Journal of Energy Chemistry最新文献_第3页

Homogenizing bandgap distribution of Sb2(S,Se)3 absorber boosting the efficiency of solar cells to 10.83% Sb2(S,Se)3吸收体的均匀化带隙分布使太阳能电池效率提高到10.83%

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-13 DOI: 10.1016/j.jechem.2025.12.007

Xiaoqi Peng , Rongfeng Tang , Zhiyuan Cai , Zequan Jiang , Zichen Ruan , Shuwei Sheng , Jianyu Li , Yawu He , Shangfeng Yang , Changfei Zhu , Yi Zhang , Tao Chen

Antimony selenosulfide (Sb₂(S,Se)₃) has recently emerged as an attractive thin-film photovoltaic absorber because of its tunable bandgap, excellent optoelectronic properties, and long-term stability. Hydrothermal synthesis using separate Sb, Se, and S precursors enables the direct preparation of ternary Sb₂(S,Se)₃ thin films, and photovoltaic devices with efficiencies above 10% have been reported. However, due to the higher chemical reactivity of selenium compared to sulfur, the incorporation of Se occurs much faster, leading to compositional inhomogeneity with selenide enrichment near the electron transport interface. This reaction characteristic produces a reverse bandgap gradient that is detrimental to charge extraction. In this study, we unveil a kinetic modulation strategy by employing thiourea (TU) as a multifunctional additive to precisely regulate precursor reaction pathways during hydrothermal growth. TU coordinating with SSeO₃²⁻ intermediates generate stable complexes, thereby suppressing uncontrolled selenide release and achieving a balanced Se/S incorporation. This manipulation engenders Sb₂(S,Se)₃ films with homogenized bandgap distributions, well-aligned interfacial energetics, and substantially reduced defect densities. Consequently, the optimized devices attain a power conversion efficiency of 10.83%, representing the state-of-the-art performance for Sb₂(S,Se)₃ photovoltaics. This study establishes a novel method for in situ bandgap homogenization and deepens the synthetic mechanism regarding mixed-anion chalcogenide thin films.

硒化硫化锑（Sb2(S,Se)3）由于其可调谐的带隙、优异的光电性能和长期稳定性，最近成为一种有吸引力的薄膜光伏吸收剂。利用分离的Sb， Se和S前驱体水热合成可以直接制备三元Sb2(S,Se)3薄膜，并且光电器件的效率超过10%。然而，由于硒比硫具有更高的化学反应活性，硒的掺入发生得更快，导致成分不均匀，硒化物在电子传递界面附近富集。这种反应特性产生反向带隙梯度，不利于电荷提取。在这项研究中，我们揭示了一种动力学调节策略，利用硫脲（TU）作为多功能添加剂来精确调节水热生长过程中的前驱体反应途径。TU与SSeO32−中间体配合产生稳定的配合物，从而抑制不受控制的硒化物释放，实现硒/硫的平衡掺入。这种操作产生了Sb2(S,Se)3薄膜，其带隙分布均匀，界面能量排列良好，缺陷密度大大降低。因此，优化后的器件实现了10.83%的功率转换效率，代表了Sb2(S,Se)3光伏电池的最新性能。本研究建立了一种原位带隙均匀化的新方法，深化了混合阴离子硫族化物薄膜的合成机理。

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引用次数: 0

Multifunctional ionic liquid additive enabled ultrastable aqueous zinc-organic batteries with bidirectional interfacial engineering 多功能离子液体添加剂通过双向界面工程实现了超稳定水性有机锌电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-13 DOI: 10.1016/j.jechem.2025.12.009

Xiao-Jie Huang , Zhi-Ying Zhao , Jian-Feng Xiong , Ruo-Bei Huang , Chao-Hang Liu , Zi-Ang Nan , Hai-Long Wang , Jing-Hua Tian , Zhong-Qun Tian

Aqueous zinc-organic batteries (AZOBs) are promising for grid-scale energy storage but suffer from interfacial instability at both electrodes. Most existing studies focus on stabilizing a single electrode, overlooking the crucial interplay between the anode and cathode. Herein, we propose a bidirectional interface engineering strategy enabled by a multifunctional ionic liquid additive, 1-butyl-2,3-dimethylimidazolium chloride (BDMIMCl), which simultaneously stabilizes the zinc anode and polyaniline (PANI) cathode. Mechanistic studies reveal that BDMIMCl enables the formation of a protective layer on the Zn anode. This layer is subsequently converted in situ into a hybrid solid electrolyte interphase (SEI) during cycling, which effectively shields the anode. Moreover, BDMIMCl restructures the Zn²⁺ solvation shell to minimize water-induced side reactions and establishes a Cl⁻-involved multi-ion storage mechanism in the PANI cathode. As a result, Zn||Zn cells exhibit exceptional cycling stability over 2400 h at 1 mA cm⁻² and 1 mA h cm⁻², and Zn||PANI cells retain 84.3 % capacity after 2000 cycles at 2 A g⁻¹. This work provides novel insights into bidirectional interface engineering, paving the way for the development of ultrastable and high-performance AZOBs.

水锌有机电池（AZOBs）在电网规模的储能方面很有前景，但在两个电极处都存在界面不稳定的问题。大多数现有的研究都集中在稳定单个电极上，忽视了阳极和阴极之间至关重要的相互作用。在此，我们提出了一种双向界面工程策略，通过多功能离子液体添加剂，1-丁基-2,3-二甲基咪唑氯（BDMIMCl），同时稳定锌阳极和聚苯胺（PANI）阴极。机理研究表明，BDMIMCl能够在锌阳极上形成保护层。该层随后在循环过程中原位转化为混合固体电解质界面（SEI），有效地屏蔽了阳极。此外，BDMIMCl重构了Zn2+溶剂化壳层，以减少水诱导的副反应，并在聚苯胺阴极中建立了Cl−参与的多离子存储机制。结果表明，Zn||锌电池在1ma cm - 2和1ma h cm - 2下2400小时内表现出优异的循环稳定性，而Zn||PANI电池在2a g - 1下循环2000次后仍保持84.3%的容量。这项工作为双向界面工程提供了新的见解，为超稳定和高性能azob的发展铺平了道路。

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引用次数: 0

Dynamic evolution of high-valence metals in high-entropy systems enabling highly enhanced oxygen evolution reaction 高熵系统中高价金属的动态演化，使高强度的析氧反应成为可能

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-13 DOI: 10.1016/j.jechem.2025.12.008

Lun Li , Di Liu , Zhichao Yu , Youpeng Cao , Chengcheng Zhong , Chunfa Liu , Jiao Yang , Wendi Zhang , Weng Fai Ip , Hui Pan

The incorporation of high-valence metals into FeCoNi-based oxide/hydroxide/oxyhydroxide matrices is widely acknowledged as an effective approach to enhance oxygen evolution reaction (OER) performance. Traditionally, it is assumed that these metals could maintain structural stability during operation. Here, our in-situ and ex-situ characterizations reveal that the dynamic electro-dissolution behavior of Mo⁶⁺ and W⁶⁺ species in FeCoNiMoW pre-catalyst leads to fast formation of catalytic-active (Mo, W) co-incorporated metal oxyhydroxides, which play a key role in the OER performance. This leaching process enables structural reconstruction, while concurrently optimizing the adsorption of the oxygen intermediate. The resulting catalyst exhibits exceptional OER activity, achieving an overpotential of 218 mV at 10 mA cm⁻², as well as remarkable stability with a degradation rate of only 8.7 μV h⁻¹ over 720 h at 500 mA cm⁻². Furthermore, anion-exchange membrane water electrolyzers based on FeCoNiMoW//Pt/C can stably operate at 500 and 1000 mA cm⁻² with low cell voltages of 1.70 and 1.84 V, respectively. The cost of the electric bill using this catalyst is notably low, at only $0.88 per kg, which is significantly below target of $2.00 per kg set by the U.S. Office of Clean Energy (OCE) for 2026. These findings offer valuable insights into the critical role of high-valence metals in advancing the OER process and underscore the substantial potential of this approach for industrial scale-up applications.

在feconi基氧化物/氢氧化物/氢氧化物基体中掺入高价金属被广泛认为是提高析氧反应（OER）性能的有效方法。传统上，人们认为这些金属在使用过程中可以保持结构的稳定性。本研究的原位和非原位表征表明，FeCoNiMoW预催化剂中Mo6+和W6+的动态电溶行为导致了催化活性（Mo， W）共掺杂金属氢氧化物的快速形成，这对OER性能起着关键作用。这种浸出过程可以实现结构重建，同时优化氧中间体的吸附。所制得的催化剂表现出优异的OER活性，在10 mA cm−2条件下可达到218 mV的过电位，在500 mA cm−2条件下720 h的降解率仅为8.7 μV h−1。此外，基于FeCoNiMoW//Pt/C的阴离子交换膜水电解槽可以在500和1000 mA cm−2下稳定工作，电池电压分别为1.70和1.84 V。使用这种催化剂的电费非常低，仅为每公斤0.88美元，大大低于美国清洁能源办公室（OCE）为2026年设定的每公斤2.00美元的目标。这些发现为高价金属在推进OER过程中的关键作用提供了有价值的见解，并强调了这种方法在工业规模应用中的巨大潜力。

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引用次数: 0

Cooperative interface catalysis and electronic regulation induced by single atomic tin in high-performance potassium-ion batteries 高性能钾离子电池中单原子锡诱导的协同界面催化和电子调控

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-13 DOI: 10.1016/j.jechem.2025.12.011

Yizhi Yuan , Fangrui Yu , Song Chen , Hongli Deng , Qingyi Zhao , Wei Chen , Xinxin Jia , Qiusheng Zhang , Hongtao Sun , Jian Zhu

Constructing single atomic metal (SAM) sites in carbon materials is considered an effective strategy to enhance their electrochemical performance in potassium ion batteries (PIBs). However, investigating the interaction between SAM and carbon skeleton, and how SAM improves potassium storage performance, remains crucial and challenging for the design of SAM-based electrode materials. Herein, we report a carbon nanosheet anchored with single-atom tin coordinated by three nitrogen atoms and two oxygen atoms (i.e., Sn₁N₃O₂), which demonstrates a synergistic effect for potassium storage. The Sn₁N₃O₂ site catalyzes anion dissociation in the electrolytes, thereby promoting the formation of an inorganic-rich solid electrolyte interphase layer, which is the key component to enhancing stability. In addition, the single-atom Sn tunes the electronic structure of N and O for appropriate K⁺ adsorption energy and reduces the diffusion barrier. Consequently, the SAM anode exhibits significantly improved capacity, rate capability, and outstanding long-term stability. Even more impressive is that a full PIB cell employing this anode also demonstrates an extremely long service life with 81 % capacity retention after 3000 cycles at 2 A g⁻¹. This work precisely elucidates the role of SAM in enhancing the performance of carbon materials in PIBs.

在碳材料上构建单原子金属（SAM）位点被认为是提高钾离子电池（PIBs）电化学性能的有效策略。然而，研究SAM和碳骨架之间的相互作用，以及SAM如何提高钾存储性能，仍然是SAM基电极材料设计的关键和挑战。在此，我们报道了一个由三个氮原子和两个氧原子（即Sn1N3O2）配位的单原子锡锚定的碳纳米片，它显示了钾储存的协同效应。Sn1N3O2位点催化电解质中的阴离子解离，从而促进富无机固体电解质间相层的形成，这是增强稳定性的关键成分。此外，单原子Sn调整了N和O的电子结构，以获得适当的K+吸附能，并降低了扩散势垒。因此，SAM阳极表现出显着提高的容量，速率能力和出色的长期稳定性。更令人印象深刻的是，采用这种阳极的全PIB电池也显示出极长的使用寿命，在2 a g−1下循环3000次后容量保持81%。这项工作准确地阐明了SAM在提高PIBs中碳材料性能方面的作用。

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引用次数: 0

Thermal runaway in lithium-ion battery systems with hybrid electrical connections: Propagation induced by spontaneous overcharge without heat transfer 混合电连接锂离子电池系统的热失控：由无热传递的自发过充引起的传播

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-11 DOI: 10.1016/j.jechem.2025.11.060

Zhizuan Zhou , Maoyu Li , Lun Li , Ping Zhang , Lizhong Yang

Lithium-ion batteries (LIBs) are inevitably connected in parallel and in series to satisfy the high-voltage and high-power requirements of practical applications. However, most efforts focus on thermal runaway (TR) in the batteries adopting open-circuit or single electrical connection configurations, neglecting the potential influence of hybrid electrical connections. This oversight contributes to the discrepancies between TR disasters observed at the experimental scale and those occurring in real-world scenarios. To address the issue, this study systematically investigates the TR characteristics of battery modules with different hybrid connections (open circuit, 1S3P, 2S3P, 3S3P, and 4S3P) and elucidates the mechanisms of TR propagation in the absence of heat transfer. The results show that the initial TR in 1S3P and 2S3P battery modules can be advanced to the opening of safety valve owing to the transferred electric energy between parallel submodules. In contrast to conventional thoughts, without the involvement of heat transfer, TR propagation may still occur in battery systems with series–parallel connections. Although the heat transfer is completely blocked, the adjacent battery connected in series with the TR battery in 2S3P module still suffers from TR owing to the spontaneous overcharge, and batteries in 3S3P and 4S3P battery modules all experience severe side reactions accompanied by significant expansions. Moreover, spontaneous overcharge is driven by voltage imbalances between parallel submodules in series–parallel battery systems, driving charge transfer that results in overcharging of adjacent batteries. The severity of this effect is governed by the voltage increment between neighboring batteries, while its influence weakens as the number of series-connected batteries increases. Overall, this study reveals an additional pathway, electricity transfer, that can also result in TR disasters in practical battery systems, providing novel insights for TR disaster mechanisms and guides for safe battery system design.

为了满足实际应用对高压、大功率的要求，锂离子电池不可避免地要采用并联和串联的方式。然而，大多数研究都集中在采用开路或单一电气连接配置的电池的热失控（TR）上，而忽略了混合电气连接的潜在影响。这种疏忽造成了在实验规模上观察到的TR灾难与在现实情景中发生的灾难之间的差异。为了解决这一问题，本研究系统地研究了不同混合连接（开路、1S3P、2S3P、3S3P和4S3P）电池模块的TR特性，并阐明了在无传热情况下TR传播的机制。结果表明，由于并联子模块之间的电能传递，1S3P和2S3P电池模块的初始TR可以提前到安全阀开启。与传统的想法相反，在没有热传递的情况下，在串并联的电池系统中仍然可能发生TR传播。虽然传热完全阻断，但相邻的2S3P模块中与TR电池串联的电池由于自发过充仍然发生TR，并且3S3P和4S3P电池模块中的电池都发生严重的副反应并伴有明显的膨胀。此外，自发过充电是由串并联电池系统中并联子模块之间的电压不平衡驱动的，从而驱动电荷转移，导致相邻电池过充电。这种影响的严重程度取决于相邻电池之间的电压增量，而其影响随着串联电池数量的增加而减弱。总的来说，本研究揭示了在实际电池系统中，另一种可能导致TR灾难的途径——电转移，为TR灾难机制提供了新的见解，并为安全电池系统设计提供了指导。

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引用次数: 0

V single-atom engineered defect-rich MoS2 to boost H2S decomposition into hydrogen and sulfur V单原子工程富缺陷MoS2促进H2S分解为氢和硫

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-09 DOI: 10.1016/j.jechem.2025.12.005

Hui Liu , Kailong Xu , Kaisong Xiang , Fenghua Shen , Hao Chen , Yelin Zhu , Xinlei Wang , Lin Wu , Liyuan Chai , Jun Wu

Hydrogen sulfide (H₂S), a toxic and prevalent industrial byproduct, poses significant environmental and safety challenges, yet it also represents an underutilized source of hydrogen. The direct decomposition of H₂S into hydrogen and sulfur provides a sustainable pathway for simultaneously mitigating pollution and recovering energy. However, its industrial implementation is hindered by sluggish kinetics and catalyst deactivation. Herein, a defect-rich V single-atom engineered MoS₂ catalyst supported on Al₂O₃ (V-MoS₂/Al₂O₃) was designed to address these challenges. Atomically dispersed V atoms possess a low coordination (3.69) environment that promotes the formation of high-density sulfur vacancies and low-valent Mo²⁺, thereby enhancing electron transfer and facilitating H–S bond activation. Density functional theory calculations further reveal that the formation of Mo-S_vacancy-V active centers synergistically reduces the energy barriers for H₂S dissociation and product (H₂ and S₂) desorption. The optimized catalyst achieves 72% H₂S conversion with approximately ∼90% hydrogen selectivity and high-purity sulfur product at 800 °C, alongside excellent operational stability. Such high H₂S conversion efficiency was achieved by the synergistic effect of the efficient catalyst developed and the fluidized-bed reactor established in this work, in which sulfur was quickly condensed and removed from the system, leading to the shift of equilibrium according to the La-Chatelier principle. This work provides fundamental insights into the cooperative mechanism of vacancy-single-atom and demonstrates a scalable atomic-level strategy for efficient hydrogen production from sulfur-rich waste streams.

硫化氢（H2S）是一种有毒且普遍存在的工业副产品，它给环境和安全带来了重大挑战，但它也是一种未充分利用的氢气来源。将H2S直接分解为氢和硫，为同时减轻污染和回收能源提供了一条可持续的途径。然而，它的工业实施受到缓慢的动力学和催化剂失活的阻碍。本文设计了一种基于Al2O3的富缺陷V单原子工程MoS2催化剂（V-MoS2/Al2O3）来解决这些问题。原子分散的V原子具有低配位（3.69）的环境，促进高密度硫空位和低价Mo2+的形成，从而增强电子转移，促进H-S键活化。密度泛函理论计算进一步表明，Mo-Svacancy-V活性中心的形成协同降低了H2S解离和产物（H2和S2）脱附的能垒。优化后的催化剂在800°C下可实现72%的H2S转化率，约90%的氢选择性和高纯度的硫产物，同时具有出色的操作稳定性。如此高的硫化氢转化效率是由本研究开发的高效催化剂和建立的流化床反应器的协同作用实现的，在流化床反应器中，硫被快速冷凝并从系统中去除，导致平衡根据拉-夏特列原理发生转移。这项工作为空位-单原子的合作机制提供了基本的见解，并展示了从富硫废物流中高效产氢的可扩展原子级策略。

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引用次数: 0

Scalable, binder-free, ultrathin, and outdoor stable passive cooling paints engineered by cellulose-weaved topological scattering network 可扩展，无粘合剂，超薄，室外稳定的被动冷却涂料由纤维素编织的拓扑散射网络设计

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-09 DOI: 10.1016/j.jechem.2025.12.003

Ting Yang , Siying Guo , Xin Zhao , Bianjing Sun , Ruey Shan Chen , Sinyee Gan , Jonathan Woon-Chung Wong , Chenyang Cai

Paints with passive daytime radiative cooling capability hold significant promise for energy-efficient buildings owing to their ease of processing. However, conventional radiative cooling paints require substantial thickness to achieve effective outdoor cooling and must be combined with binders to enhance adhesion to the substrate. Meanwhile, their long-term outdoor durability remains poor. In this work, we proposed a scattering network-enhanced ultrathin photonic cooling paint (thickness of 78 μm) fabricated without traditional binders through a universal, scalable solution-assembly strategy under a low-carbon production process. Cellulose nanofiber and cellulose nanocrystal were employed to wrap and entangle TiO₂, forming a topological scattering network that prevents near-field coupling. Together with hierarchical pores, this structure enables high solar reflectance (96.4%) and an infrared emissivity of 0.94. This novel paint achieves temperature reduction of ∼5.6 and 3.8 °C under low and high-humidity conditions of midday, respectively, while maintaining long-term outdoor stability. Importantly, the cellulose-weaved topological scattering network can also be engineered with alternative photonic cooling pigments (Al₂O₃, SiO₂, BaSO₄, and mica), demonstrating its universality. In addition, life cycle assessment reveals that the obtained cooling paint offers very low carbon emissions and minimal environmental impacts. This work provides an economically viable and environmentally sustainable alternative to existing passive cooling materials.

由于易于加工，具有被动日间辐射冷却能力的涂料对节能建筑具有重要的前景。然而，传统的辐射冷却涂料需要相当厚的厚度来实现有效的室外冷却，并且必须与粘合剂结合以增强与基材的附着力。同时，它们的长期户外耐久性仍然很差。在这项工作中，我们提出了一种散射网络增强的超薄光子冷却涂料（厚度为78 μm），在低碳生产工艺下，通过通用的、可扩展的解决方案组装策略，在没有传统粘合剂的情况下制造。采用纤维素纳米纤维和纤维素纳米晶体包裹缠绕TiO2，形成防止近场耦合的拓扑散射网络。与分层孔隙一起，这种结构使太阳反射率高（96.4%），红外发射率为0.94。这种新型涂料在正午的低湿度和高湿度条件下分别实现温度降低~ 5.6和3.8°C，同时保持长期的室外稳定性。重要的是，纤维素编织的拓扑散射网络也可以用其他光子冷却颜料（Al2O3, SiO2， BaSO4和云母）来设计，证明了它的普遍性。此外，生命周期评估显示，获得的冷却涂料提供非常低的碳排放和最小的环境影响。这项工作为现有的被动冷却材料提供了一种经济可行、环境可持续的替代方案。

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引用次数: 0

Competitive oxidation stabilizing perovskite precursor for all-air-processing perovskite solar cells with high reproducibility 具有高重复性的全空气处理钙钛矿太阳能电池的竞争性氧化稳定钙钛矿前驱体

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-09 DOI: 10.1016/j.jechem.2025.11.059

Ya Liu , Chenlong Zhang , Renni Luan , Jie Dou , Yueji Liu , Qiyao Guo , Xinyu Zhang , Benlin He , Qunwei Tang , Qingzhong Xue , Jialong Duan

The fabrication of perovskite solar cells (PSCs) in ambient air is compatible with the large-scale manufacturing industrialization, yet oxygen triggers severe halide oxidation and gradually damps the stoichiometric proportion in perovskite precursor, which goes against the formation of high-quality and reproducible films. Herein, different from hybrid species, we first reveal the oxidation mechanism in all-inorganic perovskite precursor and then introduce an ionic methylamine formate (MAFA) to competitively react with invasive oxygen. By avoiding the direct bonding between free Cs⁺ and O²⁻, we demonstrate that MAFA not only improves the chemical stability of perovskite precursor but also weakens the time-dependent evolution of perovskite films, allowing an ultrawide storage window over 30 days for crystallizing a high-quality film in ambient air. Finally, we achieve a carbon-electrode-tailored CsPbI₂Br PSC with an enhanced efficiency of 15.19% and excellent reproducibility, on a par with state-of-the-art counterparts fabricated in a N₂ atmosphere. With the higher efficiency conservation rate after aging under harsh conditions, this work provides a strategy to engineer the perovskite precursor for reproducible and efficient photoelectric devices, benefiting the large-scale fabrication in the future.

在环境空气中制备钙钛矿太阳能电池（PSCs）与大规模制造工业化相适应，但氧气会引发严重的卤化物氧化，并逐渐抑制钙钛矿前驱体中的化学计量比例，不利于形成高质量和可复制的薄膜。与杂化品种不同的是，我们首先揭示了全无机钙钛矿前驱体的氧化机理，然后引入离子甲酸甲胺（MAFA）与有创氧竞争性反应。通过避免游离Cs+和O2−之间的直接结合，我们证明了MAFA不仅提高了钙钛矿前驱体的化学稳定性，而且削弱了钙钛矿薄膜的时间依赖性演变，允许超宽的储存窗口超过30天，在环境空气中结晶出高质量的薄膜。最后，我们实现了碳电极定制的CsPbI2Br PSC，其效率提高了15.19%，并且具有出色的再现性，与在N2气氛中制造的最先进的同类产品相当。由于钙钛矿前驱体在恶劣条件下老化后具有较高的效率守恒率，本研究为可再生高效光电器件的设计提供了一种策略，有利于未来的大规模制造。

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引用次数: 0

An all-halide solid-state electrolyte capable for direct use with lithium metal anode in high energy batteries 一种全卤化物固态电解质，可直接用于高能电池中的锂金属阳极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-09 DOI: 10.1016/j.jechem.2025.12.002

Shuhao Wang , Hongyi Lu , Gaofeng Du , Jianing Liang , Renwu Han , Xizheng Liu , Huiqiao Li

Halide solid state electrolytes (SSEs) have attracted significant attention due to their outstanding advantages of better cathodic stability and higher ionic conductivity. However, the most halide SSEs are unstable against lithium, preventing their direct use with lithium anodes and thus sacrificing the energy density of all solid-state lithium batteries (ASSLBs), which significantly limits their application. Conventional strategies, such as employing Li-In anode or sulfide interface layer, suffer from reduced energy density or interfacial incompatibility. Employing a halide of the same family as the interface layer, instead of the chemically dissimilar sulfide SSEs, is expected to resolve the interfacial compatibility problem. Herein, we propose an all-halide double composite electrolyte (LTLC-LZC), where Li₂ZrCl₆ (LZC) serves as the bulk layer and Li_0.388Ta_0.238La_0.475Cl₃ (LTLC) functions as the anode-side interfacial contact layer. The two halide electrolytes exhibit excellent chemical compatibility and comparable processability, enabling facile cold-pressed bilayer assembly. Compared with single-layer LZC, the LTLC-LZC electrolyte significantly enhances interfacial stability and ionic conductivity. Therefore, Li|LTLC-LZC|Li symmetric cells cycle stably for over 2500 h, while Li|LTLC-LZC|NCM622 full cells deliver high initial coulombic efficiency and maintain ∼100 % coulombic efficiency during cycling. This work provides a viable pathway toward practical high-energy halide-based ASSLBs.

卤化物固态电解质由于具有良好的阴极稳定性和较高的离子电导率等突出优点而受到广泛关注。然而，大多数卤化物ssi对锂不稳定，无法直接与锂阳极一起使用，从而牺牲了所有固态锂电池（asslb）的能量密度，这极大地限制了它们的应用。传统的策略，如采用锂离子阳极或硫化物界面层，存在能量密度降低或界面不相容的问题。采用同族卤化物作为界面层，而不是化学性质不同的硫化物，有望解决界面相容性问题。在此，我们提出了一种全卤化物双复合电解质（LTLC-LZC），其中Li2ZrCl6 （LZC）作为本体层，Li0.388Ta0.238La0.475Cl3 （LTLC）作为阳极侧界面接触层。这两种卤化物电解质表现出优异的化学相容性和可加工性，便于冷压双层组装。与单层LZC相比，LTLC-LZC电解质显著提高了界面稳定性和离子电导率。因此，Li|LTLC-LZC|Li对称电池可稳定循环2500 h以上，而Li|LTLC-LZC|NCM622全电池可提供较高的初始库仑效率，并在循环过程中保持~ 100%的库仑效率。这项工作为实现高能卤化物基asslb提供了一条可行的途径。

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引用次数: 0

Extrinsic Er2O3-inspired H2O adsorption and dissociation on surface of industrial fly ash-derived SiO2 aerogel in electrocatalytic CO2 reduction 外源er2o3激发的水在工业粉煤灰SiO2气凝胶表面的吸附解离及电催化CO2还原

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-09 DOI: 10.1016/j.jechem.2025.12.004

Lifeng Han , Haorun Li , Kunming Hou , Yan Guo , Hao Wu , Mengbo Zou , Yulu Wang , Zhihua Guo , Huangdong Wang , Guixiang Ma , Shangpeng Liu , Xiaojun Gu , Shanghong Zeng

Industrial fly ash-derived SiO₂ aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO₂ reduction reaction (CO₂RR). However, how to select and arrange active sites on its surface poses significant challenges due to its non-conductive nature. Here, we subtly designed and synthesized multi-component architectures to achieve the high efficiency of CO₂RR to CO. The embedding of active and amorphous nitrogen-doped carbon (NC) nanosheets on the surface and inside of SiO₂ aerogel ensures the charge transport on the catalyst surface, and Er₂O₃ improves dissociation of H₂O, enabling the supply of protons for CO₂RR. Simultaneously, Er₂O₃-induced defects/vacancies, nanoclusters coordinated with N on amorphous NC and single Ni in NC play crucial role in enhancing adsorption and activation of CO₂. Consequently, the Ni-Er₂O₃/NC-SiO₂ catalyst exhibits the maintenance of FE_CO higher than 95 % over a wide potential window (−0.22 to −1.12 V vs. RHE) in a flow cell with gas–liquid-solid electrode. This work not only provides an atomistic understanding of nature of active sites in CO₂RR but also contributes to the secondary utilization of industrial fly ash for a carbon–neutral future.

工业粉煤灰SiO2气凝胶具有丰富的介孔结构，具有良好的负载活性成分的能力，可用于构建高效稳定的电化学CO2还原反应催化剂。然而，由于其不导电的性质，如何在其表面选择和排列活性位点是一个很大的挑战。在此，我们巧妙地设计和合成了多组分结构，以实现CO2RR到CO的高效率。在SiO2气凝胶表面和内部嵌入活性和非晶氮掺杂碳（NC）纳米片，确保了催化剂表面的电荷传输，Er2O3改善了H2O的解离，为CO2RR提供了质子。同时，er2o3诱导的缺陷/空位、非晶态NC上与N配合的纳米团簇以及NC中的单Ni对CO2的吸附和活化起着至关重要的作用。因此，Ni-Er2O3/NC-SiO2催化剂在具有气-液-固电极的流动电池中，在较宽的电位窗口（- 0.22 ~ - 1.12 V vs. RHE）内，FECO的维持率高于95%。这项工作不仅提供了对CO2RR活性位点性质的原子性理解，而且有助于工业粉煤灰的二次利用，以实现碳中和的未来。

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引用次数: 0