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Optimizing Adsorption-Catalysis Synergy to Accelerate Sulfur Conversion Kinetics in Room-Temperature Na-S Batteries

IF 13.3 2区材料科学

Small Pub Date : 2025-04-25 DOI: 10.1002/smll.202502257

Yujie Shi, Limou Zhang, Ting Wang, Runze Ma, Dongjiao Wang, Yujun Fu, RuiPu Du, Junfei Zhang, Dequan Liu, Liang Wu, Weihan Li, Ying Wu, Deyan He

{"title":"Optimizing Adsorption-Catalysis Synergy to Accelerate Sulfur Conversion Kinetics in Room-Temperature Na-S Batteries","authors":"Yujie Shi, Limou Zhang, Ting Wang, Runze Ma, Dongjiao Wang, Yujun Fu, RuiPu Du, Junfei Zhang, Dequan Liu, Liang Wu, Weihan Li, Ying Wu, Deyan He","doi":"10.1002/smll.202502257","DOIUrl":"https://doi.org/10.1002/smll.202502257","url":null,"abstract":"Room-temperature sodium-sulfur (RT Na-S) batteries are expected to become the next-generation energy storage system due to their ultrahigh theoretically energy density of 1274 Wh kg−1, abundant sulfur resource, and low cost. However, practical application is hindered by challenges of severe shuttle effect and sluggish S conversion kinetics. In this study, a series of nano-sized nickel-based chalcogenides are designed and fabricated as electrocatalysts for S cathode. The p orbitals originated from different anions show great effect on the partial-filled d orbital of the metal Ni site, which further regulates the electronic states of the catalytic site. Theoretical and experimental results confirm the excellent electrocatalytic performance of NiSe electrocatalyst with low reaction energy barriers, moderate adsorption capability, and strong catalytic conversion ability, consistent with Sabatier's principle. The optimized NiSe catalyst presents a high reversible capacity of 720.4 mAh g−1 with excellent durability over 200 cycles at 0.2 A g−1 retained a capacity of 401.4 mAh g−1 after 1000 cycles at 2 A g−1 in RT Na-S batteries. This work presents the balancing of adsorption and catalytic conversion toward polysulfides via the modulation of d/p orbitals of active sites.","PeriodicalId":228,"journal":{"name":"Small","volume":"67 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Inflammation Targeting and Responsive Multifunctional Drug-Delivery Nanoplatforms for Combined Therapy of Rheumatoid Arthritis

IF 13.3 2区材料科学

Small Pub Date : 2025-04-25 DOI: 10.1002/smll.202500113

Hongyang Li, Xiangbowen Jin, Binbin Chu, Kai Zhang, Xuan Qin, Sheng Pan, Yadan Zhao, Haoliang Shi, Jiawei Zhang, Houyu Wang, Zhen Wen, Yao He, Xuhui Sun

{"title":"Inflammation Targeting and Responsive Multifunctional Drug-Delivery Nanoplatforms for Combined Therapy of Rheumatoid Arthritis","authors":"Hongyang Li, Xiangbowen Jin, Binbin Chu, Kai Zhang, Xuan Qin, Sheng Pan, Yadan Zhao, Haoliang Shi, Jiawei Zhang, Houyu Wang, Zhen Wen, Yao He, Xuhui Sun","doi":"10.1002/smll.202500113","DOIUrl":"https://doi.org/10.1002/smll.202500113","url":null,"abstract":"Rheumatoid arthritis (RA) is a chronic autoimmune disorder characterized by persistent inflammation, joint swelling, pain, and progressive joint destruction. Methotrexate (MTX) is the standard first-line treatment for RA, but its clinical application is hindered by poor water solubility and non-specific delivery. In this work, a multifunctional drug-delivery nanoplatform that targets both macrophages and tumor necrosis factor α (TNFα) is developed to enhance the therapeutic efficacy of MTX in RA. The nanoplatform consists of folic acid (FA, for macrophage targeting) and a TNFα-specific Aptamer (TNFα-Apt), facilitating a dual-targeting strategy that significantly improves the accumulation of MTX at the sites of RA lesions (≈3.5-fold). Moreover, the manganese dioxide (MnO₂) and polydopamine (PDA) coatings on the nanoplatform effectively scavenge reactive oxygen species (ROS), generate oxygen, and promote the polarization of pro-inflammatory M1 macrophages to the anti-inflammatory M2 macrophages. This shift in macrophage polarization restores the expression of key inflammatory cytokines, improving the local inflammatory microenvironment. Ultimately, the nanoplatform significantly ameliorates the inflammation and joint damage in a collagen-induced arthritis (CIA) model, suggesting that this multi-target combination therapy holds considerable potential for the treatment of RA in vivo.","PeriodicalId":228,"journal":{"name":"Small","volume":"28 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Stabilize Perovskite Precursors and Inhibit Intermediates for High Performing Perovskite Solar Cells

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202503279

Zhiqian Yang, Aiqing Sun, Yingke Ren, Zhaoqian Li, Li'e Mo, Hong Zhang, Yang Huang, Linhua Hu

引用次数: 0

Real-Time Monitoring of Fe-Induced Stable γ-NiOOH in Binder-Free FeNi MOF Electrocatalysts for Enhanced Oxygen Evolution

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202501142

Kuan-Lun Chen, Yu-Hsuan Chou, Tsai-Jen Lin, Mu-Jeng Cheng, Po-Keng Hsiao, Ying-Chih Pu, I-Wen Peter Chen

{"title":"Real-Time Monitoring of Fe-Induced Stable γ-NiOOH in Binder-Free FeNi MOF Electrocatalysts for Enhanced Oxygen Evolution","authors":"Kuan-Lun Chen, Yu-Hsuan Chou, Tsai-Jen Lin, Mu-Jeng Cheng, Po-Keng Hsiao, Ying-Chih Pu, I-Wen Peter Chen","doi":"10.1002/smll.202501142","DOIUrl":"https://doi.org/10.1002/smll.202501142","url":null,"abstract":"Hydrogen energy is a promising renewable source, and metal-organic frameworks (MOFs) are considered potential electrocatalysts for water electrolysis due to their abundant active sites, high porosity, and large surface area. The synthesis of bimetallic iron-nickel-benzene-1,3,5-tricarboxylate/nickel foam (FeNi-BTC/NF) MOF is reported using a binder-free one-pot method by immersing nickel foam (NF) into a solution of benzene-1,3,5-tricarboxylic acid (BTC), N,N-dimethylformamide (DMF), and iron (Fe) salts. FeNi-BTC/NF exhibits a low overpotential of 276 mV at 100 mA cm−2, a Tafel slope of 94 mV dec−1, and stability exceeding 120 h. The Fe-Ni interaction facilitates the formation of a stable gamma-nickel oxyhydroxide (γ-NiOOH) phase, preventing its reversion to nickel hydroxyide (Ni(OH)₂), which is crucial for improving oxygen evolution reaction (OER) performance. This phase transition, revealed via in situ Raman spectroelectrochemical analysis, enhances electrocatalytic activity. Additionally, high-valent Fe modulates the electronic structure of Ni, enabling FeNi-BTC/NF to transform into γ-NiOOH at higher potentials, with Fe and γ-NiOOH synergistically boosting OER efficiency. The findings offer insights into Fe/Ni atom interactions and phase transformations in FeNi-BTC/NF MOFs for enhanced water splitting.","PeriodicalId":228,"journal":{"name":"Small","volume":"42 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Polyol-Intermediated Facile Synthesis of B5-Site-Rich Ru-Based Nanocatalysts for COx-Free Hydrogen Production via Ammonia Decomposition (Small 16/2025)

IF 13 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202570121

Kyoung Deok Kim, Jiyu Kim, Byeong-Seon An, Jung Hun Shin, Yongha Park, Unho Jung, Kwang Bok Yi, Kee Young Koo

引用次数: 0

Probing the Interplay of Protein Self-Assembly and Covalent Bond Formation in Photo-Crosslinked Silk Fibroin Hydrogels (Small 16/2025)

IF 13 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202570127

Hien A. Tran, Anton Maraldo, Trinh Thi-Phuong Ho, Mai Thanh Thai, Quinn van Hilst, Habib Joukhdar, Marija Kordanovski, Jugal Kishore Sahoo, Onur Hartsuk, Miguel Santos, Steven G. Wise, David L. Kaplan, Thanh Nho Do, Kristopher A. Kilian, Khoon S. Lim, Jelena Rnjak-Kovacina

引用次数: 0

Unleashing the Potential of Defect Engineered Persistent Pr3+-Activated Phosphors for Multi-Dimensional Anti-Counterfeiting and X-Ray Imaging Applications

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202501752

Annu Balhara, Santosh K. Gupta, Partha Sarathi Ghosh, Malini Abraham, Mohit Tyagi, Ashok Kumar Yadav, Subrata Das, Kathi Sudarshan, P. S. Sarkar

{"title":"Unleashing the Potential of Defect Engineered Persistent Pr3+-Activated Phosphors for Multi-Dimensional Anti-Counterfeiting and X-Ray Imaging Applications","authors":"Annu Balhara, Santosh K. Gupta, Partha Sarathi Ghosh, Malini Abraham, Mohit Tyagi, Ashok Kumar Yadav, Subrata Das, Kathi Sudarshan, P. S. Sarkar","doi":"10.1002/smll.202501752","DOIUrl":"https://doi.org/10.1002/smll.202501752","url":null,"abstract":"Persistent luminescence (PersL) in inorganic phosphors offers great potential for anti-counterfeiting and optical storage, with optimization of PersL, multicolor tuning, and defect engineering. This study presents a Ca3Ga2Ge3O12:Pr3+ (CGGO:Pr) phosphor with long-lasting PersL and multicolor emissions. Aliovalent codoping with Er3+ and Yb3+ ions optimizes deep/shallow trap redistribution, controlling trap depths from 0.98 to optimal 0.73 eV through the creation of new shallow electron traps (YbCa•, ErCa•) alongside existing VO levels. The smart Pr3+/Er3+/Yb3+:CGGO phosphor exhibits three-dimensional visible emissions under 275 and 380 nm excitation, as well as upconversion emissions under 980 nm laser irradiation. Hybrid density functional calculations, thermoluminescence, and positron annihilation lifetime spectroscopy revealed the nature and density of different traps controlling the PersL. Together, a single system featuring multicolor luminescence has been developed, exhibiting improved PersL and regulated trap depths (≈0.73 eV) suitable for robust and multimodal anti-counterfeiting of documents, pharmaceuticals, and industrial products. Furthermore, the composite PMMA-CGGO:Pr phosphor films have shown remarkable capability for X-ray imaging, achieving a resolution of 4 lp/mm, which exceeds that of commercial Gd2O2S:Tb screens. These findings highlight the potential of this work for advanced anti-counterfeiting and X-ray imaging applications, offering enhanced PersL with controlled trap depths.","PeriodicalId":228,"journal":{"name":"Small","volume":"32 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Diamondoid All-Carbon Porous Aromatic Framework Host for Lithium–Sulfur Batteries

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202500388

Viksit Kumar, Bharthkumar. H. Javaregowda, George Devasia, Aswini Narayanan, Sailaja Krishnamurty, Kothandam Krishnamoorthy, Sukumaran Santhosh Babu

{"title":"Diamondoid All-Carbon Porous Aromatic Framework Host for Lithium–Sulfur Batteries","authors":"Viksit Kumar, Bharthkumar. H. Javaregowda, George Devasia, Aswini Narayanan, Sailaja Krishnamurty, Kothandam Krishnamoorthy, Sukumaran Santhosh Babu","doi":"10.1002/smll.202500388","DOIUrl":"https://doi.org/10.1002/smll.202500388","url":null,"abstract":"Lithium-sulfur batteries (LSBs) hold incredible potential as next-generation energy storage systems. However, practical applications of LSBs are significantly hindered by several critical challenges. For the first time, scalable all-carbon porous 3D polymers (3DPs) that do not contain heteroatoms or functional groups and do not require post-functionalization are investigated as hosts in lithium–sulfur batteries, demonstrating enhanced cycling stability and overall battery performance. The pyrene-containing 3DP exhibits 75% capacity retention after 600 cycles at 1 C and 52% capacity retention after 1300 cycles at 0.2 C, better than phenyl comprising 3DP. Furthermore, even at higher sulfur loading (4.1 mg cm−2) with an electrolyte/sulfur ratio of 5 µL mg−1, pyrene 3DP displayed a high capacity of 600 mA h g−1 and stable performance over 250 cycles with negligible capacity fade. The defined pore structure of 3DPs prevents the migration of polysulfides through physical confinement and the large π-clouds of 3DPs interact with the negative charge-bearing polysulfides generated in charge–discharge cycles through anion-π interaction. In this way, The design ensures that the host 3DPs interact with neutral sulfur and anionic polysulfides, resulting in an excellent performance.","PeriodicalId":228,"journal":{"name":"Small","volume":"27 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867217","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cation/Anion Co-Doping Enhances Oxygen Redox Reversibility and Structural Stability in Single-Crystal Li-Rich Mn-Based Cathodes for Wide-Temperature Performance

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202501005

Biru Eshete Worku, Yang Lu, Mingzhi Song, Shumin Zheng, Bao Wang

{"title":"Cation/Anion Co-Doping Enhances Oxygen Redox Reversibility and Structural Stability in Single-Crystal Li-Rich Mn-Based Cathodes for Wide-Temperature Performance","authors":"Biru Eshete Worku, Yang Lu, Mingzhi Song, Shumin Zheng, Bao Wang","doi":"10.1002/smll.202501005","DOIUrl":"https://doi.org/10.1002/smll.202501005","url":null,"abstract":"Li-rich Mn-based cathode materials (LRMs) are the most promising cathodes for the next-generation Lithium-ion batteries due to their high energy density. However, LRMs encounter formidable challenges such as voltage/capacity decay, mediocre rate capability, low cyclability, and substantial capacity loss at low temperatures. These challenges stem from irreversible oxygen release and subsequent structural deterioration. As energy storage devices are required to operate across a wide temperature range, enhancing the electrochemical performance of LRMs at both room and low temperatures is crucial. Herein, an approach of Al and F co-doping on novel single-crystal Li1.2Mn0.54Ni0.13Co0.13O2 is proposed to promote oxygen redox reversibility and enhance structural stability. Investigations into the oxygen redox couple and manganese electronic structure demonstrate that the Al and F co-doped electrode (LRMAF) retains a higher amount of lattice oxygen (O2⁻) and a greater amount of Mn⁴⁺ after cycling. As a result, LRMAF exhibits a high energy density of 1185 Wh kg−1, an initial discharge capacity of 329 mAh g⁻¹ at 0.1C, achieves a rate performance of 155 mAh g⁻¹ at 5.0C and delivers 88% capacity retention after 100 cycles. Additionally, LRMAF exhibits excellent electrochemical performance at −20 °C. This enhancement is attributed to the novel single-crystal morphology combined with cation/anion co-doping.","PeriodicalId":228,"journal":{"name":"Small","volume":"26 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867233","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

One-Step Low-Temperature Synthesis of Metastable ε-Iron Carbide Nanoparticles with Unique Catalytic Properties Beyond Conventional Iron Catalysts

IF 13.3 2区材料科学

Small Pub Date : 2025-04-24 DOI: 10.1002/smll.202412217

Yuma Hirayama, Akira Miura, Motoaki Hirayama, Hiroyuki Nakamura, Koji Fujita, Hiroshi Kageyama, Sho Yamaguchi, Tomoo Mizugaki, Takato Mitsudome

{"title":"One-Step Low-Temperature Synthesis of Metastable ε-Iron Carbide Nanoparticles with Unique Catalytic Properties Beyond Conventional Iron Catalysts","authors":"Yuma Hirayama, Akira Miura, Motoaki Hirayama, Hiroyuki Nakamura, Koji Fujita, Hiroshi Kageyama, Sho Yamaguchi, Tomoo Mizugaki, Takato Mitsudome","doi":"10.1002/smll.202412217","DOIUrl":"https://doi.org/10.1002/smll.202412217","url":null,"abstract":"ε-Iron carbide has garnered increasing interest for its superior magnetic characteristics and catalytic performance compared to other iron carbides. However, its metastable nature has posed significant challenges for synthesis, often requiring ultrahigh pressure, multistep processes, complex reaction condition control, and highly toxic reagents. Consequently, the properties of ε-iron carbide remain largely unexplored. A simplified synthesis method for ε-iron carbide can accelerate the exploration of new functionalities. In this study, a novel one-step selective synthesis method for ε-iron carbide nanoparticles under mild conditions via a wet-chemical approach is presented. In this method, Fe3(CO)12, cetyltrimethylammonium bromide (CTAB), and bis(pinacolato)diboron (B2pin2) are added to hexadecylamine and reacted at 220 °C—a simple process that eliminates the need for extreme pressures and toxic substances. Detailed investigations elucidate the crucial roles of CTAB and B2pin2 in facilitating the selective formation of ε-iron carbide. This accessible and efficient synthesis process for ε-iron carbide can further enable the discovery of unprecedented catalytic properties in the reductive amination of benzaldehyde, distinct from those of conventional iron nanoparticle catalysts. Density functional theory calculations reveal insights into the electronic states responsible for the distinct activity of the ε-iron carbide nanoparticles.","PeriodicalId":228,"journal":{"name":"Small","volume":"72 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0