The application of smart devices and artificial intelligence (AI) technologies has led to an increase in electromagnetic interference (EMI) issues. Compared with the traditional metal-based EMI shielding materials, lighter and more efficient polymer-based EMI shielding materials have a broader application prospect. In this work, we utilized electrospinning and calcination techniques to synthesize Fe3O4 nanofibers and employed a layer-by-layer assembly method to create a Ti3C2Tx MXene/Fe3O4/carbon fiber fabric/waterborne polyurethane (Ti3C2Tx MXene/Fe3O4/CFf/WPU) composite fabric. Our findings reveal that this composite fabric possesses superior EMI shielding capabilities. Specifically, the FMC12.5–5 composite material, which contains 12.5 wt % Fe3O4 and 5 wt % Ti3C2Tx, demonstrates remarkable electromagnetic interference (EMI) shielding effectiveness (SE) (up to 43.6 dB) at a mere 0.4 mm thickness with a low MXene content. Meanwhile, the fabric achieves a significant anisotropic thermal conductivity of up to 0.46 W/(m K), fulfilling the in-plane thermal conductivity requirement. Additionally, the sandwich-structured composite exhibits excellent mechanical performance (Young’s modulus is up to 113.5 MPa and tensile strength reaches 15.7 MPa) and is flexible enough to endure repeated bending, folding, and shaping. It maintains a reliable electrothermal conversion capability, achieving temperatures of up to 106 °C at only 2.5 V. This study has expanded the exploration of enhanced electromagnetic interference (EMI) shielding and electrothermal conversion capabilities.
{"title":"Ti3C2Tx MXene/Fe3O4/Carbon Fiber Fabric/Water Polyurethane Composite Fabrics for Electromagnetic Interference Shielding and Thermal Management","authors":"Meirong Huang, Ying Huang, Hui Yang, Wenmu Li","doi":"10.1021/acsanm.4c00639","DOIUrl":"https://doi.org/10.1021/acsanm.4c00639","url":null,"abstract":"The application of smart devices and artificial intelligence (AI) technologies has led to an increase in electromagnetic interference (EMI) issues. Compared with the traditional metal-based EMI shielding materials, lighter and more efficient polymer-based EMI shielding materials have a broader application prospect. In this work, we utilized electrospinning and calcination techniques to synthesize Fe<sub>3</sub>O<sub>4</sub> nanofibers and employed a layer-by-layer assembly method to create a Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i> MXene/Fe<sub>3</sub>O<sub>4</sub>/carbon fiber fabric/waterborne polyurethane (Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i> MXene/Fe<sub>3</sub>O<sub>4</sub>/CFf/WPU) composite fabric. Our findings reveal that this composite fabric possesses superior EMI shielding capabilities. Specifically, the FMC12.5–5 composite material, which contains 12.5 wt % Fe<sub>3</sub>O<sub>4</sub> and 5 wt % Ti<sub>3</sub>C<sub>2</sub>T<i><sub>x</sub></i>, demonstrates remarkable electromagnetic interference (EMI) shielding effectiveness (SE) (up to 43.6 dB) at a mere 0.4 mm thickness with a low MXene content. Meanwhile, the fabric achieves a significant anisotropic thermal conductivity of up to 0.46 W/(m K), fulfilling the in-plane thermal conductivity requirement. Additionally, the sandwich-structured composite exhibits excellent mechanical performance (Young’s modulus is up to 113.5 MPa and tensile strength reaches 15.7 MPa) and is flexible enough to endure repeated bending, folding, and shaping. It maintains a reliable electrothermal conversion capability, achieving temperatures of up to 106 °C at only 2.5 V. This study has expanded the exploration of enhanced electromagnetic interference (EMI) shielding and electrothermal conversion capabilities.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525255","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}
Ngoc-Diem Huynh, Jayasmita Jana, Jin Suk Chung, Won Mook Choi, Seung Hyun Hur
The search for an effective, stable, and economically viable electrocatalyst for water splitting to replace expensive noble catalysts remains imperative. This investigation evaluates the impact of erbium oxide (Er2O3) on the oxygen evolution reaction (OER) activity of transition metal oxides (TMOs), including nickel oxide (NiO), cobalt oxide (Co3O4), and iron oxide (Fe2O3). Introducing Er2O3 nanoclusters into TMO nanostructures produces a heterostructure interface between Er2O3 and the active TMOs, leveraging Er2O3’s unique 4f electron occupancy as an effective electronic modulator, thus enhancing its electrocatalytic activity. Findings reveal that the Er2O3 and Fe2O3 hybrid (ErFeO) exhibits the most promising OER activity, characterized by low overpotential and Tafel slope, exceptional durability relative to synthesized materials, and outperforming the commercial noble catalyst, RuO2. Consequently, ErFeO is a prospective electrocatalyst for OER applications.
{"title":"Influence of Er2O3 Nanoclusters on Transition Metal Oxide Nanostructures in Water Oxidation","authors":"Ngoc-Diem Huynh, Jayasmita Jana, Jin Suk Chung, Won Mook Choi, Seung Hyun Hur","doi":"10.1021/acsanm.4c03420","DOIUrl":"https://doi.org/10.1021/acsanm.4c03420","url":null,"abstract":"The search for an effective, stable, and economically viable electrocatalyst for water splitting to replace expensive noble catalysts remains imperative. This investigation evaluates the impact of erbium oxide (Er<sub>2</sub>O<sub>3</sub>) on the oxygen evolution reaction (OER) activity of transition metal oxides (TMOs), including nickel oxide (NiO), cobalt oxide (Co<sub>3</sub>O<sub>4</sub>), and iron oxide (Fe<sub>2</sub>O<sub>3</sub>). Introducing Er<sub>2</sub>O<sub>3</sub> nanoclusters into TMO nanostructures produces a heterostructure interface between Er<sub>2</sub>O<sub>3</sub> and the active TMOs, leveraging Er<sub>2</sub>O<sub>3</sub>’s unique 4f electron occupancy as an effective electronic modulator, thus enhancing its electrocatalytic activity. Findings reveal that the Er<sub>2</sub>O<sub>3</sub> and Fe<sub>2</sub>O<sub>3</sub> hybrid (ErFeO) exhibits the most promising OER activity, characterized by low overpotential and Tafel slope, exceptional durability relative to synthesized materials, and outperforming the commercial noble catalyst, RuO<sub>2</sub>. Consequently, ErFeO is a prospective electrocatalyst for OER applications.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525269","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}
Ian Daniell Santos, Patrick Tjarks, Jeyavelan Muthu, You-Chen Lin, Zhi-Long Yen, Pradyumna Kumar Chand, Radha Raman, Dinh Tuan Nguyen, Mehdi Rouhani, Yeau-Ren Jeng, Ya-Png Hsieh, Mario Hofmann
We demonstrate the strengthening of graphene, an atomically thin carbon allotrope, by out-of-plane folding. Through lateral confinement of graphene at the water–air interface, nanoscale buckling was induced in suspended flakes, leading to an unexpected folding transition beyond a critical surface pressure. The emergence of folding was confirmed by in situ Brewster angle reflectivity and ex situ microscopy, showing a unique “z-laminated” nanostructure. Molecular dynamics simulations indicate that z-lamination yields an enhanced adhesion between neighboring flakes compared to lateral sliding, which was confirmed by a surface pressure hysteresis during the folding process. Mechanical testing reveals superior Young’s modulus and yield strength when compared to conventional graphene assemblies and even compared to composites. We demonstrate the potential of the z-lamination approach for applications in graphene-based structural materials, tribological layers, and functional electrochemical coatings. Finally, the complete recyclability of z-laminated graphene opens up new routes toward sustainable nanostructured materials.
我们展示了通过平面外折叠强化石墨烯这种原子级薄碳同素异形体的过程。通过在水-空气界面对石墨烯进行横向限制，在悬浮薄片中诱发了纳米级屈曲，从而导致在临界表面压力之外出现意想不到的折叠转变。折叠的出现得到了原位布儒斯特角反射和原位显微镜的证实，显示出一种独特的 "z-层状 "纳米结构。分子动力学模拟表明，与横向滑动相比，"Z "形层压增强了相邻薄片之间的粘附力，这一点通过折叠过程中的表面压力滞后得到了证实。机械测试表明，与传统石墨烯组件相比，甚至与复合材料相比，这种材料的杨氏模量和屈服强度都更胜一筹。我们展示了 z 形层压方法在石墨烯基结构材料、摩擦学层和功能性电化学涂层方面的应用潜力。最后，z-层压石墨烯的完全可回收性为实现可持续纳米结构材料开辟了新的途径。
{"title":"Z-Laminating Assembly of Graphene Nanoflakes for Super-Strong Membranes and Functional Coatings","authors":"Ian Daniell Santos, Patrick Tjarks, Jeyavelan Muthu, You-Chen Lin, Zhi-Long Yen, Pradyumna Kumar Chand, Radha Raman, Dinh Tuan Nguyen, Mehdi Rouhani, Yeau-Ren Jeng, Ya-Png Hsieh, Mario Hofmann","doi":"10.1021/acsanm.4c00954","DOIUrl":"https://doi.org/10.1021/acsanm.4c00954","url":null,"abstract":"We demonstrate the strengthening of graphene, an atomically thin carbon allotrope, by out-of-plane folding. Through lateral confinement of graphene at the water–air interface, nanoscale buckling was induced in suspended flakes, leading to an unexpected folding transition beyond a critical surface pressure. The emergence of folding was confirmed by in situ Brewster angle reflectivity and ex situ microscopy, showing a unique “z-laminated” nanostructure. Molecular dynamics simulations indicate that z-lamination yields an enhanced adhesion between neighboring flakes compared to lateral sliding, which was confirmed by a surface pressure hysteresis during the folding process. Mechanical testing reveals superior Young’s modulus and yield strength when compared to conventional graphene assemblies and even compared to composites. We demonstrate the potential of the z-lamination approach for applications in graphene-based structural materials, tribological layers, and functional electrochemical coatings. Finally, the complete recyclability of z-laminated graphene opens up new routes toward sustainable nanostructured materials.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525256","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}
Xiaoliang Ma, Yusheng Wang, Chi Wang, Yunfei Zhang, Ping Fu, Feipeng Du
Single-walled carbon nanotube (SWCNT)-based flexible thermoelectric films exhibit potential application in wearable electronics due to their good electrical conductivity (σ) and high flexibility. Nevertheless, the low Seebeck coefficient (S) greatly limits their thermoelectric application. The high S of inorganic boron nitride nanosheets is expected to make up for the low S of SWCNT. In this work, exfoliated boron nitride nanosheets (EBNS) are first prepared by solvothermal exfoliation of hexagonal boron nitride (h-BN), which are composited with SWCNT through a simple mixing and filtration method to prepare self-supporting EBNS/SWCNT films with improved thermoelectric properties. Here, the energy filtering effect at the EBNS/SWCNT interface significantly improves the S values of the films. The results show that the maximum S of the EBNS/SWCNT at room temperature is 50.6 μV K–1 and the maximum power factor (PF) is 116.1 μW m–1 K–2 at the EBNS/SWCNT mass ratio of 7.5%. Finally, six pairs of p-type EBNS/SWCNT films and n-type copper sheets are connected in series to assemble a self-powered thermoelectric device, which demonstrates an open-circuit voltage of 8.1 mV and an output power of 550 nW under a temperature difference of 60 K. Therefore, this work provides a simple and effective method to improve the performance of carbon nanotube-based thermoelectric materials.
基于单壁碳纳米管（SWCNT）的柔性热电薄膜具有良好的导电性（σ）和高柔韧性，因此在可穿戴电子设备中具有潜在的应用前景。然而，较低的塞贝克系数（S）极大地限制了它们在热电领域的应用。无机氮化硼纳米片的高 S 值有望弥补 SWCNT 的低 S 值。在这项工作中，首先通过溶解热剥离六方氮化硼（h-BN）制备出剥离氮化硼纳米片（EBNS），然后通过简单的混合和过滤方法将其与 SWCNT 复合，制备出具有更好热电性能的自支撑 EBNS/SWCNT 薄膜。在这里，EBNS/SWCNT 界面的能量过滤效应显著提高了薄膜的 S 值。结果表明，当 EBNS/SWCNT 的质量比为 7.5% 时，EBNS/SWCNT 在室温下的最大 S 值为 50.6 μV K-1，最大功率因数 (PF) 为 116.1 μW m-1 K-2。最后，将六对 p 型 EBNS/SWCNT 薄膜和 n 型铜片串联，组装成一个自供电热电装置，在 60 K 的温差下，该装置的开路电压为 8.1 mV，输出功率为 550 nW。
{"title":"Enhanced Thermoelectric Properties of Exfoliated BN Nanosheets/Single-Walled Carbon Nanotube Composite Films for Applications in Flexible Electronics","authors":"Xiaoliang Ma, Yusheng Wang, Chi Wang, Yunfei Zhang, Ping Fu, Feipeng Du","doi":"10.1021/acsanm.4c02648","DOIUrl":"https://doi.org/10.1021/acsanm.4c02648","url":null,"abstract":"Single-walled carbon nanotube (SWCNT)-based flexible thermoelectric films exhibit potential application in wearable electronics due to their good electrical conductivity (σ) and high flexibility. Nevertheless, the low Seebeck coefficient (<i>S</i>) greatly limits their thermoelectric application. The high <i>S</i> of inorganic boron nitride nanosheets is expected to make up for the low <i>S</i> of SWCNT. In this work, exfoliated boron nitride nanosheets (EBNS) are first prepared by solvothermal exfoliation of hexagonal boron nitride (h-BN), which are composited with SWCNT through a simple mixing and filtration method to prepare self-supporting EBNS/SWCNT films with improved thermoelectric properties. Here, the energy filtering effect at the EBNS/SWCNT interface significantly improves the <i>S</i> values of the films. The results show that the maximum <i>S</i> of the EBNS/SWCNT at room temperature is 50.6 μV K<sup>–1</sup> and the maximum power factor (PF) is 116.1 μW m<sup>–1</sup> K<sup>–2</sup> at the EBNS/SWCNT mass ratio of 7.5%. Finally, six pairs of p-type EBNS/SWCNT films and n-type copper sheets are connected in series to assemble a self-powered thermoelectric device, which demonstrates an open-circuit voltage of 8.1 mV and an output power of 550 nW under a temperature difference of 60 K. Therefore, this work provides a simple and effective method to improve the performance of carbon nanotube-based thermoelectric materials.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525330","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 practical applications of superhydrophobic fabrics face challenges such as inadequate durability and dependence on toxic fluorine-containing reagents. In this work, a robust, multipurpose, and fluoride-free superhydrophobic fabric is engineered. The fabrication process involves the preparation of a petal-like nano-SiO2 (PNS) using a two-phase layering approach. The pleated structure of PNS contributes to excellent roughness on the fabric surface, while the strong adhesion of polydopamine (PDA) serves as an intermediate layer, enhancing the durability and stability of the hydrophobic fabric. Additionally, the surface energy of cotton is reduced by polydimethylsiloxane (PDMS) coating. The resulting fabric coated with PDMS/PNS–PDA exhibits an exceptional water contact angle of 166.3°, a remarkably low sliding angle of only 3.6°, and excellent mechanical stability that can withstand 50 washing cycles and 30 Martindale abrasion cycles. Moreover, the superhydrophobic fabric demonstrates prominent antifouling and self-cleaning properties along with oil–water separation efficiency (>98%), water-in-oil emulsion (96%), and reusability for oil–water separation. Overall, the engineered superhydrophobic fabric shows promising potential in oil–water separation and the development of functional textiles.
{"title":"Fluorine-Free Superhydrophobic Petal-like SiO2 Nanostructure Supported on Cotton for Oil–Water Separation","authors":"Zixiu Chen, Baojie Yang, Lingling Feng, Xiaoyan Xu, Haiyang Luo, Wei Li, Keliang Wang, Hui Qiao","doi":"10.1021/acsanm.4c01888","DOIUrl":"https://doi.org/10.1021/acsanm.4c01888","url":null,"abstract":"The practical applications of superhydrophobic fabrics face challenges such as inadequate durability and dependence on toxic fluorine-containing reagents. In this work, a robust, multipurpose, and fluoride-free superhydrophobic fabric is engineered. The fabrication process involves the preparation of a petal-like nano-SiO<sub>2</sub> (PNS) using a two-phase layering approach. The pleated structure of PNS contributes to excellent roughness on the fabric surface, while the strong adhesion of polydopamine (PDA) serves as an intermediate layer, enhancing the durability and stability of the hydrophobic fabric. Additionally, the surface energy of cotton is reduced by polydimethylsiloxane (PDMS) coating. The resulting fabric coated with PDMS/PNS–PDA exhibits an exceptional water contact angle of 166.3°, a remarkably low sliding angle of only 3.6°, and excellent mechanical stability that can withstand 50 washing cycles and 30 Martindale abrasion cycles. Moreover, the superhydrophobic fabric demonstrates prominent antifouling and self-cleaning properties along with oil–water separation efficiency (>98%), water-in-oil emulsion (96%), and reusability for oil–water separation. Overall, the engineered superhydrophobic fabric shows promising potential in oil–water separation and the development of functional textiles.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525258","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 assembly of carbon dots (CDs) and metal–organic frameworks (MOFs) into MOF@CDs composite materials is rapidly advancing in the field of nanoscience, driven by the potential to harness or enhance the advantages of both CDs and MOFs. However, the exploration of MOFs@CDs with controllable morphologies poses a considerable challenge. Herein, we present a universal synthetic strategy for zeolitic imidazolate frameworks (ZIFs)@CDs composite materials with tunable morphologies and solid-state fluorescence by modulating the surface structure of carbon dots and adjusting the reaction temperature. The assembly process of this strategy is mainly governed by the competitive coordination relationship between the surface functional groups of the carbon dots and the imidazole ligand and the zinc metal sources. Besides, the incorporation of ZIFs@CDs into sodium alginate (SA) to prepare a hydrogel (SA/ZIFs@CDs) effectively enabled the identification and adsorption of copper ions in which the 24-h adsorption capacity of SA/ZIF-L@CD1 at an initial Cu2+ concentration of 500 ppm could reach 200.53 mg g–1. Moreover, the hydrogels dressing after adsorption of Cu2+ could be used to resist the growth of Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). This work provides insights for further advancements in structural design and a deeper understanding of the assembly behavior of the MOFs.
{"title":"Tailoring Morphology and Fluorescence Properties of Zeolitic Imidazolate Frameworks via Carbon Dots","authors":"Hui-Jun Li, Hao Wang, Tianran Si, Huan Wang, Shengqi Huang, Yihan Wu, Qiaobo Liao, Ding Wang, Ying Li","doi":"10.1021/acsanm.4c02441","DOIUrl":"https://doi.org/10.1021/acsanm.4c02441","url":null,"abstract":"The assembly of carbon dots (CDs) and metal–organic frameworks (MOFs) into MOF@CDs composite materials is rapidly advancing in the field of nanoscience, driven by the potential to harness or enhance the advantages of both CDs and MOFs. However, the exploration of MOFs@CDs with controllable morphologies poses a considerable challenge. Herein, we present a universal synthetic strategy for zeolitic imidazolate frameworks (ZIFs)@CDs composite materials with tunable morphologies and solid-state fluorescence by modulating the surface structure of carbon dots and adjusting the reaction temperature. The assembly process of this strategy is mainly governed by the competitive coordination relationship between the surface functional groups of the carbon dots and the imidazole ligand and the zinc metal sources. Besides, the incorporation of ZIFs@CDs into sodium alginate (SA) to prepare a hydrogel (SA/ZIFs@CDs) effectively enabled the identification and adsorption of copper ions in which the 24-h adsorption capacity of SA/ZIF-L@CD<sub>1</sub> at an initial Cu<sup>2+</sup> concentration of 500 ppm could reach 200.53 mg g<sup>–1</sup>. Moreover, the hydrogels dressing after adsorption of Cu<sup>2+</sup> could be used to resist the growth of <i>Escherichia coli</i> (<i>E. coli</i>) and <i>Staphylococcus aureus</i> (<i>S. aureus</i>). This work provides insights for further advancements in structural design and a deeper understanding of the assembly behavior of the MOFs.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525336","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}
Shuyue Li, Liangliang Wang, Liping Chen, Yong Li, Guannan Zu, Juan Wang
Aqueous zinc-ion batteries (AZIBs) are highly competitive in the realm of large-scale energy storage applications due to their characteristics, including superior power density, affordable prices, high safety, and sustainability. Nevertheless, exploring appropriate cathode materials is restricted by low electronic conductivity, sluggish Zn2+ ion diffusion kinetics, and structural degradation during cycling. Herein, we propose a three-birds-with-one-stone strategy of incorporating hydrated manganese ions into layered vanadium oxide to develop an advanced cathode material for Zn2+ storage. Experimental studies and theoretical calculations demonstrate that the incorporated Mn2+ ions not only play a vital role in improving structural stability but also regulating the electronic structure and facilitating the transportation of ions and electrons. Notably, the incorporated Mn2+ induces controllable morphology regulation and fabricated a nanoscale three-dimensional flower-like material with self-assembled nanosheets in a well-designed nanomicrohierarchical structure, thus providing sufficient active sites to accommodate more Zn2+ ions. Benefiting from the above-mentioned ternary merits, the nanoscale Mn0.5V2O5·2.4H2O cathode achieves an excellent capacity of 422 mA h g–1 at 0.1 A g–1 and high capacity retention of 89% over 1000 cycles at 5 A g–1, much higher than that of pristine V2O5·2H2O without Mn2+ (14% over 1000 cycles at 5 A g–1). The modification strategy offers perspective on an effective methodology for exploring advanced cathodes with high electrochemical properties for aqueous rechargeable batteries.
锌离子水电池（AZIBs）具有功率密度高、价格低廉、安全性高和可持续性强等特点，在大规模储能应用领域极具竞争力。然而，由于电子电导率低、Zn2+ 离子扩散动力学缓慢以及循环过程中的结构退化等原因，探索合适的阴极材料受到了限制。在此，我们提出了将水合锰离子融入层状氧化钒的 "一石三鸟 "策略，以开发一种先进的 Zn2+ 储存阴极材料。实验研究和理论计算证明，掺入的 Mn2+ 离子不仅在提高结构稳定性方面发挥着重要作用，而且还能调节电子结构，促进离子和电子的传输。值得注意的是，掺入的 Mn2+ 离子可诱导可控的形态调节，并在精心设计的纳米微层结构中制造出具有自组装纳米片的纳米级三维花朵状材料，从而为容纳更多的 Zn2+ 离子提供了足够的活性位点。得益于上述三元特性，纳米级 Mn0.5V2O5-2.4H2O 阴极在 0.1 A g-1 的条件下实现了 422 mA h g-1 的优异容量，在 5 A g-1 条件下 1000 次循环的容量保持率高达 89%，远高于不含 Mn2+ 的原始 V2O5-2H2O（在 5 A g-1 条件下 1000 次循环的容量保持率为 14%）。这种改性策略为探索具有高电化学特性的先进水性可充电电池阴极提供了一种有效的方法。
{"title":"Nanostructured Layered Vanadium Oxide Modified by Hydrated Manganese Ions for Boosting Zn2+ Storage","authors":"Shuyue Li, Liangliang Wang, Liping Chen, Yong Li, Guannan Zu, Juan Wang","doi":"10.1021/acsanm.4c01933","DOIUrl":"https://doi.org/10.1021/acsanm.4c01933","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) are highly competitive in the realm of large-scale energy storage applications due to their characteristics, including superior power density, affordable prices, high safety, and sustainability. Nevertheless, exploring appropriate cathode materials is restricted by low electronic conductivity, sluggish Zn<sup>2+</sup> ion diffusion kinetics, and structural degradation during cycling. Herein, we propose a three-birds-with-one-stone strategy of incorporating hydrated manganese ions into layered vanadium oxide to develop an advanced cathode material for Zn<sup>2+</sup> storage. Experimental studies and theoretical calculations demonstrate that the incorporated Mn<sup>2+</sup> ions not only play a vital role in improving structural stability but also regulating the electronic structure and facilitating the transportation of ions and electrons. Notably, the incorporated Mn<sup>2+</sup> induces controllable morphology regulation and fabricated a nanoscale three-dimensional flower-like material with self-assembled nanosheets in a well-designed nanomicrohierarchical structure, thus providing sufficient active sites to accommodate more Zn<sup>2+</sup> ions. Benefiting from the above-mentioned ternary merits, the nanoscale Mn<sub>0.5</sub>V<sub>2</sub>O<sub>5</sub>·2.4H<sub>2</sub>O cathode achieves an excellent capacity of 422 mA h g<sup>–1</sup> at 0.1 A g<sup>–1</sup> and high capacity retention of 89% over 1000 cycles at 5 A g<sup>–1</sup>, much higher than that of pristine V<sub>2</sub>O<sub>5</sub>·2H<sub>2</sub>O without Mn<sup>2+</sup> (14% over 1000 cycles at 5 A g<sup>–1</sup>). The modification strategy offers perspective on an effective methodology for exploring advanced cathodes with high electrochemical properties for aqueous rechargeable batteries.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525338","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}
Shuai Chen, Qinchao Xu, Haizhen Sun, Lin Ge, Dongmei Huang, Zongxi Zhang, Yan Qiao, Xili Tong, Weibin Fan
The development of cost-effective oxygen reduction reaction (ORR) catalysts is of great importance and urgency for green energy technologies. Herein, the uniform Co nanoparticles encapsulated in two-dimensional (2D) nitrogen-doped graphitic-carbon nanosheets (Co@N–C) were synthesized by a one-step solvent-free, template-free, and scalable green pyrolysis strategy. Originating from the mutually reinforcing effect between Co nanoparticles and N–C active sites in the stable 2D porous conductive nanosheet structure, the optimized Co@N–C-700 obviously accelerates the catalytic performance for the ORR under both alkaline and acidic conditions. Especially, it showed good performance compared to 20wt% Pt/C-JM in terms of higher half-wave potential (E1/2 = 0.86 V), larger current density (JL = 6.1 mA·cm–2), and better stability, as well as stronger resistance to methanol crossover. In addition, the 2D Co@N–C-700 still exhibits superior operation performance to commercial Pt/C in a hybrid Zn–air battery test.
{"title":"Cobalt-Embedded Nitrogen-Doped Carbon Nanosheets for Oxygen Reduction Reaction under Alkaline and Acidic Media","authors":"Shuai Chen, Qinchao Xu, Haizhen Sun, Lin Ge, Dongmei Huang, Zongxi Zhang, Yan Qiao, Xili Tong, Weibin Fan","doi":"10.1021/acsanm.4c02768","DOIUrl":"https://doi.org/10.1021/acsanm.4c02768","url":null,"abstract":"The development of cost-effective oxygen reduction reaction (ORR) catalysts is of great importance and urgency for green energy technologies. Herein, the uniform Co nanoparticles encapsulated in two-dimensional (2D) nitrogen-doped graphitic-carbon nanosheets (Co@N–C) were synthesized by a one-step solvent-free, template-free, and scalable green pyrolysis strategy. Originating from the mutually reinforcing effect between Co nanoparticles and N–C active sites in the stable 2D porous conductive nanosheet structure, the optimized Co@N–C-700 obviously accelerates the catalytic performance for the ORR under both alkaline and acidic conditions. Especially, it showed good performance compared to 20<sub>wt</sub>% Pt/C-JM in terms of higher half-wave potential (<i>E</i><sub>1/2</sub> = 0.86 V), larger current density (<i>J</i><sub>L</sub> = 6.1 mA·cm<sup>–2</sup>), and better stability, as well as stronger resistance to methanol crossover. In addition, the 2D Co@N–C-700 still exhibits superior operation performance to commercial Pt/C in a hybrid Zn–air battery test.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525339","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}
Florence Y. Dou, Emily Nishiwaki, Helen Larson, Micaela K. Homer, Tallie Zion, Hao A. Nguyen, Brandi M. Cossairt
CdS quantum dots (QDs) are widely employed as photocatalysts for reactions such as hydrogen evolution, and their degradation under aerobic aqueous conditions is well understood. However, despite evidence of aggregation and precipitation of CdS QD photocatalysts under anaerobic conditions, catalyst speciation and degradation under such conditions are underexplored. In this work, we demonstrate that during a reductive dehalogenation reaction, CdS QDs undergo surface ligand etching, which leads to a loss of colloidal stability and the formation of microcrystalline cadmium metal deposits. We hypothesize that this results from the accumulation of electrons on the QD surface. In addition, we demonstrate mild surface sulfur oxidation and the formation of an ammonium salt byproduct of a commonly used hole quencher. This work adds to our atomic-level understanding of the reactions occurring at the QD surface during photocatalysis, so that we can design more stable and efficient photocatalysts for organic synthesis.
{"title":"Pathways of CdS Quantum Dot Degradation during Photocatalysis: Implications for Enhancing Stability and Efficiency for Organic Synthesis","authors":"Florence Y. Dou, Emily Nishiwaki, Helen Larson, Micaela K. Homer, Tallie Zion, Hao A. Nguyen, Brandi M. Cossairt","doi":"10.1021/acsanm.4c02976","DOIUrl":"https://doi.org/10.1021/acsanm.4c02976","url":null,"abstract":"CdS quantum dots (QDs) are widely employed as photocatalysts for reactions such as hydrogen evolution, and their degradation under aerobic aqueous conditions is well understood. However, despite evidence of aggregation and precipitation of CdS QD photocatalysts under anaerobic conditions, catalyst speciation and degradation under such conditions are underexplored. In this work, we demonstrate that during a reductive dehalogenation reaction, CdS QDs undergo surface ligand etching, which leads to a loss of colloidal stability and the formation of microcrystalline cadmium metal deposits. We hypothesize that this results from the accumulation of electrons on the QD surface. In addition, we demonstrate mild surface sulfur oxidation and the formation of an ammonium salt byproduct of a commonly used hole quencher. This work adds to our atomic-level understanding of the reactions occurring at the QD surface during photocatalysis, so that we can design more stable and efficient photocatalysts for organic synthesis.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525257","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}
Nabarun Mandal, Aelton Baptista Santos, Anyesha Chakraborty, Suman Sarkar, Rahul Rao, Nicholas R. Glavin, Ajit K. Roy, Vidya Kochat, Thakur Prasad Yadav, Nilay K. Mukhopadhyay, Douglas Soares Galvão, Cristiano F. Woellner, Chandra Sekhar Tiwary
Non-noble nanomaterial-based quasicrystals (QC) are attractive structures due to their potential surface plasmon resonance (SPR) properties and ability to be easily exfoliated into two-dimensional (2D) sheets. Interaction with and sensing of organic molecules are applications where such 2D materials are a viable option due to their large surface area to volume ratio, providing abundant active sites for molecular interactions. In this work, a titanium-based multicomponent alloy (Ti45Zr38Ni17) was exfoliated into a 2D quasicrystal (2D-Ti QC) from its bulk form via liquid-phase exfoliation. Structural and optical experimental techniques were used to characterize the 2D-Ti QC. Its plasmonic nature was verified and demonstrated via the absorbance spectrum, light localization images, and far-field diffraction patterns. Dopamine sensing was demonstrated using the absorbance spectra of optically active 2D-Ti QC. The linear range of detection was obtained as ∼13–91 nM (200–1400 ppb). Molecular dynamics (MD) simulations of Ti QC were conducted to investigate its structural stability. The interaction between 2D-Ti QC and dopamine was investigated by using DFT simulations. In this way, the potential of 2D-Ti QC to be used as an organic molecule sensor has been experimentally and theoretically demonstrated.
{"title":"Plasmonically Active Atomically Thin Titanium-Based Quasicrystals for Dopamine Sensing","authors":"Nabarun Mandal, Aelton Baptista Santos, Anyesha Chakraborty, Suman Sarkar, Rahul Rao, Nicholas R. Glavin, Ajit K. Roy, Vidya Kochat, Thakur Prasad Yadav, Nilay K. Mukhopadhyay, Douglas Soares Galvão, Cristiano F. Woellner, Chandra Sekhar Tiwary","doi":"10.1021/acsanm.4c02268","DOIUrl":"https://doi.org/10.1021/acsanm.4c02268","url":null,"abstract":"Non-noble nanomaterial-based quasicrystals (QC) are attractive structures due to their potential surface plasmon resonance (SPR) properties and ability to be easily exfoliated into two-dimensional (2D) sheets. Interaction with and sensing of organic molecules are applications where such 2D materials are a viable option due to their large surface area to volume ratio, providing abundant active sites for molecular interactions. In this work, a titanium-based multicomponent alloy (Ti<sub>45</sub>Zr<sub>38</sub>Ni<sub>17</sub>) was exfoliated into a 2D quasicrystal (2D-Ti QC) from its bulk form via liquid-phase exfoliation. Structural and optical experimental techniques were used to characterize the 2D-Ti QC. Its plasmonic nature was verified and demonstrated via the absorbance spectrum, light localization images, and far-field diffraction patterns. Dopamine sensing was demonstrated using the absorbance spectra of optically active 2D-Ti QC. The linear range of detection was obtained as ∼13–91 nM (200–1400 ppb). Molecular dynamics (MD) simulations of Ti QC were conducted to investigate its structural stability. The interaction between 2D-Ti QC and dopamine was investigated by using DFT simulations. In this way, the potential of 2D-Ti QC to be used as an organic molecule sensor has been experimentally and theoretically demonstrated.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141525261","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}
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