Understanding the formation and evolution of arrays of metallic nanoparticles is a very important task as they are increasingly used in various devices. In this work, we used HRTEM mode for continuous in-situ observations of the evolution of Ag and Au nanoparticle arrays with an average size of ∼4 nm, formed on the surface of amorphous carbon by vacuum-thermal evaporation, under the influence of a microscope electron beam without any other energetic influence. Our studies show that electron beam exposure induces a process of nanoparticle coalescence for Au and simultaneous coalescence and vaporization for Ag. As a result, the evolution of Ag and Au nanoparticle arrays has different mechanisms. In the case of Ag, the aggregation of nanoparticles occurs through the gas phase by the Ostwald ripening mechanism. In the case of Au, it was found that the aggregation of nanoparticles depends on their mutual crystalline orientation, resulting in the realization of mechanisms through bridge formation or through jumping. The influence of the crystalline orientation of the nanoparticles on the coalescence mechanism was confirmed by molecular dynamics simulations. MD simulations revealed that it is most favorable for coalescence if the densely packed planes of neighboring nanoparticles have a perpendicular arrangement in space.
{"title":"Mechanisms of Au and Ag nanoparticle array evolution studied by in-situ TEM and molecular dynamics simulation","authors":"Yu.Ya. Gafner , D.G. Gromov , R.L. Volkov , S.V. Dubkov , D.А. Ryzhkova , S.L. Gafner , A.A. Cherepovskaya , D.V. Novikov , T.S. Grishin , N.I. Borgardt","doi":"10.1016/j.surfin.2024.105165","DOIUrl":"10.1016/j.surfin.2024.105165","url":null,"abstract":"<div><div>Understanding the formation and evolution of arrays of metallic nanoparticles is a very important task as they are increasingly used in various devices. In this work, we used HRTEM mode for continuous in-situ observations of the evolution of Ag and Au nanoparticle arrays with an average size of ∼4 nm, formed on the surface of amorphous carbon by vacuum-thermal evaporation, under the influence of a microscope electron beam without any other energetic influence. Our studies show that electron beam exposure induces a process of nanoparticle coalescence for Au and simultaneous coalescence and vaporization for Ag. As a result, the evolution of Ag and Au nanoparticle arrays has different mechanisms. In the case of Ag, the aggregation of nanoparticles occurs through the gas phase by the Ostwald ripening mechanism. In the case of Au, it was found that the aggregation of nanoparticles depends on their mutual crystalline orientation, resulting in the realization of mechanisms through bridge formation or through jumping. The influence of the crystalline orientation of the nanoparticles on the coalescence mechanism was confirmed by molecular dynamics simulations. MD simulations revealed that it is most favorable for coalescence if the densely packed planes of neighboring nanoparticles have a perpendicular arrangement in space.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424712","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 : 2024-10-01DOI: 10.1016/j.surfin.2024.105182
Shah Zeb , Saira Naz , Zaheen Ullah Khan , Waheed Ullah Khan , Muhammad Imran , Ahmed Uddin , Riming Hu , Muhammad Umair , Xuchuan Jiang , Yongxiang Gao
Gas sensors can achieve remarkable functionality through the optimization of particle size, shapes, crystal facets, and oxygen defects, resulting in unsaturated coordination atoms, high charge densities, and enhanced bond energies. In this study, WO2.72 nanourchins, WO3-x nanowires, and WO3 nanorods/nanocube with (010), (001), (200), and (002) dominant crystal facets were synthesized and used as gas sensing materials. It was found that WO2.72 nanourchins exhibit an excellent response of Ra/Rg=21 to 100 ppm acetone with good selectivity among other sensors as-fabricated. First-principle calculations of Density Functional Theory were performed on acetone's adsorption on different crystal planes of tungsten oxide. The results verify spontaneous and fast adsorption on the (010) crystal plane than on the (001) and (200) planes. Further characterizations indicate that WO2.72 nanourchins with (010) crystal facets contain more reactive sites with high surface energy, facilitating charge separation, increasing charge carrier mobility, and enabling the redox reactions to occur independently at different rates. Moreover, their richer electron-donor surface oxygen defects, smaller feature sizes, and higher surface area (SBET) with hierarchical porous structures, all contribute to the enhanced acetone sensing. Our work provides a strategy for improved acetone sensing based on optimizing the particle shape with different crystal facets and oxygen vacancy density. We further expect our strategy to be applicable in designing other sensor materials with efficient charge separation and fast surface redox reactions to detect toxic gases.
{"title":"Shape controlled synthesis and crystal facet dependent gas sensitivity of tungsten oxide","authors":"Shah Zeb , Saira Naz , Zaheen Ullah Khan , Waheed Ullah Khan , Muhammad Imran , Ahmed Uddin , Riming Hu , Muhammad Umair , Xuchuan Jiang , Yongxiang Gao","doi":"10.1016/j.surfin.2024.105182","DOIUrl":"10.1016/j.surfin.2024.105182","url":null,"abstract":"<div><div>Gas sensors can achieve remarkable functionality through the optimization of particle size, shapes, crystal facets, and oxygen defects, resulting in unsaturated coordination atoms, high charge densities, and enhanced bond energies. In this study, WO<sub>2.72</sub> nanourchins, WO<sub>3-x</sub> nanowires, and WO<sub>3</sub> nanorods/nanocube with (010), (001), (200), and (002) dominant crystal facets were synthesized and used as gas sensing materials. It was found that WO<sub>2.72</sub> nanourchins exhibit an excellent response of R<sub>a</sub>/R<sub>g</sub>=21 to 100 ppm acetone with good selectivity among other sensors as-fabricated. First-principle calculations of Density Functional Theory were performed on acetone's adsorption on different crystal planes of tungsten oxide. The results verify spontaneous and fast adsorption on the (010) crystal plane than on the (001) and (200) planes. Further characterizations indicate that WO<sub>2.72</sub> nanourchins with (010) crystal facets contain more reactive sites with high surface energy, facilitating charge separation, increasing charge carrier mobility, and enabling the redox reactions to occur independently at different rates. Moreover, their richer electron-donor surface oxygen defects, smaller feature sizes, and higher surface area (S<sub>BET</sub>) with hierarchical porous structures, all contribute to the enhanced acetone sensing. Our work provides a strategy for improved acetone sensing based on optimizing the particle shape with different crystal facets and oxygen vacancy density. We further expect our strategy to be applicable in designing other sensor materials with efficient charge separation and fast surface redox reactions to detect toxic gases.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424273","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 : 2024-10-01DOI: 10.1016/j.surfin.2024.105203
Siying Liu , Huohai Yang , Xingbo Ge , Yingjie Feng , Xiaoyue Fu , Xin Chen
Carbon-based single atom catalysts (SACs) are promising electrocatalysts in the field of carbon dioxide reduction reactions (CO2RR) due to their high efficiency and environmental friendliness, in which the coordination environment is the key factor determining their intrinsic catalytic activity. Furthermore, rare-earth-based SACs have shown great potential on CO2RR in recent years. Meanwhile, various studies have focused on combining metals with N-doped graphene, which together form potential Mx-Ny-C active sites. This work systematically investigates the impact of varying N/C coordination numbers on Nd atoms in graphene (Nd-NxC6-x, x = 0–5) on the CO2RR reaction mechanism and catalytic performance through density functional theory methods. Detailed Gibbs free energy calculation results indicate that most catalysts undergo a two-electron reduction pathway. For Nd-N3C3, Nd-N3C3–1, Nd-N3C3–2, Nd-N4C2, Nd-N4C2–1, Nd-N4C2–2, and Nd-N5C, HCOOH is the main product, with low UL values of -0.18, -0.17, -0.03, -0.10, -0.11, -0.09, and -0.10 V, respectively. In summary, our research results not only indicate that N atoms with different coordination numbers can improve the product selectivity and catalytic activity of catalysts, but also may provide valuable theoretical insights for studying the application of rare-earth-based SACs.
{"title":"Rare-earth metal neodymium anchored into graphene as a promising CO2 reduction electrocatalyst by regulating the coordination environment","authors":"Siying Liu , Huohai Yang , Xingbo Ge , Yingjie Feng , Xiaoyue Fu , Xin Chen","doi":"10.1016/j.surfin.2024.105203","DOIUrl":"10.1016/j.surfin.2024.105203","url":null,"abstract":"<div><div>Carbon-based single atom catalysts (SACs) are promising electrocatalysts in the field of carbon dioxide reduction reactions (CO<sub>2</sub>RR) due to their high efficiency and environmental friendliness, in which the coordination environment is the key factor determining their intrinsic catalytic activity. Furthermore, rare-earth-based SACs have shown great potential on CO<sub>2</sub>RR in recent years. Meanwhile, various studies have focused on combining metals with N-doped graphene, which together form potential M<em><sub>x</sub></em>-N<em><sub>y</sub></em>-C active sites. This work systematically investigates the impact of varying N/C coordination numbers on Nd atoms in graphene (Nd-N<em><sub>x</sub></em>C<sub>6-</sub><em><sub>x</sub>, x</em> = 0–5) on the CO<sub>2</sub>RR reaction mechanism and catalytic performance through density functional theory methods. Detailed Gibbs free energy calculation results indicate that most catalysts undergo a two-electron reduction pathway. For Nd-N<sub>3</sub>C<sub>3</sub>, Nd-N<sub>3</sub>C<sub>3</sub>–1, Nd-N<sub>3</sub>C<sub>3</sub>–2, Nd-N<sub>4</sub>C<sub>2</sub>, Nd-N<sub>4</sub>C<sub>2</sub>–1, Nd-N<sub>4</sub>C<sub>2</sub>–2, and Nd-N<sub>5</sub>C, HCOOH is the main product, with low <em>U</em><sub>L</sub> values of -0.18, -0.17, -0.03, -0.10, -0.11, -0.09, and -0.10 V, respectively. In summary, our research results not only indicate that N atoms with different coordination numbers can improve the product selectivity and catalytic activity of catalysts, but also may provide valuable theoretical insights for studying the application of rare-earth-based SACs.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424283","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 : 2024-10-01DOI: 10.1016/j.surfin.2024.105206
Xiunan Chen , Yuhong Huang , Haiping Lin , Ruhai Du , Xiumei Wei , Fei Ma , Jing Liu
The photocatalytic CO2RR is a promising strategy for carbon neutrality, while OER is a crucial half-reaction in energy storage and conversion processes, including water splitting, CO2RR and metal-air batteries. However, developing effective and eco-friendly photocatalysts remains challengeable. In this study, Janus WSSe with monovacant Se (VSe-WSSe) is designed as a bifunctional photocatalyst. Based on the evaluation of the thermodynamic stability and *CO2 capability, the light absorption and photocatalytic performance of CO2RR and OER are systematically investigated. In the lower energy range of visible light, VSe-WSSe has better light absorption than pristine WSSe, facilitating photocatalytic efficiency. As for CO2RR, all possible reaction pathways and multiple C1 products are explored, demonstrating that the products of HCOOH, CH3OH and CH4 have UL values of -0.97 V, -1.52 V and -1.57 V, respectively. The photogenerated electrons potential of 0.69 eV at pH=0 will reduce the UL values of CH3OH and CH4 to -0.83 V and -0.88 V, respectively. Moreover, the CO2RR can greatly suppress the competitive HER. The PDS of OER occurs at the step of H2O→*OH with UL= -1.57 V. The photogenerated holes potential of 1.57 eV can make all the hydrogenation steps go downhill and result in a spontaneous reaction. This research unveils the new possibility of monovacant Janus WSSe as a bifunctional photocatalyst for CO2RR and OER, which opens the application avenue of Janus materials.
光催化 CO2RR 是实现碳中和的一项前景广阔的战略，而 OER 则是能量存储和转换过程（包括水分离、CO2RR 和金属-空气电池）中的一个关键半反应。然而，开发有效且环保的光催化剂仍是一项挑战。在本研究中，设计了含有单价硒的 Janus WSSe（VSe-WSSe）作为双功能光催化剂。在评估热力学稳定性和*CO2能力的基础上，系统研究了 CO2RR 和 OER 的光吸收和光催化性能。在可见光的较低能量范围内，VSe-WSSe 比原始 WSSe 具有更好的光吸收性能，从而提高了光催化效率。对于 CO2RR，探索了所有可能的反应途径和多种 C1 产物，结果表明 HCOOH、CH3OH 和 CH4 产物的 UL 值分别为-0.97 V、-1.52 V 和-1.57 V。在 pH=0 时，光生电子电势为 0.69 eV，这将使 CH3OH 和 CH4 的 UL 值分别降至 -0.83 V 和 -0.88 V。此外，CO2RR 还能大大抑制竞争性 HER。OER 的 PDS 发生在 H2O→*OH 步骤，UL=-1.57 V。1.57 eV 的光生空穴电位可使所有氢化步骤走下坡路，导致自发反应。这项研究揭示了单价 Janus WSSe 作为 CO2RR 和 OER 双功能光催化剂的新可能性，开辟了 Janus 材料的应用途径。
{"title":"Monovacant Janus WSSe designed as a bifunctional photocatalyst for OER and CO2RR with multiple C1 products","authors":"Xiunan Chen , Yuhong Huang , Haiping Lin , Ruhai Du , Xiumei Wei , Fei Ma , Jing Liu","doi":"10.1016/j.surfin.2024.105206","DOIUrl":"10.1016/j.surfin.2024.105206","url":null,"abstract":"<div><div>The photocatalytic CO<sub>2</sub>RR is a promising strategy for carbon neutrality, while OER is a crucial half-reaction in energy storage and conversion processes, including water splitting, CO<sub>2</sub>RR and metal-air batteries. However, developing effective and eco-friendly photocatalysts remains challengeable. In this study, Janus WSSe with monovacant Se (V<sub>Se</sub>-WSSe) is designed as a bifunctional photocatalyst. Based on the evaluation of the thermodynamic stability and *CO<sub>2</sub> capability, the light absorption and photocatalytic performance of CO<sub>2</sub>RR and OER are systematically investigated. In the lower energy range of visible light, V<sub>Se</sub>-WSSe has better light absorption than pristine WSSe, facilitating photocatalytic efficiency. As for CO<sub>2</sub>RR, all possible reaction pathways and multiple C1 products are explored, demonstrating that the products of HCOOH, CH<sub>3</sub>OH and CH<sub>4</sub> have U<sub>L</sub> values of -0.97 V, -1.52 V and -1.57 V, respectively. The photogenerated electrons potential of 0.69 eV at pH=0 will reduce the U<sub>L</sub> values of CH<sub>3</sub>OH and CH<sub>4</sub> to -0.83 V and -0.88 V, respectively. Moreover, the CO<sub>2</sub>RR can greatly suppress the competitive HER. The PDS of OER occurs at the step of H<sub>2</sub>O→*OH with U<sub>L</sub>= -1.57 V. The photogenerated holes potential of 1.57 eV can make all the hydrogenation steps go downhill and result in a spontaneous reaction. This research unveils the new possibility of monovacant Janus WSSe as a bifunctional photocatalyst for CO<sub>2</sub>RR and OER, which opens the application avenue of Janus materials.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424184","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 : 2024-09-30DOI: 10.1016/j.surfin.2024.105200
Assumpta Chinwe Nwanya , Arevik Musheghyan-Avetisyan , Enikö György , Ángel Pérez del Pino
The development of supercapacitors (SCs) by using carbon electrodes obtained from biomass waste simultaneously promotes the optimized use of the renewable energy by its high-powered storage, and the reduction of contamination in nature. Such industrial sector would be an excellent opportunity also for the developing nations, promoting their economic growth by the conversion of biowaste into added value goods. However, such carbon may not reach the desired performance for SCs. In this work, we used laser processing technology for enhancing the capacitance of SC electrodes composed of activated carbon obtained from rice husk produced in Nigerian farmlands. The activated carbon powder was synthesized by conventional carbonization-chemical activation processes and treated with microwaves. Afterwards, the CO2 laser processing of thin film electrodes composed of a mixture of the carbon powder with carbon black (conductive additive), and precursors as urea (for doping of the activated carbon with nitrogen), or manganese nitrate (for the crystallization of pseudocapacitive Mn3O4 nanoparticles on the carbon surface) was carried out for obtaining enhanced positrodes and negatrodes. The resulting hybrid electrodes exhibited a 3-fold increase of the capacitance (up to 134 F/g @ 10 mV/s) as compared to the raw carbon in the [0, 0.8] V potential window. Asymmetric SC devices integrated by carbon (-)//carbon-Mn3O4 (+) laser-treated electrodes, operating at 1.2 V voltage, revealed up to 300 × higher energy and power densities than symmetric SCs composed of raw carbon electrodes.
{"title":"Fabrication of asymmetric supercapacitors by laser processing of activated carbon-based electrodes produced from rice husk waste","authors":"Assumpta Chinwe Nwanya , Arevik Musheghyan-Avetisyan , Enikö György , Ángel Pérez del Pino","doi":"10.1016/j.surfin.2024.105200","DOIUrl":"10.1016/j.surfin.2024.105200","url":null,"abstract":"<div><div>The development of supercapacitors (SCs) by using carbon electrodes obtained from biomass waste simultaneously promotes the optimized use of the renewable energy by its high-powered storage, and the reduction of contamination in nature. Such industrial sector would be an excellent opportunity also for the developing nations, promoting their economic growth by the conversion of biowaste into added value goods. However, such carbon may not reach the desired performance for SCs. In this work, we used laser processing technology for enhancing the capacitance of SC electrodes composed of activated carbon obtained from rice husk produced in Nigerian farmlands. The activated carbon powder was synthesized by conventional carbonization-chemical activation processes and treated with microwaves. Afterwards, the CO<sub>2</sub> laser processing of thin film electrodes composed of a mixture of the carbon powder with carbon black (conductive additive), and precursors as urea (for doping of the activated carbon with nitrogen), or manganese nitrate (for the crystallization of pseudocapacitive Mn<sub>3</sub>O<sub>4</sub> nanoparticles on the carbon surface) was carried out for obtaining enhanced positrodes and negatrodes. The resulting hybrid electrodes exhibited a 3-fold increase of the capacitance (up to 134 F/g @ 10 mV/s) as compared to the raw carbon in the [0, 0.8] V potential window. Asymmetric SC devices integrated by carbon (-)//carbon-Mn<sub>3</sub>O<sub>4</sub> (+) laser-treated electrodes, operating at 1.2 V voltage, revealed up to 300 × higher energy and power densities than symmetric SCs composed of raw carbon electrodes.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The AlOOH/MoO3 binary composite electrodes are synthesized by layer-by-layer method to enhance the supercapacitive property of AlOOH by taking advantage of multiple oxidation states of molybdenum. The X-ray diffraction characterization reveals the polycrystalline nature of nanocomposite. The elements and their chemical states are analysed using X-ray photoelectron spectroscopy. The binary composite exhibits interconnected network-like morphology resembling a fractal nature. The three-electrode measurement in 1 M KOH electrolyte shows the highest specific capacity (Cs) of 1638.15 C g-1@ 5 mV s-1 for binary composite, which is greater than the capacity of individual components. Also, we get Cs of 1124.41 C g-1 for 10 cycle MoO3 while its theoretical capacity is 1005 C g-1. The excellent electrochemical performance is a consequence of multiple redox active sites present in the nanocomposite, lower resistance, porous interconnected network-like structure, and shorter relaxation time. The synergy of AlOOH with MoO3 enhances its charge storage capacity. The obtained electrochemical results are also theoretically supported by fractal analysis. Among all the electrodes, the 10 cycle AlOOH/MoO3 nanocomposite displays high value of fractal dimension, which is advantageous for supercapacitor application. Furthermore, we have fabricated a symmetric supercapacitor device to understand the practicality of current work. The fabricated device displays Cs of 68.41 F g-1 within 1.6 V potential window with ∼71 % capacity retention and 100 % coulombic efficiency after 7000 charge-discharge cycles. The highest energy density of 24.32 Wh kg-1 is achieved for the power density of 3907 W kg-1.
通过逐层法合成了 AlOOH/MoO3 二元复合电极，利用钼的多种氧化态增强了 AlOOH 的超级电容特性。X 射线衍射表征揭示了纳米复合材料的多晶性质。利用 X 射线光电子能谱对元素及其化学状态进行了分析。二元复合材料呈现出类似分形的互连网状形态。在 1 M KOH 电解液中进行的三电极测量显示，二元复合材料的最高比容量（Cs）为 1638.15 C g-1@ 5 mV s-1，高于单个成分的容量。此外，10 周期 MoO3 的比容量为 1124.41 C g-1，而其理论容量为 1005 C g-1。优异的电化学性能得益于纳米复合材料中存在的多个氧化还原活性位点、较低的电阻、多孔互连的网状结构以及较短的弛豫时间。AlOOH 与 MoO3 的协同作用增强了其电荷存储能力。分形分析也从理论上支持了所获得的电化学结果。在所有电极中，10 次循环的 AlOOH/MoO3 纳米复合材料显示出较高的分形维值，这对超级电容器的应用非常有利。此外，我们还制作了一个对称超级电容器装置，以了解当前工作的实用性。在 1.6 V 的电位窗口内，所制造的装置显示出 68.41 F g-1 的 Cs，在 7000 次充放电循环后，容量保持率为 71%，库仑效率为 100%。功率密度为 3907 W kg-1 时，能量密度最高，达到 24.32 Wh kg-1。
{"title":"Fractal supported electrochemical analysis of MoO3 decorated AlOOH binary composite for supercapacitor application","authors":"Priyanka Maurya , Suneel Kumar Sharma , S.N. Pandey","doi":"10.1016/j.surfin.2024.105199","DOIUrl":"10.1016/j.surfin.2024.105199","url":null,"abstract":"<div><div>The AlOOH/MoO<sub>3</sub> binary composite electrodes are synthesized by layer-by-layer method to enhance the supercapacitive property of AlOOH by taking advantage of multiple oxidation states of molybdenum. The X-ray diffraction characterization reveals the polycrystalline nature of nanocomposite. The elements and their chemical states are analysed using X-ray photoelectron spectroscopy. The binary composite exhibits interconnected network-like morphology resembling a fractal nature. The three-electrode measurement in 1 M KOH electrolyte shows the highest specific capacity (<em>C<sub>s</sub></em>) of 1638.15 C g<sup>-1</sup>@ 5 mV s<sup>-1</sup> for binary composite, which is greater than the capacity of individual components. Also, we get <em>C<sub>s</sub></em> of 1124.41 C g<sup>-1</sup> for 10 cycle MoO<sub>3</sub> while its theoretical capacity is 1005 C g<sup>-1</sup>. The excellent electrochemical performance is a consequence of multiple redox active sites present in the nanocomposite, lower resistance, porous interconnected network-like structure, and shorter relaxation time. The synergy of AlOOH with MoO<sub>3</sub> enhances its charge storage capacity. The obtained electrochemical results are also theoretically supported by fractal analysis. Among all the electrodes, the 10 cycle AlOOH/MoO<sub>3</sub> nanocomposite displays high value of fractal dimension, which is advantageous for supercapacitor application. Furthermore, we have fabricated a symmetric supercapacitor device to understand the practicality of current work. The fabricated device displays <em>C<sub>s</sub></em> of 68.41 F g<sup>-1</sup> within 1.6 V potential window with ∼71 % capacity retention and 100 % coulombic efficiency after 7000 charge-discharge cycles. The highest energy density of 24.32 Wh kg<sup>-1</sup> is achieved for the power density of 3907 W kg<sup>-1</sup>.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424704","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 : 2024-09-30DOI: 10.1016/j.surfin.2024.105198
Wen-Ming Li , Hui Zhang , Jia-Le Yao , Xiang-Tao Xuan , Hong-Li Wang , Chen-Min Dai
The piezoelectric catalysis technique harnesses naturally occurring vibrational energy to remove organic pollutants from water in an environmentally friendly manner. In this study, a ternary heterostructure SnS2-Bi2S3-BiOCl (S-B-B) composite was successfully synthesized via a one-step hydrothermal method and simultaneously deposited on the surface of carbon felt. The S-B-B heterojunction exhibits significantly enhanced piezoelectric catalytic activity compared to SnS2, Bi2S3, and BiOCl, achieving a k value of 2.26 × 10⁻² min⁻¹ and a degradation efficiency of 89.9 % towards methyl orange (MO) dye after 100 min of ultrasonic degradation. This performance is markedly superior to the individual components, with k values of 3.80 × 10⁻⁴ min⁻¹ for SnS2, 1.16 × 10⁻² min⁻¹ for BiOCl, and 1.31 × 10⁻² min⁻¹ for Bi2S3. Moreover, in addition to levofloxacin (LV), it demonstrates high removal efficiency for Congo red (CR), methylene blue (MB), tetracycline hydrochloride (TC-HCl), and sulfanilamide (SN). Furthermore, it can be loaded onto carbon felt for use in piezoelectric catalytic degradation of dyeing wastewater, highlighting its potential for practical applications. Trapping experiments suggest that singlet oxygen non-radicals and hydroxyl radicals play a critical role in the piezocatalytic degradation of organic contaminants. Based on LC-MS results, a possible degradation pathway for MO dye is proposed. Furthermore, DFT calculations confirm electron transfer from Bi2S3 to SnS2 and BiOCl at the interfaces between SnS2/Bi2S3 and BiOCl/Bi2S3. The piezoelectric mechanism of the S-B-B composite is also elucidated, highlighting the interaction and electron dynamics within the heterostructure.
{"title":"One-step hydrothermal synthesis of ternary heterostructure stannic sulfide - bismuth sulfide - bismuth oxychloride (SnS2-Bi2S3-BiOCl) composite loaded on carbon felt for highly efficient piezocatalytic degradation of organic dyes and antibiotics","authors":"Wen-Ming Li , Hui Zhang , Jia-Le Yao , Xiang-Tao Xuan , Hong-Li Wang , Chen-Min Dai","doi":"10.1016/j.surfin.2024.105198","DOIUrl":"10.1016/j.surfin.2024.105198","url":null,"abstract":"<div><div>The piezoelectric catalysis technique harnesses naturally occurring vibrational energy to remove organic pollutants from water in an environmentally friendly manner. In this study, a ternary heterostructure SnS<sub>2</sub>-Bi<sub>2</sub>S<sub>3</sub>-BiOCl (S-B-B) composite was successfully synthesized via a one-step hydrothermal method and simultaneously deposited on the surface of carbon felt. The S-B-B heterojunction exhibits significantly enhanced piezoelectric catalytic activity compared to SnS<sub>2</sub>, Bi<sub>2</sub>S<sub>3</sub>, and BiOCl, achieving a k value of 2.26 × 10⁻² min⁻¹ and a degradation efficiency of 89.9 % towards methyl orange (MO) dye after 100 min of ultrasonic degradation. This performance is markedly superior to the individual components, with k values of 3.80 × 10⁻⁴ min⁻¹ for SnS<sub>2</sub>, 1.16 × 10⁻² min⁻¹ for BiOCl, and 1.31 × 10⁻² min⁻¹ for Bi<sub>2</sub>S<sub>3</sub>. Moreover, in addition to levofloxacin (LV), it demonstrates high removal efficiency for Congo red (CR), methylene blue (MB), tetracycline hydrochloride (TC-HCl), and sulfanilamide (SN). Furthermore, it can be loaded onto carbon felt for use in piezoelectric catalytic degradation of dyeing wastewater, highlighting its potential for practical applications. Trapping experiments suggest that singlet oxygen non-radicals and hydroxyl radicals play a critical role in the piezocatalytic degradation of organic contaminants. Based on LC-MS results, a possible degradation pathway for MO dye is proposed. Furthermore, DFT calculations confirm electron transfer from Bi<sub>2</sub>S<sub>3</sub> to SnS<sub>2</sub> and BiOCl at the interfaces between SnS<sub>2</sub>/Bi<sub>2</sub>S<sub>3</sub> and BiOCl/Bi<sub>2</sub>S<sub>3</sub>. The piezoelectric mechanism of the S-B-B composite is also elucidated, highlighting the interaction and electron dynamics within the heterostructure.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424187","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 : 2024-09-30DOI: 10.1016/j.surfin.2024.105201
Xiangyu Xu , Wei Du , Jialun Du , Lianwei Shan , Zhanbai Feng , Haitao Wu
In this work, LiF was chosen as a sintering aid to lower the sintering temperature required for monoclinic NdPO4 (NPO) ceramic. A comprehensive investigation was conducted to analyze the impact of LiF on the sintering characteristics, microstructures, phase compositions, crystalline structures, interface characteristics, and microwave dielectric properties of NPO ceramic. Structure-property relationships were discussed based on the density, crystallite size, and lattice strain. The complex impedance spectroscopy revealed the mechanism underlying the interface characteristics of LiF on NPO ceramic. Additionally, far-infrared reflectance spectra and THz time-domain spectra revealed the intrinsic dielectric properties of NdPO4–1 wt.%LiF (NPO1). Notably, 1 wt.% LiF effectively reduced the sintering temperature from 1300 °C to 850 °C, significantly improving densification and dielectric properties. Typical properties such as Q × f = 55,840 GHz (at 9.58 GHz), εr = 10.4, and τf = −43.1 ppm °C−1 were obtained for NPO1 ceramic after sintering at 850 °C. Furthermore, its compatibility with Ag was explored as a prerequisite for LTCC applications. Finally, the NPO1 ceramic was designed as a microstrip antenna with high gain (6.83 dB) and low return loss (−18.85 dB) at a centre frequency of 2.56 GHz, demonstrating its potential for Wi-Fi and Bluetooth applications. This work provides a theoretical foundation and practical guidance for developing orthophosphate ceramics.
{"title":"Low sintering temperature, interface characteristic and microwave/terahertz dielectric properties of ternary-phase Nd2O3-P2O5 based ceramics for patch antenna application","authors":"Xiangyu Xu , Wei Du , Jialun Du , Lianwei Shan , Zhanbai Feng , Haitao Wu","doi":"10.1016/j.surfin.2024.105201","DOIUrl":"10.1016/j.surfin.2024.105201","url":null,"abstract":"<div><div>In this work, LiF was chosen as a sintering aid to lower the sintering temperature required for monoclinic NdPO<sub>4</sub> (NPO) ceramic. A comprehensive investigation was conducted to analyze the impact of LiF on the sintering characteristics, microstructures, phase compositions, crystalline structures, interface characteristics, and microwave dielectric properties of NPO ceramic. Structure-property relationships were discussed based on the density, crystallite size, and lattice strain. The complex impedance spectroscopy revealed the mechanism underlying the interface characteristics of LiF on NPO ceramic. Additionally, far-infrared reflectance spectra and THz time-domain spectra revealed the intrinsic dielectric properties of NdPO<sub>4</sub>–1 wt.%LiF (NPO1). Notably, 1 wt.% LiF effectively reduced the sintering temperature from 1300 °C to 850 °C, significantly improving densification and dielectric properties. Typical properties such as <em>Q × f</em> = 55,840 GHz (at 9.58 GHz), ε<sub>r</sub> = 10.4, and τ<sub>f</sub> = −43.1 ppm °C<sup>−1</sup> were obtained for NPO1 ceramic after sintering at 850 °C. Furthermore, its compatibility with Ag was explored as a prerequisite for LTCC applications. Finally, the NPO1 ceramic was designed as a microstrip antenna with high gain (6.83 dB) and low return loss (−18.85 dB) at a centre frequency of 2.56 GHz, demonstrating its potential for Wi-Fi and Bluetooth applications. This work provides a theoretical foundation and practical guidance for developing orthophosphate ceramics.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424280","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 : 2024-09-29DOI: 10.1016/j.surfin.2024.105170
Fan Yu , Hu Yuan , Wu Jiang , Deqin He , Hong Liu , Xueqiang Qi
In this paper, we comparatively analyze the gas-sensing ability of Pb, Pd and Pt metal-doped GaNNT (M-GaNNT) materials for the hazardous H2S, SO2, NH3 and Cl2 gases. The adsorption structure, adsorption energy (Eads), density of states (DOS), differential charge density and frontier molecular orbital of the M-GaNNT adsorbed hazardous gas have been studied based on the density functional theory (DFT) calculations. The results show that the energy gap of Pb-GaNNT performs the largest change with an increasing percentage change of 358 % after the Cl2 adsorption compared with that before the Cl2 adsorption, while the energy gap of Pt-GaNNT has the least change with an average value of 20.8 %. The doping of metal atoms can effectively improve the gas-sensitivity of M-GaNNT, and the gas-sensitivity follows the order of Pb-GaNNT> Pd-GaNNT> Pt-GaNNT. The potential applications of M-GaNNT in gas sensor and adsorbent are then predicted through the analysis of the adsorption energy, sensitive response (SR) and recovery time (τ). Pb-GaNNT performs the best Cl2 gas removal since the largest Eads (-5.883 eV), largest SR (4.4 × 1015) and largest τ (2.9 × 1087s) can be determined for Cl2 adsorption on Pb-GaNNT. Furthermore, Pb-GaNNT is a good NH3 gas sensor since the related τ is only 2.9 s at 498 K, and a small Eads (-1.232 eV) with large SR (9.7 × 105) can be determined as well. The research findings in this paper provide a new sensor material option for both the detection and the removal of harmful gases, and the systematically theoretical method can spread to other systems.
{"title":"Comparison of Gas-sensitive response of three metal-doped GaNNT with Pb, Pd and Pt after adsorption of hazardous gases","authors":"Fan Yu , Hu Yuan , Wu Jiang , Deqin He , Hong Liu , Xueqiang Qi","doi":"10.1016/j.surfin.2024.105170","DOIUrl":"10.1016/j.surfin.2024.105170","url":null,"abstract":"<div><div>In this paper, we comparatively analyze the gas-sensing ability of Pb, Pd and Pt metal-doped GaNNT (M-GaNNT) materials for the hazardous H<sub>2</sub>S, SO<sub>2</sub>, NH<sub>3</sub> and Cl<sub>2</sub> gases. The adsorption structure, adsorption energy (<em>E<sub>ads</sub></em>), density of states (DOS), differential charge density and frontier molecular orbital of the M-GaNNT adsorbed hazardous gas have been studied based on the density functional theory (DFT) calculations. The results show that the energy gap of Pb-GaNNT performs the largest change with an increasing percentage change of 358 % after the Cl<sub>2</sub> adsorption compared with that before the Cl<sub>2</sub> adsorption, while the energy gap of Pt-GaNNT has the least change with an average value of 20.8 %. The doping of metal atoms can effectively improve the gas-sensitivity of M-GaNNT, and the gas-sensitivity follows the order of Pb-GaNNT> Pd-GaNNT> Pt-GaNNT. The potential applications of M-GaNNT in gas sensor and adsorbent are then predicted through the analysis of the adsorption energy, sensitive response (<em>SR</em>) and recovery time (<em>τ</em>). Pb-GaNNT performs the best Cl<sub>2</sub> gas removal since the largest <em>E<sub>ads</sub></em> (-5.883 eV), largest <em>SR</em> (4.4 × 10<sup>15</sup>) and largest <em>τ</em> (2.9 × 10<sup>87</sup>s) can be determined for Cl<sub>2</sub> adsorption on Pb-GaNNT. Furthermore, Pb-GaNNT is a good NH<sub>3</sub> gas sensor since the related <em>τ</em> is only 2.9 s at 498 K, and a small <em>E<sub>ads</sub></em> (-1.232 eV) with large <em>SR</em> (9.7 × 10<sup>5</sup>) can be determined as well. The research findings in this paper provide a new sensor material option for both the detection and the removal of harmful gases, and the systematically theoretical method can spread to other systems.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424284","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 : 2024-09-29DOI: 10.1016/j.surfin.2024.105194
Wen.Xue Zhang , Wei.Wei Wang , Cheng. He
The logical design of inexpensive, non-polluting, and extremely effective photocatalysts is a crucial step toward achieving clean energy. The currently low solar-to-hydrogen (STH) conversion efficiency (ηSTH) makes hydrogen production technologies less than optimal. Herein, novel β-XY (X = Ge, Sn, Y = S)/g-C3N4 heterostructures have been constructed. Among them, the β-SnS/g-C3N4 exhibits low carrier recombination, and its geometry, optoelectronic properties, as well as the thermodynamic feasibility of its reaction, have been thoroughly examined through DFT calculations. The results demonstrate that the β-SnS/g-C3N4 heterostructure is a type-II heterostructure, exhibiting an indirect band gap of 2.57 eV. Photocatalysis is more efficient because of the built-in electric field that extends from the g-C3N4 monolayer to the β-SnS monolayer, effectively separating electrons and holes. The continuously decreasing free energy validates the thermodynamic spontaneity of water splitting. Additionally, the heterostructure demonstrates robust absorption in both the visible and UV ranges. Notably, the ηSTH of 15.54 % underscores the commercial viability of this material. These findings thus suggest that β-SnS/g-C3N4 heterostructure is a good candidate material for water splitting via photocatalysis.
{"title":"Construction of novel β-XY (X = Ge, Sn, Y = S)/g-C3N4 heterostructures: efficient visible light-driven water splitting catalysts","authors":"Wen.Xue Zhang , Wei.Wei Wang , Cheng. He","doi":"10.1016/j.surfin.2024.105194","DOIUrl":"10.1016/j.surfin.2024.105194","url":null,"abstract":"<div><div>The logical design of inexpensive, non-polluting, and extremely effective photocatalysts is a crucial step toward achieving clean energy. The currently low solar-to-hydrogen (STH) conversion efficiency (<em>η<sub>STH</sub></em>) makes hydrogen production technologies less than optimal. Herein, novel β-XY (X = Ge, Sn, Y = S)/g-C<sub>3</sub>N<sub>4</sub> heterostructures have been constructed. Among them, the β-SnS/g-C<sub>3</sub>N<sub>4</sub> exhibits low carrier recombination, and its geometry, optoelectronic properties, as well as the thermodynamic feasibility of its reaction, have been thoroughly examined through DFT calculations. The results demonstrate that the β-SnS/g-C<sub>3</sub>N<sub>4</sub> heterostructure is a type-II heterostructure, exhibiting an indirect band gap of 2.57 eV. Photocatalysis is more efficient because of the built-in electric field that extends from the g-C<sub>3</sub>N<sub>4</sub> monolayer to the β-SnS monolayer, effectively separating electrons and holes. The continuously decreasing free energy validates the thermodynamic spontaneity of water splitting. Additionally, the heterostructure demonstrates robust absorption in both the visible and UV ranges. Notably, the <em>η<sub>STH</sub></em> of 15.54 % underscores the commercial viability of this material. These findings thus suggest that β-SnS/g-C<sub>3</sub>N<sub>4</sub> heterostructure is a good candidate material for water splitting via photocatalysis.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424279","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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