Pub Date : 2025-02-19DOI: 10.1016/j.apsusc.2025.162731
Byung Sun Yoon, Jae-Rang Youn, Wan-Gil Jung, Gwan-Joong Park, Da-Bin Kang, Sung-Bin Choi, Su-Ji Kim, Woohyun Kim, Chang Hyun Ko
Catalytic methane decomposition (CMD) is a promising reaction for hydrogen production without direct CO2 emissions. During CMD, gas-phase hydrogen and solid-phase carbon are produced, necessitating strategic catalyst design to manage carbon yield. In this study, we investigated the influence of narrow mesopores in catalysts for CMD. Using Ni supported on mesoporous silica (5.5 nm pore diameter) as a model catalyst, we prepared two types of catalysts: one with Ni0 particles located outside the pores and the other with Ni0 particles situated within the pores, and applied them to CMD. The catalysts with Ni0 particles within the pores exhibited lower carbon yield and produced carbon materials with lower graphitic quality compared to catalysts with Ni0 particles located outside the pores. Ni0 particles within the pores generated defect-rich carbon materials due to spatial limitations, resulting in decreased accessibility for CMD.
{"title":"Catalytic methane decomposition using Ni supported on mesoporous SiO2 catalyst: Ni position-dependent carbon yield change","authors":"Byung Sun Yoon, Jae-Rang Youn, Wan-Gil Jung, Gwan-Joong Park, Da-Bin Kang, Sung-Bin Choi, Su-Ji Kim, Woohyun Kim, Chang Hyun Ko","doi":"10.1016/j.apsusc.2025.162731","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162731","url":null,"abstract":"Catalytic methane decomposition (CMD) is a promising reaction for hydrogen production without direct CO<sub>2</sub> emissions. During CMD, gas-phase hydrogen and solid-phase carbon are produced, necessitating strategic catalyst design to manage carbon yield. In this study, we investigated the influence of narrow mesopores in catalysts for CMD. Using Ni supported on mesoporous silica (5.5 nm pore diameter) as a model catalyst, we prepared two types of catalysts: one with Ni<sup>0</sup> particles located outside the pores and the other with Ni<sup>0</sup> particles situated within the pores, and applied them to CMD. The catalysts with Ni<sup>0</sup> particles within the pores exhibited lower carbon yield and produced carbon materials with lower graphitic quality compared to catalysts with Ni<sup>0</sup> particles located outside the pores. Ni<sup>0</sup> particles within the pores generated defect-rich carbon materials due to spatial limitations, resulting in decreased accessibility for CMD.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"15 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451453","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 : 2025-02-19DOI: 10.1016/j.apsusc.2025.162740
Yongbing Gu, Qingshuang Ma, Xinmeng Li, Xuanhan Ye, Rongxin Zhang, Jiayi Liu, Xia Luo, Qiufang Yao, Yongyong Cao
Electrochemical synthesis using carbon dioxide (CO2) and nitric oxide (NO) offers a sustainable method for producing valuable chemicals like methylamine, yet the combined process remains underexplored, particularly in catalyst design for effective C–N coupling. Here, we present a γ-graphdiyne (GDY) −supported CuCo hybrid double atom catalyst (CuCo@GDY), designed and evaluated for the electrochemical synthesis of methylamine from CO2 and NO by density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations. CuCo@GDY demonstrates exceptional stability and catalytic activity, with synergistic Cu and Co sites that efficiently adsorb and activate NO and CO2. A new mechanism for methylamine synthesis is proposed on CuCo@GDY, emphasizing the critical role of *CH2O and *NH2OH intermediates in enabling effective C–N coupling. The methylamine formation exhibits low thermodynamic barriers of 0.75 eV and dynamic barriers of 1.10 eV on CuCo@GDY. It also effectively suppresses the hydrogen evolution reaction (HER) and other side reactions, enhancing methylamine selectivity. Its combination of single-atom and hybrid double-atom effects significantly enhances hydrogenation and C–N bond formation, leading to high selectivity and catalytic activity for methylamine production. Our findings provide a scalable approach for sustainable methylamine production, offering new insights into hybrid double atom catalyst design and advancing electrocatalytic C–N coupling with broad environmental and energy implications.
{"title":"Electrocatalytic C–N coupling on hybrid double-atom catalysts for methylamine synthesis from CO2 and NO","authors":"Yongbing Gu, Qingshuang Ma, Xinmeng Li, Xuanhan Ye, Rongxin Zhang, Jiayi Liu, Xia Luo, Qiufang Yao, Yongyong Cao","doi":"10.1016/j.apsusc.2025.162740","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162740","url":null,"abstract":"Electrochemical synthesis using carbon dioxide (CO<sub>2</sub>) and nitric oxide (NO) offers a sustainable method for producing valuable chemicals like methylamine, yet the combined process remains underexplored, particularly in catalyst design for effective C–N coupling. Here, we present a γ-graphdiyne (GDY) −supported CuCo hybrid double atom catalyst (CuCo@GDY), designed and evaluated for the electrochemical synthesis of methylamine from CO<sub>2</sub> and NO by density functional theory (DFT) and <em>ab initio</em> molecular dynamics (AIMD) calculations. CuCo@GDY demonstrates exceptional stability and catalytic activity, with synergistic Cu and Co sites that efficiently adsorb and activate NO and CO<sub>2</sub>. A new mechanism for methylamine synthesis is proposed on CuCo@GDY, emphasizing the critical role of *CH<sub>2</sub>O and *NH<sub>2</sub>OH intermediates in enabling effective C–N coupling. The methylamine formation exhibits low thermodynamic barriers of 0.75 eV and dynamic barriers of 1.10 eV on CuCo@GDY. It also effectively suppresses the hydrogen evolution reaction (HER) and other side reactions, enhancing methylamine selectivity. Its combination of single-atom and hybrid double-atom effects significantly enhances hydrogenation and C–N bond formation, leading to high selectivity and catalytic activity for methylamine production. Our findings provide a scalable approach for sustainable methylamine production, offering new insights into hybrid double atom catalyst design and advancing electrocatalytic C–N coupling with broad environmental and energy implications.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"1 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451497","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}
Non-specular effect (the lateral Goos-Hänchen (GH) shift and the photonic spin Hall effect (PSHE) induced transverse shift) of a light beam reflected from an interface with refractive index gradient has empowered metrology applications and recently been extended to the edge imaging. The structure parameter variations can exert a significant influence on the prism (Ge)-graphene terahertz (THz) surface plasmon resonance, for instance, the increment of layer number leads to a rise in the minimum reflectivity of resonance dip, and the correspondingly , and are changed, which give rise to the tunable non-specular effect. In addition, we reveal a mechanism for dimension-adjustable and orientation-switchable spatial differential operation, namely whether 2D or 1D differential is achieved and which direction differential is emerged. Compared to the previous woks, our scheme can be applied to edge detection without the aid of a quarter wave plate to achieve two-dimensional differential operations, because our results highly depending on the competition between the scale coefficients and , which are complex functions of these two shifts, and thus can be flexibly modulated via altering the Fermi energy or the incident polarization angle. Our differential scheme could have potential usage in the highly sensitive sensor and microscopic imaging.
{"title":"Graphene plasmons-assisted tunable non-specular effect for dimension-adjustable terahertz edge imaging","authors":"Jian Shi, Jing Deng, Jun Li, Yanbin Tang, Gangyun Xu, Chao Gu, Cuicui Li, Yanliang He, Jian Wu, Wen Yuan, Haimei Luo, Xianping Wang","doi":"10.1016/j.apsusc.2025.162737","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162737","url":null,"abstract":"Non-specular effect (the lateral Goos-Hänchen (GH) shift and the photonic spin Hall effect (PSHE) induced transverse shift) of a light beam reflected from an interface with refractive index gradient has empowered metrology applications and recently been extended to the edge imaging. The structure parameter variations can exert a significant influence on the prism (Ge)-graphene terahertz (THz) surface plasmon resonance, for instance, the increment of layer number leads to a rise in the minimum reflectivity of resonance dip, and the correspondingly <span><math><mfenced close=\"|\" is=\"true\" open=\"|\"><mrow is=\"true\"><mfrac is=\"true\"><msub is=\"true\"><mi is=\"true\">r</mi><mi is=\"true\">s</mi></msub><msub is=\"true\"><mi is=\"true\">r</mi><mi is=\"true\">p</mi></msub></mfrac></mrow></mfenced></math></span>, <span><math><mfenced close=\"|\" is=\"true\" open=\"|\"><mrow is=\"true\"><mfrac is=\"true\"><msub is=\"true\"><mi is=\"true\">r</mi><mi is=\"true\">p</mi></msub><msub is=\"true\"><mi is=\"true\">r</mi><mi is=\"true\">s</mi></msub></mfrac></mrow></mfenced></math></span> and <span><math><mrow is=\"true\"><mi is=\"true\">∂</mi><msub is=\"true\"><mi is=\"true\">φ</mi><mrow is=\"true\"><mi is=\"true\">p</mi><mo is=\"true\">,</mo><mi is=\"true\">s</mi></mrow></msub><mo is=\"true\" stretchy=\"false\">/</mo><mi is=\"true\">∂</mi><mi is=\"true\">θ</mi></mrow></math></span> are changed, which give rise to the tunable non-specular effect. In addition, we reveal a mechanism for dimension-adjustable and orientation-switchable spatial differential operation, namely whether 2D or 1D differential is achieved and which direction differential is emerged. Compared to the previous woks, our scheme can be applied to edge detection without the aid of a quarter wave plate to achieve two-dimensional differential operations, because our results highly depending on the competition between the scale coefficients <span><math><msub is=\"true\"><mi is=\"true\">C</mi><mi is=\"true\">x</mi></msub></math></span> and <span><math><msub is=\"true\"><mi is=\"true\">C</mi><mi is=\"true\">y</mi></msub></math></span>, which are complex functions of these two shifts, and thus can be flexibly modulated via altering the Fermi energy or the incident polarization angle. Our differential scheme could have potential usage in the highly sensitive sensor and microscopic imaging.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"47 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451455","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 : 2025-02-19DOI: 10.1016/j.apsusc.2025.162696
Hongmei Du, Yinru Li, Fei Zhao, Jingjing Xu, Yifei Su, Jinsheng Zhao, Konggang Qu, Xianxi Zhang
Finding catalysts with a high concentration of active sites and superior intrinsic activity is critical in boosting electrocatalytic efficiency. In this paper, Fe(Ni)Se2/Se-C3N4 is prepared through a hydrothermal and subsequent selenization method. The prepared Fe(Ni)Se2/Se-C3N4 catalyst exhibits outstanding OER performance, with a 225 mV overpotential at a current density of 10 mA cm−2. It also shows strong catalytic stability. After 856 h of testing at a current density of 2 mA cm−2, there is comparatively little current deterioration. The zinc-air battery assembled using Fe(Ni)Se2/Se-C3N4 as the catalyst shows a maximum specific capacity of 699.0 mAh g−1. At a current density of 273.1 mA cm−2, the power density increases to a maximum of 157.1 mW cm−2. The internal electron transport between Fe(Ni)Se2/Se and C3N4 modulates the electronic structure and subsequently enhances the catalytic performance, as demonstrated by synchronized radiation and theoretical calculations. The catalyst’s large specific surface area and abundance of active sites contribute to the improvement of catalytic activity. This work provides useful recommendations for the synthesis and design of efficient bifunctional catalysts in the future, facilitating the commercialization of electrocatalysis.
{"title":"Fe(Ni)Se2/Se nanoparticles anchored on C3N4 as highly active electrocatalysts in oxygen evolution reaction and liquid Zn-air batteries","authors":"Hongmei Du, Yinru Li, Fei Zhao, Jingjing Xu, Yifei Su, Jinsheng Zhao, Konggang Qu, Xianxi Zhang","doi":"10.1016/j.apsusc.2025.162696","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162696","url":null,"abstract":"Finding catalysts with a high concentration of active sites and superior intrinsic activity is critical in boosting electrocatalytic efficiency. In this paper, Fe(Ni)Se<sub>2</sub>/Se-C<sub>3</sub>N<sub>4</sub> is prepared through a hydrothermal and subsequent selenization method. The prepared Fe(Ni)Se<sub>2</sub>/Se-C<sub>3</sub>N<sub>4</sub> catalyst exhibits outstanding OER performance, with a 225 mV overpotential at a current density of 10 mA cm<sup>−2</sup>. It also shows strong catalytic stability. After 856 h of testing at a current density of 2 mA cm<sup>−2</sup>, there is comparatively little current deterioration. The zinc-air battery assembled using Fe(Ni)Se<sub>2</sub>/Se-C<sub>3</sub>N<sub>4</sub> as the catalyst shows a maximum specific capacity of 699.0 mAh g<sup>−1</sup>. At a current density of 273.1 mA cm<sup>−2</sup>, the power density increases to a maximum of 157.1 mW cm<sup>−2</sup>. The internal electron transport between Fe(Ni)Se<sub>2</sub>/Se and C<sub>3</sub>N<sub>4</sub> modulates the electronic structure and subsequently enhances the catalytic performance, as demonstrated by synchronized radiation and theoretical calculations. The catalyst’s large specific surface area and abundance of active sites contribute to the improvement of catalytic activity. This work provides useful recommendations for the synthesis and design of efficient bifunctional catalysts in the future, facilitating the commercialization of electrocatalysis.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"14 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451458","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 : 2025-02-19DOI: 10.1016/j.apsusc.2025.162743
Zhifei Zhu , Kejie Chai , Mengyi Wu , Lin Li , Xilin Shi , Pengfei Zhang , Weiming Xu
Electrocatalytic synthesis of high value-added nitrile from amines provides a green, sustainable, and cost-effective strategy. However, achieving high electrocatalytic efficiency often requires significant energy consumption. In this work, we designed a bimetallic co-doped Fe-Mn/NF electrocatalyst through a simple one-step hydrothermal process and utilized it for the electrocatalytic oxidation of benzylamine to produce benzonitrile. The current density of 10 mA cm−2 in the 0.5 M KOH electrolyte can be achieved with the voltage of only 1.34 V vs. reversible hydrogen electrode (RHE). The efficient electrocatalytic activity is mainly attributed to the synergistic effect and Jahn–Teller effect of the doped Fe and Mn within the Nickel Foam (NF) materials, thus promoting the formation of the active intermediate Ni3+ (NiOOH). Meanwhile, the in situ characterization confirmed the presence of NiOOH during the electrocatalytic oxidation. Notably, the benzonitrile and hydrogen, as products, can be automatically separated from the electrocatalytic system, providing a positive self-driving force for the electrocatalytic reaction. Thus, the Fe-Mn/NF electrocatalyst exhibits excellent catalytic performance, and the Faraday efficiency for benzonitrile synthesis exceeds 98 %. This work provides valuable insights for developing electrocatalysts that combine high catalytic efficiency with low energy consumption for the electrocatalytic synthesis of nitrile compounds.
{"title":"Low-overpotential, self-driving Fe-Mn co-doped nickel foam for highly efficient electrocatalytic oxidation of amines to nitriles","authors":"Zhifei Zhu , Kejie Chai , Mengyi Wu , Lin Li , Xilin Shi , Pengfei Zhang , Weiming Xu","doi":"10.1016/j.apsusc.2025.162743","DOIUrl":"10.1016/j.apsusc.2025.162743","url":null,"abstract":"<div><div>Electrocatalytic synthesis of high value-added nitrile from amines provides a green, sustainable, and cost-effective strategy. However, achieving high electrocatalytic efficiency often requires significant energy consumption. In this work, we designed a bimetallic co-doped Fe-Mn/NF electrocatalyst through a simple one-step hydrothermal process and utilized it for the electrocatalytic oxidation of benzylamine to produce benzonitrile. The current density of 10 mA cm<sup>−2</sup> in the 0.5 M KOH electrolyte can be achieved with the voltage of only 1.34 V <em>vs.</em> reversible hydrogen electrode (RHE). The efficient electrocatalytic activity is mainly attributed to the synergistic effect and Jahn–Teller effect of the doped Fe and Mn within the Nickel Foam (NF) materials, thus promoting the formation of the active intermediate Ni<sup>3+</sup> (NiOOH). Meanwhile, the in situ characterization confirmed the presence of NiOOH during the electrocatalytic oxidation. Notably, the benzonitrile and hydrogen, as products, can be automatically separated from the electrocatalytic system, providing a positive self-driving force for the electrocatalytic reaction. Thus, the Fe-Mn/NF electrocatalyst exhibits excellent catalytic performance, and the Faraday efficiency for benzonitrile synthesis exceeds 98 %. This work provides valuable insights for developing electrocatalysts that combine high catalytic efficiency with low energy consumption for the electrocatalytic synthesis of nitrile compounds.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162743"},"PeriodicalIF":6.3,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451457","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 : 2025-02-19DOI: 10.1016/j.apsusc.2025.162733
Seungwon Kang , Kiseok Lee , Keonkuk Kim , Jeongin Jang , Haeweon Jung , Bhakti D. Jadhav , Jae Sung Son , Ji Eun Lee
We report a simple, cost-effective, and environmentally friendly hydrothermal synthetic method for tellurium (Te) nanowires, using inexpensive precursors and water as a green solvent. The synthesized Te nanowires exhibit high crystallinity and uniform morphology, with lengths extending to several tens of microns. By adjusting the precursor concentration, we could easily control the length of the nanowires. The simplicity and low cost of this synthesis for Te nanowires enabled the production of sufficient quantities for consolidation into bulk pellets for thermoelectric property measurements. Compared to pellets made from commercial Te powder, the Te nanowire pellets demonstrated similar or slightly higher electrical conductivity and a significantly higher Seebeck coefficient, leading to an improved power factor. Additionally, the Te nanowire pellets exhibited reduced thermal conductivity, attributed to enhanced phonon scattering at the interfaces and the inherent porosity of the pellet. The combination of these factors resulted in superior thermoelectric performance, as indicated by higher ZT values across a range of temperatures. This study shows the potential of nanostructured Te for high-performance thermoelectric applications.
{"title":"Eco-friendly, low-cost synthesis of tellurium nanowires and their enhanced thermoelectric properties","authors":"Seungwon Kang , Kiseok Lee , Keonkuk Kim , Jeongin Jang , Haeweon Jung , Bhakti D. Jadhav , Jae Sung Son , Ji Eun Lee","doi":"10.1016/j.apsusc.2025.162733","DOIUrl":"10.1016/j.apsusc.2025.162733","url":null,"abstract":"<div><div>We report a simple, cost-effective, and environmentally friendly hydrothermal synthetic method for tellurium (Te) nanowires, using inexpensive precursors and water as a green solvent. The synthesized Te nanowires exhibit high crystallinity and uniform morphology, with lengths extending to several tens of microns. By adjusting the precursor concentration, we could easily control the length of the nanowires. The simplicity and low cost of this synthesis for Te nanowires enabled the production of sufficient quantities for consolidation into bulk pellets for thermoelectric property measurements. Compared to pellets made from commercial Te powder, the Te nanowire pellets demonstrated similar or slightly higher electrical conductivity and a significantly higher Seebeck coefficient, leading to an improved power factor. Additionally, the Te nanowire pellets exhibited reduced thermal conductivity, attributed to enhanced phonon scattering at the interfaces and the inherent porosity of the pellet. The combination of these factors resulted in superior thermoelectric performance, as indicated by higher ZT values across a range of temperatures. This study shows the potential of nanostructured Te for high-performance thermoelectric applications.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162733"},"PeriodicalIF":6.3,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451459","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 interface issues between solid-state electrolytes and electrodes severely hamper the development of solid-state lithium metal batteries. Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a competitive candidate among solid-state electrolytes due to its high ionic conductivity, air stability and low-cost. Nevertheless, the poor contact at electrolyte/electrode surface as well as the incompatibility between LATP and lithium metal obstruct its practical application. Herein, a buffer layer is designed on both sides of LATP to improve the interfacial contact and inhibit the side reaction occurs at the surface of Li anode. The in-situ formed interphase is a network structure composed of methyl methacrylate (MMA) and tetraethylene glycol dimethacrylate (TEGDMA), which can be triggered by thermal polymerization. The optimized interface enables continuous migration of lithium ions, thereby facilitating the dynamics of cations across the electrolyte and electrode interface. By this modification, the Li||Li symmetric cells assembled by the final product demonstrate high plating/stripping reversibility, and the Li||LiFePO4 cells can deliver a discharge capacity of 161 mAh g−1 at 0.1C. This study proposes a promising strategy for interfacial design and heralds an encouraging prospect for inorganic solid-state electrolytes in reliable utilization.
{"title":"Interfacial optimization of Li1.3Al0.3Ti1.7(PO4)3 based solid-state electrolyte by in-situ thermal polymerization for high reliability lithium metal batteries","authors":"Ting-Ting Chen, Yu-Hang Zhang, Yi-Wei Fan, Xin Jiang, Peng-Fei Wang, Yuhan Wu, Fa-Nian Shi","doi":"10.1016/j.apsusc.2025.162723","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162723","url":null,"abstract":"The interface issues between solid-state electrolytes and electrodes severely hamper the development of solid-state lithium metal batteries. Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LATP) is a competitive candidate among solid-state electrolytes due to its high ionic conductivity, air stability and low-cost. Nevertheless, the poor contact at electrolyte/electrode surface as well as the incompatibility between LATP and lithium metal obstruct its practical application. Herein, a buffer layer is designed on both sides of LATP to improve the interfacial contact and inhibit the side reaction occurs at the surface of Li anode. The <em>in-situ</em> formed interphase is a network structure composed of methyl methacrylate (MMA) and tetraethylene glycol dimethacrylate (TEGDMA), which can be triggered by thermal polymerization. The optimized interface enables continuous migration of lithium ions, thereby facilitating the dynamics of cations across the electrolyte and electrode interface. By this modification, the Li||Li symmetric cells assembled by the final product demonstrate high plating/stripping reversibility, and the Li||LiFePO<sub>4</sub> cells can deliver a discharge capacity of 161 mAh g<sup>−1</sup> at 0.1C. This study proposes a promising strategy for interfacial design and heralds an encouraging prospect for inorganic solid-state electrolytes in reliable utilization.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"81 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443753","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 : 2025-02-18DOI: 10.1016/j.apsusc.2025.162729
Yan Wang, Xiaoyue Fu, Yuxiu He, Xiyuan Li, Yingjie Feng
Anion exchange membrane water electrolysis (AEMWE) is a promising hydrogen production technology for clean energy storage and conversion applications. However, in practical applications, AEMWE still face various challenges, such as slow reaction kinetics and a poor durability. This study simultaneously performed chronopotentiometry for 672 h in a half-cell (200 mA cm−2) and 170 h in a single-cell (500 mA cm−2) to comprehensively evaluate the durability of a NiFe-LDH/NF electrode prepared via the hydrothermal deposition of a NiFe-layered double hydroxide (NiFe-LDH) on nickel felt (NF). The half-cell test results showed that after 672 h, the voltage degradation was only 2 mV compared to the initial voltage (1 h). The single-cell test results showed that below 30 h, the cell underwent an activation–stabilisation process, while after 170 h, the voltage degradation was only 45 mV compared to that at 30 h. In situ electrochemical Raman spectroscopy revealed that the formation of Ni(Fe)OOH at high potentials enhanced the oxygen evolution reaction activity of the NiFe-LDH/NF electrode. Meanwhile, TEM and SEM morphological observations showed that the three-dimensional flower-like cluster structure formed by the NiFe-LDH sheets was responsible for the high durability of the NiFe-LDH/NF electrode in both half-cell and single-cell tests.
{"title":"Enhanced stability of NiFe-layered double hydroxide for anion exchange membrane water electrolysis in half-cell and single-cell long-term testing","authors":"Yan Wang, Xiaoyue Fu, Yuxiu He, Xiyuan Li, Yingjie Feng","doi":"10.1016/j.apsusc.2025.162729","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162729","url":null,"abstract":"Anion exchange membrane water electrolysis (AEMWE) is a promising hydrogen production technology for clean energy storage and conversion applications. However, in practical applications, AEMWE still face various challenges, such as slow reaction kinetics and a poor durability. This study simultaneously performed chronopotentiometry for 672 h in a half-cell (200 mA cm<sup>−2</sup>) and 170 h in a single-cell (500 mA cm<sup>−2</sup>) to comprehensively evaluate the durability of a NiFe-LDH/NF electrode prepared via the hydrothermal deposition of a NiFe-layered double hydroxide (NiFe-LDH) on nickel felt (NF). The half-cell test results showed that after 672 h, the voltage degradation was only 2 mV compared to the initial voltage (1 h). The single-cell test results showed that below 30 h, the cell underwent an activation–stabilisation process, while after 170 h, the voltage degradation was only 45 mV compared to that at 30 h. In situ electrochemical Raman spectroscopy revealed that the formation of Ni(Fe)OOH at high potentials enhanced the oxygen evolution reaction activity of the NiFe-LDH/NF electrode. Meanwhile, TEM and SEM morphological observations showed that the three-dimensional flower-like cluster structure formed by the NiFe-LDH sheets was responsible for the high durability of the NiFe-LDH/NF electrode in both half-cell and single-cell tests.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"11 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443755","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 : 2025-02-18DOI: 10.1016/j.apsusc.2025.162717
Ziheng Jia , Xiaolei Song , Ziteng Su , Zhenxin Duan , Qi Sui , You Yang , Ying Han , Xu Ran , Yang Liu
TiAl alloys, known for their low density and high strength, are used as structural components in aircraft engines at high temperatures. Considering the high-temperature application environment, their oxidation resistance becomes an essential requirement. In this study, Ti-48Al-2Cr-2Nb alloy was buried in SiO2 powder and heat-treated at 1000 °C for 5 h under vacuum circumstance. After diffusion reaction, an ∼ 3 μm thick Al2O3/Ti5Si3 composite coating was successfully fabricated on the alloy surface. This novel coating was composed of a continuous Ti5Si3 layer and discontinuous Al2O3 layers surrounded by Ti5Si3. After 100 h oxidation, the mass gain of the coated sample was only 2.93 mg·cm−2, significantly lower than the 10.30 mg·cm−2 for the uncoated TiAl alloys. The higher oxidation temperature of the Ti5Si3 surface layer contributed to the excellent high-temperature oxidation resistance of the composite coating. Additionally, the formation of Al2O3 and SiO2 during oxidation and the presence of the discontinuous Al2O3 layers within the coating reduced the effective cross-sectional area for elemental diffusion, thereby delaying the inward diffusion of O and further enhancing the oxidation resistance.
{"title":"Enhancing the high-temperature oxidation resistance of TiAl alloy via a novel Al2O3/Ti5Si3 composite coating prepared through a modified pack cementation technique","authors":"Ziheng Jia , Xiaolei Song , Ziteng Su , Zhenxin Duan , Qi Sui , You Yang , Ying Han , Xu Ran , Yang Liu","doi":"10.1016/j.apsusc.2025.162717","DOIUrl":"10.1016/j.apsusc.2025.162717","url":null,"abstract":"<div><div>TiAl alloys, known for their low density and high strength, are used as structural components in aircraft engines at high temperatures. Considering the high-temperature application environment, their oxidation resistance becomes an essential requirement. In this study, Ti-48Al-2Cr-2Nb alloy was buried in SiO<sub>2</sub> powder and heat-treated at 1000 °C for 5 h under vacuum circumstance. After diffusion reaction, an ∼ 3 μm thick Al<sub>2</sub>O<sub>3</sub>/Ti<sub>5</sub>Si<sub>3</sub> composite coating was successfully fabricated on the alloy surface. This novel coating was composed of a continuous Ti<sub>5</sub>Si<sub>3</sub> layer and discontinuous Al<sub>2</sub>O<sub>3</sub> layers surrounded by Ti<sub>5</sub>Si<sub>3</sub>. After 100 h oxidation, the mass gain of the coated sample was only 2.93 mg·cm<sup>−2</sup>, significantly lower than the 10.30 mg·cm<sup>−2</sup> for the uncoated TiAl alloys. The higher oxidation temperature of the Ti<sub>5</sub>Si<sub>3</sub> surface layer contributed to the excellent high-temperature oxidation resistance of the composite coating. Additionally, the formation of Al<sub>2</sub>O<sub>3</sub> and SiO<sub>2</sub> during oxidation and the presence of the discontinuous Al<sub>2</sub>O<sub>3</sub> layers within the coating reduced the effective cross-sectional area for elemental diffusion, thereby delaying the inward diffusion of O and further enhancing the oxidation resistance.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162717"},"PeriodicalIF":6.3,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443750","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}
Palladium is widely used in hydrogen sensing due to its excellent catalytic dissociation of hydrogen. However, the size, dispersion and density of palladium particles affect its role in enhancing gas-sensitive properties. In this work, we use a simple and effective method to anchor Pd quantum dots with the help of surface oxygen vacancies. The sensing results show that the response value (S = Ra/Rg) of the material loaded with Pd quantum dots on surface oxygen vacancies (Pd-WO3/WOx) for 50 ppm hydrogen at 160℃ is 13.37. Moreover, the Pd-WO3/WOx material exhibits excellent selectivity and good linearity over the test range. Furthermore, experimental results and DFT calculations reveal that surface oxygen vacancies can shift the d-band center of metallic Pd upward, which enhances the adsorption of hydrogen by Pd. This study provides new ideas for designing high-performance precious metal-loaded metal oxide semiconductor hydrogen sensors.
{"title":"Oxygen vacancies engineering and palladium quantum dots sensitized WO3 nanosheet for highly efficiently H2 detection","authors":"Beixi An, Yifan Yang, Jiaqi Yan, Yanrong Wang, Ruixia Li, Zhengkun Wu, Tingyu Zhang, Ruiqi Han, Xu Cheng, Qiao Wang, Erqing Xie","doi":"10.1016/j.apsusc.2025.162722","DOIUrl":"10.1016/j.apsusc.2025.162722","url":null,"abstract":"<div><div>Palladium is widely used in hydrogen sensing due to its excellent catalytic dissociation of hydrogen. However, the size, dispersion and density of palladium particles affect its role in enhancing gas-sensitive properties. In this work, we use a simple and effective method to anchor Pd quantum dots with the help of surface oxygen vacancies. The sensing results show that the response value (S = R<sub>a</sub>/R<sub>g</sub>) of the material loaded with Pd quantum dots on surface oxygen vacancies (Pd-WO<sub>3</sub>/WO<sub>x</sub>) for 50 ppm hydrogen at 160℃ is 13.37. Moreover, the Pd-WO<sub>3</sub>/WO<sub>x</sub> material exhibits excellent selectivity and good linearity over the test range. Furthermore, experimental results and DFT calculations reveal that surface oxygen vacancies can shift the d-band center of metallic Pd upward, which enhances the adsorption of hydrogen by Pd. This study provides new ideas for designing high-performance precious metal-loaded metal oxide semiconductor hydrogen sensors.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162722"},"PeriodicalIF":6.3,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443751","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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