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Impact of Interface and Surface Oxide Defects on WS2 Electronic Properties from First Principles
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c08959
Benoit Van Troeye, Fabian Ducry, Mauro Dossena, Mathieu Luisier, Aryan Afzalian, Geoffrey Pourtois
{"title":"Impact of Interface and Surface Oxide Defects on WS2 Electronic Properties from First Principles","authors":"Benoit Van Troeye, Fabian Ducry, Mauro Dossena, Mathieu Luisier, Aryan Afzalian, Geoffrey Pourtois","doi":"10.1021/acsnano.4c08959","DOIUrl":"https://doi.org/10.1021/acsnano.4c08959","url":null,"abstract":"The industrial-scale growth of dielectrics on top of a 2D material transistor channel without deterioration of its transport characteristics remains challenging today. Here, we investigate the origin of the performance degradation issue by constructing several atomistic interface models between a WS<sub>2</sub> monolayer and an amorphous Al<sub>2</sub>O<sub>3</sub> or HfO<sub>2</sub> thin film. We then computed their properties using first-principles methods. We show that, while it is in principle possible to achieve a van der Waals interface between these materials, surface defects (e.g., undercoordinated metal atoms at the surface) are detrimental since they create localized states close to the bottom of the conduction band of WS<sub>2</sub>. Even in their absence, the inhomogeneity of the surface topology creates a nonuniform potential that is felt by charge carriers in WS<sub>2</sub>. While surface defects can potentially be kept under control with an appropriate oxide choice, the surface inhomogeneity appears to act as a bottleneck, limiting the performance of WS<sub>2</sub> as a transistor channel and, in general, for all 2D materials.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"42 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640266","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}
引用次数: 0
Comment on “Submicron Memtransistors Made from Monocrystalline Molybdenum Disulfide”
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c1797710.1021/acsnano.4c17977
Hei Wong*, 
{"title":"Comment on “Submicron Memtransistors Made from Monocrystalline Molybdenum Disulfide”","authors":"Hei Wong*,&nbsp;","doi":"10.1021/acsnano.4c1797710.1021/acsnano.4c17977","DOIUrl":"https://doi.org/10.1021/acsnano.4c17977https://doi.org/10.1021/acsnano.4c17977","url":null,"abstract":"<p >A three-terminal memtransistor utilizing monocrystalline molybdenum disulfide (MoS<sub>2</sub>) as the channel material and semimetal source/drain electrode has been reported by Yang et al. (<i>ACS Nano</i> <b>2024,</b> <i>18</i>, 6936–6945). The article attributes the memory characteristics to charge trapping and detrapping at the interface between the HfO<sub>2</sub> gate oxide and MoS<sub>2</sub>. Additionally, multiple memory states were achieved by applying different gate pulses, highlighting the device’s high potential for neuromorphic computing applications. According to the article, these behaviors stem from space charge-limited current (SCLC) and trap-filled limit (TFL) mechanisms. However, our in-depth analysis of the reported current–voltage characteristics indicates that these models are somewhat insufficient and inappropriate. This work offers an alternative explanation for the observed results and proposes a more accurate working model with sound physical justifications. The different physical mechanisms derived from this study are expected to significantly impact the further development and improvement of the proposed memtransistors.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 10","pages":"9435–9439 9435–9439"},"PeriodicalIF":15.8,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635808","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}
引用次数: 0
Comment on “Submicron Memtransistors Made from Monocrystalline Molybdenum Disulfide”
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c17977
Hei Wong
{"title":"Comment on “Submicron Memtransistors Made from Monocrystalline Molybdenum Disulfide”","authors":"Hei Wong","doi":"10.1021/acsnano.4c17977","DOIUrl":"https://doi.org/10.1021/acsnano.4c17977","url":null,"abstract":"A three-terminal memtransistor utilizing monocrystalline molybdenum disulfide (MoS<sub>2</sub>) as the channel material and semimetal source/drain electrode has been reported by Yang et al. (<i>ACS Nano</i> <b>2024,</b> <i>18</i>, 6936–6945). The article attributes the memory characteristics to charge trapping and detrapping at the interface between the HfO<sub>2</sub> gate oxide and MoS<sub>2</sub>. Additionally, multiple memory states were achieved by applying different gate pulses, highlighting the device’s high potential for neuromorphic computing applications. According to the article, these behaviors stem from space charge-limited current (SCLC) and trap-filled limit (TFL) mechanisms. However, our in-depth analysis of the reported current–voltage characteristics indicates that these models are somewhat insufficient and inappropriate. This work offers an alternative explanation for the observed results and proposes a more accurate working model with sound physical justifications. The different physical mechanisms derived from this study are expected to significantly impact the further development and improvement of the proposed memtransistors.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"90 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640274","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}
引用次数: 0
Potassium-Doped MnO2 Nanoparticles Reprogram Neutrophil Calcium Signaling to Accelerate Healing of Methicillin-Resistant Staphylococcus aureus-Infected Diabetic Wounds
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c14057
Jianxu Wei, Xiaomeng Zhang, Baiyan Sui, Xinxin Ding, Yuan Li, Beilei Liu, Jiale Wang, Xiaolei Lv, Yi Zhang, Xue Jiang, Yijie Yang, Hongchang Lai, Xin Liu, Junyu Shi
{"title":"Potassium-Doped MnO2 Nanoparticles Reprogram Neutrophil Calcium Signaling to Accelerate Healing of Methicillin-Resistant Staphylococcus aureus-Infected Diabetic Wounds","authors":"Jianxu Wei, Xiaomeng Zhang, Baiyan Sui, Xinxin Ding, Yuan Li, Beilei Liu, Jiale Wang, Xiaolei Lv, Yi Zhang, Xue Jiang, Yijie Yang, Hongchang Lai, Xin Liu, Junyu Shi","doi":"10.1021/acsnano.4c14057","DOIUrl":"https://doi.org/10.1021/acsnano.4c14057","url":null,"abstract":"Neutrophils, as first-line immune cells, typically lose their edge within the diabetic wounds accompanied by methicillin-resistant <i>Staphylococcus aureus</i> (MRSA) infections (the D/M setting), playing the role of “more foe than friend” during the healing process. Specifically, reduced influx of calcium ions (Ca<sup>2+</sup>) and impaired calcium homeostasis yield the dysfunction of neutrophil sequential behaviors in pathogen killing and wound healing, manifesting as suppressed chemotaxis, decreased intracellular reactive oxygen species (ROS) generation, prolonged apoptosis, and retention of neutrophil extracellular traps (NETs). To address this challenge, this study fabricated potassium (K)-doped manganese dioxide nanoparticles (MnO<sub>2</sub> NPs), which activated transmembrane Ca<sup>2+</sup> channels by inducing neutrophil depolarization via electron transfer. Subsequently, this contributed to the initial Ca<sup>2+</sup> influx and reprogrammed Ca<sup>2+</sup>-dependent behaviors of impaired neutrophils. Also, the potential antimicrobial capacity of K-MnO<sub>2</sub> NPs created a favorable extracellular environment that restored calcium homeostasis, enabling apoptotic neutrophils to be removed timely. Therefore, the wounds treated with K-MnO<sub>2</sub> NPs in the D/M setting exhibited potent resistance to MRSA and rapid healing, which could be attributed to the synergistic effects of K-MnO<sub>2</sub> NPs in leveraging Ca<sup>2+</sup> influx and maintaining calcium homeostasis. In brief, K-MnO<sub>2</sub> NPs constitute an effective strategy to resist MRSA and rapid wound healing in the D/M setting.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"197 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640228","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}
引用次数: 0
Opportunities and Challenges of DNA Materials toward Sustainable Development Goals
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c17718
Renkuan Liao, Dan Luo, Dayong Yang, Jianguo Liu
{"title":"Opportunities and Challenges of DNA Materials toward Sustainable Development Goals","authors":"Renkuan Liao, Dan Luo, Dayong Yang, Jianguo Liu","doi":"10.1021/acsnano.4c17718","DOIUrl":"https://doi.org/10.1021/acsnano.4c17718","url":null,"abstract":"Sustainable development represents a significant and pressing challenge confronting the global community at present. A wide variety of macroscopic engineering systems has been developed to promote sustainable development. Recent advancements in DNA materials have showcased their substantial contributions toward achieving sustainable development goals (SDGs). Compared to nonbiological materials, DNA materials possess exceptional properties such as genetic functionality, molecular programmability, recognition capabilities, and biocompatibility. These unique characteristics enable DNA materials to serve as general and versatile substrates beyond their genetic role. Consequently, they can be used to develop DNA-based engineering systems that offer versatile solutions to support sustainable development. In this Perspective, we critically examine the opportunities that DNA-based engineering systems present in contributing to the achievement of the SDGs within various real-world scenarios. We establish direct relationships between DNA-based engineering systems and the SDGs, highlighting their inherent merits in accelerating sustainable development. Furthermore, in order to successfully achieve SDGs, we address the challenges associated with these systems and emphasize the urgent need for developing multifunctional, reliable, biosafe, and intelligent DNA-based engineering systems to overcome these challenges.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"49 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640268","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}
引用次数: 0
Treatment of Acute Liver Injury through Selective Tropism of High Mobility Group Box 1 Gene-Silenced Large Peritoneal Macrophages
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c18345
Dhaval Oza, Fernando Ivich, Kirsten Deprey, Kelsey Bittner, Keith Bailey, Sarah Goldman, Mikyung Yu, Mark Niedre, Ho-Chou Tu, Mansoor M. Amiji
{"title":"Treatment of Acute Liver Injury through Selective Tropism of High Mobility Group Box 1 Gene-Silenced Large Peritoneal Macrophages","authors":"Dhaval Oza, Fernando Ivich, Kirsten Deprey, Kelsey Bittner, Keith Bailey, Sarah Goldman, Mikyung Yu, Mark Niedre, Ho-Chou Tu, Mansoor M. Amiji","doi":"10.1021/acsnano.4c18345","DOIUrl":"https://doi.org/10.1021/acsnano.4c18345","url":null,"abstract":"Tissue-resident macrophages (TRMs) are attractive cells to therapeutically deliver oligonucleotide and other gene-expression modifying modalities to treat a wide array of diseases ranging from inflammatory to autoimmune, and even cancer. Here, we focus on TRMs located inside the peritoneal cavity lining the abdomen that selectively express a transcription factor GATA6 called large peritoneal macrophages (GLPMs) and successfully demonstrate functional GLPM-selective delivery of a Cy5-fluorophore-labeled siRNA encapsulated in C12–200 cationic-lipidoid-based nanoparticles (siRNA-Cy5 (C12–200)). Despite being TRMs, GLPMs possess a specific migratory ability to peritoneally located liver tissue upon injury incited by acetaminophen (APAP) overdose in mice. A rapid, liver injury-driven tropism of GLPMs carrying siRNA-Cy5 (C12–200) was seen via systemic circulation, which was elegantly demonstrated by using a noninvasive live-cell tracking technique called diffuse <i>in vivo</i> flow cytometry (DiFC). Finally, RNAi-mediated silencing of a well-known pro-inflammatory damage-associated molecular pattern (DAMP) <i>High Mobility Group Box-1</i> (HMGB1) gene in GLPMs led to the mitigation of liver injury and inflammation via prevention of GLPM modulation to a pro-inflammatory state, which further translated into significant protection from APAP-driven liver injury and a reduction in liver circulating pro-inflammatory cytokines owing to a muted inflammatory response to acute liver injury. Moreover, silencing HMGB1 by a GalNAc-conjugated hepatocyte-targeting siRNA did not reciprocate the findings, further solidifying our results. Together, our data suggested that GLPMs act as delivery carriers by rapidly bringing lipid nanoparticle-encapsulated RNAi modalities to the injured liver and have emerged as a therapeutically viable strategy to address inflammatory diseases, especially those that are more acute in nature.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640270","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}
引用次数: 0
Small Twist Angles Accelerate Electron and Hole Transfer in MoSe2/WSe2 Heterostructures
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c18675
Yan Zeng, Zhenwei Ou, Zhe Li, Cheng Wang, Jiakai Yan, Wenbo Li, Yan Li, Wei Dai, Huiting Zhang, Takashi Taniguchi, Kenji Watanabe, Haoqing Jiang, Hongli Guo, Gang Lu, Tong Zhu, Ti Wang, Hongxing Xu
{"title":"Small Twist Angles Accelerate Electron and Hole Transfer in MoSe2/WSe2 Heterostructures","authors":"Yan Zeng, Zhenwei Ou, Zhe Li, Cheng Wang, Jiakai Yan, Wenbo Li, Yan Li, Wei Dai, Huiting Zhang, Takashi Taniguchi, Kenji Watanabe, Haoqing Jiang, Hongli Guo, Gang Lu, Tong Zhu, Ti Wang, Hongxing Xu","doi":"10.1021/acsnano.4c18675","DOIUrl":"https://doi.org/10.1021/acsnano.4c18675","url":null,"abstract":"Van der Waals (vdW) heterostructures host interlayer excitons that act as robust carriers of valley information and sensitive probes of strongly correlated electronic phases. The formation and properties of these interlayer excitons critically depend on efficient charge transfer across the heterointerface. Among the various factors influencing these processes, the twist angle emerges as a key degree of freedom, allowing precise modulation of the stacking configuration and electronic band structure of the heterostructure. In this study, we perform ultrafast pump–probe measurements on MoSe<sub>2</sub>/WSe<sub>2</sub> heterostructures with various twist angles. Counterintuitively, the results show that both electron and hole transfer rates are strongly influenced by twist angles, peaking at 0 and 60° twist angles, respectively. Theoretical calculations indicate that this behavior stems from reduced valley energy offsets and enhanced interlayer hybridization at small twist angles, which collectively promotes more efficient electron and hole transfer. Our findings demonstrate the influence of twist-angle engineering on interfacial carrier dynamics and its impact on the optoelectronic properties of vdW heterostructures.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"183 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640271","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}
引用次数: 0
Atomic and Electronic Structures of 1D Phosphorus Nanoring and Nanohelix
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.5c00034
Young Woo Choi, Yangjin Lee, Kwanpyo Kim, Alex Zettl, Marvin L. Cohen
{"title":"Atomic and Electronic Structures of 1D Phosphorus Nanoring and Nanohelix","authors":"Young Woo Choi, Yangjin Lee, Kwanpyo Kim, Alex Zettl, Marvin L. Cohen","doi":"10.1021/acsnano.5c00034","DOIUrl":"https://doi.org/10.1021/acsnano.5c00034","url":null,"abstract":"Elemental phosphorus, with its diverse polymorphs, presents intriguing opportunities for material design owing to its ability to stabilize in various allotropes. In this work, we investigate the one-dimensional (1D) phosphorus nanoring and nanohelix structure. 1D phosphorus allotropes are stabilized within the carbon nanotubes (CNTs) that act as nano reaction vessels. Transmission electron microscopy (TEM) imaging provides experimental evidence for the formation of nanoring and nanohelix structures. First-principles calculations show distinct orbital characters between valence and conduction bands and reveal strain-induced valence band reordering. Our findings provide a foundation for further studies into topological and optical properties of 1D phosphorus nanostructures.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"13 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640142","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}
引用次数: 0
Trimodal Hierarchical Porous Carbon Nanoplates with Edge Curvature for Faster Mass Transfer and Enhanced Oxygen Reduction
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c06404
Ruijing Xin, Ho Ngoc Nam, Quan Manh Phung, Jing Tang, Shengchun Ma, Josua Markus, Yuchen Dai, Azhar Alowasheeir, Nithima Khaorapapong, Jie Wang, Yusuke Yamauchi, Yusuf Valentino Kaneti
{"title":"Trimodal Hierarchical Porous Carbon Nanoplates with Edge Curvature for Faster Mass Transfer and Enhanced Oxygen Reduction","authors":"Ruijing Xin, Ho Ngoc Nam, Quan Manh Phung, Jing Tang, Shengchun Ma, Josua Markus, Yuchen Dai, Azhar Alowasheeir, Nithima Khaorapapong, Jie Wang, Yusuke Yamauchi, Yusuf Valentino Kaneti","doi":"10.1021/acsnano.4c06404","DOIUrl":"https://doi.org/10.1021/acsnano.4c06404","url":null,"abstract":"Although hierarchical porous carbon materials have been widely used for electrocatalysis, the role of curvature in carbon nanostructures during electrochemical reactions remains poorly understood due to a lack of experimental models featuring clearly defined curved geometries and periodic structures. In this study, we fabricate hierarchical porous cobalt- and nitrogen-containing carbon nanoplates with trimodal porosity (macro-, meso-, and micropores) and continuous, homogeneous curved edges (Co/N-CNP-CURV) using a polystyrene-directed templating approach. The Co/N-CNP-CURV catalyst exhibits excellent catalytic activity and stability for the alkaline oxygen reduction reaction, with a half-wave potential of 0.82 V and a minimal potential shift of 8 mV after 5000 cycles. The enhanced electrocatalytic activity is attributed to synergistic combinations of the trimodal porosity, abundant Co–N<i><sub>x</sub></i> active sites, a high density of curved edges, and graphitic carbon encapsulated with cobalt nanoparticles. Density functional theory calculations reveal that the presence of curvature in Co/N-CNP-CURV is beneficial for enhancing the charge transfer from the catalyst to O<sub>2</sub>, lowering the adsorption energy of O<sub>2</sub>, and reducing the activation free energy barrier for the rate-determining step (*O<sub>2</sub> + (H<sup>+</sup> + e<sup>–</sup>) → *OOH). The study provides compelling experimental evidence supporting the critical role of the curvature effect in enhancing the electrocatalytic performance of nanoporous metal-containing carbon materials.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640265","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}
引用次数: 0
Selective Adsorption-Catalysis Sites of Lithium Polysulfides Induced by the Competition between Spin Polarization and Electronegativity in High-Entropy Alloy Electrocatalysts
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-03-18 DOI: 10.1021/acsnano.4c17661
Boyu Li, Huan Wang, Yanlei Shen, Ziyao Zhang, Yuping Xiong, Mengting Wang, Weitao Li, Weitao Zhou, Jianxin He
{"title":"Selective Adsorption-Catalysis Sites of Lithium Polysulfides Induced by the Competition between Spin Polarization and Electronegativity in High-Entropy Alloy Electrocatalysts","authors":"Boyu Li, Huan Wang, Yanlei Shen, Ziyao Zhang, Yuping Xiong, Mengting Wang, Weitao Li, Weitao Zhou, Jianxin He","doi":"10.1021/acsnano.4c17661","DOIUrl":"https://doi.org/10.1021/acsnano.4c17661","url":null,"abstract":"High-entropy alloy (HEA) electrocatalysts have attracted increasing attention for improving sulfur reaction kinetics and anchoring lithium polysulfides (LiPSs) in lithium-sulfur batteries (LSBs). However, fundamentally understanding the relationship between the components of HEAs and the adsorption catalysis of LiPSs remains a challenge. Here, FeCoNiMnRu HEAs are employed as a model to first disclose the selective adsorption-catalysis effect of LiPSs, induced by the competition between spin polarization and electronegativity of Ni−Co−Ru sites in HEAs. By correlating the electron structure, we find that the high-electronegativity Ru sites induce electron transfer from Co sites, generating local electron delocalization, while the Ni sites adopt a high-spin state. Specifically, high-spin Ni sites with stronger Ni−S covalency can sustainably anchor LiPSs, while electron-delocalized Co−Ru sites function better in LiPS conversion. Consequently, benefiting from the selective adsorption-catalysis effect of Ni−Co−Ru sites, LSBs with FeCoNiMnRu/CNF interlayers deliver exceptional cycling performance (0.06% per cycle over 500 cycles at 1 C, and an outstanding areal capacity of 11.2 mAh cm<sup>−2</sup> at 0.1 C). This work offers key insights for extending HEAs electrocatalysts to enable high-performance LSBs.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"33 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640267","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}
引用次数: 0
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