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Improving the reliability of classical molecular dynamics simulations in battery electrolyte design 提高经典分子动力学模拟在电池电解质设计中的可靠性
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-30 DOI: 10.1016/j.jechem.2024.09.038
Explorations into new electrolytes have highlighted the critical impact of solvation structure on battery performance. Classical molecular dynamics (CMD) using semi-empirical force fields has become an essential tool for simulating solvation structures. However, mainstream force fields often lack accuracy in describing strong ion-solvent interactions, causing disparities between CMD simulations and experimental observations. Although some empirical methods have been employed in some of the studies to address this issue, their effectiveness has been limited. Our CMD research, supported by quantum chemical calculations and experimental data, reveals that the solvation structure is influenced not only by the charge model but also by the polarization description. Previous empirical approaches that focused solely on adjusting ion-solvent interaction strengths overlooked the importance of polarization effects. Building on this insight, we propose integrating the Drude polarization model into mainstream force fields and verify its feasibility in carbonate, ether, and nitrile electrolytes. Our experimental results demonstrate that this approach significantly enhances the accuracy of CMD-simulated solvation structures. This work is expected to provide a more reliable CMD method for electrolyte design, shielding researchers from the pitfalls of erroneous simulation outcomes.
对新型电解质的探索凸显了溶解结构对电池性能的重要影响。使用半经验力场的经典分子动力学(CMD)已成为模拟溶解结构的重要工具。然而,主流力场在描述离子与溶剂之间的强相互作用时往往缺乏准确性,导致 CMD 模拟与实验观察之间存在差异。虽然一些研究采用了一些经验方法来解决这一问题,但其效果有限。我们的 CMD 研究在量子化学计算和实验数据的支持下发现,溶解结构不仅受电荷模型的影响,还受极化描述的影响。以前的经验方法只注重调整离子与溶剂的相互作用强度,忽视了极化效应的重要性。基于这一认识,我们建议将 Drude 极化模型整合到主流力场中,并在碳酸盐、醚和腈电解质中验证其可行性。实验结果表明,这种方法大大提高了 CMD 模拟溶解结构的准确性。这项工作有望为电解质设计提供更可靠的 CMD 方法,使研究人员避免错误模拟结果的陷阱。
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引用次数: 0
Unveiling solid-solid contact states in all-solid-state lithium batteries: An electrochemical impedance spectroscopy viewpoint 揭示全固态锂电池中的固-固接触状态:从电化学阻抗谱的角度看问题
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-30 DOI: 10.1016/j.jechem.2024.09.035
All-solid-state lithium batteries (ASSLBs) are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety. The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs, which is challenging to investigate quantitatively by experimental approach. This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs. With the assistance of an equivalent circuit model and distribution of relaxation times, it is discovered that as the number of voids and the sharpness of cracks increase, the contact resistance Rc grows and ultimately dominates the battery impedance. Through accurate fitting, inverse proportional relations between contact resistance Rc and (1 − porosity) as well as crack angle was disclosed. This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.
全固态锂电池(ASSLBs)因其高能量密度和内在安全性而被视为下一代储能设备。锂金属和固体电解质之间的固-固接触对工作中的全固态锂电池的性能起着至关重要的作用,而通过实验方法对其进行定量研究则具有挑战性。本研究提出了一种基于有限元法的定量模型,用于模拟 ASSLB 中不同固-固接触状态的电化学阻抗谱。在等效电路模型和弛豫时间分布的帮助下,研究发现随着空隙数量和裂纹尖锐度的增加,接触电阻 Rc 越来越大,并最终主导电池阻抗。通过精确拟合,揭示了接触电阻 Rc 和(1 - 孔隙率)以及裂纹角度之间的反比例关系。这一贡献为阐明 ASSLB 中的固-固接触状态提供了新的视角。
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引用次数: 0
Synergistic enhancement of ion/electron transport by ultrafine nanoparticles and graphene in Li2FeTiO4/C/G nanofibers for symmetric Li-ion batteries 用于对称锂离子电池的 Li2FeTiO4/C/G 纳米纤维中的超细纳米粒子和石墨烯对离子/电子传输的协同增强作用
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-28 DOI: 10.1016/j.jechem.2024.09.031
Low-cost Fe-based disordered rock salt (DRX) Li2FeTiO4 is capable of providing high capacity (295 mA h g−1) by redox activity of cations (Fe2+/Fe4+ and Ti3+/Ti4+) and anionic oxygen. However, DRX structures lack transport channels for ions and electrons, resulting in sluggish kinetics, poor electrochemical activity, and cyclability. Herein, graphene conductive carbon network permeated Li2FeTiO4 (LFT/C/G) nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method. Ultrafine Li2FeTiO4 nanoparticles (2 nm) and one-dimensional (1D) structure provide abundant active sites and unobstructed diffusion channels, accelerating ion diffusion. In addition, introducing graphene reduces the band gap and Li+ diffusion barrier and improves the dynamic properties of Li2FeTiO4, thus achieving a relatively mild interfacial reaction and reversible redox reaction. As expected, the LFT/C/1.0G cathode delivers a remarkable discharge capacity (238.5 mA h g−1), high energy density (508.8 Wh kg−1), and excellent rate capability (51.2 mA h g−1 at 1.0 A g−1). Besides, the LFT/C/1.0G anode also displays a high capacity (514.5 mA h g−1 at 500 mA g−1) and a remarkable rate capability (243.9 mA h g−1 at 8 A g−1). Moreover, the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g−1 after 100 cycles at 50 mA g−1. This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.
低成本的铁基无序岩盐(DRX)Li2FeTiO4 能够通过阳离子(Fe2+/Fe4+ 和 Ti3+/Ti4+)和阴离子氧的氧化还原活动提供高容量(295 mA h g-1)。然而,DRX 结构缺乏离子和电子的传输通道,导致动力学缓慢、电化学活性和可循环性差。本文采用溶胶-凝胶辅助电纺丝方法,成功制备了石墨烯导电碳网络渗透 Li2FeTiO4(LFT/C/G)纳米纤维。超细的 Li2FeTiO4 纳米颗粒(2 nm)和一维(1D)结构提供了丰富的活性位点和畅通的扩散通道,加速了离子扩散。此外,石墨烯的引入降低了带隙和 Li+ 扩散阻力,改善了 Li2FeTiO4 的动态特性,从而实现了相对温和的界面反应和可逆氧化还原反应。正如预期的那样,LFT/C/1.0G 阴极具有显著的放电容量(238.5 mA h g-1)、高能量密度(508.8 Wh kg-1)和出色的速率能力(51.2 mA h g-1,1.0 A g-1)。此外,LFT/C/1.0G 阳极也显示出较高的容量(500 mA g-1 时为 514.5 mA h g-1)和出色的速率能力(8 A g-1 时为 243.9 mA h g-1)。此外,基于 LFT/C/1.0G 对称电极的全电池在 50 mA g-1 条件下循环 100 次后,显示出 117.0 mA h g-1 的可逆容量。这项研究为开发具有持久和快速锂存储能力的高性价比 DRX 阴极提供了有益的启示。
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引用次数: 0
Nickel-copper alloying arrays realizing efficient co-electrosynthesis of adipic acid and hydrogen 实现己二酸与氢高效共电解的镍铜合金阵列
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-28 DOI: 10.1016/j.jechem.2024.09.033
Constructing electrocatalytic overall reaction technology to couple the electrosynthesis of adipic acid with energy-saving hydrogen production is of significant for sustainable energy systems. However, the development of highly-active bifunctional electrocatalysts remains a challenge. Herein, 3D hierarchical nickel-copper alloying arrays with dendritic morphology are manufactured by a simple electrodeposition process, standing for the excellent bifunctional electrocatalyst towards the co-production of adipic acid and H2 from cyclohexanone and water. The membrane-free flow electrolyzer of Cu0.81Ni0.19/NF shows the superior electrooxidation performance of ketone-alcohol (KA) oil with high faradaic efficiencies of over 90% for adipic acid and H2, robust stability over 200 h as well as a high yield of 0.6 mmol h−1 for adipic acid at 100 mA cm−2. In-situ spectroscopy indicates the Cu0.81Ni0.19 alloy contributes to forming more active NiOOH species to involve in the conversion of cyclohexanone to adipic acid, while the proposed reaction pathway undergoes the 2-hydroxycyclohexanone and 2,7-oxepanedione intermediates. Moreover, the theoretical calculations confirm that the optimal electronic interaction, boosted reaction kinetics as well as improved adsorption free energy of reaction intermediates, synergistically endows Cu0.81Ni0.19 alloy with superior bifunctional performance.
构建电催化整体反应技术,将己二酸的电合成与节能制氢结合起来,对于可持续能源系统具有重要意义。然而,开发高活性双功能电催化剂仍是一项挑战。本文通过简单的电沉积工艺制备了具有树枝状形态的三维分层镍铜合金阵列,为从环己酮和水联合生产己二酸和 H2 提供了优异的双功能电催化剂。Cu0.81Ni0.19/NF 无膜流动电解槽显示出卓越的酮醇油(KA)电氧化性能,己二酸和 H2 的远红外效率高达 90% 以上,稳定性超过 200 小时,在 100 mA cm-2 的条件下,己二酸的产率高达 0.6 mmol h-1。原位光谱显示,Cu0.81Ni0.19 合金有助于形成更活跃的 NiOOH 物种,参与环己酮到己二酸的转化,而所提出的反应途径则经历了 2-hydroxycyclohexanone 和 2,7-oxepanedione 中间体。此外,理论计算证实,最佳的电子相互作用、反应动力学的提高以及反应中间产物吸附自由能的改善,协同赋予了 Cu0.81Ni0.19 合金卓越的双功能性能。
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引用次数: 0
Functional ternary salt construction enabling an in-situ Li3N/LiF-enriched interface for ultra-stable all-solid-state lithium metal batteries 功能性三元盐结构可为超稳定全固态锂金属电池提供原位 Li3N/LiF 富集界面
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-27 DOI: 10.1016/j.jechem.2024.09.034
Poly(ethylene oxide)-based polymer all-solid-state lithium metal batteries (ASSLBs) have received widespread attention due to their low cost, good process ability, and high energy density. Nevertheless, the growth of Li dendrites within polymer solid-state electrolytes damages the reversibility of Li anodes and still impedes their widespread application. One efficient strategy is to construct a superior solid electrolyte interface. Herein, a stable interface enriched with Li3N and LiF is in-situ formed between Li anode and a ternary salt electrolyte. This ternary salt electrolyte is innovatively designed by introducing lithium bis(trifluoromethane sulfonyl)imide (LiTFSI), lithium bis(fluorosulfonyl)imide (LiFSI), and LiNO3 to poly(ethylene oxide) matrix. Surface characterization indicates that LiNO3 and LiFSI contribute to forming a Li3N-LiF-enriched interface and meanwhile LiTFSI ensures excellent conductivity. Theoretically, among various Li compound components, Li3N has high ionic conductivity, which is beneficial for reducing overpotential, while LiF has high interfacial energy which can enhance nucleation energy and suppress the formation of Li dendrites. The experimental results show that ASSLBs coupled with LiFePO4 cathode display extremely excellent cycle stability approximately 2200 cycles at 2 C, with a final and corresponding discharge specific capacity of 96.7 mA h g−1. Additionally, a schematic illustration of the working mechanism for the Li3N-LiF interface is proposed.
基于聚(环氧乙烷)的聚合物全固态锂金属电池(ASSLBs)因其低成本、良好的加工能力和高能量密度而受到广泛关注。然而,锂枝晶在聚合物固态电解质中的生长破坏了锂阳极的可逆性,仍然阻碍着其广泛应用。一种有效的策略是构建一个优异的固态电解质界面。在这里,锂阳极和三元盐电解质之间原位形成了富含 Li3N 和 LiF 的稳定界面。这种三元盐电解质是通过在聚环氧乙烷基体中引入双(三氟甲烷磺酰)亚胺锂(LiTFSI)、双(氟磺酰)亚胺锂(LiFSI)和 LiNO3 而创新设计的。表面表征结果表明,LiNO3 和 LiFSI 有助于形成 Li3N-LiF 富集界面,同时 LiTFSI 确保了优异的导电性。从理论上讲,在各种锂化合物成分中,Li3N 具有较高的离子电导率,有利于降低过电位,而 LiF 具有较高的界面能,可以提高成核能,抑制锂枝晶的形成。实验结果表明,与磷酸铁锂阴极耦合的 ASSLBs 在 2 C 温度下循环约 2200 次后,显示出极其出色的循环稳定性,最终相应的放电比容量为 96.7 mA h g-1。此外,还提出了一个关于 Li3N-LiF 接口工作机制的示意图。
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引用次数: 0
Feature selection strategy optimization for lithium-ion battery state of health estimation under impedance uncertainties 阻抗不确定情况下锂离子电池健康状态估计的特征选择策略优化
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-27 DOI: 10.1016/j.jechem.2024.09.032
Battery health evaluation and management are vital for the long-term reliability and optimal performance of lithium-ion batteries in electric vehicles. Electrochemical impedance spectroscopy (EIS) offers valuable insights into battery degradation analysis and modeling. However, previous studies have not adequately addressed the impedance uncertainties, particularly during battery operating conditions, which can substantially impact the robustness and accuracy of state of health (SOH) estimation. Motivated by this, this paper proposes a comprehensive feature optimization scheme that integrates impedance validity assessment with correlation analysis. By utilizing metrics such as impedance residuals and correlation coefficients, the proposed method effectively filters out invalid and insignificant impedance data, thereby enhancing the reliability of the input features. Subsequently, the extreme gradient boosting (XGBoost) modeling framework is constructed for estimating the battery degradation trajectories. The XGBoost model incorporates a diverse range of hyperparameters, optimized by a genetic algorithm to improve its adaptability and generalization performance. Experimental validation confirms the effectiveness of the proposed feature optimization scheme, demonstrating the superior estimation performance of the proposed method in comparison with four baseline techniques.
电池健康评估和管理对于电动汽车中锂离子电池的长期可靠性和最佳性能至关重要。电化学阻抗光谱(EIS)为电池降解分析和建模提供了宝贵的见解。然而,以往的研究并未充分考虑阻抗的不确定性,尤其是在电池工作条件下,这会严重影响健康状况(SOH)估算的稳健性和准确性。受此启发,本文提出了一种将阻抗有效性评估与相关性分析相结合的综合特征优化方案。通过利用阻抗残差和相关系数等指标,本文提出的方法能有效过滤无效和不重要的阻抗数据,从而提高输入特征的可靠性。随后,构建了极端梯度提升(XGBoost)建模框架,用于估计电池退化轨迹。XGBoost 模型包含多种超参数,并通过遗传算法进行了优化,以提高其适应性和泛化性能。实验验证证实了所提出的特征优化方案的有效性,表明与四种基准技术相比,所提出的方法具有更优越的估算性能。
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引用次数: 0
Atomically precise M-N-C electrocatalysts for oxygen reduction: Effects of inter-site distance, metal–metal interaction, coordination environment, and spin states 用于氧还原的原子精确 M-N-C 电催化剂:位间距、金属-金属相互作用、配位环境和自旋态的影响
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-26 DOI: 10.1016/j.jechem.2024.08.068
Inspired by molecular catalysts, researchers developed atomically precise nitrogen-coordinated single or dual metal sites imbedded in graphitized carbon (M-N-C) to fully utilize metallic sites for O2 activation. These catalysts performed remarkably well in the electrocatalytic oxygen reduction reaction (ORR) due to their distinct coordination and electrical structures. Nonetheless, their maximum efficacy in practical applications has yet to be achieved. This agenda identifies tailoring the coordination environment, spin states, intersite distance, and metal–metal interaction as innovative approaches to regulate the ORR performance of these catalysts. However, it is necessary to undertake a precise assessment of these methodologies and the knowledge obtained to be implemented in the design of future M-N-C catalysts for ORR. Therefore, this review aims to analyze recent progress in M-N-C ORR catalysts, emphasizing their innovative engineering with aspects such as alteration in intersite distance, metal–metal interaction, coordination environment, and spin states. Additionally, we critically discuss how to logically monitor the atomic structure, local coordination, spin, and electronic states of M-N-C catalysts to modulate their ORR activity. We have also highlighted the challenges associated with M-N-C catalysts and proposed suggestions for their future design and fabrication.
受分子催化剂的启发,研究人员开发了原子精确的氮配位单金属位或双金属位嵌入石墨化碳(M-N-C),以充分利用金属位激活氧气。由于其独特的配位和电结构,这些催化剂在电催化氧还原反应(ORR)中表现出色。然而,它们在实际应用中的最大功效仍有待实现。本议程将调整配位环境、自旋态、位间距离和金属-金属相互作用作为调节这些催化剂 ORR 性能的创新方法。然而,有必要对这些方法和所获得的知识进行精确评估,以便在未来设计用于 ORR 的 M-N-C 催化剂时加以应用。因此,本综述旨在分析 M-N-C ORR 催化剂的最新进展,强调其在改变位间距离、金属-金属相互作用、配位环境和自旋状态等方面的创新工程。此外,我们还认真讨论了如何对 M-N-C 催化剂的原子结构、局部配位、自旋和电子状态进行逻辑监控,以调节其 ORR 活性。我们还强调了与 M-N-C 催化剂相关的挑战,并对其未来的设计和制造提出了建议。
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引用次数: 0
Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries 通过在锂硫电池的 Ni2P 中引入掺硼原子和磷空位,促进硫的双向转化
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-25 DOI: 10.1016/j.jechem.2024.09.027
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost, yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics. Herein, we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P (Vp-B-Ni2P), thereby enhancing the bidirectional sulfur conversion. The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms, bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species, thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species. Meanwhile, theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation processes. Thus, the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 mA h g−1 at 5 C and high areal capacity of 8.03 mA h cm−2 under E/S of 5 μL mg−1 and sulfur loading of 7.20 mg cm−2. This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
锂硫(Li-S)电池因其理论能量密度高、成本低而备受关注,但其进一步商业化却因臭名昭著的穿梭效应和缓慢的氧化还原动力学而受阻。在此,我们提供了一种优化 Ni2P 电子结构的策略,即在 Ni2P 中同时引入掺 B 原子和 P 空位(Vp-B-Ni2P),从而增强硫的双向转化。研究表明,在 Ni2P 中同时引入掺杂 B 原子和 P 空位会导致镍原子周围电子的重新分布,使镍原子的 d 带中心上移,镍原子与硫元素之间产生有效的 d-p 轨道杂化,从而加强了多硫化锂(LiPSs)的化学锚定,并加快了硫元素的双向转化动力学。同时,理论计算显示,Ni2P 中掺杂的 B 原子和 P 空位选择性地促进了 Li2S 的溶解和成核过程。因此,在 5 μL mg-1 的 E/S 和 7.20 mg cm-2 的硫载荷条件下,使用 Vp-B-Ni2P 隔离剂的锂-S 电池在 5 C 时具有 777 mA h g-1 的出色速率能力和 8.03 mA h cm-2 的高平均容量。这项工作阐明了在金属磷化物中引入杂原子和空位可协同调节电子结构,从而加速双向硫转化。
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引用次数: 0
Synthesis of intermetallic PtCo fuel cell catalysts from bimetallic core@shell structured nanoparticles 利用双金属核@壳结构纳米颗粒合成金属间铂钴燃料电池催化剂
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-25 DOI: 10.1016/j.jechem.2024.09.028
The high activity and stability of intermetallic PtCo nanocatalysts toward oxygen reduction reaction make them a top candidate as low-Pt cathode catalysts in proton exchange membrane fuel cells (PEMFCs). However, forming intermetallic structures typically requires high-temperature annealing, posing a challenge for achieving well-size control and highly ordered structures. Here we report the design and synthesis of bimetallic core@shell structured precursors for affording high-performance intermetallic PtCo catalysts. The fabrication of the core@shell precursor involves using a molecular ligand containing both sulfur and oxygen donors to selectively bind with Pt colloidal nanoparticles as the core and chelate Co ions as the shell. During high-temperature annealing, the ligand transforms into carbon coatings around alloy nanoparticles, preventing particle sintering; meanwhile, Co ions in the shell can easily diffuse into the Pt core, which helps to increase the thermodynamic driving force for forming intermetallic structures. These benefits enable us to obtain the catalyst with finely dispersed nanoparticles (∼3.5 nm) and a high ordering degree of 72%. With 0.1 mgPt/cm2 cathode loading, the catalyst delivers superior performance and durability in PEMFCs, showing an initial mass activity of 0.56 A/mgPt, an initial power density of 1.05 W/cm2 at 0.67 V (H2-air), and a voltage loss of 26 mV at 0.8 A/cm2 after the accelerated durability test.
金属间铂钴纳米催化剂对氧还原反应具有高活性和稳定性,因此是质子交换膜燃料电池(PEMFC)中低铂阴极催化剂的最佳候选材料。然而,形成金属间结构通常需要高温退火,这对实现良好的尺寸控制和高度有序的结构提出了挑战。在此,我们报告了双金属核@壳结构前驱体的设计与合成,以获得高性能的金属间铂钴催化剂。核@壳前驱体的制备包括使用一种同时含有硫和氧供体的分子配体,选择性地与作为核的铂胶体纳米粒子和作为壳的螯合钴离子结合。在高温退火过程中,配体会在合金纳米粒子周围形成碳涂层,从而防止粒子烧结;同时,外壳中的 Co 离子很容易扩散到铂核中,这有助于增加形成金属间结构的热力学驱动力。这些优点使我们能够获得分散度极小的纳米颗粒(∼3.5 nm)和高有序度(72%)的催化剂。该催化剂的阴极负载量为 0.1 mgPt/cm2,在 PEMFC 中具有优异的性能和耐久性,显示出 0.56 A/mgPt 的初始质量活性、0.67 V(H2-空气)时 1.05 W/cm2 的初始功率密度以及加速耐久性测试后 0.8 A/cm2 时 26 mV 的电压损失。
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引用次数: 0
Electronic modulation induced by coupling RuO2 with electron-donating Co3O4 for high-active and long-life rechargeable Zn-air batteries 通过将 RuO2 与电子捐赠型 Co3O4 相耦合诱导电子调制,实现高活性、长寿命的锌-空气充电电池
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-25 DOI: 10.1016/j.jechem.2024.09.029
Electronic-state modulation strategy offers great potential in designing RuO2-based bifunctional-electrocatalysts for rechargeable Zn-air batteries (ZABs). Various three-dimensional (3D) transition metal oxides are attempted to couple with RuO2 for constructing an appropriate RuOM interface. This work aims to construct Co3O4-RuO2 heterostructures on carbon sheets (Co3O4/RuO2/NCNS) for boosting electronic transfer and regulation. Experiments and theoretical calculations identify the electronic transfer from Co3O4 to RuO2 that modulates the electronic structure of metal surfaces/interfaces. Specifically, it leads to the increase in Co3+ content, electron-rich state at RuO2 surface and electronic accumulation at interfaces. Moreover, this electronic-state modulation optimizes the d-band center in Co3O4/RuO2 that lowers the reaction barriers and endows interfaces as the biggest contributor to oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance. The Co3O4/RuO2/NCNS shows a quite low potential difference of 0.62 V and remarkable durability for ORR/OER. Co3O4/RuO2/NCNS-assembled ZABs exhibit an excellent specific capacity of 818.3 mA h g−1 and a superior lifespan over 750 h.
电子状态调制策略为设计基于 RuO2 的可充电锌-空气电池(ZAB)双功能电催化剂提供了巨大的潜力。人们尝试将各种三维(3D)过渡金属氧化物与 RuO2 结合,以构建合适的 RuOM 界面。这项研究的目的是在碳片(Co3O4/RuO2/NCNS)上构建 Co3O4-RuO2 异质结构,以促进电子传输和调节。实验和理论计算发现,从 Co3O4 到 RuO2 的电子转移可调节金属表面/界面的电子结构。具体来说,它导致 Co3+ 含量的增加、RuO2 表面的富电子状态以及界面上的电子积聚。此外,这种电子状态调制优化了 Co3O4/RuO2 的 d 带中心,从而降低了反应壁垒,并使界面成为氧还原反应(ORR)和氧进化反应(OER)性能的最大贡献者。Co3O4/RuO2/NCNS 的电位差很低,仅为 0.62 V,而且在 ORR/OER 反应中具有显著的耐久性。Co3O4/RuO2/NCNS 组装的 ZAB 具有 818.3 mA h g-1 的出色比容量和 750 小时以上的超长寿命。
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引用次数: 0
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