Solid State Ionics最新文献_第5页

Hydrogen conductivity and anisotropy of ionic conductivity of LiB3O5 crystals LiB3O5晶体的氢电导率和离子电导率的各向异性

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-21 DOI: 10.1016/j.ssi.2025.117046

Mikhail N. Palatnikov, Vladimir A. Sandler, Nikolay V. Sidorov, Olga V. Palatnikova

The defect structure of LBO crystals of different orientations has been studied. Various types of macro-, meso- and micro-defects have been discovered in the crystal structure. Optical microscopy studies revealed the greatest defects in z-oriented LBO crystalline samples. Dendrite fractal structures have spontaneously formed on the surface of LBO samples. Features of the structures indicate internal stresses in the crystalline plates upper layers, and crystal defects. The anisotropy of ionic conductivity of LiB₃O₅ (LBO) crystals containing H⁺ cations as a technological impurity has been studied. A pronounced effect of high-temperature annealing of LBO crystals on the dielectric properties and conductivity features has been found. The obtained results explain some contradictions in the literature data on the phase states, conductivity character and pyroelectric properties of LBO crystals. The contributions of intrinsic (Li⁺) and impurity (H⁺) conductivity have been separated in LBO samples of x, z orientation with small values of intrinsic conductivity, and their temperature dependences have been obtained. The transition temperatures from impurity to intrinsic conductivity with the corresponding increase in the activation enthalpy for x, y, z cuts of LBO crystals have been established. It has been shown that in LBO crystal technology it is desirable to reduce the concentration of doping H⁺ cations.

研究了不同取向LBO晶体的缺陷结构。在晶体结构中发现了各种宏观、中观和微观缺陷。光学显微镜研究揭示了z取向LBO晶体样品中最大的缺陷。LBO样品表面自发形成了枝晶分形结构。这些结构的特征表明了晶片上层的内应力和晶体缺陷。研究了含氢离子为工艺杂质的li3o5 （LBO）晶体离子电导率的各向异性。高温退火对LBO晶体的介电性能和电导率有显著影响。所得结果解释了LBO晶体的相态、电导率和热释电性质等方面的文献数据中存在的矛盾。在x、z两种取向的LBO样品中，本征电导率（Li+）和杂质电导率（H+）的贡献被分离出来，其本征电导率值较小，并得到了它们的温度依赖关系。确定了LBO晶体x、y、z切割从杂质到本征电导率的转变温度和相应的激活焓的增加。研究表明，在LBO晶体技术中，降低掺杂H+阳离子的浓度是可取的。

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引用次数: 0

Enhancement of oxide ion and proton conductivity in Sr3-xCaxV2O8 palmierites through tuning of the crystal structure 通过调整晶体结构增强Sr3-xCaxV2O8棕榈石中氧化离子和质子的电导率

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-11 DOI: 10.1016/j.ssi.2025.117041

Sophie G. Martin , Oscar J.B. Ballantyne , Clemens Ritter , Ying Zhou , Frazer N. Forrester , James A. Dawson , Abbie C. Mclaughlin

Sizeable oxide ion and proton conductivity have recently been reported in A₃V₂O₈ (A = Ba, Sr) palmierites. The solid solution Sr_3-xCa_xV₂O₈ (x = 0.0–0.2) has been synthesised and investigated by electrochemical characterisation and atomistic modelling, revealing key insights into the design principles for enhancing oxide and proton conduction in palmierites. Neutron diffraction data shows that at 20 °C there is a reduction in crystal symmetry from

R \bar{3} m

to

C 2 / c

for x ≥ 0.05. Upon heating to 600 °C,

R \bar{3} m

symmetry is restored for all phases. An increase in both the oxide ion and proton conductivity are observed with Ca²⁺ doping. The oxide ion conductivity scales with the magnitude of displacement of the V⁵⁺ cation and VO2 bond length.

最近报道了A3V2O8 （A = Ba, Sr）棕榈岩中较大的氧化物离子和质子电导率。合成了固溶体Sr3-xCaxV2O8 (x = 0.0-0.2)，并通过电化学表征和原子建模对其进行了研究，揭示了增强棕榈石中氧化物和质子传导的设计原理。中子衍射数据表明，在20℃时，当x≥0.05时，晶体对称性从R3¯m降低到C2/ C。当加热到600°C时，所有相的R3¯m对称性恢复。钙离子掺杂后，氧化离子和质子电导率均有所提高。氧化离子的电导率与V5+阳离子的位移大小和VO2键的长度成正比。

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引用次数: 0

Investigation on electrochemical behavior and degradation mechanism of a reversible solid oxide cell operating at high current densities 高电流密度下可逆固体氧化物电池的电化学行为及降解机理研究

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-10 DOI: 10.1016/j.ssi.2025.117044

Haoshen Wang , Qing Shao , Yue Lu , Dun Jin , Fupeng Cheng , Chengzhi Guan , Zhi Li , Guoping Xiao , Juncai Sun , Jian-Qiang Wang

Reversible solid oxide cell have significant potential for storing energy from intermittent renewable sources. However, the current densities must be increased to improve the energy conversion efficiency and reduce system costs. In this study, a fuel electrode-supported cell with an effective area of 16 cm² was operated for 288 h, switching between solid oxide fuel cell and solid oxide electrolysis cell modes at the current densities of ±1.88 A cm⁻². The electrochemical impedance spectroscopy collected at the open-circuit voltage were analyzed using the distribution of relaxation times and equivalent circuit modeling methods to evaluate the contribution of each electrode process to degradation. The results demonstrated that charge transfer reactions in the fuel and oxygen electrodes were the primary cause of cell performance degradation. According to the post-test analysis, the primary degradation mechanisms are the migration of nickel from the active layer to support layer and the coarsening of nickel in the fuel electrode. Other degradation mechanisms included the segregation of strontium and valence fluctuations of cobalt, which acted synergistically to the oxygen electrode. At elevated current densities, the concurrent migration of nickel in the same direction reduced to a reduction in the triple-phase boundary, which could not be adequately compensated for. This phenomenon significantly impaired the cell performance.

可逆固体氧化物电池在存储间歇性可再生能源方面具有重要的潜力。然而，为了提高能量转换效率和降低系统成本，必须增加电流密度。在本研究中，有效面积为16 cm2的燃料电极支撑电池在±1.88 a cm−2的电流密度下工作288 h，在固体氧化物燃料电池和固体氧化物电解电池模式之间切换。利用弛豫时间分布和等效电路建模方法对开路电压下采集的电化学阻抗谱进行分析，评价各电极过程对降解的贡献。结果表明，燃料电极和氧电极中的电荷转移反应是导致电池性能下降的主要原因。后测分析表明，镍的主要降解机制是镍从活性层向支撑层的迁移和燃料电极中镍的粗化。其他降解机制包括锶的分离和钴的价态波动，它们对氧电极起协同作用。在较高的电流密度下，镍在同一方向上的同时迁移减少为三相边界的减少，这无法得到充分补偿。这种现象严重损害了电池的性能。

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引用次数: 0

Poly(ionic liquid)/expanded pore NH2-UiO-66 composite solid-state electrolyte for high-performance solid-state lithium-ion batteries 高性能固态锂离子电池用聚（离子液体）/膨胀孔NH2-UiO-66复合固态电解质

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-13 DOI: 10.1016/j.ssi.2025.117040

Yang Zhang , Donghao Zhang , Jian Zhang, Xin Li, Xiaoling Hu, Ping Guan, Xin Wang

The development of high-performance solid electrolytes is essential for advancing ion batteries. This research introduces a novel approach for the simultaneous construction of poly(ionic liquid) and ionic conductors, creating a synergistic system that integrates a new polycationic ionic liquid matrix with ionic liquid-modified ionic conductors (Li-IL@PA-UiO-66-NH₂). This method markedly improves the interfacial compatibility between the polymer substrate and the functional filler. The filler enhances the composite electrolyte, achieving a higher transference number and ionic conductivity documented in recent studies, alongside improved voltage stability. We engineer and manufacture poly(1-vinyl-3-dodecylimidazole) bis(trifluoromethanesulfonimide) ([P(VIM-R)]TFSI) ionic liquids, which are subsequently utilized as the primary polymer, resulting in the formation of a poly(ionic liquid) solid-state electrolyte (P-GPE). Subsequently, we integrate it with the Li-IL@PA-UiO-66-NH₂ ionic conductor to formulate a poly(ionic liquid) composite solid-state electrolyte (P-CPE). The findings indicate that the ionic conductivity of P-CPE at 30 °C is 2.35 × 10⁻⁴ S cm⁻¹, with a transference number of 0.77. This value is 1.85 and 1.33 times higher than that of P-GPE, and the material can function safely up to 5 V. This study emphasizes the role of solid-state electrolytes in advancing the development of next-generation solid-state batteries.

高性能固体电解质的开发对离子电池的发展至关重要。本研究介绍了一种同时构建聚离子液体和离子导体的新方法，创建了一种将新型聚阳离子离子液体基质与离子液体修饰的离子导体相结合的协同体系（Li-IL@PA-UiO-66-NH2）。该方法显著改善了聚合物基板与功能填料之间的界面相容性。在最近的研究中，填料增强了复合电解质，实现了更高的转移数和离子电导率，同时改善了电压稳定性。我们设计和制造聚（1-乙烯基-3-十二烷基咪唑）双（三氟甲烷磺酰亚胺）（[P(VIM-R)]TFSI）离子液体，随后将其用作初级聚合物，从而形成聚（离子液体）固态电解质（P- gpe）。随后，我们将其与Li-IL@PA-UiO-66-NH2离子导体集成，形成聚（离子液体）复合固态电解质（P-CPE）。结果表明，P-CPE在30℃时的离子电导率为2.35 × 10−4 S cm−1，迁移数为0.77。该值分别是P-GPE的1.85倍和1.33倍，该材料在5v电压下可以安全工作。这项研究强调了固态电解质在推动下一代固态电池发展中的作用。

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引用次数: 0

Effect of LiNbO3 surface dry-coating on the air stability of Ga-doped LLZO solid electrolytes LiNbO3表面干涂对掺ga LLZO固体电解质空气稳定性的影响

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-18 DOI: 10.1016/j.ssi.2025.117056

Hyein Song , Young-Woong Song , Hyochan Lee , Jinsub Lim , Jieun Ryu , Yoojeong Noh , Sung-Won Kang , Seung Heon Lee , Jin Geon Yang , Jaekook Kim , Min-Young Kim

Oxide-based garnet-type Li₇La₃Zr₂O₁₂ (LLZO) solid electrolytes (SEs) have attracted significant attention as promising candidates for next-generation all-solid-state batteries (ASSBs) with high ionic conductivity of 1 × 10⁻³–10⁻⁴ S cm⁻¹. However, LLZO is prone to surface degradation upon exposure to H₂O and CO₂ in the air, leading to the formation of Li₂CO₃ impurities. This not only reduces the ionic conductivity but also increases interfacial resistance with the electrode, ultimately impairing the electrochemical and mechanical performance of the cell. In this study, we investigated and compared the air stability of LiNbO₃-coated Ga-LLZO and the pristine Ga-LLZO. According to the Accelerated Durability Test (ADT), the formation of Li₂CO₃ on the surface of LiNbO₃-coated Ga-LLZO pellets was suppressed compared to the pristine Ga-LLZO. The total ionic conductivity of the pristine Ga-LLZO was 3.90 × 10⁻⁴ S cm⁻¹, while the LiNbO₃-coated Ga-LLZO was 9.17 × 10⁻⁴ S cm⁻¹. Therefore, the ionic conductivity maintenance rates after ADT were 79 % for the LiNbO₃-coated Ga-LLZO, compared to only 23 % for the pristine Ga-LLZO. These results demonstrate that surface coating of Ga-LLZO particles with LiNbO₃ effectively suppresses air degradation reactions and significantly contributes to long-term ionic conductivity maintenance and improved air stability.

氧化基石榴石型Li7La3Zr2O12 （LLZO）固体电解质（SEs）具有1 × 10−3-10−4 S cm−1的高离子电导率，作为下一代全固态电池（assb）的有希望的候选者受到了广泛的关注。然而，LLZO暴露在空气中的H2O和CO2中容易发生表面降解，导致Li2CO3杂质的形成。这不仅降低了离子电导率，还增加了与电极的界面电阻，最终损害了电池的电化学和机械性能。在这项研究中，我们研究并比较了linbo3涂层的Ga-LLZO和原始Ga-LLZO的空气稳定性。通过加速耐久性试验（ADT），与原始Ga-LLZO相比，linbo3涂层的Ga-LLZO球团表面Li2CO3的形成受到抑制。原始Ga-LLZO的总离子电导率为3.90 × 10−4 S cm−1，而涂覆linbo3的Ga-LLZO的总离子电导率为9.17 × 10−4 S cm−1。因此，经过ADT处理后，linbo3涂层的Ga-LLZO的离子电导率维持率为79%，而原始Ga-LLZO的离子电导率仅为23%。这些结果表明，在Ga-LLZO颗粒表面涂覆LiNbO3可以有效抑制空气降解反应，并显著有助于长期维持离子电导率和提高空气稳定性。

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引用次数: 0

Influence of succinonitrile on structural, thermal, electrochemical and optical properties of sodium-ion conducting PVdF-HFP based gel polymer electrolyte membranes 丁二腈对钠离子导电PVdF-HFP基凝胶聚合物电解质膜结构、热、电化学和光学性能的影响

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-14 DOI: 10.1016/j.ssi.2025.117045

Vishalkumar Oli , M. Initha , Vaishali Madhani , Kalappa Prashantha , Neeladri Das , Sujeet Kumar Chaurasia , Kuldeep Mishra , Rahul Gera , Jehova Jire L. Hmar , Deepak Kumar

A novel sodium (Na)-ion conducting gel polymer electrolyte composed of poly(vinylidine-fluoride-co-hexafluoropropylene) (PVdF-HFP) complexed with sodium tetrafluoro-borate (NaBF₄) and ethylene carbonate (EC)-propylene carbonate (PC) as a co-solvent, coupled via differing fractions of a non-ionic plastic crystal succinonitrile (SN) are developed and studied. X-ray diffraction and Fourier transform infra-red studies identifies significant structural alterations in terms of reduced crystallinity and the interactions among the polymeric components on incorporation of SN. The thermogravimetric and differential scanning calorimetry investigations indicate that the synthesized electrolytes experience a weight reduction of less than 5 % up to 100 °C and maintain the gel stage up to 125 °C, respectively. The elevated polarity and rotational disorder of the SN molecules in the plastic-crystalline phase facilitate the improvement of ionic conductivity in the PVdF-HFP/EC-PC/NaBF₄ complex system, achieving an optimal RT ionic conductivity of about 4.55 × 10⁻³ S cm⁻¹ with the incorporation of 50 wt% of SN with purely ionic character. The working voltage range for the optimized electrolyte specimen was 4.9 V. The UV–Vis studies demonstrate the enhancement in absorbance and the reduction of the optical band gap by adding SN up to 50 wt%. The experimental results of the contact angle indicated an improvement in hydrophobicity with higher concentrations of SN across the PVdF-HFP matrix. The operational attributes for the SN-incorporated polymeric system suggest their possible use as electrolytes in electrochemical energy storage applications.

研究了以聚偏乙烯-氟-共六氟丙烯（PVdF-HFP）与四氟硼酸钠（NaBF4）和碳酸乙烯(EC)-碳酸丙烯（PC）为共溶剂，通过不同馏分的非离子塑料晶体丁二腈（SN）偶联的新型钠离子导电凝胶聚合物电解质。x射线衍射和傅里叶变换红外研究发现，SN加入后，聚合物的结晶度降低，聚合物组分之间的相互作用发生了显著的结构变化。热重法和差示扫描量热法研究表明，合成的电解质在100°C时重量减轻不到5%，在125°C时保持凝胶状态。在PVdF-HFP/EC-PC/NaBF4复合体系中，SN分子的极性和旋转无序性的提高促进了离子电导率的提高，当纯离子性质的SN加入量为50%时，其RT离子电导率约为4.55 × 10−3 S cm−1。优化后电解质试样的工作电压范围为4.9 V。紫外-可见研究表明，当SN添加到50%时，吸光度增强，光学带隙减小。接触角实验结果表明，随着SN浓度的增加，PVdF-HFP基质的疏水性得到改善。sn掺杂聚合物体系的操作特性表明它们可能在电化学储能应用中用作电解质。

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引用次数: 0

Novel oxygen-ion conductors Ln10W22O81 (Ln = La, Ce, Pr, Nd) 新型氧离子导体Ln10W22O81 （Ln = La, Ce, Pr, Nd）

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-11-15 DOI: 10.1016/j.ssi.2025.117072

A. Guseva, N. Pestereva, V. Gardt, D. Kuznetsov

Lanthanide tungstates Ln₁₀W₂₂O₈₁ (Ln = La, Ce, Pr, Nd) were prepared by the by solid-state reaction technique and their electrical conductivity have been examined by the electrochemical impedance method. Predominant ionic conductivity in Ln₁₀W₂₂O₈₁ (Ln = La, Pr, Nd) was established both by the EMF method and from independence of conductivity versus oxygen partial pressure. Ce₁₀W₂₂O₈₁ reveals some contribution of the electronic p-type component. The Tubandt method established that the ionic charge carriers in lanthanide tungstates are oxygen ions. It was found that the electrical conductivity of the studied lanthanide tungstates decreases in the order Ce₁₀W₂₂O_81, Pr₁₀W₂₂O₈₁, La₁₀W₂₂O₈₁, Nd₁₀W₂₂O₈₁. Of all the compounds studied, praseodymium tungstate has the highest oxygen-ion conductivity (3.2 × 10⁻⁴ S/cm at 800 °C), which makes it the most promising for further research and application in solid-state ionics.

采用固相反应法制备了镧系钨酸盐Ln10W22O81 (Ln = La, Ce, Pr, Nd)，并用电化学阻抗法对其电导率进行了测试。通过电动势法和电导率与氧分压的独立关系，确定了Ln10W22O81的主要离子电导率（Ln = La, Pr, Nd）。Ce10W22O81显示了电子p型元件的一些贡献。Tubandt方法确定了镧系钨酸盐中的离子载流子是氧离子。结果表明，镧系钨酸盐的电导率依次为Ce10W22O81、Pr10W22O81、La10W22O81、Nd10W22O81。在所研究的化合物中，钨酸镨具有最高的氧离子电导率（在800°C时为3.2 × 10−4 S/cm），这使其在固态离子中具有进一步研究和应用的前景。

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引用次数: 0

Preparation of partially Y- or Yb-substituted SrFeO3-δ with cubic perovskite structure and its electrical conduction properties 立方钙钛矿结构部分Y或yb取代SrFeO3-δ的制备及其导电性能

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-11-21 DOI: 10.1016/j.ssi.2025.117073

Keina Nagai , Chihiro Kato , Ryutaro Maehara , Taizo Yoshino , Takayuki Sugimoto , Kosuke Shido , Takuya Hashimoto , Fumito Fujishiro , Eiki Niwa , Motoyuki Matsuo

SrFeO_3-δ prepared in air exhibits a tetragonal or orthorhombic perovskite crystal structure with an ordered distribution of oxide-ion vacancies at room temperature. Changing the crystal structure to cubic perovskite with a random distribution of oxide-ion vacancies is expected to improve the hole or oxide-ion conductivity. In this study, the crystal structure of SrFeO_3-δ was altered by partially substituting Y or Yb at the Sr or Fe sites. X-ray diffraction and X-ray absorption spectroscopy revealed that Y partially substituted only at the Sr site, whereas Yb could substitute at both the Sr and Fe sites. Both substitutions resulted in a cubic perovskite structure. Mössbauer spectroscopy detected charge delocalization from the Y- or Yb-substitution in the cubic phase. The degree of delocalization was higher in the Sr-site-substituted specimen than in the Fe-site-substituted specimen. The cubic phases of Sr_1-xY_xFeO_3-δ, Sr_1-xYb_xFeO_3-δ, and SrFe_1-xYb_xO_3-δ exhibited a semiconducting temperature dependence devoid of phase transition effects. The lower electrical conductivity of SrFe_1-xYb_xO_3-δ compared with that of Sr_1-xYb_xFeO_3-δ corresponded to the lower delocalization degree observed by Mössbauer spectroscopy. Sr_0.9Y_0.1FeO_3-δ and Sr_0.9Yb_0.1FeO_3-δ exhibited electrical conductivity comparable with that of cubic SrFeO_2.75 above 420 °C without the structural phase transition influence, indicating their application potential, e.g., for gas separation and electrodes in solid oxide fuel cells.

在空气中制备的SrFeO3-δ在室温下表现为四方或正交钙钛矿晶体结构，氧化离子空位分布有序。将晶体结构改变为具有随机分布的氧化离子空位的立方钙钛矿有望改善空穴或氧化离子的电导率。在本研究中，通过在Sr或Fe位点部分取代Y或Yb，改变了SrFeO3-δ的晶体结构。x射线衍射和x射线吸收光谱显示，Y仅部分取代Sr位，而Yb可以取代Sr位和Fe位。这两种取代都产生了立方钙钛矿结构。Mössbauer光谱检测到立方相中Y-或Y-取代的电荷离域。sr -取代样品的离域程度高于fe -取代样品。Sr1-xYxFeO3-δ、Sr1-xYbxFeO3-δ和SrFe1-xYbxO3-δ的立方相表现出半导体温度依赖性，没有相变效应。与sr1 - xybxo3 -δ相比，srfe1 - xybxfeo3 -δ的电导率较低，这与Mössbauer光谱观察到的较低的离域程度相对应。Sr0.9Y0.1FeO3-δ和Sr0.9Yb0.1FeO3-δ在420°C以上表现出与立方SrFeO2.75相当的电导率，而不受结构相变的影响，表明它们的应用潜力，例如用于气体分离和固体氧化物燃料电池的电极。

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引用次数: 0

Highly conductive Na5YSi4O12 ceramic solid electrolyte by controlling Na deficiency in the precursors 通过控制前驱体钠缺乏制备高导电性Na5YSi4O12陶瓷固体电解质

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-16 DOI: 10.1016/j.ssi.2025.117049

Yoshiki Yasuda, Genta Tateno, Tomohiro Tojo, Ryoji Inada

Na₅YSi₄O₁₂ (NYSO) is known as a fast sodium-ion conductive oxide with both high ionic conductivity above 1 mS cm⁻¹ at room temperature and excellent electrochemical stability against sodium metal anode, making it promising for solid-state sodium battery application. In this study, we investigated the influence of non-stoichiometry in the precursor composition on the crystal phase, microstructure and ionic conducting property of NYSO. It is found that NYSO prepared from the precursor with slight sodium-deficient composition showed the highest total (bulk + grain boundary) conductivity of 2.8 mS cm⁻¹ at room temperature, which is superior to NYSO with stoichiometric precursor composition (∼ 1 mS cm⁻¹). Although excess Na deficiency in the precursor results in the formation of Na₃YSi₃O₉ phase, it does not influence so much on the sinterability and grain-boundary resistance of NYSO. Mitigation of Na₉YSi₆O₁₈ phase formation during the fabrication is very important for the densification and reduction of grain-boundary resistance in NYSO ceramic electrolyte.

Na5YSi4O12 （NYSO）是一种快速的钠离子导电氧化物，在室温下具有高于1ms cm - 1的高离子电导率，并且对钠金属阳极具有良好的电化学稳定性，使其在固态钠电池中的应用前景广阔。在本研究中，我们研究了前驱体组成中的非化学计量对NYSO晶体相、微观结构和离子导电性能的影响。研究发现，由微缺钠前驱体制备的NYSO在室温下表现出最高的总电导率（体积+晶界），为2.8 mS cm−1，优于由化学测量前驱体组成的NYSO （~ 1 mS cm−1）。虽然前驱体中过量的Na缺乏导致了Na3YSi3O9相的形成，但对NYSO的烧结性能和晶界电阻影响不大。在制备过程中减缓Na9YSi6O18相的形成对于NYSO陶瓷电解质的致密化和降低晶界电阻非常重要。

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引用次数: 0

Direct electrochemical ammonia synthesis from water and air via solid-state protonic electrochemical cells – A critical review 通过固态质子电化学电池从水和空气中直接电化学合成氨

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 Epub Date: 2025-10-15 DOI: 10.1016/j.ssi.2025.117042

Jonathan Perry, Jafar Zanganeh, Behdad Moghtaderi

Solid-state protonic electrochemical cells (SSPECs) are gaining attention as a technology that has great potential for sustainable ammonia (NH₃) synthesis, energy storage, and power generation, while providing seamless integration with renewable energy thereby offering a pathway towards a low-carbon economy. However, challenges remain in achieving industrially relevant NH₃ production rates and overall energy efficiencies required for commercial applications. Key barriers are outlined, including the thermodynamically favoured hydrogen evolution reaction (HER) at the cathode, which limits selectivity and lowers efficiencies. Recent advancements are highlighted including the importance of rational catalyst design, often focusing on functionalisation or defect-engineered sites, and integrated systems optimisation. In particular, co-fed electrochemical nitrogen reduction (eNRR) presents a strategy for enhancing NH₃ yields, while plasma-assisted processes also show promise in increasing both NH₃ production rates and selectivity. Furthermore, the lack of consistent ammonia detection methods has been outlined as a critical variable in comparative performance evaluation, which significantly impacts robust benchmarking of new catalyst and system designs. Despite these current limitations, SSPECs present a compelling opportunity for converting renewable electricity into liquid fuels, with significant potential for scaling solid-state protonic eNRR.

固态质子电化学电池（SSPECs）在合成氨（NH₃）、能源储存、发电等方面具有巨大潜力，而且与可再生能源无缝结合，为低碳经济提供了途径，因此备受关注。然而，在实现商业应用所需的工业相关的NH₃生产率和整体能源效率方面仍然存在挑战。概述了关键的障碍，包括热力学上有利的阴极析氢反应（HER），它限制了选择性和降低了效率。最近的进展包括合理催化剂设计的重要性，通常侧重于功能化或缺陷工程位点，以及集成系统优化。特别是，共馈电化学氮还原（eNRR）提出了一种提高NH3产率的策略，而等离子体辅助工艺也显示出提高NH₃产率和选择性的希望。此外，缺乏一致的氨检测方法已被概述为比较性能评估的关键变量，这将显著影响新催化剂和系统设计的稳健基准。尽管目前存在这些限制，但SSPECs为将可再生电力转化为液体燃料提供了一个引人注目的机会，具有扩大固态质子eNRR的巨大潜力。

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引用次数: 0