Journal of Power Sources最新文献_第4页

One-dimensional flexible supercapacitors based on ZnCo2O4/MnCoP composite electrodes with enhanced electrochemical performance 基于提高电化学性能的ZnCo2O4/MnCoP复合电极的一维柔性超级电容器

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-06 DOI: 10.1016/j.jpowsour.2026.239764

Haoran Shi , Danfeng Zhang , Zihao Guo , Jianhua Yu , Jing Sui , Qian Zhang , Liyan Yu , Lifeng Dong

The increasing demand for flexible electronics in modern applications intensifies the need for adaptable, high-performance energy storage systems. Among them, one-dimensional flexible supercapacitors gain considerable attention for their structural integrity and mechanical flexibility. In this work, a ZnCo₂O₄@MnCoP (ZCO/MCP) composite is synthesized on nickel wire (NW) via a two-step hydrothermal method, while helical carbon fibers are grown on copper wire (CW) using chemical vapor deposition. The hierarchical structure of ZCO nanosheets decorated with MCP nanoparticles effectively enlarges the electroactive surface area and provides abundant redox sites. The synergistic interaction between the metal oxide and phosphide phases further enhances electrical conductivity and charge storage capability. An asymmetric flexible supercapacitor is assembled using NW@ZCO@MCP and CW@CF as the positive and negative electrodes, respectively. The device achieves volumetric and areal capacitances of 3.515 F cm⁻³ and 0.0185 F cm⁻² at 0.2 A cm⁻³, with an energy density of 2.5 mWh cm⁻³ and a power density of 320.011 mW cm⁻³. It also exhibits excellent cycling stability, retaining 85.54% of its initial capacitance after 7500 charge-discharge cycles. These results demonstrate the strong potential of the NW@ZCO@MCP//CW@CF architecture for flexible and miniaturized energy storage applications.

在现代应用中，对柔性电子器件的需求日益增长，这加强了对适应性强的高性能储能系统的需求。其中，一维柔性超级电容器因其结构完整性和机械柔韧性而备受关注。在这项工作中，通过两步水热法在镍丝（NW）上合成了ZnCo2O4@MnCoP （ZCO/MCP）复合材料，而通过化学气相沉积在铜丝（CW）上生长螺旋碳纤维。MCP纳米粒子修饰的ZCO纳米片的分层结构有效地扩大了电活性表面积，并提供了丰富的氧化还原位点。金属氧化物和磷化物相之间的协同作用进一步提高了电导率和电荷存储能力。以NW@ZCO@MCP和CW@CF分别作为正极和负极，组装了非对称柔性超级电容器。该器件在0.2 A cm - 3时的体积和面电容分别为3.515 F cm - 3和0.0185 F cm - 2，能量密度为2.5 mWh cm - 3，功率密度为320.011 mW cm - 3。它还具有优异的循环稳定性，在7500次充放电循环后保持了85.54%的初始电容。这些结果证明了NW@ZCO@MCP//CW@CF架构在灵活和小型化储能应用方面的强大潜力。

{"title":"One-dimensional flexible supercapacitors based on ZnCo2O4/MnCoP composite electrodes with enhanced electrochemical performance","authors":"Haoran Shi , Danfeng Zhang , Zihao Guo , Jianhua Yu , Jing Sui , Qian Zhang , Liyan Yu , Lifeng Dong","doi":"10.1016/j.jpowsour.2026.239764","DOIUrl":"10.1016/j.jpowsour.2026.239764","url":null,"abstract":"<div><div>The increasing demand for flexible electronics in modern applications intensifies the need for adaptable, high-performance energy storage systems. Among them, one-dimensional flexible supercapacitors gain considerable attention for their structural integrity and mechanical flexibility. In this work, a ZnCo<sub>2</sub>O<sub>4</sub>@MnCoP (ZCO/MCP) composite is synthesized on nickel wire (NW) via a two-step hydrothermal method, while helical carbon fibers are grown on copper wire (CW) using chemical vapor deposition. The hierarchical structure of ZCO nanosheets decorated with MCP nanoparticles effectively enlarges the electroactive surface area and provides abundant redox sites. The synergistic interaction between the metal oxide and phosphide phases further enhances electrical conductivity and charge storage capability. An asymmetric flexible supercapacitor is assembled using NW@ZCO@MCP and CW@CF as the positive and negative electrodes, respectively. The device achieves volumetric and areal capacitances of 3.515 F cm<sup>−3</sup> and 0.0185 F cm<sup>−2</sup> at 0.2 A cm<sup>−3</sup>, with an energy density of 2.5 mWh cm<sup>−3</sup> and a power density of 320.011 mW cm<sup>−3</sup>. It also exhibits excellent cycling stability, retaining 85.54% of its initial capacitance after 7500 charge-discharge cycles. These results demonstrate the strong potential of the NW@ZCO@MCP//CW@CF architecture for flexible and miniaturized energy storage applications.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239764"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147388084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

New fluorine-free triazine-anion-based ionic liquids as supercapacitors electrolytes 新型无氟三嗪阴离子液体作为超级电容器电解质

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-04 DOI: 10.1016/j.jpowsour.2026.239760

Mukhtiar Ahmed , Gaurav Tatrari , Sayantika Bhakta , Jyri-Pekka Mikkola , Solomon Tesfalidet

Fluorine-free supercapacitor (SCs) electrolytes are desirable to minimize environmental impact and toxicity while maintaining high electrochemical performance and long-term sustainability. Here, we introduce the new class of fluorine-free ionic liquids (ILs) engineered around the unique electron-deficient triazine-derived anion, 4,6-diethoxy-2-oxo-2H-1,3,5-triazin-5-ide (DET), coupled with n-tetrabutyl- phosphonium and ammonium cations. Both the ILs exhibit distinct and well-defined thermal behaviors, the former behaves as a glass-forming liquid, that is, have glass transition at −63 °C, while the latter exists as a supercooled liquid with complex thermal events and is ca. 90 K less thermally stable. We find relatively weaker cation–anion interactions – well supported by the FTIR data – and, thus higher ionic conductivity and higher electrochemical stability, with supporting voltage range up to 4.4 V, for (P₄₄₄₄)(DET) than in (N₄₄₄₄)(DET). (P₄₄₄₄)(DET) as SCs electrolyte delivers excellent capacitive performance within the 2.0 V window at 30 °C and 60 °C. The device achieved areal capacitance of 78 mF cm⁻² (at 0.146 mA cm⁻²) and gravimetric capacitance of 60.6 F g⁻¹ (at 0.15 A g⁻¹) at 60 °C and delivered an energy density of 34.6 Wh kg⁻¹ and the power density of 1873 W kg⁻¹ while maintaining ∼94% capacitance retention and ∼98% coulombic efficiency after 1000 cycles. SCs.

无氟超级电容器（SCs）电解质是理想的，以尽量减少对环境的影响和毒性，同时保持高电化学性能和长期可持续性。在这里，我们介绍了一类新的无氟离子液体（ILs），它围绕着独特的缺电子的三嗪衍生阴离子4,6-二氧基-2-氧- 2h -1,3,5-三嗪-5-ide (DET)，与n-四丁基-磷和铵离子偶联。两者都表现出明显而明确的热行为，前者表现为玻璃化形成液体，即在- 63℃发生玻璃化转变，而后者则表现为具有复杂热事件的过冷液体，热稳定性低约90 K。我们发现（P4444）（DET）的阳离子-阴离子相互作用相对较弱——FTIR数据很好地支持了这一点——因此，与（N4444）（DET）相比，（P4444）（DET）的离子电导率和电化学稳定性更高，支持电压范围高达4.4 V。（P4444）（DET）作为SCs电解质在30°C和60°C的2.0 V窗口内具有优异的电容性能。该器件在60℃条件下的面电容为78 mF cm−2 (0.146 mA cm−2)，重量电容为60.6 F g−1 (0.15 A g−1)，能量密度为34.6 Wh kg−1，功率密度为1873 W kg−1，在1000次循环后保持94%的电容保持率和98%的库仑效率。SCs。

{"title":"New fluorine-free triazine-anion-based ionic liquids as supercapacitors electrolytes","authors":"Mukhtiar Ahmed , Gaurav Tatrari , Sayantika Bhakta , Jyri-Pekka Mikkola , Solomon Tesfalidet","doi":"10.1016/j.jpowsour.2026.239760","DOIUrl":"10.1016/j.jpowsour.2026.239760","url":null,"abstract":"<div><div>Fluorine-free supercapacitor (SCs) electrolytes are desirable to minimize environmental impact and toxicity while maintaining high electrochemical performance and long-term sustainability. Here, we introduce the new class of fluorine-free ionic liquids (ILs) engineered around the unique electron-deficient triazine-derived anion, 4,6-diethoxy-2-oxo-2H-1,3,5-triazin-5-ide (DET), coupled with <em>n</em>-tetrabutyl- phosphonium and ammonium cations. Both the ILs exhibit distinct and well-defined thermal behaviors, the former behaves as a glass-forming liquid, that is, have glass transition at −63 °C, while the latter exists as a supercooled liquid with complex thermal events and is <em>ca.</em> 90 K less thermally stable. We find relatively weaker cation–anion interactions – well supported by the FTIR data – and, thus higher ionic conductivity and higher electrochemical stability, with supporting voltage range up to 4.4 V, for (P<sub>4444</sub>)(DET) than in (N<sub>4444</sub>)(DET). (P<sub>4444</sub>)(DET) as SCs electrolyte delivers excellent capacitive performance within the 2.0 V window at 30 °C and 60 °C. The device achieved areal capacitance of 78 mF cm<sup>−2</sup> (at 0.146 mA cm<sup>−2</sup>) and gravimetric capacitance of 60.6 F g<sup>−1</sup> (at 0.15 A g<sup>−1</sup>) at 60 °C and delivered an energy density of 34.6 Wh kg<sup>−1</sup> and the power density of 1873 W kg<sup>−1</sup> while maintaining ∼94% capacitance retention and ∼98% coulombic efficiency after 1000 cycles. SCs.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239760"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147388080","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual-interface film manipulated by single electrolyte additive containing -CF/-SO2F for cycling stability of graphite||NCM622 full cells 含-CF/-SO2F单电解质添加剂操纵双界面膜对石墨||NCM622全电池循环稳定性的影响

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-07 DOI: 10.1016/j.jpowsour.2026.239741

Haonan Huang , Lingling Huang , Shuai Chen , Youhao Liao , Weishan Li

Commercial lithium-ion batteries (LIBs) utilizing graphite anodes paired with high nickel layered oxide cathodes offer high energy density but face challenges related to electrode/electrolyte interface compatibility, limiting their large-scale applications in power and energy storage systems. This work proposes a single film-forming additive, methyl fluorosulfonyl difluoroacetate (MFSA) containing -CF and -SO₂F groups, to simultaneously construct interfacial films on the anode and cathode surfaces, which significantly addresses the prevalent issues in LIBs. Electrochemical results demonstrate that the capacity retention of graphite||LiNi_0.6Co_0.2Mn_0.2O₂ pouch cell with 1 wt% MFSA improves from 53% to 86% after 150 cycles. Quantitative calculations and spectroscopic analysis reveal that MFSA preferentially reduces on the anode surface, forming a solid electrolyte interphase (SEI) film enriched with LiF, Li₂SO₃, and fluorinated polymers, thereby enhancing the structural stability of graphite anode. Furthermore, MFSA helps remove free HF while constructing a low-impedance cathode electrolyte interphase (CEI) film rich in LiF through early oxidation, which protects the structural integrity of NCM622 cathode and suppresses continuous electrolyte decomposition, finally improving the battery electrochemical performance. This work highlights the excellent film-forming characteristics of MFSA and its protective mechanism on both electrodes, providing valuable insights into designing electrolyte additives for enhanced electrochemical characteristics in high-energy-density LIBs.

商用锂离子电池（lib）利用石墨阳极与高镍层状氧化物阴极配对提供高能量密度，但面临与电极/电解质界面兼容性相关的挑战，限制了其在电力和储能系统中的大规模应用。这项工作提出了一种单一的成膜添加剂，含-CF和-SO2F基团的氟磺酰二氟乙酸甲酯（MFSA），可以同时在阳极和阴极表面构建界面膜，这极大地解决了lib中普遍存在的问题。电化学结果表明，添加1 wt% MFSA的石墨||LiNi0.6Co0.2Mn0.2O2袋状电池在循环150次后容量保持率由53%提高到86%。定量计算和光谱分析表明，MFSA在阳极表面优先还原，形成富含LiF、Li2SO3和氟化聚合物的固体电解质界面（SEI）膜，从而增强了石墨阳极的结构稳定性。此外，MFSA通过早期氧化作用去除游离HF，形成富含LiF的低阻抗阴极电解质界面（CEI）膜，保护了NCM622阴极的结构完整性，抑制了电解质的持续分解，最终提高了电池的电化学性能。这项工作突出了MFSA优异的成膜特性及其在两个电极上的保护机制，为设计用于增强高能量密度锂离子电池电化学特性的电解质添加剂提供了有价值的见解。

{"title":"Dual-interface film manipulated by single electrolyte additive containing -CF/-SO2F for cycling stability of graphite||NCM622 full cells","authors":"Haonan Huang , Lingling Huang , Shuai Chen , Youhao Liao , Weishan Li","doi":"10.1016/j.jpowsour.2026.239741","DOIUrl":"10.1016/j.jpowsour.2026.239741","url":null,"abstract":"<div><div>Commercial lithium-ion batteries (LIBs) utilizing graphite anodes paired with high nickel layered oxide cathodes offer high energy density but face challenges related to electrode/electrolyte interface compatibility, limiting their large-scale applications in power and energy storage systems. This work proposes a single film-forming additive, methyl fluorosulfonyl difluoroacetate (MFSA) containing -CF and -SO<sub>2</sub>F groups, to simultaneously construct interfacial films on the anode and cathode surfaces, which significantly addresses the prevalent issues in LIBs. Electrochemical results demonstrate that the capacity retention of graphite||LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> pouch cell with 1 wt% MFSA improves from 53% to 86% after 150 cycles. Quantitative calculations and spectroscopic analysis reveal that MFSA preferentially reduces on the anode surface, forming a solid electrolyte interphase (SEI) film enriched with LiF, Li<sub>2</sub>SO<sub>3</sub>, and fluorinated polymers, thereby enhancing the structural stability of graphite anode. Furthermore, MFSA helps remove free HF while constructing a low-impedance cathode electrolyte interphase (CEI) film rich in LiF through early oxidation, which protects the structural integrity of NCM622 cathode and suppresses continuous electrolyte decomposition, finally improving the battery electrochemical performance. This work highlights the excellent film-forming characteristics of MFSA and its protective mechanism on both electrodes, providing valuable insights into designing electrolyte additives for enhanced electrochemical characteristics in high-energy-density LIBs.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239741"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147387638","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unraveling activity-durability trade-off in coated Fe-N-C catalysts for oxygen reduction via pyrolysis-duration-driven structural evolution 通过热解-持续时间驱动的结构演化揭示Fe-N-C涂层氧还原催化剂的活性-耐久性权衡

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-06 DOI: 10.1016/j.jpowsour.2026.239758

Li Jiao , Geunsu Bae , Nicolas Donzel , Marc Dupont , Frédéric Lecoeur , Min Wook Noh , Anastassiya Khan , Andrea Zitolo , Laetitia Dubau , Goran Dražić , Chang Hyuck Choi , Frédéric Jaouen

Fe-N-C catalysts stand out among precious-metal-free materials for the oxygen reduction reaction (ORR), yet their durability in acidic environments remains a critical challenge. The degradation pathways, particularly following high-temperature post-treatments, are not fully understood. In this study, we coated a benchmark Fe-N-C catalyst via chemical vapor deposition (CVD) using Zeolitic Imidazolate Framework-8 (ZIF-8), with dwell times ranging from 1 to 10 h at 1050 °C to tune the catalyst structure. During CVD process, a fraction of the Fe-N₄ sites was transformed into Fe nanoparticles due to the reducing environment created by volatile species derived from ZIF-8. This leads to decreased Fe-N₄ site density and turnover frequency, both contributing to decreased ORR activity. However, improved durability is observed, and can be explained in part by promoted graphitization catalyzed by Fe particles during pyrolysis. We reveal with online differential electrochemical mass spectrometry that CVD with ZIF-8 leads to strongly reduced carbon corrosion, an effect not observed when applying the same annealing treatment but without ZIF-8, supporting the deposition of a N-doped carbon coating in the former case. The study also reports the complex effect of CVD duration on activity, site density, turnover frequency and durability. Overall, these findings highlight the structural effects on ORR activity and durability of Fe-N-C catalysts, providing valuable insights for designing more robust Fe-N-C catalysts.

Fe-N-C催化剂在氧还原反应（ORR）的无贵金属材料中脱颖而出，但其在酸性环境中的耐久性仍然是一个关键挑战。降解途径，特别是高温后处理后的降解途径，尚不完全清楚。在这项研究中，我们使用咪唑酸分子筛骨架-8 （ZIF-8）通过化学气相沉积（CVD）涂覆了一个基准的Fe-N-C催化剂，在1050°C下停留时间从1到10小时，以调整催化剂的结构。在化学气相沉积过程中，由于ZIF-8衍生的挥发性物质产生的还原环境，一部分Fe- n4位点转化为Fe纳米颗粒。这导致Fe-N4位点密度和转换频率降低，两者都导致ORR活性降低。然而，观察到耐久性的提高，这可以部分解释为在热解过程中铁颗粒催化促进石墨化。我们通过在线差分电化学质谱分析发现，使用ZIF-8的CVD导致强烈的还原性碳腐蚀，当使用相同的退火处理但不使用ZIF-8时，没有观察到这种效果，这支持了前一种情况下n掺杂碳涂层的沉积。该研究还报告了CVD持续时间对活动、站点密度、周转频率和持久性的复杂影响。总的来说，这些发现突出了结构对Fe-N-C催化剂ORR活性和耐久性的影响，为设计更坚固的Fe-N-C催化剂提供了有价值的见解。

{"title":"Unraveling activity-durability trade-off in coated Fe-N-C catalysts for oxygen reduction via pyrolysis-duration-driven structural evolution","authors":"Li Jiao , Geunsu Bae , Nicolas Donzel , Marc Dupont , Frédéric Lecoeur , Min Wook Noh , Anastassiya Khan , Andrea Zitolo , Laetitia Dubau , Goran Dražić , Chang Hyuck Choi , Frédéric Jaouen","doi":"10.1016/j.jpowsour.2026.239758","DOIUrl":"10.1016/j.jpowsour.2026.239758","url":null,"abstract":"<div><div>Fe-N-C catalysts stand out among precious-metal-free materials for the oxygen reduction reaction (ORR), yet their durability in acidic environments remains a critical challenge. The degradation pathways, particularly following high-temperature post-treatments, are not fully understood. In this study, we coated a benchmark Fe-N-C catalyst via chemical vapor deposition (CVD) using Zeolitic Imidazolate Framework-8 (ZIF-8), with dwell times ranging from 1 to 10 h at 1050 °C to tune the catalyst structure. During CVD process, a fraction of the Fe-N<sub>4</sub> sites was transformed into Fe nanoparticles due to the reducing environment created by volatile species derived from ZIF-8. This leads to decreased Fe-N<sub>4</sub> site density and turnover frequency, both contributing to decreased ORR activity. However, improved durability is observed, and can be explained in part by promoted graphitization catalyzed by Fe particles during pyrolysis. We reveal with online differential electrochemical mass spectrometry that CVD with ZIF-8 leads to strongly reduced carbon corrosion, an effect not observed when applying the same annealing treatment but without ZIF-8, supporting the deposition of a N-doped carbon coating in the former case. The study also reports the complex effect of CVD duration on activity, site density, turnover frequency and durability. Overall, these findings highlight the structural effects on ORR activity and durability of Fe-N-C catalysts, providing valuable insights for designing more robust Fe-N-C catalysts.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239758"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147388127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrosynthesis of formic acid and hydrogen via efficient glycerol oxidation on a 2-methylimidazole-modified NiCo LDH 2-甲基咪唑修饰NiCo LDH上甘油氧化电合成甲酸和氢

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-04 DOI: 10.1016/j.jpowsour.2026.239769

Jiaqi Tong, Zhi Ying, Pengfei Guo, Xiaoyuan Zheng, Binlin Dou, Guomin Cui

The electrocatalytic glycerol oxidation reaction (GOR) coupled with the hydrogen evolution reaction (HER) presents an innovative strategy for the co-production of value-added chemicals and green hydrogen. However, its efficiency is often hindered by the sluggish kinetics of conventional layered metal catalysts. Herein, we report a nickel-cobalt layered double hydroxide (NiCo LDH) electrocatalyst synthesized via a 2-methylimidazole-modified strategy, which significantly enhances GOR performance. The optimized catalyst exhibits a low potential of 1.44 V vs. RHE to deliver 100 mA cm⁻² and achieves a high Faradaic efficiency of 93.7% for formic acid. When integrated into a two-electrode GOR||HER system, the catalyst enables stable operation at 300 mA cm⁻² with a hydrogen Faradaic efficiency of 96.5%. Both experimental and mechanistic studies demonstrate that 2-methylimidazole not only directs the formation of a well-defined layered architecture but also modulates the surface chemistry by increasing oxygen content and optimizing Ni–Co electronic synergy, which collectively enhance the adsorption of active oxygen intermediates and boost GOR performance. This work provides a rational ligand-mediated approach for designing high-performance layered electrocatalysts toward the efficient glycerol valorization and hydrogen production.

电催化甘油氧化反应（GOR）与析氢反应（HER）相结合，为绿色氢与高附加值化学品的协同生产提供了一种创新策略。然而，其效率往往受到传统层状金属催化剂的缓慢动力学的阻碍。本文报道了一种通过2-甲基咪唑修饰策略合成的镍钴层状双氢氧化物（NiCo LDH）电催化剂，该催化剂显著提高了GOR性能。优化后的催化剂相对于RHE具有1.44 V的低电位，输出100 mA cm−2，对甲酸的法拉第效率高达93.7%。当集成到双电极GOR||HER系统中时，催化剂可以在300 mA cm - 2下稳定运行，氢法拉第效率为96.5%。实验和机理研究均表明，2-甲基咪唑不仅指导层状结构的形成，而且通过增加氧含量和优化Ni-Co电子协同作用调节表面化学，共同增强活性氧中间体的吸附，提高GOR性能。这项工作为设计高效的层状电催化剂提供了一种合理的配体介导的方法，以实现高效的甘油增值和制氢。

{"title":"Electrosynthesis of formic acid and hydrogen via efficient glycerol oxidation on a 2-methylimidazole-modified NiCo LDH","authors":"Jiaqi Tong, Zhi Ying, Pengfei Guo, Xiaoyuan Zheng, Binlin Dou, Guomin Cui","doi":"10.1016/j.jpowsour.2026.239769","DOIUrl":"10.1016/j.jpowsour.2026.239769","url":null,"abstract":"<div><div>The electrocatalytic glycerol oxidation reaction (GOR) coupled with the hydrogen evolution reaction (HER) presents an innovative strategy for the co-production of value-added chemicals and green hydrogen. However, its efficiency is often hindered by the sluggish kinetics of conventional layered metal catalysts. Herein, we report a nickel-cobalt layered double hydroxide (NiCo LDH) electrocatalyst synthesized via a 2-methylimidazole-modified strategy, which significantly enhances GOR performance. The optimized catalyst exhibits a low potential of 1.44 V vs. RHE to deliver 100 mA cm<sup>−2</sup> and achieves a high Faradaic efficiency of 93.7% for formic acid. When integrated into a two-electrode GOR||HER system, the catalyst enables stable operation at 300 mA cm<sup>−2</sup> with a hydrogen Faradaic efficiency of 96.5%. Both experimental and mechanistic studies demonstrate that 2-methylimidazole not only directs the formation of a well-defined layered architecture but also modulates the surface chemistry by increasing oxygen content and optimizing Ni–Co electronic synergy, which collectively enhance the adsorption of active oxygen intermediates and boost GOR performance. This work provides a rational ligand-mediated approach for designing high-performance layered electrocatalysts toward the efficient glycerol valorization and hydrogen production.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239769"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147388133","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synergistic interfacial effects in NiFe layered double hydroxide-coupled ZnO/α-Fe2O3 photoanodes toward improved photoelectrochemical functionality NiFe层状双氢氧化物耦合ZnO/α-Fe2O3光阳极的协同界面效应对提高光电电化学功能的影响

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-04 DOI: 10.1016/j.jpowsour.2026.239787

Yuan-Chang Liang, Kun-Hsien Chang

In this study, we develop ternary heterojunction photoanodes with a hierarchical structure by electrodepositing a NiFe Layered Double Hydroxide (NiFe-LDH) cocatalyst onto ZnO/α-Fe₂O₃ (ZF) heterojunction materials. Surface imaging reveals that the distinct structures of ZnO nanosheets, α-Fe₂O₃ nanorods, and NiFe-LDH nanosheets are linked to improved photoelectrochemical performance. A ladder-like Type-II band alignment in the ZnO/α-Fe₂O₃/NiFe-LDH (ZFL) architecture promotes efficient separation of photogenerated electrons and holes, thereby suppressing recombination and enhancing the visible-light photoresponse, reducing recombination and enhancing visible light absorption. We also propose how changing the Ni/Fe molar ratio in NiFe-LDH affects performance, confirmed by compositional analysis. The NiFe-LDH cocatalyst speeds up surface oxidation by forming NiOOH intermediates, which increases the electrode's hydrophilicity and decreases charge transfer resistance. This research proposes a strategy that combines band structure control and surface wettability improvement to boost photoelectrochemical efficiency in ternary heterostructures.

在这项研究中，我们通过在ZnO/α-Fe2O3 （ZF）异质结材料上电沉积NiFe层状双氢氧化物（NiFe- ldh）共催化剂，开发了具有分层结构的三元异质结光阳极。表面成像显示ZnO纳米片、α-Fe2O3纳米棒和NiFe-LDH纳米片的不同结构与提高的光电化学性能有关。ZnO/α-Fe2O3/NiFe-LDH （ZFL）结构中的梯状ii型带排列促进了光生电子和空穴的有效分离，从而抑制复合并增强可见光光响应，减少复合并增强可见光吸收。我们还提出了改变Ni/Fe摩尔比对Ni - ldh性能的影响，并通过成分分析证实了这一点。NiFe-LDH助催化剂通过形成NiOOH中间体加速表面氧化，从而提高电极的亲水性，降低电荷转移阻力。本研究提出了一种结合带结构控制和表面润湿性改善的策略来提高三元异质结构的光电化学效率。

{"title":"Synergistic interfacial effects in NiFe layered double hydroxide-coupled ZnO/α-Fe2O3 photoanodes toward improved photoelectrochemical functionality","authors":"Yuan-Chang Liang, Kun-Hsien Chang","doi":"10.1016/j.jpowsour.2026.239787","DOIUrl":"10.1016/j.jpowsour.2026.239787","url":null,"abstract":"<div><div>In this study, we develop ternary heterojunction photoanodes with a hierarchical structure by electrodepositing a NiFe Layered Double Hydroxide (NiFe-LDH) cocatalyst onto ZnO/α-Fe<sub>2</sub>O<sub>3</sub> (ZF) heterojunction materials. Surface imaging reveals that the distinct structures of ZnO nanosheets, α-Fe<sub>2</sub>O<sub>3</sub> nanorods, and NiFe-LDH nanosheets are linked to improved photoelectrochemical performance. A ladder-like Type-II band alignment in the ZnO/α-Fe<sub>2</sub>O<sub>3</sub>/NiFe-LDH (ZFL) architecture promotes efficient separation of photogenerated electrons and holes, thereby suppressing recombination and enhancing the visible-light photoresponse, reducing recombination and enhancing visible light absorption. We also propose how changing the Ni/Fe molar ratio in NiFe-LDH affects performance, confirmed by compositional analysis. The NiFe-LDH cocatalyst speeds up surface oxidation by forming NiOOH intermediates, which increases the electrode's hydrophilicity and decreases charge transfer resistance. This research proposes a strategy that combines band structure control and surface wettability improvement to boost photoelectrochemical efficiency in ternary heterostructures.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239787"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147388085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Deep learning-enabled large-scale analysis of particle geometry-lithiation correlations in battery cathode materials 电池正极材料中颗粒几何与锂化相关的深度学习大规模分析

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-06 DOI: 10.1016/j.jpowsour.2026.239806

Binbin Lin , Luis J. Carrillo , Xiang-Long Peng , Wan-Xin Chen , David A. Santos , Sarbajit Banerjee , Bai-Xiang Xu

A deep learning model is employed to address the challenging problem of V

_{2}

O

_{5}

nanoparticle segmentation and the correlation between the chemical composition and the geometrical features of lithiated V

_{2}

O

_{5}

nanoparticles as an exemplar of a phase-transforming battery cathode material. First, the deep learning-enabled segmentation model is integrated with the singular value decomposition technique and a spectral database to generate accurate composition and phase maps capturing lithiation heterogeneities as imaged using scanning transmission X-ray microscopy. These phase maps act as the output properties for correlation analysis. Subsequently, the quantitative influences of the geometrical features of nanoparticles such as the particle size (i.e., projected perimeter and area), the aspect ratio, circularity, convexity, and orientation on the lithiation phase maps are revealed. These findings inform strategies to improve lithiation uniformity and reduce stress in phase-transforming lithium battery materials via optimized particle geometry.

以一种相变电池正极材料为例，采用深度学习模型解决了V2O5纳米颗粒的分割问题，以及锂化V2O5纳米颗粒的化学成分与几何特征之间的关系。首先，将基于深度学习的分割模型与奇异值分解技术和光谱数据库相结合，生成准确的成分和相位图，捕捉利用扫描透射x射线显微镜成像的岩化非均质性。这些相位图作为相关分析的输出属性。随后，揭示了纳米颗粒的几何特征，如粒径（即投影周长和面积）、纵横比、圆度、凹凸度和取向对岩化相图的定量影响。这些发现为通过优化颗粒几何形状来改善相变锂电池材料的锂化均匀性和减少应力提供了策略依据。

{"title":"Deep learning-enabled large-scale analysis of particle geometry-lithiation correlations in battery cathode materials","authors":"Binbin Lin , Luis J. Carrillo , Xiang-Long Peng , Wan-Xin Chen , David A. Santos , Sarbajit Banerjee , Bai-Xiang Xu","doi":"10.1016/j.jpowsour.2026.239806","DOIUrl":"10.1016/j.jpowsour.2026.239806","url":null,"abstract":"<div><div>A deep learning model is employed to address the challenging problem of V<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O<span><math><msub><mrow></mrow><mrow><mn>5</mn></mrow></msub></math></span> nanoparticle segmentation and the correlation between the chemical composition and the geometrical features of lithiated V<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O<span><math><msub><mrow></mrow><mrow><mn>5</mn></mrow></msub></math></span> nanoparticles as an exemplar of a phase-transforming battery cathode material. First, the deep learning-enabled segmentation model is integrated with the singular value decomposition technique and a spectral database to generate accurate composition and phase maps capturing lithiation heterogeneities as imaged using scanning transmission X-ray microscopy. These phase maps act as the output properties for correlation analysis. Subsequently, the quantitative influences of the geometrical features of nanoparticles such as the particle size (i.e., projected perimeter and area), the aspect ratio, circularity, convexity, and orientation on the lithiation phase maps are revealed. These findings inform strategies to improve lithiation uniformity and reduce stress in phase-transforming lithium battery materials via optimized particle geometry.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239806"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147387660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High potential activated multifunctional additive inducing favorable electrode-electrolyte interface for nickel-rich batteries cycling at 4.7 V 高电位活化多功能添加剂诱导富镍电池在4.7 V循环时良好的电极-电解质界面

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-07 DOI: 10.1016/j.jpowsour.2026.239803

Chaoqi Shen, Chenxi Fu, Lulu Liu, Peng Yang, Kexin Cai, Lianbang Wang

Lithium metal batteries paired with high-voltage nickel-rich cathodes offer high energy density. However, stable operation at ultra-high voltages (>4.5 V) requires suppression of severe interfacial degradation. Herein, difluoropyridine-boronic acid (DFPBA) is proposed as a multifunctional electrolyte additive to construct synergistic electrode/electrolyte interphases (EEIs). DFPBA preferentially decomposes to form a dense hybrid cathode electrolyte interface (CEI) comprising LiF, Li₃N and LiB_xO_y. Simultaneously, DFPBA optimizes the solid electrolyte interphase (SEI) on lithium metal anodes, enhancing structural integrity. The lone-pair electrons of nitrogen (N) atoms in DFPBA suppress HF formation, while boric acid derivatives reinforce EEI mechanical stability. Consequently, the rapidly formed CEI at 4.7 V enables the Li||NCM622 cells to achieve 80.4% capacity retention after 400 cycles, surpassing cells without DFPBA (45.5%). This study demonstrates the exceptional electrochemical performance achieved with NCM622 cathodes at high voltages, providing pivotal insights for developing advanced electrolytes targeting demanding energy storage systems.

锂金属电池与高电压富镍阴极配对，提供高能量密度。然而，在超高压（>4.5 V）下稳定运行需要抑制严重的界面退化。本文提出了二氟吡啶-硼酸（DFPBA）作为构建协同电极/电解质界面（eei）的多功能电解质添加剂。DFPBA优先分解形成由LiF、Li3N和LiBxOy组成的致密杂化阴极电解质界面（CEI）。同时，DFPBA优化了锂金属阳极上的固体电解质界面（SEI），提高了结构完整性。DFPBA中氮(N)原子的孤对电子抑制HF的形成，而硼酸衍生物增强EEI的机械稳定性。因此，在4.7 V下快速形成的CEI使Li||NCM622电池在400次循环后的容量保持率达到80.4%，超过了没有DFPBA的电池（45.5%）。该研究证明了NCM622阴极在高压下实现的卓越电化学性能，为开发针对苛刻储能系统的先进电解质提供了关键见解。

{"title":"High potential activated multifunctional additive inducing favorable electrode-electrolyte interface for nickel-rich batteries cycling at 4.7 V","authors":"Chaoqi Shen, Chenxi Fu, Lulu Liu, Peng Yang, Kexin Cai, Lianbang Wang","doi":"10.1016/j.jpowsour.2026.239803","DOIUrl":"10.1016/j.jpowsour.2026.239803","url":null,"abstract":"<div><div>Lithium metal batteries paired with high-voltage nickel-rich cathodes offer high energy density. However, stable operation at ultra-high voltages (>4.5 V) requires suppression of severe interfacial degradation. Herein, difluoropyridine-boronic acid (DFPBA) is proposed as a multifunctional electrolyte additive to construct synergistic electrode/electrolyte interphases (EEIs). DFPBA preferentially decomposes to form a dense hybrid cathode electrolyte interface (CEI) comprising LiF, Li<sub>3</sub>N and LiB<sub>x</sub>O<sub>y</sub>. Simultaneously, DFPBA optimizes the solid electrolyte interphase (SEI) on lithium metal anodes, enhancing structural integrity. The lone-pair electrons of nitrogen (N) atoms in DFPBA suppress HF formation, while boric acid derivatives reinforce EEI mechanical stability. Consequently, the rapidly formed CEI at 4.7 V enables the Li||NCM622 cells to achieve 80.4% capacity retention after 400 cycles, surpassing cells without DFPBA (45.5%). This study demonstrates the exceptional electrochemical performance achieved with NCM622 cathodes at high voltages, providing pivotal insights for developing advanced electrolytes targeting demanding energy storage systems.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239803"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147387662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pathways to cost-effective electrochemical CO2 reduction: Role of energy mix, intermittency, and weather conditions in formic acid production 具有成本效益的电化学CO2减排途径：能源组合、间歇性和天气条件在甲酸生产中的作用

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-04 DOI: 10.1016/j.jpowsour.2026.239776

Mohamed B. El Ghrib , Youssef Elaouzy , Jaouad Eddouibi , Houssam Bouaboula , Dawid P. Hanak , Youssef Belmabkhout , Abdelghafour Zaabout

The electrochemical reduction of CO₂ to formic acid represents a promising avenue for renewable energy storage and carbon utilization. Its feasibility depends on electricity supply configuration, intermittency, and regional energy characteristics. This study introduces an intermittency-aware, system-level framework that explicitly addresses hourly renewable variability and modular electrolyzer load-following under dynamic power conditions, in contrast to conventional techno-economic assessments that assume a steady-state electricity input. A dynamic model incorporating a three-compartment electrolyzer, downstream separations, and renewable intermittency is developed across four locations with varying weather and grid profiles. Economic and environmental performance is evaluated, including levelized cost of formic acid, net present value, return on investment, CO₂ abatement cost, and global warming intensity under conservative, moderate, and optimistic scenarios across the period 2030-2050. Wind-rich locations enable renewable-only CO₂ electrolysis, achieving levelized formic acid costs of 0.46-0.50 $/kg by 2050, below current market prices, while reaching negative CO₂ abatement costs. Hybrid PV-wind systems approach competitiveness (0.53-0.57 $/kg) without storage, whereas battery integration becomes unfavorable beyond short durations (>4 h). Grid electricity significantly degrades economic and environmental performance, especially under carbon pricing. Overall, CO₂ electrolysis viability is strongly location-dependent and governed by renewable quality, limited storage, and constrained grid use.

电化学还原CO2为甲酸代表了可再生能源储存和碳利用的一个有前途的途径。其可行性取决于电力供应配置、间歇性和区域能源特性。本研究引入了一个间歇性感知的系统级框架，该框架明确解决了动态电力条件下每小时可再生能源的可变性和模块化电解槽负载跟踪问题，与传统的技术经济评估相反，该评估假设了稳态电力输入。一个包含三室电解槽、下游分离和可再生间歇性的动态模型在四个不同天气和电网剖面的地点开发。经济和环境绩效评估，包括甲酸平准化成本、净现值、投资回报、二氧化碳减排成本和全球变暖强度在保守、中等和乐观的情景下，从2030年到2050年。风能丰富的地区可以实现纯可再生二氧化碳电解，到2050年，甲酸成本将达到0.46-0.50美元/公斤，低于目前的市场价格，同时二氧化碳减排成本为负。混合光伏-风能系统在没有存储的情况下具有竞争力（0.53-0.57美元/公斤），而电池集成在短时间内（4小时）就变得不利。电网电力显著降低了经济和环境绩效，尤其是在碳定价的情况下。总的来说，二氧化碳电解的可行性与可再生能源的质量、有限的储存和有限的电网使用密切相关。

{"title":"Pathways to cost-effective electrochemical CO2 reduction: Role of energy mix, intermittency, and weather conditions in formic acid production","authors":"Mohamed B. El Ghrib , Youssef Elaouzy , Jaouad Eddouibi , Houssam Bouaboula , Dawid P. Hanak , Youssef Belmabkhout , Abdelghafour Zaabout","doi":"10.1016/j.jpowsour.2026.239776","DOIUrl":"10.1016/j.jpowsour.2026.239776","url":null,"abstract":"<div><div>The electrochemical reduction of CO<sub>2</sub> to formic acid represents a promising avenue for renewable energy storage and carbon utilization. Its feasibility depends on electricity supply configuration, intermittency, and regional energy characteristics. This study introduces an intermittency-aware, system-level framework that explicitly addresses hourly renewable variability and modular electrolyzer load-following under dynamic power conditions, in contrast to conventional techno-economic assessments that assume a steady-state electricity input. A dynamic model incorporating a three-compartment electrolyzer, downstream separations, and renewable intermittency is developed across four locations with varying weather and grid profiles. Economic and environmental performance is evaluated, including levelized cost of formic acid, net present value, return on investment, CO<sub>2</sub> abatement cost, and global warming intensity under conservative, moderate, and optimistic scenarios across the period 2030-2050. Wind-rich locations enable renewable-only CO<sub>2</sub> electrolysis, achieving levelized formic acid costs of 0.46-0.50 $/kg by 2050, below current market prices, while reaching negative CO<sub>2</sub> abatement costs. Hybrid PV-wind systems approach competitiveness (0.53-0.57 $/kg) without storage, whereas battery integration becomes unfavorable beyond short durations (>4 h). Grid electricity significantly degrades economic and environmental performance, especially under carbon pricing. Overall, CO<sub>2</sub> electrolysis viability is strongly location-dependent and governed by renewable quality, limited storage, and constrained grid use.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239776"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147387663","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Defect-engineered exfoliated MoS2/rGO hybrids for dual-function oxygen electrocatalysis and high-capacity Li-O2 batteries 用于双功能氧电催化和高容量Li-O2电池的缺陷工程剥离MoS2/rGO混合材料

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-05-15 Epub Date: 2026-03-07 DOI: 10.1016/j.jpowsour.2026.239800

Sekar Sandhiya , Rajendran Saravanan , Perumal Elumalai

Pristine bulk MoS₂ (BMS) and the bulk MoS₂@reduced graphene oxide (BMR) composites are synthesized via a single-step hydrothermal method, while exfoliated MoS₂ (EMS) nanosheets and their respective composites (EMR) with the reduced graphene oxide (rGO) are prepared using a simple sonication-assisted route. The synthesized catalysts are systematically characterized to elucidate their phase composition, defect chemistry and morphology, and were evaluated as bifunctional oxygen electrocatalysts using rotating ring-disk electrode (RRDE) analysis. Among all the catalysts, the exfoliated MoS₂ containing 80 wt% rGO (EMR80) catalyst achieves a positive ORR onset potential of 0.90 V, a high limiting current density of 6.85 mA cm⁻², very low OER overpotential of 290 mV, and a low bifunctionality index of 0.21 V. The improved electrocatalytic performance arises from the 1T phase of exfoliated MoS₂, which possesses defect-rich features, such as few MoS₂ layers having reduced crystallite size and increased lattice disorder. When applied as the air cathode in a coin-type Li-O₂ battery (LOB), the EMR80 catalyst delivers an impressive discharge capacity of 17000 mA h g⁻¹ at a current density of 100 mA g⁻¹ with a low charge overpotential of 1 V.

通过单步水热法合成了原始块体MoS2 （BMS）和块体MoS2@reduced氧化石墨烯（BMR）复合材料，而通过简单的超声辅助方法制备了剥离的MoS2 （EMS）纳米片及其与还原氧化石墨烯（rGO）的复合材料（EMR）。对合成的催化剂进行了相组成、缺陷化学和形貌表征，并采用旋转环盘电极（RRDE）对其进行了表征。在所有催化剂中，含有80 wt% rGO （EMR80）的剥离二硫化钼催化剂具有0.90 V的正ORR起始电位，6.85 mA cm−2的高极限电流密度，极低的OER过电位为290 mV，低双功能指数为0.21 V。剥离后的MoS2的1T相具有缺陷丰富的特征，如较少的MoS2层，晶粒尺寸减小，晶格无序性增加。当用作硬币型锂氧电池（LOB）的空气阴极时，EMR80催化剂在100 mA g - 1的电流密度下提供了令人印象深刻的17000 mA h g - 1的放电容量，充电过电位低至1 V。

{"title":"Defect-engineered exfoliated MoS2/rGO hybrids for dual-function oxygen electrocatalysis and high-capacity Li-O2 batteries","authors":"Sekar Sandhiya , Rajendran Saravanan , Perumal Elumalai","doi":"10.1016/j.jpowsour.2026.239800","DOIUrl":"10.1016/j.jpowsour.2026.239800","url":null,"abstract":"<div><div>Pristine bulk MoS<sub>2</sub> (BMS) and the bulk MoS<sub>2</sub>@reduced graphene oxide (BMR) composites are synthesized via a single-step hydrothermal method, while exfoliated MoS<sub>2</sub> (EMS) nanosheets and their respective composites (EMR) with the reduced graphene oxide (rGO) are prepared using a simple sonication-assisted route. The synthesized catalysts are systematically characterized to elucidate their phase composition, defect chemistry and morphology, and were evaluated as bifunctional oxygen electrocatalysts using rotating ring-disk electrode (RRDE) analysis. Among all the catalysts, the exfoliated MoS<sub>2</sub> containing 80 wt% rGO (EMR80) catalyst achieves a positive ORR onset potential of 0.90 V, a high limiting current density of 6.85 mA cm<sup>−2</sup>, very low OER overpotential of 290 mV, and a low bifunctionality index of 0.21 V. The improved electrocatalytic performance arises from the 1T phase of exfoliated MoS<sub>2</sub>, which possesses defect-rich features, such as few MoS<sub>2</sub> layers having reduced crystallite size and increased lattice disorder. When applied as the air cathode in a coin-type Li-O<sub>2</sub> battery (LOB), the EMR80 catalyst delivers an impressive discharge capacity of 17000 mA h g<sup>−1</sup> at a current density of 100 mA g<sup>−1</sup> with a low charge overpotential of 1 V.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"674 ","pages":"Article 239800"},"PeriodicalIF":7.9,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147387746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0