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At least 1,117 records · Page 62
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Electrochemistry of PUREX: R is for Reduction and Ion Transfer

The PUREX (Plutonium, Uranium, Reduction, EXtraction) process is the foundation of all industrial activities that involve the recycling of plutonium and uranium from used nuclear fuel. With over 70 years of research, engineering, and operations, it can be argued that little opportunity is left for further discovery and new fundamental understandings regarding PUREX, in general, and tri-n-butyl phosphate (TBP), in particular. Through use of an advanced electroanalytical approach, molecular-level insights regarding the back-extraction of Pu(IV) by reductive separation is reported. Studies of model PUREX systems, with lanthanide ions extracted into 20 % TBP in n-dodecane, are used to demonstrate the approach. These studies reveal knowledge pertinent to mass transfer aspects of the biphasic reductive stripping reaction central to the separation of U and Pu in PUREX. Two lanthanide ions—Ce(IV) and Yb(III)—were extracted from their concentrated solutions in aqueous 3 M HNO 3 to expressly provide electrically conducting third phases to facilitate electrochemical data acquisition. To simplify the diabolically-complicated reductive separation aspects of PUREX, the controlled polarization of electrode surfaces was used to reduce Ce(IV) and Yb(III) in place of chemical reductants. Electroanalyses of the biphasic systems with Ce(IV) and Yb(III) using three-phase electrode differential pulse voltammetry demonstrate the effects of mass transfer across water-oil interfaces on the electrode potentials for the reduction to Ce(III) and Yb(II). These reductions trigger nitrate transfer out of the oil phase for Ce and proton transfer into the organic phase for Yb. This is in correlation with the transfer of the charge-neutral ion pairs Ce·3NO 3 and Yb·2NO 3 out of the oil phases. Here, the differences in ion transfer steps reflect significant variations in the equilibrium speciation of multinuclear Ce(IV) and mononuclear Yb(III) solvates of TBP in the oil phases and the loading of the organic phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Creating Favorable Pt/Co Interfaces via a Two‐Step Approach for Constructing Highly Durable PtCo Intermetallic Fuel Cell Catalysts

Structurally ordered PtCo intermetallics are one of the most promising oxygen-reduction catalysts in proton exchange membrane fuel cells (PEMFCs) due to their intrinsically improved catalytic activity and stability relative to PtCo solid-solution alloys. However, increasing the heating temperature to achieve a desirable high degree of ordering results in severe particle agglomeration and low mass activity and stability. Herein, a two-step synthesis approach is developed to create an L1 2 -Pt 3 Co intermetallic structure with an increased ordering degree and well-dispersed ultrafine particles. The first step of the synthesis yields ultrafine Pt nanoparticles that are well-dispersed on the ZIF-8-derived carbon support. The second adsorption step enables us to fine-tune the Pt and Co interfaces, assisted by optimal amino acids, to establish a favorable Co-rich environment around fine Pt nanoparticles, facilitating Co diffusion into the Pt crystalline under mild thermal conditions (<800 °C). In conclusion, this two-step ordered L1 2 -Pt 3 Co catalyst is systematically evaluated using membrane electrode assemblies under heavy-duty vehicle (HDV) conditions and demonstrated exceptional performance and durability, retaining 1.35 A cm -2 only a 7% loss in current density at 0.7 V after an extensive accelerated stress test of 150,000 voltage cycles.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2025

Electrocatalytic Ammonia Oxidation by Pyridyl-Substituted Ferrocenes

Ammonia (NH 3 ) is a promising carbon-free fuel when prepared from sustainable resources. First-row transition metal electrocatalysts for ammonia oxidation are an enabling technology for sustainable energy production. We describe electrocatalytic ammonia oxidation using robust molecular complexes based on Earth-abundant iron. Electrochemical studies of ferrocenes with covalently attached pyridine arms reveal facile ammonia oxidation in DMSO (2.4 M NH 3 ) with modest overpotentials (η = 770–820 mV) and turnover frequencies (125–560 h –1 ). Experimental and computational studies indicate that the pendant pyridyl base serves as an H-bond acceptor with an N–H bond of ammonia that transfers a proton to the pyridine following oxidation by the attached ferrocenium moiety in a proton-coupled electron transfer (PCET) step. This generates an amidyl (•NH 2 ) radical stabilized via H-bonding to a pendant pyridinium moiety that rapidly dimerizes to hydrazine (H 2 N–NH 2 ), which is easily oxidized to nitrogen (N 2 ) at the glassy carbon working electrode. This report identifies a general strategy to oxidize ammonia via H-bonding to a base (B:), thereby activating [B···H-NH 2 ] toward PCET by a proximal oxidant to form [BH···NH 2 ] +/• radical cations, which are susceptible to dimerization to form easily oxidized hydrazine.

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

Improving Performance and Durability of Low Temperature Direct Ammonia Fuel Cells: Effect of Backpressure and Oxygen Reduction Catalysts

Low temperature direct ammonia fuel cells (DAFCs) are attractive for transportation applications. The primary obstacle to their commercial use is their low performance and poor durability. In the present work, we focus on improving DAFCs performance and durability by examining the effect of operating backpressure and oxygen reduction reaction (ORR) catalysts such as Acta 4020, Pd/C and Pt/C. DAFCs with Acta 4020 cathode can reach a peak power density of 390 mW cm -2 which is among the best reported performance, but they can be operated for a period of 11 h at 300 mA cm -2 . DAFCs with Pd/C cathode offer a moderate performance with a peak power density of 304 mW cm -2 , but has a much improved durability - a continuous operation for up to 36 h with a slow decay rate of ~1 mV h -1 at 300 mA cm -2 . In addition, the degradation pathways for DAFCs with Pd/C cathode are probed by characterizing the initial and final electrodes by XPS, suggesting that cathodic Pd dissolution occurs during the durability test.

Electrochemistry↗
DOE OSTI2022

A case study of high-temperature polyetherimide film capacitor fabrication

Capacitors, as the basic building block of power electronics and electrical systems, are the major constraint of the increasingly integrated power systems that require new capable polymer dielectric films operating at higher temperatures >125 °C. Despite tremendous research efforts on the lab scale, there remains a considerable barrier and knowledge basis for converting polymeric films to functioning capacitors desired in actual applications. Here, the authors tackled the polyetherimide (PEI) film scale up issues and developed various engineering processes for film de-wrinkling, optimal metallization, static elimination, and capacitor fabrication improvement. The authors discovered various fabrication challenges such as the electrostatic charge, metallization scheme, winding tension, and end electrode disconnects. To fabricate a high yield of PEI capacitor bobbins, it is necessary to utilize static eliminators (radioactive ionizers), moderately thick aluminum metallization (15–30 Ω/sq), and winding tension (60–100 g). It is also effective to evaluate capacitance, dielectric loss, equivalent series resistance, and thermal cycling stability of capacitors. This work sheds some light on converting PEI films and other polymeric films to capacitors on a scale up fabrication effort. The practical learning from film handling to capacitor fabrication in this work provided the necessary knowledge for manufacturing high-temperature polar film capacitors.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Operational and scaling-up barriers of SOEC and mitigation strategies to boost H 2 production- a comprehensive review

Solid oxide electrolysis cells (SOECs) proffer a flexible and environmentally friendly solution to reduce CO 2 emissions and/or produce H 2 fuel for various applications. Here, the integration of this technology with renewable energy systems makes them even more promising in realizing a near-perpetual green energy infrastructure in the near future. SOEC technology has achieved stupendous improvement in recent years, and some of the limiting factors to the commercialization of this technology have been explored. It is, therefore, necessary to have a succinct outlook of the different factors that contribute to the recent developments in SOEC technology. The current work presents a comprehensive review of the state-of-the-art SOEC component materials and their degradation mechanisms, SOEC modeling essentials and efficiencies, and the scalability of SOECs. Although SOEC is considered a highly promising technology and sufficient multifaceted research has been done, yet not been widely commercialized. Despite the improvement to mitigate degradation of the SOEC materials, a large share of the degradation concerns sprang from charge transfer reaction at the triple-phase boundaries of the H 2 -electrode. Part of which can be improved by microkinetic modeling of these materials supported by their characterization to give insight into their development. Some other directions for the future in advancing this technology toward the commercialization stage are thoroughly addressed.

08 HYDROGEN↗
DOE OSTI2022

Understanding Mass Transport in Copper Electrolyte-Based Dye-Sensitized Solar Cells

Copper redox shuttles, particularly [Cu(tmby) 2 ] 2+/1+ (tmby = bis(4,4',6,6'-tetramethyl-2,2'-bipyridine)), proved to be among the best electrolytes for dye-sensitized solar cells (DSCs), realizing higher power conversion efficiencies both under full sun and indoor illumination than conventional iodide/triiodide and cobalt electrolytes. Even though [Cu(tmby) 2 ] 2+/1+ renders a relatively higher performance, this metal complex is bulky and is limited by mass transport. Since the regeneration of the dye ground state by Cu I and the reaction of Cu II at the counter electrode are comparatively faster processes, the efficiency of DSC involving Cu I /Cu II electrolytes under relatively high light intensities is largely governed by the diffusion of Cu I /Cu II species. Understanding mass transport in these solar cells will enable further improvements in the performance of such copper-based DSCs. Here in the present study, the role of illumination intensity on the photogenerated current and its relationship to mass transport is evaluated using the best cosensitized dye (D35:XY1) and copper electrolyte ([Cu(tmby) 2 ] 2+/1+ ) combination.

14 SOLAR ENERGY↗
NASA NTRS1992

Catalysts for ultrahigh current density oxygen cathodes for space fuel cell applications

The objective was to identify promising electrocatalyst/support systems for oxygen cathodes capable of operating at ultrahigh current densities in alkaline fuel cells. Such cells will require operation at relatively high temperatures and O2 pressures. A number of materials were prepared, including Pb-Ru and Pb-Ir pyrochlores, RuO2 and Pt-doped RuO2, lithiated NiO and La-Ni perovskites. Several of these materials were prepared using techniques that had not been previously used to prepare them. Particularly interesting was the use of the alkaline solution technique to prepare Pt-doped and Pb-Ru pyrochlores in high area form. Also interesting was the use of the fusion (melt) method for preparing the Pb-Ru pyrochlore. Several of the materials were also deposited with platinum. Well-crystallized Pb2Ru2O(7-y) was used to fabricate very high performance O2 cathodes with good stability in room temperature KOH. This material was also found to be stable over a useful potential range at approx. 140 C in concentrated KOH. For some of the samples, fabrication of the gas-fed electrodes could not be fully optimized during this project period. Future work may be directed at this problem. Pyrochlores that were not well-crystallized were found to be unstable in alkaline solution. Very good O2 reduction performance and stability were observed with Pb2RuO(7-y) in a carbon-based gas-fed electrode with an anion-conducting membrane placed on the electrolyte side of the electrode. The performance came within a factor of about two of that observed without carbon. High area platinum and gold supported on several conductive metal oxide supports were examined. Only small improvements in O2 reduction performance at room temperature were observed for Pb2Ru2O(7-y) as a support because of the high intrinsic activity of the pyrochlore. In contrast, a large improvement was observed for Li-doped NiO as a support for Pt. Very poor performance was observed for Au deposited on Li-NiO at approx. 150 C. Nearly reversible behavior was observed for the O2/OH(-) couple for Li-doped NiO at approx. 200 C. The temperature dependence for the O2 reduction was examined.

Tryk, Donald A.↗
DOE OSTI2023

Ionomer-free and recyclable porous-transport electrode for high-performing proton-exchange-membrane water electrolysis

Abstract Clean hydrogen production requires large-scale deployment of water-electrolysis technologies, particularly proton-exchange-membrane water electrolyzers (PEMWEs). However, as iridium-based electrocatalysts remain the only practical option for PEMWEs, their low abundance will become a bottleneck for a sustainable hydrogen economy. Herein, we propose high-performing and durable ionomer-free porous transport electrodes (PTEs) with facile recycling features enabling Ir thrifting and reclamation. The ionomer-free porous transport electrodes offer a practical pathway to investigate the role of ionomer in the catalyst layer and, from microelectrode measurements, point to an ionomer poisoning effect for the oxygen evolution reaction. The ionomer-free porous transport electrodes demonstrate a voltage reduction of > 600 mV compared to conventional ionomer-coated porous transport electrodes at 1.8 A cm −2 and <0.1 mg Ir cm −2 , and a voltage degradation of 29 mV at average rate of 0.58 mV per 1000-cycles after 50k cycles of accelerated-stress tests at 4 A cm −2 . Moreover, the ionomer-free feature enables facile recycling of multiple components of PEMWEs, which is critical to a circular clean hydrogen economy.

08 HYDROGEN↗
DOE OSTI2022

Developing reactors for electrifying bio-methanation: a perspective from bio-electrochemistry

The integration of microbial synthesis with renewable electricity is an emerging route for both CO 2 utilization and seasonal energy storage in the form of stored bio-electrofuels. The major benefits of electrifying bioreactors include: using highly selective bio-catalysts for CO 2 conversion under mild reaction conditions; decoupling the production of more facile electrochemical intermediates, such as hydrogen, at the electrode from the production of bio-catalyzed multi-electron and/or carbon products, such as methane or acetate; using microbes as robust and self-regenerating catalysts enabling higher efficiency and durability in CO 2 conversion systems compared to inorganic catalysis. In this Perspective, we propose research aimed at developing electro-bioreactor components that will increase the productivity of the reactor while maintaining high energy efficiency and biocompatible reaction conditions to fully realize the benefits of electrified bioreactors. Furthermore, these developments include: flow reactors with tailored 3D electrodes to optimally use the reactor volume, electrocatalysts designed for peak performance in neutral pH electrolytes, high conductivity microbial media, and new membrane separator materials with high ion conductivity and low gas permeability. Production of methane via a hybrid electrical-biological approach is taken as a case study to motivate these developments. Finally, an iterative design–manufacture–test cycle, enabled by additive manufacturing and 3D printing technologies, is proposed to rapidly prototype components prior to large-scale manufacturing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Longevity evaluation of SiC based alpha voltaic batteries with surface alpha sources

The alpha emitting actinide 241 Am is electrodeposited on the surface of the Pt electrode of in-house fabricated SiC Schottky diodes. With 17 nCi 241 Am directly coated on the top of a device, the 2-pi geometry yields a high energy (5.486 MeV) and a long-term irradiation accumulating to a high fluence (1.6 × 10 9 alpha particles’ infusion/month). The forward, reverse I/V, and dark current, are periodically measured to monitor key characteristics of device durability for any sign of degradation over time. The direct deposition of actinides on the surface of the device also enables the evaluation of radiation damage through alpha particles’ energy spectroscopic performance, which shows a clear spectrum degradation that can be reversed by optical excitation of the device prior to spectrum acquisition. As an analytical aide, the device performance is also simulated by Allpix 2 . Lastly, this study provides an insight into the durability of 4H-SiC as an energy converter option for alpha-voltaic batteries and the survivability in the other harsh environment found in nuclear fuel cycle, high energy physics, fission, fusion, and space exploration where rad-hard sensors are required.

Americium↗
DOE OSTI2025

Long-Range Resonant Charge Transport through Open-Shell Donor–Acceptor Macromolecules

A grand challenge in molecular electronics is the development of molecular materials that can facilitate efficient longrange charge transport. Research spanning more than two decades has been fueled by the prospects of creating a new generation of miniaturized electronic technologies based on molecules whose synthetic tunability offers tailored electronic properties and functions unattainable with conventional electronic materials. However, current design paradigms produce molecules that exhibit off-resonant transport under low bias, which limits the conductance of molecular materials to unsatisfactorily low levels several orders of magnitude below the conductance quantum 1 G 0 and often results in an exponential decay in conductance with length. Here, we demonstrate a chemically robust, air-stable, and highly tunable molecular wire platform comprised of open-shell donor−acceptor macromolecules that exhibit remarkably high conductance close to 1 G 0 over a length surpassing 20 nm under low bias, with no discernible decay with length. Single-molecule transport measurements and ab initio calculations show that the ultralong-range resonant transport arises from extended π-conjugation, a narrow bandgap, and diradical character, which synergistically enables excellent alignment of frontier molecular orbitals with the electrode Fermi energy. The implementation of this long-sought-after transport regime within molecular materials offers new opportunities for the integration of manifold properties within emerging nanoelectronic technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Gradient synthesis of carbon quantum dots and activated carbon from pulp black liquor for photocatalytic hydrogen evolution and supercapacitor

Black liquor (BL) is a by-product of the chemical pulping industry and is mainly used as a low-value fuel; however, its potential to produce high-value products has not been fully exploited. In this study, a green and simple strategy is reported for the gradient production of Na + -functionalized carbon quantum dots (Na + -CQDs) for the first time, N and S co-doped CQDs (N/S-CQDs), and N and S co-doped KOH-activated carbon (N/S-KAC) from BL by dialysis, hydrothermal carbonization and activation-carbonization, respectively. Due to the good electron trapping ability, photoluminescence and promising up-conversion luminescence of CQDs, the hydrogen evolution efficiency of Na + -CQDs/TiO 2 and N/S-CQDs/TiO 2 photocatalysts was improved by 2.45 and 1.46 times, respectively, compared with pure TiO 2 . N/S-KAC with a high specific surface area of 2294 m 2 g -1 provides an excellent specific capacitance of 253 F g -1 at 0.5 A g -1 and a promising energy density of 26.92 Wh kg -1 under a power density of 566 W kg -1 for the fabricated symmetrical supercapacitor. Moreover, the electrode material has good cycling stability with a capacitance retention of ~ 93.91% after 5000 cycles. In conclusion, this pathway provides a versatile and scalable approach for the construction and co-production of nanostructured materials, photocatalysts and energy storage devices.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Fluorine-Tuned Carbon-Based Nickel Single-Atom Catalysts for Scalable and Highly Efficient CO 2 Electrocatalytic Reduction

Electrocatalytic CO 2 reduction is garnering significant interest due to its potential applications in mitigating CO 2 and producing fuel. However, the scaling up of related catalysis is still hindered by several challenges, including the cost of the catalytic materials, low selectivity, small current densities to maintain desirable selectivity. In this study, Fluorine (F) atoms were introduced into an N-doped carbon-supported single nickel (Ni) atom catalyst via facile polymer-assisted pyrolysis. This method not only maintains the high atom utilization efficiency of Ni in a cost-effective and sustainable manner but also effectively manipulates the electronic structure of the active Ni-N 4 site through F doping. The catalyst has also been further optimized by controlling the F states, including convalent and semi-ionic states, by adjusting the fluorine sources involved. Consequently, this catalyst with unique structure exhibited comparable electrocatalytic performance for CO 2 -to-CO conversion, achieving a Faradaic efficiency (FE) of over 99% across a wide potential range and an exceptional CO evolution rate of 9.5 x 10 4 h -1 at -1.16 V vs reversible hydrogen electrode (RHE). It also delivered a practical current of 400 mA cm -2 while maintaining more than 95% CO FE. Experimental analysis combined with density functional theory (DFT) calculations have also shown that F-doping modifies the electron configuration at the central Ni-N 4 sites. In conclusion, this modification lowers the energy barrier for CO 2 activation, thereby facilitating the production of the crucial *COOH intermediate.

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

N-Doped Graphene (N-G)/MOF(ZIF-8)-Based/Derived Materials for Electrochemical Energy Applications: Synthesis, Characteristics, and Functionality

In recent years, graphene-type materials originating from metal–organic frameworks (MOFs) or integrated with MOFs have exhibited notable performances across various applications. However, a comprehensive understanding of these complex materials and their functionalities remains obscure. While some studies have reviewed graphene/MOF composites from different perspectives, due to their structural–functional intricacies, it is crucial to conduct more in-depth reviews focusing on specific sets of graphene/MOF composites designed for particular applications. In this review, we thoroughly investigate the syntheses, characteristics, and performances of N-G/MOF(ZIF-8)-based/derived materials employed in electrochemical energy conversion and storage systems. Special attention is given to realizing their fundamental functionalities. The discussions are divided into three segments based on the application of N-G/ZIF-8-based/derived materials as electrode materials for batteries, electrodes for electrochemical capacitors, and electrocatalysts. As electrodes for batteries, N-G/MOF(ZIF-8) materials can mitigate issues like an electrode volume expansion for Li-ion batteries and the ‘shuttle effect’ for Li-S batteries. As electrodes for electrochemical capacitors, these materials can considerably improve the ion transfer rate and electronic conductivity, thereby enhancing the specific capacitance while maintaining the structural stability. Also, it was observed that these materials could occasionally outperform standard platinum-based catalysts for the electrochemical oxygen reduction reaction (ORR). The reported electrochemical performances and structural parameters of these materials were carefully tabulated in uniform units and scales. Through a critical analysis of the present synthesis trends, characteristics, and functionalities of these materials, specific aspects were identified that required further exploration to fully utilize their inherent capabilities.

Electrochemistry↗
DOE OSTI2024

Computational modeling of coupled mechanical damage and electrochemistry in ternary oxide composite electrodes

Performance degradation of ternary layered oxide cathodes largely originates from their loss of structural integrity in cyclic usage. Mechanical damage, such as intergranular fracture of the active particles, is not only a mechanical cleavage process but also interferes with electrochemical kinetics such as infiltration of liquid electrolyte, surface corrosion of the constituent primary particles, and may eventually isolate the primary grains from the electron conducting network. Here, in this work, we develop a computational framework that integrates electrochemistry of a LiNi x Mn y Co 1−x−y O 2 (NMC) composite cathode with mechanical damage of the active particles. To fully examine the intricate chemomechanical behavior of the electrode, we evaluate the effects of the anisotropic material properties, the influence of mechanical potential on Li transport, and the concurrent intergranular fracture and electrolyte penetration along the grain boundaries upon multiple cycles. Electrolyte infiltration benefits capacity retention but aggravates further mechanical damage by corrosion. Structural failure mostly occurs in the first charging due to the anisotropic mechanical strain between the primary grains, while the resulting damage remains stable in the later few cycles. The results are consistent with experimental observations and the integration of electrochemistry and mechanical failure enables a step further understanding of the complex mechanism of battery degradation.

Battery degradation↗
DOE OSTI2020

Photo-cleaned Backgroundless Ion Chambers (Final Report for PDRD SR18010)

Ion chambers are often employed to measure the concentration of tritium within flowing gases. In real world environments the active surfaces of ion chambers become covered with tritiated surface contaminants. This tritiated surface contamination will create a large background response that can mask the signature of interest, which is the tritium concentration in the gas phase. Previous efforts to reduce the effects of surface contamination in ion chambers utilize inert coatings (e.g., gold) and low surface area electrodes (e.g., wire mesh), but this route only reduces the effect and does not necessarily alter the ratio of surface contamination to current collection area. Additionally, gold coating may add a substantial cost to the instrument. In the Tritium Facility, ion chambers are periodically cleaned using an alcohol-based process. This process is time consuming and often leads to ion chamber wear and breakage. In addition, periodic cleaning does not address tritium level ambiguities in gloveboxes. An ideal solution to this issue would be to either develop an ion chamber that does not accrue surface contamination, or one that is self-cleaning while it is in operation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

High Performance SOFCs with a Superior Stability for Reliable and Durable Power Systems

Next generation of fuel cells, electrolyzers, and batteries requires higher power, faster kinetics, and larger energy density, which necessitate the use of compositionally complex oxides to achieve multifunctionalities and activity. These compositionally complex oxides may change their phases and structures during an electrochemical process – a so-called “electrochemically driven phase transformation”. The origin for such a phase change has remained obscure. More importantly, there is a need to develop high performance solid oxide fuel cells with an enhanced stability. In this work, the La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3 (LSCF) cathode surface is modified by infiltration of Pr 6 O 11 and the power density at 0.8V and 750 °C is improved by 21%. In addition, by replacing the traditional barrier layer Gd 0.2 Ce 0.8 O 1.9 with mixed conducting Pr 0.1 Gd 0.1 Ce 0.8 O 1.9 , the power density increases by 38%. The different mechanism of promotions was investigated by electrochemical impedance spectroscopy. The ohmic resistance is dramatically reduced by applying the PGCO interlayer, and the distribution of relaxation time was used to analyze the mechanism for which the polarization resistance was decreased attributing to the mixed conduction nature in PrO x . An increase of power density at 0.8 V of 0.358 W/cm 2 (71%) is achieved with the implementation of both surface modification and buffer layer engineering. An experimental study and a theoretical analysis were then carried out on phase evolution in praseodymium nickelates. Nickelate-based electrodes show up to 60× greater phase transformation during operation when compared to thermally annealed ones. Theoretical analysis suggests that the presence of a reduced oxygen partial pressure at the interface between the oxygen electrode and the electrolyte is the origin for the phase change in an oxygen electrode. Guided by the theory, an addition of the electronic conduction in the interface layer leads to the significant suppression of phase change, while improving cell performance and performance stability. When an oxygen electrode is under polarization, the oxygen partial pressure at the interface between the oxygen electrode and the electrolyte is lower than that of incoming oxidant. Under a high polarization, the environment at the aforementioned interface may lead to phase transformation of the oxygen electrode. The local oxygen partial pressure is determined by the transport properties at the interfaces. An addition of the electronic conduction in the interface layer, for instance using (Pr,Gd)-doped ceria to replace Gd-doped ceria, results in improved cell performance and performance stability, while the phase transformation is significantly suppressed. This work provides a fundamental understanding of the origin for phase transformation in oxygen electrodes during operation and use this knowledge to develop a high-performance electrode that exhibits improved performance stability.

30 DIRECT ENERGY CONVERSION↗