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A Biohybrid Nanoengine Powered Probiotics-Mediated Cancer Therapy 生物混合纳米引擎驱动的益生菌介导的癌症治疗
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202503629
Bin Luo, Yu Zhang, Jiadai Yi, Yue Sun, Junlin Ya, Yuxi Fang, Mengmeng Liu, Jinsong Ren, Xiaogang Qu
{"title":"A Biohybrid Nanoengine Powered Probiotics-Mediated Cancer Therapy","authors":"Bin Luo, Yu Zhang, Jiadai Yi, Yue Sun, Junlin Ya, Yuxi Fang, Mengmeng Liu, Jinsong Ren, Xiaogang Qu","doi":"10.1002/smll.202503629","DOIUrl":"https://doi.org/10.1002/smll.202503629","url":null,"abstract":"Although probiotics can modulate immune cell function and secrete antineoplastic metabolites, their clinical application is hindered by inherently poor motility and the accumulation of detrimental metabolites within the tumor microenvironment (TME). Herein, a biohybrid nanodevice is designed, which can serve as an adaptive “nano-engine” and “TME-regulator” by engineering clinically relevant probiotics. The <i>Lactobacillus reuteri</i> (<i>Lr</i>) can secrete anticancer compounds but is restricted by non-motility and detrimental metabolites, such as hydrogen peroxide and glutathione in the TME. These engineered probiotics with Janus structure are prepared by asymmetrically modifying <i>Lr</i> surfaces with PEGylated Fe/Co/Cu/W nanoparticles (Fcw) via electrostatic interactions. With catalase-like and S-nitrosoglutathione (GSNO)-degrading activity, Fcw enables the decomposition of hydrogen peroxide and GSNO to generate oxygen and nitric oxide, propelling <i>Lr</i> to overcome complex biological barriers while reducing local hydrogen peroxide levels to enhance <i>Lr</i> survival. Importantly, Fcw with glutathione peroxidase-like activity can enhance the oxidative stress induced by <i>Lr</i>, thereby improving the anticancer activity of probiotics. Therefore, the design can not only enhance the <i>Lr</i> motility to increase tumor infiltration but also modulate the TME to improve probiotic viability and efficiency. This method can also be adopted for other probiotics and will certainly promote the design of nanoengine-powered probiotics-mediated therapy.","PeriodicalId":228,"journal":{"name":"Small","volume":"69 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177179","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
Cold-Adaptive Haloperoxidase-Mimicking Copper-Dipeptide Hybrid Nanoparticle for Antibiofilm Formation 模拟冷适应卤素过氧化物酶的铜-二肽杂化纳米颗粒用于抗生素膜的形成
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202502509
Yongfang Zheng, Lisha Feng, Yuyuan Chen, Xinyu Zhu, Shuli Tian, Jianbin Ye, Hu Zhu
{"title":"Cold-Adaptive Haloperoxidase-Mimicking Copper-Dipeptide Hybrid Nanoparticle for Antibiofilm Formation","authors":"Yongfang Zheng, Lisha Feng, Yuyuan Chen, Xinyu Zhu, Shuli Tian, Jianbin Ye, Hu Zhu","doi":"10.1002/smll.202502509","DOIUrl":"https://doi.org/10.1002/smll.202502509","url":null,"abstract":"Marine biofouling causes significant economic and environmental challenges. Inspired by marine algae's natural defense through haloperoxidase (HPO) secretion, researchers have developed HPO mimics as effective antifouling agents. However, their application in marine environments is limited by the scarcity of HPO mimics, their preference for acidic conditions, and the complexity of their synthesis. The study introduces a novel HPO mimic, HH-Cu, synthesized through a one-step precipitation reaction by mixing copper ions and dipeptides in phosphate-buffered saline. HH-Cu exhibits exceptional stability under extreme conditions, including varying pH levels, high temperatures, various interfering substances, and long-term storage. It maintains 90% of its activity even after ten uses. Notably, it exhibits high activity under neutral and alkaline conditions, with optimal HPO-like activity at pH 8, which coincides with the pH range of seawater (pH 7.8–8.2). Leveraging its strong HPO-like activity, HH-Cu exhibits significant antibacterial effects and biofilm inhibition. Importantly, HH-Cu is wide-temperature adaptive (0-50 °C), displaying substantial HPO-like activity and antibacterial properties even at temperatures as low as 0 °C. This is the first example of a HPO mimic with low-temperature adaptability. The study not only broadens the range of HPO mimics but also highlights the potential of HH-Cu in biofouling treatment.","PeriodicalId":228,"journal":{"name":"Small","volume":"14 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177177","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
Light‐Actuated, Tunable Micromachines from Photo‐Swellable Colloidal Ionogels 光致动、可调谐的微机械,由光可膨胀的胶体电离胶制成
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202503698
Dezhou Cao, Jingru Xu, Dongqing He, Mohd Yasir Khan, Xing Ma, Wei Wang
{"title":"Light‐Actuated, Tunable Micromachines from Photo‐Swellable Colloidal Ionogels","authors":"Dezhou Cao, Jingru Xu, Dongqing He, Mohd Yasir Khan, Xing Ma, Wei Wang","doi":"10.1002/smll.202503698","DOIUrl":"https://doi.org/10.1002/smll.202503698","url":null,"abstract":"Active colloids that release ions hold potential for building micromachines capable of dynamically responding to environmental stimuli. Harnessing light to precisely regulate and fine‐tune their performance is essential for unlocking their versatility and expanding their range of applications. To address this challenge, light‐actuated, tunable micromachines are developed based on photo‐swellable colloidal ionogels—an azobenzene‐modified co‐polymer microsphere infused with azobenzene‐based ionic liquids (Azo‐ILs)—that undergo reversible cis‐trans isomerization under UV/visible light. UV irradiation increases the colloidal ionogel's hydrophilicity and causes it to swell by H<jats:sub>2</jats:sub>O, releasing Azo‐ILs into aqueous environments with a rapid photoresponse (milliseconds), while visible light irradiation stops the swelling. The dissociated ions lead to diffusiophoresis and diffusioosmosis, enabling two functionalities: isotropic ion release from the ionogel pumps water outward with exclusion zones up to 30 µm, while anisotropic release from partially coated ionogel microspheres leads to micromotors at speeds of ≈3 µm s<jats:sup>−1</jats:sup> and a lifetime of ≈15 min. Importantly, the magnitude and range of these interactions are precisely modulated by light intensity and azobenzene content in co‐polymers. Finite element and Brownian dynamics simulations validate the electrokinetic mechanisms underlying the pump and motor's operation. This work establishes a platform for designing micromachines potentially useful in fluid manipulation, drug delivery, and soft robotics.","PeriodicalId":228,"journal":{"name":"Small","volume":"13 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176537","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
Electrodeposited ZnO/Zn(OH)2 Nanosheets as a Functional Interface for Dendrite-Free Lithium Metal Anodes 电沉积ZnO/Zn(OH)2纳米片作为无枝晶锂金属阳极的功能界面
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202503607
Da-Eun Hyun, Jong Chan Choi, Yoon Ho Kim, Yejin Ra, Jae Sol Sim, Jung-Kul Lee, Yun Chan Kang
{"title":"Electrodeposited ZnO/Zn(OH)2 Nanosheets as a Functional Interface for Dendrite-Free Lithium Metal Anodes","authors":"Da-Eun Hyun, Jong Chan Choi, Yoon Ho Kim, Yejin Ra, Jae Sol Sim, Jung-Kul Lee, Yun Chan Kang","doi":"10.1002/smll.202503607","DOIUrl":"https://doi.org/10.1002/smll.202503607","url":null,"abstract":"Modifying the current collector is a promising strategy to enable Li metal anodes with minimal Li consumption. Herein, a scalable electrodeposition method is introduced to construct 3D ZnO/Zn(OH)<sub>2</sub> nanosheets on Cu foil (ZOH NSs–Cu foil). Cu(OH)<sub>2</sub> nanowires are first formed via anodization, followed by electroconversion of Cu<sup>2+</sup> and Zn<sup>2+</sup> ions. DFT calculations reveal that the ZOH NSs–Cu foil exhibits high Li adsorption energy, imparting strong lithiophilicity and lowering the Li nucleation overpotential. The 3D nanosheet structure provides a large electrochemically active surface, reducing the effective current density. Furthermore, ZOH NSs–Cu foil exhibits low charge transfer resistance and promotes a Li<sub>2</sub>O/LiF-rich solid electrolyte interphase (SEI) layer, further reducing interfacial resistance. SEM analysis and simulations confirm uniform Li deposition on ZOH NSs–Cu foil. In asymmetric cells (1 mAh cm<sup>−2</sup> at 1 mA cm<sup>−2</sup>), ZOH NSs–Cu foil supports stable cycling for over 400 cycles. Furthermore, a full cell coupling a LiFePO<sub>4</sub> (LFP) cathode with a Li@ZOH NSs–Cu foil anode retains high capacity with ≈100% Coulombic efficiency over 350 cycles at 1 C, even at an N/P ratio of ≈1.9. This binder-free, scalable approach offers precise Li deposition control and excellent electrochemical performance, advancing the practical application of Li metal anodes.","PeriodicalId":228,"journal":{"name":"Small","volume":"70 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177143","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
Plasmonic Polymorphs by Combining Shape Anisotropy and Soft Interactions in Bipyramid Thin Films 双棱锥薄膜中结合形状各向异性和软相互作用的等离子体多晶型
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202500389
Jules Marcone, Sabrina Juergensen, Juan Barrios-Capuchino, Xiaoyian Li, Claire Goldmann, Andrea Köppen, Winnie Pfeiffer, Felix Lehmkühler, Wolfgang J. Parak, Mathieu Kociak, Marianne Impéror-Clerc, Stephanie Reich, Cyrille Hamon, Florian Schulz
{"title":"Plasmonic Polymorphs by Combining Shape Anisotropy and Soft Interactions in Bipyramid Thin Films","authors":"Jules Marcone, Sabrina Juergensen, Juan Barrios-Capuchino, Xiaoyian Li, Claire Goldmann, Andrea Köppen, Winnie Pfeiffer, Felix Lehmkühler, Wolfgang J. Parak, Mathieu Kociak, Marianne Impéror-Clerc, Stephanie Reich, Cyrille Hamon, Florian Schulz","doi":"10.1002/smll.202500389","DOIUrl":"https://doi.org/10.1002/smll.202500389","url":null,"abstract":"Thin-film plasmonic supercrystals of pentagonal gold nanobipyramids (AuBP) exhibit a diverse range of packing structures that influence the near-field distribution of the enhanced electric field and the far-field response. By varying the molecular weight of the coating ligands, the softness of the anisotropic building blocks is changed. A thorough structural characterization reveals that this affects the resulting superstructures from self-assembly more intricately than with isotropic building blocks. Softer coatings lead to smaller aligned domains in monolayers, while bilayers exhibit more crystalline domains with dominant interlayer twist angles near 0° and 90°. The far-field distribution and near-field response are measured using micro-absorbance and electron energy loss spectroscopy (EELS). Correlating these data with high-resolution transmission electron microscopy (HR-TEM) structural analysis enabled the identification of the longitudinal and transverse individual and collective plasmonic modes. Notably, for large crystalline bilayer domains, a strong polarization-dependent optical response is observed. These features underline the potential of these superstructures for applications in surface-enhanced spectroscopies, plasmonic photocatalysis, and advanced optical manipulation in switchable optical metamaterials.","PeriodicalId":228,"journal":{"name":"Small","volume":"16 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177176","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
Augmented Thermoelectric in-Plane Power Factor of 0.8 mW M∙K−2 in Solution-Processed 2D MoS2 at Room-Temperature by Current Confinement 室温下溶液处理的二维二硫化钼中0.8 mW M∙K−2的平面热电功率因数
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202502374
Jung-Min Cho, Hyeok Jun Kwon, Won-Yong Lee, Myeongjin Jung, Jiwon Hong, Jae Won Choi, Yun Ho Kim, No-Won Park, Min-Sung Kang, Gil-Sung Kim, Young-Gui Yoon, Joohoon Kang, Sang-Kwon Lee
{"title":"Augmented Thermoelectric in-Plane Power Factor of 0.8 mW M∙K−2 in Solution-Processed 2D MoS2 at Room-Temperature by Current Confinement","authors":"Jung-Min Cho, Hyeok Jun Kwon, Won-Yong Lee, Myeongjin Jung, Jiwon Hong, Jae Won Choi, Yun Ho Kim, No-Won Park, Min-Sung Kang, Gil-Sung Kim, Young-Gui Yoon, Joohoon Kang, Sang-Kwon Lee","doi":"10.1002/smll.202502374","DOIUrl":"https://doi.org/10.1002/smll.202502374","url":null,"abstract":"In the past decade, 2D transition metal dichalcogenides (TMDCs) have gained significant attention as energy materials because of their unique structure and promising properties. Specifically, TMDC-based thermoelectric (TE) power generation has emerged as a sustainable solution to produce electricity using waste heat. However, the dimensional requirement of TMDC thin films for device utilization and their low electrical conductivity have constrained their in-plane TE properties. Here, the TE properties, including the Seebeck coefficient and power factor of solution-processed MoS<sub>2</sub> films, which are chemically exfoliated and processed by spin-coating are presented, and report an innovative approach to increase the in-plane TE power factor by simple Pt-coating of the exfoliated MoS<sub>2</sub> films. These films exhibit a high TE power factor of ≈810 µW m·K<sup>2</sup> at 300 K — an increase of more than 9200% compared with that of a restacked MoS<sub>2</sub> thin film with the same thickness. Our study indicates that the free carriers in the top-Pt layer carry and transfer the thermally-induced heat current accumulated at the interface between the Pt and MoS<sub>2</sub> layers under a temperature gradient applied along the samples. This distinctive approach to enhancing the TE power factor provides an effective strategy for high-performance TMDC-based TE energy generating devices.","PeriodicalId":228,"journal":{"name":"Small","volume":"41 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177323","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
Selective Electrochemical CO2-to-Syngas Conversion Enabled by Electronic-Structure-Modulated Copper-Zinc Alloy Nanosheets 电子结构调制铜锌合金纳米片实现co2到合成气的选择性电化学转换
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202501030
Ruyu Zou, Rui Luo, Fanghuang Liu, Yan Wang, Muhammad Sohail Riaz, Shuling Shen, Guangzhi Yang, Zhihong Tang, Hengbo Huang, Guisheng Li, Qingyuan Bi
{"title":"Selective Electrochemical CO2-to-Syngas Conversion Enabled by Electronic-Structure-Modulated Copper-Zinc Alloy Nanosheets","authors":"Ruyu Zou, Rui Luo, Fanghuang Liu, Yan Wang, Muhammad Sohail Riaz, Shuling Shen, Guangzhi Yang, Zhihong Tang, Hengbo Huang, Guisheng Li, Qingyuan Bi","doi":"10.1002/smll.202501030","DOIUrl":"https://doi.org/10.1002/smll.202501030","url":null,"abstract":"Developing cost-effective materials for efficient selective electrochemical CO<sub>2</sub>-to-syngas under actionable conditions is a practical and promising way to sustain low-carbon energy supplies, which remains a significant challenge. Herein, the efficient CuZn alloy nanosheets with prominent electronic structure modulation and alloy effect and the active CuZn<sub>5</sub> phase are successfully fabricated by the facile electrodeposition strategy are reported. The electronic synergy via electron transferring from Zn to Cu can influence the catalyst's surface electron density and thus regulate the chemical adsorption properties of both small molecules and the key step of C═O bond cleavage. Significantly, the engineered Cu<sub>0.07 </sub>Zn alloy catalyst achieves an outstanding electrochemical CO<sub>2</sub>-to-syngas conversion, accompanying Faraday efficiency of near 100% and a high production rate of syngas with tunable CO/H<sub>2</sub> ratio of 1.1 to 4.3 over a wide potential range of −0.65 to −1.25 V as well as excellent stability in CO<sub>2</sub>-saturated 0.1 <span>m</span> KHCO<sub>3</sub> system. Moreover, the comprehensive understanding of the alloy phase evolution, electronic structure modulation, structure-activity relationship, and possible CO<sub>2</sub>-to-syngas conversion mechanism involving the rate-determining step of C═O bond breakage to <sup>*</sup>CO species over the versatile CuZn alloy catalyst via theoretical calculations and in situ spectroscopy is demonstrated.","PeriodicalId":228,"journal":{"name":"Small","volume":"176 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177175","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
A Facile Coordination Polymer Nanoparticle for Sonodynamic Therapy Combating Drug-Resistant Bacteria 一种用于声动力治疗耐药细菌的易配位聚合物纳米颗粒
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202501131
Xianhui Song, Jie Li, Siyuan Huang, Yufei Zhang, Shihao Hong, Xinge Zhang
{"title":"A Facile Coordination Polymer Nanoparticle for Sonodynamic Therapy Combating Drug-Resistant Bacteria","authors":"Xianhui Song, Jie Li, Siyuan Huang, Yufei Zhang, Shihao Hong, Xinge Zhang","doi":"10.1002/smll.202501131","DOIUrl":"https://doi.org/10.1002/smll.202501131","url":null,"abstract":"The emergence of drug resistance in bacteria, along with the protective nature and intricate environment of biofilms, impedes the effective treatment of severe bacterial infections, posing significant health risks. Herein, a coordination polymer nanoparticle (LZC) is fabricated via a facile in situ strategy for sonodynamic therapy (SDT) combating drug-resistant bacteria-induced infections. By conjugating the Food and Drug Administration (FDA)-approved safe sonosensitizer porphyrin chlorin e6 (Ce6) with a positively charged antimicrobial peptide LL37 through coordination interaction, the resultant LZC exhibits uniform size and a positively charged surface, which is beneficial for the efficient capture of bacteria and improved nanoparticle penetration into biofilms. Under ultrasound (US) stimuli, the nanoparticle generates a higher reactive oxygen species (ROS) compared with the free sonosensitizers, as well as the production of heat, leading to bacterial cell death and biofilm disruption. In vitro evaluations reveal the robust antibacterial activity of LZC, achieving up to 99% eradication of multi-drug resistant <i>Pseudomonas aeruginosa</i> (MDRPA) and significant biofilm eradication under deep-penetrating US irradiation. Moreover, the establishment of coordination polymer nanoparticles represents an innovative strategy to enhance SDT in an MDRPA-induced-pneumonia mice model and provides a great promise for advancing therapeutic interventions in deep tissue bacterial infections.","PeriodicalId":228,"journal":{"name":"Small","volume":"29 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177178","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
Oxygen Reduction Intermediates-Mediated Electron Transport in Single-Molecule Junctions 单分子结中氧还原中间体介导的电子传递
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202503254
Bo Wang, Hong-Yang Guo, Yue-Tong Sun, Qiang Wan, Yongchun Fu, Ju-Fang Zheng, Yong Shao, Emmanuel Maisonhaute, Ya-Hao Wang, Xiao-Shun Zhou
{"title":"Oxygen Reduction Intermediates-Mediated Electron Transport in Single-Molecule Junctions","authors":"Bo Wang, Hong-Yang Guo, Yue-Tong Sun, Qiang Wan, Yongchun Fu, Ju-Fang Zheng, Yong Shao, Emmanuel Maisonhaute, Ya-Hao Wang, Xiao-Shun Zhou","doi":"10.1002/smll.202503254","DOIUrl":"https://doi.org/10.1002/smll.202503254","url":null,"abstract":"Single-molecule electrical measurements have recently emerged as a unique platform for exploring single-molecule physical chemistry and reaction processes. Herein, the electrochemical technique has been first for exploring oxygen reduction reaction (ORR) in single-molecule junctions of iron porphyrins modified with pyridine groups (Fe-TPyP). Single-molecule conductance measurements in O<sub>2</sub>-saturated solutions clearly show that the FeTPyP binds to O<sub>2</sub> to form the ferric-superoxide porphyrin complex ((Fe-O<sub>2</sub><sup>• −</sup>)-TPyP) and form the intermediate molecular junctions. This is further supported by the observed molecular evidence of Fe─O and FeO─O stretching vibrations of (Fe-O<sub>2</sub><sup>• −</sup>)-TPyP during in situ Raman and ex situ electron paramagnetic resonance (EPR) experiments. DFT calculations also reveal that the potential determining step in ORR is the protonation of (Fe-O<sub>2</sub><sup>• −</sup>)-TPyP, resulting in the highest probability for forming Au-(Fe-O<sub>2</sub><sup>• −</sup>)-TPyP-Au junctions during the ORR process. This work reveals the impact of ORR on electron transport in single-molecule junctions and provides a new way to explore the electrocatalytic processes of molecular catalysts at a single-molecule level by using the break junction method.","PeriodicalId":228,"journal":{"name":"Small","volume":"58 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177141","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
Dual-Ion Directed Synergistic Doping for Regulating Film Crystallization and Carrier Dynamics in High-Efficiency Antimony Selenosulfide Thin-Film Solar Cells 双离子定向协同掺杂调控高效硒化锑薄膜太阳能电池的薄膜结晶和载流子动力学
IF 13.3 2区 材料科学
Small Pub Date : 2025-05-30 DOI: 10.1002/smll.202501748
Kangjun Geng, Junjie Dong, Bangzhi Shen, Boning Dong, Jingling Zhang, Huliang Zhuang, Jingjing Liu, Xiulin Jiang, LvZhou Li, Shuai Zhang, Ding Gu, Sai Jiang, Jianhua Qiu, Huafei Guo, Ningyi Yuan, Jianning Ding
{"title":"Dual-Ion Directed Synergistic Doping for Regulating Film Crystallization and Carrier Dynamics in High-Efficiency Antimony Selenosulfide Thin-Film Solar Cells","authors":"Kangjun Geng, Junjie Dong, Bangzhi Shen, Boning Dong, Jingling Zhang, Huliang Zhuang, Jingjing Liu, Xiulin Jiang, LvZhou Li, Shuai Zhang, Ding Gu, Sai Jiang, Jianhua Qiu, Huafei Guo, Ningyi Yuan, Jianning Ding","doi":"10.1002/smll.202501748","DOIUrl":"https://doi.org/10.1002/smll.202501748","url":null,"abstract":"Antimony selenosulfide (Sb<sub>2</sub>(S,Se)<sub>3</sub>) has attracted significant attention in photovoltaic applications due to its excellent optoelectronic properties. However, despite the recent progress, the efficiency of Sb<sub>2</sub>(S,Se)<sub>3</sub> thin-film solar cells remains significantly lower than the theoretical limit. Reducing carrier recombination and enhancing crystal orientation-induced carrier transport is crucial to further improving device performance. In this study, a novel dual-ion synergistic regulation strategy based on interface passivation layer soaking modification is employed to enhance the crystallization and crystal orientation of Sb<sub>2</sub>(S,Se)<sub>3</sub> thin films. The results demonstrate that soaking and modifying the aluminum oxide (Al<sub>2</sub>O<sub>3</sub>) interfacial layer with a sodium hydroxide (NaOH) solution effectively reduces the oxygen content on the cadmium sulfide (CdS) surface, thereby suppressing oxygen-induced [<i>hk</i>0] crystal orientation growth in Sb<sub>2</sub>(S,Se)<sub>3</sub> thin films. Moreover, for the first time, this study reveals that the synergistic doping of Na and Al ions regulates the crystallization kinetics of Sb<sub>2</sub>(S,Se)<sub>3</sub>, leading to improve carrier transport, reduce deep-level defect density, and optimize band structure, ultimately suppressing carrier recombination. As a result, a Sb<sub>2</sub>(S,Se)<sub>3</sub> thin-film solar cell with an efficiency of 9.79% is achieved under this dual-ion synergistic regulation strategy.","PeriodicalId":228,"journal":{"name":"Small","volume":"27 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144177142","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
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