{"title":"Nanoparticles of Ru on RuO2 from Pyrolysis of Ru-MOFs for Catalytic Hydrogenation","authors":"Jun Xie, Yanxu Ma, Jiazhen Shi, Yuan Xu, Hua Cheng, Meng Gao, Kunhua Wang, Meili Guan, Liangmin Ning, Hao Yu","doi":"10.1021/acsanm.4c04033","DOIUrl":"https://doi.org/10.1021/acsanm.4c04033","url":null,"abstract":"The domain-limited catalyst, with its unique design of encapsulating active sites within nanoscale domains, significantly enhances catalytic efficiency and selectivity, while improving the stability and recyclability of the catalyst, which holds great significance for industrial applications. This paper presents a design strategy for a Ru-RuO<sub>2</sub>/N–C domain-limited catalyst. This catalyst utilizes the porous structure of metal–organic frameworks (ZJU-100) to optimize the stability and selectivity of the ruthenium active site through spatial confinement effects. During the preparation process, the ruthenium complex (Ru(bpy)<sub>3</sub>Cl<sub>2</sub>·6H<sub>2</sub>O) is first introduced in situ into the synthetic system of ZJU-100 (Zn-MOFs), followed by high-temperature pyrolysis of the precursor at 900 °C. In this process, the zinc metal nodes in the MOFs are reduced and evaporated, while the nitrogen from the ruthenium complex and the carbon from the MOFs framework confine the growth and distribution of ruthenium species, resulting in a uniform particle size distribution of 2–5 nm. The presence of Ru(0) and RuO<sub>2</sub> species in the catalyst is confirmed through XPS and HRTEM characterizations. This structural characteristic greatly promotes the selective hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). Further studies reveal the reaction mechanism, finding that the formation of Ru–O bonds and the modulation of the oxidation state of ruthenium atoms play a crucial role in the catalytic activity of ruthenium catalysts. This provides an important theoretical foundation for designing efficient and stable ruthenium-based catalysts.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142267689","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}
{"title":"Manganese and Cobalt Heterostructures in Carbon Aerogels for the Improved Electrochemical Performance of Supercapacitors","authors":"Xiaochan Liu, Tingwei Wang, Xibin Yi, Jing Zhang, Xinfu Zhao, Sijia Liu, Sheng Cui","doi":"10.1021/acsanm.4c01802","DOIUrl":"https://doi.org/10.1021/acsanm.4c01802","url":null,"abstract":"The structural characteristics of electrodes are very important for supercapacitors (SCs) to improve their performance. Introducing transition metals in carbon aerogels (CAs) is an effective way to boost the application of supercapacitors. We develop a simple method to introduce two kinds of transition metals in a CA in one synthesis step, denoted MnCo/CA. There are small-sized Co nanocrystals and MnO<sub>2</sub> generated in situ, which not only produce abundant heterointerfaces but also enhance the specific surface area of the CA. Thanks to hierarchical porous structures and various MnO<sub>2</sub>/Co/C heterostructure interfaces, the obtained MnCo/CA nanomaterials exhibit an excellent capacitance of 395.9 ± 5.0% F/g under 1.0 A/g, an outstanding rate capacity of 130.8 ± 3.0% F/g under 25.0 A/g, and a superior cycle life of 74.0% after 5000 cycles. Noticeably, benefiting from synergistic effects among metallic cobalt, manganese oxide, and CA, the MnCo/CA//MnCo/CA double-electrode supercapacitor presents a large voltage window (2.5 V) and then reaches a higher energy density of 63.1 ± 1.0% Wh/kg at 312.5 ± 5.0% W/kg. This research emphasizes the synergy effect between metal/metal and metal/carbon in CAs, which offers a simple way for advanced SC electrode materials.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142267601","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}
{"title":"Correction to “Cu-Doped CsPb2Br5 Nanocrystals for Soft Crystal Lattice-Induced Self-Trapped Excitonic Emission: Implications for Solid-State Lighting”","authors":"Yubin Zhao, Xing Cao, Huanhui Chen, Ya Liu, Liubiao Zhong, Yejun Qiu","doi":"10.1021/acsanm.4c05081","DOIUrl":"https://doi.org/10.1021/acsanm.4c05081","url":null,"abstract":"In our original article, on page 18949, the authors discovered a mistake in the caption of Figure 5c–e. The caption should refer to CsPbBr<sub>3</sub> and Cu/CsPbBr<sub>3</sub>, not CsPb<sub>2</sub>Br<sub>5</sub> and Cu/CsPb<sub>2</sub>Br<sub>5</sub>. The modified caption is below: Figure 5. (a) Emission spectra and (b) XRD patterns of Cu/CsPbBr<sub>3</sub> NCs before and after (Cu/CsPb<sub>2</sub>Br<sub>5</sub>) adding water at room temperature. (c–e) Schematic diagrams of the design of three possible anticounterfeiting modes through introducing different treatment solutions of H<sub>2</sub>O and CuBr<sub>2</sub> based on different material routes: (c) CsPbBr<sub>3</sub> NCs for HITSZ, (d) Cu/CsPbBr<sub>3</sub> NCs for HITSZ, and (e) a mixture of CsPbBr<sub>3</sub> NCs for HIT and Cu/CsPbBr<sub>3</sub> NCs for SZ. This correction does not affect the conclusions of the work. The authors apologize for the mistake. This article has not yet been cited by other publications.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142267699","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}
{"title":"Li-Doped NaYF4:Ho,Yb Upconversion Nanoparticles for Chemotherapy and Radionuclide Therapy of Cancer","authors":"Ruchi Agrawal, Sourav Patra, Sandeep Balu Shelar, Chandan Kumar, Manas Srivastava, Sudipta Chakraborty* and Raghumani Singh Ningthoujam*, ","doi":"10.1021/acsanm.4c0377710.1021/acsanm.4c03777","DOIUrl":"https://doi.org/10.1021/acsanm.4c03777https://doi.org/10.1021/acsanm.4c03777","url":null,"abstract":"<p >Highly luminescent, biocompatible, and water-dispersible monodispersed NaYF<sub>4</sub>:Ho,Yb,Li (YHYL) upconversion nanoparticles (NPs) entrapped into mesoporous silica (YHYL@m-SiO<sub>2</sub>) have been prepared. The surface area of YHYL@m-SiO<sub>2</sub> NPs is found to be 128 m<sup>2</sup>/g with pore sizes of 3–4 nm. To illustrate the use of these YHYL@m-SiO<sub>2</sub> NPs as drug (DOX) carriers, an in-depth analysis is conducted. In order to use these nanoparticles for targeted cancer therapy, folic acid (FA) is also chemically conjugated to them. The affinity of YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs with folate receptors (FRs) are proved by <i>in vitro</i> studies. To demonstrate the potential utility of DOX-loaded and folic acid–conjugated nanoparticles (YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs) in targeted radionuclide therapy, these NPs are radiolabeled with <sup>177</sup>Lu, a β<sup>–</sup>-emitting radionuclide [<i>T</i><sub>1/2</sub>= 6.65 d, <i>E</i><sub>β</sub>(max) = 497 keV, <i>E</i><sub>γ</sub> = 113 keV (6.4%), 208 keV (11%)] extensively used for targeted radionuclide therapy. It is experimentally established that the adsorption of <sup>177</sup>Lu on YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs follows a combination of Langmuir and Freundlich isotherm models and pseudo-second-order kinetics. Cell toxicity and apoptotic cell death studies are conducted for [<sup>177</sup>Lu]Lu-YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs in the MCF-7 cell line, which demonstrated the therapeutic potential of the radiolabeled and drug-loaded formulation in an <i>in vitro</i> model. Overall, the syntheses of YHYL@m-SiO<sub>2</sub>, YHYL@m-SiO<sub>2</sub>-DOX, YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX and [<sup>177</sup>Lu]Lu-YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs, their physicochemical characterization, and their potential applications in combination cancer therapy have been amply demonstrated.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.3,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326018","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}
{"title":"Density Functional Theory and Machine Learning of Transition Metals in Mo2C for Gas Sensors","authors":"Weiguang Huang, Zhongzhou Dong* and Long Lin, ","doi":"10.1021/acsanm.4c0427410.1021/acsanm.4c04274","DOIUrl":"https://doi.org/10.1021/acsanm.4c04274https://doi.org/10.1021/acsanm.4c04274","url":null,"abstract":"<p >Gas accumulation is the primary cause of explosions in underground mines, and preventing it requires effective gas detection. To address this, we propose an approach combining machine learning (ML) and density functional theory (DFT) for designing nanoscale gas sensors. Our study demonstrates that a back-propagation neural network (BPNN) model, optimized with suitable hyperparameters, achieves high accuracy with an R<sup>2</sup> (coefficient of determination) of 0.92 and a low RMSE (root-mean-square error) of 0.24 in predicting the substrate material formed by transition metal (TM)-doped Mo<sub>2</sub>C and its interaction with key gas molecules (CO, H<sub>2</sub>S, CH<sub>4</sub>, and C<sub>2</sub>H<sub>6</sub>). Based on these interaction strengths, we have analyzed the materials in more depth. Additionally, we find that certain features directly affect the increase or decrease of interaction strengths within a specific range, providing insights that contribute to the design of more efficient nanoscale sensors.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.3,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326014","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}
{"title":"Label-free Biosensing Using Hybrid Plasmonic Substrates Generated via Nanosphere Lithography","authors":"Elif Lulek, Arif E. Cetin, Yavuz Nuri Ertas","doi":"10.1021/acsanm.4c03945","DOIUrl":"https://doi.org/10.1021/acsanm.4c03945","url":null,"abstract":"The rapid advancement of air/water interface coatings transcends multiple domains. These coatings, valued for expansive coverage, facile acquisition, and economic efficiency, hold pivotal roles in nanosurface engineering. Conventional approaches to achieving 2D periodic structures, such as electron-beam lithography, suffer from cost and complexity challenges. Nanosphere lithography presents an alternative avenue by harnessing the inherent self-assembly propensity of colloidal nanoparticles and offers simplicity, cost-effectiveness, and compatibility with various techniques. The use of nanosphere lithography in coating metal templates gains traction in plasmonics because of its simplicity and speed. The fusion of plasmonics and biosensing enables label-free detection with unprecedented sensitivity, revolutionizing areas such as medicine, diagnostics, and environmental monitoring. In the realm of label-free biosensing, attaining uniform large-area fabrication is critical for robust sensing signals. Detecting spectral variations in low analyte concentrations necessitates a precise response profile. The creation of a potent and accessible local electromagnetic field is vital for enhancing light–biomolecule interactions. We introduce a hybrid plasmonic substrate via nanosphere lithography, combining antenna and aperture responses. The hybrid plasmonic design caters to the prerequisites of efficient label-free biosensing, uniform large-scale fabrication, narrow spectral response, and strong local electromagnetic fields. The hybrid plasmonic substrate promises to advance label-free biosensing capabilities by integrating antenna and aperture responses, facilitating sensitive and robust biosensing applications. Demonstrating these parameters resulted in a high refractive index sensitivity of up to 553 nm/RIU. The hybrid nature further facilitated an impressive detection limit of 0.5 ng/mL for label-free protein IgG detection.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142267602","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}
Wei-Long Xu, Erwei Du, Sisi Pang, Yuebin Lian, Min Zheng
{"title":"Construction of ZnO/C3N4 Composite for Photocatalytic Activity through Charge Transfer","authors":"Wei-Long Xu, Erwei Du, Sisi Pang, Yuebin Lian, Min Zheng","doi":"10.1021/acsanm.4c04416","DOIUrl":"https://doi.org/10.1021/acsanm.4c04416","url":null,"abstract":"The photocatalyst based on the ZnO/C<sub>3</sub>N<sub>4</sub> composite can harness the high carrier mobility of ZnO along with the visible light absorption characteristics of C<sub>3</sub>N<sub>4</sub>. The key to enhance photocatalytic performance through the synergistic effect of these two materials lies in the effective charge transfer. In this work, a combination of ultrasonic dispersion and hydrothermal method was employed to prepare a ZnO/C<sub>3</sub>N<sub>4</sub> composite. The structure of this composite consists of C<sub>3</sub>N<sub>4</sub> thin layers covering ZnO nanoparticles with a size of several tens of nanometers. Theoretical calculations combined with photoluminescence spectroscopy techniques confirmed that charge transfer occurs in ZnO/C<sub>3</sub>N<sub>4</sub> staggered gap heterojunction, which reduces the recombination of photogenerated carriers and enhances the photocatalytic efficiency. The variations of charge-transfer efficiency in different regions of the ZnO/C<sub>3</sub>N<sub>4</sub> composite were observed by spatially and temporally resolved fluorescence imaging measurements. The photocatalytic degradation of pollutants revealed that the optimal amount of C<sub>3</sub>N<sub>4</sub> is 8%. It achieved an impressive 88% degradation efficiency of the pollutant within 100 min and the fastest degradation rate of 0.022 min<sup>–1</sup> under the solar simulator. This high efficiency is closely associated with the tight integration between ZnO and C<sub>3</sub>N<sub>4</sub> and their effective charge-transfer rates. Furthermore, the ZnO/C<sub>3</sub>N<sub>4</sub> composite demonstrated a stable photocatalytic performance.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142267697","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}
{"title":"Li-Doped NaYF4:Ho,Yb Upconversion Nanoparticles for Chemotherapy and Radionuclide Therapy of Cancer","authors":"Ruchi Agrawal, Sourav Patra, Sandeep Balu Shelar, Chandan Kumar, Manas Srivastava, Sudipta Chakraborty, Raghumani Singh Ningthoujam","doi":"10.1021/acsanm.4c03777","DOIUrl":"https://doi.org/10.1021/acsanm.4c03777","url":null,"abstract":"Highly luminescent, biocompatible, and water-dispersible monodispersed NaYF<sub>4</sub>:Ho,Yb,Li (YHYL) upconversion nanoparticles (NPs) entrapped into mesoporous silica (YHYL@m-SiO<sub>2</sub>) have been prepared. The surface area of YHYL@m-SiO<sub>2</sub> NPs is found to be 128 m<sup>2</sup>/g with pore sizes of 3–4 nm. To illustrate the use of these YHYL@m-SiO<sub>2</sub> NPs as drug (DOX) carriers, an in-depth analysis is conducted. In order to use these nanoparticles for targeted cancer therapy, folic acid (FA) is also chemically conjugated to them. The affinity of YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs with folate receptors (FRs) are proved by <i>in vitro</i> studies. To demonstrate the potential utility of DOX-loaded and folic acid–conjugated nanoparticles (YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs) in targeted radionuclide therapy, these NPs are radiolabeled with <sup>177</sup>Lu, a β<sup>–</sup>-emitting radionuclide [<i>T</i><sub>1/2</sub>= 6.65 d, <i>E</i><sub>β</sub>(max) = 497 keV, <i>E</i><sub>γ</sub> = 113 keV (6.4%), 208 keV (11%)] extensively used for targeted radionuclide therapy. It is experimentally established that the adsorption of <sup>177</sup>Lu on YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs follows a combination of Langmuir and Freundlich isotherm models and pseudo-second-order kinetics. Cell toxicity and apoptotic cell death studies are conducted for [<sup>177</sup>Lu]Lu-YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs in the MCF-7 cell line, which demonstrated the therapeutic potential of the radiolabeled and drug-loaded formulation in an <i>in vitro</i> model. Overall, the syntheses of YHYL@m-SiO<sub>2</sub>, YHYL@m-SiO<sub>2</sub>-DOX, YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX and [<sup>177</sup>Lu]Lu-YHYL@m-SiO<sub>2</sub>-NH<sub>2</sub>-FA-DOX NPs, their physicochemical characterization, and their potential applications in combination cancer therapy have been amply demonstrated.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269655","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}
Rifat Hasan Rupom, Md Nurul Islam, Zoriana Demchuk, Rigoberto Advincula, Narendra B. Dahotre, Yijie Jiang, Wonbong Choi
{"title":"Tailoring Piezoelectricity of 3D Printing PVDF-MoS2 Nanocomposite via In Situ Induced Shear Stress","authors":"Rifat Hasan Rupom, Md Nurul Islam, Zoriana Demchuk, Rigoberto Advincula, Narendra B. Dahotre, Yijie Jiang, Wonbong Choi","doi":"10.1021/acsanm.4c03695","DOIUrl":"https://doi.org/10.1021/acsanm.4c03695","url":null,"abstract":"3D printing of unique structures with tunable properties offers significant advantages in the fabrication of complex and customized electronic devices. This study introduces a process-microstructure–property-guided manufacturing route to fabricate PVDF-2D MoS<sub>2</sub> piezoelectric nanocomposites with tunable piezoelectric properties without having a postprocess. We control PVDF’s microstructure through direct ink writing (DIW) 3D printing while tuning PVDF-MoS<sub>2</sub> interfacial strain by controlling rheology and 3D printing parameters, such as nozzle size and printing speed. Our approach demonstrates tunable piezoelectricity in PVDF-MoS<sub>2</sub>, achieving a 15-fold increase in the piezoelectric coefficient (d<sub>33</sub>) at a printing-induced shear stress of 6685 Pa. This enhancement arises from the electrostatic interactions between PVDF and MoS<sub>2</sub> and the filler distribution and alignment caused by the in situ shear stress in 3D printing, as confirmed by XPS and Raman mapping analyses. Our findings advance the understanding of piezoelectric mechanisms in PVDF-based nanocomposites, laying the foundation for 3D printing of piezoelectric sensors in wearable device applications with enhanced performance and customization capabilities.","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269646","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}