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Li, Xiaxi

Publications and source records attributed to Li, Xiaxi.

7 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

In Situ and Surface-Enhanced Raman Spectroscopy Study of Electrode Materials in Solid Oxide Fuel Cells

Solid oxide fuel cells (SOFCs) represent next-generation energy sources with high energy conversion efficiencies, low pollutant emissions, good flexibility with a wide variety of fuels, and excellent modularity suitable for distributed power generation. As an electrochemical energy conversion device, the SOFC’s performance and reliability depend sensitively on the catalytic activity and stability of electrode materials. To date, however, the development of electrode materials and microstructures is still based largely on trial-and-error methods because of the inadequate understanding of electrode process mechanisms. Therefore, the identification of key descriptors/properties for electrode materials or functional heterogeneous interfaces, especially under in situ/operando conditions, may provide guidance for the design of optimal electrode materials and microstructures. Here, Raman spectroscopy is ideally suited for the probing and mapping of chemical species present on electrode surfaces under operating conditions. And to boost the sensitivity toward electrode surface species, the surface-enhanced Raman spectroscopy (SERS) technique can be employed, in which thermally robust SERS probes (e.g., Ag@SiO 2 core–shell nanoparticles) are designed to make in situ/operando analysis possible. Furthermore, this review summarizes recent progresses in the investigation of SOFC electrode materials through Raman spectroscopic techniques, including topics of early stage carbon deposition (coking), coking-resistant anode modification, sulfur poisoning, and cathode degradation. In addition, future perspectives for utilizing the in situ/operando SERS for investigations of other electrochemical surfaces and interfaces are also discussed.

25 ENERGY STORAGE↗
DOE OSTI2018

An effective strategy to enhancing tolerance to contaminants poisoning of solid oxide fuel cell cathodes

Commercialization of solid oxide fuel cells (SOFCs) is impeded by severe cathode degradation from the poisoning effect of contaminants commonly encountered in air (such as H 2 O and CO 2 ) and from other cell components (e.g., Cr species from chromium-containing interconnector). Here we report our findings in unraveling the mechanism of Cr poisoning of La .6 Sr .4 Co .2 Fe .8 O 3 (LSCF) cathodes using our unique in situ/operando surface enhanced Raman spectroscopy. Further, we present an effective strategy to enhancing the tolerance to contaminants poisoning of LSCF cathode through infiltration of a hybrid catalyst coating, which is composed of a conformal film of perovskite PrNi .5 Mn .5 O 3 (PNM) and exsoluted PrO x nano-particles. The coating is catalytically active to oxygen reduction reaction but inert to contaminant poisoning. When subjected to an accelerated Cr-poisoning test, the cells with a hybrid catalyst-coated LSCF cathode show excellent peak power density (P max of 0.71 Wcm -2 ) and significantly enhanced durability (degradation rate of 0.0434% h -1 at 0.7 V), much better than those of cells with a bare LSCF cathode (P max of ~0.46 Wcm -2 and degradation rate of 0.4% h -1 at 0.7 V). The results suggest that surface modification of electrodes with a coating of rationally designed catalysts is a cost-effective approach to dramatically reducing electrode degradation caused by contaminations.

25 ENERGY STORAGE↗
DOE OSTI2015

Probing the Charge Storage Mechanism of a Pseudocapacitive MnO 2 Electrode Using in Operando Raman Spectroscopy

Although manganese oxide (MnO 2 ) has been extensively studied as an electrode material for pseudocapacitors, a clear understanding of its charge storage mechanism is still lacking. Here we report our findings in probing the structural changes of a thin-film model MnO 2 electrode during cycling using in operando Raman spectroscopy. The spectral features (e.g., band position, intensity, and width) are correlated quantitatively with the size (Li + , Na + , and K + ) of cations in different electrolytes and with the degree of discharge to gain better understanding of the cation-incorporation mechanism into the interlayers of pseudocapacitive MnO 2 . Also, theoretical calculations of phonon energy associated with the models of interlayer cation-incorporated MnO 2 agree with the experimental observations of cation-size effect on the positions of Raman bands. Additionally, the cation-size effects on spectral features at different potentials of MnO 2 electrode are correlated quantitatively with the amount of charge stored in the MnO 2 electrode. The understanding of the structural changes associated with charge storage gained from Raman spectroscopy provides valuable insights into the cation-size effects on the electrochemical performances of the MnO 2 electrode.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electrostatic Force Microscopic Characterization of Early Stage Carbon Deposition on Nickel Anodes in Solid Oxide Fuel Cells

Carbon deposition on nickel anodes degrades the performance of solid oxide fuel cells that utilize hydrocarbon fuels. Nickel anodes with BaO nanoclusters deposited on the surface exhibit improved performance by delaying carbon deposition (i.e., coking). Here, the goal of this research was to visualize early stage deposition of carbon on nickel surface and to identify the role BaO nanoclusters play in coking resistance. Electrostatic force microscopy was employed to spatially map carbon deposition on nickel foils patterned with BaO nanoclusters. Image analysis reveals that upon propane exposure initial carbon deposition occurs on the Ni surface at a distance from the BaO features. With continued exposure, carbon deposits penetrate into the BaO-modified regions. After extended exposure, carbon accumulates on and covers BaO. The morphology and spatial distribution of deposited carbon was found to be sensitive to experimental conditions.

25 ENERGY STORAGE↗
DOE OSTI2015

An operando surface enhanced Raman spectroscopy (SERS) study of carbon deposition on SOFC anodes

Thermally robust and chemically inert Ag@SiO 2 nanoprobes are employed to provide the surface enhanced Raman scattering (SERS) effect for an in situ/operando study of the early stage of carbon deposition on nickel-based solid oxide fuel cell (SOFC) anodes. The enhanced sensitivity to carbon enables the detection of different stages of coking, offering insights into intrinsic coking tolerance of material surfaces. Application of a thin coating of gadolinium doped ceria (GDC) enhances the resistance to coking of nickel surfaces. The electrochemically active Ni–YSZ interface appears to be more active for hydrocarbon reforming, resulting in the accumulation of different hydrocarbon molecules, which can be readily removed upon the application of an anodic current. Operando SERS is a powerful tool for the mechanistic study of coking in SOFC systems. It is also applicable to the study of other catalytic and electrochemical processes in a wide range of conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗