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1. Fabrication and preliminary testing of patterned silver cathodes for proton conducting IT-SOFCs

   https://doi.org/10.1039/D3MA00793F  

   Sozal, Md Shariful; Li, Wenhao; Das, Suprabha; Jafarizadeh, Borzooye; Chowdhury, Azmal Huda; Wang, Chunlei; Cheng, Zhe (January 2024, Materials Advances)

   Dense silver (Ag) cathodes with defined triple phase boundary (TPB between the interface of electrolyte, electrode, and gas) lengths (LTPB) and electrode areas (AELT) were fabricated by photolithography and E-beam evaporation over a proton conducting BaZr0.4Ce0.4Y0.1Yb0.1O3−δ (BZCYYb4411) electrolyte. A bi-layer lift-off resist method appears to be more versatile than a single layer lift-off resist method for successful patterned cathode fabrication. The electrochemical behaviors of the patterned Ag cathodes over the BZCYYb4411 electrolyte were tested by electrochemical impedance spectroscopy (EIS) at different temperatures in atmospheres with different concentrations of O2 and H2O. The results were processed using Distribution of Relaxation Times (DRT) and reaction order analyses and also fitted to equivalent circuits. The directions for future work on patterned electrodes with different LTPB and AELT and theoretical calculations to gain further insights into the kinetics and mechanism of the cathode oxygen reduction reaction (ORR) over proton conducting electrolytes are pointed out. 

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2. A Novel Self‐Assembled Cobalt‐Free Perovskite Composite Cathode with Triple‐Conduction for Intermediate Proton‐Conducting Solid Oxide Fuel Cells

   https://doi.org/10.1002/adfm.202209695  

   Tong, Hua; Fu, Min; Yang, Yang; Chen, Fanglin; Tao, Zetian (September 2022, Advanced Functional Materials)

   Abstract A traditional composite cathode for proton‐conducting solid oxide fuel cells (H‐SOFCs) is typically obtained by mixing cathode materials and proton conducting electrolyte of BaCe_0.7Y_0.2Zr_0.1O_3–δ(BZCY), providing chemical and thermal compatibility with the electrolyte. Here, a series of triple‐conducing and cobalt‐free iron‐based perovskites as cathodes for H‐SOFCs is reported. Specifically, BaCe_xFe_1–xO_3–δ(x = 0.36, 0.43, and 0.50) shows various contents of two single phase perovskites with an in situ heterojunction structure as well as triple conductivity by tailoring the Ce/Fe ratios. The cell performance with the optimized BaCe_0.36Fe_0.64O_3–δ(BCF36) cathode composition reaches 1056 mW cm⁻²at 700 °C. Moreover, a record cell performance of 1525 mW cm⁻²at 700 °C is obtained by modifying the BCF36 cathode microstructure through a spraying method, demonstrating high promise with Co‐free cathodes for H‐SOFCs. 

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3. Universal Cathode Design Strategies to Engineer Cathode Electrolyte Interfaces for High Performance All-Solid-State Batteries

   Zhang, Yuxuan; Song, Han Wook; Lee, Sunghwan (May 2022, Materials Research Society)

   Metal-ion batteries (e.g., lithium and sodium ion batteries) are the promising power sources for portable electronics, electric vehicles, and smart grids. Recent metal-ion batteries with organic liquid electrolytes still suffer from safety issues regarding inflammability and insufficient lifetime.1 As the next generation energy storage devices, all-solid-state batteries (ASSBs) have promising potentials for the improved safety, higher energy density, and longer cycle life than conventional Li-ion batteries.2 The nonflammable solid electrolytes (SEs), where only Li ions are mobile, could prevent battery combustion and explosion since the side reactions that cause safety issues as well as degradation of the battery performance are largely suppressed. However, their practical application is hampered by the high resistance arising at the solid–solid electrode–electrolyte interface (including cathode-electrolyte interface and anode-electrolyte interface).3 Several methods have been introduced to optimize the contact capability as well as the electrochemical/chemical stability between the metal anodes (i.e.: Li and Na) and the SEs, which exhibited decent results in decreasing the charge transfer resistance and broadening the range of the stable energy window (i.e., lowing the chemical potential of metal anode below the highest occupied molecular orbital of the SEs).4 Nevertheless, mitigation for the cathode in ASSB is tardily developed because: (1) the porous structure of the cathode is hard to be infiltrated by SEs;5 (2) SEs would be oxidized and decomposed by the high valence state elements at the surface of the cathode at high state of charge.5 Herein, we demonstrate a universal cathode design strategy to achieve superior contact capability and high electrochemical/chemical stability with SEs. Stereolithography is adopted as a manufacturing technique to realize a hierarchical three-dimensional (HTD) electrode architecture with micro-size channels, which is expected to provide larger contact areas with SEs. Then, the manufactured cathode is sintered at 700 °C in a reducing atmosphere (e.g.: H2) to accomplish the carbonization of the resin, delivering sufficiently high electronic conductivity for the cathode. To avoid the direct exposure of the cathode active materials to the SEs, oxidative chemical vapor deposition technique (oCVD) is leveraged to build conformal and highly conducting poly(3,4-ethylenedioxythiophene) (PEDOT) on the surface of the HTD cathode.6 To demonstrate our design strategy, both NCM811 and Na3V2(PO4)3 is selected as active materials in the HTD cathode, then each cathode is paired with organic (polyacrylonitrile-based) and inorganic (sulfur-based) SEs assembled into two batteries (total four batteries). SEM and TEM reveal the micro-size HTD structure with built-in channels. Featured by the HTD architecture, the intrinsic kinetic and thermodynamic conditions will be enhanced by larger surface contact areas, more active sites, improved infusion and electrolyte ion accessibility, and larger volume expansion capability. Disclosed by X-ray computed tomography, the interface between cathode and SEs in the four modified samples demonstrates higher homogeneity at the interface between the cathode and SEs than that of all other pristine samples. Atomic force microscopy is employed to measure the potential image of the cross-sectional interface by the peak force tapping mode. The average potential of modified samples is lower than that of pristine samples, which confirms a weakened space charge layer by the enhanced contact capability. In addition, through Electron Energy Loss Spectroscopy coupled with Scanning Transmission Electron Microscopy, the preserved interface between HTD cathode and SE is identified; however, the decomposing of the pristine cathode is clearly observed. In addition, Finite element method simulations validate that the diffusion dynamics of lithium ions is favored by HTD structure. Such a demonstrated universal strategy provides a new guideline to engineer cathode electrolyte interface by reconstructing electrode structures that can be applicable to all solid-state batteries in a wide range of chemical conditions. 

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4. Progress in proton‐conducting oxides as electrolytes for low‐temperature solid oxide fuel cells: From materials to devices

   https://doi.org/10.1002/ese3.886  

   Zhang, Wei; Hu, Yun_Hang (March 2021, Energy Science & Engineering)

   Abstract Among various types of alternative energy devices, solid oxide fuel cells (SOFCs) operating at low temperatures (300‐600°C) show the advantages for both stationary and mobile electricity production. Proton‐conducting oxides as electrolyte materials play a critical role in the low‐temperature SOFCs (LT‐SOFCs). This review summarizes progress in proton‐conducting solid oxide electrolytes for LT‐SOFCs from materials to devices, with emphases on (1) strategies that have been proposed to tune the structures and properties of proton‐conducting oxides and ceramics, (2) techniques that have been employed for improving the performance of the protonic ceramic‐based SOFCs (known as PCFCs), and (3) challenges and opportunities in the development of proton‐conducting electrolyte‐based PCFCs. 

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5. Beyond Composition: Surface Reactivity and Structural Arrangement of the Cathode–Electrolyte Interphase

   https://doi.org/10.1021/acsenergylett.3c01529  

   Hestenes, Julia C; Marbella, Lauren E (November 2023, ACS Energy Letters)

   The role of the cathode–electrolyte interphase (CEI) on battery performance has been historically overlooked due to the anodic stability of carbonate-based electrolytes used in Li-ion batteries. Yet, over the past few decades, degradation in device lifetime has been attributed to cathode surface reactivity, ion transport at the cathode/electrolyte interface, and structural transformations that occur at the cathode surface. In this review, we highlight recent progress in analytical techniques that have facilitated these insights and elucidated not only the CEI composition but also the spatial distribution of electrolyte decomposition products in the CEI as well as cathode-driven reactions that occur during battery operation. With a deeper understanding of the CEI and the processes that lead to its formation, these advanced characterization tools can unlock routes to mitigate impedance rise, particle cracking, transition metal dissolution, and electrolyte consumption, ultimately enabling longer lasting, safer batteries. 

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