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Inversion of the Impedance Response Towards Physical Parameter Extraction Using Interpretable Machine Learning 利用可解释机器学习反演物理参数提取的阻抗响应
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-26 DOI: 10.1002/aenm.202506352
Mahmoud Nabil, Isel Grau, Ricardo Grau-Crespo, Said Hamad, Juan A. Anta
Interpreting the impedance response of perovskite solar cells (PSCs) is challenging due to the complex coupling of ionic and electronic motion. While drift-diffusion (DD) modelling is a reliable method, its mathematical complexity makes directly extracting physical parameters from experimental data infeasible. This work uses DD modelling to generate a large synthetic dataset of impedance spectra for a standard TiO2/MAPI/spiro configuration. This dataset trains machine learning (ML) models to predict recombination and ionic parameters from impedance measurements. A Gradient Boosting Regressor, using features from a generalized equivalent circuit, showed the best performance. Interpretative analysis indicates that open-circuit impedance experiments best probe recombination losses, while short-circuit conditions are more adequate for extracting ionic features like concentrations and mobilities. The trained ML models were tested on experimental spectra, confirming that the inferred physical parameters could reproduce the data. For the studied configuration, predicted ion concentrations were (1.3–3.3) × 1017 cm3, ion mobilities were (5–7) × 1011 cm2V1s1, and surface recombination velocities were 7–9 and 23–40 ms−1. This approach provides insights into the physical information extractable from impedance measurements and paves the way for ML models to unambiguously derive efficiency-determining parameters for solar cells.
由于离子和电子运动的复杂耦合,解释钙钛矿太阳能电池(PSCs)的阻抗响应具有挑战性。漂移扩散(DD)模型是一种可靠的建模方法,但其数学复杂性使得直接从实验数据中提取物理参数变得不可行。这项工作使用DD建模来生成标准TiO2/MAPI/spiro配置的大型合成阻抗谱数据集。该数据集训练机器学习(ML)模型来预测阻抗测量的重组和离子参数。使用广义等效电路特征的梯度增强回归器表现出最好的性能。解释分析表明,开路阻抗实验最适合探测复合损失,而短路条件更适合提取离子浓度和迁移率等特征。训练后的ML模型在实验光谱上进行了测试,证实了推断的物理参数可以再现数据。对于所研究的构型,预测离子浓度为(1.3-3.3)× 1017 cm−3,离子迁移率为(5-7)× 10−11 cm2V−1s−1,表面复合速度为7-9和23-40 ms−1。这种方法提供了从阻抗测量中提取物理信息的见解,并为ML模型明确地推导太阳能电池的效率决定参数铺平了道路。
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引用次数: 0
Interface-Engineered Wood-Based Composite Phase Change Materials Integrating Superhydrophobic, Flame-Retardant, and Antimicrobial Properties for Sustainable Solar–Electric Energy Conversion 集成超疏水、阻燃和抗菌性能的界面工程木基复合相变材料,用于可持续的太阳能-电能转换
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-26 DOI: 10.1002/aenm.70872
Yang Meng, Feng Wu, Yuchan Li, Zhe Xiang, Mengyuan Luo, Xinxin Sheng, Delong Xie
Efficient and durable solar thermal utilization requires composite phase change materials (CPCMs) that integrate high photothermal efficiency, stable energy storage, and environmental robustness within a scalable architecture. However, most CPCMs rely on energy-intensive processing or carbon-based frameworks, hindering the simultaneous realization of multifunctionality and sustainability. Herein, a series of carbonization-free, interface-engineered bio-based CPCMs are developed by functionalizing the anisotropic microchannel structure of delignified balsa wood with black phosphorene and metal-polyphenol network (tannin-Fe3+). The hybrid interface is further in situ reduced Ag nanoparticles and post-grafted octadecyl chains, creating a robust superhydrophobic surface. Interfacial regulation improves wood-based CPCMs compatibility and stability, delivering a latent heat of ∼175.03 kJ kg−1 with suppressed supercooling. Leveraging directional heat pathways, photothermal–plasmonic coupling, and broadband absorption, the CPCMs achieve a photothermal conversion efficiency of 91.27% and a ∼3.9-fold increase in axial thermal conductivity. The as-prepared CPCMs further integrates flame retardancy, superhydrophobicity, and antimicrobial activity, thereby mitigating dust adhesion and microbial colonization that would otherwise deteriorate the outdoor photothermal performance. As a proof of concept, stable solar–thermal–electric conversion is demonstrated with an output voltage of up to 0.65 V under one-sun irradiation. This work presents a scalable and environmentally friendly wood-based platform for advanced solar thermal energy harvesting.
高效和持久的太阳能热利用需要复合相变材料(CPCMs)在可扩展的架构内集成高光热效率,稳定的能量存储和环境鲁棒性。然而,大多数cpcm依赖于能源密集型加工或碳基框架,阻碍了多功能和可持续性的同时实现。本研究通过黑色磷烯和金属-多酚网络(单宁- fe3 +)功能化去木质素轻木的各向异性微通道结构,开发了一系列无碳化、界面工程的生物基cpcm。杂化界面进一步在原位还原银纳米颗粒和接枝十八烷基链,创造了一个强大的超疏水表面。界面调节提高了木质cpcm的兼容性和稳定性,提供了约175.03 kJ kg - 1的潜热,抑制了过冷。利用定向热通道、光热-等离子体耦合和宽带吸收,cpcm实现了91.27%的光热转换效率和约3.9倍的轴向导热系数。所制备的CPCMs进一步集成了阻燃性、超疏水性和抗菌活性,从而减轻了灰尘粘附和微生物定植,否则会降低室外光热性能。作为概念验证,在一次太阳照射下,稳定的太阳能-热电转换的输出电压高达0.65 V。这项工作为先进的太阳能热能收集提供了一个可扩展和环保的木质平台。
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引用次数: 0
Chelation Mediated Outer-Sphere Electron Transfer for High-Voltage and Long-Lifespan Neutral Zinc-Iron Flow Batteries 高电压和长寿命中性锌-铁液流电池螯合介导的外球电子转移
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-26 DOI: 10.1002/aenm.70849
Jinpeng Cao, Hang Zhang, Kaifeng Yu, Hongbo Qu, Bo Liu, Qing Wang, Feifei Zhang, Junmin Yan
Neutral zinc-iron flow batteries (ZIFBs) are promising candidates for grid-scale energy storage due to their safety, low cost, and sustainability. However, their cycle stability and energy density are restricted by zinc dendrite growth, hydrogen evolution, and more positive Zn anode potential in neutral media compared to alkaline conditions. Herein, we propose a ligand-coordination strategy using tetrasodium iminodisuccinate (IDs) to rationally tune the redox behavior of Zn2+. The formation of a stable [H4Zn(C8H7NO8)2]2− complex converts the conversional Zn(H2O)62+ structure into a chelate-dominated configuration, inducing an outer-sphere electron transfer pathway by preventing direct Zn-electrode interactions. Meanwhile, it results in a significant negative shift in redox potential of 350 mV (from −0.814 to −1.164 V vs. SHE), enabling a record-high cell voltage of 1.63 V in neutral ZIFBs. The stabilized coordination environment facilitates highly reversible Zn plating/stripping while suppressing hydrogen evolution, dendrite formation and other side reactions. As a result, such high-voltage ZIFB demonstrates a remarkable energy efficiency of 88.77% at 40 mA cm−2 and excellent cycling stability over 320 cycles, advancing durable and high-performance neutral ZIFBs.
中性锌铁液流电池(zifb)因其安全、低成本和可持续性而成为电网规模储能的有希望的候选者。然而,与碱性条件相比,它们的循环稳定性和能量密度受到锌枝晶生长、析氢和中性介质中更正的锌阳极电位的限制。在此,我们提出了一种使用亚氨基二磺酸四钠(IDs)的配位策略来合理调节Zn2+的氧化还原行为。稳定的[H4Zn(C8H7NO8)2]2 -配合物的形成将Zn(H2O)62+结构转化为螯合物主导的构型,通过阻止Zn-电极的直接相互作用诱导了外球电子转移途径。同时,它导致350 mV的氧化还原电位显著负移(与SHE相比,从- 0.814 V变为- 1.164 V),使中性zifb的电池电压达到创纪录的1.63 V。稳定的配位环境有利于高可逆的锌镀/剥离,同时抑制析氢、枝晶形成和其他副反应。因此,这种高压ZIFB在40 mA cm - 2下的能量效率达到了88.77%,并且在320次循环中具有出色的循环稳定性,从而推进了耐用和高性能的中性ZIFB。
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引用次数: 0
Roadmap for High-Throughput Ceramic Materials Synthesis and Discovery for Batteries 电池用高通量陶瓷材料合成与发现路线图
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-25 DOI: 10.1002/aenm.202506213
Jesse J. Hinricher, Katarzyna P. Sokol, Philipp Simons, Kun Joong Kim, Michael Foshey, Yunsheng Tian, Thorben Prein, Lincoln J. Miara, Elsa Olivetti, Wojciech Matusik, Jennifer L. M. Rupp
Global energy demand is projected to grow 30% within the next three decades, driven primarily by population growth and urbanization, leading to greater material needs in energy, and necessitates a new regime of accelerated research via a fundamentally improved strategy. In this perspective, we examine traditional ceramic synthesis methods for high-throughput synthesis and optimization, and highlight requirements and opportunities of synthesis routes for rapid alterations in the future. Such a strategy relies on flexible direct liquid precursor-to-solid film methods rather than traditional, but slower, solid-state methods. Application of computer-aided decision making takes in variables at all levels of fabrication and operates on both material and device characteristics to initialize and optimize the search for higher-performance devices, not just narrow materials optimization. Collectively, we provide a blueprint for accelerated ceramic materials and device improvements of next-generation materials research targeting energy storage.
全球能源需求预计将在未来三十年增长30%,主要受人口增长和城市化的推动,导致对能源的物质需求增加,并需要通过从根本上改进战略来加速研究的新制度。从这个角度来看,我们研究了传统的陶瓷合成方法的高通量合成和优化,并强调了未来快速改变合成路线的要求和机会。这种策略依赖于灵活的直接液体前驱体到固体薄膜的方法,而不是传统的,但速度较慢的固态方法。计算机辅助决策的应用考虑了制造各个层面的变量,并对材料和器件特性进行了操作,以初始化和优化对高性能器件的搜索,而不仅仅是狭隘的材料优化。总的来说,我们为加速陶瓷材料和以储能为目标的下一代材料研究的器件改进提供了蓝图。
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引用次数: 0
Role of Wadsley Defects and Cation Disorder to Enhance MoNb12O33 Diffusion (Adv. Energy Mater. 12/2026) Wadsley缺陷和阳离子紊乱在促进MoNb12O33扩散中的作用(能源材料,12/2026)
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-25 DOI: 10.1002/aenm.70770
CJ Sturgill, Manish Kumar, Nima Karimitari, Iva Milisavljevic, Coby S. Collins, Aaron Hegler, Hsin-Yun Joy Chao, Santosh Kiran Balijepalli, Scott T. Misture, Christopher Sutton, Morgan Stefik
Wadsley Defects
Wadsley缺陷
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引用次数: 0
Neutron Scattering in Sodium-Ion Battery Research: Progress and Prospects 钠离子电池中子散射研究进展与展望
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-25 DOI: 10.1002/aenm.202506774
Jue Liu, Lilin He, Naresh C. Osti, Yuxuang Zhang
Sodium-ion batteries have attracted renewed interest in recent years and are widely studied as a complementary power source to Li-ion batteries for large-scale stationary energy storage and small electric vehicles. Compared with Li-ion batteries, Na-ion batteries offer several advantages, including elemental abundance, lower cost, improved safety, and better low-temperature performance. An in-depth understanding of Na-ion batteries across multiple length and time scales has further accelerated the rapid development of this technology. Among the various advanced characterization techniques used to study Na-ion batteries, neutron scattering has gained significant traction in recent years. It has become a powerful and versatile tool for probing structure, morphology, and sodium-ion dynamics over a wide range of length and time scales. In this article, we will briefly review the development of neutron scattering technology and highlight recent advances in applying neutron-based techniques—including neutron diffraction, total scattering, small-angle scattering, quasi-elastic/inelastic scattering, and neutron imaging—to Na-ion battery materials. We also provide perspectives on future technique developments, particularly in the realm of in situ and operando neutron scattering characterization, and discuss how these approaches could further enhance our understanding of Na-ion battery systems.
近年来,钠离子电池作为锂离子电池的补充电源被广泛研究,用于大型固定式储能和小型电动汽车。与锂离子电池相比,钠离子电池具有元素丰富、成本更低、安全性更高、低温性能更好等优点。对钠离子电池在多个长度和时间尺度上的深入了解进一步加速了这项技术的快速发展。在用于研究钠离子电池的各种先进表征技术中,中子散射技术近年来受到了极大的关注。它已经成为一种强大而通用的工具,用于探测结构、形态和钠离子动力学在大范围的长度和时间尺度上。本文将简要回顾中子散射技术的发展,重点介绍中子衍射、全散射、小角散射、准弹性/非弹性散射和中子成像等中子基技术在钠离子电池材料中的应用进展。我们还提供了对未来技术发展的看法,特别是在原位和操作中子散射表征领域,并讨论了这些方法如何进一步增强我们对钠离子电池系统的理解。
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引用次数: 0
Highly Electronegative Anions Doping Effects in Sulfide-Based Electrolytes: Toward High-Voltage All-Solid-State Batteries 高电负性阴离子在硫化物基电解质中的掺杂效应:面向高压全固态电池
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-25 DOI: 10.1002/aenm.70855
Yujun Li, Wei Hao, Xinyang Yue, Tinghu Liu, Tong Duan, Jiangkai Kong, Siyuan Shen, Junjian Zhao, Xiaoya He, Yakun Liu, Zheng Liang, Song Du
The decomposition of sulfide-based electrolytes (SEs), notably Li3PS4 (LPS), at the electrode interface during battery cycling significantly hinders their practical application in all-solid-state batteries (ASSBs). However, the underlying mechanism through which chemical bonding modification enhances the electrochemical stability of SEs without compromising other properties remains unclear. Herein, we investigate the effect of introducing highly electronegative elements Q (Q ═ N, O, F) into LPS to strengthen chemical bonds and optimize lithium-ion (Li+) migration pathways in LPSQ electrolytes. Our results reveal that N and O facilitate the formation of PS3Q polyanions, whereas F tends to exist as LiF. All LPSQ systems exhibit an extended electrochemical stability window than pristine LPS, substantially enhancing their compatibility with high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes. The strengthened chemical bonding environment further proves beneficial for both electronic and ionic conductivities, leading to superior performance in Li|LPSQ|Li symmetric batteries. Furthermore, by achieving an optimal balance between electronic and ionic conductivity, LPSN enables stable long-term cycling for over 300 cycles at 1C in LiIn||NCM811 full battery, while maintaining high Coulombic efficiency and minimal interfacial degradation. These findings provide guidelines for dopant selection in SE design and offer perspectives on SE engineering aimed at enhancing the high-voltage stability of ASSBs.
在电池循环过程中,硫化物基电解质(SEs),特别是Li3PS4 (LPS)在电极界面的分解严重阻碍了它们在全固态电池(assb)中的实际应用。然而,通过化学键修饰提高se的电化学稳定性而不影响其他性能的潜在机制尚不清楚。在这里,我们研究了在LPS中引入高电负性元素Q (Q = N, O, F)来加强化学键和优化锂离子(Li+)在LPSQ电解质中的迁移途径的影响。我们的研究结果表明,N和O有利于PS3Q聚阴离子的形成,而F倾向于以LiF的形式存在。所有LPSQ系统都比原始LPS具有更大的电化学稳定性窗口,大大提高了它们与高压LiNi0.8Co0.1Mn0.1O2 (NCM811)阴极的兼容性。增强的化学键环境进一步证明有利于电子和离子电导率,从而导致Li|LPSQ|Li对称电池的优越性能。此外,通过实现电子和离子电导率之间的最佳平衡,LPSN可以在LiIn b| NCM811全电池中在1C下稳定地长期循环超过300次,同时保持高库仑效率和最小的界面退化。这些发现为SE设计中掺杂剂的选择提供了指导,并为旨在提高assb高压稳定性的SE工程提供了前景。
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引用次数: 0
Dual-Phase Engineering Coupled With Valence Gradient and Entropy Assistance Unlocking 4.9 V-Tolerant Co-Free High-Ni Cathodes 双相工程耦合价梯度和熵辅助解锁4.9耐v无共镍高镍阴极
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-24 DOI: 10.1002/aenm.70868
Longwei Liang, Yahui Chen, Jiahui Ye, Qingyun Zhang, Hongqiang Xi, Youfeng Tian, Linrui Hou, Changzhou Yuan
Layered high-Ni (Ni ≥ 0.9) cathodes are being developed to endure high-voltage operations above 4.5 V for unlocking unprecedented energy density, but they still suffer from exacerbated chemomechanical and electrochemical degradation primarily due to excessive lattice strain, oxygen loss, and phase distortion during prolonged cycling. Herein, we design a high-Ni, Co-free cathode, which features an entropy-assisted core–shell layered/spinel dual-phase, coupled with a Ni-valence gradient framework, via a multi-component complex doping involved co-precipitation strategy. The coherent structural ordering from surface spinel phase to bulk layered phase, driven by the Ni-enriched core/Mn-enriched shell arrangement, and the entropy-assistance and valence-gradient layout, hugely prevents mechanical degradation, surface side-reactions, and oxygen loss, delivering a pseudo strain-free cathode. Thanks to these appealing merits, the cathode breaks through current voltage limitations while maintaining an optimal balance between capacity and sustainability, enabling the stable high-voltage operation up to 4.9 V. Moreover, an exceptional cyclability under strenuous conditions is achieved in practical Ah-level pouch-type cells employing graphite and metallic Li anodes, operating at ultrahigh voltages of 4.65 and 4.8 V, respectively. Besides, the oxygen loss-triggered phase transitions upon heating are markedly delayed. More significantly, our contribution here propels the tremendous advancement of high-Ni, Co-free cathodes to the commercializable levels.
层状高Ni (Ni≥0.9)阴极正在开发中,以承受高于4.5 V的高压操作,以释放前所未有的能量密度,但由于过度的晶格应变、氧损失和长时间循环过程中的相位畸变,它们仍然会加剧化学力学和电化学降解。在此,我们设计了一种高ni,无co阴极,它具有熵辅助核-壳层/尖晶石双相,加上ni价梯度框架,通过多组分复杂掺杂共沉淀策略。从表面尖晶石相到大块层状相的结构有序,由富镍核/富锰壳排列驱动,以及熵辅助和价梯度布局,极大地防止了机械降解,表面副反应和氧损失,提供了伪无应变阴极。由于这些吸引人的优点,阴极突破了电流电压限制,同时保持了容量和可持续性之间的最佳平衡,实现了高达4.9 V的稳定高压工作。此外,在使用石墨和金属锂阳极的实际ah级袋式电池中,分别在4.65 V和4.8 V的超高电压下工作,在艰苦条件下实现了卓越的可循环性。此外,氧损失触发的相变在加热时明显延迟。更重要的是,我们在这里的贡献推动了高镍、无钴阴极的巨大进步,达到了可商业化的水平。
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引用次数: 0
Bidirectional Lattice Anchoring Enhances Composition Reconfiguration of Spent Lithium-Ion Cathodes 双向点阵锚定增强废锂离子阴极的成分重构
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-24 DOI: 10.1002/aenm.70869
Ahui Zhu, Ersha Fan, Xiaodong Zhang, Renjie Chen, Li Li
High-value recycling of retired lithium-ion battery materials is pivotal for the circular economy. The nickel-rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi0.54Co0.16Mn0.3O2 (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre-anchoring Al species on both SNCM and Ni(OH)2 surfaces. This method reduces the energy barrier for lithiation in the surface-disordered structures of SNCM and suppresses the structural degradation of nickel-rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g−1 at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid-state regeneration and establishes a pathway toward the high-value recycling of degraded lithium-ion batteries, demonstrating great potential for practical application.
退役锂离子电池材料的高价值回收是循环经济的关键。富镍策略具有提高能量密度的优点,是升级回收废LiNi0.54Co0.16Mn0.3O2 (SNCM)的关键方法。然而,SNCM固有的结构缺陷和再生过程中前驱体之间的非均相反应共同诱导了不可逆的相变,阻碍了理想有序层状结构的形成。因此,我们开发了一种有针对性的双向锚定策略,包括在SNCM和Ni(OH)2表面预锚定Al物质。该方法降低了SNCM表面无序结构中的锂化能垒,抑制了富镍中间相的结构降解,从而解决了升级回收过程中结构无序的根本原因。升级后的正极材料具有稳定的层状结构和从表面到本体的独特的镍浓度梯度。它具有出色的电化学性能,包括在0.2C时的可逆容量为186.84 mAh g - 1,在1C下循环200次后保持其初始容量的90.17%,优于目前的商用材料。此外,该研究为固态再生提供了重要的见解,并为降解锂离子电池的高价值回收开辟了一条途径,显示了巨大的实际应用潜力。
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引用次数: 0
The Reconstruction Mechanism and NH3-SCR Kinetics of Mn Clusters on MoS2 by Ab Initio Data Driven Machine Learning Simulations 基于Ab Initio数据驱动机器学习模拟的MoS2上Mn簇重构机理和NH3-SCR动力学
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-03-24 DOI: 10.1002/aenm.70851
Ziyi Wang, Luneng Zhao, Yuan Chang, Chunqiang Zhuang, Hongsheng Liu, Jiaxu Liu, Tao Liu, Junfeng Gao
The strong metal-support interactions (SMSI) between supported clusters and substrate can drive the local structure reconstructions, which stabilize the supported clusters to avoid migration and aggregation. Such reconstruction and stabilization mechanism are crucial to construct the atomically dispersed catalysts (ADCs), but they are too complex to simulate in most catalyst theoretical studies for a relative long time. Herein, an accurate machine learning potential (MLP) is employed into Monte Carlo simulation on the MnN (1 ≤ N ≤ 7) clusters supported on MoS2 layer. The adsorption, reconstruction and thermodynamic and kinetical stabilization of Mn clusters on perfect and defective MoS2 are compared studied. The results indicate that the S vacancies can effectively anchor Mn clusters and are feasible to control the dual-atom catalysts (DACs) on the MoS2 surface. Besides, Comparative analysis reveals that the Mn2@MoS2-S2V exhibits superior NH3-SCR catalytic activity. The complete reaction process of Mn2@MoS2-S2V following the “Fast-SCR” mechanism and the NO2 reduction pathway is the dominant route, with a rate-determining barrier of 1.03 eV. This work provides a pioneer way to disclose the very complex reconstruction of supported clusters with SMSI in simulation, which is indeed helpful to design real atomic structure of ADCs.
支撑团簇与衬底之间的强金属-支撑相互作用(SMSI)可以驱动局部结构重构,从而稳定支撑团簇,避免迁移和聚集。这种重构和稳定化机制对于构建原子分散催化剂至关重要,但长期以来在大多数催化剂理论研究中由于其过于复杂而难以模拟。本文在MoS2层支持的MnN(1≤N≤7)簇上,采用精确的机器学习潜力(MLP)进行蒙特卡罗模拟。比较研究了锰团簇在完美和缺陷二硫化钼上的吸附、重构以及热力学和动力学稳定性。结果表明,S空位可以有效地锚定Mn簇,并且可以控制MoS2表面的双原子催化剂(dac)。此外,对比分析表明Mn2@MoS2-S2V具有较好的NH3-SCR催化活性。Mn2@MoS2-S2V遵循“Fast-SCR”机制和NO2还原途径的完整反应过程为主导路线,其定速势垒为1.03 eV。这项工作为揭示SMSI在模拟中非常复杂的支持簇重建提供了一种开创性的方法,这对adc的真实原子结构设计确实有帮助。
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引用次数: 0
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Advanced Energy Materials
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