Pub Date : 2026-01-18DOI: 10.1016/j.nanoen.2026.111736
Yi Tang , Shoumeng Yang , Congcong Liu , Yu Yao , Zhijun Wu , Wubin Du , Hongge Pan , Yang Yang , Xianhong Rui , Yan Yu
All-solid-state Na-S batteries (ASSNSBs) are promising candidates for grid-scale energy storage owing to their high energy density and intrinsic safety. However, the practical utilization of Na3SbS4 (NSS) as a solid electrolyte is hindered by its limited intrinsic Na+ transport capability. Drawing on insights from first-principles analysis of aliovalent doping and vacancy formation, we design and synthesize Ca-doped NSS electrolytes with enhanced ionic conductivity and improved compatibility with Na3Sn alloy anodes. The optimized Na2.9Ca0.05SbS4 (NCSS-0.05) achieves a room-temperature ionic conductivity of 0.51 mS cm−1 and a reduced activation energy of 0.237 eV, alongside highly stable symmetric cell cycling for over 400 h. When incorporated into ASSNSBs, NCSS-0.05 enables an initial discharge capacity of 1601 mAh g−1 at 0.17 A g−1 and maintains 97.2 % capacity retention over 250 cycles at 0.5 A g−1. Moreover, the Ca-modified electrolyte exhibits strong compatibility with various sulfide-based cathodes, including TiS2 and VS2, further demonstrating its broad applicability. These results establish a robust aliovalent-doping strategy for engineering fast-ion-conducting sulfide solid electrolytes and advancing high-performance all-solid-state sodium battery technologies.
全固态Na-S电池（assnsb）因其高能量密度和固有安全性而成为电网规模储能的有希望的候选者。然而，Na3SbS4 （NSS）作为固体电解质的实际应用受到其有限的固有Na+传输能力的阻碍。根据对共价掺杂和空位形成的第一性原理分析，我们设计并合成了具有增强离子电导率和改善与Na3Sn合金阳极相容性的ca掺杂NSS电解质。优化后的Na2.9Ca0.05SbS4 （NCSS-0.05）室温离子电导率为0.51 mS cm−1，活化能降低为0.237 eV，并具有高度稳定的对称循环400 h以上。当纳入assnsb时，NCSS-0.05使初始放电容量为1601 mAh g−1，在0.17 A g−1下，并在0.5 A g−1下保持97.2 %的容量保持超过250次循环。此外，ca修饰的电解质与多种硫化物基阴极（包括TiS2和VS2）具有较强的相容性，进一步证明了其广泛的适用性。这些结果为快速离子导电硫化物固体电解质的工程设计和高性能全固态钠电池技术的发展奠定了坚实的共价掺杂策略。
{"title":"Engineering calcium-doped Na3SbS4 with enhanced ion transport and interfacial compatibility for all-solid-state sodium-sulfur batteries","authors":"Yi Tang , Shoumeng Yang , Congcong Liu , Yu Yao , Zhijun Wu , Wubin Du , Hongge Pan , Yang Yang , Xianhong Rui , Yan Yu","doi":"10.1016/j.nanoen.2026.111736","DOIUrl":"10.1016/j.nanoen.2026.111736","url":null,"abstract":"<div><div>All-solid-state Na-S batteries (ASSNSBs) are promising candidates for grid-scale energy storage owing to their high energy density and intrinsic safety. However, the practical utilization of Na<sub>3</sub>SbS<sub>4</sub> (NSS) as a solid electrolyte is hindered by its limited intrinsic Na<sup>+</sup> transport capability. Drawing on insights from first-principles analysis of aliovalent doping and vacancy formation, we design and synthesize Ca-doped NSS electrolytes with enhanced ionic conductivity and improved compatibility with Na<sub>3</sub>Sn alloy anodes. The optimized Na<sub>2.9</sub>Ca<sub>0.05</sub>SbS<sub>4</sub> (NCSS-0.05) achieves a room-temperature ionic conductivity of 0.51 mS cm<sup>−1</sup> and a reduced activation energy of 0.237 eV, alongside highly stable symmetric cell cycling for over 400 h. When incorporated into ASSNSBs, NCSS-0.05 enables an initial discharge capacity of 1601 mAh g<sup>−1</sup> at 0.17 A g<sup>−1</sup> and maintains 97.2 % capacity retention over 250 cycles at 0.5 A g<sup>−1</sup>. Moreover, the Ca-modified electrolyte exhibits strong compatibility with various sulfide-based cathodes, including TiS<sub>2</sub> and VS<sub>2</sub>, further demonstrating its broad applicability. These results establish a robust aliovalent-doping strategy for engineering fast-ion-conducting sulfide solid electrolytes and advancing high-performance all-solid-state sodium battery technologies.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111736"},"PeriodicalIF":17.1,"publicationDate":"2026-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-16DOI: 10.1016/j.nanoen.2026.111735
Kun Han , Jianxing Yang , Chenglong Wang , Junfeng Li , Zhijing Zhu , Wenjie Mai , Jinliang Li , Guang Yang , Likun Pan
Understanding and predicting the electrochemical behavior of high-nickel cathode materials remains a central challenge in developing advanced lithium-ion energy storage systems. Although recent machine learning methods have achieved remarkable predictive performance, their generic architectures seldom embody the underlying physical and chemical mechanisms governing electrochemical processes, which limits both interpretability and generalization. We present MEMFNet, a deep learning framework specifically designed to reflect materials science knowledge through a dual-pathway architecture that mirrors the distinction between static material properties and dynamic electrochemical processes. Trained on 158,200 voltage-capacity data points from 791 discharge profiles of high-nickel cathode materials, MEMFNet reduces prediction error by 48.64 % compared to state-of-the-art methods. More importantly, the knowledge-guided architecture transforms the model from a black box into an interpretable system whose learned representations align with established electrochemical principles. By integrating domain knowledge, MEMFNet enables interpretable and scientifically meaningful learning in materials informatics.
{"title":"MEMFNet: Toward a knowledge-guided paradigm for interpretable electrochemical performance prediction","authors":"Kun Han , Jianxing Yang , Chenglong Wang , Junfeng Li , Zhijing Zhu , Wenjie Mai , Jinliang Li , Guang Yang , Likun Pan","doi":"10.1016/j.nanoen.2026.111735","DOIUrl":"10.1016/j.nanoen.2026.111735","url":null,"abstract":"<div><div>Understanding and predicting the electrochemical behavior of high-nickel cathode materials remains a central challenge in developing advanced lithium-ion energy storage systems. Although recent machine learning methods have achieved remarkable predictive performance, their generic architectures seldom embody the underlying physical and chemical mechanisms governing electrochemical processes, which limits both interpretability and generalization. We present MEMFNet, a deep learning framework specifically designed to reflect materials science knowledge through a dual-pathway architecture that mirrors the distinction between static material properties and dynamic electrochemical processes. Trained on 158,200 voltage-capacity data points from 791 discharge profiles of high-nickel cathode materials, MEMFNet reduces prediction error by 48.64 % compared to state-of-the-art methods. More importantly, the knowledge-guided architecture transforms the model from a black box into an interpretable system whose learned representations align with established electrochemical principles. By integrating domain knowledge, MEMFNet enables interpretable and scientifically meaningful learning in materials informatics.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111735"},"PeriodicalIF":17.1,"publicationDate":"2026-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-16DOI: 10.1016/j.nanoen.2026.111714
Sangmi Park , Hye Seung Kim , Seongwook Chae , Ye In Kim , Min Ah Park , Jinkyu Yang , Heunjeong Lee , Shinuk Cho , Seung Geol Lee , Myoung Hoon Song
One-dimensional (1D) perovskite capping layers present a promising pathway to improve the efficiency and stability of perovskite solar cells (PeSCs), though their integration into inverted architectures remains limited. In this study, we reveal how the dissociation behavior of ionic liquids (ILs) governs the morphology, surface termination, and optoelectronic characteristics of 1D perovskite (EMIMPbI3) layers. Highly dissociative 1-ethyl-3-methylimidazolium (EMIM⁺)-based ILs enable the controlled growth of rod-shaped 1D EMIMPbI3 with preferred (200) facet orientation. Density functional theory calculations identify the (200) facet as a high electron-density surface that provides superior charge transport and interfacial contact compared to the (102) facet. However, excessive IL dissociation leads to an undesired 3D-to-1D phase transition, reducing device stability. To overcome this limitation, we employ a low-dissociation IL in combination with a strongly PbI2-coordinating solvent, which modulates PbI2 sites and allows low-dissociation ILs to replicate the benefits of highly dissociative ones. This approach enables the formation of rod-shaped 1D perovskites with dominant (200) facets while preserving long-term stability. Consequently, the optimized 1D/3D heterojunction PeSC achieves a power conversion efficiency of 25.40 % and exhibits excellent device stability under ISOS-D1 and ISOS-L testing. These results present a viable strategy for employing 1D perovskites as functional interfacial layers in stable, high-efficiency photovoltaic devices.
{"title":"Faceted growth of 1D perovskite layers via ionic liquid control for efficient and stable inverted perovskite solar cells","authors":"Sangmi Park , Hye Seung Kim , Seongwook Chae , Ye In Kim , Min Ah Park , Jinkyu Yang , Heunjeong Lee , Shinuk Cho , Seung Geol Lee , Myoung Hoon Song","doi":"10.1016/j.nanoen.2026.111714","DOIUrl":"10.1016/j.nanoen.2026.111714","url":null,"abstract":"<div><div>One-dimensional (1D) perovskite capping layers present a promising pathway to improve the efficiency and stability of perovskite solar cells (PeSCs), though their integration into inverted architectures remains limited. In this study, we reveal how the dissociation behavior of ionic liquids (ILs) governs the morphology, surface termination, and optoelectronic characteristics of 1D perovskite (EMIMPbI<sub>3</sub>) layers. Highly dissociative 1-ethyl-3-methylimidazolium (EMIM⁺)-based ILs enable the controlled growth of rod-shaped 1D EMIMPbI<sub>3</sub> with preferred (200) facet orientation. Density functional theory calculations identify the (200) facet as a high electron-density surface that provides superior charge transport and interfacial contact compared to the (102) facet. However, excessive IL dissociation leads to an undesired 3D-to-1D phase transition, reducing device stability. To overcome this limitation, we employ a low-dissociation IL in combination with a strongly PbI<sub>2</sub>-coordinating solvent, which modulates PbI<sub>2</sub> sites and allows low-dissociation ILs to replicate the benefits of highly dissociative ones. This approach enables the formation of rod-shaped 1D perovskites with dominant (200) facets while preserving long-term stability. Consequently, the optimized 1D/3D heterojunction PeSC achieves a power conversion efficiency of 25.40 % and exhibits excellent device stability under ISOS-D1 and ISOS-L testing. These results present a viable strategy for employing 1D perovskites as functional interfacial layers in stable, high-efficiency photovoltaic devices.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111714"},"PeriodicalIF":17.1,"publicationDate":"2026-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precise control over battery interphase formation is critical yet challenging, since its compositional and spatial characteristics dictate cyclability and fast-charging performance. Compared to the anode interphase, revealing and engineering the cathode–electrolyte interphase (CEI), which is rooted in the electrode surface chemistry, has received less attention. Herein, we employ biomass-derived porous carbon as the platform with tailorable oxygen-containing functional groups to control the CEI formation on the carbon-sulfur cathode. The results demonstrate that oxygen functional groups suppress the excessive localized growth of inorganic phases and promote the formation of a dense and uniform inorganic–organic hybrid CEI. This microstructurally engineered interphase not only effectively inhibits the polysulfide dissolution but also markedly enhances Na+ transport. By adopting the oxygen-rich surface engineering strategy, the room-temperature sodium–sulfur batteries deliver outstanding cycling stability with a capacity of 694.2 mAh g−1 after 500 cycles and exhibit excellent rate performance. This study establishes a clear correlation between surface chemistry and CEI microstructure and provides fundamental guidance for the rational design of advanced electrodes for metal–sulfur batteries.
由于其成分和空间特性决定了电池的可循环性和快速充电性能，因此对电池间相形成的精确控制至关重要，但也具有挑战性。与阳极界面相相比，扎根于电极表面化学的阴极-电解质界面的揭示和工程化受到的关注较少。在此，我们采用生物质衍生的多孔碳作为平台，具有定制的含氧官能团来控制碳硫阴极上CEI的形成。结果表明，氧官能团抑制了无机相的过度局域生长，促进了致密均匀的无机-有机杂化CEI的形成。这种微结构工程间相不仅有效地抑制了多硫化物的溶解，而且显著地增强了Na+的转运。通过采用富氧表面工程策略，室温钠硫电池具有出色的循环稳定性，循环500次后容量为694.2 mAh g−1，并具有优异的倍率性能。该研究建立了表面化学与CEI微观结构之间的明确相关性，为金属硫电池先进电极的合理设计提供了基础指导。
{"title":"Unraveling the role of oxygen functional groups in inducing the spatial distribution of the cathode–electrolyte interphase in room-temperature sodium–sulfur batteries","authors":"Kai Zhang, Feng Gong, Zongqi Chen, Shaohuan Hong, Tengfei Zheng, Shenglin Liu, Rui Xiao","doi":"10.1016/j.nanoen.2026.111730","DOIUrl":"10.1016/j.nanoen.2026.111730","url":null,"abstract":"<div><div>Precise control over battery interphase formation is critical yet challenging, since its compositional and spatial characteristics dictate cyclability and fast-charging performance. Compared to the anode interphase, revealing and engineering the cathode–electrolyte interphase (CEI), which is rooted in the electrode surface chemistry, has received less attention. Herein, we employ biomass-derived porous carbon as the platform with tailorable oxygen-containing functional groups to control the CEI formation on the carbon-sulfur cathode. The results demonstrate that oxygen functional groups suppress the excessive localized growth of inorganic phases and promote the formation of a dense and uniform inorganic–organic hybrid CEI. This microstructurally engineered interphase not only effectively inhibits the polysulfide dissolution but also markedly enhances Na<sup>+</sup> transport. By adopting the oxygen-rich surface engineering strategy, the room-temperature sodium–sulfur batteries deliver outstanding cycling stability with a capacity of 694.2 mAh g<sup>−1</sup> after 500 cycles and exhibit excellent rate performance. This study establishes a clear correlation between surface chemistry and CEI microstructure and provides fundamental guidance for the rational design of advanced electrodes for metal–sulfur batteries.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111730"},"PeriodicalIF":17.1,"publicationDate":"2026-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-15DOI: 10.1016/j.nanoen.2026.111729
Mustehsan Beg , Vishnu Sam , Jithin Kanathedath, Prasutha Rani Markapudi, Keith M. Alcock, Keng Goh, Hongnian Yu, Libu Manjakkal
Optimising ultra-low voltage with high capacity in batteries presents a challenge for emerging applications, such as wearable technology. In this study, we developed a multifunctional ultra-low voltage, sweat-activated fabric battery (SFB) using a biomaterial-based piezo-ionic hydrogel from water hyacinth carboxymethyl cellulose, mitigating risks of high-power and toxic materials near human skin. The SFB's multi-layer active material enhances conductivity and reduces resistance, enabling a 1 cm² device to discharge for 10 + h below 0.4 V, with an areal capacity of 4.1 mAh cm⁻² at 400 μA cm⁻². Furthermore, SFB with piezo-ionic hydrogel, when affixed to the elbow, generates a peak current of 115 nA cm⁻² as the elbow is fully flexed. Consequently, SFB can be utilised for energy storage, along with force and bending sensing. This study opens new avenues in advancing research on ultra-low voltage batteries for wearable and biomedical devices.
在可穿戴技术等新兴应用中，优化超低电压高容量电池是一个挑战。在这项研究中，我们开发了一种多功能超低电压，汗活化织物电池（SFB），使用水信子羧甲基纤维素的生物材料为基础的压电离子水凝胶，降低了人体皮肤附近高功率和有毒物质的风险。SFB的多层活性材料提高了电导率，降低了电阻，使1 平方厘米的器件在0.4 V以下放电10 + h，在400 μA cm⁻²时的面容量为4.1 mAh cm⁻²。此外，带有压电离子水凝胶的SFB，当贴在肘部时，当肘部完全弯曲时，会产生115 nA cm⁻²的峰值电流。因此，SFB可以用于能量存储，以及力和弯曲传感。这项研究为推进可穿戴和生物医学设备的超低电压电池的研究开辟了新的途径。
{"title":"Multifunctional ultra-low voltage sweat-activated battery using piezo-ionic hydrogel","authors":"Mustehsan Beg , Vishnu Sam , Jithin Kanathedath, Prasutha Rani Markapudi, Keith M. Alcock, Keng Goh, Hongnian Yu, Libu Manjakkal","doi":"10.1016/j.nanoen.2026.111729","DOIUrl":"10.1016/j.nanoen.2026.111729","url":null,"abstract":"<div><div>Optimising ultra-low voltage with high capacity in batteries presents a challenge for emerging applications, such as wearable technology. In this study, we developed a multifunctional ultra-low voltage, sweat-activated fabric battery (SFB) using a biomaterial-based piezo-ionic hydrogel from water hyacinth carboxymethyl cellulose, mitigating risks of high-power and toxic materials near human skin. The SFB's multi-layer active material enhances conductivity and reduces resistance, enabling a 1 cm² device to discharge for 10 + h below 0.4 V, with an areal capacity of 4.1 mAh cm⁻² at 400 μA cm⁻². Furthermore, SFB with piezo-ionic hydrogel, when affixed to the elbow, generates a peak current of 115 nA cm⁻² as the elbow is fully flexed. Consequently, SFB can be utilised for energy storage, along with force and bending sensing. This study opens new avenues in advancing research on ultra-low voltage batteries for wearable and biomedical devices.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111729"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-15DOI: 10.1016/j.nanoen.2026.111717
Zinan Wang , Zhengping Sun , Peng Wang , Xiaoyu Yang , Tianxu Ji , Shuchang Wei , Yangfan Niu , Wei Duan , Ying Yue , Yunpeng Liu , Yang Ju
Aqueous zinc-ion batteries (AZBs) hold great promise for sustainable energy storage; however, their performance remains constrained by the interfacial instability of the Zn anode, which leads to parasitic hydrogen evolution, dendritic deposition, and surface corrosion. Inspired by the selective uptake of polar molecules by plant root hairs, this study proposes a bioinspired strategy involving the in situ growth of a hydrophobic–ethanolophilic ZIF-71 interlayer coupled with an ethylene glycol (EG) additive. The hydrophobic Cl groups in ZIF-71 repel water molecules to suppress side reactions, while its porous structure selectively adsorbs EG to form a "Zn2 + –EG–ZIF-71" coordination bridge that promotes desolvation and directed ion migration. Theoretical calculations reveal that the negatively charged regions associated with the Cl groups in ZIF-71 pores exhibit a stronger adsorption affinity for EG, promoting preferential molecular enrichment. Molecular dynamics simulations further confirm that EG molecules enter the Zn2+ solvation sheath, reconstructing [Zn(H2O)6]2+ into [Zn(H2O)5(EG)]2+, thereby accelerating desolvation and facilitating uniform Zn deposition. This synergistic mechanism enables the ZIF-71@Zn(+EG) symmetric coin cell to operate stably for over 5000 h at 2 mA cm−2, and a pouch cell to function for 4000 h at 3 mA cm−2 without noticeable swelling. Moreover, the ZIF-71@Zn(+EG)//AlVO-NMP full cell achieved a capacity retention of 73.8 % after 4000 cycles at 5 A g−1. This work provides valuable insights and a feasible solution for constructing highly stable AZBs through the cooperative regulation of interfacial chemistry and solvation structure.
水锌离子电池（AZBs）在可持续能源存储方面前景广阔；然而，它们的性能仍然受到Zn阳极界面不稳定性的限制，这导致了寄生析氢、枝晶沉积和表面腐蚀。受植物根毛选择性摄取极性分子的启发，本研究提出了一种生物启发策略，涉及疏水-亲乙醇ZIF-71中间层与乙二醇（EG）添加剂耦合的原位生长。ZIF-71中疏水Cl基团排斥水分子抑制副反应，而其多孔结构选择性吸附EG，形成“Zn2 + -EG-ZIF-71”配位桥，促进脱溶和离子定向迁移。理论计算表明，ZIF-71孔隙中与Cl基团相关的负电荷区对EG具有更强的吸附亲和力，促进了分子的优先富集。分子动力学模拟进一步证实了EG分子进入Zn2+溶剂化鞘层，将[Zn(H2O)6]2+重构为[Zn(H2O)5(EG)]2+，从而加速了脱溶，促进了锌的均匀沉积。这种协同机制使ZIF-71@Zn（+EG）对称硬币电池在2 mA cm−2下稳定运行超过5000 h，而袋状电池在3 mA cm−2下稳定运行4000 h，而不会出现明显的肿胀。此外，ZIF-71@Zn(+EG)//AlVO-NMP全电池在5 a g−1下循环4000次后，容量保持率达到73.8 %。这项工作为通过界面化学和溶剂化结构的协同调节构建高稳定的azb提供了有价值的见解和可行的解决方案。
{"title":"Synergistic integration of in situ Grown ZIF-71 and organic additives toward a stable cooperative interface in advanced aqueous zinc-ion batteries","authors":"Zinan Wang , Zhengping Sun , Peng Wang , Xiaoyu Yang , Tianxu Ji , Shuchang Wei , Yangfan Niu , Wei Duan , Ying Yue , Yunpeng Liu , Yang Ju","doi":"10.1016/j.nanoen.2026.111717","DOIUrl":"10.1016/j.nanoen.2026.111717","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZBs) hold great promise for sustainable energy storage; however, their performance remains constrained by the interfacial instability of the Zn anode, which leads to parasitic hydrogen evolution, dendritic deposition, and surface corrosion. Inspired by the selective uptake of polar molecules by plant root hairs, this study proposes a bioinspired strategy involving the in situ growth of a hydrophobic–ethanolophilic ZIF-71 interlayer coupled with an ethylene glycol (EG) additive. The hydrophobic Cl groups in ZIF-71 repel water molecules to suppress side reactions, while its porous structure selectively adsorbs EG to form a \"Zn<sup>2 +</sup> –EG–ZIF-71\" coordination bridge that promotes desolvation and directed ion migration. Theoretical calculations reveal that the negatively charged regions associated with the Cl groups in ZIF-71 pores exhibit a stronger adsorption affinity for EG, promoting preferential molecular enrichment. Molecular dynamics simulations further confirm that EG molecules enter the Zn<sup>2+</sup> solvation sheath, reconstructing [Zn(H<sub>2</sub>O)<sub>6</sub>]<sup>2+</sup> into [Zn(H<sub>2</sub>O)<sub>5</sub>(EG)]<sup>2+</sup>, thereby accelerating desolvation and facilitating uniform Zn deposition. This synergistic mechanism enables the ZIF-71@Zn(+EG) symmetric coin cell to operate stably for over 5000 h at 2 mA cm<sup>−2</sup>, and a pouch cell to function for 4000 h at 3 mA cm<sup>−2</sup> without noticeable swelling. Moreover, the ZIF-71@Zn(+EG)//AlVO-NMP full cell achieved a capacity retention of 73.8 % after 4000 cycles at 5 A g<sup>−1</sup>. This work provides valuable insights and a feasible solution for constructing highly stable AZBs through the cooperative regulation of interfacial chemistry and solvation structure.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111717"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-15DOI: 10.1016/j.nanoen.2026.111728
Huilin Zhao , Xiaojun Wang , Fengyuan Tian , Weiping Xiao , Junwu Liang , Wenli Yu , Tianyi Ma , Lei Wang , Zexing Wu
Engineering bifunctional electrocatalysts featuring promoted adsorption for multiple intermediates and reactants via interface modulation strategies is critical for urea-assisted water splitting toward sustainable energy conversion. However, exploring efficient bifunctional electrocatalysts capable of driving both the hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) at high current densities remains challenging. Herein, a self-supported bifunctional electrode is constructed on nickel foam, where the cooperative CoNi LDH is decorated with low-content Pt nanospheres (Pt-CoNi LDH/NF) for urea-assisted H2 production. The strong metal-support interaction (SMSI) and multi-metal synergy collectively regulate the adsorption/desorption behavior of key reaction species, thereby lowering the energy barrier for the rate-determining step and improving overall catalytic efficiency. The optimized catalyst exhibits substantially reduced potentials of 1.32 V (UOR) and −30 mV (HER) to reach 10 mA cm−2. A urea-assisted electrolytic cell merely requires 1.36 V to afford 10 mA cm−2. Notably, in a practical anion-exchange membrane (AEM) electrolyzer configuration, the Pt-CoNi LDH/NF electrode maintains stable at 2 A cm−2, while preserving high UOR/HER bifunctional activity. This study develops an integrated approach that couples urea-containing wastewater remediation with energy-efficient hydrogen production.
通过界面调节策略促进多种中间体和反应物吸附的工程双功能电催化剂是实现尿素助水分解可持续能量转化的关键。然而，探索能够在高电流密度下同时驱动析氢反应（HER）和尿素氧化反应（UOR）的高效双功能电催化剂仍然具有挑战性。本文在泡沫镍上构建了一种自支撑双功能电极，其中协同的CoNi LDH表面装饰有低含量的Pt纳米球（Pt-CoNi LDH/NF），用于尿素辅助制氢。强金属-载体相互作用（SMSI）和多金属协同作用共同调节了关键反应物质的吸附/解吸行为，从而降低了决定速率步骤的能垒，提高了整体催化效率。优化后的催化剂电势大幅降低，分别为1.32 V （UOR）和- 30 mV (HER)，达到10 mA cm−2。一个尿素辅助的电解电池只需要1.36 V来提供10 mA cm−2。值得注意的是，在实际的阴离子交换膜（AEM）电解槽配置中，Pt-CoNi LDH/NF电极在2 a cm−2下保持稳定，同时保持高UOR/HER双功能活性。本研究开发了一种将含尿素废水修复与节能制氢相结合的综合方法。
{"title":"Interface cooperative Pt-CoNi LDH for urea-assisted energy-saving hydrogen production under ampere-level current density","authors":"Huilin Zhao , Xiaojun Wang , Fengyuan Tian , Weiping Xiao , Junwu Liang , Wenli Yu , Tianyi Ma , Lei Wang , Zexing Wu","doi":"10.1016/j.nanoen.2026.111728","DOIUrl":"10.1016/j.nanoen.2026.111728","url":null,"abstract":"<div><div>Engineering bifunctional electrocatalysts featuring promoted adsorption for multiple intermediates and reactants via interface modulation strategies is critical for urea-assisted water splitting toward sustainable energy conversion. However, exploring efficient bifunctional electrocatalysts capable of driving both the hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) at high current densities remains challenging. Herein, a self-supported bifunctional electrode is constructed on nickel foam, where the cooperative CoNi LDH is decorated with low-content Pt nanospheres (Pt-CoNi LDH/NF) for urea-assisted H<sub>2</sub> production. The strong metal-support interaction (SMSI) and multi-metal synergy collectively regulate the adsorption/desorption behavior of key reaction species, thereby lowering the energy barrier for the rate-determining step and improving overall catalytic efficiency. The optimized catalyst exhibits substantially reduced potentials of 1.32 V (UOR) and −30 mV (HER) to reach 10 mA cm<sup>−2</sup>. A urea-assisted electrolytic cell merely requires 1.36 V to afford 10 mA cm<sup>−2</sup>. Notably, in a practical anion-exchange membrane (AEM) electrolyzer configuration, the Pt-CoNi LDH/NF electrode maintains stable at 2 A cm<sup>−2</sup>, while preserving high UOR/HER bifunctional activity. This study develops an integrated approach that couples urea-containing wastewater remediation with energy-efficient hydrogen production.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111728"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995969","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-15DOI: 10.1016/j.nanoen.2026.111733
Zhihao Lou , Pengfei Wu , Yuanshuo Ma , Da Xue , Pengfei Wang , Fangyi Ma , Xuejing Cui , Guangbo Liu , Xin Zhou , Erdong Wang , Wenzhen Li , Luhua Jiang
Single atom catalysts (SACs) have attracted great attention due to their unique atomic structure and exceptional catalytic activity. Nevertheless, persistent challenges in fabricating high-density SACs on specific oxide supports have hindered their broad application. Herein, we report a facile microwave-assisted hydrothermal synthesis method to fabricate osmium-SACs on a defect-rich tungsten oxide support (Os-SAC@WO3) with an unprecedented loading up to 31.7 wt% (12.4 at%). Impressively, the as-obtained Os-SAC@WO3 exhibits excellent hydrogen evolution reaction (HER) activity with overpotentials of only 24/23 mV at 10 mA cm−2 in alkaline freshwater/seawater media, surpassing commercial Pt/C (39/34 mV). Moreover, an anion-exchange membrane water electrolyzer (AEMWE) with Os-SAC@WO3 as the cathode achieves remarkable long-term stability in alkaline seawater, enabling stable operation at 100 mA cm−2 for more than 1000 h with a decay rate of merely 53.2 μV h−1. Coupling in-situ Fourier transform infrared (FTIR) and electrochemical impedance spectroscopy with theoretical calculations, it is revealed that Os-SAC not only effectively increases the fraction of active water and the coverage of surface hydrogen (H*), but also exhibits an optimal hydrogen adsorption free energy (ΔGH*), which collectively endow a kinetically efficient Volmer-Tafel pathway for the alkaline HER, thereby achieving boosted HER activity. This study provides a simple and effective strategy for synthesizing ultrahigh-loading SACs on oxide supports, which strongly promotes their application in water electrolysis and beyond.
单原子催化剂由于其独特的原子结构和优异的催化活性而受到人们的广泛关注。然而，在特定氧化物载体上制造高密度sac的持续挑战阻碍了它们的广泛应用。在此，我们报告了一种简单的微波辅助水热合成方法，在富含缺陷的氧化钨载体（Os-SAC@WO3）上制备锇- sacs，其负载高达31.7 wt%（12.4 at%）。令人印象深刻的是，获得的Os-SAC@WO3在碱性淡水/海水介质中表现出优异的析氢反应（HER）活性，在10 mA cm−2时，过电位仅为24/23 mV，超过了商业Pt/C（39/34 mV）。此外，以Os-SAC@WO3为阴极的阴离子交换膜水电解槽（AEMWE）在碱性海水中具有显著的长期稳定性，在100 mA cm−2下稳定运行1000 h以上，衰变率仅为53.2 μV h−1。结合原位傅里叶变换红外（FTIR）和电化学阻抗谱与理论计算，发现Os-SAC不仅有效地提高了活性水的分数和表面氢的覆盖率（H*），而且表现出最佳的氢吸附自由能（ΔGH*），这共同赋予了碱性HER的动力学高效的Volmer-Tafel途径，从而实现了HER活性的提高。该研究为在氧化物载体上合成超高负载SACs提供了一种简单有效的策略，有力地促进了其在水电解等领域的应用。
{"title":"Microwave-assisted synthesis of defect-rich oxide-stabilized ultrahigh-density osmium single atoms for hydrogen production","authors":"Zhihao Lou , Pengfei Wu , Yuanshuo Ma , Da Xue , Pengfei Wang , Fangyi Ma , Xuejing Cui , Guangbo Liu , Xin Zhou , Erdong Wang , Wenzhen Li , Luhua Jiang","doi":"10.1016/j.nanoen.2026.111733","DOIUrl":"10.1016/j.nanoen.2026.111733","url":null,"abstract":"<div><div>Single atom catalysts (SACs) have attracted great attention due to their unique atomic structure and exceptional catalytic activity. Nevertheless, persistent challenges in fabricating high-density SACs on specific oxide supports have hindered their broad application. Herein, we report a facile microwave-assisted hydrothermal synthesis method to fabricate osmium-SACs on a defect-rich tungsten oxide support (Os-SAC@WO<sub>3</sub>) with an unprecedented loading up to 31.7 wt% (12.4 at%). Impressively, the as-obtained Os-SAC@WO<sub>3</sub> exhibits excellent hydrogen evolution reaction (HER) activity with overpotentials of only 24/23 mV at 10 mA cm<sup>−2</sup> in alkaline freshwater/seawater media, surpassing commercial Pt/C (39/34 mV). Moreover, an anion-exchange membrane water electrolyzer (AEMWE) with Os-SAC@WO<sub>3</sub> as the cathode achieves remarkable long-term stability in alkaline seawater, enabling stable operation at 100 mA cm<sup>−2</sup> for more than 1000 h with a decay rate of merely 53.2 μV h<sup>−1</sup>. Coupling in-situ Fourier transform infrared (FTIR) and electrochemical impedance spectroscopy with theoretical calculations, it is revealed that Os-SAC not only effectively increases the fraction of active water and the coverage of surface hydrogen (H*), but also exhibits an optimal hydrogen adsorption free energy (Δ<em>G</em><sub>H*</sub>), which collectively endow a kinetically efficient Volmer-Tafel pathway for the alkaline HER, thereby achieving boosted HER activity. This study provides a simple and effective strategy for synthesizing ultrahigh-loading SACs on oxide supports, which strongly promotes their application in water electrolysis and beyond.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111733"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995972","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-15DOI: 10.1016/j.nanoen.2026.111732
Linhan Dong , Dongdong Feng , Yichun Li , Yu Zhang , Yijun Zhao , Qian Du , Jianmin Gao , Shaozeng Sun
The integration of CO2 capture and electrochemical CO2 reduction reaction (ECO2RR) enables low-energy conversion of CO2 from the emission end to the product end. To effectively address issues such as the consumption of products from new ammonia-based carbon capture technology and the high energy consumption of CO2 regeneration, this study prepared a Cu single-atom catalyst (SACu/CNTs) and proposed using NH4HCO3 as the electrolyte for ECO2RR. The Cu-N3 structure of the catalyst is confirmed by X-ray absorption fine structure testing. Benefiting from the double hydrolysis characteristics of NH4HCO3 solution, Faraday efficiency (FE) of 60 % for CO is achieved at −1.4 V. In-situ Raman spectroscopy confirms that the adsorption of NH4+ on the catalyst and the coverage of H+ resulted in suboptimal CO selectivity. By dynamically regulating the valence state of Cu using a pulsed potential to avoid NH4+ and H+ coverage, FE of CO is increased to 78 %. Density functional theory (DFT) calculations indicate that the ηCO of the Cu-N3V-SAC structure of the catalyst is 1.161, indicating a suitable adsorption strength for CO. The decrease in the coordination number of N enhances the adsorption strength for *COOH, the rate-determining step of the reaction shifts from CO2 → *COOH to *CO → CO. Using the carbon capture product NH4HCO3 as the electrolyte for ECO2RR demonstrates potential application prospects. This study provides new ideas and theoretical support for catalyst design in integrated carbon capture and utilization (ICCU).
{"title":"New ammonia-based CO2 capture product (NH4HCO3) for electrochemical reduction of single-atom Cu catalyst to CO","authors":"Linhan Dong , Dongdong Feng , Yichun Li , Yu Zhang , Yijun Zhao , Qian Du , Jianmin Gao , Shaozeng Sun","doi":"10.1016/j.nanoen.2026.111732","DOIUrl":"10.1016/j.nanoen.2026.111732","url":null,"abstract":"<div><div>The integration of CO<sub>2</sub> capture and electrochemical CO<sub>2</sub> reduction reaction (ECO<sub>2</sub>RR) enables low-energy conversion of CO<sub>2</sub> from the emission end to the product end. To effectively address issues such as the consumption of products from new ammonia-based carbon capture technology and the high energy consumption of CO<sub>2</sub> regeneration, this study prepared a Cu single-atom catalyst (SACu/CNTs) and proposed using NH<sub>4</sub>HCO<sub>3</sub> as the electrolyte for ECO<sub>2</sub>RR. The Cu-N<sub>3</sub> structure of the catalyst is confirmed by X-ray absorption fine structure testing. Benefiting from the double hydrolysis characteristics of NH<sub>4</sub>HCO<sub>3</sub> solution, Faraday efficiency (FE) of 60 % for CO is achieved at −1.4 V. In-situ Raman spectroscopy confirms that the adsorption of NH<sub>4</sub><sup>+</sup> on the catalyst and the coverage of H<sup>+</sup> resulted in suboptimal CO selectivity. By dynamically regulating the valence state of Cu using a pulsed potential to avoid NH<sub>4</sub><sup>+</sup> and H<sup>+</sup> coverage, FE of CO is increased to 78 %. Density functional theory (DFT) calculations indicate that the <em>η</em><sub>CO</sub> of the Cu-N<sub>3</sub>V-SAC structure of the catalyst is 1.161, indicating a suitable adsorption strength for CO. The decrease in the coordination number of N enhances the adsorption strength for *COOH, the rate-determining step of the reaction shifts from CO<sub>2</sub> → *COOH to *CO → CO. Using the carbon capture product NH<sub>4</sub>HCO<sub>3</sub> as the electrolyte for ECO<sub>2</sub>RR demonstrates potential application prospects. This study provides new ideas and theoretical support for catalyst design in integrated carbon capture and utilization (ICCU).</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111732"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Perovskite materials have emerged as one of the most promising classes of coordination compounds towards electrocatalytic water splitting. The structural flexibility, tunable electronic configurations, and rich surface redox chemistry make such materials potential candidates for electrochemical hydrogen generation. This review presents an extensive investigation of recent advancements in understanding and design of perovskite-based hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalysts. Importance is emphasized on correlating crystal field effects, metal-oxygen covalency, and eg orbital occupancy to catalytic activity, offering mechanistic insights into reaction energetics and rate-determining steps. Progress in theoretical descriptors and computational screening are critically reviewed towards predictive catalyst design. Besides mechanistic considerations, this review discusses efficiency benchmarks, stability targets, and techno-economic factors defining translational potential of perovskites-based water splitting systems. A dedicated section critically evaluates commercialization pathways, SWOT analysis and the realistic R&D priorities for accessing benchmark activity and durability against industry standards, while highlighting opportunities and challenges for bridging lab to commercial-scale deployment gap. By integrating fundamental coordination chemistry with practical feasibility, this review aims to deliver both conceptual clarity and a roadmap for accelerating perovskite-based electrocatalysis towards impactful and sustained hydrogen generation.
{"title":"Perovskite-based electrocatalysts: A new frontier in water splitting for sustainable hydrogen production","authors":"Iqra Hamdani , Pinky Sagar , Faisal Shahzad , Vinay Gupta , Gobind Das","doi":"10.1016/j.nanoen.2026.111721","DOIUrl":"10.1016/j.nanoen.2026.111721","url":null,"abstract":"<div><div>Perovskite materials have emerged as one of the most promising classes of coordination compounds towards electrocatalytic water splitting. The structural flexibility, tunable electronic configurations, and rich surface redox chemistry make such materials potential candidates for electrochemical hydrogen generation. This review presents an extensive investigation of recent advancements in understanding and design of perovskite-based hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalysts. Importance is emphasized on correlating crystal field effects, metal-oxygen covalency, and e<sub>g</sub> orbital occupancy to catalytic activity, offering mechanistic insights into reaction energetics and rate-determining steps. Progress in theoretical descriptors and computational screening are critically reviewed towards predictive catalyst design. Besides mechanistic considerations, this review discusses efficiency benchmarks, stability targets, and techno-economic factors defining translational potential of perovskites-based water splitting systems. A dedicated section critically evaluates commercialization pathways, SWOT analysis and the realistic R&D priorities for accessing benchmark activity and durability against industry standards, while highlighting opportunities and challenges for bridging lab to commercial-scale deployment gap. By integrating fundamental coordination chemistry with practical feasibility, this review aims to deliver both conceptual clarity and a roadmap for accelerating perovskite-based electrocatalysis towards impactful and sustained hydrogen generation.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111721"},"PeriodicalIF":17.1,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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