Xifeng Zhang, Bilan Wang, Xin Qi, Zhiyong Qian, Xiang Gao, Yongzhong Cheng, Xiang Wang
Glioblastoma represents a highly aggressive form of malignant tumor within the central nervous system. Although chemotherapy remains the primary therapeutic strategy, its efficacy is often limited. To overcome the limitations associated with chemotherapeutic agents, such as high toxicity and non-specific adverse effects, a novel nanoparticle system comprising cRGD-modified and glutathione (GSH)-responsive polymers, and PEG-ss-Dox and apatinib (AP) (PDOX-AP/cRGD-NPs) is developed. PDOX-AP/cRGD-NPs show effective penetration of the blood-brain barrier (BBB), facilitate targeted delivery to brain tumors, and exhibit controlled drug release. PDOX-AP/cRGD-NPs show more effect in reducing the viability of GL-261, U87-MG, and LN-229 cells, inhibiting clonogenicity, and suppressing anti-apoptotic protein expression than PDOX/cRGD-NPs or AP/cRGD-NPs. Additionally, PDOX-AP/cRGD-NPs substantially increase drug uptake, BBB penetration, apoptosis rates, and the proportion of cells in the G2 phase. In vivo experiments further reveal that cRGD-directed nanoparticles exhibit superior accumulation in glioma regions compared to their non-cRGD-modified counterparts. In the interim, PDOX-AP/cRGD-NPs demonstrate significant efficacy in suppressing both ectopic and orthotopic growth of GL-261 gliomas, as well as orthotopic LN-229 gliomas, thereby markedly extending the median survival duration. This study introduces a promising targeted co-delivery system for combination chemotherapy.
{"title":"A Glutathione-Responsive System with Prodrug and Sensitization Strategies for Targeted Therapy of Glioma","authors":"Xifeng Zhang, Bilan Wang, Xin Qi, Zhiyong Qian, Xiang Gao, Yongzhong Cheng, Xiang Wang","doi":"10.1002/smll.202501620","DOIUrl":"https://doi.org/10.1002/smll.202501620","url":null,"abstract":"Glioblastoma represents a highly aggressive form of malignant tumor within the central nervous system. Although chemotherapy remains the primary therapeutic strategy, its efficacy is often limited. To overcome the limitations associated with chemotherapeutic agents, such as high toxicity and non-specific adverse effects, a novel nanoparticle system comprising cRGD-modified and glutathione (GSH)-responsive polymers, and PEG-ss-Dox and apatinib (AP) (PDOX-AP/cRGD-NPs) is developed. PDOX-AP/cRGD-NPs show effective penetration of the blood-brain barrier (BBB), facilitate targeted delivery to brain tumors, and exhibit controlled drug release. PDOX-AP/cRGD-NPs show more effect in reducing the viability of GL-261, U87-MG, and LN-229 cells, inhibiting clonogenicity, and suppressing anti-apoptotic protein expression than PDOX/cRGD-NPs or AP/cRGD-NPs. Additionally, PDOX-AP/cRGD-NPs substantially increase drug uptake, BBB penetration, apoptosis rates, and the proportion of cells in the G2 phase. In vivo experiments further reveal that cRGD-directed nanoparticles exhibit superior accumulation in glioma regions compared to their non-cRGD-modified counterparts. In the interim, PDOX-AP/cRGD-NPs demonstrate significant efficacy in suppressing both ectopic and orthotopic growth of GL-261 gliomas, as well as orthotopic LN-229 gliomas, thereby markedly extending the median survival duration. This study introduces a promising targeted co-delivery system for combination chemotherapy.","PeriodicalId":228,"journal":{"name":"Small","volume":"55 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672635","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}
Min Zhang, Yongshun Song, Jun Wang, Xinlei Shi, Qiang Chen, Rui Ding, Junjie Mou, Haiping Fang, Yunlong Zhou, Ruoyang Chen
The biological effects of magnetic fields are pervasive in microorganisms, with significant attention given to alternating magnetic fields (AMFs). However, AMFs induce electrical and magnetothermal effects, which complicate the interpretation of magnetic field-induced biological effects and introduce uncertainties regarding cytotoxicity in practical applications. The static magnetic field (SMF) with few variables and high biocompatibility presents a promising alternative for both understanding biological mechanisms and ensuring safe applications, but has a remaining problem on weak interactions with microorganisms. Here we show that the combination of SMF with paramagnetic calcium-polypyrrole nanoparticles (Ca-PPy) remarkably enhances bactericidal activity. Our experiments indicate that the synergistic action of SMF and Ca-PPy significantly promotes the generation of reactive oxygen species (ROS), i.e., singlet oxygen and superoxide anion radicals, in Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), coupled with the physical disruption of bacterial membrane, exhibiting the extraordinary bactericidal performance (the bactericidal rate is over 94%). The mechanism disclosed by computations is that the singlet-to-triplet transition of radical pairs can be increased by the introduction of magnetic fields. These findings offer new insights into the biological effects of magnetic fields and pave the way for their safe, highly effective use in bactericidal applications.
{"title":"Enhancement Effect of Static Magnetic Field on Bactericidal Activity","authors":"Min Zhang, Yongshun Song, Jun Wang, Xinlei Shi, Qiang Chen, Rui Ding, Junjie Mou, Haiping Fang, Yunlong Zhou, Ruoyang Chen","doi":"10.1002/smll.202412334","DOIUrl":"https://doi.org/10.1002/smll.202412334","url":null,"abstract":"The biological effects of magnetic fields are pervasive in microorganisms, with significant attention given to alternating magnetic fields (AMFs). However, AMFs induce electrical and magnetothermal effects, which complicate the interpretation of magnetic field-induced biological effects and introduce uncertainties regarding cytotoxicity in practical applications. The static magnetic field (SMF) with few variables and high biocompatibility presents a promising alternative for both understanding biological mechanisms and ensuring safe applications, but has a remaining problem on weak interactions with microorganisms. Here we show that the combination of SMF with paramagnetic calcium-polypyrrole nanoparticles (Ca-PPy) remarkably enhances bactericidal activity. Our experiments indicate that the synergistic action of SMF and Ca-PPy significantly promotes the generation of reactive oxygen species (ROS), i.e., singlet oxygen and superoxide anion radicals, in <i>Escherichia coli</i> (<i>E. coli</i>) and <i>Staphylococcus aureus</i> (<i>S. aureus</i>), coupled with the physical disruption of bacterial membrane, exhibiting the extraordinary bactericidal performance (the bactericidal rate is over 94%). The mechanism disclosed by computations is that the singlet-to-triplet transition of radical pairs can be increased by the introduction of magnetic fields. These findings offer new insights into the biological effects of magnetic fields and pave the way for their safe, highly effective use in bactericidal applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"17 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672636","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}
The application of self-assembled monolayers (SAMs) as hole-transporting materials has greatly improved the performance of inverted perovskite solar cells. Structure engineering of SAMs has proven to be an effective approach to enhance device performance. In this work, a novel SAM featuring extended conjugation is designed and synthesized, designated E-CbzBT. Compared with CbzBT, E-CbzBT exhibits enhanced asymmetric and noncoplanar screw-shaped configuration, leading to uniform and tight packing on ITO. The uniform packing of E-CbzBT increases the wettability of the perovskite precursor solution on the substrate, thereby facilitating perovskite crystallinity and suppressing interfacial trap density more effectively than CbzBT. Accordingly, inverted PSCs employing E-CbzBT reach a champion power conversion efficiency of 25.15%, surpassing 24.06% for CbzBT-based devices. Importantly, the E-CbzBT-based PSCs demonstrate superior ambient and thermal stability. The extending conjugation approach in SAMs represents a promising avenue for further advancements in perovskite solar cell technology.
{"title":"A Novel Self-Assembled Hole-Transporting Monolayer with Extending Conjugation for Inverted Perovskite Solar Cells","authors":"Qian Wang, Botong Li, Hanqin Yang, Zongxu Na, Yijin Wei, Xuepeng Liu, Mingyuan Han, Xianfu Zhang, Weilun Du, Ghadari Rahim, Yong Ding, Zhipeng Shao, Huai Yang, Songyuan Dai","doi":"10.1002/smll.202500296","DOIUrl":"https://doi.org/10.1002/smll.202500296","url":null,"abstract":"The application of self-assembled monolayers (SAMs) as hole-transporting materials has greatly improved the performance of inverted perovskite solar cells. Structure engineering of SAMs has proven to be an effective approach to enhance device performance. In this work, a novel SAM featuring extended conjugation is designed and synthesized, designated E-CbzBT. Compared with CbzBT, E-CbzBT exhibits enhanced asymmetric and noncoplanar screw-shaped configuration, leading to uniform and tight packing on ITO. The uniform packing of E-CbzBT increases the wettability of the perovskite precursor solution on the substrate, thereby facilitating perovskite crystallinity and suppressing interfacial trap density more effectively than CbzBT. Accordingly, inverted PSCs employing E-CbzBT reach a champion power conversion efficiency of 25.15%, surpassing 24.06% for CbzBT-based devices. Importantly, the E-CbzBT-based PSCs demonstrate superior ambient and thermal stability. The extending conjugation approach in SAMs represents a promising avenue for further advancements in perovskite solar cell technology.","PeriodicalId":228,"journal":{"name":"Small","volume":"61 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672637","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}
Zhongwei Zhao, Bingshu Guo, Yun Huang, Xichang Wang, Jin Bao, Chunmei Feng, Xing Li, Mingshan Wang, Yuanhua Lin, Haijun Cao
Aqueous zinc-ion batteries (AZIB) are significantly constrained by the poor stability of Zn anodes in aqueous electrolytes, which is caused by uncontrollable deposition behavior and parasitic reactions. The construction of specific crystalline surfaces represents an effective method for stabilizing Zn anodes. Therefore, a stable Malic acid@Zn (MA@Zn) anode with a highly (101) texture configuration is developed through acid etching. The mechanism of MA selective etching is investigated through theoretical calculations, where Zn atoms detach from the (002) crystal surface due to the strong interaction of MA with the (002) surface, leading to the preferential corrosion of the (002) surface and the formation of a unique (101) texture configuration morphology. This texture is conducive to the MA@Zn anode, as it enhances the affinity of MA@Zn for Zn2+ and optimizes the electric field distribution on the surface, thereby facilitating a more stable Zn deposition. Consequently, the MA@Zn symmetric battery is subjected to stable cycling for a period exceeding 2400 h at a current density of 5 mA cm−2. In comparison, the cycle life of the Zn//V2O5 full battery is significantly improved by >6000 cycles, pouch battery also shows better performance.
{"title":"Selective Acid Etching Construction of High (101) Texture Zinc Metal Anodes for High-Performance Zinc Ion Batteries","authors":"Zhongwei Zhao, Bingshu Guo, Yun Huang, Xichang Wang, Jin Bao, Chunmei Feng, Xing Li, Mingshan Wang, Yuanhua Lin, Haijun Cao","doi":"10.1002/smll.202501569","DOIUrl":"https://doi.org/10.1002/smll.202501569","url":null,"abstract":"Aqueous zinc-ion batteries (AZIB) are significantly constrained by the poor stability of Zn anodes in aqueous electrolytes, which is caused by uncontrollable deposition behavior and parasitic reactions. The construction of specific crystalline surfaces represents an effective method for stabilizing Zn anodes. Therefore, a stable Malic acid@Zn (MA@Zn) anode with a highly (101) texture configuration is developed through acid etching. The mechanism of MA selective etching is investigated through theoretical calculations, where Zn atoms detach from the (002) crystal surface due to the strong interaction of MA with the (002) surface, leading to the preferential corrosion of the (002) surface and the formation of a unique (101) texture configuration morphology. This texture is conducive to the MA@Zn anode, as it enhances the affinity of MA@Zn for Zn<sup>2+</sup> and optimizes the electric field distribution on the surface, thereby facilitating a more stable Zn deposition. Consequently, the MA@Zn symmetric battery is subjected to stable cycling for a period exceeding 2400 h at a current density of 5 mA cm<sup>−2</sup>. In comparison, the cycle life of the Zn//V<sub>2</sub>O<sub>5</sub> full battery is significantly improved by >6000 cycles, pouch battery also shows better performance.","PeriodicalId":228,"journal":{"name":"Small","volume":"37 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666507","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}
Qianwei Liu, Xinhong Xiong, Yuanlai Fang, Jiaxi Cui
Inspired by the actin-myosin-mediated growth mechanisms in skeletal muscle, cyclic crystallization is employed to induce hydrogel self-growth. Using polyacrylamide-sodium acetate (PAM-NaAc) hydrogel as a model system, the crystallization of NaAc triggers the stretching and subsequent fracture of polymer chains, generating mechanoradicals at strain-concentrated regions. These reactive species facilitate the incorporation of polymerizable compounds (monomers and crosslinkers). Specifically, localized polymerization of poly(ethylene glycol) diacrylate (PEGDA) monomers occurs at fracture sites, leading to covalent network integration and achieving a 51.5-fold Young's modulus enhancement (from 0.024 to 1.24 MPa over 50 crystallization cycles). This crystallization-induced self-growth mechanism enables programmable topology engineering in soft matter systems, with implications for adaptive biomedical implants and fatigue-resistant soft robots.
{"title":"Crystallization-Induced Network Growth for Enhancing Hydrogel Mechanical Properties","authors":"Qianwei Liu, Xinhong Xiong, Yuanlai Fang, Jiaxi Cui","doi":"10.1002/smll.202500976","DOIUrl":"https://doi.org/10.1002/smll.202500976","url":null,"abstract":"Inspired by the actin-myosin-mediated growth mechanisms in skeletal muscle, cyclic crystallization is employed to induce hydrogel self-growth. Using polyacrylamide-sodium acetate (PAM-NaAc) hydrogel as a model system, the crystallization of NaAc triggers the stretching and subsequent fracture of polymer chains, generating mechanoradicals at strain-concentrated regions. These reactive species facilitate the incorporation of polymerizable compounds (monomers and crosslinkers). Specifically, localized polymerization of poly(ethylene glycol) diacrylate (PEGDA) monomers occurs at fracture sites, leading to covalent network integration and achieving a 51.5-fold Young's modulus enhancement (from 0.024 to 1.24 MPa over 50 crystallization cycles). This crystallization-induced self-growth mechanism enables programmable topology engineering in soft matter systems, with implications for adaptive biomedical implants and fatigue-resistant soft robots.","PeriodicalId":228,"journal":{"name":"Small","volume":"1 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666509","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}
Sungwon Jung, Young Gyun Choi, Bumgyu Choi, Sung-eun Heo, Tae Suk Jun, Kyungtae Park, Sohyeon Park, Du Yeol Ryu, Jong Hyeok Park, Jinkee Hong
Water-based electrolytes provide safe, reliable, and cost-effective energy storage solutions; however, their application in aqueous lithium-ion batteries is hindered by low energy density and short cycling life due to the limited electrochemical stability window. While high lithium salt concentrations can mitigate some of these issues, they often lead to increased solvent viscosity and higher costs, limiting commercialization. In this study, a boron-stabilized anisotropic polyvinyl alcohol (PVA) hydrogel electrolyte, referred to as BaP, is proposed to address the challenges related to high lithium salt (LiTFSI) concentrations. Due to the Hofmeister effect, the BaP water-in-polymer electrolyte can retain a high concentration of lithium salt even when low concentrations of lithium salt are used. Briefly, the BaP promotes the salting-in phenomenon of Li ions, while the TFSI ions induce salting-out, allowing BaP to synergistically achieve high lithium salt concentrations. Due to these unique characteristics, the BaP hydrogel exhibits a wide electrochemical stability window similar to that of highly concentrated electrolytes, enabling stable operation in a LiMn2O4||Li4Ti5O12 full cell by suppressing hydrogen evolution. Moreover, the biodegradability of BaP contributes to the development of a more environmentally friendly battery system.
{"title":"Boron-Stabilized Anisotropic Water-in-Polymer Salt Electrolyte with an Exceptionally Low Salt Concentration by Hofmeister Effect for Aqueous Lithium-Ion Batteries","authors":"Sungwon Jung, Young Gyun Choi, Bumgyu Choi, Sung-eun Heo, Tae Suk Jun, Kyungtae Park, Sohyeon Park, Du Yeol Ryu, Jong Hyeok Park, Jinkee Hong","doi":"10.1002/smll.202502776","DOIUrl":"https://doi.org/10.1002/smll.202502776","url":null,"abstract":"Water-based electrolytes provide safe, reliable, and cost-effective energy storage solutions; however, their application in aqueous lithium-ion batteries is hindered by low energy density and short cycling life due to the limited electrochemical stability window. While high lithium salt concentrations can mitigate some of these issues, they often lead to increased solvent viscosity and higher costs, limiting commercialization. In this study, a boron-stabilized anisotropic polyvinyl alcohol (PVA) hydrogel electrolyte, referred to as BaP, is proposed to address the challenges related to high lithium salt (LiTFSI) concentrations. Due to the Hofmeister effect, the BaP water-in-polymer electrolyte can retain a high concentration of lithium salt even when low concentrations of lithium salt are used. Briefly, the BaP promotes the salting-in phenomenon of Li ions, while the TFSI ions induce salting-out, allowing BaP to synergistically achieve high lithium salt concentrations. Due to these unique characteristics, the BaP hydrogel exhibits a wide electrochemical stability window similar to that of highly concentrated electrolytes, enabling stable operation in a LiMn<sub>2</sub>O<sub>4</sub>||Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> full cell by suppressing hydrogen evolution. Moreover, the biodegradability of BaP contributes to the development of a more environmentally friendly battery system.","PeriodicalId":228,"journal":{"name":"Small","volume":"91 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666601","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}
Xinqi Huang, Yapeng Tian, Xiaokai Ma, Yuanjie Zheng, Ling Zhang, Yunfeng Chao, Liu Wang, Xinwei Cui
The development of Zn metal anodes is challenged by non-uniformity of ion flux causing inhomogeneous deposition and strong solvation of Zn(H2O)62+ resulting in adverse side reactions. Applying intermediate protecting layers with high affinity to Zn2+ is a popular and effective solution, but it also limits the ion migration. A functional MXene-based interlayer is designed in this work to modify the glass fiber separator achieving balanced adsorption energy and ion migration. By coating porous silica on the MXene surface, the instinct advanatges of MXene are mostly reserved while the adsorption energy to Zn2+ is optimized. Such an interlayer enables high flux and uniformity of desolvated Zn2+, contributing to rapid deposition kinetic for excellent rate performance and inhibited side reactions for long-term cycling stability. As a result, the functionalized Zn metal anode delivers steady plating/stripping cycles for more than 5000 h at 0.1 mA cm−2 and 700 h at 5.0 mA cm−2. The Zn||MnO2 full cells with this separator also exhibit superior rate capabilities (173 mAh g−1 at 2.0 A g−1) and excellent cycle performance (254.7 mAh g−1 after 1000 cycles at 0.5 A g−1). This work provides a feasible strategy for preparing functional interlayers toward superior Zn or other metal anodes.
{"title":"Promoting Migration Kinetic of Desolvated Zn2+ by Functional Interlayer Toward Superior Zn Metal Anode","authors":"Xinqi Huang, Yapeng Tian, Xiaokai Ma, Yuanjie Zheng, Ling Zhang, Yunfeng Chao, Liu Wang, Xinwei Cui","doi":"10.1002/smll.202500503","DOIUrl":"https://doi.org/10.1002/smll.202500503","url":null,"abstract":"The development of Zn metal anodes is challenged by non-uniformity of ion flux causing inhomogeneous deposition and strong solvation of Zn(H<sub>2</sub>O)<sub>6</sub><sup>2+</sup> resulting in adverse side reactions. Applying intermediate protecting layers with high affinity to Zn<sup>2+</sup> is a popular and effective solution, but it also limits the ion migration. A functional MXene-based interlayer is designed in this work to modify the glass fiber separator achieving balanced adsorption energy and ion migration. By coating porous silica on the MXene surface, the instinct advanatges of MXene are mostly reserved while the adsorption energy to Zn<sup>2+</sup> is optimized. Such an interlayer enables high flux and uniformity of desolvated Zn<sup>2+</sup>, contributing to rapid deposition kinetic for excellent rate performance and inhibited side reactions for long-term cycling stability. As a result, the functionalized Zn metal anode delivers steady plating/stripping cycles for more than 5000 h at 0.1 mA cm<sup>−2</sup> and 700 h at 5.0 mA cm<sup>−2</sup>. The Zn||MnO<sub>2</sub> full cells with this separator also exhibit superior rate capabilities (173 mAh g<sup>−1</sup> at 2.0 A g<sup>−1</sup>) and excellent cycle performance (254.7 mAh g<sup>−1</sup> after 1000 cycles at 0.5 A g<sup>−1</sup>). This work provides a feasible strategy for preparing functional interlayers toward superior Zn or other metal anodes.","PeriodicalId":228,"journal":{"name":"Small","volume":"6 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666508","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}
Furi Wang, Xujiao Ma, Xiaofang Su, Zhong Zhang, Wei Liu, Jiahui Peng, Zongyin Gao, Jian Zhang, Yiwei Liu
The inherent sluggish kinetics of the conventional four-electron transfer pathway fundamentally limits the oxygen reduction reaction (ORR) efficiency. While electronic structure modulation offers potential solutions, developing effective catalytic regulation strategies remains challenging due to elusive structure-activity correlations. In this study, Fe4 cluster sites are engineered with dual parallel electron transfer channels that enable concurrent O─O bond cleavage and dual oxygen atom protonation. This unique configuration facilitates an optimized two-step double electron transfer mechanism, significantly enhancing ORR kinetics. Synergistic Mn single atom sites, strategically positioned as electron reservoirs, substantially elevate the electron density of Fe4 clusters while reinforcing Fe─N coordination bonds through charge redistribution. Remarkably, the spatial configuration of Fe4 clusters at the support periphery minimizes steric confinement effects, allowing simultaneous product desorption and oxygen adsorption – a critical advantage for sustaining continuous catalytic cycles. Through combined experimental and theoretical analyses, it is demonstrated that this dual-channel electron transport system effectively reduces activation barriers for elementary steps while accelerating charge transfer kinetics. This fundamental study establishes a new paradigm for designing high-performance ORR catalysts through multi-site collaborative engineering and reaction pathway optimization.
{"title":"Efficient Oxygen Reduction Catalysis on Fe4 Cluster Site Facilitated by Adjacent Single Atom","authors":"Furi Wang, Xujiao Ma, Xiaofang Su, Zhong Zhang, Wei Liu, Jiahui Peng, Zongyin Gao, Jian Zhang, Yiwei Liu","doi":"10.1002/smll.202501746","DOIUrl":"https://doi.org/10.1002/smll.202501746","url":null,"abstract":"The inherent sluggish kinetics of the conventional four-electron transfer pathway fundamentally limits the oxygen reduction reaction (ORR) efficiency. While electronic structure modulation offers potential solutions, developing effective catalytic regulation strategies remains challenging due to elusive structure-activity correlations. In this study, Fe<sub>4</sub> cluster sites are engineered with dual parallel electron transfer channels that enable concurrent O─O bond cleavage and dual oxygen atom protonation. This unique configuration facilitates an optimized two-step double electron transfer mechanism, significantly enhancing ORR kinetics. Synergistic Mn single atom sites, strategically positioned as electron reservoirs, substantially elevate the electron density of Fe<sub>4</sub> clusters while reinforcing Fe─N coordination bonds through charge redistribution. Remarkably, the spatial configuration of Fe<sub>4</sub> clusters at the support periphery minimizes steric confinement effects, allowing simultaneous product desorption and oxygen adsorption – a critical advantage for sustaining continuous catalytic cycles. Through combined experimental and theoretical analyses, it is demonstrated that this dual-channel electron transport system effectively reduces activation barriers for elementary steps while accelerating charge transfer kinetics. This fundamental study establishes a new paradigm for designing high-performance ORR catalysts through multi-site collaborative engineering and reaction pathway optimization.","PeriodicalId":228,"journal":{"name":"Small","volume":"27 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666510","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}
Karlin Hilai, Daniil Grubich, Marcus Akrawi, Hui Zhu, Razanne Zaghloul, Chenjun Shi, Man Do, Dongxiao Zhu, Jitao Zhang
Cellular biomechanics plays a critical role in cancer metastasis and tumor progression. Existing studies on cancer cell biomechanics are mostly conducted in flat 2D conditions, where cells’ behavior can differ considerably from those in 3D physiological environments. Despite great advances in developing 3D in vitro models, probing cellular elasticity in 3D conditions remains a major challenge for existing technologies. In this work, optical Brillouin microscopy is utilized to longitudinally acquire mechanical images of growing cancerous spheroids over the period of 8 days. The dense mechanical mapping from Brillouin microscopy enables us to extract spatially resolved and temporally evolving mechanical features that were previously inaccessible. Using an established machine learning algorithm, it is demonstrated that incorporating these extracted mechanical features significantly improves the classification accuracy of cancer cells, from 74% to 95%. Building on this finding, a deep learning pipeline capable of accurately differentiating cancerous spheroids from normal ones solely using Brillouin images have been developed, suggesting the mechanical features of cancer cells can potentially serve as a new biomarker in cancer classification and detection.
{"title":"Mechanical Evolution of Metastatic Cancer Cells in 3D Microenvironment","authors":"Karlin Hilai, Daniil Grubich, Marcus Akrawi, Hui Zhu, Razanne Zaghloul, Chenjun Shi, Man Do, Dongxiao Zhu, Jitao Zhang","doi":"10.1002/smll.202403242","DOIUrl":"https://doi.org/10.1002/smll.202403242","url":null,"abstract":"Cellular biomechanics plays a critical role in cancer metastasis and tumor progression. Existing studies on cancer cell biomechanics are mostly conducted in flat 2D conditions, where cells’ behavior can differ considerably from those in 3D physiological environments. Despite great advances in developing 3D in vitro models, probing cellular elasticity in 3D conditions remains a major challenge for existing technologies. In this work, optical Brillouin microscopy is utilized to longitudinally acquire mechanical images of growing cancerous spheroids over the period of 8 days. The dense mechanical mapping from Brillouin microscopy enables us to extract spatially resolved and temporally evolving mechanical features that were previously inaccessible. Using an established machine learning algorithm, it is demonstrated that incorporating these extracted mechanical features significantly improves the classification accuracy of cancer cells, from 74% to 95%. Building on this finding, a deep learning pipeline capable of accurately differentiating cancerous spheroids from normal ones solely using Brillouin images have been developed, suggesting the mechanical features of cancer cells can potentially serve as a new biomarker in cancer classification and detection.","PeriodicalId":228,"journal":{"name":"Small","volume":"214 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666506","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}
Achieving a precise understanding and accurate design of heterogeneous catalysts based on bioinspired principles is challenging yet crucial to digging out optimal materials for artificial catalysis. Here, an ADH-mimicking dual-site photocatalyst (YCuCdS) is developed, and demonstrates the powerful effects of atomic site configuration and proton transfer environments on alcohol-amine coupling. Mechanism studies reveal that the alcohol substrate is effectively dehydrogenated at the Y sites, forming the carbonyl intermediates that rapidly experience condensation with the amine. Meanwhile, the released hydrogen species (Hads) migrate from adjacent Cu sites to active S atoms, promoting H2 production and hindering the over-hydrogenation of imine. As a result, a high imine yield of 92% is achieved, along with an H2 production rate of 7400 µmol g−1 h−1. This work showcases an effective strategy for the design of heterogeneous catalysts with bioinspiration.
{"title":"Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol-Amine Coupling","authors":"Huimin Yi, Chenyi Wang, Baoxin Ge, Fangjie Xu, Pengyang Jiang, Min Zhou, Fangshu Xing, Caijin Huang","doi":"10.1002/smll.202500253","DOIUrl":"https://doi.org/10.1002/smll.202500253","url":null,"abstract":"Achieving a precise understanding and accurate design of heterogeneous catalysts based on bioinspired principles is challenging yet crucial to digging out optimal materials for artificial catalysis. Here, an ADH-mimicking dual-site photocatalyst (YCuCdS) is developed, and demonstrates the powerful effects of atomic site configuration and proton transfer environments on alcohol-amine coupling. Mechanism studies reveal that the alcohol substrate is effectively dehydrogenated at the Y sites, forming the carbonyl intermediates that rapidly experience condensation with the amine. Meanwhile, the released hydrogen species (H<sub>ads</sub>) migrate from adjacent Cu sites to active S atoms, promoting H<sub>2</sub> production and hindering the over-hydrogenation of imine. As a result, a high imine yield of 92% is achieved, along with an H<sub>2</sub> production rate of 7400 µmol g<sup>−1</sup> h<sup>−1</sup>. This work showcases an effective strategy for the design of heterogeneous catalysts with bioinspiration.","PeriodicalId":228,"journal":{"name":"Small","volume":"37 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666511","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：