Pub Date : 2025-04-14DOI: 10.1016/j.apsusc.2025.163262
Xiaoli Ran , Yanlong Gong , Hao Zeng , Yang Bai , Sijie Li , Lei Zhang , Haitao Fu , Xizhong An , Dawei Su , Xiaohong Yang
The photoelectrochemical (PEC) activity of Strontium titanate (SrTiO3) is constrained by its insufficient light absorption and significant carrier recombination. In this study, carbon dots (CDs) are integrated as co-catalysts onto the surface of oxygen-vacancy-doped mesoporous spherical SrTiO3 nanoparticles to address these limitations and enhance PEC activity. Experimental characterizations and DFT calculations elucidate that the CDs demonstrated significant synergistic enhancements in PEC performance, particularly in band alignment, visible light absorption, and charge carrier transport, which collectively accelerated surface catalytic reactions. Most importantly, the electronic structure of SrTiO3 was optimized by CDs, and their interfacial interaction plays an important role in enhancing its PEC performance. As a result, the optimal 0.005 %CDs/SrXTiO3-δ photoanode achieves a photocurrent density of 1.37 mA/cm2 at 1.23 V vs. RHE, significantly surpassing that of SrXTiO3-δ (0.73 mA/cm2) and pristine SrTiO3 (0.109 mA/cm2). Additionally, the incident photon-to-current conversion efficiency (IPCE) reaches 34 % for 0.005 %CDs/SrXTiO3-δ, compared to 18.2 % for SrXTiO3-δ and 2.6 % for SrTiO3. These findings present a straightforward and effective method for designing high-performance catalysts for PEC water splitting.
{"title":"Carbon dots enhance photoelectrochemical water splitting activity of SrTiO3 nanoparticles: Band tuning and excellent charge separation","authors":"Xiaoli Ran , Yanlong Gong , Hao Zeng , Yang Bai , Sijie Li , Lei Zhang , Haitao Fu , Xizhong An , Dawei Su , Xiaohong Yang","doi":"10.1016/j.apsusc.2025.163262","DOIUrl":"10.1016/j.apsusc.2025.163262","url":null,"abstract":"<div><div>The photoelectrochemical (PEC) activity of Strontium titanate (SrTiO<sub>3</sub>) is constrained by its insufficient light absorption and significant carrier recombination. In this study, carbon dots (CDs) are integrated as co-catalysts onto the surface of oxygen-vacancy-doped mesoporous spherical SrTiO<sub>3</sub> nanoparticles to address these limitations and enhance PEC activity. Experimental characterizations and DFT calculations elucidate that the CDs demonstrated significant synergistic enhancements in PEC performance, particularly in band alignment, visible light absorption, and charge carrier transport, which collectively accelerated surface catalytic reactions. Most importantly, the electronic structure of SrTiO<sub>3</sub> was optimized by CDs, and their interfacial interaction plays an important role in enhancing its PEC performance. As a result, the optimal 0.005 %CDs/Sr<em><sub>X</sub></em>TiO<sub>3-</sub><em><sub>δ</sub></em> photoanode achieves a photocurrent density of 1.37 mA/cm<sup>2</sup> at 1.23 V vs. RHE, significantly surpassing that of Sr<em><sub>X</sub></em>TiO<sub>3</sub><em><sub>-δ</sub></em> (0.73 mA/cm<sup>2</sup>) and pristine SrTiO<sub>3</sub> (0.109 mA/cm<sup>2</sup>). Additionally, the incident photon-to-current conversion efficiency (IPCE) reaches 34 % for 0.005 %CDs/Sr<em><sub>X</sub></em>TiO<sub>3</sub><em><sub>-δ</sub></em>, compared to 18.2 % for Sr<em><sub>X</sub></em>TiO<sub>3</sub><em><sub>-δ</sub></em> and 2.6 % for SrTiO<sub>3</sub>. These findings present a straightforward and effective method for designing high-performance catalysts for PEC water splitting.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"701 ","pages":"Article 163262"},"PeriodicalIF":6.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831891","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}
Pub Date : 2025-04-14DOI: 10.1016/j.apsusc.2025.163266
Lingxue Meng , Hongwei Hao , Lan Ma , Hangyu Yue , Hang Ye , Linhai Guo , Zunkai Huang , Li Tian
With the increasing computational demands faced by computing systems based on the von Neumann architecture, artificial synaptic devices that mimic the neural synapses of the human brain have emerged as a potential solution to this challenge. This study presents a photoelectric synaptic thin-film transistor (TFT) based on an ITO/IGZO composite active layer, aiming to enhance the device’s responsiveness to visible light and synaptic plasticity. Compared to traditional single-layer devices, the ITO/IGZO bilayer structure exhibits significantly improved visible light response, particularly in the red and green light bands. X-ray photoelectron spectroscopy (XPS) analysis revealed an increase in oxygen vacancies and sub-bandgap states at the ITO/IGZO interface, which facilitates the generation of carriers excited by low-energy photons, thereby further enhancing the photoelectric performance. The photoelectric synaptic device demonstrates good short-term and long-term plasticity (STP and LTP) in mimicking synaptic plasticity and achieved an accuracy rate of 93% in the Modified National Institute of Standards and Technology (MNIST) handwritten digit recognition experiment. The results indicate that ITO/IGZO TFTs not only enhance visible light response but also have the potential to simulate neural synaptic behavior, making them a promising component in neuromorphic computing and visual perception systems.
{"title":"Visible light-modulated photoelectric synaptic transistor based on ITO and IGZO bilayer channel","authors":"Lingxue Meng , Hongwei Hao , Lan Ma , Hangyu Yue , Hang Ye , Linhai Guo , Zunkai Huang , Li Tian","doi":"10.1016/j.apsusc.2025.163266","DOIUrl":"10.1016/j.apsusc.2025.163266","url":null,"abstract":"<div><div>With the increasing computational demands faced by computing systems based on the von Neumann architecture, artificial synaptic devices that mimic the neural synapses of the human brain have emerged as a potential solution to this challenge. This study presents a photoelectric synaptic thin-film transistor (TFT) based on an ITO/IGZO composite active layer, aiming to enhance the device’s responsiveness to visible light and synaptic plasticity. Compared to traditional single-layer devices, the ITO/IGZO bilayer structure exhibits significantly improved visible light response, particularly in the red and green light bands. X-ray photoelectron spectroscopy (XPS) analysis revealed an increase in oxygen vacancies and sub-bandgap states at the ITO/IGZO interface, which facilitates the generation of carriers excited by low-energy photons, thereby further enhancing the photoelectric performance. The photoelectric synaptic device demonstrates good short-term and long-term plasticity (STP and LTP) in mimicking synaptic plasticity and achieved an accuracy rate of 93% in the Modified National Institute of Standards and Technology (MNIST) handwritten digit recognition experiment. The results indicate that ITO/IGZO TFTs not only enhance visible light response but also have the potential to simulate neural synaptic behavior, making them a promising component in neuromorphic computing and visual perception systems.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"701 ","pages":"Article 163266"},"PeriodicalIF":6.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827592","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 synergistic combination of sp2- and sp3-hybridized carbons has multiple applications. Among various structural parameters, the texture of the interface layer in sp2-sp3 composites is perhaps one of the most important factor affecting their functional properties. In the present study, we investigated the early stages of graphitization of a synthetic diamond during high-vacuum annealing at 1250 °C. This was achieved using high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and angle-resolved near-edge X-ray absorption fine structure spectroscopy in combination with density functional theory modeling. Our results showed that the texture of the graphitized layer can be controlled by the symmetry of the annealed diamond crystal face and by defect engineering. Specifically, arches merging with the diamond layer were formed on the (100) face, while nanographites were formed on the (111) face. In the latter case, the graphene sheets had a predominantly vertical orientation to the crystal face and could grew parallel in the etch pits. The stages of the structural evolution of diamond graphitization are discussed, including the rearrangement of the diamond surface, the detachment of carbon atoms, the formation of an amorphous sp2 carbon layer, and its subsequent condensation into nanographite covalently bonded to the diamond surface.
{"title":"Texture of (100) and (111) faces of annealed diamond crystal","authors":"A.V. Okotrub , O.V. Sedelnikova , D.V. Gorodetskiy , A.V. Gusel’nikov , Yu.N. Palyanov , L.G. Bulusheva","doi":"10.1016/j.apsusc.2025.163270","DOIUrl":"10.1016/j.apsusc.2025.163270","url":null,"abstract":"<div><div>The synergistic combination of sp<sup>2</sup>- and sp<sup>3</sup>-hybridized carbons has multiple applications. Among various structural parameters, the texture of the interface layer in sp<sup>2</sup>-sp<sup>3</sup> composites is perhaps one of the most important factor affecting their functional properties. In the present study, we investigated the early stages of graphitization of a synthetic diamond during high-vacuum annealing at 1250 °C. This was achieved using high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and angle-resolved near-edge X-ray absorption fine structure spectroscopy in combination with density functional theory modeling. Our results showed that the texture of the graphitized layer can be controlled by the symmetry of the annealed diamond crystal face and by defect engineering. Specifically, arches merging with the diamond layer were formed on the (100) face, while nanographites were formed on the (111) face. In the latter case, the graphene sheets had a predominantly vertical orientation to the crystal face and could grew parallel in the etch pits. The stages of the structural evolution of diamond graphitization are discussed, including the rearrangement of the diamond surface, the detachment of carbon atoms, the formation of an amorphous sp<sup>2</sup> carbon layer, and its subsequent condensation into nanographite covalently bonded to the diamond surface.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"701 ","pages":"Article 163270"},"PeriodicalIF":6.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831875","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}
In this study, we report the synthesis and characterization of MoS2-PVA and MoS2-NiO-PVA composite nanofibers, focusing on their structural, chemical, and electrocatalytic properties before and after plasma treatment. X-ray diffraction (XRD) results verify that the incorporation of NiO nanoparticles into MoS2-PVA further enhances the crystallinity of the composite, as evidenced by the XRD patterns. Fourier-transform infrared (FTIR) spectroscopy reveals characteristic vibrations of hydroxyl, carbonyl, Mo-S, Mo-O, and Ni-O bonds, providing strong evidence of chemical interactions between MoS2, PVA, and NiO. X-ray photoelectron spectroscopy (XPS) analysis indicates the successful formation of MoS2-NiO-PVA nanofibers, with significant interactions between MoS2 and NiO, enhancing electron transport properties. Scanning electron microscopy (FE-SEM) analysis shows that plasma treatment leads to significant morphological changes, including surface roughening and reduced fiber thickness. Water contact angle measurements demonstrate that plasma treatment improves the hydrophilicity of the nanofibers, facilitating better electrolyte interaction and increasing their electrocatalytic performance. The HER efficiency of MoS2-PVA and MoS2-NiO-PVA nanofibers was enhanced through plasma treatment, resulting in a lower overpotential (213 mV) and Tafel slope (135 mV/dec) for MoS2-NiO-PVA. The increase in capacitance (2.92 mF/cm2) and reduction in charge transfer resistance (Rct) confirmed improved electrocatalytic activity. The electrocatalyst demonstrated excellent stability, maintaining 92 % of its initial performance after 12 h of continuous operation, as evidenced by cyclic voltammetry at 50 mV/s and a stable potential at 1.5 mA/cm2.These enhancements highlight plasma treatment as an effective strategy for optimizing HER kinetics in electrocatalysts. These improvements result from enhanced surface area, hydrophilicity, and accessibility of active sites, making plasma-treated nanofibers promising for energy applications.
{"title":"Enhanced electrocatalytic properties of plasma-treated MoS2-NiO-PVA nanofibers for hydrogen evolution reaction: A study of surface modifications and charge transfer kinetics","authors":"Hamed Fayaz Rouhi , Fatemeh Aghaei , Farhad Chaharganeh Kalangestani , Hossein Mahmoudi Chenari , Maryam Nilkar","doi":"10.1016/j.apsusc.2025.163274","DOIUrl":"10.1016/j.apsusc.2025.163274","url":null,"abstract":"<div><div>In this study, we report the synthesis and characterization of MoS<sub>2</sub>-PVA and MoS<sub>2</sub>-NiO-PVA composite nanofibers, focusing on their structural, chemical, and electrocatalytic properties before and after plasma treatment. X-ray diffraction (XRD) results verify that the incorporation of NiO nanoparticles into MoS<sub>2</sub>-PVA further enhances the crystallinity of the composite, as evidenced by the XRD patterns. Fourier-transform infrared (FTIR) spectroscopy reveals characteristic vibrations of hydroxyl, carbonyl, Mo-S, Mo-O, and Ni-O bonds, providing strong evidence of chemical interactions between MoS<sub>2</sub>, PVA, and NiO. X-ray photoelectron spectroscopy (XPS) analysis indicates the successful formation of MoS<sub>2</sub>-NiO-PVA nanofibers, with significant interactions between MoS<sub>2</sub> and NiO, enhancing electron transport properties. Scanning electron microscopy (FE-SEM) analysis shows that plasma treatment leads to significant morphological changes, including surface roughening and reduced fiber thickness. Water contact angle measurements demonstrate that plasma treatment improves the hydrophilicity of the nanofibers, facilitating better electrolyte interaction and increasing their electrocatalytic performance. The HER efficiency of MoS<sub>2</sub>-PVA and MoS<sub>2</sub>-NiO-PVA nanofibers was enhanced through plasma treatment, resulting in a lower overpotential (213 mV) and Tafel slope (135 mV/dec) for MoS<sub>2</sub>-NiO-PVA. The increase in capacitance (2.92 mF/cm<sup>2</sup>) and reduction in charge transfer resistance (<em>R<sub>ct</sub></em>) confirmed improved electrocatalytic activity. The electrocatalyst demonstrated excellent stability, maintaining 92 % of its initial performance after 12 h of continuous operation, as evidenced by cyclic voltammetry at 50 mV/s and a stable potential at 1.5 mA/cm<sup>2</sup>.These enhancements highlight plasma treatment as an effective strategy for optimizing HER kinetics in electrocatalysts. These improvements result from enhanced surface area, hydrophilicity, and accessibility of active sites, making plasma-treated nanofibers promising for energy applications.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"700 ","pages":"Article 163274"},"PeriodicalIF":6.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831708","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 magnetization roasting-magnetic separation process can realize the efficient utilization of iron and manganese ore resources, but the magnetic separation of manganese concentrate products often contain a large amount of roasted diaspore products, reducing the grade of manganese concentrate. Therefore, it is significance to separate new generated aluminium oxide from magnetic separation of manganese concentrate products and produce high-quality manganese concentrate. In this paper, sodium dodecyl aminopropionate (SDA) was synthesized and used as a collector for flotation separation of the new generated aluminium oxide from the manganese ore produced by reduction roasting of pyrolusite. The flotation performance and mechanism of SDA collector on the surface of the new generated aluminium oxide and new generated manganosite were studied by density functional theory (DFT) calculation, flotation experiment, Zeta potential measurement, Fourier-transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that under the conditions of pH 11, concentration of SDA 40 mg/L and concentration of CaCl2 1600 mg/L, SDA had a good ability to collect new generated aluminium oxide, and the recovery difference between new generated aluminium oxide and new generated manganosite was about 60 %. DFT calculation, Zeta potential, FTIR spectra and XPS confirmed that SDA was adsorbed on the new generated manganosite in a small amount, and the adsorption of SDA on the surface of the new generated aluminium oxide was mainly the chemical adsorption of Ca-O and Al-O bonds.
{"title":"Rational design of sodium dodecyl aminopropionate collector for high-efficiency flotation separation of reduction-roasted pyrolusite and diaspore","authors":"Chenlu Chen , Xun Wang , Xian Xie , Xiong Tong , Ruiqi Xie","doi":"10.1016/j.apsusc.2025.163264","DOIUrl":"10.1016/j.apsusc.2025.163264","url":null,"abstract":"<div><div>The magnetization roasting-magnetic separation process can realize the efficient utilization of iron and manganese ore resources, but the magnetic separation of manganese concentrate products often contain a large amount of roasted diaspore products, reducing the grade of manganese concentrate. Therefore, it is significance to separate new generated aluminium oxide from magnetic separation of manganese concentrate products and produce high-quality manganese concentrate. In this paper, sodium dodecyl aminopropionate (SDA) was synthesized and used as a collector for flotation separation of the new generated aluminium oxide from the manganese ore produced by reduction roasting of pyrolusite. The flotation performance and mechanism of SDA collector on the surface of the new generated aluminium oxide and new generated manganosite were studied by density functional theory (DFT) calculation, flotation experiment, Zeta potential measurement, Fourier-transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that under the conditions of pH 11, concentration of SDA 40 mg/L and concentration of CaCl<sub>2</sub> 1600 mg/L, SDA had a good ability to collect new generated aluminium oxide, and the recovery difference between new generated aluminium oxide and new generated manganosite was about 60 %. DFT calculation, Zeta potential, FTIR spectra and XPS confirmed that SDA was adsorbed on the new generated manganosite in a small amount, and the adsorption of SDA on the surface of the new generated aluminium oxide was mainly the chemical adsorption of Ca-O and Al-O bonds.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"700 ","pages":"Article 163264"},"PeriodicalIF":6.3,"publicationDate":"2025-04-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827594","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}
Pub Date : 2025-04-12DOI: 10.1016/j.apsusc.2025.163156
Yiqing Zhang , Jiayi Fu , Yan Yu , Guangtao Chang , Ruoxin Li
Titanium dioxide nanoparticles (TiO2 NPs) are highly effective UV-blocking agents with potential for textile applications. However, their tendency to aggregate compromises their performance and limits their use. This study addresses this challenge by employing a novel two-step surface modification strategy using ODA-KH570 and ECH-KH590 to enhance TiO2 NPs dispersion within polyacrylonitrile (PAN) fibers. FTIR, XPS, and XRD analyses confirmed successful grafting of the modifiers. Crucially, incorporating 1 % ECH-KH590-TiO2/PAN fibers via wet spinning yielded a remarkable increase in mechanical properties, with break tensile strength reaching 7.49 MPa and elongation at 21.0 % – significantly surpassing pure PAN fibers. This demonstrates the effectiveness of the modification strategy in achieving superior dispersion and reinforcement, paving the way for high-performance UV-protective textiles. The experimental results demonstrate that the optimized ECH-KH590-TiO2/PAN fibers exhibit excellent UV shielding performance (UPF ∼ 45.21) and remarkable antibacterial properties (E. coli: ∼92.57 %, S. aureus: ∼90.77 %). These features highlight their potential for applications in multifunctional textiles.
{"title":"A novel two-step modification of TiO2 nanoparticles for PAN fibers with enhanced mechanical strength, UV shielding and antibacterial properties","authors":"Yiqing Zhang , Jiayi Fu , Yan Yu , Guangtao Chang , Ruoxin Li","doi":"10.1016/j.apsusc.2025.163156","DOIUrl":"10.1016/j.apsusc.2025.163156","url":null,"abstract":"<div><div>Titanium dioxide nanoparticles (TiO<sub>2</sub> NPs) are highly effective UV-blocking agents with potential for textile applications. However, their tendency to aggregate compromises their performance and limits their use. This study addresses this challenge by employing a novel two-step surface modification strategy using ODA-KH570 and ECH-KH590 to enhance TiO<sub>2</sub> NPs dispersion within polyacrylonitrile (PAN) fibers. FTIR, XPS, and XRD analyses confirmed successful grafting of the modifiers. Crucially, incorporating 1 % ECH-KH590-TiO<sub>2</sub>/PAN fibers via wet spinning yielded a remarkable increase in mechanical properties, with break tensile strength reaching 7.49 MPa and elongation at 21.0 % – significantly surpassing pure PAN fibers. This demonstrates the effectiveness of the modification strategy in achieving superior dispersion and reinforcement, paving the way for high-performance UV-protective textiles. The experimental results demonstrate that the optimized ECH-KH590-TiO<sub>2</sub>/PAN fibers exhibit excellent UV shielding performance (UPF ∼ 45.21) and remarkable antibacterial properties (E. coli: ∼92.57 %, S. aureus: ∼90.77 %). These features highlight their potential for applications in multifunctional textiles.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"700 ","pages":"Article 163156"},"PeriodicalIF":6.3,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822519","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}
Pub Date : 2025-04-12DOI: 10.1016/j.apsusc.2025.163249
Manyuan Gan , Yanhui Song , Jingyuan Wei , Yongqing Shen , Peizhi Liu , Mengxue Xia , Pengfei Zhang , Zhiyuan Tian , Bingshe Xu , Junjie Guo
Manipulating the electronic structure of iridium (Ir)-based catalyst has been recognized as an effective strategy to boost the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities of overall water splitting (OWS). It is, however, still a challenge to develop bifunctional HER/OER Ir-based electrocatalysts in a wide range of pH conditions (alkaline and neutral). Herein, a novel heterostructure comprising Ir nanoparticles anchored on Ni(OH)2/FeOOH electrocatalyst (Ir@Ni(OH)2/FeOOH) was constructed. Experimental and theoretical results demonstrated that the charge transfer from Ni(OH)2/FeOOH to Ir nanoparticles could steer the electronic density of Ir sites, reduce the HER and OER process Gibbs free energy, and thus facilitate the adsorption and dissociation of water. Profiting from these favorable factors, the optimized Ir@Ni(OH)2/FeOOH exhibited excellent HER/OER electrocatalytic performances in both alkaline (1.0 M KOH, 20/183 mV@10 mA cm−2) and neutral (1.0 M PBS, 14/288 mV@10 mA cm−2), respectively. Further, the constructed Ir@Ni(OH)2/FeOOH)||Ir@Ni(OH)2/FeOOH electrolyzer demands only 1.47 and 1.58 V to afford 10 mA cm−2 in 1.0 M KOH and 1.0 M PBS, and exhibit a stability of more than 200 h. This work contributes to understanding the catalytic mechanism of carrier and nanoparticle co-catalysis during water splitting.
{"title":"Steering the electronic transfer between Ir nanoparticles and Ni(OH)2/FeOOH for overall water splitting in both alkaline and neutral media","authors":"Manyuan Gan , Yanhui Song , Jingyuan Wei , Yongqing Shen , Peizhi Liu , Mengxue Xia , Pengfei Zhang , Zhiyuan Tian , Bingshe Xu , Junjie Guo","doi":"10.1016/j.apsusc.2025.163249","DOIUrl":"10.1016/j.apsusc.2025.163249","url":null,"abstract":"<div><div>Manipulating the electronic structure of iridium (Ir)-based catalyst has been recognized as an effective strategy to boost the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities of overall water splitting (OWS). It is, however, still a challenge to develop bifunctional HER/OER Ir-based electrocatalysts in a wide range of pH conditions (alkaline and neutral). Herein, a novel heterostructure comprising Ir nanoparticles anchored on Ni(OH)<sub>2</sub>/FeOOH electrocatalyst (Ir@Ni(OH)<sub>2</sub>/FeOOH) was constructed. Experimental and theoretical results demonstrated that the charge transfer from Ni(OH)<sub>2</sub>/FeOOH to Ir nanoparticles could steer the electronic density of Ir sites, reduce the HER and OER process Gibbs free energy, and thus facilitate the adsorption and dissociation of water. Profiting from these favorable factors, the optimized Ir@Ni(OH)<sub>2</sub>/FeOOH exhibited excellent HER/OER electrocatalytic performances in both alkaline (1.0 M KOH, 20/183 mV@10 mA cm<sup>−2</sup>) and neutral (1.0 M PBS, 14/288 mV@10 mA cm<sup>−2</sup>), respectively. Further, the constructed Ir@Ni(OH)<sub>2</sub>/FeOOH)||Ir@Ni(OH)<sub>2</sub>/FeOOH electrolyzer demands only 1.47 and 1.58 V to afford 10 mA cm<sup>−2</sup> in 1.0 M KOH and 1.0 M PBS, and exhibit a stability of more than 200 h. This work contributes to understanding the catalytic mechanism of carrier and nanoparticle co-catalysis during water splitting.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"700 ","pages":"Article 163249"},"PeriodicalIF":6.3,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822524","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}
Pub Date : 2025-04-12DOI: 10.1016/j.apsusc.2025.163257
L. Ma , H. Zhao , F. Zheng , X.M. Wang , N. Tian , C.Y. You
L10 (FexNi1-x)0.5Pt0.5 ordered alloy films with a face-centered tetragonal (fct) structure were successfully fabricated via magnetron sputtering. The effects of Fermi level shifts and impurity scattering on the anomalous Hall effect in these films were studied with both experiments and first-principles calculations. Both residual resistivity and phonon scattering were found to contribute to skew scattering, with their contributions decreasing as Fe content increases. Ab initio calculations reveal that the position of the Fermi surface rises with increasing the Fe content x , leading to a transition of intrinsic scattering parameter b from negative to positive between x = 0.4 and x = 0.6. Moreover, larger spin-slip on the Fe-rich side significantly enhances the anomalous Hall resistivity. Our results reveal that intrinsic mechanisms dominate on the Fe-rich side, whereas skew scattering mechanisms prevail on the Ni-rich side. This study establishes a comprehensive correlation among band features, Fermi level positioning, and impurity scattering in this prototypical system.
通过磁控溅射法成功制造了具有面心四方（ct）结构的 L10 (FexNi1-x)0.5Pt0.5 有序合金薄膜。通过实验和第一原理计算，研究了费米级移动和杂质散射对这些薄膜中反常霍尔效应的影响。研究发现，残余电阻率和声子散射都会对偏斜散射产生影响，而随着铁含量的增加，它们的影响会逐渐减小。Ab initio 计算显示，费米面的位置随着铁含量 x 的增加而上升，导致本征散射参数 b 在 x = 0.4 和 x = 0.6 之间由负转正。此外，富铁侧较大的自旋滑移会显著增强反常霍尔电阻率。我们的研究结果表明，本征机制在富铁侧占主导地位，而倾斜散射机制则在富镍侧占主导地位。这项研究在这一原型系统中建立了带状特征、费米级定位和杂质散射之间的全面关联。
{"title":"Influence of Fermi level and impurity scattering on anomalous Hall effect in L10 FeNiPt alloy films","authors":"L. Ma , H. Zhao , F. Zheng , X.M. Wang , N. Tian , C.Y. You","doi":"10.1016/j.apsusc.2025.163257","DOIUrl":"10.1016/j.apsusc.2025.163257","url":null,"abstract":"<div><div>L1<sub>0</sub> (Fe<em><sub>x</sub></em>Ni<sub>1-</sub><em><sub>x</sub></em>)<sub>0.5</sub>Pt<sub>0.5</sub> ordered alloy films with a face-centered tetragonal (fct) structure were successfully fabricated via magnetron sputtering. The effects of Fermi level shifts and impurity scattering on the anomalous Hall effect in these films were studied with both experiments and first-principles calculations. Both residual resistivity and phonon scattering were found to contribute to skew scattering, with their contributions decreasing as Fe content increases. <em>Ab initio</em> calculations reveal that the position of the Fermi surface rises with increasing the Fe content <em>x</em> , leading to a transition of intrinsic scattering parameter <em>b</em> from negative to positive between <em>x</em> = 0.4 and <em>x</em> = 0.6. Moreover, larger spin-slip on the Fe-rich side significantly enhances the anomalous Hall resistivity. Our results reveal that intrinsic mechanisms dominate on the Fe-rich side, whereas skew scattering mechanisms prevail on the Ni-rich side. This study establishes a comprehensive correlation among band features, Fermi level positioning, and impurity scattering in this prototypical system.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"700 ","pages":"Article 163257"},"PeriodicalIF":6.3,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143824862","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}
Pub Date : 2025-04-12DOI: 10.1016/j.apsusc.2025.163223
Manjulla Subramaniam , Abdul Rahman Mohamed , Mélanie Emo , Brigitte Vigolo , Pooya Lahijani , Sin Yuan Lai
A revolutionary approach unveiling a novel, sustainable pathway for reducing sulfur dioxide (SO2) to stable, elemental sulfur by valorizing waste chicken eggshells into highly effective, regenerative calcium sulfate/calcium sulfide-supported γ-alumina (CaSO4/CaS-γ-Al2O3) catalytic system was presented. In this work, composite catalysts of CaO-supported γ-Al2O3 (CaO-γ-Al2O3) at various CaO loading percentages (30, 50, 70 and 90 wt%) were prepared via impregnation method. The composites improved chemical and structural properties attributed to strong basicity, thereby increasing SO2 reduction efficiency. At 800 °C and a gas hourly space velocity of 18 L/h·g, the catalyst with 70 wt% CaO-γ-Al2O3 achieved optimum conditions, resulting in a high sulfur yield of 85.60 % and SO2 conversion of 48.99 % after 16.5 h. The reaction mechanistic pathways, including Langmuir–Hinshelwood (L–H), Eley–Rideal (E–R) and Mars-van Krevelen (MvK), revealed a cyclic calcium-based catalytic system supported γ-Al2O3 and elemental sulfur production.
{"title":"One-pot regenerative CaSO4/CaS-supported γ-Al2O3 catalytic system for sulfur dioxide reduction to elemental sulfur","authors":"Manjulla Subramaniam , Abdul Rahman Mohamed , Mélanie Emo , Brigitte Vigolo , Pooya Lahijani , Sin Yuan Lai","doi":"10.1016/j.apsusc.2025.163223","DOIUrl":"10.1016/j.apsusc.2025.163223","url":null,"abstract":"<div><div>A revolutionary approach unveiling a novel, sustainable pathway for reducing sulfur dioxide (SO<sub>2</sub>) to stable, elemental sulfur by valorizing waste chicken eggshells into highly effective, regenerative calcium sulfate/calcium sulfide-supported γ-alumina (CaSO<sub>4</sub>/CaS-γ-Al<sub>2</sub>O<sub>3</sub>) catalytic system was presented. In this work, composite catalysts of CaO-supported γ-Al<sub>2</sub>O<sub>3</sub> (CaO-γ-Al<sub>2</sub>O<sub>3</sub>) at various CaO loading percentages (30, 50, 70 and 90 wt%) were prepared via impregnation method. The composites improved chemical and structural properties attributed to strong basicity, thereby increasing SO<sub>2</sub> reduction efficiency. At 800 °C and a gas hourly space velocity of 18 L/h·g, the catalyst with 70 wt% CaO-γ-Al<sub>2</sub>O<sub>3</sub> achieved optimum conditions, resulting in a high sulfur yield of 85.60 % and SO<sub>2</sub> conversion of 48.99 % after 16.5 h. The reaction mechanistic pathways, including Langmuir–Hinshelwood (L–H), Eley–Rideal (E–R) and Mars-van Krevelen (MvK), revealed a cyclic calcium-based catalytic system supported γ-Al<sub>2</sub>O<sub>3</sub> and elemental sulfur production.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"701 ","pages":"Article 163223"},"PeriodicalIF":6.3,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143824861","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}
Pub Date : 2025-04-12DOI: 10.1016/j.apsusc.2025.163252
Yunqiu Liu , Yu Zhang , Dengpan Nie , Qian Shang , Juan Tian , Wenxing Chen
Low-grade barite ore can be utilized as a substitute for barite resources, and its exploitation is becoming more and more important. High-grade, easily extracted barite resources have been rapidly depleted. For flotation studies on barite ore, this thesis combined forward and reverse flotation using a combination of maize starch and aluminum sulfate as a depressant. The flotation concentrates BaSO4 grade was 92.18%, and the recovery was 91.38%, which was 7.51% higher than that with a single CS acting as a depressant. Contact angle measurements and zeta potential indicate that SO42- or Al(OH)4- in aluminum sulfate increases the hydrophilicity of barite through complex formation or interaction with CS in a weakly alkaline environment. AFM analysis showed that the barite surface presented dense and uniform layered adsorption, and the co-adsorption characteristics of the mixed depressant were stronger than those of the single depressant. With the presence of double-dentate mononuclear and double-dentate dinuclear connections, the CS/AS mixed depressant exhibits strong selectivity, according to the results of molecular simulations. Its adsorption on the barite surface is primarily achieved through hydrogen bonding. Water molecules hydroxylate the barite surface to increase its hydrophilicity by acting as a bridge between the CS/AS and barite (001) surfaces.
{"title":"Mechanism of flotation separation of barite and quartz by starch/aluminum sulfate composite depressant","authors":"Yunqiu Liu , Yu Zhang , Dengpan Nie , Qian Shang , Juan Tian , Wenxing Chen","doi":"10.1016/j.apsusc.2025.163252","DOIUrl":"10.1016/j.apsusc.2025.163252","url":null,"abstract":"<div><div>Low-grade barite ore can be utilized as a substitute for barite resources, and its exploitation is becoming more and more important. High-grade, easily extracted barite resources have been rapidly depleted. For flotation studies on barite ore, this thesis combined forward and reverse flotation using a combination of maize starch and aluminum sulfate as a depressant. The flotation concentrates BaSO<sub>4</sub> grade was 92.18%, and the recovery was 91.38%, which was 7.51% higher than that with a single CS acting as a depressant. Contact angle measurements and zeta potential indicate that SO<sub>4</sub><sup>2-</sup> or Al(OH)<sub>4</sub><sup>-</sup> in aluminum sulfate increases the hydrophilicity of barite through complex formation or interaction with CS in a weakly alkaline environment. AFM analysis showed that the barite surface presented dense and uniform layered adsorption, and the co-adsorption characteristics of the mixed depressant were stronger than those of the single depressant. With the presence of double-dentate mononuclear and double-dentate dinuclear connections, the CS/AS mixed depressant exhibits strong selectivity, according to the results of molecular simulations. Its adsorption on the barite surface is primarily achieved through hydrogen bonding. Water molecules hydroxylate the barite surface to increase its hydrophilicity by acting as a bridge between the CS/AS and barite (001) surfaces.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"701 ","pages":"Article 163252"},"PeriodicalIF":6.3,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143824857","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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