Journal of Energy Chemistry最新文献_第3页

Phase-separated polymer electrolytes with dual-interface enhancement effect for high-loading lithium metal batteries 高负荷锂金属电池用双界面增强相分离聚合物电解质

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-19 DOI: 10.1016/j.jechem.2026.01.017

Zhipeng He , Enhua Dong , Cheng Li , Jiaxuan Liu , Yutong Jing , Mingyu Yin , Lei Wang , Yuhang Zhang , Shen Liu , Dianlong Wang , Pengfei Yan , Huakun Liu , Shixue Dou , Bo Wang

Solid polymer electrolytes (SPEs) offered enhanced safety and superior lithium dendrite suppression compared to liquid electrolytes, yet suffered from inadequate ionic conductivity and poor interfacial stability. Phase-separated polymer electrolytes (PSPEs) partially addressed these limitations but introduced dual-interface challenges, including insufficient electrode contact and inhomogeneous phase distribution. This work presented a novel BSF composite electrolyte fabricated through in situ polymerization of a PSPEs system comprising butyl acrylate (BA), succinonitrile (SN), and LiTFSI, with fluoroethylene carbonate (FEC) as a critical additive. This design simultaneously enhanced the compatibility between the polymerized BA matrix and the SN liquid phase, established continuous ion transport pathways, improved interfacial wettability, and generated stable LiF-rich interphases at both electrodes. The structural evolution and interfacial chemistry were systematically verified through Raman mapping, HAADF-STEM, and TOF-SIMS analyses. Electrochemical evaluation demonstrated exceptional performance. The constructed Li|BSF|Li symmetric cells achieved stable cycling for over 2000 h at 0.5 mA/cm² with a critical current density (CCD) of 4.2 mA/cm². Moreover, Li|BSF|NCM811 full cells with a high mass loading (18 mg/cm²) retained 80.5% of their capacity after 100 cycles. These results represented state-of-the-art performance among polymer-based solid electrolytes, underscoring the potential of the BSF system for high-energy–density lithium metal batteries.

与液体电解质相比，固体聚合物电解质（spe）具有更高的安全性和更好的锂枝晶抑制能力，但存在离子电导率不足和界面稳定性差的问题。相分离聚合物电解质（pspe）部分解决了这些限制，但引入了双界面挑战，包括电极接触不足和相分布不均匀。本文提出了一种新型的BSF复合电解质，该电解质由丙烯酸丁酯（BA）、丁二腈（SN）和LiTFSI组成，以氟碳酸乙烯（FEC）为关键添加剂，通过原位聚合制备。该设计同时增强了聚合BA基质与SN液相之间的相容性，建立了连续的离子传输途径，提高了界面润湿性，并在两个电极上生成了稳定的富liff界面相。通过Raman mapping、HAADF-STEM和TOF-SIMS分析系统地验证了结构演化和界面化学。电化学评价显示出优异的性能。所构建的Li|BSF|Li对称电池在0.5 mA/cm2下稳定循环超过2000小时，临界电流密度（CCD）为4.2 mA/cm2。此外，高质量负载（18 mg/cm2）的Li|BSF|NCM811充满电池在100次循环后保持了80.5%的容量。这些结果代表了聚合物固体电解质中最先进的性能，强调了BSF系统在高能量密度锂金属电池中的潜力。

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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 : 2026-05-01 Epub 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

Unlocking high-rate MXenes as lithium-ion battery anodes via Σ7 coincidence site lattice grain boundaries 通过Σ7重合点晶格晶界解锁高速率MXenes作为锂离子电池阳极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-19 DOI: 10.1016/j.jechem.2025.12.023

Yifan Wu , Zhongyong Zhang , Shangquan Zhao , Bin Huang , Neng Li , Naigen Zhou

Grain boundaries (GBs), particularly Σ7 coincidence site lattice (CSL) defects experimentally observed in MXenes, significantly influence their performance as lithium-ion battery (LIB) anodes. This work systematically investigates the impact of Σ7 GBs on MXene electrochemical properties, with a focus on rate capability. The results indicated that Σ7 GB formation is thermodynamically favored in Ti₂C, Nb₂C, and Mo₂C MXenes compared to other M₂C compositions, with stability further enhanced by oxygen and sulfur surface functionalization. These GBs induce substantial geometric distortions that reduce surface charge localization while enhancing electrical conductivity in Ti₂CO₂. The altered electronic structure at GB sites weakens lithium adsorption strength without promoting lithium dendrite formation. Furthermore, diffusion kinetics calculations reveal significantly reduced lithium diffusion barriers at Σ7 GBs in Ti₂C, Mo₂C, and Mo₂CS₂ compared to pristine materials. Mechanistic analysis attributes this enhancement to diminished charge localization at GB regions, which generates a “charge pool” effect—a zone of uniformly distributed free charge observed in Ti₂C and Mo₂C. This charge pool not only facilitates ultra-low lithium diffusion barriers (as low as 11 meV in M₂C at 0.1 V vs. Li⁺/Li) but also enhances potential responsiveness of diffusion kinetics. Our findings establish the intentional introduction of Σ7 GBs as an effective strategy for designing high-rate MXene anodes. This work provides fundamental insights into GB-enhanced electrochemical mechanisms in 2D materials, offering crucial theoretical guidance for the design of high-rate anode materials.

MXenes中晶界（GBs），特别是Σ7重合点阵（CSL）缺陷，对其作为锂离子电池（LIB）阳极的性能有显著影响。这项工作系统地研究了Σ7 gb对MXene电化学性能的影响，重点是速率能力。结果表明，与其他M2C组分相比，在Ti2C、Nb2C和Mo2C MXenes中Σ7 GB的形成在热力学上更有利，并且通过氧和硫的表面官能化进一步增强了稳定性。这些gb诱导了大量的几何畸变，减少了表面电荷的局部化，同时增强了Ti2CO2中的导电性。GB位电子结构的改变削弱了锂的吸附强度，但没有促进锂枝晶的形成。此外，扩散动力学计算表明，与原始材料相比，Ti2C， Mo2C和Mo2CS2中Σ7 gb的锂扩散屏障显著降低。机理分析将这种增强归因于GB区域电荷局域化的减弱，这产生了“电荷池”效应——在Ti2C和Mo2C中观察到一个均匀分布的自由电荷区。这种电荷池不仅有利于超低锂扩散势垒（与Li+/Li相比，0.1 V时M2C的锂离子扩散势垒低至11 meV），而且还增强了扩散动力学的潜在响应性。我们的研究结果确立了有意引入Σ7 gb作为设计高速率MXene阳极的有效策略。这项工作为二维材料中gb增强的电化学机制提供了基本的见解，为设计高速率阳极材料提供了重要的理论指导。

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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 : 2026-05-01 Epub 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

Synergistic engineering of the electric double layer and solid electrolyte interphase by a trace glutamate-derived additive for stable aqueous zinc-ion batteries 用微量谷氨酸衍生添加剂对稳定水锌离子电池双电层和固体电解质界面的协同工程

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-17 DOI: 10.1016/j.jechem.2025.12.019

Dongyin Liu , Yuanjun Zhang , Yuhao Wu , Xiaoyang Zheng , Guanyao Wang , Hua-Kun Liu , Shi-Xue Dou , Chao Wu

Aqueous zinc-ion batteries (AZIBs) have garnered considerable attention as promising candidates for next-generation energy storage systems due to their inherent advantages. However, AZIBs have also constantly encountered interfacial challenges arising from the structure of the electric double layer (EDL) and the composition of the solid electrolyte interphase (SEI), fundamentally limiting their reversibility and cycling stability. Herein, we propose a novel trace additive strategy employing tetrasodium glutamate diacetate (TGD) to simultaneously reconstruct the EDL and form a stable SEI on the zinc anode surface. TGD molecules could preferentially adsorb on the zinc anode surface, which could displace water molecules from the inner Helmholtz plane (IHP) to reconstruct a water-deficient EDL and suppress hydrogen evolution reactions/water-induced parasitic reactions. Moreover, the adsorbed TGD molecules could also be involved in the formation of a stable organic–inorganic hybrid SEI, effectively stabilizing the anode/electrolyte interface, reducing interfacial impedance and facilitating uniform zinc deposition. Consequently, the symmetric cells deliver an outstanding cycling life of over 4800 h at 1 mA cm⁻² and 1 mA h cm⁻², and Zn||Cu cells achieve a high average Coulombic efficiency of 99.64 % for up to 2250 cycles. The Zn||PANI full cell with TGD-based electrolyte retains 91.32 % capacity after 2000 cycles at 3 A g⁻¹. These findings highlight TGD-based interface engineering as a viable strategy for high-performance AZIBs.

水性锌离子电池（azib）由于其固有的优点，作为下一代储能系统的有前途的候选者，已经引起了相当大的关注。然而，azib也不断遇到来自双电层（EDL）结构和固体电解质界面相（SEI）组成的界面挑战，从根本上限制了它们的可逆性和循环稳定性。在此，我们提出了一种新的微量添加剂策略，使用谷氨酸四钠（TGD）来同时重建EDL并在锌阳极表面形成稳定的SEI。TGD分子可以优先吸附在锌阳极表面，取代内部亥姆霍兹面（IHP）中的水分子，重建缺水EDL，抑制析氢反应/水诱导寄生反应。此外，吸附的TGD分子还可以参与形成稳定的有机-无机杂化SEI，有效地稳定阳极/电解质界面，降低界面阻抗，促进均匀的锌沉积。因此，对称电池在1ma cm - 2和1ma h cm - 2下的循环寿命超过4800小时，而Zn||Cu电池在2250次循环中实现了99.64%的平均库仑效率。采用tgd基电解质的Zn||PANI全电池在3ag−1下循环2000次后容量保持在91.32%。这些发现强调了基于tgd的界面工程是高性能azib的可行策略。

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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 : 2026-05-01 Epub 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

Covalent network topology engineering for synergistic ionogels in stable lithium metal batteries 稳定锂金属电池中协同离子凝胶的共价网络拓扑工程

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-12 DOI: 10.1016/j.jechem.2026.01.002

Meng Wang, Huangxuanyu Yang, Zhaoyuan Ding, Hu Zhang, Hao Wu, Ruiping Liu

Unraveling the critical role of network topology in ionogel electrolytes, this study demonstrates that a covalent integration strategy is paramount for synergizing mechanical robustness and ion transport. Through a comparative design, a multi-network ionogel featuring covalently anchored poly(ethylene glycol) diacrylate segments within a rigid-flexible liquid crystal polymer/polyacrylamide framework was developed. In contrast to its physically blended counterpart, this covalently engineered ionogel exhibits a well-defined, bi-continuous architecture, as confirmed by multi-scale characterization. This optimized topology confers the material with a remarkable combination of properties: high ionic conductivity (5.55 mS cm^–1), exceptional toughness (3.217 MJ m^–3), and a low activation energy (6.87 kJ mol^–1). Mechanistically, the covalent network not only provides continuous ion pathways but also facilitates the in-situ formation of a stable, LiF/Li₃N-rich solid electrolyte interphase at the electrode-electrolyte interface. Consequently, it enables ultra-stable Li||Li symmetric cells exceeding 1600 h at 0.1 mA cm^–2 and demonstrates excellent performance in Li||LiFePO₄ cells. This work demonstrates that, within the multi-network ionogel design, precise topological control via covalent engineering proves to be a more effective strategy than physical blending for developing high-performance electrolytes for stable lithium metal batteries.

这项研究揭示了网络拓扑在离子凝胶电解质中的关键作用，表明共价整合策略对于协同机械稳健性和离子传输至关重要。通过比较设计，在刚柔液晶聚合物/聚丙烯酰胺框架内开发了一种具有共价锚定聚乙二醇二丙烯酸酯片段的多网络离子凝胶。与物理混合的电离子凝胶相比，这种共价工程的电离子凝胶具有良好定义的双连续结构，多尺度表征证实了这一点。这种优化的拓扑结构赋予了材料显著的性能组合：高离子电导率（5.55 mS cm-1），优异的韧性（3.217 MJ m-3）和低活化能（6.87 kJ mol-1）。从机制上讲，共价网络不仅提供了连续的离子通路，而且还促进了在电极-电解质界面处原位形成稳定的、富含LiF/ li3n的固体电解质界面相。因此，它可以实现在0.1 mA cm-2下超过1600小时的超稳定Li||Li对称电池，并且在Li||LiFePO4电池中表现出优异的性能。这项工作表明，在多网络离子凝胶设计中，通过共价工程进行精确的拓扑控制被证明是一种比物理混合更有效的策略，可以开发用于稳定锂金属电池的高性能电解质。

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引用次数: 0

Assembling atomically dispersed tungsten co-catalysts on organometal halide perovskite for superior interfacial charge transfer and photocatalytic hydrogen production 在有机金属卤化物钙钛矿上组装原子分散的钨共催化剂，用于优越的界面电荷转移和光催化制氢

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-19 DOI: 10.1016/j.jechem.2026.01.016

Ting Xu , Zexi Zhang , Shengliang Qi , Hefeng Zhang , Junhui Wang , Yuying Gao , Wenjun Fan , Chenghua Sun , Xu Zong , Lianzhou Wang

Intensifying the electronic metal-support interaction (EMSI) between organometal halide perovskites (OMHPs) photocatalysts and hydrogen evolution reaction (HER) co-catalyst is crucial for realizing efficient interfacial charge transfer and solar-to-hydrogen (STH) conversion. Although atomically dispersed catalysts (ADCs) are prone to form stronger EMSI than nanoparticles with support, assembling ADCs on OMHPs remains a great challenge due to the ionic nature and thermal instability of OMHPs. Herein, we realize the design of two-dimensional (2D) OMHP PMA₂PbI₄ (PMA = C₆H₅(CH₂)NH₃⁺) loaded with non-noble metal-based ADCs, namely tungsten ADCs (W_ADCs), for the first time. We show that W_ADCs coordinated with two sulfur and two oxygen atoms are anchored on the surface of PMA₂PbI₄ via a W–O–Pb link. The resulting W_ADCs-decorated PMA₂PbI₄ (W_ADCs/S-PMA₂PbI₄) exhibits an extraordinary interfacial charge transfer efficiency of 94.7%, which is much higher than that of Pt/PMA₂PbI₄ (61.7%). Moreover, W_ADCs can effectively extend the lifetime of hot carriers and work as the active sites for HER. Consequently, W_ADCs/S-PMA₂PbI₄ shows a photocatalytic HER activity superior to that of Pt/PMA₂PbI₄ and 30 times that of bare PMA₂PbI₄ with a record turnover frequency (TOF) of 516.3 h⁻¹ per W atom. This work opens a new avenue for designing cost-effective perovskite-based catalysts for solar hydrogen production.

强化有机金属卤化物钙钛矿（OMHPs）光催化剂与析氢反应（HER）助催化剂之间的电子金属-载体相互作用（EMSI）是实现高效界面电荷转移和太阳-氢（STH）转化的关键。虽然原子分散的催化剂（adc）比有载体的纳米颗粒更容易形成强EMSI，但由于omhp的离子性质和热不稳定性，在omhp上组装adc仍然是一个巨大的挑战。本文首次实现了二维（2D） OMHP PMA2PbI4 （PMA = C6H5(CH2)NH3+）负载非贵金属基adc即钨基adc （wadc）的设计。结果表明，与两个氧原子和两个硫原子配合的wadc通过W-O-Pb链固定在PMA2PbI4表面。wadc修饰后的PMA2PbI4 （wadc /S-PMA2PbI4）具有94.7%的界面电荷转移效率，远高于Pt/PMA2PbI4的61.7%。此外，wadc可以有效地延长热载流子的寿命，并作为HER的活性位点。因此，wadc /S-PMA2PbI4的光催化HER活性优于Pt/PMA2PbI4，是裸PMA2PbI4的30倍，每W原子的转换频率（TOF）达到516.3 h−1。这项工作为设计具有成本效益的钙钛矿基太阳能制氢催化剂开辟了新的途径。

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引用次数: 0

A versatile route to tailor-made catalysts via molten salt-assisted synthesis for catalytic conversion 通过熔盐辅助合成用于催化转化的定制催化剂的通用路线

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-28 DOI: 10.1016/j.jechem.2026.01.021

Shasha Gao , Jinteng Guan , Rui Zhang , Feifei Mao , Dong Guo , Chaolong Wang , Gonglei Shao

Amidst global energy transition and carbon neutrality initiatives, the development of high-performance catalysts to address energy and environmental challenges has become imperative. Molten salt-assisted synthesis (MSAS) offers a novel and robust route for catalyst preparation. It overcomes the critical drawbacks of conventional methods, such as limited mass transfer in solid-phase synthesis and constrained thermodynamics in wet-chemical processes. By harnessing high-temperature ion-mediated effects and dynamic interfacial regulation mechanisms, MSAS establishes a pragmatic paradigm for the precise synthesis of catalysts. In this review, we first outline the physicochemical properties of diverse molten salt systems, examine the molten salt system selection criteria and the theoretical mechanism basis for synthesizing catalysts via MSAS. Then recent advances in various MSAS-derived catalysts and their applications in electrochemical energy conversion are systematically reviewed. Finally, current challenges and future prospects for MSAS in catalyst design are comprehensively discussed. The systematic assessments and insights presented herein not only deepen the understanding of MSAS, but also bridge theoretical knowledge and practical design for novel, high-performance electrocatalysts.

在全球能源转型和碳中和倡议的背景下，开发高性能催化剂以应对能源和环境挑战已势在必行。熔盐辅助合成（MSAS）为催化剂的制备提供了一条新颖、可靠的途径。它克服了传统方法的关键缺陷，如固相合成中的有限传质和湿化学过程中的受限热力学。通过利用高温离子介导效应和动态界面调节机制，MSAS为精确合成催化剂建立了实用范例。本文首先概述了不同熔盐体系的物理化学性质，探讨了熔盐体系的选择标准以及通过MSAS法合成催化剂的理论机理基础。然后系统地综述了近年来各种msas衍生催化剂的研究进展及其在电化学能量转换中的应用。最后，全面讨论了MSAS在催化剂设计中面临的挑战和未来前景。本文提出的系统评估和见解不仅加深了对MSAS的理解，而且为新型高性能电催化剂的理论知识和实际设计架起了桥梁。

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引用次数: 0

Regulating solvation chemistry via co-solvent electrolyte for ultralow-temperature aqueous zinc-ion batteries 用助溶剂电解质调节超低温锌离子电池的溶剂化化学

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-17 DOI: 10.1016/j.jechem.2025.12.020

Jintao Qi , Yahan Meng , Apeng Li , Ze Xu , Xiang Li , Lei Yang , Mingming Wang , Pengfei Gao , Shaoming Huang

Aqueous zinc-ion batteries (AZIBs) hold great promise for large-scale energy storage due to their safety, low cost, and environmental compatibility. However, AZIBs face severe challenges, including cathode dissolution and anode dendrite growth, while their reliability under extreme conditions is limited by electrolyte instability. Electrolyte additives, especially organic molecule additives, provide an effective and cost-efficient strategy to address these issues. Herein, we report a novel nontoxic, green, low-cost, and water-miscible organic molecule additive used as a co-solvent, which synergistically reconstructs the solvation structure of Zn²⁺ and disrupts the strong bonding among H₂O molecules by modulating the electrostatic interactions among Zn²⁺, H₂O, and ClO₄⁻, suppressing water-induced side reactions and lowering the freezing point of the electrolyte, thereby optimizing Zn ion migration and deposition behavior. Consequently, Zn||Zn batteries exhibit excellent performance at ambient temperature (25 °C) and can still achieve over 2500 h of cycling life at a low temperature of −40 °C. It is worth noting that Zn||Zn batteries can also operate stably under the ultra-low temperature condition of −60 °C. Additionally, the co-solvent electrolyte suppresses the dissolution of vanadium-based cathodes under low-rate conditions, enabling Zn||VO₂ batteries to maintain a high capacity retention of 91 % after 600 cycles at 0.5 A g⁻¹ under ambient temperature (25 °C). Furthermore, at −40 °C, the Zn||VO₂ battery can operate for over 1000 h at a current density of 0.1 A g⁻¹. This work provides a new strategy for constructing high-performance AZIBs over a wide temperature range.

水锌离子电池（azib）由于其安全、低成本和环境兼容性，在大规模储能方面具有很大的前景。然而，azib面临着严峻的挑战，包括阴极溶解和阳极枝晶生长，而其在极端条件下的可靠性受到电解质不稳定性的限制。电解质添加剂，特别是有机分子添加剂，为解决这些问题提供了一种有效且经济的策略。本文报道了一种新型无毒、绿色、低成本、水可混溶的有机分子添加剂作为助溶剂，通过调节Zn2+、H2O和ClO4−之间的静电相互作用，抑制水诱导的副反应，降低电解质的冰点，从而协同重建Zn2+的溶剂化结构，破坏H2O分子之间的强键，从而优化Zn离子的迁移和沉积行为。因此，锌电池在环境温度（25°C）下表现出优异的性能，并且在- 40°C的低温下仍然可以实现超过2500 h的循环寿命。值得注意的是，Zn||锌电池在−60℃的超低温条件下也能稳定运行。此外，在低倍率条件下，共溶剂电解质抑制了钒基阴极的溶解，使Zn||VO2电池在环境温度（25°C）下，在0.5 a g−1下循环600次后保持91%的高容量保持率。此外，在−40°C下，Zn||VO2电池可以在0.1 a g−1的电流密度下工作超过1000小时。这项工作为在宽温度范围内构建高性能azib提供了一种新的策略。

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