Pub Date : 2024-09-29DOI: 10.1016/j.surfin.2024.105169
Liansheng Zheng , Hongwei Zang , Dingdi Wang , Yingbo Cong , Bin Gao , Shuo Wang , Huailiang Xu
Nano- and micro-droplets provide a platform for microanalysis of a variety of biochemical reactions with less consumption of reagents and large-extent elimination of cross-contamination, but stable generation of such monodisperse droplets with an on-demand size and repetition rate should be first established. Here, we present a simple and robust approach to generate nano/microliter (nL/μL) droplets with predetermined size and repetition rate by using femtosecond laser filament-fabricated stainless bevel needle nozzles (BNNs). We demonstrate that hierarchically heterogeneous micro/nanostructures can be directly formed on both the inner and outer surfaces of BNNs by femtosecond laser filament processing, and that after a heat treatment the fabricated BNNs show an excellent superhydrophobic property with the water contact angle of ∼160° and the rolling-off angle of ∼0.4°. With the superhydrophobic BNNs (19–27 gauge), we produce monodisperse water droplets (2.5 μL–87 nL) with nearly the same sizes as the needle diameters, and dispense them repeatedly with on-demand repetition rates from sub-1 Hz to more than 100 Hz over several orders of the flow rate. The results provide a new way for generating microdroplets on demand for various droplet-based applications.
{"title":"Generating nano/microliter droplets with on-demand repetition rates by femtosecond filament-fabricated superhydrophobic bevel needle nozzles","authors":"Liansheng Zheng , Hongwei Zang , Dingdi Wang , Yingbo Cong , Bin Gao , Shuo Wang , Huailiang Xu","doi":"10.1016/j.surfin.2024.105169","DOIUrl":"10.1016/j.surfin.2024.105169","url":null,"abstract":"<div><div>Nano- and micro-droplets provide a platform for microanalysis of a variety of biochemical reactions with less consumption of reagents and large-extent elimination of cross-contamination, but stable generation of such monodisperse droplets with an on-demand size and repetition rate should be first established. Here, we present a simple and robust approach to generate nano/microliter (nL/μL) droplets with predetermined size and repetition rate by using femtosecond laser filament-fabricated stainless bevel needle nozzles (BNNs). We demonstrate that hierarchically heterogeneous micro/nanostructures can be directly formed on both the inner and outer surfaces of BNNs by femtosecond laser filament processing, and that after a heat treatment the fabricated BNNs show an excellent superhydrophobic property with the water contact angle of ∼160° and the rolling-off angle of ∼0.4°. With the superhydrophobic BNNs (19–27 gauge), we produce monodisperse water droplets (2.5 μL–87 nL) with nearly the same sizes as the needle diameters, and dispense them repeatedly with on-demand repetition rates from sub-1 Hz to more than 100 Hz over several orders of the flow rate. The results provide a new way for generating microdroplets on demand for various droplet-based applications.</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":"142424183","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}
Crystalline transition metal (TM) sulfides exhibit metallic behavior and have been identified as ideal electrocatalytic candidates for electrochemical sulfion oxidation reaction (SOR). However, the SOR performance for amorphous TM sulfides is still poorly understood so far. Herein, we sulfurized NiFeOOH clusters deposited on ZnIn2S4 nanosheets arrays to amorphous NiFe-based sulfides (denoted as NiFeS) for photoelectrochemical SOR. We found amorphous NiFeS presented a n-type semiconductor property, the elaborate band alignment between NiFeS band gap structure and the oxidation potential of S2− promoted the superimposing effect of electrocatalytic and photocatalytic current for SOR under illumination. The overall SOR current density of ZnIn2S4/NiFeS reaches the maximum value about 7.6 mA cm−2 at 0.6 V vs. RHE after 6 h stability test, which was composed by 2.6 mA cm−2 electrocatalytic current density and 5.0 mA cm−2 photocatalytic current density. Our work presents a new strategy for sulfion oxidation reaction based on amorphous transition metal sulfides.
结晶过渡金属（TM）硫化物表现出金属特性，已被确定为电化学亚硫酰氧化反应（SOR）的理想电催化候选物质。然而，迄今为止，人们对非晶态过渡金属硫化物的硫化性能仍知之甚少。在此，我们将沉积在 ZnIn2S4 纳米片阵列上的 NiFeOOH 簇硫化成非晶态 NiFe 基硫化物（简称为 NiFeS），用于光电化学 SOR。我们发现无定形的 NiFeS 具有 n 型半导体特性，NiFeS 带隙结构与 S2- 氧化电位之间精心设计的带排列促进了光照下 SOR 的电催化电流和光催化电流的叠加效应。经过 6 h 的稳定性测试，ZnIn2S4/NiFeS 的整体 SOR 电流密度在 0.6 V 对 RHE 时达到最大值约 7.6 mA cm-2，由 2.6 mA cm-2 的电催化电流密度和 5.0 mA cm-2 的光催化电流密度组成。我们的工作提出了一种基于无定形过渡金属硫化物的磺胺氧化反应新策略。
{"title":"Superimposing effect of electrocatalytic activity and photocatalytic activity for amorphous NiFe-sulfides photoanode in sulfion oxidation reaction","authors":"Qianqian Huang , Qianyang Chang , Zhenyu Luo , Minfei Xie , Nanbing Jiang , Xiaoning Zhang , Ming Zhou , Yunhuai Zhang , Peng Xiao","doi":"10.1016/j.surfin.2024.105163","DOIUrl":"10.1016/j.surfin.2024.105163","url":null,"abstract":"<div><div>Crystalline transition metal (TM) sulfides exhibit metallic behavior and have been identified as ideal electrocatalytic candidates for electrochemical sulfion oxidation reaction (SOR). However, the SOR performance for amorphous TM sulfides is still poorly understood so far. Herein, we sulfurized NiFeOOH clusters deposited on ZnIn<sub>2</sub>S<sub>4</sub> nanosheets arrays to amorphous NiFe-based sulfides (denoted as NiFeS) for photoelectrochemical SOR. We found amorphous NiFeS presented a n-type semiconductor property, the elaborate band alignment between NiFeS band gap structure and the oxidation potential of S<sup>2−</sup> promoted the superimposing effect of electrocatalytic and photocatalytic current for SOR under illumination. The overall SOR current density of ZnIn<sub>2</sub>S<sub>4</sub>/NiFeS reaches the maximum value about 7.6 mA cm<sup>−2</sup> at 0.6 V vs. RHE after 6 h stability test, which was composed by 2.6 mA cm<sup>−2</sup> electrocatalytic current density and 5.0 mA cm<sup>−2</sup> photocatalytic current density. Our work presents a new strategy for sulfion oxidation reaction based on amorphous transition metal sulfides.</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":"142423865","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.2024.105195
Avijit Ghosh , Nondon Lal Dey , Nasser S. Awwad , Abul Kashem Mohammad Yahia , Mohammad Shahjalal , Hala A. Ibrahium
A significant amount of interest in the field of solar energy has recently been generated by the remarkable optical, structural, and electronic attributes of inorganic perovskite-based substances. A thorough investigation was conducted on how tensile along with compressive strains influence the electronic and optical properties of halide perovskite Sr3AsBr3, utilizing FP-DFT. The PBE functional is used to determine the direct bandgap of 1.512 eV for unstrained Sr3AsBr3 at the Γ position. The bandgap redshifts (1.216 eV at -4 % strain) under compressive strain and slightly increases (1.728 eV at +4 % strain) under tensile tension, causing the absorption coefficient to blueshift. The optical properties, including the functions of dielectric, electron energy loss function, and absorption coefficient, all indicate a considerable capacity for absorption in the area of the visible spectrum, and the band characteristics of this component agree with these qualities. We used Sr3AsBr3 absorbers and CdS electron transport layers (ETL) with different thicknesses, defect densities, and doping concentrations to study solar power capabilities using the SCAPS-1D simulator. The most effective arrangement (at -4 % strain) had a fill factor (FF) of 86.76 %, a short-circuit current density (JSC) of 37.5593 mAcm−2, an open-circuit voltage (VOC) of 0.8712 V, and a power conversion efficiency (PCE) of 28.39 %. Our findings support additional research into Sr3AsBr3, a promising perovskite for optoelectronic uses.
{"title":"Examining the electronic, structural, optical, and photovoltaic capabilities of Sr3AsBr3 perovskite under tensile and compressive strains with DFT and SCAPS-1D","authors":"Avijit Ghosh , Nondon Lal Dey , Nasser S. Awwad , Abul Kashem Mohammad Yahia , Mohammad Shahjalal , Hala A. Ibrahium","doi":"10.1016/j.surfin.2024.105195","DOIUrl":"10.1016/j.surfin.2024.105195","url":null,"abstract":"<div><div>A significant amount of interest in the field of solar energy has recently been generated by the remarkable optical, structural, and electronic attributes of inorganic perovskite-based substances. A thorough investigation was conducted on how tensile along with compressive strains influence the electronic and optical properties of halide perovskite Sr<sub>3</sub>AsBr<sub>3</sub>, utilizing FP-DFT. The PBE functional is used to determine the direct bandgap of 1.512 eV for unstrained Sr<sub>3</sub>AsBr<sub>3</sub> at the Γ position. The bandgap redshifts (1.216 eV at -4 % strain) under compressive strain and slightly increases (1.728 eV at +4 % strain) under tensile tension, causing the absorption coefficient to blueshift. The optical properties, including the functions of dielectric, electron energy loss function, and absorption coefficient, all indicate a considerable capacity for absorption in the area of the visible spectrum, and the band characteristics of this component agree with these qualities. We used Sr<sub>3</sub>AsBr<sub>3</sub> absorbers and CdS electron transport layers (ETL) with different thicknesses, defect densities, and doping concentrations to study solar power capabilities using the SCAPS-1D simulator. The most effective arrangement (at -4 % strain) had a fill factor (FF) of 86.76 %, a short-circuit current density (J<sub>SC</sub>) of 37.5593 mAcm<sup>−2</sup>, an open-circuit voltage (V<sub>OC</sub>) of 0.8712 V, and a power conversion efficiency (PCE) of 28.39 %. Our findings support additional research into Sr<sub>3</sub>AsBr<sub>3</sub>, a promising perovskite for optoelectronic uses.</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":"142424705","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.2024.105192
Yanan Liu , Yiman Gao , Hongpu Shi , Dong Gui , Wen Zhou , Yang Liu , Deng-Guang Yu
Amidst the escalating global concern over heavy metal discharge from industrial effluents, Mo(VI), as a potentially toxic trace element, poses significant risks to human and environmental health. Traditional treatment methods such as biodegradation and ion exchange have low removal efficiency, hence, the efficient removal of Mo (VI) ions from industrial wastewater assumes paramount importance. Emerging materials, Metal-Organic Frameworks (MOFs), have garnered extensive attention in water treatment due to their strong adsorption properties, and MOFs membrane materials are hailed as the most promising adsorbents. Therefore, this study aims to prepare a novel membrane material with high efficiency for the removal of Mo (VI) by loading MOFs into nanofibers. Given the water stability of MIL-101, MIL-101-R(-H, -NH2, -NO2) with different functional groups were prepared and subsequently loaded into PAN nanofibrous for the adsorption of Mo(VI). Adsorption kinetics and isotherm studies revealed PAN/MIL-101(Cr)-NH2 to exhibit superior adsorption performance, achieving a maximum adsorption capacity of 171.81 mg g-1. Density functional theory (DFT) calculations and molecular dynamics simulations elucidated the adsorption mechanism, highlighting the role of amino modification in facilitating Mo(VI) adsorption through electrostatic attraction and high reactivity. This work not only offers novel materials and approaches for Mo(VI) wastewater treatment but also advances the industrial application of MOF materials in the domain of heavy metal wastewater treatment.
{"title":"Enhanced absorption capacity and fundamental mechanism of electrospun MIL-101(Cr)-NH2/PAN nanofibrous membranes for Mo(VI) removal","authors":"Yanan Liu , Yiman Gao , Hongpu Shi , Dong Gui , Wen Zhou , Yang Liu , Deng-Guang Yu","doi":"10.1016/j.surfin.2024.105192","DOIUrl":"10.1016/j.surfin.2024.105192","url":null,"abstract":"<div><div>Amidst the escalating global concern over heavy metal discharge from industrial effluents, Mo(VI), as a potentially toxic trace element, poses significant risks to human and environmental health. Traditional treatment methods such as biodegradation and ion exchange have low removal efficiency, hence, the efficient removal of Mo (VI) ions from industrial wastewater assumes paramount importance. Emerging materials, Metal-Organic Frameworks (MOFs), have garnered extensive attention in water treatment due to their strong adsorption properties, and MOFs membrane materials are hailed as the most promising adsorbents. Therefore, this study aims to prepare a novel membrane material with high efficiency for the removal of Mo (VI) by loading MOFs into nanofibers. Given the water stability of MIL-101, MIL-101-R(-H, -NH<sub>2</sub>, -NO<sub>2</sub>) with different functional groups were prepared and subsequently loaded into PAN nanofibrous for the adsorption of Mo(VI). Adsorption kinetics and isotherm studies revealed PAN/MIL-101(Cr)-NH<sub>2</sub> to exhibit superior adsorption performance, achieving a maximum adsorption capacity of 171.81 mg g<sup>-1</sup>. Density functional theory (DFT) calculations and molecular dynamics simulations elucidated the adsorption mechanism, highlighting the role of amino modification in facilitating Mo(VI) adsorption through electrostatic attraction and high reactivity. This work not only offers novel materials and approaches for Mo(VI) wastewater treatment but also advances the industrial application of MOF materials in the domain of heavy metal wastewater treatment.</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":"142424274","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.2024.105190
Yashwanth Arcot , Minchen Mu , Monica Iepure , Rae Karell Yodong , Wentao Zhou , Younjin Min , Luis Cisneros-Zevallos , Mustafa E.S. Akbulut
Nanopesticidal adsorption on plant surfaces is a critical determinant of their application efficacy, persistence, and ecological impact. In this study, we systematically investigate the impact of surface chemistry on the attachment of nanopesticides for seven different nanocarriers: ethyl lauroyl arginate (ELA, cationic), cocamidopropyl betaine (CAPB, zwitterionic), tween 80 (TW80, nonionic), β-cyclodextrin (βCD), sodium dodecyl sulfate (SDS, anionic), whey protein isolate (WPI), and poloxamer 407 (PXL, nonionic). Azadirachtin from neem seed extract was employed as a model pesticide active ingredient. The nanopesticides were characterized using dynamic light scattering, UV–visible spectroscopy, static contact angle (SCA, θ), and zeta (ζ) potential measurements. Pepper leaves (ζ = −11.6 mV) and candelilla wax (ζ = −2.6 mV) films were utilized to analyze the effect of nanocarrier chemical composition on nanopesticide adsorption. Fluorescence microscopy was utilized to quantify the adsorption of nanopesticides (with fluorophore tagging) on the substrates. It was found that the choice of nanocarrier significantly influenced the adsorption behavior. Nanopesticides with ELA corona, which was cationic with a zeta potential of ∼+19 mV and θ of ∼ 61°, exhibited the highest affinity towards the leaf cuticle and wax substrates, attributed to favorable electrostatic interactions forces. Conversely, nanopesticides with SDS (ζ = −48 mV; θ = 45°), WPI (ζ = −24 mV; θ = 54°), and PXL (ζ = −31 mV; θ = 64°) corona demonstrated the least adsorption. These findings indicate a weak correlation between the wetting behavior of nanopesticide suspensions and nanopesticide adsorption on plant and wax surfaces, as well as a strong correlation between nanopesticide zeta potential and nanopesticide adsorption. These findings heuristically recommend that aqueous cationic and zwitterionic nanocarriers for pesticides provide superior adsorption characteristics on pepper leaves and candelilla wax surfaces. Aqueous macromolecular carriers such as PXL and WPI have performed less effectively in adherence compared to shorter chain amphiphiles with similar zeta potential and wetting characteristics, indicating that the steric and osmotic chain effects of hydrophilic macromolecules hinder the adsorption relative to shorter chains.
{"title":"Influence of nanopesticide surface chemistry on adsorption to plant cuticle and wax layer: The role of zeta potential and wetting","authors":"Yashwanth Arcot , Minchen Mu , Monica Iepure , Rae Karell Yodong , Wentao Zhou , Younjin Min , Luis Cisneros-Zevallos , Mustafa E.S. Akbulut","doi":"10.1016/j.surfin.2024.105190","DOIUrl":"10.1016/j.surfin.2024.105190","url":null,"abstract":"<div><div>Nanopesticidal adsorption on plant surfaces is a critical determinant of their application efficacy, persistence, and ecological impact. In this study, we systematically investigate the impact of surface chemistry on the attachment of nanopesticides for seven different nanocarriers: ethyl lauroyl arginate (ELA, cationic), cocamidopropyl betaine (CAPB, zwitterionic), tween 80 (TW80, nonionic), β-cyclodextrin (βCD), sodium dodecyl sulfate (SDS, anionic), whey protein isolate (WPI), and poloxamer 407 (PXL, nonionic). Azadirachtin from neem seed extract was employed as a model pesticide active ingredient. The nanopesticides were characterized using dynamic light scattering, UV–visible spectroscopy, static contact angle (SCA, θ), and zeta (<em>ζ</em>) potential measurements. Pepper leaves (ζ = −11.6 mV) and candelilla wax (ζ = −2.6 mV) films were utilized to analyze the effect of nanocarrier chemical composition on nanopesticide adsorption. Fluorescence microscopy was utilized to quantify the adsorption of nanopesticides (with fluorophore tagging) on the substrates. It was found that the choice of nanocarrier significantly influenced the adsorption behavior. Nanopesticides with ELA corona, which was cationic with a zeta potential of ∼+19 mV and θ of ∼ 61°, exhibited the highest affinity towards the leaf cuticle and wax substrates, attributed to favorable electrostatic interactions forces. Conversely, nanopesticides with SDS (ζ = −48 mV; θ = 45°), WPI (ζ = −24 mV; θ = 54°), and PXL (ζ = −31 mV; θ = 64°) corona demonstrated the least adsorption. These findings indicate a weak correlation between the wetting behavior of nanopesticide suspensions and nanopesticide adsorption on plant and wax surfaces, as well as a strong correlation between nanopesticide zeta potential and nanopesticide adsorption. These findings heuristically recommend that aqueous cationic and zwitterionic nanocarriers for pesticides provide superior adsorption characteristics on pepper leaves and candelilla wax surfaces. Aqueous macromolecular carriers such as PXL and WPI have performed less effectively in adherence compared to shorter chain amphiphiles with similar zeta potential and wetting characteristics, indicating that the steric and osmotic chain effects of hydrophilic macromolecules hinder the adsorption relative to shorter chains.</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":"142424281","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.2024.105193
Ziyang Dang , Jingzhuo Tian , Jun Fan , Yang Yang , Enzhou Liu
The construction of S-scheme heterojunctions via exploring semiconductors with suitable energy band structures can effectively improve the photocatalytic performance of TiO2. In this work, CuCoSe2/TiO2 heterojunction were prepared using solvent evaporation strategy by their different surface charge properties. The investigation indicates that rates of H2 evolution (rH2) of the system increases significantly from 138.1 (TiO2) to 3773.8 μmol·g−1·h−1 (CuCoSe2/TiO2). It is found that the incorporation of CuCoSe2 can extend the visible light absorption range of the system, increase the electrochemically active surface area, facilitate charge generation and decrease the transfer resistance, reduce the H2 production overpotential and the water contact angle. Further investigation reveals that a bimetallic selenide CuCoSe2 exhibit superior enhancement activity compared to their monometallic selenides (CuSe2, CoSe2) due to the synergistic effect of Co and Cu. Especially, the charge transfer between CuCoSe2 and TiO2 follows S-scheme charge separation route, which can effectively enhance charge separation/migration, reserve e− with strong reducing ability in TiO2, thereby promoting the H2 evolution kinetics. Moreover, the heterojunction also demonstrates exceptional stability throughout the cycle experiment. The present work establishes an experimental basis for the advancement of highly efficient and stable bimetallic selenides related heterojunctions in the field of photocatalytic H2 evolution.
通过探索具有合适能带结构的半导体来构建 S 型异质结，可以有效提高 TiO2 的光催化性能。本研究采用溶剂蒸发策略制备了具有不同表面电荷特性的 CuCoSe2/TiO2 异质结。研究表明，该体系的 H2 演化速率（rH2）从 138.1（TiO2）显著增加到 3773.8 μmol-g-1-h-1（CuCoSe2/TiO2）。研究发现，CuCoSe2 的加入可以扩大体系的可见光吸收范围，增加电化学活性表面积，促进电荷生成并降低传递电阻，降低 H2 生成过电位和水接触角。进一步的研究发现，与单金属硒化物（CuSe2、CoSe2）相比，双金属硒化物 CuCoSe2 由于 Co 和 Cu 的协同作用而表现出更高的增强活性。特别是 CuCoSe2 与 TiO2 之间的电荷转移遵循 S 型电荷分离路线，可有效增强电荷分离/迁移，在 TiO2 中保留具有较强还原能力的 e-，从而促进 H2 的演化动力学。此外，异质结在整个循环实验过程中也表现出卓越的稳定性。本研究为在光催化 H2 演化领域开发高效、稳定的双金属硒化物相关异质结奠定了实验基础。
{"title":"Photocatalytic H2 evolution over CuCoSe2 nanoparticles decorated TiO2 nanosheets with S-scheme charge separation route","authors":"Ziyang Dang , Jingzhuo Tian , Jun Fan , Yang Yang , Enzhou Liu","doi":"10.1016/j.surfin.2024.105193","DOIUrl":"10.1016/j.surfin.2024.105193","url":null,"abstract":"<div><div>The construction of S-scheme heterojunctions via exploring semiconductors with suitable energy band structures can effectively improve the photocatalytic performance of TiO<sub>2</sub>. In this work, CuCoSe<sub>2</sub>/TiO<sub>2</sub> heterojunction were prepared using solvent evaporation strategy by their different surface charge properties. The investigation indicates that rates of H<sub>2</sub> evolution (rH<sub>2</sub>) of the system increases significantly from 138.1 (TiO<sub>2</sub>) to 3773.8 μmol·g<sup>−1</sup>·h<sup>−1</sup> (CuCoSe<sub>2</sub>/TiO<sub>2</sub>). It is found that the incorporation of CuCoSe<sub>2</sub> can extend the visible light absorption range of the system, increase the electrochemically active surface area, facilitate charge generation and decrease the transfer resistance, reduce the H<sub>2</sub> production overpotential and the water contact angle. Further investigation reveals that a bimetallic selenide CuCoSe<sub>2</sub> exhibit superior enhancement activity compared to their monometallic selenides (CuSe<sub>2</sub>, CoSe<sub>2</sub>) due to the synergistic effect of Co and Cu. Especially, the charge transfer between CuCoSe<sub>2</sub> and TiO<sub>2</sub> follows S-scheme charge separation route, which can effectively enhance charge separation/migration, reserve <em>e</em><sup>−</sup> with strong reducing ability in TiO<sub>2</sub>, thereby promoting the H<sub>2</sub> evolution kinetics. Moreover, the heterojunction also demonstrates exceptional stability throughout the cycle experiment. The present work establishes an experimental basis for the advancement of highly efficient and stable bimetallic selenides related heterojunctions in the field of photocatalytic H<sub>2</sub> evolution.</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":"142424157","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.2024.105197
Xinyu Wang , Yanqing Shen , Xianghui Meng , Xin Yang , Qing Ai , Yong Shuai , Zhongxiang Zhou
The arsenic and lead compounds produced by coal combustion have serious impacts on human health and the environment, making it urgent to simultaneously remove arsenic and lead. In this work, the adsorption characteristics of As2, As2O3, Pb and PbO on 2D Double Transition-Metal Pyridine-Tetranitrogen-Annulene membrane (DTM-PTA, TM=Co, Cu, Zn) are investigated through density functional theory calculations. The adsorption energy, bonding mechanism, electronic and magnetic properties are analyzed in detailed. Firstly, the distribution density of transition metal atoms as adsorption active sites is high, which is conducive to the adsorption of molecules. The results demonstrate that the DCo-PTA is a promising adsorbent for simultaneously removing As2, As2O3, Pb and PbO with highest adsorption energy. According to the variation of magnetic moment, DCu-PTA and DZn-PTA can detect the adsorption of PbO in the mixture of As2, As2O3, Pb and PbO. In addition, the adsorbed molecules can regulate the array of spin electron. Although temperature hinders the adsorption process of molecules, DCo-PTA can still spontaneously adsorb these molecules within the temperature range of 300–1000 K. This indicates that DCo-PTA is an excellent adsorbent which can work in high temperature.
{"title":"The adsorption characteristic of As2, As2O3, Pb, PbO on double transition-metal pyridine-tetranitrogen-annulene membrane","authors":"Xinyu Wang , Yanqing Shen , Xianghui Meng , Xin Yang , Qing Ai , Yong Shuai , Zhongxiang Zhou","doi":"10.1016/j.surfin.2024.105197","DOIUrl":"10.1016/j.surfin.2024.105197","url":null,"abstract":"<div><div>The arsenic and lead compounds produced by coal combustion have serious impacts on human health and the environment, making it urgent to simultaneously remove arsenic and lead. In this work, the adsorption characteristics of As<sub>2</sub>, As<sub>2</sub>O<sub>3</sub>, Pb and PbO on 2D Double Transition-Metal Pyridine-Tetranitrogen-Annulene membrane (DTM-PTA, TM=Co, Cu, Zn) are investigated through density functional theory calculations. The adsorption energy, bonding mechanism, electronic and magnetic properties are analyzed in detailed. Firstly, the distribution density of transition metal atoms as adsorption active sites is high, which is conducive to the adsorption of molecules. The results demonstrate that the DCo-PTA is a promising adsorbent for simultaneously removing As<sub>2</sub>, As<sub>2</sub>O<sub>3</sub>, Pb and PbO with highest adsorption energy. According to the variation of magnetic moment, DCu-PTA and DZn-PTA can detect the adsorption of PbO in the mixture of As<sub>2</sub>, As<sub>2</sub>O<sub>3</sub>, Pb and PbO. In addition, the adsorbed molecules can regulate the array of spin electron. Although temperature hinders the adsorption process of molecules, DCo-PTA can still spontaneously adsorb these molecules within the temperature range of 300–1000 K. This indicates that DCo-PTA is an excellent adsorbent which can work in high temperature.</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":"142424185","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 : 2024-09-28DOI: 10.1016/j.surfin.2024.105191
Zien Deng , Yong Luo , Juntao Wang , Xin Guo , Caiping Fu , Ning Zhang
Tungsten (W), mainly existing as hexavalent oxidation state in nature, has been considered as an increasingly prominent waterborne pollutant, but it is also a critical metal. Therefore, it is important to develop a material to adsorb W(VI) from the waste water containing W(VI) to realize the high-efficiency enrichment and recovery of W(VI). Inspired by self-assembly of phosphate and W(VI) ions in the acidic solutions to form phosphotungstic polyoxoanions (e.g., Keggin-type PW12O403−), in this work, we have loaded the phosphate ion to surface of the magnetic Fe3O4 nanoparticles (Fe3O4 NPs) by β particle irradiation to synthesize a composite adsorbent, HxPO4@Fe3O4 solid-solution (SS). This novel adsorbent is very efficient for W(VI) adsorption and recovery. The results of a batch of adsorption experiments indicate that HxPO4@Fe3O4 SS has a high adsorption efficiency for W(VI) in aqueous environments and strong anti-interference of coexist ions especially PO43−. Under room temperature conditions (∼25 °C), the maximum adsorption capacity reaches 88.44 mg g−1. This method not only ensures a substantial increase in W(VI) adsorption but also provides a facile means for adsorbent recovery, while minimizing additional environmental burdens. Based on the characterization results from Fourier transform infrared, Zeta potential, and X-ray photoelectron spectroscopies, we speculated that the possible mechanism of the adsorption process is that formed W(VI) polyoxoanions in acidic solutions are initially attracted by electrostatic attraction to the positively charged HxPO4@Fe3O4 surface, and then oxolation reaction occurs between W-OH of polyoxoanions and phosphate hydroxyl (P-OH) on the HxPO4@Fe3O4 surface to form P-O-W bridging oxygen group. This adsorption mechanism is also reflected in the adsorption kinetics, following a pseudo-second-order kinetic model, and adsorption thermodynamics, exhibiting a large enthalpy change (−76.3 kJ/mol) and a significant entropy reduction (−174.5 J/(mol K)).
{"title":"The solid-solution HxPO4@Fe3O4 synthesized by irradiation enhances the adsorption capacity of tungsten(VI) and anti-interference of coexisting oxoanion in waste water: Surface oxolation interaction","authors":"Zien Deng , Yong Luo , Juntao Wang , Xin Guo , Caiping Fu , Ning Zhang","doi":"10.1016/j.surfin.2024.105191","DOIUrl":"10.1016/j.surfin.2024.105191","url":null,"abstract":"<div><div>Tungsten (W), mainly existing as hexavalent oxidation state in nature, has been considered as an increasingly prominent waterborne pollutant, but it is also a critical metal. Therefore, it is important to develop a material to adsorb W(VI) from the waste water containing W(VI) to realize the high-efficiency enrichment and recovery of W(VI). Inspired by self-assembly of phosphate and W(VI) ions in the acidic solutions to form phosphotungstic polyoxoanions (e.g., Keggin-type PW<sub>12</sub>O<sub>40</sub><sup>3</sup><sup>−</sup>), in this work, we have loaded the phosphate ion to surface of the magnetic Fe<sub>3</sub>O<sub>4</sub> nanoparticles (Fe<sub>3</sub>O<sub>4</sub> NPs) by β particle irradiation to synthesize a composite adsorbent, H<em><sub>x</sub></em>PO<sub>4</sub>@Fe<sub>3</sub>O<sub>4</sub> solid-solution (SS). This novel adsorbent is very efficient for W(VI) adsorption and recovery. The results of a batch of adsorption experiments indicate that H<em><sub>x</sub></em>PO<sub>4</sub>@Fe<sub>3</sub>O<sub>4</sub> SS has a high adsorption efficiency for W(VI) in aqueous environments and strong anti-interference of coexist ions especially PO<sub>4</sub><sup>3</sup><sup>−</sup>. Under room temperature conditions (∼25 °C), the maximum adsorption capacity reaches 88.44 mg g<sup>−</sup><sup>1</sup>. This method not only ensures a substantial increase in W(VI) adsorption but also provides a facile means for adsorbent recovery, while minimizing additional environmental burdens. Based on the characterization results from Fourier transform infrared, Zeta potential, and X-ray photoelectron spectroscopies, we speculated that the possible mechanism of the adsorption process is that formed W(VI) polyoxoanions in acidic solutions are initially attracted by electrostatic attraction to the positively charged H<em><sub>x</sub></em>PO<sub>4</sub>@Fe<sub>3</sub>O<sub>4</sub> surface, and then oxolation reaction occurs between W-OH of polyoxoanions and phosphate hydroxyl (P-OH) on the H<em><sub>x</sub></em>PO<sub>4</sub>@Fe<sub>3</sub>O<sub>4</sub> surface to form P-O-W bridging oxygen group. This adsorption mechanism is also reflected in the adsorption kinetics, following a pseudo-second-order kinetic model, and adsorption thermodynamics, exhibiting a large enthalpy change (−76.3 kJ/mol) and a significant entropy reduction (−174.5 J/(mol K)).</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424180","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 : 2024-09-28DOI: 10.1016/j.surfin.2024.105187
Sarfraz Ahmad , Muhammad Imran , Fayyaz Hussain , Niaz Ahmad Niaz , Ammar Mohamed Tighezza , R.M.A. Khalil , M. Irfan , Muhammad Fahad Ehsan
Supercapacitor plays a pivotal role as energy storage devices in the context of eliminating energy resources. Black Phosphorene (BP) is highly regarded as a potential electrode for supercapacitor (SC) because of its outstanding properties, including excellent carrier mobility and unique electronic properties. In this research work, the monolayer of BP and bilayer of BP (BP/BP) structure is investigated by using DFT. Moreover, the effect of doping and co-doping of non-metal (oxygen, nitrogen) in the mono- and bi-layer was also investigated to increase their performance by modulating the charge storage, and electronic properties of BP. The structural properties, density of states, quantum capacitance, surface charge density, bader charge analysis, isosurface charge density difference, integrated charge density of monolayer and bilayer are studied. The density functional theory (DFT) is used to calculate all above mention properties. DFT-D3 method with Becke-Johnson damping function is used as dispersion correction factor for all the calculations of bilayer. The calculated results find that bilayer structure gives better results as compared to monolayer structure. In this work, results also revealed that doping of oxygen and nitrogen atom significantly enhance the CQ and Q of mono- and bi-layer structure. For aqueous system, all the composites exhibited asymmetrical behavior except BP/BP bilayer. BP-N/BP-N (1369.8µC/cm2), and BP-O/BP-O (-1298.1µC/cm2) bilayer structure are best for anode and cathode material. In case of ionic/organic system, all composites showed asymmetrical behavior. BP-O/BP-O (-6053.5µC/cm2), and BP-N/BP-N (9329.8µC/cm2) bilayer structure is best cathode and anode material.
超级电容器作为一种储能设备，在消除能源资源方面发挥着举足轻重的作用。黑磷烯（BP）因其优异的性能，包括出色的载流子迁移率和独特的电子特性，被高度评价为超级电容器（SC）的潜在电极。在这项研究工作中，利用 DFT 研究了单层 BP 和双层 BP（BP/BP）结构。此外，还研究了在单层和双层中掺杂和共掺杂非金属（氧、氮）的影响，以通过调节 BP 的电荷存储和电子特性来提高其性能。研究了单层和双层的结构特性、状态密度、量子电容、表面电荷密度、巴德电荷分析、等表面电荷密度差、综合电荷密度。密度泛函理论（DFT）用于计算上述所有特性。双电层的所有计算都使用了带有贝克-约翰逊阻尼函数的 DFT-D3 方法作为分散校正因子。计算结果发现，与单层结构相比，双层结构的结果更好。这项工作的结果还显示，氧原子和氮原子的掺杂大大提高了单层和双层结构的 CQ 和 Q 值。在水体系中，除 BP/BP 双层结构外，所有复合材料都表现出不对称行为。BP-N/BP-N（1369.8µC/cm2）和 BP-O/BP-O （-1298.1µC/cm2）双层结构最适合作为阳极和阴极材料。在离子/有机体系中，所有复合材料都表现出不对称行为。BP-O/BP-O（-6053.5µC/cm2）和 BP-N/BP-N （9329.8µC/cm2）双层结构是最佳的阴极和阳极材料。
{"title":"Unraveling quantum capacitance of black phosphorene by the doping of non-metals for energy storage applications using DFT method","authors":"Sarfraz Ahmad , Muhammad Imran , Fayyaz Hussain , Niaz Ahmad Niaz , Ammar Mohamed Tighezza , R.M.A. Khalil , M. Irfan , Muhammad Fahad Ehsan","doi":"10.1016/j.surfin.2024.105187","DOIUrl":"10.1016/j.surfin.2024.105187","url":null,"abstract":"<div><div>Supercapacitor plays a pivotal role as energy storage devices in the context of eliminating energy resources. Black Phosphorene (BP) is highly regarded as a potential electrode for supercapacitor (SC) because of its outstanding properties, including excellent carrier mobility and unique electronic properties. In this research work, the monolayer of BP and bilayer of BP (BP/BP) structure is investigated by using DFT. Moreover, the effect of doping and co-doping of non-metal (oxygen, nitrogen) in the mono- and bi-layer was also investigated to increase their performance by modulating the charge storage, and electronic properties of BP. The structural properties, density of states, quantum capacitance, surface charge density, bader charge analysis, isosurface charge density difference, integrated charge density of monolayer and bilayer are studied. The density functional theory (DFT) is used to calculate all above mention properties. DFT-D3 method with Becke-Johnson damping function is used as dispersion correction factor for all the calculations of bilayer. The calculated results find that bilayer structure gives better results as compared to monolayer structure. In this work, results also revealed that doping of oxygen and nitrogen atom significantly enhance the C<sub>Q</sub> and Q of mono- and bi-layer structure. For aqueous system, all the composites exhibited asymmetrical behavior except BP/BP bilayer. BP-N/BP-N (1369.8µC/cm<sup>2</sup>), and BP-O/BP-O (-1298.1µC/cm<sup>2</sup>) bilayer structure are best for anode and cathode material. In case of ionic/organic system, all composites showed asymmetrical behavior. BP-O/BP-O (-6053.5µC/cm<sup>2</sup>), and BP-N/BP-N (9329.8µC/cm<sup>2</sup>) bilayer structure is best cathode and anode material.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424702","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 : 2024-09-28DOI: 10.1016/j.surfin.2024.105188
Rui Zhang , Wen Zhang , Qiuyu Zhu , Qinxue Nie , Saifeng Zhang , Yuhuan Zhang , Ren Liu , Yuanxu Liu , Xiangang Lin , Yangyang Li
Methods for the precise construction of NH2-MIL-125 (Ti) with chemical bonding are indispensable for the synthesis of MOF-based photocatalytic materials, which possess high activity, stability and biocompatibility. Herein, polydopamine (PDA)-functionalized NH2-MIL-125 (Ti) was prepared using cross-linking reaction between catechol groups in PDA and amine groups in NH2-MIL-125 (Ti), instead of the self-polymerization process. The conjugation of functional groups had strong chemical bonding interactions. Benefiting from the assembly of PDA, the optimum photocatalyst presented superior tetracycline (TC) degradation efficiency, as well as 99.9 % and 99.4 % antimicrobial rates against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), respectively. The possible photocatalytic mechanisms of TC degradation and antibacterial activity were proposed and verified by EPR results. This work provides in-depth scientific insights for photocatalysis and biomedical field.
{"title":"Engineering polydopamine-functionalized NH2-MIL-125 (Ti) for tetracycline degradation and antibacterial applications","authors":"Rui Zhang , Wen Zhang , Qiuyu Zhu , Qinxue Nie , Saifeng Zhang , Yuhuan Zhang , Ren Liu , Yuanxu Liu , Xiangang Lin , Yangyang Li","doi":"10.1016/j.surfin.2024.105188","DOIUrl":"10.1016/j.surfin.2024.105188","url":null,"abstract":"<div><div>Methods for the precise construction of NH<sub>2</sub>-MIL-125 (Ti) with chemical bonding are indispensable for the synthesis of MOF-based photocatalytic materials, which possess high activity, stability and biocompatibility. Herein, polydopamine (PDA)-functionalized NH<sub>2</sub>-MIL-125 (Ti) was prepared using cross-linking reaction between catechol groups in PDA and amine groups in NH<sub>2</sub>-MIL-125 (Ti), instead of the self-polymerization process. The conjugation of functional groups had strong chemical bonding interactions. Benefiting from the assembly of PDA, the optimum photocatalyst presented superior tetracycline (TC) degradation efficiency, as well as 99.9 % and 99.4 % antimicrobial rates against Escherichia coli (<em>E. coli</em>) and Staphylococcus aureus (<em>S. aureus</em>), respectively. The possible photocatalytic mechanisms of TC degradation and antibacterial activity were proposed and verified by EPR results. This work provides in-depth scientific insights for photocatalysis and biomedical field.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142424181","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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