Van der Waals heterojunctions (vdWHs) have garnered significant attention for their promising applications in optoelectronics, attributed to their exceptional physical attributes. In this study, we present a straightforward approach to fabricating high-performance vdWHs photodetectors. Specifically, we prepared WSOx/WS2 vdWH photodetectors through the ozone oxidation of a WS2 thin films at 100 °C. To characterize the morphology and optical properties of both the WS2 and WSOx/WS2 thin films, we utilized atomic force microscopy (AFM) and Raman spectroscopy. Additionally, X-ray photoelectron spectroscopy (XPS) was employed to delve into the structural evolution by scrutinizing the bonding states of W, O, and S in the WS2 before and after the ozone oxidation process. The resultant WSOx/WS2 vdWH photodetectors exhibited impressive photoelectric performance at wavelengths of 475 nm and 532 nm. It demonstrated a high responsivity of 230.7 A/W, a remarkable specific detectivity of 1.794 × 1011 Jones, and a swift response speed of 60 ms at 475 nm. Furthermore, first-principles calculations based on density functional theory (DFT) were conducted to validate the oxidation kinetics of monolayer WS2, the type II energy band alignment, and the interlayer charge transfer within the WSOx/WS2 vdWH. This research contributes novel insights into the synthesis of two-dimensional transition metal oxides (TMOs)-transition metal dichalcogenides (TMDCs) heterostructures for photodetector applications.
{"title":"High-performance type II WSOx/WS2-based heterojunction photodetectors","authors":"Weiqi shi, Yifang Ding, Shaojun Fang, Hong Zhou, Jiao Qi, Jiajie Fan, Rongjun Zhang, Guoqi Zhang, Hongyu Tang","doi":"10.1016/j.apsusc.2024.161848","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161848","url":null,"abstract":"Van der Waals heterojunctions (vdWHs) have garnered significant attention for their promising applications in optoelectronics, attributed to their exceptional physical attributes. In this study, we present a straightforward approach to fabricating high-performance vdWHs photodetectors. Specifically, we prepared WSO<sub>x</sub>/WS<sub>2</sub> vdWH photodetectors through the ozone oxidation of a WS<sub>2</sub> thin films at 100 °C. To characterize the morphology and optical properties of both the WS<sub>2</sub> and WSO<sub>x</sub>/WS<sub>2</sub> thin films, we utilized atomic force microscopy (AFM) and Raman spectroscopy. Additionally, X-ray photoelectron spectroscopy (XPS) was employed to delve into the structural evolution by scrutinizing the bonding states of W, O, and S in the WS<sub>2</sub> before and after the ozone oxidation process. The resultant WSO<sub>x</sub>/WS<sub>2</sub> vdWH photodetectors exhibited impressive photoelectric performance at wavelengths of 475 nm and 532 nm. It demonstrated a high responsivity of 230.7 A/W, a remarkable specific detectivity of 1.794 × 10<sup>11</sup> Jones, and a swift response speed of 60 ms at 475 nm. Furthermore, first-principles calculations based on density functional theory (DFT) were conducted to validate the oxidation kinetics of monolayer WS<sub>2</sub>, the type II energy band alignment, and the interlayer charge transfer within the WSO<sub>x</sub>/WS<sub>2</sub> vdWH. This research contributes novel insights into the synthesis of two-dimensional transition metal oxides (TMOs)-transition metal dichalcogenides (TMDCs) heterostructures for photodetector applications.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"128 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670877","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 : 2024-11-19DOI: 10.1016/j.apsusc.2024.161838
Roland Milatz, Joost Duvigneau, G.Julius Vancso
Catechol-containing copolymers are a class of polymers often encompassing polydopamine and are considered as biomimetic candidates for high-performance adhesives. However, improvements in adhesive layer stability are needed for high-performance applications to enhance the cohesive strength of the adhesive layers. In this paper, we address this challenge by introducing multiple strategies, including thermal treatment and codeposition. We synthesize a copolymer with adhesive dopamine methacrylamide (DOMA), segmental “filler” methyl methacrylate (MMA), and ATRP-initiator 2-(2-bromoisobutyryloxy)ethyl methacrylate (BIEM). This copolymer is spin coated on silicon wafers, annealed at increasing temperatures, and deposited in combination with (3-aminopropyl)triethoxysilane (APTES), iron chloride (FeCl3), or copper chloride (CuCl2) on silicon and polyethylene substrates. The layers are characterized using ellipsometry, atomic force microscopy (AFM), and Fourier transform infrared (FTIR) spectroscopy. Subsequently, we demonstrate the grafting of a zwitterionic polysulfobetaine methacrylate (PSBMA) layer from the BIEM moiety of the codeposited films. Annealing at 200 °C crosslinks the polymer so that almost no physisorbed material remains to be washed off, resulting in enhanced layer stability. Reinforcement through co-deposition shows that using APTES and FeCl3 improved the copolymer layer to graft PSBMA layers from the surface, something that copolymer films cannot exhibit without codeposition. Thus, we demonstrate two pathways based on lessons learned from mussel-based adhesion that can be used to improve PDA-based film formation.
{"title":"Codeposition strategies for improved layer stability in bio-inspired catechol-containing adhesives","authors":"Roland Milatz, Joost Duvigneau, G.Julius Vancso","doi":"10.1016/j.apsusc.2024.161838","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161838","url":null,"abstract":"Catechol-containing copolymers are a class of polymers often encompassing polydopamine and are considered as biomimetic candidates for high-performance adhesives. However, improvements in adhesive layer stability are needed for high-performance applications to enhance the cohesive strength of the adhesive layers. In this paper, we address this challenge by introducing multiple strategies, including thermal treatment and codeposition. We synthesize a copolymer with adhesive dopamine methacrylamide (DOMA), segmental “filler” methyl methacrylate (MMA), and ATRP-initiator 2-(2-bromoisobutyryloxy)ethyl methacrylate (BIEM). This copolymer is spin coated on silicon wafers, annealed at increasing temperatures, and deposited in combination with (3-aminopropyl)triethoxysilane (APTES), iron chloride (FeCl<sub>3</sub>), or copper chloride (CuCl<sub>2</sub>) on silicon and polyethylene substrates. The layers are characterized using ellipsometry, atomic force microscopy (AFM), and Fourier transform infrared (FTIR) spectroscopy. Subsequently, we demonstrate the grafting of a zwitterionic polysulfobetaine methacrylate (PSBMA) layer from the BIEM moiety of the codeposited films. Annealing at 200 °C crosslinks the polymer so that almost no physisorbed material remains to be washed off, resulting in enhanced layer stability. Reinforcement through co-deposition shows that using APTES and FeCl3 improved the copolymer layer to graft PSBMA layers from the surface, something that copolymer films cannot exhibit without codeposition. Thus, we demonstrate two pathways based on lessons learned from mussel-based adhesion that can be used to improve PDA-based film formation.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"7 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670865","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}
Herein, mesoporous Mg(OH)2 is prepared by one-step hydration method using microcrystalline magnesite as raw material and acetic acid as hydration agent, and the mesoporous MgO is obtained after thermal conversion. The adsorption experiments on three single dye systems (Congo red (CR), methyl orange (MO) and methylene blue (MB)) and three binary mixed dye systems (CR/MO, CR/MB and MO/MB) show that mesoporous MgO possesses superior adsorption selectivity towards anionic dyes. The mesoporous Mg(OH)2 with cardroom-like structure, obvious pore channel and abundant edge and concern shows good adsorption capacity for CR (6591.96 mg/g) and MO (3087.04 mg/g). The mesoporous MgO obtained by calcination has high specific surface area (66 m2/g) and partially inherits the cardroom-like structure of Mg(OH)2, exhibiting remarkable adsorption performance (CR: 10521.89 mg/g; MO: 6694.65 mg/g). CR and MO adsorption on the Mg(OH)2/MgO accords with the Langmuir model and pseudo-second-order kinetic model. The density functional theory (DFT) is employed to evaluate the reactivity of CR/MO, such as molecular frontier orbital energies and energy gap, demonstrating that CR exhibits superior reactivity and adsorptive capacity in comparison to MO. The MgO sample is regenerated by calcination after CR/MO adsorption and the CR removal efficiency of MgO reaches above 85 % after 10 cycles.
{"title":"Carboxylic acid-assisted hydration for the preparation of mesoporous magnesium hydroxide/magnesium oxide with ultra-high adsorption performance and selective adsorption: Experiments and DFT investigations","authors":"Jun Li, Yanran Li, Ziyu Zhang, Rongzheng Gao, Zihan Zhao, Shichen Xing, Dongmo Wu, Heqi Qi, Dong Zhang, Xiaoli Tian, Cheng Liu, Lingling Zhu, Chengliang Ma","doi":"10.1016/j.apsusc.2024.161849","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161849","url":null,"abstract":"Herein, mesoporous Mg(OH)<sub>2</sub> is prepared by one-step hydration method using microcrystalline magnesite as raw material and acetic acid as hydration agent, and the mesoporous MgO is obtained after thermal conversion. The adsorption experiments on three single dye systems (Congo red (CR), methyl orange (MO) and methylene blue (MB)) and three binary mixed dye systems (CR/MO, CR/MB and MO/MB) show that mesoporous MgO possesses superior adsorption selectivity towards anionic dyes. The mesoporous Mg(OH)<sub>2</sub> with cardroom-like structure, obvious pore channel and abundant edge and concern shows good adsorption capacity for CR (6591.96 mg/g) and MO (3087.04 mg/g). The mesoporous MgO obtained by calcination has high specific surface area (66 m<sup>2</sup>/g) and partially inherits the cardroom-like structure of Mg(OH)<sub>2</sub>, exhibiting remarkable adsorption performance (CR: 10521.89 mg/g; MO: 6694.65 mg/g). CR and MO adsorption on the Mg(OH)<sub>2</sub>/MgO accords with the Langmuir model and pseudo-second-order kinetic model. The density functional theory (DFT) is employed to evaluate the reactivity of CR/MO, such as molecular frontier orbital energies and energy gap, demonstrating that CR exhibits superior reactivity and adsorptive capacity in comparison to MO. The MgO sample is regenerated by calcination after CR/MO adsorption and the CR removal efficiency of MgO reaches above 85 % after 10 cycles.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"9 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670906","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 : 2024-11-19DOI: 10.1016/j.apsusc.2024.161839
Bao Zhang, Chao Zheng, Zhiming Xiao, Keyi Xian, Heng Wen, Na Lu, Xinyou He, Long Ye, Jiexi Wang, Xing Ou, Chunhui Wang
Nickel-rich cobalt-low layered oxides have attracted much attention as positive electrode materials for high-energy lithium-ion batteries due to their high capacity and low cost, but their inherent stress accumulation and severe cationic mixed reactions will deteriorate the cycling performance. Herein, the nickel-rich single-crystalline LiNi0.90Co0.06Mn0.04O2 cathode material doped with W and Mg (NCM-WM) has been fabricated to overcome its structure degradation issues. It can be found that the Li/Ni cation mixture can be suppressed by the introduction of Mg2+ into Li+ situs and the replacement of transition metal ions by W6+. Meanwhile, the co-doing strategy synergistically depresses the irreversible H2-H3 phase transition to weaken the internal stress, and employs the heteroatoms as the pillar ions to prevent layer structure collapse. In addition, the reduced particle size induced by the W6+ and increased free electron resulted by Mg2+ can cooperatively improve the migration kinetics of ions and electrons in the process of cycling. As expected, the above advanced effects result in the prominent cycling properties (capacity retention of 86.7 %, 150 cycles, 2C) of the designed Ni-rich electrode materials. These results demonstrate that the co-doped design is a greatly effective strategy to reinforce the cycling performance of Ni-rich single-crystalline materials.
{"title":"Synergistic doping chemistry enable the cycling properties of single-crystal Ni-rich cathode for lithium-ion batteries","authors":"Bao Zhang, Chao Zheng, Zhiming Xiao, Keyi Xian, Heng Wen, Na Lu, Xinyou He, Long Ye, Jiexi Wang, Xing Ou, Chunhui Wang","doi":"10.1016/j.apsusc.2024.161839","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161839","url":null,"abstract":"Nickel-rich cobalt-low layered oxides have attracted much attention as positive electrode materials for high-energy lithium-ion batteries due to their high capacity and low cost, but their inherent stress accumulation and severe cationic mixed reactions will deteriorate the cycling performance. Herein, the nickel-rich single-crystalline LiNi<sub>0.90</sub>Co<sub>0.06</sub>Mn<sub>0.04</sub>O<sub>2</sub> cathode material doped with W and Mg (NCM-WM) has been fabricated to overcome its structure degradation issues. It can be found that the Li/Ni cation mixture can be suppressed by the introduction of Mg<sup>2+</sup> into Li<sup>+</sup> situs and the replacement of transition metal ions by W<sup>6+</sup>. Meanwhile, the co-doing strategy synergistically depresses the irreversible H2-H3 phase transition to weaken the internal stress, and employs the heteroatoms as the pillar ions to prevent layer structure collapse. In addition, the reduced particle size induced by the W<sup>6+</sup> and increased free electron resulted by Mg<sup>2+</sup> can cooperatively improve the migration kinetics of ions and electrons in the process of cycling. As expected, the above advanced effects result in the prominent cycling properties (capacity retention of 86.7 %, 150 cycles, 2C) of the designed Ni-rich electrode materials. These results demonstrate that the co-doped design is a greatly effective strategy to reinforce the cycling performance of Ni-rich single-crystalline materials.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"40 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670868","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 : 2024-11-19DOI: 10.1016/j.apsusc.2024.161828
Yan Zheng, Jinshu Lu, Xuan Wang, Tianbo Jia, Jinyi Cai, Dingkai Zhou, Yuexin Qian, Yamin Fu, Chunyang Zhai, Hengcong Tao, Yingtang Zhou, Shunli Li
Seawater splitting to produce hydrogen holds promise for renewable energy but faces challenges from chloride ions, causing electrode corrosion and competition between chlorine oxidation reaction (ClOR) and oxygen evolution reaction (OER). Therefore, it is crucial to develop highly efficient and stable electrocatalysts for seawater splitting. Here, we employ a dual-doping strategy of Mo/Cr cations and a sulfuration approach to fabricate the S-MoCr-NiFe@NF bifunctional catalyst with a 3D nano-flower structure. The S-MoCr-NiFe@NF catalyst exhibits remarkable catalytic performance for the oxygen evolution reaction (OER) in 1.0 M KOH + 0.5 M NaCl and 1.0 M KOH + Seawater, achieving current densities of 10 mA cm−2 at low overpotentials of 116 and 141 mV, respectively. Furthermore, it was demonstrated that the S-MoCr-NiFe@NF catalyst exhibited remarkable performance in alkaline overall seawater splitting, requiring only 1.48 and 1.57 V to achieve current densities of 10 mA cm−2 in 1.0 M KOH + 0.5 M NaCl and 1.0 M KOH + Seawater, respectively. The in-situ Raman and DFT calculations confirm Ni as the primary active sites, reducing the energy barrier of the rate-determining step and enhancing OER performance. This study will offer a viable approach to developing and creating highly effective bifunctional catalysts for seawater splitting.
海水裂解制氢有望成为可再生能源，但面临着氯离子造成的电极腐蚀以及氯氧化反应（ClOR）和氧进化反应（OER）之间的竞争等挑战。因此，开发高效稳定的海水裂解电催化剂至关重要。在此，我们采用钼/铬阳离子双掺杂策略和硫化方法，制备出具有三维纳米花结构的 S-MoCr-NiFe@NF 双功能催化剂。S-MoCr-NiFe@NF 催化剂在 1.0 M KOH + 0.5 M NaCl 和 1.0 M KOH + 海水中的氧进化反应（OER）中表现出卓越的催化性能，分别在 116 和 141 mV 的低过电位下实现了 10 mA cm-2 的电流密度。此外，研究还表明，S-MoCr-NiFe@NF 催化剂在碱性整体海水拆分中表现出卓越的性能，在 1.0 M KOH + 0.5 M NaCl 和 1.0 M KOH + 海水中分别只需要 1.48 和 1.57 V 就能达到 10 mA cm-2 的电流密度。原位拉曼和 DFT 计算证实，镍是主要的活性位点，可降低决定速率步骤的能障，提高 OER 性能。这项研究将为开发和创造用于海水分离的高效双功能催化剂提供一种可行的方法。
{"title":"Modulation of oxygen vacancies in NiFe layered double hydroxides through dual-doping with Mo/Cr cations for efficient seawater hydrogen production","authors":"Yan Zheng, Jinshu Lu, Xuan Wang, Tianbo Jia, Jinyi Cai, Dingkai Zhou, Yuexin Qian, Yamin Fu, Chunyang Zhai, Hengcong Tao, Yingtang Zhou, Shunli Li","doi":"10.1016/j.apsusc.2024.161828","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161828","url":null,"abstract":"Seawater splitting to produce hydrogen holds promise for renewable energy but faces challenges from chloride ions, causing electrode corrosion and competition between chlorine oxidation reaction (ClOR) and oxygen evolution reaction (OER). Therefore, it is crucial to develop highly efficient and stable electrocatalysts for seawater splitting. Here, we employ a dual-doping strategy of Mo/Cr cations and a sulfuration approach to fabricate the S-MoCr-NiFe@NF bifunctional catalyst with a 3D nano-flower structure. The S-MoCr-NiFe@NF catalyst exhibits remarkable catalytic performance for the oxygen evolution reaction (OER) in 1.0 M KOH + 0.5 M NaCl and 1.0 M KOH + Seawater, achieving current densities of 10 mA cm<sup>−2</sup> at low overpotentials of 116 and 141 mV, respectively. Furthermore, it was demonstrated that the S-MoCr-NiFe@NF catalyst exhibited remarkable performance in alkaline overall seawater splitting, requiring only 1.48 and 1.57 V to achieve current densities of 10 mA cm<sup>−2</sup> in 1.0 M KOH + 0.5 M NaCl and 1.0 M KOH + Seawater, respectively. The in-situ Raman and DFT calculations confirm Ni as the primary active sites, reducing the energy barrier of the rate-determining step and enhancing OER performance. This study will offer a viable approach to developing and creating highly effective bifunctional catalysts for seawater splitting.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"106 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670870","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 development of biomass materials can effectively mitigate the scarcity of energy and minimize resource waste. In this work, onion-like biomass carbon nanoparticles (OLCs) were prepared using rice husk ash (RHA) which was subjected to a high-temperature graphitization reaction catalyzed by iron nitrate. OLCs/molybdenum disulfide (MoS2) composite particles were prepared and incorporated into polyimide (PI), and a composite coating of OLCs/MoS2/PI with excellent tribological properties was successfully prepared. The tribological properties of coatings were evaluated using a controlled atmosphere tribometer (WMT-2E) under dry friction conditions. The related friction and wear mechanism of PI coatings including particles was clarified by the SEM/EDS, XPS, HRTEM and DFT theory. Results show that the wear rate of the three composite coatings of polyimide with OLC, MoS2, and OLC/MoS2 particles were reduced by 52.9 %, 48.2 %, and 58.1 %, respectively. For the coefficient of friction, PI-0.20 OLC/MoS2 coating material decreased by 16.1 %. Anti-wear and friction reduction mechanism is attributed to the presence of a transfer film on the surface of the steel balls. The addition of MoS2 facilitated the deposition of nanoparticles, which further improved the stability and densification of the friction film, resulting in better protection of the metal surface against severe wear. Besides, the component structure changes of OLCs and MoS2 and adsorption energy of friction products on the surface of tribo-pairs were also important reasons for clarifying the modification tribological behavior of PI coatings including three kinds of nanoparticles.
{"title":"Investigate on preparation and dry tribological behaviors of onion-like carbon/MoS2 polyimide coatings","authors":"XingPeng Fei, Shusheng Liu, Ayush Subedi, Xinkai Ding, Enzhu Hu, Kunhong Hu","doi":"10.1016/j.apsusc.2024.161846","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161846","url":null,"abstract":"The development of biomass materials can effectively mitigate the scarcity of energy and minimize resource waste. In this work, onion-like biomass carbon nanoparticles (OLCs) were prepared using rice husk ash (RHA) which was subjected to a high-temperature graphitization reaction catalyzed by iron nitrate. OLCs/molybdenum disulfide (MoS<sub>2</sub>) composite particles were prepared and incorporated into polyimide (PI), and a composite coating of OLCs/MoS<sub>2</sub>/PI with excellent tribological properties was successfully prepared. The tribological properties of coatings were evaluated using a controlled atmosphere tribometer (WMT-2E) under dry friction conditions. The related friction and wear mechanism of PI coatings including particles was clarified by the SEM/EDS, XPS, HRTEM and DFT theory. Results show that the wear rate of the three composite coatings of polyimide with OLC, MoS<sub>2</sub>, and OLC/MoS<sub>2</sub> particles were reduced by 52.9 %, 48.2 %, and 58.1 %, respectively. For the coefficient of friction, PI-0.20 OLC/MoS<sub>2</sub> coating material decreased by 16.1 %. Anti-wear and friction reduction mechanism is attributed to the presence of a transfer film on the surface of the steel balls. The addition of MoS<sub>2</sub> facilitated the deposition of nanoparticles, which further improved the stability and densification of the friction film, resulting in better protection of the metal surface against severe wear. Besides, the component structure changes of OLCs and MoS<sub>2</sub> and adsorption energy of friction products on the surface of tribo-pairs were also important reasons for clarifying the modification tribological behavior of PI coatings including three kinds of nanoparticles.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"69 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670875","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 : 2024-11-19DOI: 10.1016/j.apsusc.2024.161844
Hongxiong Shu, Mei Zhao, Congming Tang, Kai Ma, Xinli Li
Controlling regioselectivity in lactic acid conversion is a key for production of bio-based chemicals due to bio-lactic acid molecule containing active bifunctional groups such as hydroxyl (–OH) and carboxyl (–COOH). Here, we report that the Ru-stabilized MoO3-x overlayers with rich oxygen vacancies overturn lactic acid hydrogenation regioselectivity to propionic acid (PA) via C-OH hydrodeoxygenation, achieving a high PA selectivity of 95.9%, which is completely different from the catalytic feature of the Ru particle surfaces with dominating 1,2-propanediol selectivity through hydrogenation of –COOH. Furthermore, the activity on the encapsulating oxide layers can be extended to other hydroxy acids such as glycolic acid, 3-hydroxypropionic acid, and DL-2-hydroxybutylic acid to generate their corresponding carboxylic acids, displaying a unique ability for hydrodeoxygenation of –OH group. The encapsulating oxide layers with rich oxygen vacancies can be dynamically generated in the presence of the reductive atmosphere such as H2-Ar mixture, and efficiently stabilized by Ru nanoparticles, thus endowing more excellent activity of Ru-MoO3-x than that of MoO3, MoO3-x and Ru-MoO3. Encouragingly, lactic acid conversion and propionic acid selectivity have hardly decayed during running 5 cycles due to Ru-stabilized MoO3-x overlayers. This work provides an efficient strategy for constructing the defective encapsulation oxide layers with rich oxygen vacancies, which helps to produce the desired bio-based chemical of PA from bio-lactic acid.
{"title":"Overturning lactic acid hydrogenation regioselectivity via Ru-stabilized MoO3-x overlayers","authors":"Hongxiong Shu, Mei Zhao, Congming Tang, Kai Ma, Xinli Li","doi":"10.1016/j.apsusc.2024.161844","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161844","url":null,"abstract":"Controlling regioselectivity in lactic acid conversion is a key for production of bio-based chemicals due to bio-lactic acid molecule containing active bifunctional groups such as hydroxyl (–OH) and carboxyl (–COOH). Here, we report that the Ru-stabilized MoO<sub>3-x</sub> overlayers with rich oxygen vacancies overturn lactic acid hydrogenation regioselectivity to propionic acid (PA) via C-OH hydrodeoxygenation, achieving a high PA selectivity of 95.9%, which is completely different from the catalytic feature of the Ru particle surfaces with dominating 1,2-propanediol selectivity through hydrogenation of –COOH. Furthermore, the activity on the encapsulating oxide layers can be extended to other hydroxy acids such as glycolic acid, 3-hydroxypropionic acid, and DL-2-hydroxybutylic acid to generate their corresponding carboxylic acids, displaying a unique ability for hydrodeoxygenation of –OH group. The encapsulating oxide layers with rich oxygen vacancies can be dynamically generated in the presence of the reductive atmosphere such as H<sub>2</sub>-Ar mixture, and efficiently stabilized by Ru nanoparticles, thus endowing more excellent activity of Ru-MoO<sub>3-x</sub> than that of MoO<sub>3</sub>, MoO<sub>3-x</sub> and Ru-MoO<sub>3</sub>. Encouragingly, lactic acid conversion and propionic acid selectivity have hardly decayed during running 5 cycles due to Ru-stabilized MoO<sub>3-x</sub> overlayers. This work provides an efficient strategy for constructing the defective encapsulation oxide layers with rich oxygen vacancies, which helps to produce the desired bio-based chemical of PA from bio-lactic acid.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"36 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673442","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 modulation of peroxymonosulfate (PMS) activation pathway to achieve effective degradation of pollutants is significant, but still challenging. Herein, a series of hydroxyl- and size-controlled MnFe2O4 catalysts were synthesized through an alkaline microenvironment regulation strategy. The variable-sized MnFe2O4 (submicron, nanoscale and microscale) exhibited size-dependent catalytic behavior, while the changes in surface hydroxyl content altered the activation pathway from dissolved radicals to surface-bound radicals. The quenching experiments, electron spin resonance spectroscopy, electrochemical studies, in-situ Raman spectra and density functional theory calculations were conducted to reveal the evolution of reactive oxygen species. Due to strong binding energy, PMS was stabilized by the rich surface hydroxyl to form surface complexed MnFe2O4-HOOSO3− and simultaneously activated by the active bimetallic components, resulting in oriented-production of surface-bonded radicals. Benefiting from smaller particle size and rich hydroxyl groups, the optimal nano-MnFe2O4-OH/PMS system could massively generate surface-bound SO4•−, which achieved a highly efficient removal efficiency (88.6 %) for ofloxacin (10 mg/L) degradation under wide pH ranges from 3.0 to 9.0. The evaluation of ecotoxicity, reusability, pH applicability, universality and anti-interference property confirmed the practical application prospect of nano-MnFe2O4-OH/PMS system.
{"title":"Switching peroxymonosulfate activation pathway from free radical to surface-bound radical over MnFe2O4 for enhanced degradation of ofloxacin: Key role of size effect and surface hydroxyl group","authors":"Siyue Huo, Wenxian Fu, Quanyou Zhao, Yichao Wang, Xuan Wu, Mengchun Gao, Xie Haijiao","doi":"10.1016/j.apsusc.2024.161762","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161762","url":null,"abstract":"The modulation of peroxymonosulfate (PMS) activation pathway to achieve effective degradation of pollutants is significant, but still challenging. Herein, a series of hydroxyl- and size-controlled MnFe<sub>2</sub>O<sub>4</sub> catalysts were synthesized through an alkaline microenvironment regulation strategy. The variable-sized MnFe<sub>2</sub>O<sub>4</sub> (submicron, nanoscale and microscale) exhibited size-dependent catalytic behavior, while the changes in surface hydroxyl content altered the activation pathway from dissolved radicals to surface-bound radicals. The quenching experiments, electron spin resonance spectroscopy, electrochemical studies, in-situ Raman spectra and density functional theory calculations were conducted to reveal the evolution of reactive oxygen species. Due to strong binding energy, PMS was stabilized by the rich surface hydroxyl to form surface complexed MnFe<sub>2</sub>O<sub>4</sub>-HOOSO<sub>3</sub><sup>−</sup> and simultaneously activated by the active bimetallic components, resulting in oriented-production of surface-bonded radicals. Benefiting from smaller particle size and rich hydroxyl groups, the optimal nano-MnFe<sub>2</sub>O<sub>4</sub>-OH/PMS system could massively generate surface-bound SO<sub>4</sub><sup>•−</sup>, which achieved a highly efficient removal efficiency (88.6 %) for ofloxacin (10 mg/L) degradation under wide pH ranges from 3.0 to 9.0. The evaluation of ecotoxicity, reusability, pH applicability, universality and anti-interference property confirmed the practical application prospect of nano-MnFe<sub>2</sub>O<sub>4</sub>-OH/PMS system.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"33 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673443","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 application of mechanization in different environments has put forward strict requirements for mechanical components, which also means higher requirements for cutting tools. It is precisely these requirements that drive the development of cutting tool preparation methods towards novelty and innovation. To effectively enhance the performance of dry cutting tools, laser micro-cladding technology has been innovatively adopted to achieve additive manufacturing of new textured cutting tools. The mechanical properties, tribological properties, and cutting performance of the newly textured tools were evaluated. The results indicate that the EHDA process can achieve uniformity and thickness controllability of the preset powder layer. In friction experiments, the friction coefficient of textured surfaces can be reduced by up to 44.3% compared to polished surfaces. In the cutting experiment, the cutting force of LCT tools has decreased by up to 26.7%, and the cutting temperature has decreased by a maximum of 32.5%. The research mechanism indicates that at lower cutting speeds, WS2 forms a lubricating film at the tool-chip contact interface, reducing shear strength and achieving a reduction in cutting force and cutting temperature. And the micro-textures are the main way for the LCT tool to reduce cutting force and cutting temperature at higher cutting speeds.
{"title":"In-situ forming textured cutting tools based on electrohydrodynamic atomization and laser micro-cladding technology","authors":"Yichen Bao, Jianxin Deng, Shenghan Cao, Xianshun Sun, Zhihui Zhang, Xujie Tang","doi":"10.1016/j.apsusc.2024.161856","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161856","url":null,"abstract":"The application of mechanization in different environments has put forward strict requirements for mechanical components, which also means higher requirements for cutting tools. It is precisely these requirements that drive the development of cutting tool preparation methods towards novelty and innovation. To effectively enhance the performance of dry cutting tools, laser micro-cladding technology has been innovatively adopted to achieve additive manufacturing of new textured cutting tools. The mechanical properties, tribological properties, and cutting performance of the newly textured tools were evaluated. The results indicate that the EHDA process can achieve uniformity and thickness controllability of the preset powder layer. In friction experiments, the friction coefficient of textured surfaces can be reduced by up to 44.3% compared to polished surfaces. In the cutting experiment, the cutting force of LCT tools has decreased by up to 26.7%, and the cutting temperature has decreased by a maximum of 32.5%. The research mechanism indicates that at lower cutting speeds, WS<sub>2</sub> forms a lubricating film at the tool-chip contact interface, reducing shear strength and achieving a reduction in cutting force and cutting temperature. And the micro-textures are the main way for the LCT tool to reduce cutting force and cutting temperature at higher cutting speeds.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"178 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673445","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 : 2024-11-19DOI: 10.1016/j.apsusc.2024.161851
Anna G. Dymerska, Grzegorz Leniec, Ewa Mijowska
Oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are crucial for renewable energy technologies such as water splitting. Borophene, a two-dimensional (2D) boron material, has attracted significant interest for its unique electron deficiency and potential applications in energy conversion. However, practical studies on borophene’s electrocatalytic performance remain limited. Here, we demonstrate a strategy to enhance the bifunctional electrocatalytic activity in HER and OER of borophene by doping with zirconium compounds. The addition of Zr to boron enhances electrocatalytic properties by improving performance in both OER and HER, achieving overpotentials and Tafel slopes of 252 and 240 mV, 43 and 203 mV/dec, respectively. Additionally, conducting the measurements at 40 °C led to achieving the overall water-splitting potential of 1.541 (V vs. RHE). Stability tests over 1000 h at ± 10 mA/cm2 highlight the composite’s robustness, outperforming Pt/C in HER and matching the stability of RuO2 in OER. Ex-situ analyses: X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR), and X-ray diffraction (XRD) reveal insights into the chemical structure evolution during the electrochemical process. This study not only advances the understanding of borophene’s electrocatalytic mechanisms but also paves the way for its application in efficient and sustainable energy technologies.
氧进化反应（OER）和氢进化反应（HER）对于水分离等可再生能源技术至关重要。硼吩是一种二维（2D）硼材料，因其独特的电子缺陷和在能源转换中的潜在应用而备受关注。然而，有关硼吩电催化性能的实际研究仍然有限。在这里，我们展示了一种通过掺杂锆化合物来增强硼吩在 HER 和 OER 中的双功能电催化活性的策略。在硼中添加锆可提高 OER 和 HER 的性能，从而增强电催化特性，使过电位和 Tafel 斜率分别达到 252 和 240 mV、43 和 203 mV/dec。此外，在 40 °C 温度下进行测量可使整体水分离电位达到 1.541（V vs. RHE）。在 ± 10 mA/cm2 条件下进行 1000 小时的稳定性测试凸显了该复合材料的稳定性，在 HER 中优于 Pt/C，在 OER 中与 RuO2 的稳定性相当。原位分析：X 射线光电子能谱 (XPS)、电子顺磁共振 (EPR) 和 X 射线衍射 (XRD) 揭示了电化学过程中的化学结构演变。这项研究不仅加深了人们对硼吩电催化机理的理解，还为其在高效和可持续能源技术中的应用铺平了道路。
{"title":"Electrocatalytic water splitting by bifunctional Zircon-doped borophene","authors":"Anna G. Dymerska, Grzegorz Leniec, Ewa Mijowska","doi":"10.1016/j.apsusc.2024.161851","DOIUrl":"https://doi.org/10.1016/j.apsusc.2024.161851","url":null,"abstract":"Oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are crucial for renewable energy technologies such as water splitting. Borophene, a two-dimensional (2D) boron material, has attracted significant interest for its unique electron deficiency and potential applications in energy conversion. However, practical studies on borophene’s electrocatalytic performance remain limited. Here, we demonstrate a strategy to enhance the bifunctional electrocatalytic activity in HER and OER of borophene by doping with zirconium compounds. The addition of Zr to boron enhances electrocatalytic properties by improving performance in both OER and HER, achieving overpotentials and Tafel slopes of 252 and 240 mV, 43 and 203 mV/dec, respectively. Additionally, conducting the measurements at 40 °C led to achieving the overall water-splitting potential of 1.541 (V vs. RHE). Stability tests over 1000 h at ± 10 mA/cm2 highlight the composite’s robustness, outperforming Pt/C in HER and matching the stability of RuO<sub>2</sub> in OER. Ex-situ analyses: X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR), and X-ray diffraction (XRD) reveal insights into the chemical structure evolution during the electrochemical process. This study not only advances the understanding of borophene’s electrocatalytic mechanisms but also paves the way for its application in efficient and sustainable energy technologies.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"99 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670867","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：