ACS Applied Energy Materials最新文献

{"title":"Performance Limitations of CaCoSO as a Positive Electrode Material for Calcium Storage","authors":"Da Tie,&nbsp;Petru Apostol,&nbsp;Mengyuan Du,&nbsp;Zhao Li,&nbsp;Xiaodong Lin,&nbsp;Shubhadeep Pal,&nbsp;Robert Markowski,&nbsp;Xiaolong Guo,&nbsp;Hewei Xu,&nbsp;Andrii Kachmar,&nbsp;Vasudeva Rao Bakuru,&nbsp;Darsi Rambabu,&nbsp;Yinghui Zhang,&nbsp;Fang Xia,&nbsp;Yaroslav Filinchuk,&nbsp;Jean-François Gohy and Alexandru Vlad*,&nbsp;","doi":"10.1021/acsaem.4c0328810.1021/acsaem.4c03288","DOIUrl":"https://doi.org/10.1021/acsaem.4c03288https://doi.org/10.1021/acsaem.4c03288","url":null,"abstract":"<p >Calcium metal batteries (CMBs) are promising candidates for next-generation electrochemical energy storage systems due to their high volumetric capacity, abundance, sustainability, and safety. Recent DFT predictions suggested that the layered CaCoSO phase can enable sequential Co²⁺/Co³⁺ and Co³⁺/Co⁴⁺ redox activity at an average potential of 2.8 V vs Ca²⁺/Ca, making it a promising candidate for high-energy-density CMBs [<contrib-group><span>Torres, A.</span></contrib-group> <cite><i>Chem. Mater.</i></cite> <span>2021</span>, <em>33</em>(7), 2488–2497]. Inspired by these metrics, in this work, we present the synthesis and electrochemical analysis of the CaCoSO phase. Theoretical capacity can be extracted through galvanostatic cycling, albeit accompanied by high polarization. <i>In situ</i> XRD and DEMS analyses, however, reveal that the capacity arises primarily from a combination of material decomposition and electrolyte degradation rather than reversible Ca²⁺ ion storage. The apparent discharge capacity is attributed to the cathodic decomposition of generated water during the subsequent anodic step, making the overall electrochemical process appear as reversible. This work underscores the complexity of achieving stable calcium-ion storage and aligns with similar challenges reported for other systems, highlighting the need for realistic testing conditions and providing critical insights to guide the development of advanced electrode materials and electrolytes for CMBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3688–3697 3688–3697"},"PeriodicalIF":5.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ag/Bi Iodide Films Fabricated by Single-Source Thermal Ablation for Lead-Free Perovskite-Inspired Solar Cells","authors":"Lucia Nasi,&nbsp;Roberto Mosca*,&nbsp;Francesco Mezzadri,&nbsp;Giulia Spaggiari,&nbsp;Patrizia Ferro,&nbsp;Jessica Barichello,&nbsp;Paolo Mariani,&nbsp;Aldo Di Carlo,&nbsp;Fabio Matteocci and Davide Calestani*,&nbsp;","doi":"10.1021/acsaem.4c0296410.1021/acsaem.4c02964","DOIUrl":"https://doi.org/10.1021/acsaem.4c02964https://doi.org/10.1021/acsaem.4c02964","url":null,"abstract":"<p >For the first time, we investigate the preparation of Ag/Bi halide double salts with the formula Ag_aBi_bI_a+3b by single source thermal ablation (SSTA), using different precursor stoichiometries (2.0 ≥ Ag/Bi ≥ 0.5). Silver bismuth iodides are interesting because they combine outstanding stability under ambient conditions with low toxicity and large light absorption coefficients. Thanks to their optical band gaps in the 1.4–2.0 eV range, they have been proposed for different applications, such as indoor photovoltaics and top cell in Si- and CIGS-based tandem solar cells. Independently of the precursor composition, films obtained by SSTA are all characterized by a dominant phase that is closely related to that of Ag₂BiI₅. We demonstrate that the Ag₂BiI₅ and BiI₃ rhombohedral phases coexist in the films prepared from precursors with Ag/Bi ≤ 1 even though no evidence of BiI₃ is achieved by XRD powder diffractometry in the θ–2θ Bragg–Brentano geometry or by UV–vis absorption measurements. The presence of the BiI₃ phase worsens the performance of planar solar cells, so the Ag/Bi = 2.0 precursor provides the best solar cells. Remarkably, these devices show a power conversion efficiency of 1.02%, an open-circuit voltage (<i>V</i>_OC) of 0.71 V, and a short-circuit current density (<i>J</i>_SC) of 3.09 mA/cm², which are comparable to those reported in the literature for planar solar cells, despite the lack of any device optimization. The reported results confirm that SSTA can be successfully used for the exploitation of silver bismuth iodides in photovoltaic applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3441–3448 3441–3448"},"PeriodicalIF":5.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Theoretical Design of High-Performance Solid-State Electrolyte Na3La3Gd1Sm1Cl18","authors":"Syed Jawad Hussain,&nbsp;Tongyu Liu,&nbsp;Rizwan Raza and Qiang Sun*,&nbsp;","doi":"10.1021/acsaem.5c0052910.1021/acsaem.5c00529","DOIUrl":"https://doi.org/10.1021/acsaem.5c00529https://doi.org/10.1021/acsaem.5c00529","url":null,"abstract":"<p >Leveraging density functional theory, deep potential model, and grand potential phase diagram analysis, we have developed a promising solid-state electrolyte based on sodium chloride, Na₃La₃GdSmCl₁₈ (NLGSC). This material demonstrates outstanding stability in thermal, dynamical, mechanical, and thermodynamic aspects, complemented by a wide band gap of 5.6 eV and excellent ductility with a Pugh’s ratio of 2.30. Importantly, NLGSC achieves a high ionic conductivity of 3.00 mS/cm at 300 K, a low activation energy of 0.24 eV, and a migration barrier of only 0.20 eV along the crystallographic <i>c</i>-axis. Furthermore, it displays a broad electrochemical stability window spanning 0.65 to 3.78 V and superior chemical compatibility with high-voltage cathode materials such as Na₂FePO₄F, Na₃V₂(PO₄)₃, and Na₃V₂P₂O₈F₃. These findings establish NLGSC as a promising solid-state electrolyte for Na-ion batteries, further expanding the applications of the recently synthesized chloride superionic conductors [<i>Nature</i> <b>2023</b>, 616, and 77].</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3963–3972 3963–3972"},"PeriodicalIF":5.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675689","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Optimization of the Thermoelectric Performance of Cu22Sn10S32 through Doping and Nanostructure Engineering","authors":"Xiangbin Chen,&nbsp;Qixian Zheng,&nbsp;Xiang Qu,&nbsp;Tian Yu,&nbsp;Ning Qi* and Zhiquan Chen*,&nbsp;","doi":"10.1021/acsaem.5c0011510.1021/acsaem.5c00115","DOIUrl":"https://doi.org/10.1021/acsaem.5c00115https://doi.org/10.1021/acsaem.5c00115","url":null,"abstract":"<p >Cu₂₂Sn₁₀S₃₂ thermoelectric materials show great potential among Cu-based chalcogenides due to their high power factor and environmentally friendly chemical composition. However, its ultrahigh intrinsic hole carrier concentration deteriorates the thermoelectric performance. In this work, a synergistic strategy combining doping and nanostructure engineering is proposed to optimize the thermoelectric performance of Cu₂₂Sn₁₀S₃₂. On the one hand, Sb is doped into the Sn sublattice to provide donors, which compensate hole carriers and thus reduces the carrier concentration, leading to an optimized power factor. On the other hand, the composite of Cu₂₂Sn₁₀S₃₂ with Sb₂O₅ results in the simultaneous doping of Sb elements and introduction of SnO₂ nanoparticles. While maintaining the optimized electrical performance, the SnO₂ nanoparticles as additional phonon scattering centers significantly lower the lattice thermal conductivity of Cu₂₂Sn₁₀S₃₂, ultimately achieving a maximum <i>zT</i> value of 0.68 at 723 K. Our results demonstrate that cation substitutional doping and nanostructure engineering can effectively enhance the thermoelectric performance of Cu₂₂Sn₁₀S₃₂.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3846–3853 3846–3853"},"PeriodicalIF":5.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Desorption Kinetics from Different Structures: The Influence of Short- and Long-Range Orders","authors":"Sanja Milošević Govedarović*,&nbsp;Željka Rašković-Lovre,&nbsp;Tijana Pantić,&nbsp;Ana Mraković,&nbsp;Fabrice Leardini,&nbsp;Jose Ramón Ares and Jasmina Grbović Novaković,&nbsp;","doi":"10.1021/acsaem.4c0278510.1021/acsaem.4c02785","DOIUrl":"https://doi.org/10.1021/acsaem.4c02785https://doi.org/10.1021/acsaem.4c02785","url":null,"abstract":"<p >This research focuses on the influence of grain size and boundaries on hydrogen diffusion in thin films and powders. The isoconversion kinetic method was applied to investigate the hydrogen desorption properties of Mg–Ni–H thin films and powders. The desorption behavior of Mg–Ni–H films was monitored using <i>in situ</i> optical microscopy and thermal desorption spectroscopy (TDS). <i>In situ</i> investigation of hydrogen release provided valuable insights into heterogeneous nucleation in thin films. The TDS curves of crystalline Mg–Ni–H indicate that desorption occurs in a one-step process, starting at <i>T</i>_onset = 212 °C, with the peak maximum observed at <i>T</i>_des = 250 °C. The apparent activation energy for the crystalline sample was estimated to be 52.1 ± 0.6 kJ/mol. These findings suggested that the desorption mechanism is strongly influenced by the grain size and the density of defects, such as the grain boundaries. Powders are prepared by mechanical milling of MgH₂ with Ni, maintaining the same molar ratio as in the preparation process of thin films. Four samples were prepared with different milling times ranging from 30 min to 2 h. The temperature-programmed desorption coupled with mass spectroscopy (TPD-MS) was used to analyze the prepared powders. Milling-induced defects in the MgH₂ crystal structures, combined with the uniform distribution of the catalytic phase, significantly impacted hydrogen desorption kinetic and reduced the desorption temperature by 2 times. In this paper, we compare the amorphous <i>vs</i> the crystalline state, highlighting how the material’s morphology controls the thermodynamics, while the amount and position of defects within the crystal structure influence the desorption kinetics.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3338–3345 3338–3345"},"PeriodicalIF":5.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675904","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interaction between Cu–S-Based Sphalerite-like Frameworks and Interstitial Cations in Colusite-Based Thermoelectric Materials","authors":"Koichiro Suekuni*,&nbsp;Takashi Hagiwara,&nbsp;Susumu Fujii*,&nbsp;Shota Ochi,&nbsp;Seiya Takahashi,&nbsp;Eiji Nishibori,&nbsp;Hidetaka Kasai,&nbsp;Philipp Sauerschnig,&nbsp;Michihiro Ohta,&nbsp;Emmanuel Guilmeau,&nbsp;Kosuke Naemura,&nbsp;Masato Yoshiya and Michitaka Ohtaki,&nbsp;","doi":"10.1021/acsaem.4c0314210.1021/acsaem.4c03142","DOIUrl":"https://doi.org/10.1021/acsaem.4c03142https://doi.org/10.1021/acsaem.4c03142","url":null,"abstract":"<p >Cu–S-based multicomponent compounds with sphalerite-like frameworks have garnered attention as midtemperature p-type thermoelectric (TE) materials. Their valence bands, primarily comprising Cu–S hybridized orbitals, control electronic properties. Herein, for colusites Cu₂₆Tr₂M₆S₃₂ (Tr = V, Nb, and Ta; M = Ge and Sn), we investigate the distinctive interaction between the Cu–S-based sphalerite-like framework and Tr at the interstitial tetrahedral sites to improve the Seebeck coefficient (<i>S</i>). According to ab initio calculations, the d(<i>t</i>₂) and d(<i>e</i>) orbitals of Tr interact with the valence band maxima at the Γ and M points, respectively. The hybridization between the Tr-<i>t</i>₂ and S orbitals (under the presence of Tr), along with structural modifications, reduces the energy of the Γ band maximum toward the Fermi level, thereby increasing <i>S</i>. This understanding is expected to be a foundation for further advancements in the TE properties of Cu–S-based compounds.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3563–3569 3563–3569"},"PeriodicalIF":5.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Electrocatalytic Oxygen Evolution Reaction through Inductive Effects of Cobalt in Nickel Orthophosphates","authors":"Jamal Bencaid,&nbsp;Abdelhadi El Jaouhari,&nbsp;Anouar Belhboub,&nbsp;Mustapha Matrouf,&nbsp;Ikram Cheras,&nbsp;Maimoune Adnane,&nbsp;Abdelghani Ghanam,&nbsp;Bouchaib Manoun and Fouad Ghamouss*,&nbsp;","doi":"10.1021/acsaem.4c0325210.1021/acsaem.4c03252","DOIUrl":"https://doi.org/10.1021/acsaem.4c03252https://doi.org/10.1021/acsaem.4c03252","url":null,"abstract":"<p >Efficient oxygen evolution reaction (OER) electrocatalysts are crucial for various electrochemical processes, including water splitting. In this study, we investigated the effect of cobalt substitution on the OER activity of nickel orthophosphate by employing a straightforward coprecipitation synthesis route. A series of Ni/Co orthophosphate catalysts, Ni_3–<i>x</i>Co_<i>x</i>(PO₄)₂·8H₂O (<i>x</i> = 0, 1, 1.5, 2, and 3), were prepared. Among them, <b>NC15</b> (Ni/Co = 1.5) exhibited the lowest overpotential of 321 mV for achieving 10 mA/cm² and a turnover frequency (TOF) of 605.9 s^–1 at 600 mV vs RHE, with a Tafel slope of 100.15 mV dec^–1. This enhanced performance can be attributed to the synergistic interplay of the highest TOF; disorder in the cobalt and nickel cations in the crystallographic sites within the crystal structure; and, importantly, a cathodic shift in the Ni oxidation peaks observed in the Co-containing catalysts. Here, we report the novel observation of an inductive effect of cobalt within the nickel phosphate structure, which influences the Ni redox behavior and contributes significantly to improved OER activity. XPS analysis revealed shifts in the binding energies of Co 2p, O 1s, P 2p, and Ni 2p, indicating a change in the electronic structure of the elements. DFT calculations suggest that Co substitution leads to band gap narrowing and charge redistribution, with excess charge accumulating at the Co site and transferring to the neighboring oxygen atoms.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3676–3687 3676–3687"},"PeriodicalIF":5.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Stability of LiF Deposited by ALD on High-Voltage Spinel/Polyimide Composite Electrodes","authors":"Matthias Audren-Paul*,&nbsp;Yann Tison,&nbsp;Hervé Martinez,&nbsp;David Peralta,&nbsp;Gunay Yildirim,&nbsp;Frédéric Le Cras and Maxime Legallais*,&nbsp;","doi":"10.1021/acsaem.4c0293010.1021/acsaem.4c02930","DOIUrl":"https://doi.org/10.1021/acsaem.4c02930https://doi.org/10.1021/acsaem.4c02930","url":null,"abstract":"<p >Li–Ni–Mn-O spinel cathode materials operating at ∼5 V vs Li⁺/Li appear to be very interesting alternatives to Co-containing layered materials in terms of rate capability, energy and power densities, and sustainability of material resources. Nevertheless, their high operating voltage, which has been an asset to date, does not allow them to be used with conventional carbonate-based electrolytes. The latter undergoes spontaneous oxidation when in contact with the charged electrode, resulting in a reduction of the cathode material, an imbalance in the Li-ion system, and a subsequent rapid loss of capacity. This incompatibility could be overcome by creating a stable, electronically insulating solid interphase at the surface of the composite electrode. Here, we report the direct deposition of lithium fluoride (LiF) on LNMO electrodes by atomic layer deposition (ALD). LiF prepared with a specific combination of precursors (lithium bis(trimethylsilyl)amide and titanium tetrafluoride) has a total impurity content of less than 2% in the bulk. In addition, to enable direct coating by ALD on the positive electrode, a commonly used binder (polyvinylidene fluoride) was replaced with polyimide (PI), a more thermally stable and nonfluorinated polymer. Using X-ray photoelectron spectroscopy (XPS) and electrochemical analysis, we demonstrate the excellent thermal stability of this LNMO/PI electrode up to 300 °C as well as its electrochemical and chemical stability in a standard carbonate electrolyte. Electrochemical data show that LiF extends the cycle life of the LNMO/PI half-cell at a high C-rate (1C). The LiF layer has been proven to be stable on the pristine electrode upon prolonged exposure to the electrolyte. However, when charged at a low C-rate, the layer exhibits a tendency to disappear. The reasons for this behavior are not yet clear but could be linked to the degradation reactions in the electrolyte or to the local concentration changes.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3392–3403 3392–3403"},"PeriodicalIF":5.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Influence of Cation and Anion Chemistry on the Ionic Conductivity and Transference Number of Zwitterionic Polymer-Supported Ionic Liquid Electrolytes","authors":"Meron Y. Tadesse,&nbsp;Nico Marioni,&nbsp;Zidan Zhang and Venkat Ganesan*,&nbsp;","doi":"10.1021/acsaem.4c0265010.1021/acsaem.4c02650","DOIUrl":"https://doi.org/10.1021/acsaem.4c02650https://doi.org/10.1021/acsaem.4c02650","url":null,"abstract":"<p >Polyzwitterionic (polyZI) ionogels have been demonstrated to be promising candidates for battery electrolyte applications. In this study, we used atomistic molecular dynamics simulations to study the influence of alkali metal cation (Li⁺ or Na⁺) and anion (<i></i><math><msubsup><mrow><mi>BF</mi></mrow><mrow><mn>4</mn></mrow><mrow><mo>−</mo></mrow></msubsup></math>, <i></i><math><msubsup><mrow><mi>PF</mi></mrow><mrow><mn>6</mn></mrow><mrow><mo>−</mo></mrow></msubsup></math>, TFS^–, and TFSI^–) chemistry on the dynamic and structural properties of poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] supported ionic liquid electrolytes. With an increase in the poly(MPC) content, our simulations revealed a decrease in the diffusivities and conductivities in both the Li⁺ and Na⁺ ionogels. With the increasing polyZI content, the results show a simultaneous increase in the inverse Haven ratios and transference numbers. While varying the anion identities, our findings indicate that chemistries in which a higher fraction of alkali metal cations coordinate with the polymers result in enhanced inverse Haven ratios, while systems with stronger alkali metal cation–polyZI interactions exhibit improved transference numbers. Overall, our results shed light on the complex nature and influence of the electrostatic interactions between the polyZI, ionic liquid, and salt ions on the mobility and structural properties of polyZI ionogels.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3314–3326 3314–3326"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Influence of Commercial Ionomers and Membranes on a PGM-Free Catalyst in the Alkaline Oxygen Reduction","authors":"Simon Kellner,&nbsp;Ziyang Liu,&nbsp;Francesco D’Acierno,&nbsp;Angus Pedersen,&nbsp;Jesús Barrio,&nbsp;Sandrine Heutz,&nbsp;Ifan E. L. Stephens,&nbsp;Silvia Favero* and Maria-Magdalena Titirici*,&nbsp;","doi":"10.1021/acsaem.4c0292910.1021/acsaem.4c02929","DOIUrl":"https://doi.org/10.1021/acsaem.4c02929https://doi.org/10.1021/acsaem.4c02929","url":null,"abstract":"<p >Hitherto, research into alkaline exchange membrane fuel cells lacked a commercial benchmark anionomer and membrane, analogous to Nafion in proton-exchange membrane fuel cells. Three commercial alkaline exchange ionomers (AEIs) have been scrutinized for that role in combination with a commercial platinum-group-metal-free Fe–N–C (Pajarito Powder) catalyst for the cathode. The initial rotating disc electrode benchmarking of the Fe–N–C catalyst’s oxygen reduction reaction activity using Nafion in an alkaline electrolyte seems to neglect the restricted oxygen diffusion in the AEIs and is recommended to be complemented by measurements with the same AEI as used in the alkaline exchange membrane fuel cell (AEMFC) testing. Evaluation of the catalyst layer in a gas-diffusion electrode setup offers a way to assess the performance in realistic operating conditions, without the additional complications of device-level water management. Blending of a porous Fe–N–C catalyst with different types of AEI yields catalyst layers with different pore size distributions. The catalyst layer with Piperion retains the highest proportion of the original BET surface area of the Fe–N–C catalyst. The water adsorption capacity is also influenced by the AEI, with Fumion FAA-3 and Piperion having equally high capabilities surpassing Sustainion. Finally, the choice of the membrane influences the ORR performance as well; particularly, the low hydroxide conductivity of Fumion FAA-3 in the room temperature experiments mitigates the ORR performance irrespective of the AEI in the catalyst layer. The best overall performance at high current densities is shown by the Piperion anion exchange ionomer matched with Sustainion X37–50 membrane.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3470–3480 3470–3480"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaem.4c02929","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}