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Universal synthesis strategy for preparation of transition metal oxide electrocatalysts doped with noble metal single atoms for oxygen evolution reaction† 制备掺杂贵金属单原子用于氧进化反应的过渡金属氧化物电催化剂的通用合成策略
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-04 DOI: 10.1039/D4YA00238E
Jingyao Wang, Yiming Zhu, Xuepeng Zhong, Zhiwei Hu, Wei-Hsiang Huang, Chih-Wen Pao, Hongfei Cheng, Nicolas Alonso-Vante and Jiwei Ma

Electrochemical water splitting is expected to be a promising solution to the growing problem of fossil fuel depletion, but is limited by the slow anodic oxygen evolution reaction (OER). Currently, nanomaterials such as Ru/Ir-based noble metal compounds have been used as highly active electrocatalysts for OER, but the high cost and scarcity hinder their wide application. Therefore, it is crucial to develop OER electrocatalysts that combine economic efficiency with high catalytic performance. In this work, we propose a universal synthesis strategy for the preparation of various noble metals-doped 3d-transition metal oxides (NM-TMO) electrocatalysts by the salt-template method. Our characterization analyses demonstrate that the noble metals are homogeneously dispersed as single atoms in transition metal oxides. Notably, Ir-doped Co3O4 catalysts, with Ir content as low as 1.35 at% (Ir–Co3O4), exhibit excellent OER performance in acidic, alkaline, and neutral media, compared to commercial IrO2 as well as undoped Co3O4. This work demonstrates that the synthesis method is applicable to a wide range of noble metals and 3d-transition metal oxide matrix. This method results in reduced costs by significantly decreasing the noble metal, but improving catalytic performance.

电化学分水技术有望成为解决日益严重的化石燃料枯竭问题的一个可行方案,但却受到缓慢的阳极氧进化反应(OER)的限制。目前,Ru/Ir 基贵金属化合物等纳米材料已被用作 OER 的高活性电催化剂,但其高昂的成本和稀缺性阻碍了它们的广泛应用。因此,开发兼具经济效益和高催化性能的 OER 电催化剂至关重要。在这项工作中,我们提出了一种通用合成策略,通过盐模板法制备各种掺杂贵金属的 3d 过渡金属氧化物(NM-TMO)电催化剂。我们的表征分析表明,贵金属以单个原子的形式均匀地分散在过渡金属氧化物中。值得注意的是,掺杂 Ir 的 Co3O4 催化剂(Ir 含量低至 1.35%(Ir-Co3O4))在酸性、碱性和中性介质中与商用 IrO2 以及未掺杂的 Co3O4 相比,均表现出优异的 OER 性能。这项研究表明,该合成方法适用于多种贵金属和 3d 过渡金属氧化物基质。该方法显著减少了贵金属的用量,从而降低了成本,但提高了催化性能。
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引用次数: 0
Effective transport properties of porous composites applied to MIEC SOC electrodes† 应用于 MIEC SOC 电极的多孔复合材料的有效传输特性
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-03 DOI: 10.1039/D4YA00074A
Philip Marmet, Lorenz Holzer, Thomas Hocker, Gernot K. Boiger and Joseph M. Brader

Semi-analytical models describing transport phenomena governed by the Laplace equation (like conduction of charge carriers or heat) are presented for the case of a porous composite with two solid phases and one pore-phase (i.e., two conducting and one insulating phase), closing the existing gap in the literature for fast and accurate predictions for this particular case. The models allow for an efficient screening of promising concepts and material combinations, as they are computationally much more efficient compared to numerical simulations on a 3D geometry. Three different semi-analytical models (Maxwell, Xu and MST models) are compared and validated using a microstructure dataset of perovskite–CGO solid oxide cell electrodes obtained by stochastic modeling. Based on the results from both numerical and semi-analytical models, the effects of the resulting composite transport properties are discussed for the application example of these fully ceramic electrodes. CGO and the used LSTN perovskite are both mixed ionic and electronic conductors (MIECs), which leads to different reaction mechanisms and associated requirements for the microstructure design compared to, e.g., Ni–YSZ. Due to the MIEC-property of both solid phases, the transport of neither electrons nor oxygen ions is limited to a single phase. Consequently, the composite conductivity, which is inherent to MIEC electrodes, opens a much larger design space for microstructure optimization compared to the single-phase conductivity of conventional electrodes, which are prone to percolation failure.

针对具有两个固相和一个孔相(即两个导电相和一个绝缘相)的多孔复合材料的情况,提出了描述拉普拉斯方程控制的传输现象(如电荷载流子或热的传导)的半解析模型,填补了现有文献在快速准确预测这种特殊情况方面的空白。与三维几何上的数值模拟相比,这些模型的计算效率要高得多,因此可以有效地筛选出有前景的概念和材料组合。此外,如果没有微观结构的全三维几何图形,半解析模型也同样适用。通过随机建模获得的包晶石-CGO 固体氧化物电池电极微观结构数据集,对三种不同的半解析模型(麦克斯韦模型、徐模型和 MST 模型)进行了比较和验证。根据数值模型和半分析模型的结果,针对这些全陶瓷电极的应用实例,讨论了由此产生的复合传输特性的影响。CGO 和所使用的 LSTN 包晶都是混合离子和电子导体 (MIEC),与 Ni-YSZ 等相比,它们的反应机制不同,对微结构设计的要求也不同。由于这两种固相都具有 MIEC 特性,电子和氧离子的传输都不局限于单相。因此,MIEC 电极固有的复合导电性为微结构优化开辟了更大的设计空间,而传统的单相导电电极则容易发生渗滤失效。
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引用次数: 0
Outstanding Reviewers for Energy Advances in 2023 2023 年能源进步》杰出评审员
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-03 DOI: 10.1039/D4YA90021A

We would like to take this opportunity to thank all of Energy Advances's reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for Energy Advances in 2023.

我们想借此机会感谢《能源进展》的所有审稿人,感谢他们帮助维护化学科学文献的质量和完整性。我们还想特别表扬一下 2023 年《能源进展》的杰出审稿人。
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引用次数: 0
Techno-economic assessment of aluminum as a clean energy carrier to decarbonize remote industries† 铝作为清洁能源载体实现偏远地区工业去碳化的技术经济评估
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-03 DOI: 10.1039/D4YA00151F
Pascal Boudreau, Michael Johnson and Jeffrey M. Bergthorson

The energy sector is transitioning to a low-carbon era requiring the wide use of renewable energy sources, mainly wind and solar. In this context, aluminum could serve as a sustainable energy carrier as it stores energy in a safe and compact way. It could be used to help decarbonize remote communities and industries, trade energy on a global scale, or provide seasonal energy storage. The Hall–Héroult process, reducing aluminum oxides to aluminum, is already a technology deployed at an industrial scale. The maturity of this industry could therefore be leveraged to store electricity. To convert aluminum back to power, it can be fully oxidized with high-temperature liquid water. The hydrogen and high-temperature heat produced can then be converted to power using a combination of heat engines and/or fuel cells. For this concept to be viable, the oxides produced must be collected and reduced in a sustainable way. In this work, aluminum recharging costs were evaluated by reviewing the current reduction process and the literature available on the development of inert anodes, a technology enabling carbon-free smelting. Results show that aluminum can be cost-competitive on a chemical energy basis with most common hydrogen carriers discussed in the literature. To contextualize the findings, a remote mine case study integrates transportation, storage and power generation costs for aluminum, compared to liquefied hydrogen and ammonia. The analysis reveals that aluminum is comparable to other carbon-free solutions, although they all currently remain more expensive than diesel fuel at an input electricity price of $30/MWhe. Aluminum emerges as marginally more expensive than the direct use of ammonia, while avoiding concerns related to toxicity and NOx emissions. This study thus positions aluminum as a promising energy carrier that merits further consideration in various other applications.

能源行业正在向低碳时代过渡,需要广泛使用可再生能源,主要是风能和太阳能。在这种情况下,铝可以作为一种可持续的能源载体,因为它能以安全、紧凑的方式储存能源。它可用于帮助偏远社区和工业去碳化,在全球范围内进行能源交易,或提供季节性能源储存。将铝氧化物还原成铝的霍尔-赫鲁特工艺已经是一项工业规模的技术。因此,可以利用这一行业的成熟性来储存电力。要将铝重新转化为电能,可以用高温液态水将其完全氧化。产生的氢气和高温热量可通过热机和/或燃料电池组合转化为电力。要使这一概念可行,必须以可持续的方式收集和还原产生的氧化物。在这项工作中,通过审查当前的还原工艺和有关开发惰性阳极(一种实现无碳冶炼的技术)的文献,对铝的再充电成本进行了评估。结果表明,就化学能而言,铝的成本与文献中讨论的大多数常见氢载体相比具有竞争力。为了说明研究结果的来龙去脉,一项偏远矿山案例研究将铝的运输、储存和发电成本与液化氢和氨进行了综合比较。分析表明,铝与其他无碳解决方案不相上下,尽管在输入电价为 30 美元/兆瓦时,铝的成本仍高于柴油。与直接使用氨气相比,铝的成本略高,同时避免了与毒性和氮氧化物排放相关的问题。因此,本研究将铝定位为一种有前途的能源载体,值得在其他各种应用中进一步考虑。
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引用次数: 0
Optimization framework for redox flow battery electrodes with improved microstructural characteristics 具有更佳微结构特性的氧化还原液流电池电极优化框架
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-03 DOI: 10.1039/D4YA00248B
Alina Berkowitz, Ashley A. Caiado, Sundar Rajan Aravamuthan, Aaron Roy, Ertan Agar and Murat Inalpolat

This research aims to advance the field of vanadium redox flow batteries (VRFBs) by introducing a pioneering approach to optimize the microstructural characteristics of carbon cloth electrodes. Addressing the traditional challenge of developing high-performance electrode materials for VRFBs, this study employs a robust, generalizable, and cost-effective data-driven modeling and optimization framework. A novel sampling strategy using low-discrepancy Latin Hypercube and quasi-Monte Carlo methods generates a small-scale, high-fidelity dataset with essential space-filling qualities for training supervised machine learning models. This study goes beyond conventional methods by constructing two surrogate models: a random forest regressor and a gradient boosting regressor as objective functions for optimization. The integration of a non-dominated sorting genetic algorithm II (NSGA-II) for multi-objective optimization facilitates exhaustive exploration of the surrogate models, leading to the identification of electrode designs that yield enhanced energy efficiencies (EEs) under specific operating conditions. The application of NSGA-II in exploring surrogate models not only facilitates the discovery of realistic design combinations but also adeptly manages trade-offs between features. The mean pore diameter was reduced compared to the tested carbon cloth electrodes while maintaining a similar permeability value based on the results obtained using the developed algorithms. Based on this suggestion, a new type of carbon cloth electrode has been fabricated by introducing a carbonaceous binder into the woven fabric to make carbon cloths with more complex pore structures and reduced mean pore diameter. The new electrode demonstrates 24% and 66% reduction in average ohmic and mass transport resistances, respectively, validating the machine-learning recommendations. This research highlights the critical role of improved electrical conductivity and porosity in carbon materials, showing their direct correlation with increased EE. Overall, this study represents a significant step forward in developing more efficient and practical VRFBs, offering a valuable contribution to the renewable energy storage landscape.

这项研究通过引入一种优化碳电极微结构特性的开创性方法,极大地推动了钒氧化还原液流电池(VRFB)领域的发展。为了应对为钒氧化还原液流电池开发高性能电极材料这一传统挑战,本研究采用了一种稳健、可推广且经济高效的数据驱动建模和优化框架。采用低差异拉丁超立方和准蒙特卡罗方法的新型采样策略生成了一个小规模、高保真的数据集,该数据集具有重要的空间填充特性,可用于训练有监督的机器学习模型。这项研究超越了传统方法,构建了两个代理模型:一个随机森林回归模型和一个梯度提升回归模型,作为优化的目标函数。将非支配排序遗传算法 II (NSGA-II) 集成到多目标优化中,有助于对代理模型进行详尽的探索,从而确定在特定操作条件下可提高能效 (EE) 的电极设计。在探索代用模型时应用 NSGA-II 不仅有助于发现现实的设计组合,还能巧妙地管理特征之间的权衡。根据从优化框架中获得的洞察力,制造出了新的电极类型,显示出 EE 的明显改善,并验证了机器学习的建议。这项研究强调了提高碳材料导电性和孔隙率的关键作用,显示了它们与提高 EE 的直接相关性。总之,这项研究在开发更高效、更实用的 VRFB 方面迈出了重要一步,为可再生能源存储领域做出了宝贵贡献。
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引用次数: 0
Quinacridone dyes: versatile molecules and materials for photo- and photoelectrochemical processes 喹吖啶酮染料:光化学和光电化学过程中的多功能分子和材料
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 10.1039/D4YA00273C
Elena Rossin, Yunshuo Yang, Martina Chirico, Greta Rossi, Pierluca Galloni and Andrea Sartorel

The renaissance of photochemistry and the explosion of photo- and photoelectro-catalysis open new opportunities in organic photocatalyst design and applications towards solar fuels and sustainable organic reactivity. In this perspective, we discuss the relevant case of quinacridone (QA) dyes: these have long been known to the scientific community, but their application in photocatalysis is recent and still explored in a limited way. This is somehow surprising given that QA is a cheap and readily available organic pigment, and in front of the appealing properties of QA derivatives, including intense absorption in the visible region, balanced redox properties making them suitable for both oxidative and reductive photochemistry, and versatility to several operative conditions. We will discuss recent examples of photo- and photoelectrochemical processes taking advantage of QA dyes, from solution photocatalysis to photoactive materials and devices (nanoparticles, covalent organic frameworks, photoelectrodes); the target applications include water splitting, carbon dioxide reduction, and organic transformations. We aim to show the potential of organic photocatalyst design and implementation, and to inspire the readers with new opportunities in this field.

光化学的复兴以及光催化和光电催化的蓬勃发展,为有机光催化剂的设计和应用提供了新的机遇,使其能用于太阳能燃料和可持续有机反应。从这个角度出发,我们讨论了喹吖啶酮(QA)染料的相关案例:这些染料早已为科学界所熟知,但它们在光催化中的应用却是最近才开始的,而且探索的方式仍然有限。考虑到 QA 是一种廉价且易于获得的有机颜料,以及 QA 衍生物的诱人特性(包括在可见光区域的强烈吸收、使其同时适用于氧化和还原光化学的平衡氧化还原特性,以及在多种操作条件下的通用性),这种情况多少有些出人意料。我们将讨论利用 QA 染料的光化学和光电化学过程的最新实例,从溶液光催化到光活性材料和器件(纳米粒子、共价有机框架、光电杆);目标应用包括水分离、二氧化碳还原和有机转化。我们旨在展示有机光催化剂设计和实施的潜力,并为读者带来该领域的新机遇。
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引用次数: 0
Slow hole diffusion limits the efficiency of p-type dye-sensitized solar cells based on the P1 dye† 缓慢的空穴扩散限制了基于 P1 染料的 p 型染料敏化太阳能电池的效率
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 10.1039/D4YA00271G
Maria B. Brands, Olivier C. M. Lugier, Kaijian Zhu, Annemarie Huijser, Stefania Tanase and Joost N. H. Reek

NiO electrodes are widely applied in p-type dye-sensitized solar cells (DSSCs) and photoelectrochemical cells, but due to excessive charge recombination, the efficiencies of these devices are still too low for commercial applications. To understand which factors induce charge recombination, we studied electrodes with a varying number of NiO layers in benchmark P1 p-DSSCs. We obtained the most efficient DSSCs with four layers of NiO (0.134%), and further insights into this optimum were obtained via dye loading studies and in operando photoelectrochemical immittance spectroscopy. These results revealed that more NiO layers led to an increasing light harvesting efficiency (ηLH), but a decreasing hole collection efficiency (ηCC), giving rise to the maximum efficiency at four NiO layers. The decreasing ηCC with more NiO layers is caused by longer hole collection times, which ultimately limits the overall efficiency. Notably, the recombination rates were independent of the number of NiO layers, and similar to those observed in the more efficient n-type DSSC analogues, but hole collection was an order of magnitude slower. Therefore, with more NiO layers, the beneficial increase in ηLH can no longer counteract the decrease in ηCC due to slow hole collection, resulting in the overall efficiency of the solar cells to maximize at four NiO layers.

氧化镍电极被广泛应用于对型染料敏化太阳能电池(DSSC)和光电化学电池中,但由于过多的电荷重组,这些器件的效率仍然太低,无法进行商业应用。为了了解哪些因素会导致电荷重组,我们在基准 P1 p-DSSC 中研究了具有不同数量氧化镍层的电极。我们用四层氧化镍(0.134%)获得了最高效的 DSSC,并通过染料负载研究和操作中光电化学瞬态光谱进一步了解了这一最佳值。这些结果表明,NiO 层数越多,光收集效率(ηLH)越高,但空穴收集效率(ηCC)却越低,当 NiO 层数达到 4 层时,光收集效率达到最高。ηCC随着氧化镍层数的增加而降低,这是由于空穴收集时间延长,最终限制了整体效率。值得注意的是,重组率与氧化镍层数无关,与在更高效的 n 型 DSSC 类似物中观察到的重组率相似,但空穴收集速度要慢一个数量级。因此,随着镍氧化物层数的增加,ηLH的有益增加不再能抵消由于空穴收集速度慢而导致的ηCC的减少,从而导致太阳能电池的整体效率在镍氧化物层数达到四层时达到最高。
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引用次数: 0
Unrevealing the potential of multicomponent metal-ion incorporation and sulfide modification in cobalt oxide for efficient water oxidation† 揭示氧化钴中多组分金属离子掺入和硫化物改性在高效水氧化中的潜力
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-07-01 DOI: 10.1039/D4YA00327F
Muzzayab Masood, Muhammad Aamir, Muhammad Ejaz Khan, Muhammad Sher, Khush Bakhat Akram, Hafiz Zahid Shafi, Hamad Almohamadi, M. d. Akhtaruzzaman and M. d. Shahiduzzaman

The design and development of highly efficient electrocatalysts from transition metals have shown a great potential for substituting precious metal-based electrocatalysts in water-splitting processes. Cobalt oxide is one of the promising materials for oxygen evolution reaction (OER). Modifying the metal oxide by the incorporation of metal ions and substituting sulfides are effective but challenging strategies for achieving efficient OER activities. In the present work, we report the synthesis of CdCoO and CdCoS electrocatalysts deposited on the surface of nickel foam. These electrocatalysts and their composites CdCoO@CuCoO and CdCoS@CuCoS could deliver high catalytic activity for oxygen evolution reaction. The as-synthesized electrocatalysts were characterized using pXRD, FTIR spectroscopy, Raman spectroscopy, XPS, and SEM techniques. The CdCoS showed a lower OER overpotential of 199 mV at a current density of 10 mA cm−2 and 522 mV at 60 mA cm−2. The incorporation of Cd2+ ions in the cobalt oxides optimized the electronic states around the Co active sites, leading to improved catalytic activities and a lower overpotential compared to other reported cobalt oxides (such as oxyhydroxides). This work emphasizes the effect of metal-ion incorporation and sulfide modification on the OER activity of cobalt oxide for water splitting and provides a multicomponent engineering strategy for designing efficient electrocatalysts.

氧化钴是氧气进化反应(OER)的理想材料之一。通过加入金属离子和硫化物改性来定制金属氧化物是实现高效 OER 的有效但具有挑战性的策略。在本研究中,我们报告了通过加入镉金属离子合成 CdCoO 和 CdCoS 材料的情况。与已报道的各种钴氧化物(氧氢化物)相比,钴氧化物(氧氢化物)周围的电子特性得到了优化,因而过电位更低,从而提高了催化活性。在 10 mAcm-2 条件下,CdCoS 的过电位为 199 mV,具有卓越的 OER 活性。这项工作强调了金属离子公司和硫化物改性对氧化钴水分离 OER 活性的影响,并为设计高效电催化剂提供了一种新的多组分工程策略。
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引用次数: 0
Recent progress in 2D inorganic non-conductive materials for alkali metal-based batteries 用于碱金属基电池的二维无机非导电材料的最新进展
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-26 DOI: 10.1039/D4YA00209A
Yuxi Shen, Zengquan Zhu, Zhefeng Xu and Yueming Li

The urgent need for new energy storage devices has promoted studies on alkaline metal-based batteries with high energy density and long life. In this case, two-dimensional (2D) inorganic non-conductive materials have exhibited unique physicochemical properties, making them ideal candidates for energy storage and conversion owing to their planar structure, high surface-to-volume ratio, and non-electronic conductive nature. Among the 2D inorganic non-conductive materials, hexagonal boron nitride (h-BN), graphitic nitride (g-C3N4), montmorillonite (MMT), and vermiculite (VMT) have shown potential application in alkaline metal-based batteries. Herein, the strategies developed for the synthesis of these inorganic two-dimensional non-conductive materials in recent years and their applications as electrode material additives, metal anode supports, and building blocks of solid interfacial and separator additives in alkali metal-based batteries are comprehensively reviewed. Subsequently, challenges associated with the use of 2D materials in alkali metal-based batteries to improve their performance are discussed and possible solutions are proposed. These 2D inorganic non-conductive materials have potential to be widely used in alkali-based batteries in the future considering their unique structure and properties.

开发储能设备的迫切需要促进了对高能量密度和长寿命碱性金属电池的研究。二维(2D)无机非导电材料具有独特的物理化学特性,由于其平面结构、高表面体积比和非电子导电性,使其在能量存储和转换方面具有巨大潜力。在二维无机非导电材料中,六方氮化硼(h-BN)、氮化石墨(g-C3N4)、蒙脱石(MMT)和蛭石(VMT)在碱性金属电池中具有一定的应用潜力。在此,我们将回顾近年来这些无机二维非导电材料的合成策略,并讨论它们近年来在碱金属基电池中作为电极材料添加剂、金属阳极支撑物、固体界面构件和隔膜添加剂的应用。讨论了在碱金属基电池中使用二维材料以提高性能所面临的挑战,并提出了可能的解决方案。考虑到这些二维无机非导电材料的独特结构和性能,它们未来有可能在碱基电池中得到更广泛的应用。
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引用次数: 0
Understanding moisture stability and degradation mechanisms of 2D hybrid perovskites: insights from ab initio molecular dynamics simulations† 了解二维混合包光体的湿度稳定性和降解机制:来自 Ab Initio 分子动力学模拟的启示
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-06-25 DOI: 10.1039/D4YA00235K
Eti Mahal, Surya Sekhar Manna, Sandeep Das and Biswarup Pathak

2D hybrid perovskites have been in focus as better alternatives to their 3D counterparts to solve long-term stability issues. In this regard, investigation of their stability and possible degradation mechanism in the presence of moisture is of utmost necessity. A detailed analysis with the help of ab initio molecular dynamics simulations has been carried out to understand their interaction with water interfaces for the first time. Various possible terminations of Ruddlesden–Popper (RP) and Dion–Jacobson (DJ) phases of 2D hybrid perovskites have been considered. We monitor the various possible interactions in the perovskite/water interface model to reveal the robustness of various terminations. PbI2 terminated structures are found to interact mainly through Pb–O interactions, and the DJ phase is found to be more robust. I2 formation is found to be the possible degradation route for I terminated phases. The importance of the bulky hydrophobic organic cation layer is highlighted, whose unique arrangement plays an essential role in resisting water infiltration and dissolution of surface components in the case of organic cation terminated phases. Interestingly, the organic cation layer is found to be robust in 2D hybrid perovskites compared to reported 3D perovskites. Our study signifies the opportunity to tune the cation layer, thereby maintaining moisture stability without compromising the optoelectronic properties of 2D hybrid perovskites, thus contributing to the fundamental understanding of 2D hybrid perovskites at water interfaces.

二维杂化过氧化物一直是解决长期稳定性问题的焦点,是其三维对应物的更好替代品。在这方面,研究它们的稳定性以及在潮湿环境下可能出现的降解机制至关重要。我们利用原子分子动力学模拟进行了详细分析,首次了解了它们与水界面的相互作用。我们考虑了二维过氧化物的 Ruddlesden-Popper (RP) 和 Dion-Jacobson (DJ) 相的各种可能终止。我们对包晶石/水界面模型中各种可能的相互作用进行了监测,以揭示各种端接的稳健性。我们发现,PbI2 端接结构主要通过 Pb-O 相互作用而发生相互作用,而 DJ 相则更为稳固。发现 I2 的形成可能是 I 端相的降解途径。在有机阳离子终止相中,笨重的疏水性有机阳离子层的重要性凸显出来,其独特的排列方式对防止水的渗透和表面成分的溶解起着至关重要的作用。有趣的是,与已报道的三维包晶石相比,二维混合包晶石中的有机阳离子层更为坚固。我们的研究为调整阳离子层从而保持湿度稳定性提供了机会,同时又不会损害二维包光体的光电特性,从而有助于从根本上了解水界面上的二维包光体。
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引用次数: 0
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