Applied Surface Science Advances最新文献

Structural features of graphene and silver functionalized graphene oxide loaded with perfluorinated compounds during thermal heating

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-03-01 DOI: 10.1016/j.apsadv.2025.100720

M. Mancinelli , L. Adami , L. Gigli , N.C.O. Sousa , J.J. Pedrotti , J. Plaisier , L. Pasti , C. Stevanin , A. Martucci

Perfluorinated substances (PFAS) are environmental pollutants that are difficult to break down chemically, thermally, or biologically. Due to its aqueous dispersibility, reactivity, high stability, flexibility, and economical synthesis, graphene oxide (GO) has been extensively researched in water purification. Adsorption is the most efficient and cost-efficient approach for PFAS removal from aqueous environments. Layered graphene-based materials have demonstrated a strong capacity for binding cationic ions and the capacity to build bridges between their deprotonated functional groups on the surface and anionic species like PFAS. In the present work, in situ powder diffraction data were collected as a function of time in temperature ramp up to 400 °C to explore the real-time evolution of the GO crystal structure before and after Ag functionalization and perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) loading. The PFOA and PFOS loading in the GO structure is mainly revealed by the (001) peak shift to greater 2θ values due to PFOA and PFOS interaction with GO interlayers and consequently decreasing of d-spacing distance. Around 150 °C, functional groups are expelled, structural defects are formed, and the (001, 2Θ≈10°) GO characteristic peak migrates. This is followed by a contraction that is accompanied by a reduction in d-spacing. At 350 °C, the reflection (001) disappears and the peak intensity of (002) increases, indicating that GO has been converted to reduced graphene oxide (rGO). The temperature at which PFOA and PFOS molecules degrade is between 375 and 400 °C, according to the GO-PFOA and GO-PFOS patterns. GO and AgGO samples underwent a partial but significant reduction at 400 °C. In the presence of silver, the dhkl values decrease (AgGO-PFOA, AgGO-PFOS < AgGO < GO-PFOA, GO-PFOS < GO). The above process found further confirmation when compared with the thermal analysis indicating that the thermal decomposition of GO and AgGO loaded with PFOA, PFOS is a multi-step reaction. Furthermore, differences in both shape and peak position for the DTA and DTG peaks also indicated that the thermal stability of PFOA was lower compared with PFOS. This information will help design an easy method based on graphene-Ag nanocomposites for removing hazardous perfluorinated contaminants from water and wastewater.

{"title":"Structural features of graphene and silver functionalized graphene oxide loaded with perfluorinated compounds during thermal heating","authors":"M. Mancinelli , L. Adami , L. Gigli , N.C.O. Sousa , J.J. Pedrotti , J. Plaisier , L. Pasti , C. Stevanin , A. Martucci","doi":"10.1016/j.apsadv.2025.100720","DOIUrl":"10.1016/j.apsadv.2025.100720","url":null,"abstract":"<div><div>Perfluorinated substances (PFAS) are environmental pollutants that are difficult to break down chemically, thermally, or biologically. Due to its aqueous dispersibility, reactivity, high stability, flexibility, and economical synthesis, graphene oxide (GO) has been extensively researched in water purification. Adsorption is the most efficient and cost-efficient approach for PFAS removal from aqueous environments. Layered graphene-based materials have demonstrated a strong capacity for binding cationic ions and the capacity to build bridges between their deprotonated functional groups on the surface and anionic species like PFAS. In the present work, <em>in situ</em> powder diffraction data were collected as a function of time in temperature ramp up to 400 °C to explore the real-time evolution of the GO crystal structure before and after Ag functionalization and perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) loading. The PFOA and PFOS loading in the GO structure is mainly revealed by the (001) peak shift to greater 2θ values due to PFOA and PFOS interaction with GO interlayers and consequently decreasing of <span>d</span>-spacing distance. Around 150 °C, functional groups are expelled, structural defects are formed, and the (001, 2Θ≈10°) GO characteristic peak migrates. This is followed by a contraction that is accompanied by a reduction in <span>d</span>-spacing. At 350 °C, the reflection (001) disappears and the peak intensity of (002) increases, indicating that GO has been converted to reduced graphene oxide (rGO). The temperature at which PFOA and PFOS molecules degrade is between 375 and 400 °C, according to the GO-PFOA and GO-PFOS patterns. GO and AgGO samples underwent a partial but significant reduction at 400 °C. In the presence of silver, the <em>dhkl</em> values decrease (AgGO-PFOA, AgGO-PFOS < AgGO < GO-PFOA, GO-PFOS < GO). The above process found further confirmation when compared with the thermal analysis indicating that the thermal decomposition of GO and AgGO loaded with PFOA, PFOS is a multi-step reaction. Furthermore, differences in both shape and peak position for the DTA and DTG peaks also indicated that the thermal stability of PFOA was lower compared with PFOS. This information will help design an easy method based on graphene-Ag nanocomposites for removing hazardous perfluorinated contaminants from water and wastewater.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100720"},"PeriodicalIF":7.5,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Influence of pretreatments on the surface charge of anode and cathode materials in spent lithium-ion batteries - a key point for recycling

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-22 DOI: 10.1016/j.apsadv.2025.100719

Sabereh Nazari , Pengxin Su , Jinlong Li , Yaqun He , Chenlong Duan , Saeed Chehreh Chelgani

The flotation process for separating anode and cathode materials (blackmass) is a critical step in recycling lithium-ion batteries (LIBs), particularly before the extraction of lithium-bearing materials. Surface electric charge, measured via zeta potential, plays a pivotal role in the flotation separation of these electrode materials. The pH, roasting temperature, thermal treatment duration, and bubbles' presence can significantly influence these materials' surface properties. However, a comprehensive investigation addressing the combined effects of these factors on the zeta potential of electrode active materials is still lacking. This study aims to bridge this gap by systematically exploring the effects of pH (4.5, 7, and 10.5), roasting temperatures (0–500 °C), varied thermal treatment times (1 to 2 h), and the presence or absence of bubbles (nano and microbubbles) on the zeta potential of both anode and cathode materials. The study also examines the impact of conditioning with n-dodecane, a typical flotation collector. While zeta potential is largely pH-dependent, roasting temperature significantly influences surface charge, whereas thermal treatment duration has a minimal effect. Notably, the most considerable zeta potential difference (28.3 mV) between the anode (-18.63 mV) and cathode (9.67 mV) surfaces occurred in the absence of both collector and bubbles, at pH 7, 500 °C, and a thermal treatment time of 2 h. Under conditioning involving bubbles and collector, the highest difference observed was 2.21 mV at pH 7, 250 °C, and 1 h of thermal treatment. These findings contribute to a deeper understanding of surface charge behavior in LIB recycling processes, with implications for improving flotation separation efficiency through surface science and engineering.

{"title":"Influence of pretreatments on the surface charge of anode and cathode materials in spent lithium-ion batteries - a key point for recycling","authors":"Sabereh Nazari , Pengxin Su , Jinlong Li , Yaqun He , Chenlong Duan , Saeed Chehreh Chelgani","doi":"10.1016/j.apsadv.2025.100719","DOIUrl":"10.1016/j.apsadv.2025.100719","url":null,"abstract":"<div><div>The flotation process for separating anode and cathode materials (blackmass) is a critical step in recycling lithium-ion batteries (LIBs), particularly before the extraction of lithium-bearing materials. Surface electric charge, measured via zeta potential, plays a pivotal role in the flotation separation of these electrode materials. The pH, roasting temperature, thermal treatment duration, and bubbles' presence can significantly influence these materials' surface properties. However, a comprehensive investigation addressing the combined effects of these factors on the zeta potential of electrode active materials is still lacking. This study aims to bridge this gap by systematically exploring the effects of pH (4.5, 7, and 10.5), roasting temperatures (0–500 °C), varied thermal treatment times (1 to 2 h), and the presence or absence of bubbles (nano and microbubbles) on the zeta potential of both anode and cathode materials. The study also examines the impact of conditioning with n-dodecane, a typical flotation collector. While zeta potential is largely pH-dependent, roasting temperature significantly influences surface charge, whereas thermal treatment duration has a minimal effect. Notably, the most considerable zeta potential difference (28.3 mV) between the anode (-18.63 mV) and cathode (9.67 mV) surfaces occurred in the absence of both collector and bubbles, at pH 7, 500 °C, and a thermal treatment time of 2 h. Under conditioning involving bubbles and collector, the highest difference observed was 2.21 mV at pH 7, 250 °C, and 1 h of thermal treatment. These findings contribute to a deeper understanding of surface charge behavior in LIB recycling processes, with implications for improving flotation separation efficiency through surface science and engineering.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100719"},"PeriodicalIF":7.5,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143465498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Localized creation of bubble domains in Fe3GaTe2 by conductive atomic force microscopy

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-22 DOI: 10.1016/j.apsadv.2025.100718

Chak-Ming Liu , Yi-Jia Liu , Po-Chun Chang , Po-Wei Chen , Masahiro Haze , Ming-Hsien Hsu , Neleena Nair Gopakumar , Yishui Zhou , Yung-Hsiang Tung , Sabreen Hammouda , Chao-Hung Du , Yukio Hasegawa , Yixi Su , Hsiang-Chih Chiu , Wen-Chin Lin

This study demonstrates the localized creation of bubble domains in the two-dimensional (2D) ferromagnetic material Fe₃GaTe₂ using conductive atomic force microscopy. By applying bias voltage to the tip under a perpendicular magnetic field, sufficient current is generated to induce localized Joule heating, transforming random stripe domains into bubble domains. The bubble domains were successfully induced under ambient conditions at room temperature and remained stable, as confirmed by magnetic force microscopy. For Fe₃GaTe₂ layers with thicknesses of 1 μm, 200 nm, and 100 nm, the average diameters of bubble domains were measured at 620 ± 100 nm, 325 ± 80 nm, and 230 ± 70 nm, respectively, approximately 20 % larger than the pristine stripe width. By optimizing parameters such as bias voltage, application duration, and tip temperature based on Fe₃GaTe₂ thickness, the induced bubble domain density could be precisely controlled, ranging from few bubble domains within areas < 5 μm² to nearly 10⁴ bubble domains within 1200 μm². Furthermore, multi-point triggering demonstrated the re-writability of the domain structures, with non-overlapping domains remaining unaffected. These findings offer critical insights into the tunability of magnetic textures in 2D ferromagnets, providing a foundation for developing next-generation spintronic devices based on 2D heterostructures.

{"title":"Localized creation of bubble domains in Fe3GaTe2 by conductive atomic force microscopy","authors":"Chak-Ming Liu , Yi-Jia Liu , Po-Chun Chang , Po-Wei Chen , Masahiro Haze , Ming-Hsien Hsu , Neleena Nair Gopakumar , Yishui Zhou , Yung-Hsiang Tung , Sabreen Hammouda , Chao-Hung Du , Yukio Hasegawa , Yixi Su , Hsiang-Chih Chiu , Wen-Chin Lin","doi":"10.1016/j.apsadv.2025.100718","DOIUrl":"10.1016/j.apsadv.2025.100718","url":null,"abstract":"<div><div>This study demonstrates the localized creation of bubble domains in the two-dimensional (2D) ferromagnetic material Fe₃GaTe₂ using conductive atomic force microscopy. By applying bias voltage to the tip under a perpendicular magnetic field, sufficient current is generated to induce localized Joule heating, transforming random stripe domains into bubble domains. The bubble domains were successfully induced under ambient conditions at room temperature and remained stable, as confirmed by magnetic force microscopy. For Fe₃GaTe₂ layers with thicknesses of 1 μm, 200 nm, and 100 nm, the average diameters of bubble domains were measured at 620 ± 100 nm, 325 ± 80 nm, and 230 ± 70 nm, respectively, approximately 20 % larger than the pristine stripe width. By optimizing parameters such as bias voltage, application duration, and tip temperature based on Fe₃GaTe₂ thickness, the induced bubble domain density could be precisely controlled, ranging from few bubble domains within areas < 5 μm² to nearly 10⁴ bubble domains within 1200 μm². Furthermore, multi-point triggering demonstrated the re-writability of the domain structures, with non-overlapping domains remaining unaffected. These findings offer critical insights into the tunability of magnetic textures in 2D ferromagnets, providing a foundation for developing next-generation spintronic devices based on 2D heterostructures.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100718"},"PeriodicalIF":7.5,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143464951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Prussian blue nanocubes growth by electrochemical deposition on sulfur-doped graphene as nanozyme: Optimization and application in the field of environmental sensors

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-21 DOI: 10.1016/j.apsadv.2025.100716

Oana Brincoveanu , Elisabeta-Irina Geana , Cosmin Romanitan , Cristina Pachiu , Alexandra Mocanu , Sabrina State , Adi Ghebaur , Sevinc Kurbanoglu , Gregor Marolt , Livia Alexandra Dinu

This study presents the electrochemical deposition of Prussian blue (PB) nanomaterial on top of a sulfur-doped graphene (S-Gr) drop-casted on a screen-printed carbon working electrode (SPCE) for the development of environmental sensing devices with higher sensitivity to phenolic pollutants. The deposition process was optimized by carefully controlling the deposition parameters to achieve PB nanocubes (PBNCs) with an average size of ∼ 50 nm. The resulting nanocomposite material, PBNCs-S-Gr, was evaluated for the electrooxidation of hydroquinone (HQ), a widely studied phenolic compound, to demonstrate its catalytic activity in oxidizing phenolic substrates, effectively mimicking the enzymatic behavior of natural peroxidase. The obtained PBNCs-S-Gr/SPCE presented a calculated limit of detection (LOD) of 0.33 nM and an increased sensitivity of 1.5 µA × M^-1, with a wide linear concentration range from 0.001 to 10 µM for HQ detection. Notably, the recovery values obtained for surface water samples fall within the range of 92.1 % to 98.9 %, indicating strong agreement with results derived from the standard method, ultra high-performance liquid chromatography system with diode array detection (UHPLC-DAD).

{"title":"Prussian blue nanocubes growth by electrochemical deposition on sulfur-doped graphene as nanozyme: Optimization and application in the field of environmental sensors","authors":"Oana Brincoveanu , Elisabeta-Irina Geana , Cosmin Romanitan , Cristina Pachiu , Alexandra Mocanu , Sabrina State , Adi Ghebaur , Sevinc Kurbanoglu , Gregor Marolt , Livia Alexandra Dinu","doi":"10.1016/j.apsadv.2025.100716","DOIUrl":"10.1016/j.apsadv.2025.100716","url":null,"abstract":"<div><div>This study presents the electrochemical deposition of Prussian blue (PB) nanomaterial on top of a sulfur-doped graphene (S-Gr) drop-casted on a screen-printed carbon working electrode (SPCE) for the development of environmental sensing devices with higher sensitivity to phenolic pollutants. The deposition process was optimized by carefully controlling the deposition parameters to achieve PB nanocubes (PBNCs) with an average size of ∼ 50 nm. The resulting nanocomposite material, PBNCs-S-Gr, was evaluated for the electrooxidation of hydroquinone (HQ), a widely studied phenolic compound, to demonstrate its catalytic activity in oxidizing phenolic substrates, effectively mimicking the enzymatic behavior of natural peroxidase. The obtained PBNCs-S-Gr/SPCE presented a calculated limit of detection (LOD) of 0.33 nM and an increased sensitivity of 1.5 µA × <em>M</em><sup>-1</sup>, with a wide linear concentration range from 0.001 to 10 µM for HQ detection. Notably, the recovery values obtained for surface water samples fall within the range of 92.1 % to 98.9 %, indicating strong agreement with results derived from the standard method, ultra high-performance liquid chromatography system with diode array detection (UHPLC-DAD).</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100716"},"PeriodicalIF":7.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143453339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Morphology-dependent near-infrared photothermal activity of plasmonic TiN nanobars and nanospheres for anticancer, antibacterial therapy and deep in vivo photoacoustic imaging

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-20 DOI: 10.1016/j.apsadv.2025.100713

Katerina Polakova , Sourav Rej , Sarka Hradilova , Jan Belza , Tomas Malina , Katerina Barton Tomankova , Renata Vecerova , Petr Matous , Petr Paral , Ariana Opletalova , Jana Soukupova , Tomas Pluhacek , Ludek Sefc , Radek Zboril , Stepan Kment , Alberto Naldoni

Plasmonic titanium nitride (TiN) nanoparticles are emerging nanomaterials possessing several orders of magnitude higher absorption cross section, but also exhibit higher photostability compared to conventional photosenzitizers. In the recent years, TiN has emerged as a highly effective electrocatalytic and environmentally friendly material with good biocompatibility. Its unique physicochemical properties and cost-effectiveness are essential for wide utilization in biomedicine. However, the effect of morphology of TiN on the photothermal therapy (PTT) efficiency has not been studied yet. Here, TiN nanocrystals of two precisely defined morphologies - nanobars and nanospheres - were prepared by unique pseudomorphic conversion of TiO₂ nanowires and nanospheres via nitridation at 800 °C. Due to their multiple plasmonic resonances, the resulting materials show broad optical absorption spanning the entire solar spectrum and biological window including the NIR-I (750 – 1000 nm) and NIR-II (1000 – 1350 nm). Using low power illumination 318 mW/cm² and NIR LED irradiation 940 nm, we observed a morphology-dependent PTT bioactivity, with the TiN nanobars being more efficient in cancer HeLa cells killing, while nanospheres showed higher antimicrobial activity toward Staphylococcus aureus and Escherichia coli bacteria strains. Moreover, acute and long-term in vitro biocompatibility together with in vivo monitoring of biodistribution showing enhanced permeability and retention (EPR) effect were confirmed by photoacoustic (PA) imaging in tumor bearing mice (C57BL/6J albino, EL4 lymphoma cell line). Thus, both TiN morphologies - nanobars and nanospheres are promising candidates in theranostic application via PTT therapy and PA imaging.

{"title":"Morphology-dependent near-infrared photothermal activity of plasmonic TiN nanobars and nanospheres for anticancer, antibacterial therapy and deep in vivo photoacoustic imaging","authors":"Katerina Polakova , Sourav Rej , Sarka Hradilova , Jan Belza , Tomas Malina , Katerina Barton Tomankova , Renata Vecerova , Petr Matous , Petr Paral , Ariana Opletalova , Jana Soukupova , Tomas Pluhacek , Ludek Sefc , Radek Zboril , Stepan Kment , Alberto Naldoni","doi":"10.1016/j.apsadv.2025.100713","DOIUrl":"10.1016/j.apsadv.2025.100713","url":null,"abstract":"<div><div>Plasmonic titanium nitride (TiN) nanoparticles are emerging nanomaterials possessing several orders of magnitude higher absorption cross section, but also exhibit higher photostability compared to conventional photosenzitizers. In the recent years, TiN has emerged as a highly effective electrocatalytic and environmentally friendly material with good biocompatibility. Its unique physicochemical properties and cost-effectiveness are essential for wide utilization in biomedicine. However, the effect of morphology of TiN on the photothermal therapy (PTT) efficiency has not been studied yet. Here, TiN nanocrystals of two precisely defined morphologies - nanobars and nanospheres - were prepared by unique pseudomorphic conversion of TiO<sub>2</sub> nanowires and nanospheres via nitridation at 800 °C. Due to their multiple plasmonic resonances, the resulting materials show broad optical absorption spanning the entire solar spectrum and biological window including the NIR-I (750 – 1000 nm) and NIR-II (1000 – 1350 nm). Using low power illumination 318 mW/cm<sup>2</sup> and NIR LED irradiation 940 nm, we observed a morphology-dependent PTT bioactivity, with the TiN nanobars being more efficient in cancer HeLa cells killing, while nanospheres showed higher antimicrobial activity toward <em>Staphylococcus aureus</em> and <em>Escherichia coli</em> bacteria strains. Moreover, acute and long-term <em>in vitro</em> biocompatibility together with <em>in vivo</em> monitoring of biodistribution showing enhanced permeability and retention (EPR) effect were confirmed by photoacoustic (PA) imaging in tumor bearing mice (C57BL/6J albino, EL4 lymphoma cell line). Thus, both TiN morphologies - nanobars and nanospheres are promising candidates in theranostic application via PTT therapy and PA imaging.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100713"},"PeriodicalIF":7.5,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444933","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rapid and sensitive melamine detection via paper-based surface-enhanced Raman scattering substrate: Plasma-assisted in situ growth of closely packed gold nanoparticles on cellulose paper

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-19 DOI: 10.1016/j.apsadv.2025.100717

Ba-Thong Trinh , Rashida Akter , Hanjun Cho , Oleksii Omelianovych , Kwanghyeon Jo , Hongki Kim , Taejoon Kang , Huu-Quang Nguyen , Jaebeom Lee , Kwanyong Seo , Ho-Suk Choi , Ilsun Yoon

Cellulose-paper-type surface-enhanced Raman scattering (SERS) substrates have shown promise for constructing economical high-performance molecular sensors. However, conventional paper-based SERS substrate fabrication methods are complex. Therefore, in this study, dry plasma reduction (DPR) – a simple and green process – was tailored to develop a paper-based SERS substrate featuring Au-nanoparticle (AuNP)-impregnated cellulose fiber surfaces. Au ions pre-adsorbed on fiber surfaces were reduced by abundant injected electrons and grown into AuNPs by high-energy Ar-ion bombardment during DPR. Fiber surfaces of the AuNP–cellulose paper, enriched with AuNPs having nanometer-scale gaps and SERS hotspots, exhibited broadband absorption and a large SERS enhancement factor of 1.7 × 10⁷. The SERS sensitivity of the AuNP–cellulose paper was leveraged to realize label-free sensing of melamine, an illegally added milk contaminant. The AuNP–cellulose paper not only exhibited a low detection limit (23 nM (2.9 ppb)) for melamine, adulterated in milk, after sample pretreatments but also enabled rapid detection of 0.2 ppm melamine in formula and low-fat milk within 30 s without any pretreatments, with the supports of principal component analysis (PCA) method. The AuNP–cellulose paper, cost-effective and permitting low-ppb-level label-free molecular sensing, can be a feasible SERS sensor for environmental and biomedical applications.

{"title":"Rapid and sensitive melamine detection via paper-based surface-enhanced Raman scattering substrate: Plasma-assisted in situ growth of closely packed gold nanoparticles on cellulose paper","authors":"Ba-Thong Trinh , Rashida Akter , Hanjun Cho , Oleksii Omelianovych , Kwanghyeon Jo , Hongki Kim , Taejoon Kang , Huu-Quang Nguyen , Jaebeom Lee , Kwanyong Seo , Ho-Suk Choi , Ilsun Yoon","doi":"10.1016/j.apsadv.2025.100717","DOIUrl":"10.1016/j.apsadv.2025.100717","url":null,"abstract":"<div><div>Cellulose-paper-type surface-enhanced Raman scattering (SERS) substrates have shown promise for constructing economical high-performance molecular sensors. However, conventional paper-based SERS substrate fabrication methods are complex. Therefore, in this study, dry plasma reduction (DPR) – a simple and green process – was tailored to develop a paper-based SERS substrate featuring Au-nanoparticle (AuNP)-impregnated cellulose fiber surfaces. Au ions pre-adsorbed on fiber surfaces were reduced by abundant injected electrons and grown into AuNPs by high-energy Ar-ion bombardment during DPR. Fiber surfaces of the AuNP–cellulose paper, enriched with AuNPs having nanometer-scale gaps and SERS hotspots, exhibited broadband absorption and a large SERS enhancement factor of 1.7 × 10<sup>7</sup>. The SERS sensitivity of the AuNP–cellulose paper was leveraged to realize label-free sensing of melamine, an illegally added milk contaminant. The AuNP–cellulose paper not only exhibited a low detection limit (23 nM (2.9 ppb)) for melamine, adulterated in milk, after sample pretreatments but also enabled rapid detection of 0.2 ppm melamine in formula and low-fat milk within 30 s without any pretreatments, with the supports of principal component analysis (PCA) method. The AuNP–cellulose paper, cost-effective and permitting low-ppb-level label-free molecular sensing, can be a feasible SERS sensor for environmental and biomedical applications.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100717"},"PeriodicalIF":7.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Graphene-coated Si/C composites for high-density electrodes: Mitigating silicon degradation and enhancing cycle life in lithium-ion batteries

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-18 DOI: 10.1016/j.apsadv.2025.100715

Jun Myoung Sheem , Jin Kyo Koo , Chaeyeon Ha , Young Min Kim , Young Ugk Kim , Jae Hou Nah , Young-Jun Kim

Silicon, which serves as the anode active material in lithium-ion batteries (LIBs) because of its high capacity, suffers from performance degradation during continuous cycling. In this study, we designed a high-energy density electrode using artificial graphite (AG) with a graphene-coated Si/C active material (Gr@Si/C). The Gr@Si/C composite synthesized via iterative coating processes not only ensures the electronic conductivity of adjacent silicon particles but also provides a buffering capability against volumetric expansion during repeated charge/discharge cycles at high loading and increased electrode density. Remarkably, the prepared Gr@Si/C‒AG blended electrode exhibited enhanced cycle life characteristics compared with those reported in previous studies. X-ray diffraction analysis confirmed the establishment of an electron conduction path and revealed the effect of impeding particle isolation from the conducting network. Furthermore, full cells incorporating the Gr@Si/C‒AG composite electrode harmonized with the cathode exhibited superior capacity retention of more than 70 % over 200 cycles. These findings suggest that graphene-coated Si/C composites are promising anode active materials for LIBs.

{"title":"Graphene-coated Si/C composites for high-density electrodes: Mitigating silicon degradation and enhancing cycle life in lithium-ion batteries","authors":"Jun Myoung Sheem , Jin Kyo Koo , Chaeyeon Ha , Young Min Kim , Young Ugk Kim , Jae Hou Nah , Young-Jun Kim","doi":"10.1016/j.apsadv.2025.100715","DOIUrl":"10.1016/j.apsadv.2025.100715","url":null,"abstract":"<div><div>Silicon, which serves as the anode active material in lithium-ion batteries (LIBs) because of its high capacity, suffers from performance degradation during continuous cycling. In this study, we designed a high-energy density electrode using artificial graphite (AG) with a graphene-coated Si/C active material (Gr@Si/C). The Gr@Si/C composite synthesized via iterative coating processes not only ensures the electronic conductivity of adjacent silicon particles but also provides a buffering capability against volumetric expansion during repeated charge/discharge cycles at high loading and increased electrode density. Remarkably, the prepared Gr@Si/C‒AG blended electrode exhibited enhanced cycle life characteristics compared with those reported in previous studies. X-ray diffraction analysis confirmed the establishment of an electron conduction path and revealed the effect of impeding particle isolation from the conducting network. Furthermore, full cells incorporating the Gr@Si/C‒AG composite electrode harmonized with the cathode exhibited superior capacity retention of more than 70 % over 200 cycles. These findings suggest that graphene-coated Si/C composites are promising anode active materials for LIBs.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100715"},"PeriodicalIF":7.5,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pulsed Laser Ablation of Recycled Copper in Methanol: A new route toward sustainable plasmonic and catalytic nanostructures

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-15 DOI: 10.1016/j.apsadv.2025.100712

Cristiano Lo Pò , Stefano Boscarino , Silvia Scalese , Simona Boninelli , Maria Grazia Grimaldi , Francesco Ruffino

Copper Nanoparticles (NPs) are widely used for their versatility, specifically in plasmonic and catalysis. Now copper has become a critical raw material so an alternative must be found. In this work we compare the plasmonic and catalytic activity of Cu NPs produced by using an industrial ultrapure target and a Cu target obtained from a commercial wire. The technique used for the NPs production is the Pulsed Laser Ablation in Liquid with a

1064 nm

nanosecond laser that allows to produce NPs directly from a bulk target without any treatment.

Both kinds of NPs exhibit their plasmonic peak at around

600 nm

, typically of Cu. Both kind of NPs exhibit the same catalytic activity, in terms of water splitting, as catalyst, in anode or cathode, with performance comparable with the state of the art.

引用次数: 0

Selective phase growth of ultra-smooth Ti2O3 and TiO2 thin films at low growth temperature controlled by the oxygen partial pressure

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-08 DOI: 10.1016/j.apsadv.2025.100706

Jiayi Tang , Okkyun Seo , Jaemyung Kim , Ibrahima Gueye , L.S.R. Kumara , Ho Jun Oh , Wan-Gil Jung , Won-Jin Moon , Yong Tae Kim , Satoshi Yasuno , Tappei Nishihara , Akifumi Matsuda , Osami Sakata

The selective phase growth of Ti-based oxide thin films on sapphire substrates is crucial in controlling the electronic properties, such as the insulator-to-metal transition (IMT). Thin films are generally prepared by pulsed laser deposition under high temperatures, but it is challenging to obtain a smooth surface. In this study, we deposited ultra-smooth epitaxial TiO₂ and Ti₂O₃ thin films with roughnesses below 0.34 Å on sapphire substrates. By controlling the oxygen partial pressure at a relatively low temperature, at 473 K, we obtained highly crystalline thin films with selective growth. The thin films grown at 1 and 10⁻³ Pa exhibited a rutile-type TiO₂ phase, and those grown at 10⁻⁶ Pa exhibited a hexagonal Ti₂O₃ phase. The crystal structures and electronic structures were consistent with the previous reports on TiO₂ and Ti₂O₃ thin films. Moreover, Ti₂O₃ underwent an IMT, whereas TiO₂ was unchanged.

{"title":"Selective phase growth of ultra-smooth Ti2O3 and TiO2 thin films at low growth temperature controlled by the oxygen partial pressure","authors":"Jiayi Tang , Okkyun Seo , Jaemyung Kim , Ibrahima Gueye , L.S.R. Kumara , Ho Jun Oh , Wan-Gil Jung , Won-Jin Moon , Yong Tae Kim , Satoshi Yasuno , Tappei Nishihara , Akifumi Matsuda , Osami Sakata","doi":"10.1016/j.apsadv.2025.100706","DOIUrl":"10.1016/j.apsadv.2025.100706","url":null,"abstract":"<div><div>The selective phase growth of Ti-based oxide thin films on sapphire substrates is crucial in controlling the electronic properties, such as the insulator-to-metal transition (IMT). Thin films are generally prepared by pulsed laser deposition under high temperatures, but it is challenging to obtain a smooth surface. In this study, we deposited ultra-smooth epitaxial TiO<sub>2</sub> and Ti<sub>2</sub>O<sub>3</sub> thin films with roughnesses below 0.34 Å on sapphire substrates. By controlling the oxygen partial pressure at a relatively low temperature, at 473 K, we obtained highly crystalline thin films with selective growth. The thin films grown at 1 and 10<sup>−3</sup> Pa exhibited a rutile-type TiO<sub>2</sub> phase, and those grown at 10<sup>−6</sup> Pa exhibited a hexagonal Ti<sub>2</sub>O<sub>3</sub> phase. The crystal structures and electronic structures were consistent with the previous reports on TiO<sub>2</sub> and Ti<sub>2</sub>O<sub>3</sub> thin films. Moreover, Ti<sub>2</sub>O<sub>3</sub> underwent an IMT, whereas TiO<sub>2</sub> was unchanged.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100706"},"PeriodicalIF":7.5,"publicationDate":"2025-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143351021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect of Nb0.5 and Mo0.75 addition on in-vitro corrosion and wear resistance of high-speed laser metal deposited Al0.3CrFeCoNi high-entropy alloy coatings

IF 7.5 Q1 CHEMISTRY, PHYSICAL

Applied Surface Science Advances

Pub Date : 2025-02-06 DOI: 10.1016/j.apsadv.2025.100710

Burak Dikici , Thomas Lindner , Thomas Lampke , Thomas Grund , Asli Gunay Bulutsuz

High-entropy alloy (HEA) coatings offer unique advantages for enhancing the surface properties of biomedical implants, including improved wear and corrosion resistance. In this study, Al_0.3CrFeCoNi-based HEA coatings were produced by high-speed laser metal deposition (HS-LMD) with the addition of Nb and Mo. The coatings were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive spectroscopy (EDS). Electrochemical corrosion tests, including potentiodynamic scanning (PDS) and electrochemical impedance spectroscopy (EIS), were conducted using Hanks' solution at body temperature to simulate the body environment. Wear tests were also performed under both dry and in-vitro conditions. Contact angle measurements were performed to assess the surface wettability, which is crucial for understanding the interaction between the coating and biological fluids. The results demonstrated that the Mo-containing coating exhibited superior corrosion and wear performance under in-vitro conditions. This was due to the slower progression of deeper corrosion attacks in unmelted particles, which minimized the micro-galvanic effects associated with the eutectic structures within these particles. Additionally, the coating's stable microstructure and effective formation of a protective passive layer contributed to its enhanced performance.

{"title":"Effect of Nb0.5 and Mo0.75 addition on in-vitro corrosion and wear resistance of high-speed laser metal deposited Al0.3CrFeCoNi high-entropy alloy coatings","authors":"Burak Dikici , Thomas Lindner , Thomas Lampke , Thomas Grund , Asli Gunay Bulutsuz","doi":"10.1016/j.apsadv.2025.100710","DOIUrl":"10.1016/j.apsadv.2025.100710","url":null,"abstract":"<div><div>High-entropy alloy (HEA) coatings offer unique advantages for enhancing the surface properties of biomedical implants, including improved wear and corrosion resistance. In this study, Al<sub>0.3</sub>CrFeCoNi-based HEA coatings were produced by high-speed laser metal deposition (HS-LMD) with the addition of Nb and Mo. The coatings were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive spectroscopy (EDS). Electrochemical corrosion tests, including potentiodynamic scanning (PDS) and electrochemical impedance spectroscopy (EIS), were conducted using Hanks' solution at body temperature to simulate the body environment. Wear tests were also performed under both dry and <em>in-vitro</em> conditions. Contact angle measurements were performed to assess the surface wettability, which is crucial for understanding the interaction between the coating and biological fluids. The results demonstrated that the Mo-containing coating exhibited superior corrosion and wear performance under <em>in-vitro</em> conditions. This was due to the slower progression of deeper corrosion attacks in unmelted particles, which minimized the micro-galvanic effects associated with the eutectic structures within these particles. Additionally, the coating's stable microstructure and effective formation of a protective passive layer contributed to its enhanced performance.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":"26 ","pages":"Article 100710"},"PeriodicalIF":7.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143358416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0