Journal of Energy Chemistry最新文献_第4页

Interfacial Ni–W bridge bond enabling Ni3ZnC0.7/WC heterostructure with enhanced hydrogen evolution activity and stability 界面Ni-W桥键使Ni3ZnC0.7/WC异质结构具有增强的析氢活性和稳定性

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-08 DOI: 10.1016/j.jechem.2025.12.056

Liangliang Feng , Jingyi Chen , Qianqian Liu , Yijun Liu , Mengfei Zhou , Xi Hu , Liyun Cao , Guodong Li , Yong Zhao , Jianfeng Huang

The chemical bonds at heterogeneous interfaces can optimize the hydrogen adsorption free energy (ΔG_H*) by reconfiguring the electronic structure, while an in-depth understanding of the hydrogen adsorption configuration is key to identifying the optimal active sites for enhancing hydrogen evolution performance. Here, we synthesize a wide-pH hydrogen evolution reaction (HER)-active Ni₃ZnC_0.7/WC heterostructure electrocatalyst uniformly anchored on a carbon framework through a one-step calcination method. Experimental and theoretical results demonstrate that Ni–W bridge bonds within the Ni₃ZnC_0.7/WC heterointerfaces can induce strong electronic interactions, which help to facilitate electron transfer and optimize the ΔG_H*, thereby enabling extremely excellent catalytic activity. Consequently, owing to its enhanced inherent activity and favorable electrical conductivity, Ni₃ZnC_0.7/WC exhibits exceptional catalytic performance for HER (94 and 173 mV at 10 mA/cm²) in alkaline and acidic conditions. Additionally, it can maintain durability for at least 565 h under acidic conditions and 582 h under alkaline conditions, respectively, validating its excellent catalytic stability across a broad pH range. This research provides a new perspective and theoretical basis for designing efficient and stable HER electrocatalysts through interface chemical bond engineering.

非均相界面上的化学键可以通过重新配置电子结构来优化氢的吸附自由能（ΔGH*），而深入了解氢的吸附构型是确定提高析氢性能的最佳活性位点的关键。本研究通过一步煅烧的方法，合成了一种均匀锚定在碳骨架上的具有HER活性的宽ph Ni3ZnC0.7/WC异质结构电催化剂。实验和理论结果表明，Ni3ZnC0.7/WC异质界面内的Ni-W桥键可以诱导强电子相互作用，促进电子转移并优化ΔGH*，从而获得极好的催化活性。因此，由于其增强的固有活性和良好的导电性，Ni3ZnC0.7/WC在碱性和酸性条件下表现出优异的HER催化性能（94和173 mV， 10 mA/cm2）。此外，它可以在酸性条件下保持至少565小时的耐久性，在碱性条件下保持至少582小时的耐久性，验证了它在很宽的pH范围内的优异催化稳定性。本研究为通过界面化学键工程设计高效稳定的HER电催化剂提供了新的视角和理论依据。

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引用次数: 0

Enhanced coke resistance of Fe-based garnets by in-situ formed CuFe alloy for chemical looping partial oxidation of methane 原位成形CuFe合金化学环部分氧化甲烷增强铁基石榴石抗焦炭性能

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-08 DOI: 10.1016/j.jechem.2025.12.057

Teng Zong , Xing Zhu , Ming Tian , Chaojie Wang , Nanxin Wang , Jiachen Yang , Shu Liu , Xiaodong Wang

It remains a grand challenge to inhibit coke formation for Fe-based oxygen carriers with extensive reduction due to the mismatch between the CH₄ decomposition rate on metallic Fe (Fe⁰) and the rate of the lattice oxygen migration to the surface for carbon oxidation, which led to unsatisfactory syngas selectivity and productivity for chemical looping partial oxidation of methane (CLPOM). Herein, Cu-modified Fe-based garnets (Y₃Fe₃Cu_xAl₂₋_xO₁₂ abbreviated as Fe₃Cu_xAl₂₋_x, x equals 0, 0.01, and 0.05) were designed, which exhibited boosted carbon-resistance with both CH₄ conversion and CO selectivity of 94% and extraordinary syngas productivity of almost 8 mmol g⁻¹ for Fe₃Cu_0.05Al_1.95, surpassing most of the state-of-the-art Fe-based oxygen carriers in CLPOM. This could be attributed to the in-situ formation of a CuFe alloy under reaction conditions, which remarkably decreased the activity of CH₄ decomposition over Fe⁰ sites to generate carbon and thus allowed lattice oxygen migration to the surface timely for the oxidation of coke formed.

由于CH4在金属铁（Fe0）上的分解速率与晶格氧迁移到碳氧化表面的速率不匹配，导致甲烷化学环部分氧化（CLPOM）的合成气选择性和产率不理想，抑制铁基氧载体的广泛还原结焦仍然是一个巨大的挑战。本文设计了cu修饰的fe基石榴石（Y3Fe3CuxAl2−xO12，简称Fe3CuxAl2−x， x分别为0、0.01和0.05），其CH4转化率和CO选择性均达到94%，且Fe3Cu0.05Al1.95的合成气产量接近8 mmol g−1，超过了CLPOM中大多数最先进的fe基氧载体。这可能是由于在反应条件下原位形成CuFe合金，显著降低了CH4在Fe0位点上分解生成碳的活性，从而使晶格氧及时迁移到表面氧化形成的焦炭。

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引用次数: 0

Boosting methanol steam reforming performance via crystal-phase-driven strong metal-support interactions: From encapsulated Pt nanoparticles to deeply embedded PtOx-induced Pt single atoms 通过晶体相驱动的强金属支持相互作用提高甲醇蒸汽重整性能：从封装的Pt纳米颗粒到深嵌入的pxo诱导的Pt单原子

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-07 DOI: 10.1016/j.jechem.2025.12.054

Zheng Wei, Shengfang Shi, Fei Dong, Hekun Jia, Zhiling Chen, Hongqi Wang, Bifeng Yin

Traditional strong metal-support interactions (SMSIs) induced by encapsulated reducible oxide overlayers on metal nanoparticles can suppress sintering but has a strong negative impact on the catalytic activity because of decreased availability of active sites. Herein, we design three SMSIs configurations on Pt-TiO₂ via crystal-phase engineering. These configurations comprised encapsulated Pt nanoparticle (NPs) with TiO₂₋_x overlayer on anatase, weakly embedded Pt clusters on P25, and deeply embedded PtO_x-induced Pt single-atom (SA) structure on rutile. These configurations exhibited Pt species at multiple scales, ranging from NPs to SAs. Among them, Pt supported rutile TiO₂ sample (Pt-TiO₂(R)-H) achieved extremely low CO selectivity (2.05%, 200 °C) and optimal H₂ production performance due to the enhanced SMSIs from Pt–Ti coordination in the deeply embedded PtO_x region. This Pt–Ti coordination facilitated the electron transfer from Pt to Ti and induced dual-function centers of electron-deficient Pt^δ⁺–Pt²⁺ pairs (0 < δ < 2, where Pt^δ⁺ represent Pt SAs) for methanol decomposition and electron-rich Ti³⁺–oxygen vacancies for water dissociation. Such unique configuration altered the MSR reaction pathway and the kinetic rates of each elementary step in these reaction pathways were systematically analyzed. This work proposes an SMSIs configuration induced by a deeply embedded structure, which mitigates the negative impact on catalytic activity from encapsulated overlayers, meanwhile providing a strategy for developing high-loading Pt SAs catalysts.

传统的强金属-支撑相互作用（SMSIs）是由金属纳米颗粒上的可还原性氧化物包覆层诱导的，可以抑制烧结，但由于活性位点的可用性降低，对催化活性有很强的负面影响。本文采用晶相工程的方法在Pt-TiO2上设计了三种smsi结构。这些结构包括锐钛矿上包覆TiO2−x的纳米Pt粒子（NPs）、P25上弱嵌入的Pt簇和金红石上深嵌入的pxo诱导的Pt单原子（SA）结构。这些构型显示了从NPs到SAs的多个尺度上的铂种。其中，Pt负载的金红石型TiO2样品（Pt-TiO2(R)-H）由于Pt- ti在深度嵌入PtOx区域的配位增强了smsi，实现了极低的CO选择性（2.05%,200℃）和最佳的制氢性能。这种Pt - Ti配位促进了电子从Pt到Ti的转移，并诱导了甲醇分解的缺电子Ptδ+ -Pt2 +对（0 < δ < 2，其中Ptδ+代表Pt SAs）和水解离的富电子Ti3+ -氧空位的双功能中心。这种独特的构型改变了MSR反应途径，并系统地分析了这些反应途径中每个基本步骤的动力学速率。本研究提出了一种由深嵌入结构诱导的smsi结构，该结构减轻了封装层对催化活性的负面影响，同时为开发高负载Pt SAs催化剂提供了一种策略。

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引用次数: 0

Spatially decoupled Co nanoparticles and atomic Co-N4 sites with exceptional bifunctional activity for high-power and durable Zn-air batteries 空间解耦的Co纳米粒子和具有特殊双功能活性的原子Co- n4位点用于高功率和耐用的锌空气电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-07 DOI: 10.1016/j.jechem.2025.12.055

Yiwen Cheng, Yan Tan, Aoshuang Li, Yuzhong Zhang, Chuanwei Cheng

Development of efficient and durable bifunctional oxygen electrocatalysts at a low cost and on a large scale is highly desirable, while it remains challenging for the practical application of zinc-air batteries (ZABs). Herein, we develop a bifunctional catalyst of acetylene black-supported hybrid Co nanoparticles/single atoms (Co-NPs/SACs) through a facile and scalable one-step pyrolysis strategy. The spatial decoupling of bifunctional catalytic active centers enables Co-N₄ sites to facilitate oxygen reduction reaction (ORR), while Co metal nanoparticle sites promote oxygen evolution reaction (OER). As expected, the Co-NPs/SACs exhibit exceptional bifunctional activity, achieving a high half-wave potential (E_1/2) of 0.90 V for ORR and an overpotential of 338 mV at 10 mA cm⁻² for OER. When assembled in zinc-air batteries, it delivers a superior peak power density of 303.9 mW cm⁻² and excellent cycling stability exceeding 1800 h (>4900 cycles). Remarkably, scalable catalyst fabrication and large-format (82.48 Ah) zinc-air batteries for practical application are demonstrated. Theoretical calculations elucidate that the decoupled ORR/OER active sites and interfacial electronic coupling between Co NPs and atomic Co-N₄ configuration can effectively modulate the d-band center of Co active sites and optimize the adsorption/desorption behavior of oxygen intermediates, substantially reducing the energy barrier of the rate-determining steps for both ORR and OER. This work presents a viable design concept for a bifunctional electrocatalyst in ZABs and the scalable synthesis toward practical implementation.

开发高效、耐用、低成本、大规模的双功能氧电催化剂是迫切需要的，但锌空气电池（ZABs）的实际应用仍然具有挑战性。在此，我们通过简单和可扩展的一步热解策略，开发了乙炔黑负载的杂化Co纳米颗粒/单原子（Co- nps /SACs）双功能催化剂。双功能催化活性中心的空间解耦使得Co- n4位点促进氧还原反应（ORR），而Co金属纳米粒子位点促进氧析反应（OER）。正如预期的那样，Co-NPs/SACs表现出特殊的双功能活性，ORR达到0.90 V的高半波电位（E1/2）， OER在10 mA cm - 2时达到338 mV的过电位。当在锌空气电池中组装时，它提供了303.9 mW cm - 2的卓越峰值功率密度和超过1800小时（>；4900次循环）的优异循环稳定性。值得注意的是，展示了可扩展催化剂的制造和实际应用的大尺寸（82.48 Ah）锌空气电池。理论计算表明，解耦的ORR/OER活性位点和Co NPs与Co- n4原子构型之间的界面电子耦合可以有效地调节Co活性位点的d波段中心，优化氧中间体的吸附/解吸行为，大大降低ORR和OER的速率决定步骤的能量势垒。这项工作提出了一个可行的设计概念，为ZABs双功能电催化剂和可扩展的合成走向实际实施。

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引用次数: 0

Activating sulfur redox chemistry with 1T-MoS2 for high-performance Li-S batteries 用1T-MoS2激活硫氧化还原化学用于高性能Li-S电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-07 DOI: 10.1016/j.jechem.2025.12.053

Abhimanyu Kumar Prajapati , Manas Ranjan Panda , Md. Joynul Abedin , Vu Hoang Nguyen , Maleesha M. Nishshanke , Peter Francis Prashanth , Lakshay Girdhar , Paramita Haldar , Mainak Majumder , Ashish Bhatnagar

The 1T-phase molybdenum disulfide (1T-MoS₂) has gained recognition as a valuable electrocatalyst material for lithium-sulfur (Li-S) batteries due to its outstanding physicochemical properties, including high electrical conductivity, abundant active sites, and strong polysulfides adsorption. These features effectively tackle major issues in Li-S batteries, such as polysulfide shuttling, sluggish redox reactions, low-rate capability, and limited cycle stability. In this study, a simple and scalable route has been adapted to employ 1T-MoS₂ as a catalytic sulfur host in Li-S batteries, which results in improved effectiveness of the electrocatalyst. The findings of the present studies reveal that 1T-MoS₂ significantly enhances the adsorption and conversion of lithium polysulfides (LiPSs) and diminishes the shuttle effect, resulting in a remarkable electrochemical performance compared to 2H-MoS₂. The S/1T-MoS₂ cathode achieved an impressive initial discharge capacity of 920 mAh/g and retained 750 mAh/g at a rate of 1 C after 200 cycles with a capacity retention of 81.5%. Density functional theory (DFT) calculations, including density of states (DOS) and Bader charge analysis, were also performed to further understand the mechanistic insights behind the improved electrochemical behaviour of Li-S batteries using 1T-MoS₂ as an electrocatalyst.

1t相二硫化钼（1T-MoS2）由于其优异的物理化学性能，包括高导电性、丰富的活性位点和强的多硫化物吸附，已被公认为锂硫电池（Li-S）的一种有价值的电催化剂材料。这些特性有效地解决了锂硫电池的主要问题，如多硫化物穿梭、氧化还原反应缓慢、低倍率能力和有限的循环稳定性。在本研究中，采用了一种简单且可扩展的方法，将1T-MoS2用作Li-S电池中的催化硫宿主，从而提高了电催化剂的有效性。本研究结果表明，与2H-MoS2相比，1T-MoS2显著提高了锂多硫化物（LiPSs）的吸附和转化，减少了穿梭效应，从而获得了显著的电化学性能。S/1T-MoS2阴极获得了令人印象深刻的920 mAh/g的初始放电容量，并在200次循环后以1℃的速率保持750 mAh/g，容量保持率为81.5%。密度泛函理论（DFT）计算，包括态密度（DOS）和Bader电荷分析，也被用于进一步了解使用1T-MoS2作为电催化剂改善Li-S电池电化学行为背后的机制。

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引用次数: 0

Mechano-electrochemical effects in electrochemical energy storage and catalytic materials 电化学储能和催化材料中的机械电化学效应

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-06 DOI: 10.1016/j.jechem.2025.12.050

Bin Wang , Bowen Liu , Yang Gao

The realization of dual-carbon goals heavily relies on advancing electrochemical energy storage and catalytic technologies. The performance of related functional materials is inherently linked to their mechanical stress states—a coupling known as the mechano-electrochemical (MEC) effect. Gaining a deeper understanding of this effect is essential for designing more efficient and durable electrochemical systems. This review systematically summarizes and analyzes recent progress in studying the MEC effect across energy storage and electrocatalytic materials. We first outline the fundamental principles of the MEC effect and then comparatively discuss its manifestations in both domains. For energy storage materials, we introduce in situ characterization techniques for probing mechanical-electrochemical coupling, elucidate underlying mechanisms, and summarize material design strategies that utilize the MEC effect. In electrocatalysis, we analyze the sources of intrinsic and extrinsic strain, the mechanisms of the MEC effect, and its application in enhancing catalytic performance. Finally, we provide a critical overview of current research challenges and offer perspectives on future directions in this emerging field, highlighting potential breakthroughs in MEC-guided material design.

双碳目标的实现在很大程度上依赖于电化学储能和催化技术的发展。相关功能材料的性能与它们的机械应力状态有着内在的联系，这种耦合被称为机械-电化学（MEC）效应。深入了解这种效应对于设计更高效、更耐用的电化学系统至关重要。本文系统地总结和分析了近年来在储能和电催化材料中MEC效应的研究进展。我们首先概述了MEC效应的基本原理，然后比较讨论了MEC效应在两个领域的表现。对于储能材料，我们介绍了用于探测机械-电化学耦合的原位表征技术，阐明了潜在的机制，并总结了利用MEC效应的材料设计策略。在电催化中，我们分析了内源应变和外源应变的来源、MEC效应的机理及其在提高催化性能方面的应用。最后，我们对当前的研究挑战进行了综述，并对这一新兴领域的未来发展方向提出了展望，强调了mec引导材料设计的潜在突破。

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引用次数: 0

Small-dihedral-angle solid additive engineering for optimized nanomorphology in donor/acceptor blends toward high performance organic solar cells 小二面角固体添加剂工程优化纳米形态的供体/受体共混物用于高性能有机太阳能电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-06 DOI: 10.1016/j.jechem.2025.12.051

Dan Liu, Yonghao Yang, Zhuojun Jiang, Hui Shen, Xiaosi Qi, Xiu Gong

The nanoscale morphology of the bulk-heterojunction (BHJ) active layer plays a pivotal role in governing charge dynamics and overall performance of organic solar cells (OSCs). However, Y-series acceptors, especially Y6 derivatives, exhibit strong self-aggregation tendencies that drive rapid crystallization, leading to excessive phase segregation with overly pure domains and a coarse donor/acceptor (D/A) interface, thereby impeding exciton diffusion and dissociation. Herein, we introduce a small dihedral-angle fused-ring molecule, 3,3′-Dibromo-2,2′-bithiophene (TTBr), as a solid-state morphology regulator to fine-tune the PM6:Y6 blend morphology. The planar geometry of TTBr first templates a uniform face-on π–π stacking with Y6, kinetically slowing acceptor crystallization and suppressing excessive phase aggregation. This slower crystallization affords the polymer donor sufficient time to inter-diffuse, generating a finely interpenetrated nanoscale network that restrains domain coarsening and optimizes donor/acceptor mixing. Consequently, the modified films exhibit reduced trap-assisted recombination, prolonged exciton lifetimes, and enhanced charge mobility. OSCs incorporating TTBr achieve a high efficiency of 17.91%, significantly outperforming the additive-free devices. Furthermore, the strategy demonstrates broad compatibility, yielding PCEs of 18.49 % and 18.43 % in PM6:BTP-eC9 and PM6:L8-BO, respectively. These results highlight the dihedral-angle engineering of solid additives as an effective route for controlling morphology and achieving high-efficiency OSCs.

体积异质结（BHJ）活性层的纳米形貌对有机太阳能电池（OSCs）的电荷动力学和整体性能起着至关重要的作用。然而，y系列受体，特别是Y6衍生物，表现出强烈的自聚集倾向，驱动快速结晶，导致过度的相偏析，畴过纯，供体/受体（D/ a）界面粗糙，从而阻碍了激子的扩散和解离。在此，我们引入了一个小的二面角融合环分子，3,3 ' -二溴-2,2 ' -双噻吩（TTBr），作为固态形态调节剂来微调PM6:Y6共混物的形态。TTBr的平面几何形状首先与Y6形成了均匀的面对π -π堆叠，从动力学上减缓了受体结晶并抑制了过度的相聚集。这种较慢的结晶为聚合物供体提供了足够的时间进行相互扩散，从而产生精细的互穿纳米网络，从而抑制了区域粗化并优化了供体/受体混合。因此，改性薄膜表现出减少陷阱辅助重组，延长激子寿命和增强电荷迁移率。含TTBr的OSCs效率高达17.91%，显著优于无添加剂器件。此外，该策略具有广泛的兼容性，PM6:BTP-eC9和PM6:L8-BO的pce分别为18.49%和18.43%。这些结果表明，固体添加剂的二面角工程是控制形貌和实现高效osc的有效途径。

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引用次数: 0

Proton-regulated nitrite release enables anion-derived solid electrolyte interphase for stable lithium metal anodes 质子调节的亚硝酸盐释放使阴离子衍生的固体电解质界面稳定的锂金属阳极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-06 DOI: 10.1016/j.jechem.2025.12.052

Ting-Ting Lv , Jia Liu , Li-Jie He , Xi-Long Wang , Shi-Jie Yang , Zi-Hao Zuo , Xue-Qiang Zhang , Tong-Qi Yuan , Hong Yuan

Lithium (Li) metal anodes hold exceptional promise for next-generation high-energy-density batteries, yet their practical application is hindered by unstable solid electrolyte interphase (SEI) and uncontrolled dendritic growth. Here, we proposed a proton-regulated nitrite release strategy that dynamically modulates the electrolyte solvation structure to engineer a robust and inorganic-rich SEI. Specifically, highly soluble nitrocellulose is introduced as a nitrite (NO₂⁻) reservoir, which continuously releases NO₂⁻ via proton-mediated dissociation triggered by LiPF₆ hydrolysis. The released NO₂⁻ preferentially coordinates with Li⁺, generating an anion-rich solvation sheath, and subsequently undergoes preferential reduction to form an inorganic-rich SEI enriched with Li₃N and LiN_xO_y. The resulting mechanically robust and ionically conductive interphase ensures homogeneous Li⁺ flux, enabling uniform, dendrite-free Li deposition. Moreover, the sustained NO₂⁻ release facilitates dynamic SEI repair during cycling. Consequently, Li||Li symmetric cells operate stably for over 1000 h. Li||LiNi_0.5Co_0.2Mn_0.3O₂ full cells with high-areal-loading cathodes (3.0 mAh cm⁻²) retain 80% capacity after 150 cycles at 1.0 C. Moreover, a practical 409 Wh kg⁻¹ Li||LiNi_0.83Co_0.12Mn_0.05O₂ pouch cell demonstrates stable operation over 50 cycles. This work establishes a dynamically proton-regulated anion-release paradigm for solvation structure regulation, offering a scalable pathway toward high-performance Li metal batteries.

锂（Li）金属阳极在下一代高能量密度电池中具有非凡的前景，但其实际应用受到不稳定的固体电解质界面（SEI）和不受控制的枝晶生长的阻碍。在这里，我们提出了一种质子调节的亚硝酸盐释放策略，该策略动态调节电解质溶剂化结构，以设计一个坚固且无机丰富的SEI。具体来说，高可溶性硝化纤维素作为亚硝酸盐（NO2 -）储层被引入，通过LiPF6水解引发的质子介导的解离解持续释放NO2 -。释放的NO2−优先与Li+配位，形成富阴离子的溶剂化鞘，随后优先还原形成富含Li3N和LiNxOy的富无机SEI。由此产生的机械坚固性和离子导电性界面确保了均匀的Li+通量，实现了均匀的、无枝晶的Li沉积。此外，持续的NO2−释放促进了循环过程中SEI的动态修复。因此，Li||Li对称电池稳定运行超过1000小时。Li||LiNi0.5Co0.2Mn0.3O2全电池具有高面积负载阴极（3.0 mAh cm−2）在1.0℃下150次循环后保持80%的容量。此外，一个实用的409 Wh kg−1 Li||LiNi0.83Co0.12Mn0.05O2袋电池在50次循环后显示稳定运行。这项工作建立了一个动态质子调节的阴离子释放模式，用于溶剂化结构调节，为高性能锂金属电池提供了可扩展的途径。

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引用次数: 0

Solid additive-mediated modulation of donor and acceptor aggregation for regulating phase separation in efficient all-polymer solar cells 固体添加剂介导的供体和受体聚集调节高效全聚合物太阳能电池的相分离

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-06 DOI: 10.1016/j.jechem.2025.12.042

Zhenmin Zhao , Yuanxian Liang , Hua Tang , Jiancheng Zhong , Chenxi Cao , Yuanyuan Qin , Hongxiang Li , Liang Bai , Wei Pang , Guanlin Chen , Safakath Karuthedath , Zhipeng Kan

By tuning the active layer morphology with additives, the power conversion efficiency (PCE) of all-polymer solar cells (all-PSCs) has surpassed 19%. However, the distinct aggregation behaviors of donors and acceptors often pose limitations to further performance enhancements. Herein, we introduce a novel solid additive, biphenyl (BPE), to simultaneously modulate the morphologies of both donor and acceptor materials. Characterized by its strong crystallinity and excellent compatibility with the acceptor material, BPE effectively increases the aggregation of the donor while reducing that of the acceptor. Therefore, the blend film processed with BPE achieves superior phase separation, resulting in a reduced trap density and lower energetic disorder, which culminates in an optimum PCE of 18.5% with an open-circuit voltage of 942 mV in binary devices composed of PBQx-TCl: PY-IT. Moreover, when BPE was used to selectively modulate the acceptor phase using a pseudo-planar heterojunction (PPHJ) active layer, a PCE of 17.4% was achieved, highlighting the effectiveness of enhancing the solubility of the acceptor phase in fabricating all-PSCs based on PPHJ. Our findings underscore the role of BPE-based additives in optimizing active layer phase separation, thereby facilitating the solution-processable fabrication of highly efficient all-PSCs.

通过添加添加剂调节活性层形态，全聚合物太阳能电池的功率转换效率（PCE）超过19%。然而，供体和受体不同的聚合行为往往会限制进一步的性能增强。在此，我们引入了一种新的固体添加剂，联苯（BPE），以同时调节供体和受体材料的形态。BPE具有很强的结晶度和与受体材料良好的相容性，可以有效地增加供体的聚集，同时降低受体的聚集。因此，在PBQx-TCl: PY-IT组成的二元器件中，用BPE加工的共混膜实现了优异的相分离，从而降低了陷阱密度，降低了能量无序，最终达到了最佳PCE为18.5%，开路电压为942 mV。此外，当BPE利用伪平面异质结（PPHJ）活性层选择性调制受体相时，PCE达到17.4%，突出了增强受体相溶解度在基于PPHJ制备全pscs中的有效性。我们的研究结果强调了基于bpe的添加剂在优化活性层相分离中的作用，从而促进了高效全psc的溶液可加工制造。

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引用次数: 0

Bifunctional crosslinking-induced structural engineering towards improved sodium storage in pitch-derived hard carbon 改善沥青衍生硬碳中钠储存的双功能交联诱导结构工程

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-04 DOI: 10.1016/j.jechem.2025.12.048

Yanqing Wu , Ying Mo , Wang Zhou , Liqiang Ouyang , Biao Zheng , Guoku Liu , Hui Liu , Aiping Hu , Yan Duan , Wenbin Zhong , Jilei Liu

The construction of crosslinking structures in pitch-derived carbons is essential for disrupting intrinsic π-π stacking and achieving high performance sodium-ion batteries. However, the structural collapse caused by the pyrolysis-oxidation kinetic mismatch and the challenge of rational crosslinker selection remain significant obstacles. Herein, we introduce a bifunctional crosslinking agent that simultaneously accelerates oxidative ring-opening and reinforces covalent network formation, thereby overcoming the kinetic imbalance between oxidation and pyrolysis. Specifically, 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) not only promotes generating oxygen-free radicals due to the low bond energy of its C–O bonds but also reacts with oxygen-containing functional groups in oxidized pitch to form covalent linkages, thereby further increasing crosslinking density. Consequently, the resulting hard carbons exhibit expanded interlayer spacing (d₀₀₂) and a defect-rich hierarchical porous structure. This gives rise to high reversible capacity (328.32 mAh g⁻¹), excellent rate capability (171.54 mAh g⁻¹ at 400 mA g⁻¹), and outstanding cycling stability (93.4% capacity retention after 200 cycles at 40 mA g⁻¹). Moreover, its practical feasibility is demonstrated in full cells. This work establishes a robust paradigm for developing next-generation hard carbon anodes by synergistically optimizing the bonding configuration of precursors, pore architecture, and carbon framework, while offering deep mechanistic insight into the pitch crosslinking process.

在沥青衍生碳中构建交联结构对于破坏本征π-π堆积和实现高性能钠离子电池至关重要。然而，由热解氧化动力学失配引起的结构崩溃和合理选择交联剂的挑战仍然是重要的障碍。本文介绍了一种双功能交联剂，该交联剂可以同时加速氧化开环和加强共价网络的形成，从而克服氧化和热解之间的动力学不平衡。具体来说，3,4,9,10 -苝四羧酸二酐（PTCDA）由于其C-O键的键能较低，不仅能促进氧自由基的生成，还能与氧化沥青中的含氧官能团反应形成共价键，从而进一步提高交联密度。因此，所得到的硬碳表现出扩大的层间距（d002）和富含缺陷的分层多孔结构。这产生了高可逆容量（328.32 mAh g - 1），出色的倍率容量（171.54 mAh g - 1, 400 mA g - 1），以及出色的循环稳定性（在40 mA g - 1下200次循环后，容量保持率为93.4%）。并在全电池中验证了其实际可行性。这项工作通过协同优化前驱体、孔隙结构和碳框架的键合配置，为开发下一代硬碳阳极建立了一个强大的范例，同时为节距交联过程提供了深入的机制见解。

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引用次数: 0