confirmed PdAu alloy formation, but also demonstrated that significant surface structural disorder was present. The catalytic activity of the materials was studied for olefin hydrogenation, which demonstrated enhanced reactivity from the bimetallic structures.These results present a pathway to the bioinspired production of multimetallic materials with enhanced properties, which can be assessed via a suite of characterization methods to fully ascertain structure/function relationships.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Altered Binding of Tumor Antigenic Peptides to MHC Class I Affects CD8 + T Cell–Effector Responses

T-cell priming occurs when a naïve T cell recognizes cognate peptide–MHC complexes on an activated antigen-presenting cell. The circumstances of this initial priming have ramifications on the fate of the newly primed T cell. Newly primed CD8 + T cells can embark onto different trajectories, with some becoming short-lived effector cells and others adopting a tissue resident or memory cell fate. To determine whether T-cell priming influences the quality of the effector T-cell response to tumors, here we used transnuclear CD8 + T cells that recognize the melanoma antigen TRP1 using TRP1 high or TRP1 low TCRs that differ in both affinity and fine specificity. From a series of altered peptide ligands, we identified a point mutation (K8) in a nonanchor residue that, when analyzed crystallographically and biophysically, destabilized the peptide interaction with the MHC binding groove. In vitro, the K8 peptide induced robust proliferation of both TRP1 high and TRP1 low CD8 + T cells but did not induce expression of PD-1. Cytokine production from K8-stimulated TRP1 cells was minimal, whereas cytotoxicity was increased. Upon transfer into B16 tumor–bearing mice, the reference peptide (TRP1-M9)- and K8-stimulated TRP1 cells were equally effective at controlling tumor growth but accomplished this through different mechanisms. TRP1-M9–stimulated cells produced more IFNγ, whereas K8-stimulated cells accumulated to higher numbers and were more cytotoxic. We, therefore, conclude that TCR recognition of weakly binding peptides during priming can skew the effector function of tumor-specific CD8 + T cells.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

Generation, Detection and characterization of Gas-Phase Transition Metal containing Molecules

The objective of this project was to generate, detect, and characterize small, gas-phase, metal containing molecules. In addition to being relevant to high temperature chemical environments (e.g. plasmas and combustion), gas-phase experiments on metal containing molecules serve as the most direct link to a molecular-level theoretical model for catalysis. Catalysis (i.e. the addition of a small about of recoverable material to control the rate and direction of a chemical reaction) is critical to the petroleum and pharmaceutical industries as well as environmental remediation. Currently, the majority of catalytic materials are based on very expensive metals such as platinum (Pt), palladium (Pd), iridium (Ir,) rhenium (Re), and rhodium (Rh). For example, the catalyst used for converting linear hydrocarbon molecules (e.g. hexane) to cyclic molecules (e.g. cyclohexane) is a mixture of Pt and Re suspended on alumina. It enables straight chain alkanes to be converted into branched-chain alkanes, cyclohexanes and aromatic hydrocarbons which are used, amongst other things, to enhance the octane number of petrol. A second example is the heterogeneous catalysis used in automobile exhaust systems to: a) decrease nitrogen oxide; b) reduce carbon monoxide; and c) oxidize unburned hydrocarbons. The exhaust is vented through a high-surface area chamber lined with Pt, Pd, and Rh. For example, the carbon monoxide is catalytically converted to carbon dioxide by reaction with oxygen. The research results from this work have been published in readily accessible journals1-28. The ground and excited electronic state properties of small metal containing molecules that we determine were: a) electronic state distributions and lifetimes, b) vibrational frequencies, c) bond lengths and angles, d) hyperfine interactions, e) permanent electric dipole moments, mel, and f) magnetic dipoles, μ m . In general terms, μ el , gives insight into the charge distribution and mm into the number and nature of the unpaired electrons. Analysis of the hyperfine interactions (i.e. Fermi-contact, nuclear electric quadrupole, etc.) is particularly insightful because it results from the interaction of nuclei with non-zero spin and the chemically important valence electrons. The bulk of the spectroscopic techniques used in these studies exploit the sensitivity of laser induced fluorescence (LIF) detection. The spectroscopic schemes employed include: a) cw and pulsed laser field-free(FF) excitation and dispersed LIF (DLIF); b) optical Stark; c) optical Zeeman; d) pump/probe microwave double resonance (PPMODR); e) fluorescence lifetimes, and f) resonant and non-resonant two-photon ionization TOF mass spectrometry. Vibrational spacing, force constants and electronic states distributions are derived from the analysis of pulsed dye laser excitation and DLIF spectra. Geometric structure (bond lengths and angles) and hyperfine parameters are derived from the analysis of cw-laser LIF and PPMODR spectra. Permanent electric dipole moments, mel,, and magnetic dipole moments, mm, are derived from the analysis of optical Stark and Zeeman spectra, respectively. Transition moments are derived from the analysis of radiative lifetimes. A supersonic molecular beam sample of these ephemeral molecules is generated by skimming the products of either a laser ablation/reaction source or a d.c. discharge source.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Mechanistic and Kinetic Analysis of Complete Methane Oxidation on a Practical PtPd/Al 2 O 3 Catalyst

A PtPd/Al 2 O 3 catalyst developed for the complete oxidation of methane from the ventilation air of underground coal mines is compared against a model PdO/Al 2 O 3 catalyst. Although the PtPd/Al 2 O 3 catalyst is substantially more active and stable than the model catalyst, the nature of active sites between the two catalysts is deemed to be fundamentally the same based on their response to different feed gas compositions and the evolution of surface CO adsorption complexes during time-resolved CO adsorption DRIFTS experiment. For both catalysts, coordinatively unsaturated Pd sites are considered the active centers for methane activation and the subsequent oxidation reaction. H 2 O competes with CH 4 for the same active sites, resulting in severe inhibition. Additionally, the CH 4 oxidation reaction also causes self-inhibition. Taking both inhibition effects into consideration, a relatively simple kinetic model is developed. The model provides a good fit of the 72 sets of kinetic data collected on the PtPd/Al 2 O 3 catalyst under practically relevant reaction conditions with CH 4 concentration in the range of 0.05–0.4%, H 2 O concentration of 1.0–5.0%, and reaction temperatures of 450–700 °C. Kinetic parameters based on the model suggest that the CH 4 activation energy on the PtPd/Al 2 O 3 catalyst is 96.7 kJ/mol, and the H 2 O adsorption energy is –31.0 kJ/mol. Both values are consistent with the parameters reported in the literature. The model can be used to develop catalyst sizing guidelines and be incorporated into the control algorithm of the catalytic system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Sub-second and ppm-level optical sensing of hydrogen using templated control of nano-hydride geometry and composition

Abstract The use of hydrogen as a clean and renewable alternative to fossil fuels requires a suite of flammability mitigating technologies, particularly robust sensors for hydrogen leak detection and concentration monitoring. To this end, we have developed a class of lightweight optical hydrogen sensors based on a metasurface of Pd nano-patchy particle arrays, which fulfills the increasing requirements of a safe hydrogen fuel sensing system with no risk of sparking. The structure of the optical sensor is readily nano-engineered to yield extraordinarily rapid response to hydrogen gas (<3 s at 1 mbar H 2 ) with a high degree of accuracy (<5%). By incorporating 20% Ag, Au or Co, the sensing performances of the Pd-alloy sensor are significantly enhanced, especially for the Pd 80 Co 20 sensor whose optical response time at 1 mbar of H 2 is just ~0.85 s, while preserving the excellent accuracy (<2.5%), limit of detection (2.5 ppm), and robustness against aging, temperature, and interfering gases. The superior performance of our sensor places it among the fastest and most sensitive optical hydrogen sensors.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Computational modeling predicts the stability of both Pd + and Pd2 + ion-exchanged into H-CHA

Passive NO x adsorbers (PNA) using Pd/zeolites have emerged as a promising solution for the reduction of cold-start emissions from vehicle exhaust. However, the nature of the active sites and the mechanisms underlying NO x adsorption in Pd/zeolites remain a subject of ongoing investigation. In this study, we employ quantum chemical simulations to investigate the structure of Pd species in cation-exchange sites at isolated Al and Al pairs in the 6-ring and 8-ring of the CHA framework before the introduction of NO x . Our calculations show that the speciation of Pd in these exchange sites strongly depends on the precise Al arrangement within the framework, as well as the operating conditions. Ionically dispersed Pd is found to be the most favorable species over a wide range of oxidizing and reducing conditions. Small oligomers of PdO and metallic Pd do not appear to be competitive at either isolated Al or Al pairs. Notably, our calculations show that ion exchange sites other than next–next–nearest neighbor Al pairs in the 6-ring will be preferentially occupied by Pd + instead of Pd 2+ . The stability of Pd + in the zeolite environment is an interesting contrast with its rareness in molecular Pd compounds. Nonetheless, a detailed analysis of the electronic structure shows that predicted Pd oxidation states are consistent with chemical intuition for all complexes investigated in this study. We also discuss the potential ambiguity in Pd characterization provided by typical experimental techniques such as XANES, EXAFS and UV-Vis, and highlight the need for additional EPR spectroscopy studies to further elucidate the initial Pd speciation in zeolites for PNA applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Strong Damping‐Like Spin‐Orbit Torque and Tunable Dzyaloshinskii–Moriya Interaction Generated by Low‐Resistivity Pd 1− x Pt x Alloys

Abstract Despite their great promise for providing a pathway for very efficient and fast manipulation of magnetization, spin‐orbit torque (SOT) operations are currently energy inefficient due to a low damping‐like SOT efficiency per unit current bias, and/or the very high resistivity of the spin Hall materials. This work reports an advantageous spin Hall material, Pd 1− x Pt x , which combines a low resistivity with a giant spin Hall effect as evidenced with three independent SOT ferromagnetic detectors. The optimal Pd 0.25 Pt 0.75 alloy has a giant internal spin Hall ratio of >0.60 (damping‐like SOT efficiency of ≈0.26 for all three ferromagnets) and a low resistivity of ≈57.5 µΩ cm at a 4 nm thickness. Moreover, it is found that the Dzyaloshinskii–Moriya interaction (DMI), the key ingredient for the manipulation of chiral spin arrangements (e.g., magnetic skyrmions and chiral domain walls), is considerably strong at the Pd 1− x Pt x /Fe 0.6 Co 0.2 B 0.2 interface when compared to that at Ta/Fe 0.6 Co 0.2 B 0.2 or W/Fe 0.6 Co 0.2 B 0.2 interfaces and can be tuned by a factor of 5 through control of the interfacial spin‐orbital coupling via the heavy metal composition. This work establishes a very effective spin current generator that combines a notably high energy efficiency with a very strong and tunable DMI for advanced chiral spintronics and spin torque applications.

Zhu, Lijun↗
DOE OSTI2023

Dual-site catalysts featuring platinum-group-metal atoms on copper shapes boost hydrocarbon formations in electrocatalytic CO2 reduction

Abstract Copper-based catalyst is uniquely positioned to catalyze the hydrocarbon formations through electrochemical CO 2 reduction. The catalyst design freedom is limited for alloying copper with H-affinitive elements represented by platinum group metals because the latter would easily drive the hydrogen evolution reaction to override CO 2 reduction. We report an adept design of anchoring atomically dispersed platinum group metal species on both polycrystalline and shape-controlled Cu catalysts, which now promote targeted CO 2 reduction reaction while frustrating the undesired hydrogen evolution reaction. Notably, alloys with similar metal formulations but comprising small platinum or palladium clusters would fail this objective. With an appreciable amount of CO-Pd 1 moieties on copper surfaces, facile CO * hydrogenation to CHO * or CO-CHO * coupling is now viable as one of the main pathways on Cu(111) or Cu(100) to selectively produce CH 4 or C 2 H 4 through Pd-Cu dual-site pathways. The work broadens copper alloying choices for CO 2 reduction in aqueous phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation

Pd-impregnated Ce-based catalysts were tested for carbon monoxide (CO) and hydrocarbon (HC) oxidation under challenging low-temperature diesel combustion conditions. The results indicate that the light-off temperatures for CO over Pd/CeO 2 , Pd/MnO x -CeO 2 (Pd/MC), and Pd/SnO 2 -MnO x -CeO 2 (Pd/SMC) catalysts shift to higher temperatures in the presence of simulated diesel exhaust gas. The lowest T 50 for CO is observed over Pd/MC at 173 °C, whereas Pd/CeO 2 is shown to oxidize most of the HCs at temperatures below 400 °C. In all catalysts, the oxidation of HCs starts right after the onset of CO oxidation, revealing that the competitive adsorption of CO, NO, and alkenes controls the catalytic activity. Further evaluation of the catalytic activity in the presence of only CO and C 3 H 6 reveals the immediate inhibiting effect of C 3 H 6 at catalyst temperatures below 150 °C. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments performed over Pd/CeO 2 , Pd/MC, and Pd/SMC show that C 3 H 6 inhibits the formation of carbonyl species on Pd n+ sites, which limits the catalytic activity for CO. Lastly, such inhibition is observed on all supports, implying that the activity is independent of oxygen storage capacity (OSC) or lattice oxygen reducibility of the supports in the presence of C 3 H 6 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Dose-rate controlled energy dispersive x-ray spectroscopic mapping of the metallic components in a biohybrid nanosystem

In this work, we showcase that through precise control of the electron dose rate, state-of-the-art large solid angle energy dispersive X-ray spectroscopy (EDS) mapping in aberration-corrected scanning transmission electron microscope (STEM) is capable of faithful and unambiguous chemical characterization of the Pt and Pd distribution in a peptide-mediated nanosystem. This low-dose-rate recording scheme adds another dimension of flexibility to the design of elemental mapping experiments, and holds significant potential for extending its application to a wide variety of beam sensitive hybrid nanostructures.

composition mapping↗
DOE OSTI2022

The effects of SO 2 exposure on three-way catalysts for passive SCR operation

We report efficient lean-burn gasoline engines cannot employ traditional three-way catalysts (TWCs) to control NO X emissions due to excess oxygen. Passive selective catalytic reduction (pSCR) is a process designed to control NOx by generating NH 3 over the TWC during fuel-rich operation, storing it on a downstream SCR, and then converting NOx during fuel-lean operation. This work is focused on studying sulfur effects on this promising strategy. Two hydrothermally-aged commercial catalysts were studied for their effectiveness in the presence of SO 2 : a Pd-based TWC and a TWC with NO X storage. The sulfated samples were evaluated in a flow reactor under pSCR conditions and with targeted reactions. SO 2 inhibited the water gas shift and steam reforming reactions, decreasing (but not eliminating) NH 3 production; however, initial activity is recoverable after a simple thermal treatment at 650 °C. This work will prove valuable in understanding, mitigating, and even reversing the effects of SO 2 inhibition on real pSCR systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗