Pub Date : 2025-02-13DOI: 10.1016/j.apsusc.2025.162684
Hossein Nourmohamadi , Sanaz Keyvan
Activated carbon is characterized by its high surface area, porosity, and ability to adsorb a wide range of organic and inorganic substances, making it an effective material for various applications. In the present study, molecular simulations, experimental tests, and instrumental analyses (such as atomic absorption and Raman spectroscopy) were employed to investigate the adsorption of (copper, manganese, and zinc) diperrhenate complexes by activated carbon. The results demonstrated that activated carbon interacts well with each of the target complexes and can effectively enhance the concentration of rhenium compounds. However, the surface affinity for the manganese diperrhenate complex was higher than that of the other two complexes. The d orbitals of the metal atom and the p orbitals of the nitrogen atom in the complexes provide conditions for electron exchange with the p orbitals of the surface atoms. As a result, strong electrostatic bonds are formed between the adsorbent and the adsorbate.
活性炭的特点是比表面积大、孔隙率高，能够吸附多种有机和无机物质，因此是一种可用于多种用途的有效材料。本研究采用分子模拟、实验测试和仪器分析（如原子吸收和拉曼光谱）来研究活性炭对（铜、锰和锌）二errhenate 复合物的吸附。结果表明，活性炭与每种目标络合物都有良好的相互作用，能有效提高铼化合物的浓度。但二errhenate 锰络合物的表面亲和力高于其他两种络合物。络合物中金属原子的 d 轨道和氮原子的 p 轨道为与表面原子的 p 轨道进行电子交换提供了条件。因此，吸附剂和吸附物之间形成了很强的静电键。
{"title":"Adsorption mechanisms of Cu, Mn, and Zn diperrhenate complexes on activated carbon: Molecular simulations and experimental insights","authors":"Hossein Nourmohamadi , Sanaz Keyvan","doi":"10.1016/j.apsusc.2025.162684","DOIUrl":"10.1016/j.apsusc.2025.162684","url":null,"abstract":"<div><div>Activated carbon is characterized by its high surface area, porosity, and ability to adsorb a wide range of organic and inorganic substances, making it an effective material for various applications. In the present study, molecular simulations, experimental tests, and instrumental analyses (such as atomic absorption and Raman spectroscopy) were employed to investigate the adsorption of (copper, manganese, and zinc) diperrhenate complexes by activated carbon. The results demonstrated that activated carbon interacts well with each of the target complexes and can effectively enhance the concentration of rhenium compounds. However, the surface affinity for the manganese diperrhenate complex was higher than that of the other two complexes. The d orbitals of the metal atom and the p orbitals of the nitrogen atom in the complexes provide conditions for electron exchange with the p orbitals of the surface atoms. As a result, strong electrostatic bonds are formed between the adsorbent and the adsorbate.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162684"},"PeriodicalIF":6.3,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417676","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 : 2025-02-13DOI: 10.1016/j.apsusc.2025.162625
Yong Han , Shen Chen , Marek Kolmer , Lin-Lin Wang , James W. Evans , Michael C. Tringides
Electronic properties of two-dimensional (2D) materials are strongly influenced by their atomic arrangements, making the theoretically-aided characterization of experimentally-synthesized 2D structures crucial. Using first-principles density functional theory, we analyze nearly 200 configurations of intercalated Gd layers beneath buffer-layer graphene on SiC(0001) over a Gd coverage range of . By fully relaxing selectively-constructed configurations at each coverage within a large, low-strain supercell, we determine the coverage dependence of the chemical potential for intercalated Gd structures. Thermodynamically-preferred configurations below form single-atom-thick monolayers, while 3D-like or multilayer structures emerge beyond . Most structures are amorphous-like, including the configuration at the chemical potential minimum around . In contrast, a strongly stretched Gd(0001)-like monolayer at and a nearly perfect Gd(0001) monolayer at are significantly less favorable with 0.16 eV and 0.82 eV higher chemical potentials above the minimum, respectively. Furthermore, the graphene layer decoupled by intercalated Gd near the chemical potential minimum is significantly flatter compared to its morphology above intercalated 3D structures at higher coverages and nearly isolated Gd atoms in the lowest coverage region. These findings align with our experimental results and underscore the need for further research on this unique intercalated system, which holds significant potential for diverse applications.
{"title":"Coverage-dependent structures and thermodynamic stability of intercalated Gd layers beneath buffer-layer graphene on SiC(0001)","authors":"Yong Han , Shen Chen , Marek Kolmer , Lin-Lin Wang , James W. Evans , Michael C. Tringides","doi":"10.1016/j.apsusc.2025.162625","DOIUrl":"10.1016/j.apsusc.2025.162625","url":null,"abstract":"<div><div>Electronic properties of two-dimensional (2D) materials are strongly influenced by their atomic arrangements, making the theoretically-aided characterization of experimentally-synthesized 2D structures crucial. Using first-principles density functional theory, we analyze nearly 200 configurations of intercalated Gd layers beneath buffer-layer graphene on SiC(0001) over a Gd coverage range of <span><math><mrow><mn>0.01</mn><mo><</mo><mi>θ</mi><mo><</mo><mn>1.2</mn></mrow></math></span>. By fully relaxing selectively-constructed configurations at each coverage within a large, low-strain supercell, we determine the coverage dependence of the chemical potential for intercalated Gd structures. Thermodynamically-preferred configurations below <span><math><mrow><mi>θ</mi><mo>≈</mo><mn>0.8</mn></mrow></math></span> form single-atom-thick monolayers, while 3D-like or multilayer structures emerge beyond <span><math><mrow><mi>θ</mi><mo>≈</mo><mn>0.9</mn></mrow></math></span>. Most structures are amorphous-like, including the configuration at the chemical potential minimum around <span><math><mrow><mi>θ</mi><mo>≈</mo><mn>0.4</mn></mrow></math></span>. In contrast, a strongly stretched Gd(0001)-like monolayer at <span><math><mrow><mi>θ</mi><mo>=</mo><mn>1</mn><mo>/</mo><mn>3</mn></mrow></math></span> and a nearly perfect Gd(0001) monolayer at <span><math><mrow><mi>θ</mi><mo>=</mo><mn>1</mn></mrow></math></span> are significantly less favorable with 0.16 eV and 0.82 eV higher chemical potentials above the minimum, respectively. Furthermore, the graphene layer decoupled by intercalated Gd near the chemical potential minimum is significantly flatter compared to its morphology above intercalated 3D structures at higher coverages and nearly isolated Gd atoms in the lowest coverage region. These findings align with our experimental results and underscore the need for further research on this unique intercalated system, which holds significant potential for diverse applications.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162625"},"PeriodicalIF":6.3,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143395110","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 : 2025-02-13DOI: 10.1016/j.apsusc.2025.162682
Yanjun Liu , Lin Hao , Hanshuo Ma , Ming Su , Yufan Zhang
In this study, zeolite imidazolate framework (ZIF-67) was used as a cobalt source, and Co3O4 hollow cubes were obtained after air carbonization. Nickel-iron layered double hydroxides (NiFe-LDH) were subsequently synthesized on the Co3O4 hollow cubes using an oil bath method to produce the final material for nitrobenzene (NB) detection. The hollow-cube structure not only provides more active sites and increases surface area but also offers numerous channels for ion and electron transfer, thereby enhancing charge transfer and improving sensing performance. The incorporation of NiFe-LDH further amplifies the synergistic catalytic effect between the transition metals, with each metal playing a distinct role in achieving a coordinated catalytic effect. Under optimized conditions, the composite exhibits a wide linear range (1.5–1765.5 μM) and the limit of detection of 0.162 μM. Additionally, it demonstrates anti-interference, stability, and reproducibility, offering an effective method for trace detection of NB in environmental samples.
{"title":"Convenient preparation of Ni-Fe layered double hydroxide nanosheets on Co3O4 hollow cube for Monitoring the environmental pollutant Nitrobenzene","authors":"Yanjun Liu , Lin Hao , Hanshuo Ma , Ming Su , Yufan Zhang","doi":"10.1016/j.apsusc.2025.162682","DOIUrl":"10.1016/j.apsusc.2025.162682","url":null,"abstract":"<div><div>In this study, zeolite imidazolate framework (ZIF-67) was used as a cobalt source, and Co<sub>3</sub>O<sub>4</sub> hollow cubes were obtained after air carbonization. Nickel-iron layered double hydroxides (NiFe-LDH) were subsequently synthesized on the Co<sub>3</sub>O<sub>4</sub> hollow cubes using an oil bath method to produce the final material for nitrobenzene (NB) detection. The hollow-cube structure not only provides more active sites and increases surface area but also offers numerous channels for ion and electron transfer, thereby enhancing charge transfer and improving sensing performance. The incorporation of NiFe-LDH further amplifies the synergistic catalytic effect between the transition metals, with each metal playing a distinct role in achieving a coordinated catalytic effect. Under optimized conditions, the composite exhibits a wide linear range (1.5–1765.5 μM) and the limit of detection of 0.162 μM. Additionally, it demonstrates anti-interference, stability, and reproducibility, offering an effective method for trace detection of NB in environmental samples.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162682"},"PeriodicalIF":6.3,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417325","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 : 2025-02-13DOI: 10.1016/j.apsusc.2025.162689
Jai Bhagwan, Jeong In Han
A simple synthesis process for hybrid transition metal oxides is a crucial way for their application in energy storage system. In this work, multi-walled carbon nanotubes (MWCNTs) decorated CdO/Co3O4 hexagonal like nanoplates are prepared by fast emerging co-precipitation process. Further, CdO/Co3O4/MWCNT composite is used for energy storage performance and, specific capacity of 214.5 mAh g−1 is obtained at 1 A g−1. The capacity of CdO/Co3O4/MWCNT is found to be higher from the capacities of CdO (40.25 mAh g−1), Co3O4 (100.5 mAh g−1) and CdO/Co3O4 (171.63 mAh g−1). Further, hybrid supercapacitor (HSC) is designed by CdO/Co3O4/MWCNT (positive electrode) and activated carbon (AC) (negative electrode). The CdO/Co3O4/MWCNT//AC delivers the high energy density of 37 W h kg−1 with the power density of 750 W kg−1. In addition, to confirm the electronic applicability for portable appliances, four green color light-emitting diodes (LEDs), kitchen timer and toy motor fan are operated separately by two CdO/Co3O4/MWCNT//AC hybrid supercapacitor connected in series.
{"title":"Multi-walled carbon nanotubes decorated CdO/Co3O4 hexagonal nanoplates: Unveiling their potential in hybrid supercapacitor","authors":"Jai Bhagwan, Jeong In Han","doi":"10.1016/j.apsusc.2025.162689","DOIUrl":"10.1016/j.apsusc.2025.162689","url":null,"abstract":"<div><div>A simple synthesis process for hybrid transition metal oxides is a crucial way for their application in energy storage system. In this work, multi-walled carbon nanotubes (MWCNTs) decorated CdO/Co<sub>3</sub>O<sub>4</sub> hexagonal like nanoplates are prepared by fast emerging co-precipitation process. Further, CdO/Co<sub>3</sub>O<sub>4</sub>/MWCNT composite is used for energy storage performance and, specific capacity of 214.5 mAh g<sup>−1</sup> is obtained at 1 A g<sup>−1</sup>. The capacity of CdO/Co<sub>3</sub>O<sub>4</sub>/MWCNT is found to be higher from the capacities of CdO (40.25 mAh g<sup>−1</sup>), Co<sub>3</sub>O<sub>4</sub> (100.5 mAh g<sup>−1</sup>) and CdO/Co<sub>3</sub>O<sub>4</sub> (171.63 mAh g<sup>−1</sup>). Further, hybrid supercapacitor (HSC) is designed by CdO/Co<sub>3</sub>O<sub>4</sub>/MWCNT (positive electrode) and activated carbon (AC) (negative electrode). The CdO/Co<sub>3</sub>O<sub>4</sub>/MWCNT//AC delivers the high energy density of 37 W h kg<sup>−1</sup> with the power density of 750 W kg<sup>−1</sup>. In addition, to confirm the electronic applicability for portable appliances, four green color light-emitting diodes (LEDs), kitchen timer and toy motor fan are operated separately by two CdO/Co<sub>3</sub>O<sub>4</sub>/MWCNT//AC hybrid supercapacitor connected in series.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162689"},"PeriodicalIF":6.3,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417326","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162676
Reneesha Valiyaveettil Basheer , Nurhaslina Abd Rahman , So Yeon Yoon , Choe Earn Choong , Jun Sup Lim , Eun Ha Choi , Yeomin Yoon , Min Jang
The rising demand for hydrogen peroxide (H2O2) has driven interest in electrocatalytic ORR due to the environmental impact of the anthraquinone process. Ar jet plasma treatment on trimethoxyphenylsilane (TMPS)-coated carbon felt (CF) led to varying polymerized TMPS (P-TMPS) formations. An optimized 15-min Ar jet plasma-treated TMPS-loaded CF (CF-S10-P15) electrode consistently produced H2O2 at ∼1.8 % over 5 hrs across five cycles. Solid-state attenuated total reflectance (ATR)-Fourier transform infrared spectroscopy (FTIR), carbon-13 and hydrogen-1 (13C/1H) nuclear magnetic resonance spectroscopy (NMR), temperature-programmed desorption (TPD) of ammonia, X-ray photoelectron spectroscopy (XPS), and in situ Raman analyses indicated that the isolated silanol (Si-OH) functional group was crucial for the ORR, significantly enhancing H2O2 yield. ATR-FTIR confirmed Si-OH sites as Lewis acid sites, while XPS showed a linear correlation of Si3+/Sitotal and Oads/Ototal ratios with H2O2 production. 13C/1H NMR revealed plasma treatment time influences TMPS polymerization, with mature Si–OH polymerization at 15 min. In situ Raman analysis indicated Si–O electron transfer, facilitating •OOH reduction to H2O2 under potential. Time-lapse ATR-FTIR captured •OOH and •O2– intermediates on CF-S10-P15 during ORR, elucidating the H2O2 generation mechanism. Optimizing P-TMPS on CF via Ar jet plasma yielded a cost-effective electrode for efficient H2O2 production.
{"title":"Enhanced electrocatalytic H2O2 production using Ar jet plasma-polymerized trimethoxyphenylsilane forming Lewis acid sites","authors":"Reneesha Valiyaveettil Basheer , Nurhaslina Abd Rahman , So Yeon Yoon , Choe Earn Choong , Jun Sup Lim , Eun Ha Choi , Yeomin Yoon , Min Jang","doi":"10.1016/j.apsusc.2025.162676","DOIUrl":"10.1016/j.apsusc.2025.162676","url":null,"abstract":"<div><div>The rising demand for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) has driven interest in electrocatalytic ORR due to the environmental impact of the anthraquinone process. Ar jet plasma treatment on trimethoxyphenylsilane (TMPS)-coated carbon felt (CF) led to varying polymerized TMPS (P-TMPS) formations. An optimized 15-min Ar jet plasma-treated TMPS-loaded CF (CF-S<sub>10</sub>-P<sub>15</sub>) electrode consistently produced H<sub>2</sub>O<sub>2</sub> at ∼1.8 % over 5 hrs across five cycles. Solid-state attenuated total reflectance (ATR)-Fourier transform infrared spectroscopy (FTIR), carbon-13 and hydrogen-1 (<sup>13</sup>C/<sup>1</sup>H) nuclear magnetic resonance spectroscopy (NMR), temperature-programmed desorption (TPD) of ammonia, X-ray photoelectron spectroscopy (XPS), and <em>in situ</em> Raman analyses indicated that the isolated silanol (Si-OH) functional group was crucial for the ORR, significantly enhancing H<sub>2</sub>O<sub>2</sub> yield. ATR-FTIR confirmed Si-OH sites as Lewis acid sites, while XPS showed a linear correlation of Si<sup>3+</sup>/Si<sub>total</sub> and O<sub>ads</sub>/O<sub>total</sub> ratios with H<sub>2</sub>O<sub>2</sub> production. <sup>13</sup>C/<sup>1</sup>H NMR revealed plasma treatment time influences TMPS polymerization, with mature Si–OH polymerization at 15 min. <em>In situ</em> Raman analysis indicated Si–O electron transfer, facilitating •OOH reduction to H<sub>2</sub>O<sub>2</sub> under potential. Time-lapse ATR-FTIR captured •OOH and •O<sub>2</sub><sup>–</sup> intermediates on CF-S<sub>10</sub>-P<sub>15</sub> during ORR, elucidating the H<sub>2</sub>O<sub>2</sub> generation mechanism. Optimizing P-TMPS on CF via Ar jet plasma yielded a cost-effective electrode for efficient H<sub>2</sub>O<sub>2</sub> production.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162676"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401785","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162671
Ting Xu , Chi Fei , Houqi Zhou , Yilong Fan , Keying Tang , Chunyu Chen , Dianchun Ju , Zuoqiao Zhu , Rui Mao
In this work, a layered double hydroxide with three-dimensional structure (3D-MgAl-LDH) was synthesized by the template-assisted method, the growth mechanism of the three-dimensional structure was investigated through a structure-modulation process, and the adsorption properties were tested. Adsorption experiments revealed that, compared to the conventional 2D inorganic LDHs, the 3D organic LDHs intercalated with SDS exhibited superior adsorption performance for dyes under all conditions. Specifically, the maximum removal capacity of MO reached 1282.5 mg·L-1, which was almost six times higher than 2D inorganic LDHs, this enhancement was attributed to the pore space formed by the aggregation of 2D lamellae, which provided additional adsorption sites. Adsorption kinetics and isotherm modeling indicated that the removal behavior closely followed the Tempkin isotherm model, and the adsorption process was better described by the Elovich kinetic model. Analysis using XPS and FT-IR indicated that anion exchange was the primary mechanism driving the removal of MO. The interaction energy between 3D-MgAl-LDH and MO was calculated by using density functional theory (DFT), which further confirmed the adsorption mechanism. Moreover, 3D-MgAl-LDH maintained stable adsorption performance after five cycling experiments. This work introduces a novel structural material for industrial wastewater treatment and broadens the dimensional options for LDHs.
{"title":"The formation and adsorption mechanism studies of three-dimensional (3D flower-like) layered double hydroxide","authors":"Ting Xu , Chi Fei , Houqi Zhou , Yilong Fan , Keying Tang , Chunyu Chen , Dianchun Ju , Zuoqiao Zhu , Rui Mao","doi":"10.1016/j.apsusc.2025.162671","DOIUrl":"10.1016/j.apsusc.2025.162671","url":null,"abstract":"<div><div>In this work, a layered double hydroxide with three-dimensional structure (3D-MgAl-LDH) was synthesized by the template-assisted method, the growth mechanism of the three-dimensional structure was investigated through a structure-modulation process, and the adsorption properties were tested. Adsorption experiments revealed that, compared to the conventional 2D inorganic LDHs, the 3D organic LDHs intercalated with SDS exhibited superior adsorption performance for dyes under all conditions. Specifically, the maximum removal capacity of MO reached 1282.5 mg·L<sup>-1</sup>, which was almost six times higher than 2D inorganic LDHs, this enhancement was attributed to the pore space formed by the aggregation of 2D lamellae, which provided additional adsorption sites. Adsorption kinetics and isotherm modeling indicated that the removal behavior closely followed the Tempkin isotherm model, and the adsorption process was better described by the Elovich kinetic model. Analysis using XPS and FT-IR indicated that anion exchange was the primary mechanism driving the removal of MO. The interaction energy between 3D-MgAl-LDH and MO was calculated by using density functional theory (DFT), which further confirmed the adsorption mechanism. Moreover, 3D-MgAl-LDH maintained stable adsorption performance after five cycling experiments. This work introduces a novel structural material for industrial wastewater treatment and broadens the dimensional options for LDHs.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162671"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393463","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162683
Bo Dang , Xiang-Le Meng , Dong Chen , Kai Yang , Tian Tian , Dong-Bo Wei , Ping-Ze Zhang
Cr-based coatings show great potential for serving as accident tolerant fuel (ATF) claddings in pressurized water reactors (PWRs). In this paper, CrxN coatings were produced on Zr-4 alloy by double glow plasma alloying technology at different Ar/N2 ratios (7:3, 5:5, and 3:7). The CrxN coatings consist of CrN and Cr2N phases and without the formation of (Zr, Cr) phase. The hardness (H) and elastic modulus (E) increase with the rise of nitrogen flow rate, which is consistent with the nitride content on the surface. Under the 3:7 Ar/N2 ratio, the highest H/E and H3/E2 values indicate the CrxN coating has great toughness and load bearing capacity, the critical load of the coating in scratch test is 26.2 N. The coating has a low volumetric wear rate, which indicates excellent resistance to fretting wear, the main wear mechanisms of coated Zr-4 alloy were observed to be abrasive wear, adhesive wear and oxidation wear. The tribocorrosion test results show that the coating (Ar/N2 ratio = 3:7) has the best resistance to the synergistic effects of wear and corrosion. In addition, a deep understanding of this paper can provide a new method for the service of ATF coatings on Zr alloy cladding.
{"title":"Mechanical, fretting wear and tribocorrosion properties of CrxN coatings on Zr-4 alloy prepared by double glow plasma alloying technology","authors":"Bo Dang , Xiang-Le Meng , Dong Chen , Kai Yang , Tian Tian , Dong-Bo Wei , Ping-Ze Zhang","doi":"10.1016/j.apsusc.2025.162683","DOIUrl":"10.1016/j.apsusc.2025.162683","url":null,"abstract":"<div><div>Cr-based coatings show great potential for serving as accident tolerant fuel (ATF) claddings in pressurized water reactors (PWRs). In this paper, Cr<sub>x</sub>N coatings were produced on Zr-4 alloy by double glow plasma alloying technology at different Ar/N<sub>2</sub> ratios (7:3, 5:5, and 3:7). The Cr<sub>x</sub>N coatings consist of CrN and Cr<sub>2</sub>N phases and without the formation of (Zr, Cr) phase. The hardness (H) and elastic modulus (E) increase with the rise of nitrogen flow rate, which is consistent with the nitride content on the surface. Under the 3:7 Ar/N<sub>2</sub> ratio, the highest H/E and H<sup>3</sup>/E<sup>2</sup> values indicate the Cr<sub>x</sub>N coating has great toughness and load bearing capacity, the critical load of the coating in scratch test is 26.2 N. The coating has a low volumetric wear rate, which indicates excellent resistance to fretting wear, the main wear mechanisms of coated Zr-4 alloy were observed to be abrasive wear, adhesive wear and oxidation wear. The tribocorrosion test results show that the coating (Ar/N<sub>2</sub> ratio = 3:7) has the best resistance to the synergistic effects of wear and corrosion. In addition, a deep understanding of this paper can provide a new method for the service of ATF coatings on Zr alloy cladding.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"692 ","pages":"Article 162683"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401788","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162678
Mohammed Abdillah Ahmad Farid , Jacqueline Lease , Yoshito Andou
The objective of this study was to elucidate the sulfonation behaviour of graphene oxide (GO) across a temperature range of 50 °C, 100 °C, and 150 °C under a nitrogen atmosphere. Analysis revealed a significant reduction in –OH, C-O, and O-C-O functional groups, facilitating a substantial conversion from sp3 to sp2 carbon hybridization. Specifically, the sp2 carbon content increased from 37.43 ± 2.0 % in GO to 50.32 ± 2.5 % in GO-SO3H50, 43.72 ± 3.0 % in GO-SO3H100, and 47.92 ± 2.8 % in GO-SO3H150. At higher temperatures, deoxygenation led to a decrease in C-S density due to the pronounced removal of oxygen moieties, which constrained the availability of functional groups for −SO3H binding. SEM imaging corroborated that sulfonated GO retained its disordered stacked layer configuration, consistent with the precursor. These results affirm that sulfonation is a viable alternative for synthesizing reduced graphene oxide (rGO), with enhanced sp2 carbon content and modified structural characteristics.
{"title":"Temperature-dependent deoxygenation during sulfonation for graphene oxide reduction","authors":"Mohammed Abdillah Ahmad Farid , Jacqueline Lease , Yoshito Andou","doi":"10.1016/j.apsusc.2025.162678","DOIUrl":"10.1016/j.apsusc.2025.162678","url":null,"abstract":"<div><div>The objective of this study was to elucidate the sulfonation behaviour of graphene oxide (GO) across a temperature range of 50 °C, 100 °C, and 150 °C under a nitrogen atmosphere. Analysis revealed a significant reduction in –OH, C-O, and O-C-O functional groups, facilitating a substantial conversion from sp<sup>3</sup> to sp<sup>2</sup> carbon hybridization. Specifically, the sp<sup>2</sup> carbon content increased from 37.43 ± 2.0 % in GO to 50.32 ± 2.5 % in GO-SO<sub>3</sub>H50, 43.72 ± 3.0 % in GO-SO<sub>3</sub>H100, and 47.92 ± 2.8 % in GO-SO<sub>3</sub>H150. At higher temperatures, deoxygenation led to a decrease in C-S density due to the pronounced removal of oxygen moieties, which constrained the availability of functional groups for −SO<sub>3</sub>H binding. SEM imaging corroborated that sulfonated GO retained its disordered stacked layer configuration, consistent with the precursor. These results affirm that sulfonation is a viable alternative for synthesizing reduced graphene oxide (rGO), with enhanced sp<sup>2</sup> carbon content and modified structural characteristics.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162678"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401786","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162670
Cong Wang , Jian Li , Xin Wang , Min Zhang
With fossil fuel reserves diminishing, designing and synthesizing electrocatalysts with controllable active sites is essential for converting carbon dioxide (CO2) into valuable chemicals. Inspired by the experimental advancement of two-dimensional π-conjugated metal–organic framework (2D c-MOF) nanosheets, we have performed a computational screening to identify optimal single-atom catalysts for the CO2 reduction reaction (CO2RR) across eleven 2D c-MOFs (HTHATN-TM). These frameworks comprise transition metals (TM = Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Rh, Pd, or Ag) and hexathiohexaazatrinaphthylene (HTHATN) organic ligands. Our first-principles calculations reveal that HTHATN-Cr and HTHATN-Ru emerge as highly promising CO2RR catalysts, exhibiting low limiting potentials of −0.38 V and −0.53 V, respectively, and favoring the production of HCOOH and CH4. These findings provide valuable insights for the development of more efficient CO2RR catalysts.
{"title":"Two-dimensional π-conjugated metal–organic frameworks as highly efficient catalysts for CO2 electroreduction","authors":"Cong Wang , Jian Li , Xin Wang , Min Zhang","doi":"10.1016/j.apsusc.2025.162670","DOIUrl":"10.1016/j.apsusc.2025.162670","url":null,"abstract":"<div><div>With fossil fuel reserves diminishing, designing and synthesizing electrocatalysts with controllable active sites is essential for converting carbon dioxide (CO<sub>2</sub>) into valuable chemicals. Inspired by the experimental advancement of two-dimensional π-conjugated metal–organic framework (2D <em>c</em>-MOF) nanosheets, we have performed a computational screening to identify optimal single-atom catalysts for the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) across eleven 2D <em>c</em>-MOFs (HTHATN-TM). These frameworks comprise transition metals (TM = Cr, Mn, Fe, Co, Ni, Cu, Zn, Ru, Rh, Pd, or Ag) and hexathiohexaazatrinaphthylene (HTHATN) organic ligands. Our first-principles calculations reveal that HTHATN-Cr and HTHATN-Ru emerge as highly promising CO<sub>2</sub>RR catalysts, exhibiting low limiting potentials of −0.38 V and −0.53 V, respectively, and favoring the production of HCOOH and CH<sub>4</sub>. These findings provide valuable insights for the development of more efficient CO<sub>2</sub>RR catalysts.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162670"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401932","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 : 2025-02-12DOI: 10.1016/j.apsusc.2025.162673
Yingnan Ma , Na Liu , Yulu Zhang , Zhen Xu , Yang Yang , Dongliang Jin , Mengqi Qu , Miaomiao Su , Kang Zhang , Panliang Zhang
Thin film composite (TFC) membranes are pivotal in gas separation technologies, particularly for CO2 capture and separation. The gutter layer can promote the ultra-thin structure of top layer thus achieving high gas permeance. MOFs are considered to be the promising gutter layer materials while suffer from poor deformability, thereby easy to produce defects during bending, which significantly reduce the separation performance. In this work, 2-D CuBDC nanosheets were utilized as the gutter layer, the nanosheets linked with porous support and each other with hydrogen bonds. Benefitting from the outstanding inner mechanical strength and the additional separation performance of the 2-D MOFs nanosheets gutter layer, the obtained TFC membranes with ultra-thin Pebax top layer exhibited outstanding deformation resistance capability which could maintain the similar CO2 separation performance after bending deformation of 65 %. As a result, the CO2 permeance reached 1267 GPU, the CO2/N2 selectivity was maintained at 39.2 and the CO2/CH4 selectivity reached 23.6. The obtained TFC membranes exhibited excellent CO2 separation performance which surpassed the Robeson upper bound 2008. We believe that such a Pebax TFC membrane design based on CuBDC nanosheets gutter layers is a promising approach for high-performance CO2 separation membranes.
{"title":"Flexible thin film composite membranes based on deformable metal organic frameworks gutter layer for efficient CO2 separation","authors":"Yingnan Ma , Na Liu , Yulu Zhang , Zhen Xu , Yang Yang , Dongliang Jin , Mengqi Qu , Miaomiao Su , Kang Zhang , Panliang Zhang","doi":"10.1016/j.apsusc.2025.162673","DOIUrl":"10.1016/j.apsusc.2025.162673","url":null,"abstract":"<div><div>Thin film composite (TFC) membranes are pivotal in gas separation technologies, particularly for CO<sub>2</sub> capture and separation. The gutter layer can promote the ultra-thin structure of top layer thus achieving high gas permeance. MOFs are considered to be the promising gutter layer materials while suffer from poor deformability, thereby easy to produce defects during bending, which significantly reduce the separation performance. In this work, 2-D CuBDC nanosheets were utilized as the gutter layer, the nanosheets linked with porous support and each other with hydrogen bonds. Benefitting from the outstanding inner mechanical strength and the additional separation performance of the 2-D MOFs nanosheets gutter layer, the obtained TFC membranes with ultra-thin Pebax top layer exhibited outstanding deformation resistance capability which could maintain the similar CO<sub>2</sub> separation performance after bending deformation of 65 %. As a result, the CO<sub>2</sub> permeance reached 1267 GPU, the CO<sub>2</sub>/N<sub>2</sub> selectivity was maintained at 39.2 and the CO<sub>2</sub>/CH<sub>4</sub> selectivity reached 23.6. The obtained TFC membranes exhibited excellent CO<sub>2</sub> separation performance which surpassed the Robeson upper bound 2008. We believe that such a Pebax TFC membrane design based on CuBDC nanosheets gutter layers is a promising approach for high-performance CO<sub>2</sub> separation membranes.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"691 ","pages":"Article 162673"},"PeriodicalIF":6.3,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401787","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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