Journal of Energy Chemistry最新文献_第9页

Remarkable photoexciton enhancement induced by heterogeneous facet engineering for benchmark CO2 photothermal reduction 非均质面工程诱导CO2基准光热还原的显著光激子增强

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-16 DOI: 10.1016/j.jechem.2025.12.016

Wenyu Yuan, Rou-Yu Li, Hui Zhang, Meng-Ru Cui, Jing-Qiao Sun, Quan-Guo Zhai

Developing effective strategies to modulate carrier concentration and migration is crucial for advancing photocatalysis. In this study, we pioneer that the built-in electrical field (BIEF), induced by heterogeneous facet engineering, can efficiently promote photoexciton concentration and enhance carrier mobility. As a proof-of-concept, hetero-faceted MOFs coupled with noble metals were successfully constructed via a novel water modulation strategy, where water served as a “Ti⁴⁺ release capsule” for precise crystal facet control. The resulting hetero-facets established a tailorable BIEF, which facilitated efficient transfer of thermally excited electrons and significantly enhanced photoexciton concentration. The optimized Pd/t-MUV-10 catalyst achieved an unprecedented CO production rate of 1.87 mmol g⁻¹ h⁻¹ was achieved via photothermal conversion of CO₂ and H₂O, representing a 21-fold enhancement over Pd, which surpassed all previously reported photothermal catalysts. In situ characterizations and theoretical calculations further confirmed that facet-induced BIEF effectively suppressed random electron scattering, modulated electron distribution, increased photoexciton concentration, and thereby boosted catalytic activity. These findings establish facet engineering as a novel paradigm for modulating carrier concentration, providing new insights into the design of efficient photothermal catalytic systems.

开发有效的策略来调节载流子浓度和迁移是推进光催化的关键。在这项研究中，我们率先提出了由非均质面工程诱导的内置电场（BIEF）可以有效地促进光激子浓度和增强载流子迁移率。作为概念验证，通过一种新的水调制策略，成功构建了与贵金属耦合的异质面mof，其中水作为“Ti4+释放胶囊”，用于精确的晶体面控制。由此产生的异质面建立了一个可定制的BIEF，促进了热激发电子的有效转移，并显着提高了光激子浓度。优化后的Pd/t-MUV-10催化剂通过CO2和H2O的光热转化实现了前所未有的1.87 mmol g−1 h−1的CO产率，比Pd提高了21倍，超过了之前报道的所有光热催化剂。原位表征和理论计算进一步证实了面诱导BIEF有效抑制了随机电子散射，调制了电子分布，增加了光激子浓度，从而提高了催化活性。这些发现确立了面工程作为调节载流子浓度的新范式，为设计高效光热催化系统提供了新的见解。

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引用次数: 0

A nano-island surface architecture that unlocks synergistic kinetic and stability enhancements in P2-type sodium-ion battery cathodes 一种纳米岛表面结构，解锁了p2型钠离子电池阴极的协同动力学和稳定性增强

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-17 DOI: 10.1016/j.jechem.2025.12.021

Yu Huang , Gui Chu , Mao Wang , Kehan Li , Tongen Lin , Lili Wang , Yongqi Sun , Kui Li , Xiaobo Zhu

P2-type layered oxides are promising cathodes for sodium-ion batteries, yet their practical application is hindered by structural instability and parasitic interfacial reactions. Conventional surface coatings face a fundamental trade-off, where protective layers inevitably introduce additional Na⁺ transport paths and barriers. Here, we overcome this limitation by designing a multifunctional Nd-rich nano-island heterostructure on the P2-type cathode surface. Driven by a large lattice mismatch, this non-continuous architecture creates a thermodynamically stable interface where chemically rooted, electronically conductive nano-islands enhance charge transfer, while inter-island channels maintain open pathways for rapid Na⁺ diffusion. Theoretical calculations reveal that the heterostructure improves surface conductivity and anchors lattice oxygen via strong Nd–O bonds. Experimentally, in situ XRD confirms the mitigation of the detrimental P2-O2 phase transition by a buffering Z-phase and the recovery of lattice parameters upon discharge, while depth-resolved ToF-SIMS validates the formation of a thin, compact, and inorganic-rich cathode-electrolyte interphase that reduces interfacial side reactions. Consequently, the engineered cathode demonstrates exceptional rate performance (90 mA h g⁻¹ at 20 C), outstanding cycling stability (85.8 % retention over 200 cycles), and demonstrated potential in practical pouch cell configurations.

p2型层状氧化物是一种很有前途的钠离子电池阴极材料，但其实际应用受到结构不稳定性和寄生界面反应的阻碍。传统的表面涂层面临着一个基本的权衡，其中保护层不可避免地引入额外的Na+传输路径和屏障。在这里，我们通过在p2型阴极表面设计多功能富nd纳米岛异质结构来克服这一限制。在大晶格失配的驱动下，这种非连续结构创造了一个热力学稳定的界面，其中化学扎根的电子导电纳米岛增强了电荷转移，而岛间通道保持了Na+快速扩散的开放途径。理论计算表明，异质结构提高了表面导电性，并通过强Nd-O键锚定晶格氧。实验中，原位XRD证实了缓冲z相减缓了有害的P2-O2相变，并在放电时恢复了晶格参数，而深度分辨ToF-SIMS证实了薄、致密、富无机的阴极电解质界面相的形成，减少了界面副反应。因此，该工程阴极表现出优异的倍率性能（20℃下90 mA h g−1），出色的循环稳定性（200次循环保持率85.8%），并在实际的袋状电池配置中显示出潜力。

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引用次数: 0

Layer-dependent ammonia activation on VOx/Cu inverse catalysts VOx/Cu反相催化剂的层依赖氨活化

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-16 DOI: 10.1016/j.jechem.2025.12.015

Youbin Wu , Dongsen Zhang , Shengdi Zhao , Ruihan Rao , Yingli Liu , Yuanjie Bao , Yan Zhang , Geng Sun , Rentao Mu , Wenpo Shan , Yun Liu , Hong He

Overcoming the kinetic barrier of N–H bond activation in NH₃ remains a central challenge in enabling efficient ammonia decomposition as well as thermocatalytic and electrocatalytic ammonia oxidation. Oxide-on-metal inverse catalysts offer promising opportunities to address this challenge; however, the role of oxide overlayer thickness in governing surface structures and reactivity is still poorly understood. Herein, we have elucidated the layer-dependent atomic structure of vanadium oxide overlayers on Cu(1 1 1) surfaces and its implications for NH₃ adsorption, using a combination of high-resolution scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. Despite sharing the same vanadium oxidation state (V³⁺), VO_x overlayers on Cu(1 1 1) adopt distinct atomic structures depending on the overlayer thickness. A nonlinear correlation is observed between VO_x overlayer thickness and N–H activation capability. The surface-V₂O₃ phase formed by 2–3 VO_x layers exhibits the highest activity, enabling both molecular and dissociative adsorption of NH₃. In contrast, thicker bulk-V₂O₃(0001) (>3 VO_x layers) only shows molecular adsorption without dissociation, while the monolayer VO(1 1 1) surface exhibits negligible NH₃ adsorption. These findings underscore the pivotal influence of oxide overlayer thickness in modulating oxide-on-metal inverse catalyst systems, providing atomic-level insights that can guide the rational design of high-performance catalytic materials for NH₃ activation.

克服NH3中N-H键激活的动力学障碍仍然是实现高效氨分解以及热催化和电催化氨氧化的核心挑战。金属上氧化物反催化剂为解决这一挑战提供了很有希望的机会；然而，氧化层厚度在控制表面结构和反应性中的作用仍然知之甚少。在此，我们利用高分辨率扫描隧道显微镜（STM）、x射线光电子能谱（XPS）和密度泛函理论（DFT）计算，阐明了Cu（11 11）表面氧化钒覆盖层的层依赖原子结构及其对NH3吸附的影响。尽管具有相同的钒氧化态（V3+），但Cu（11 11 1）上的VOx覆盖层根据覆盖层厚度采用不同的原子结构。VOx层厚度与N-H活化能力之间存在非线性相关关系。由2-3层VOx形成的表面- v2o3相表现出最高的活性，可以同时进行NH3的分子吸附和解离吸附。相比之下，较厚的大块v2o3 (0001) （>；3 VOx层）只表现出分子吸附而不解离，而单层VO（11 11）表面对NH3的吸附可以忽略不计。这些发现强调了氧化物覆盖层厚度对调节氧化物-金属逆催化剂体系的关键影响，提供了原子水平的见解，可以指导合理设计用于NH3活化的高性能催化材料。

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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 : 2026-04-01 Epub 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

Sulfurization-induced uniform Ag nanoparticles anchoring for long-lasting anode protection in alkaline seawater electrolysis 硫酸诱导均匀银纳米颗粒锚定在碱性海水电解中持久阳极保护的研究

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-02 DOI: 10.1016/j.jechem.2025.11.048

Haocheng Chen , Sixie Zhang , Yingjie Wen , Li Yi , Denggui Wang , Jinchao Zhu , Xu Chen , Wuyong Zhang , Wenwen Xu , Jianwei Nai , Zhiyi Lu

Seawater electrolysis is a promising approach for sustainable hydrogen production, while the abundant halides in seawater (particularly Cl⁻, ∼0.4–0.5 M) aggressively corrode the anode substrate, drastically shortening the lifespan of the anode. Here, we report a rigid corrosion-resistant anode composed of Ag nanoparticles anchored on sulfurized NiFe nanosheets (NiFeS@Ag) for highly durable oxygen evolution reaction (OER) in alkaline seawater. In experiments, NiFeS@Ag delivers excellent OER activity (400 mA cm⁻² in 280 mV overpotential) and exceptional durability, maintaining operation for over 1000 h in high-concentrated alkaline brine electrolyte and exceeding 7000 h in alkaline seawater. Characterizations and simulations reveal that, during OER, Ag nanoparticles remain uniformly dispersed without obvious agglomeration due to the robust Ag–S bridges between Ag and NiFeS, further immobilizing more Cl⁻ in the form of AgCl to effectively repel corrosive halide, underpinning the long-term stability. The scaled-up NiFeS@Ag/Ni mesh anode further demonstrates stable operation over 1000 h in a multi-cell electrolyzer at 200 mA cm⁻² and 80 °C. Our anode protection strategy provides significant guidance for designing long-life anodes for commercial alkaline seawater electrolysis.

海水电解是一种很有前途的可持续制氢方法，而海水中丰富的卤化物（特别是Cl−，~ 0.4-0.5 M）会严重腐蚀阳极基体，大大缩短阳极的使用寿命。在这里，我们报道了一种刚性耐腐蚀阳极，该阳极由银纳米粒子组成，锚定在硫化NiFe纳米片上（NiFeS@Ag），用于碱性海水中高度持久的出氧反应（OER）。在实验中，NiFeS@Ag具有优异的OER活性（在280 mV过电位下400 mA cm - 2）和优异的耐久性，在高浓度碱性盐水电解质中保持超过1000小时的运行，在碱性海水中保持超过7000小时的运行。表征和模拟表明，在OER过程中，由于Ag和NiFeS之间存在强大的Ag - s桥接，Ag纳米粒子保持均匀分散，没有明显的团聚，进一步以AgCl的形式固定更多的Cl−，有效地抵抗腐蚀性卤化物，支撑了长期稳定性。放大NiFeS@Ag/Ni网状阳极进一步证明了在200 mA cm - 2和80°C的多电池电解槽中稳定运行超过1000小时。我们的阳极保护策略对商业碱性海水电解长寿命阳极的设计具有重要的指导意义。

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引用次数: 0

Machine learning predicts microstructure impact on discharge performance in hard carbon anodes for K-ion batteries 机器学习预测k离子电池硬碳阳极的微观结构对放电性能的影响

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-11-17 DOI: 10.1016/j.jechem.2025.10.061

Tianshuang Qi , Kai Xiong , Xiong Zhang , Honggang Ding , Haiping Yang

To address the challenges of weak cycling stability and low capacity in hard carbon (HC), elucidating the structure-performance relationship between their microstructure and potassium-ion battery (PIB) performance is crucial. To this end, this study developed an interpretable machine learning workflow that identified optimal machine learning models for six key electrochemical performance metrics, including cycling performance, through multi-model comparison. All performance prediction models demonstrated excellent generalization capability, with the AdaBoost model achieving the highest test set coefficient of determination (R²) of 0.819 for the cyclic factor, while all models maintain root mean square error (RMSE) below 8 %. By integrating advanced interpretable ML methods such as Shapley additive explanations (SHAP) and accumulated local effects (ALE), the study systematically identified critical thresholds and synergistic interaction ranges where key structural features exert positive effects. Taking the cyclic factor as an example, the results reveal that optimal synergistic enhancement of cycling performance is achieved when degree of graphitization ranges between 100 % and 200 %, S content exceeds 7 at%, and the number of graphene layers exceeds 3. The data-driven paradigm of “structural features-performance output-synergistic thresholds” established in this work provides a reliable theoretical foundation and experimentally verifiable optimization pathway for the targeted design of high-performance HC anodes.

为了解决硬碳（HC）的弱循环稳定性和低容量的挑战，阐明其微观结构与钾离子电池（PIB）性能之间的结构性能关系至关重要。为此，本研究开发了一个可解释的机器学习工作流程，通过多模型比较，确定了六个关键电化学性能指标（包括循环性能）的最佳机器学习模型。所有性能预测模型均表现出优异的概化能力，其中AdaBoost模型的循环因子的检验集决定系数（R2）最高为0.819，而所有模型的均方根误差（RMSE）均保持在8%以下。通过整合Shapley加性解释（SHAP）和累积局部效应（ALE）等先进的可解释ML方法，该研究系统地确定了关键结构特征发挥积极作用的关键阈值和协同作用范围。以循环因子为例，当石墨化度在100% ~ 200%之间，S含量超过7at %，石墨烯层数超过3层时，循环性能的协同增强效果最佳。本文建立的“结构特征-性能输出-协同阈值”的数据驱动范式，为高性能HC阳极的定向设计提供了可靠的理论基础和实验验证的优化路径。

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引用次数: 0

Pre-sodiation strategies for high reversibility of hard carbon anodes: a review 高可逆性硬碳阳极的预酸化策略综述

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-16 DOI: 10.1016/j.jechem.2025.12.013

Yuqi Dong , Yanbin Ning , Lin Zhou , Shengwei Dong , Zhuomin Qiang , Kun Lin , Dalong Li , Li Guan , Shuaifeng Lou

Sodium-ion batteries (SIBs) represent a promising next-generation energy storage technology, yet their commercialization is impeded by low initial Coulombic efficiency, which severely limits energy density. This issue stems from irreversible sodium consumption during cycling, primarily caused by solid electrolyte interphase (SEI) formation and parasitic side reactions. Such sodium loss not only reduces energy output but also accelerates electrode degradation, thereby shortening cycle life. Pre-sodiation has emerged as an essential strategy to mitigate these challenges by introducing an external sodium source to compensate for irreversible sodium loss, thereby improving both energy density and long-term cyclability. However, developing efficient, scalable, and economically viable pre-sodiation methods remains a critical hurdle. This review is motivated by the urgent need to systematize and evaluate emerging pre-sodiation strategies specifically for hard carbon anodes—a leading candidate in SIB applications—and to provide strategic guidance for future research. We comprehensively summarize and analyze both conventional and novel pre-sodiation methods, correlating their mechanisms with the fundamental sources of sodium loss. Furthermore, we compare the practicality and scalability of recent advances, identify key technical barriers, and propose a holistic framework combining complementary sodium supplementation and storage approaches. Finally, we offer forward-looking perspectives on the development of industrially applicable pre-sodiation techniques, underscoring their vital role in achieving high-energy–density and long-life sodium-ion batteries.

钠离子电池（sib）是一种很有前途的下一代储能技术，但其商业化受到低初始库仑效率的阻碍，这严重限制了能量密度。这个问题源于循环过程中不可逆的钠消耗，主要是由固体电解质间相（SEI）的形成和寄生副反应引起的。这种钠的损失不仅降低了能量输出，而且加速了电极的降解，从而缩短了循环寿命。通过引入外部钠源来补偿不可逆的钠损失，从而提高能量密度和长期可循环性，预钠化已成为缓解这些挑战的重要策略。然而，开发高效、可扩展且经济可行的预酸化方法仍然是一个关键障碍。这篇综述的动机是迫切需要系统化和评估专门针对硬碳阳极（SIB应用的主要候选材料）的新兴预调解策略，并为未来的研究提供战略指导。我们全面总结和分析了传统的和新型的预钠化方法，并将它们的机制与钠损失的基本来源联系起来。此外，我们比较了最近进展的实用性和可扩展性，确定了关键的技术障碍，并提出了一个将补充钠补充和储存方法相结合的整体框架。最后，我们对工业应用的预钠化技术的发展提供了前瞻性的观点，强调了它们在实现高能量密度和长寿命钠离子电池中的重要作用。

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引用次数: 0

Surface chemistry in regulating electrolyte stability on lithium metal anodes: the role of LiF and Li2O 表面化学在调节锂金属阳极上电解质稳定性中的作用：LiF和Li2O的作用

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-01 DOI: 10.1016/j.jechem.2025.11.043

Zi-Yue Jiang , Nan Yao , Yan-Bin Gao , Yu-Hang Yuan , Yao-Peng Chen , Yu-Chen Gao , Rui Zhang , Xiang Chen

Lithium (Li) metal batteries hold great promise due to their high energy density, yet severe side reactions between routine organic electrolytes and the Li metal anode hinder their practical implementation. Elucidating the fundamental mechanisms that govern electrolyte stability on the Li metal anode is crucial to stabilizing the electrolyte–anode interface and promoting the practical applications of Li metal batteries. Herein, the regulation mechanism of the anode surface on the electrolyte stability is revealed at the atomic scale by density functional theory calculations. Indicated by the changes in the lowest unoccupied molecular orbital (LUMO) energy levels, solvents exhibit markedly lower reductive stability on Li metal surfaces compared with bulk molecules, making them more prone to parasitic reactions. Two major components in solid electrolyte interphase (SEI), i.e., LiF and Li₂O, can passivate the solvent reduction through an average increase of 1.46 eV in their LUMO energy levels. The LUMO energy changes are further correlated with the Li–O distance between the solvents and SEI components, exhibiting an approximately linear relationship. This work reveals the role of the SEI in protecting Li metal anodes from electrolyte corrosion and identifies key factors regulating solvent stability, providing fundamental insights for the rational design of advanced electrolytes and robust SEI for practical Li metal batteries.

锂（Li）金属电池由于其高能量密度而具有很大的前景，但常规有机电解质与锂金属阳极之间的严重副反应阻碍了其实际应用。阐明锂金属阳极上电解液稳定性的基本机制，对于稳定电解阳极界面，促进锂金属电池的实际应用具有重要意义。本文通过密度泛函理论计算，揭示了阳极表面在原子尺度上对电解质稳定性的调控机理。最低未占据分子轨道（LUMO）能级的变化表明，溶剂在Li金属表面上的还原稳定性明显低于散装分子，使其更容易发生寄生反应。固体电解质界面（SEI）中的两种主要成分LiF和Li2O可以通过平均增加1.46 eV的LUMO能级来钝化溶剂还原。LUMO能量的变化与溶剂和SEI组分之间的Li-O距离进一步相关，呈现近似线性关系。这项工作揭示了SEI在保护锂金属阳极免受电解质腐蚀中的作用，并确定了调节溶剂稳定性的关键因素，为合理设计先进电解质和实用锂金属电池的坚固SEI提供了基本见解。

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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 : 2026-04-01 Epub 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

Dimensionality-engineered electron channels for directional acceleration of 1,4-NADH-dependent photoenzymatic CO2-to-liquid fuels 定向加速1,4- nadh依赖光酶二氧化碳到液体燃料的维度工程电子通道

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-04-01 Epub Date: 2025-12-02 DOI: 10.1016/j.jechem.2025.11.050

Jinde Cai , Xiuling Ji , Wanrong Dong , Boxia Guo , Hongguang Zhang , Jinguang Hu , Yuhong Huang

Efficient and selective regeneration of enzymatically active 1,4-NADH from NAD⁺ is pivotal for accelerating photoenzymatic CO₂ conversion. However, constructing photocatalysts that sustain continuous electron flow and provide sufficient hydride supply remains a major challenge. Herein, we report a rhodium-coordinated three-dimensional conjugated polymer (3D-Bpy-Rh) photocatalyst featuring multiple electron channels, designed through dimensionality engineering and incorporation of hydride-forming active centers. Such a 3D structure promotes rapid charge separation and multidimensional electron migration, while facilitating trapped-electron release to Rh centers for accelerated electron transfer. As a result, 3D-Bpy-Rh achieves a visible-light driven NADH regeneration efficiency of 90.8 % with 99.2 % selectivity toward 1,4-NADH, surpassing state-of-the-art photocatalysts. Furthermore, the mechanism between the electron reduction capability of the photocatalyst and the selective formation of 1,4-NADH was elucidated, combining transient absorption spectroscopy analysis and DFT calculations. When integrated into photoenzymatic systems, this photocatalyst enhances CO₂ conversion, boosting methanol and ethanol yields by 5.2- and 2.0-fold, respectively. These results highlighted the potential of dimensionality-engineered photocatalysts for selective 1,4-NADH regeneration and efficient photoenzymatic fuel synthesis.

高效和选择性地从NAD+中再生酶活性1,4- nadh是加速光酶CO2转化的关键。然而，构建维持连续电子流和提供足够氢化物供应的光催化剂仍然是一个主要挑战。在此，我们报道了一种具有多电子通道的铑配位三维共轭聚合物（3D-Bpy-Rh）光催化剂，该催化剂通过维度工程和氢化物形成活性中心的结合而设计。这种三维结构促进了快速的电荷分离和多维电子迁移，同时促进了被困电子释放到Rh中心以加速电子转移。结果，3D-Bpy-Rh实现了90.8%的可见光驱动NADH再生效率，对1,4-NADH的选择性为99.2%，超过了目前最先进的光催化剂。结合瞬态吸收光谱分析和DFT计算，阐明了光催化剂的电子还原能力与1,4- nadh选择性生成之间的机理。当整合到光酶系统中时，这种光催化剂可以提高二氧化碳的转化率，将甲醇和乙醇的产量分别提高5.2倍和2.0倍。这些结果突出了尺寸工程光催化剂在选择性1,4- nadh再生和高效光酶燃料合成方面的潜力。

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