Constructing 2D/3D perovskite heterojunction is an effective method to improve performance and stability of perovskite solar cells (PSCs), while the quantum well in 2D perovskites hinders carrier transport. To address this issue, π-conjugated semiconducting ligands have been introduced to enhance carrier-transfer capability of 2D perovskites. Here, two triphenylamine (TPA)-based ligands are specifically designed through π-extension with a fused (N-TPEAI) or covalently linked (P-TPEAI) benzene ring. For the first time, TPA semiconductor-based ligands have been incorporated to construct 2D/3D PSCs with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as hole-transport materials (HTMs). Combined experimental and computational analyses reveal that this π-conjugation extension strategy proves to be effective in strengthening intermolecular interactions both between the adjacent spacer cations within 2D perovskites and at perovskite/PTAA interfaces, particularly in the case of P-TPEAI. Ultimately, the resultant 2D/3D PSCs employing P-TPEAI achieve an outstanding efficiency of 26.13%, which, to the best of our knowledge, is the highest value reported for 2D/3D PSCs incorporating PTAA HTMs. Moreover, benefiting from the robustness of both 2D perovskites and PTAA, the corresponding devices also exhibit excellent light-heat stability, meeting ISOS-L-2 protocol. These findings provide important guidelines for future design of organic spacers in advancing efficient and robust PSCs and related optoelectronic devices.
构建二维/三维钙钛矿异质结是提高钙钛矿太阳能电池(PSCs)性能和稳定性的有效方法,而二维钙钛矿中的量子阱阻碍了载流子的输运。为了解决这一问题,引入π共轭半导体配体来提高二维钙钛矿的载流子转移能力。本文设计了两种以三苯胺(TPA)为基础的配体,通过π扩展与一个融合苯环(N-TPEAI)或共价连接苯环(P-TPEAI)。首次将TPA半导体配体与聚[双(4-苯基)(2,4,6-三甲基苯基)胺](PTAA)作为空穴传输材料(HTMs)构建2D/3D PSCs。结合实验和计算分析表明,这种π共轭扩展策略在增强二维钙钛矿内相邻间隔阳离子之间和钙钛矿/PTAA界面上的分子间相互作用方面是有效的,特别是在P-TPEAI的情况下。最终,采用P-TPEAI的2D/3D PSCs的效率达到了26.13%,据我们所知,这是采用PTAA HTMs的2D/3D PSCs的最高效率。此外,得益于二维钙钛矿和PTAA的鲁棒性,相应的器件也表现出优异的光热稳定性,符合iso - l -2协议。这些发现为未来有机间隔材料的设计提供了重要的指导,以推进高效、稳健的psc和相关光电器件。
{"title":"Interfacial Coupling Design Enhancing Hole Transport in PTAA-Based Perovskite Solar Cells with Efficiency over 26.","authors":"Huaiman Cao,Xufan Zheng,Yue Qiang,Liangyu Zhao,Yulong Chen,Zhiguang Sun,Yingguo Yang,Hin-Lap Yip,Ze Yu","doi":"10.1007/s40820-026-02145-4","DOIUrl":"https://doi.org/10.1007/s40820-026-02145-4","url":null,"abstract":"Constructing 2D/3D perovskite heterojunction is an effective method to improve performance and stability of perovskite solar cells (PSCs), while the quantum well in 2D perovskites hinders carrier transport. To address this issue, π-conjugated semiconducting ligands have been introduced to enhance carrier-transfer capability of 2D perovskites. Here, two triphenylamine (TPA)-based ligands are specifically designed through π-extension with a fused (N-TPEAI) or covalently linked (P-TPEAI) benzene ring. For the first time, TPA semiconductor-based ligands have been incorporated to construct 2D/3D PSCs with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as hole-transport materials (HTMs). Combined experimental and computational analyses reveal that this π-conjugation extension strategy proves to be effective in strengthening intermolecular interactions both between the adjacent spacer cations within 2D perovskites and at perovskite/PTAA interfaces, particularly in the case of P-TPEAI. Ultimately, the resultant 2D/3D PSCs employing P-TPEAI achieve an outstanding efficiency of 26.13%, which, to the best of our knowledge, is the highest value reported for 2D/3D PSCs incorporating PTAA HTMs. Moreover, benefiting from the robustness of both 2D perovskites and PTAA, the corresponding devices also exhibit excellent light-heat stability, meeting ISOS-L-2 protocol. These findings provide important guidelines for future design of organic spacers in advancing efficient and robust PSCs and related optoelectronic devices.","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"16 1","pages":""},"PeriodicalIF":26.6,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147471756","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}
Self-powered flexible sensors exhibit revolutionary potential in next-generation wearable technologies owing to their exceptional sensitivity and self-sustaining energy harvesting capabilities. Nevertheless, their widespread deployment remains constrained by three fundamental challenges: dynamic mechanical mismatch between biological tissues and rigid devices, suboptimal energy conversion efficiency, and interfacial impedance fluctuation under deformation. Drawing inspiration from the unique negative Poisson's ratio mesh architecture of lacewing wings, we present a bioinspired auxetic metastructure-engineered triboelectric nanogenerator. This innovative design integrates engineered collagen and micropatterned fluorinated ethylene propylene as triboelectric layers, unified by an auxetic framework with re-entrant hexagonal unit cells interconnected via triangular ligaments. The metastructure enables exceptional lateral expansion under longitudinal strain while simultaneously enhancing structural rigidity and deformation adaptability. This dual functionality effectively minimizes tissue-device mechanical mismatch, thereby significantly improving signal fidelity, sensitivity, and mechanical-to-electrical conversion efficiency during multi-axial deformations. The optimized device achieves remarkable performance metrics, delivering 478 V output voltage with 13.8% energy conversion efficiency in linear configuration, while demonstrating threefold enhanced stability (58 V, 7.58% efficiency) under complex bending compared to conventional designs. Integrated with a convolutional neural network-based machine learning enables exceptional classification accuracy (> 99%) across diverse material recognition tasks, validating its robustness as a next-generation platform for adaptive self-powered wearable sensing.
{"title":"Bioinspired Auxetic Metastructures Enable Biomechanically Adaptive, Machine Learning-Enhanced Self-Powered Sensing with Ultrahigh Efficiency.","authors":"Wei Wang,Xuechuan Wang,Linbin Li,Yi Zhou,Wenlong Zhang,Long Xing,Long Xie,Yitong Wang,Ouyang Yue,Xinhua Liu","doi":"10.1007/s40820-026-02125-8","DOIUrl":"https://doi.org/10.1007/s40820-026-02125-8","url":null,"abstract":"Self-powered flexible sensors exhibit revolutionary potential in next-generation wearable technologies owing to their exceptional sensitivity and self-sustaining energy harvesting capabilities. Nevertheless, their widespread deployment remains constrained by three fundamental challenges: dynamic mechanical mismatch between biological tissues and rigid devices, suboptimal energy conversion efficiency, and interfacial impedance fluctuation under deformation. Drawing inspiration from the unique negative Poisson's ratio mesh architecture of lacewing wings, we present a bioinspired auxetic metastructure-engineered triboelectric nanogenerator. This innovative design integrates engineered collagen and micropatterned fluorinated ethylene propylene as triboelectric layers, unified by an auxetic framework with re-entrant hexagonal unit cells interconnected via triangular ligaments. The metastructure enables exceptional lateral expansion under longitudinal strain while simultaneously enhancing structural rigidity and deformation adaptability. This dual functionality effectively minimizes tissue-device mechanical mismatch, thereby significantly improving signal fidelity, sensitivity, and mechanical-to-electrical conversion efficiency during multi-axial deformations. The optimized device achieves remarkable performance metrics, delivering 478 V output voltage with 13.8% energy conversion efficiency in linear configuration, while demonstrating threefold enhanced stability (58 V, 7.58% efficiency) under complex bending compared to conventional designs. Integrated with a convolutional neural network-based machine learning enables exceptional classification accuracy (> 99%) across diverse material recognition tasks, validating its robustness as a next-generation platform for adaptive self-powered wearable sensing.","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"27 1","pages":""},"PeriodicalIF":26.6,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147471761","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}
The oxygen evolution reaction (OER) in seawater electrolysis is pivotal for sustainable hydrogen production, yet severe chloride ion (Cl-)-induced corrosion at the anode critically limits catalyst durability. Herein, we design a heterostructured catalyst comprising NiFe-layered double hydroxide and Ce(OH)CO3 (denoted as NiFe-LDH/Ce(OH)CO3) that exhibits remarkable OER stability in alkaline-simulated seawater. Experimental results and density functional theory calculations reveal that Ce(OH)CO3 incorporation modulates interfacial charge redistribution and enhances the Lewis acidity of Ni and Fe sites, thereby tuning the adsorption energetics of Cl- and OH-. Time-of-flight secondary ion mass spectrometry further confirms the preferential adsorption of OH- over Cl-, effectively suppressing Cl--induced corrosion. As a result, NiFe-LDH/Ce(OH)CO3 demonstrates exceptional long-term stability, maintaining continuous operation for over 450 h at 1 A cm-2 in alkaline seawater. When integrated into an anion exchange membrane electrolyzer, the catalyst achieves 1 A cm-2 at a low cell voltage of 1.92 V and operates stably for over 60 h. The system delivers an impressive energy efficiency of 68.59% in alkaline-simulated seawater, corresponding to a hydrogen production cost as low as $0.97 per gasoline gallon equivalent at 500 mA cm-2.
海水电解中的析氧反应(OER)是可持续制氢的关键,但阳极严重的氯离子(Cl-)腐蚀严重限制了催化剂的耐久性。本文设计了一种异质结构催化剂,由nife层状双氢氧化物和Ce(OH)CO3组成(表示为NiFe-LDH/Ce(OH)CO3),该催化剂在碱性模拟海水中表现出显著的OER稳定性。实验结果和密度泛函理论计算表明,Ce(OH)CO3的掺入调节了界面电荷重分布,增强了Ni和Fe位点的Lewis酸度,从而调节了Cl-和OH-的吸附能量。飞行时间二次离子质谱进一步证实了OH-比Cl-优先吸附,有效抑制Cl-引起的腐蚀。因此,nfe - ldh /Ce(OH)CO3表现出优异的长期稳定性,在碱性海水中以1 a cm-2的温度连续运行超过450小时。当集成到阴离子交换膜电解槽中时,催化剂在1.92 V的低电池电压下达到1 A cm-2,并稳定运行超过60小时。该系统在碱性模拟海水中提供了令人印象深刻的68.59%的能源效率,相当于在500 mA cm-2下每加仑汽油的制氢成本低至0.97美元。
{"title":"Enhancing the Selective OH- Adsorption for Durable Alkaline Seawater Oxidation at Industrial Current Densities.","authors":"Shangshu Hu,Jiao Yang,Yujuan Zhuang,Xueyao Li,Han Xu,Fuwang Hu,Zhishuo Yan,Chao Liu,Jianmin Yu,Lishan Peng","doi":"10.1007/s40820-026-02133-8","DOIUrl":"https://doi.org/10.1007/s40820-026-02133-8","url":null,"abstract":"The oxygen evolution reaction (OER) in seawater electrolysis is pivotal for sustainable hydrogen production, yet severe chloride ion (Cl-)-induced corrosion at the anode critically limits catalyst durability. Herein, we design a heterostructured catalyst comprising NiFe-layered double hydroxide and Ce(OH)CO3 (denoted as NiFe-LDH/Ce(OH)CO3) that exhibits remarkable OER stability in alkaline-simulated seawater. Experimental results and density functional theory calculations reveal that Ce(OH)CO3 incorporation modulates interfacial charge redistribution and enhances the Lewis acidity of Ni and Fe sites, thereby tuning the adsorption energetics of Cl- and OH-. Time-of-flight secondary ion mass spectrometry further confirms the preferential adsorption of OH- over Cl-, effectively suppressing Cl--induced corrosion. As a result, NiFe-LDH/Ce(OH)CO3 demonstrates exceptional long-term stability, maintaining continuous operation for over 450 h at 1 A cm-2 in alkaline seawater. When integrated into an anion exchange membrane electrolyzer, the catalyst achieves 1 A cm-2 at a low cell voltage of 1.92 V and operates stably for over 60 h. The system delivers an impressive energy efficiency of 68.59% in alkaline-simulated seawater, corresponding to a hydrogen production cost as low as $0.97 per gasoline gallon equivalent at 500 mA cm-2.","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"9 1","pages":""},"PeriodicalIF":26.6,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147471762","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}
The improvement in efficiency and stability of inverted perovskite solar cells (PSCs) is primarily constrained by the charge-carrier and energy losses at the interface of perovskite active layer/charge-carrier transport layers. Herein, a kind of dipolar molecule, 4-aminocyclohexanone hydrochloride (ACHCl), is introduced to the surface of perovskite films in PSCs with p-i-n structure. This surface modification ingeniously utilizes the surface defects of perovskite films to anchor the dipolar molecule, thus inducing surface polarization, which not only effectively reduces interfacial defects but also optimizes the energy-level alignment between the interfaces. Specifically, the carbonyl group and chloride ion on ACHCl anchors on the uncoordinated lead ion defects and fills in the halide vacancies on perovskite surface, respectively, which effectively alleviates the trap-state density, thereby reducing the carrier losses caused by defect-assisted recombination at the interface of perovskite layer/hole transport layer. Meanwhile, the anchoring effect of ACHCl facilitates the formation of a relatively ordered cation-dipole layer and induces surface polarization, resulting in more favorable energy-level alignment and enhanced charge-carrier extraction, ultimately reducing interfacial energy losses. Consequently, the effective reduction in interfacial losses facilitates the ACHCl-modified devices to achieve a power conversion efficiency of 26.12% and improved stability.
{"title":"Defect-Anchored Dipole Molecules Induce Surface Polarization Facilitating High-Performance Inverted Perovskite Solar Cells.","authors":"Weichun Pan,Jihuai Wu,Jiexi Pan,Shanyue Wei,Lina Tan,Wenjing Li,Deng Wang,Xuping Liu,Yiming Xie,Jianming Lin,Zhang Lan","doi":"10.1007/s40820-026-02150-7","DOIUrl":"https://doi.org/10.1007/s40820-026-02150-7","url":null,"abstract":"The improvement in efficiency and stability of inverted perovskite solar cells (PSCs) is primarily constrained by the charge-carrier and energy losses at the interface of perovskite active layer/charge-carrier transport layers. Herein, a kind of dipolar molecule, 4-aminocyclohexanone hydrochloride (ACHCl), is introduced to the surface of perovskite films in PSCs with p-i-n structure. This surface modification ingeniously utilizes the surface defects of perovskite films to anchor the dipolar molecule, thus inducing surface polarization, which not only effectively reduces interfacial defects but also optimizes the energy-level alignment between the interfaces. Specifically, the carbonyl group and chloride ion on ACHCl anchors on the uncoordinated lead ion defects and fills in the halide vacancies on perovskite surface, respectively, which effectively alleviates the trap-state density, thereby reducing the carrier losses caused by defect-assisted recombination at the interface of perovskite layer/hole transport layer. Meanwhile, the anchoring effect of ACHCl facilitates the formation of a relatively ordered cation-dipole layer and induces surface polarization, resulting in more favorable energy-level alignment and enhanced charge-carrier extraction, ultimately reducing interfacial energy losses. Consequently, the effective reduction in interfacial losses facilitates the ACHCl-modified devices to achieve a power conversion efficiency of 26.12% and improved stability.","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"24 1","pages":""},"PeriodicalIF":26.6,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147471713","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 : 2026-03-18DOI: 10.1007/s40820-026-02140-9
Qi-Fan Xuan,Pei-Yan Zhao,Hualong Peng,Shan Zhang,Bo Cai,Fang-Yu Niu,Martin C Koo,Xiao-Bo Sun,Xiangyu Jiang,Guang-Sheng Wang
Integrated wearable thermal management technologies have greatly enhanced human adaptability to complex environments. However, conventional thermal management strategies, which lack environmental risk perception and stable human-machine interaction, are increasingly inadequate for ensuring personal health. Here, we introduce a hierarchical modular design strategy to develop a wearable intelligent thermal management film with robust electromagnetic interference (EMI) shielding capabilities. A sensitive biomimetic serpentine dual-mode temperature-humidity sensing module is coupled with a low-power electro-/photothermal conversion module to enable intelligent thermal regulation. The resulting thermal management system offers stable and sensitive front-end temperature-humidity monitoring, alongside low-power electrothermal (51.79 °C at 1.5 V) and photothermal (56.38 °C at 45.51 mW cm-2) temperature regulation capabilities. Additionally, the system exhibits outstanding EMI shielding performance, with an EMI SE/t value of 1600 dB mm-1 at a thickness of just 35 μm, ensuring stable signal transmission. The hierarchical modular design enables functional allocation with higher, thereby optimizing material performance while enhancing the decoupling and synergistic effects between different functionalities. These findings provide a scalable and practical pathway for the multifunctional integration and performance optimization of next-generation flexible wearable electronic composites.
集成可穿戴热管理技术大大提高了人类对复杂环境的适应能力。然而,传统的热管理策略缺乏环境风险感知和稳定的人机交互,越来越不足以确保个人健康。本文介绍了一种分层模块化设计策略,用于开发具有强大电磁干扰屏蔽能力的可穿戴智能热管理膜。一个灵敏的仿生蛇形双模温湿度传感模块与一个低功耗电/光热转换模块相结合,实现智能热调节。由此产生的热管理系统提供稳定而敏感的前端温度湿度监测,以及低功耗电热(1.5 V时51.79°C)和光热(45.51 mW cm-2时56.38°C)温度调节能力。此外,该系统具有出色的EMI屏蔽性能,在厚度仅为35 μm的情况下,EMI SE/t值为1600 dB mm-1,确保了稳定的信号传输。层次化的模块化设计使功能配置更高,从而优化材料性能,同时增强不同功能之间的解耦和协同效应。这些发现为下一代柔性可穿戴电子复合材料的多功能集成和性能优化提供了可扩展和实用的途径。
{"title":"Hierarchical Modular Architecture Enabling Intelligent Dynamic Thermal Management and Superior Electromagnetic Interference Shielding.","authors":"Qi-Fan Xuan,Pei-Yan Zhao,Hualong Peng,Shan Zhang,Bo Cai,Fang-Yu Niu,Martin C Koo,Xiao-Bo Sun,Xiangyu Jiang,Guang-Sheng Wang","doi":"10.1007/s40820-026-02140-9","DOIUrl":"https://doi.org/10.1007/s40820-026-02140-9","url":null,"abstract":"Integrated wearable thermal management technologies have greatly enhanced human adaptability to complex environments. However, conventional thermal management strategies, which lack environmental risk perception and stable human-machine interaction, are increasingly inadequate for ensuring personal health. Here, we introduce a hierarchical modular design strategy to develop a wearable intelligent thermal management film with robust electromagnetic interference (EMI) shielding capabilities. A sensitive biomimetic serpentine dual-mode temperature-humidity sensing module is coupled with a low-power electro-/photothermal conversion module to enable intelligent thermal regulation. The resulting thermal management system offers stable and sensitive front-end temperature-humidity monitoring, alongside low-power electrothermal (51.79 °C at 1.5 V) and photothermal (56.38 °C at 45.51 mW cm-2) temperature regulation capabilities. Additionally, the system exhibits outstanding EMI shielding performance, with an EMI SE/t value of 1600 dB mm-1 at a thickness of just 35 μm, ensuring stable signal transmission. The hierarchical modular design enables functional allocation with higher, thereby optimizing material performance while enhancing the decoupling and synergistic effects between different functionalities. These findings provide a scalable and practical pathway for the multifunctional integration and performance optimization of next-generation flexible wearable electronic composites.","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"34 1","pages":""},"PeriodicalIF":26.6,"publicationDate":"2026-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147471759","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}
Energy-efficient and selective hydrocarbon reforming techniques are crucial for a sustainable future. This study develops a highly active and selective NiO/CeO2 oxygen carrier (OC) for low-temperature chemical looping partial oxidation of methane and water splitting. By using cubic CeO2 (cCeO2) as support and precisely tailoring the size and electronic structure of Ni active sites, simultaneous low-temperature CH4 activation and high syngas selectivity (CH4-to-syngas selectivity: > 98.5%) were achieved, effectively suppressing CH4 cracking and complete oxidation. The as-synthesized NiO/cCeO2 OCs operate efficiently at 600 °C, significantly lower than the conventional temperature, 800-900 °C. Nearly pure H2 is produced in the water splitting step. High selectivity eliminates the need for additional gas separation and purification units. It is noteworthy that reaction-driven OC activation pretreatment plays a significant role in achieving the stable low-temperature activity, which leads to the moderate aggregation (10-20 nm) of Ni species and transforms Ni2+ from a low-spin state into a high-spin state. The OC structural evolution during reaction, key active sites responsible for water splitting, and the support effect are systematically investigated. The highly precise microstructural manipulation strategies outlined here are expected to guide further advancements in high-performance low-temperature OCs for chemical looping processes.
{"title":"Low-Temperature CH<sub>4</sub> Reforming and Water Splitting with Activated NiO/CeO<sub>2</sub> as Oxygen Carrier.","authors":"Chunli Han, Akira Yoko, Yi-Ping Chang, Manuel Harder, Kakeru Ninomiya, Maiko Nishibori, Zhong Yin, Ardiansyah Taufik, Satoshi Ohara, Tadafumi Adschiri","doi":"10.1007/s40820-026-02097-9","DOIUrl":"10.1007/s40820-026-02097-9","url":null,"abstract":"<p><p>Energy-efficient and selective hydrocarbon reforming techniques are crucial for a sustainable future. This study develops a highly active and selective NiO/CeO<sub>2</sub> oxygen carrier (OC) for low-temperature chemical looping partial oxidation of methane and water splitting. By using cubic CeO<sub>2</sub> (cCeO<sub>2</sub>) as support and precisely tailoring the size and electronic structure of Ni active sites, simultaneous low-temperature CH<sub>4</sub> activation and high syngas selectivity (CH<sub>4</sub>-to-syngas selectivity: > 98.5%) were achieved, effectively suppressing CH<sub>4</sub> cracking and complete oxidation. The as-synthesized NiO/cCeO<sub>2</sub> OCs operate efficiently at 600 °C, significantly lower than the conventional temperature, 800-900 °C. Nearly pure H<sub>2</sub> is produced in the water splitting step. High selectivity eliminates the need for additional gas separation and purification units. It is noteworthy that reaction-driven OC activation pretreatment plays a significant role in achieving the stable low-temperature activity, which leads to the moderate aggregation (10-20 nm) of Ni species and transforms Ni<sup>2+</sup> from a low-spin state into a high-spin state. The OC structural evolution during reaction, key active sites responsible for water splitting, and the support effect are systematically investigated. The highly precise microstructural manipulation strategies outlined here are expected to guide further advancements in high-performance low-temperature OCs for chemical looping processes.</p>","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"18 1","pages":""},"PeriodicalIF":36.3,"publicationDate":"2026-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12996510/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147472337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}