Surfaces and Interfaces最新文献_第7页

The electrochemical synthesis of urea on triatomic cluster/Cu catalysts: A theoretical study 在三原子团簇/铜催化剂上电化学合成尿素：理论研究

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105349

Qiang Liu , Jingnan Wang , Yongan Yang , Xi Wang

Urea (NH₂CONH₂), a crucial nitrogen fertilizer and industrial raw material, is typically synthesized under rigorous reaction conditions. Currently, the electrocatalytic transformation of N₂ and CO₂ into urea is a promising strategy. However, finding a high-selectivity and high-activity catalyst remains a significant challenge. Herein, the activity of a series of transition metal clusters (VIII and IB groups) on copper-based catalysts for electrochemical coupling of CO₂ and N₂ has been systematically studied to produce urea via density functional theory (DFT). Most catalysts exhibit good thermodynamic stability and accomplish co-adsorb CO₂ and N₂. Notably, Fe3 and Ni3/Cu100 catalysts achieve C-N coupling via *CO and *N₂, whereas Ru3, Rh3, Os3, and Ir3/Cu100 catalysts accomplish C-N coupling via *CO and *NHNH. Among all catalysts, the Ni3/Cu100 catalyst features excellent catalytic activity with a rate-determining step as low as 0.480 eV, and its C-N coupling only needs to overcome a barrier of 0.844 eV. Additionally, the Ni3/Cu100 catalyst can effectively inhibit the hydrogen evolution reaction (HER), further protonation of *CO and ammonia formation, thereby ensuring high selectivity for urea. Electronic structures analysis further reveals an “acceptance-donation” mechanism for the activation of *CO₂ and *N₂, with the introduction of the Ni3 cluster showing a decisive role. Therefore, this study may establish the foundation for the electrochemical synthesis of urea.

尿素（NH2CONH2）是一种重要的氮肥和工业原料，通常在严格的反应条件下合成。目前，通过电催化将 N2 和 CO2 转化为尿素是一种很有前景的策略。然而，寻找一种高选择性和高活性催化剂仍是一项重大挑战。在此，我们通过密度泛函理论（DFT）系统地研究了铜基催化剂上的一系列过渡金属团簇（VIII 和 IB 基团）在 CO2 和 N2 电化学偶联生成尿素过程中的活性。大多数催化剂都表现出良好的热力学稳定性，并能完成 CO2 和 N2 的共吸附。值得注意的是，Fe3 和 Ni3/Cu100 催化剂通过 *CO 和 *N2 实现 C-N 偶联，而 Ru3、Rh3、Os3 和 Ir3/Cu100 催化剂则通过 *CO 和 *NHNH 实现 C-N 偶联。在所有催化剂中，Ni3/Cu100 催化剂具有出色的催化活性，其速率决定阶跃低至 0.480 eV，其 C-N 偶联只需克服 0.844 eV 的势垒。此外，Ni3/Cu100 催化剂还能有效抑制氢进化反应（HER）、*CO 的进一步质子化和氨的生成，从而确保尿素的高选择性。电子结构分析进一步揭示了*CO2 和*N2 活化的 "接受-捐献 "机制，其中 Ni3 团簇的引入起了决定性作用。因此，这项研究可为尿素的电化学合成奠定基础。

{"title":"The electrochemical synthesis of urea on triatomic cluster/Cu catalysts: A theoretical study","authors":"Qiang Liu , Jingnan Wang , Yongan Yang , Xi Wang","doi":"10.1016/j.surfin.2024.105349","DOIUrl":"10.1016/j.surfin.2024.105349","url":null,"abstract":"<div><div>Urea (NH<sub>2</sub>CONH<sub>2</sub>), a crucial nitrogen fertilizer and industrial raw material, is typically synthesized under rigorous reaction conditions. Currently, the electrocatalytic transformation of N<sub>2</sub> and CO<sub>2</sub> into urea is a promising strategy. However, finding a high-selectivity and high-activity catalyst remains a significant challenge. Herein, the activity of a series of transition metal clusters (VIII and IB groups) on copper-based catalysts for electrochemical coupling of CO<sub>2</sub> and N<sub>2</sub> has been systematically studied to produce urea via density functional theory (DFT). Most catalysts exhibit good thermodynamic stability and accomplish co-adsorb CO<sub>2</sub> and N<sub>2</sub>. Notably, Fe3 and Ni3/Cu100 catalysts achieve C-N coupling via *CO and *N<sub>2</sub>, whereas Ru3, Rh3, Os3, and Ir3/Cu100 catalysts accomplish C-N coupling via *CO and *NHNH. Among all catalysts, the Ni3/Cu100 catalyst features excellent catalytic activity with a rate-determining step as low as 0.480 eV, and its C-N coupling only needs to overcome a barrier of 0.844 eV. Additionally, the Ni3/Cu100 catalyst can effectively inhibit the hydrogen evolution reaction (HER), further protonation of *CO and ammonia formation, thereby ensuring high selectivity for urea. Electronic structures analysis further reveals an “acceptance-donation” mechanism for the activation of *CO<sub>2</sub> and *N<sub>2</sub>, with the introduction of the Ni3 cluster showing a decisive role. Therefore, this study may establish the foundation for the electrochemical synthesis of urea.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105349"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552359","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}

引用次数: 0

Rapid preparation of N,P co-doped carbon for advanced oxidative degradation of wastewater 快速制备用于废水高级氧化降解的 N、P 共掺杂碳

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105347

Weining Li , Xiaping Lu , Jiakang Li , Yingchun Yan , Junfeng Li , Kun Chen , Aijun Guo , He Liu , Dong Liu

Heteroatom-doped porous carbon materials are highly favored as catalysts for activating persulfates in the oxidative degradation of organic pollutants due to their low metal leaching risk and cost-effectiveness. Nonetheless, the complex process of creating heteroatom-doped carbon materials often results in suboptimal doping effects. This study uses N,P-enriched plants (Eichhornia crassipes after being used for nutrient-rich water remediation) as a raw material to prepare N-P co-doped catalysts in a single step. We thoroughly investigated their performance and mechanisms in dye degradation. The findings demonstrated that the adsorbent, with its rich pore structures, surface chemical functional groups, and graphite defect structures, could completely degrade a 100 mg L⁻¹ MB solution within 20 min. Free radical quenching experiments and EPR analysis confirmed the presence of •OH, SO₄^•—, O₂^•— and ¹O₂, verifying their oxidative contributions. Moreover, it was determined that the non-radical pathway (¹O₂ oxidation) primarily drives the oxidative degradation in this system. Additionally, tests using a small-scale fixed-bed reactor and interference resistance highlighted the practical application potential of the adsorbent developed in this study. This study not only offers a dual solution for tackling nutrient enrichment and organic pollution in water bodies but also introduces a straightforward method for preparing N, P co-doped catalysts, significantly benefiting environmental protection.

掺杂杂原子的多孔碳材料因其金属沥滤风险低和成本效益高，在有机污染物的氧化降解过程中作为活化过硫酸盐的催化剂备受青睐。然而，杂原子掺杂碳材料的复杂制备过程往往会导致掺杂效果不理想。本研究以富含 N、P 的植物（用于富营养化水体修复后的 Eichhornia crassipes）为原料，一步制备出 N-P 共掺催化剂。我们深入研究了它们在染料降解过程中的性能和机理。研究结果表明，该吸附剂具有丰富的孔隙结构、表面化学官能团和石墨缺陷结构，可在 20 分钟内完全降解 100 mg L-1 的甲基溴溶液。自由基淬灭实验和 EPR 分析证实了 -OH、SO4--、O2-- 和 1O2 的存在，验证了它们的氧化作用。此外，还确定非自由基途径（1O2 氧化）是该系统中氧化降解的主要驱动力。此外，使用小规模固定床反应器和抗干扰性能进行的测试凸显了本研究开发的吸附剂的实际应用潜力。本研究不仅为解决水体中营养物质富集和有机物污染问题提供了双重解决方案，还介绍了制备 N、P 共掺催化剂的简单方法，极大地促进了环境保护。

{"title":"Rapid preparation of N,P co-doped carbon for advanced oxidative degradation of wastewater","authors":"Weining Li , Xiaping Lu , Jiakang Li , Yingchun Yan , Junfeng Li , Kun Chen , Aijun Guo , He Liu , Dong Liu","doi":"10.1016/j.surfin.2024.105347","DOIUrl":"10.1016/j.surfin.2024.105347","url":null,"abstract":"<div><div>Heteroatom-doped porous carbon materials are highly favored as catalysts for activating persulfates in the oxidative degradation of organic pollutants due to their low metal leaching risk and cost-effectiveness. Nonetheless, the complex process of creating heteroatom-doped carbon materials often results in suboptimal doping effects. This study uses N,P-enriched plants (Eichhornia crassipes after being used for nutrient-rich water remediation) as a raw material to prepare N-P co-doped catalysts in a single step. We thoroughly investigated their performance and mechanisms in dye degradation. The findings demonstrated that the adsorbent, with its rich pore structures, surface chemical functional groups, and graphite defect structures, could completely degrade a 100 mg L<sup>−1</sup> MB solution within 20 min. Free radical quenching experiments and EPR analysis confirmed the presence of •OH, SO<sub>4</sub><sup>•—</sup>, O<sub>2</sub><sup>•—</sup> and <sup>1</sup>O<sub>2</sub>, verifying their oxidative contributions. Moreover, it was determined that the non-radical pathway (<sup>1</sup>O<sub>2</sub> oxidation) primarily drives the oxidative degradation in this system. Additionally, tests using a small-scale fixed-bed reactor and interference resistance highlighted the practical application potential of the adsorbent developed in this study. This study not only offers a dual solution for tackling nutrient enrichment and organic pollution in water bodies but also introduces a straightforward method for preparing N, P co-doped catalysts, significantly benefiting environmental protection.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105347"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594132","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}

引用次数: 0

Water collection through a directional leaf vein pattern by fast laser marker ablation of stainless-steel 利用快速激光标记烧蚀不锈钢，通过定向叶脉图案集水

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105332

Hongtao Cui, Xiaolong Fang, Xiaowen Qi, Chengling Liu, Youfu Wang, Xiangfu Chen, Chenrui Wang

Inspired by the natural water harvesting mechanisms of desert beetles, cactus thorns, and leaf veins, we designed a heterogeneous wettability surface with superhydrophilic pattern integrating leaf vein as the directional water transport main channel, attached capillary triangles as auxiliary channel plus a deep rough desorption channel on an overall superhydrophobic surface for an efficient water collection. A superhydrophilic surface was initially fabricated on the stainless steel disc by laser marker ablation allowing 1 μL droplet to spread completely to 0° within 0.12 s, followed by fluorine-containing coating transforming superhydrophilic surface to superhydrophobic one. Directional water transport patterns were then etched on the superhydrophobic surfaces by the secondary laser marker. The surface energy gradient and Laplace pressure induced by the pattern facilitated directional fast transport and efficient desorption of droplets, thus improving water collection efficiency. The enhancement mechanism of the water harvesting behavior for such surfaces was analyzed, with one focus on enhancing collection in hydrophobic regions with capillaries to reduce bouncing off loss and the other on improving balanced cycling of the collection process. At a fog flow rate of 1500 ml/h and 20 cm away from the fog outlet, the directional leaf vein-patterned 19.625 cm² sized surface demonstrated a fog water collection rate (WCR) of 5.6 Kg·m^-2·h^-1 and first drop collection at the 49th s, an impressively short time rarely reported. Compared to the superhydrophobic, superhydrophilic samples, and the reference, WCR increased by 180 %, 62 %, and 59 %, respectively, and the first droplet collection time decreased by 73 %, 46 %, and 62 %, respectively. This efficient water collection method has huge potential in arid regions.

受沙漠甲虫、仙人掌刺和叶脉等自然集水机制的启发，我们设计了一种具有超亲水性图案的异质润湿表面，将叶脉作为定向输水主通道，附着的毛细三角形作为辅助通道，并在整体超疏水表面上设计了一个深层粗糙解吸通道，以实现高效集水。首先通过激光标记烧蚀在不锈钢圆盘上形成超亲水表面，使 1 μL 水滴在 0.12 秒内完全扩散到 0°，然后通过含氟涂层将超亲水表面转化为超疏水表面。然后用二次激光标记在超疏水表面蚀刻出定向水传输图案。图案引起的表面能量梯度和拉普拉斯压力促进了水滴的定向快速传输和高效解吸，从而提高了集水效率。我们分析了这种表面集水行为的增强机制，其中一个重点是通过毛细管增强疏水区域的集水效果，以减少反弹损失，另一个重点是改进集水过程的平衡循环。在雾流量为 1500 毫升/小时、距离雾出口 20 厘米的条件下，19.625 平方厘米大小的定向叶脉图案表面的雾水收集率（WCR）为 5.6 Kg-m-2-h-1，在第 49 秒时收集到第一滴水珠，这一时间之短令人印象深刻，鲜有报道。与超疏水样品、超亲水样品和参照物相比，雾水收集率分别提高了 180%、62% 和 59%，第一滴收集时间分别缩短了 73%、46% 和 62%。这种高效的集水方法在干旱地区具有巨大的潜力。

{"title":"Water collection through a directional leaf vein pattern by fast laser marker ablation of stainless-steel","authors":"Hongtao Cui, Xiaolong Fang, Xiaowen Qi, Chengling Liu, Youfu Wang, Xiangfu Chen, Chenrui Wang","doi":"10.1016/j.surfin.2024.105332","DOIUrl":"10.1016/j.surfin.2024.105332","url":null,"abstract":"<div><div>Inspired by the natural water harvesting mechanisms of desert beetles, cactus thorns, and leaf veins, we designed a heterogeneous wettability surface with superhydrophilic pattern integrating leaf vein as the directional water transport main channel, attached capillary triangles as auxiliary channel plus a deep rough desorption channel on an overall superhydrophobic surface for an efficient water collection. A superhydrophilic surface was initially fabricated on the stainless steel disc by laser marker ablation allowing 1 μL droplet to spread completely to 0° within 0.12 s, followed by fluorine-containing coating transforming superhydrophilic surface to superhydrophobic one. Directional water transport patterns were then etched on the superhydrophobic surfaces by the secondary laser marker. The surface energy gradient and Laplace pressure induced by the pattern facilitated directional fast transport and efficient desorption of droplets, thus improving water collection efficiency. The enhancement mechanism of the water harvesting behavior for such surfaces was analyzed, with one focus on enhancing collection in hydrophobic regions with capillaries to reduce bouncing off loss and the other on improving balanced cycling of the collection process. At a fog flow rate of 1500 ml/h and 20 cm away from the fog outlet, the directional leaf vein-patterned 19.625 cm<sup>2</sup> sized surface demonstrated a fog water collection rate (WCR) of 5.6 Kg·m<sup>-2</sup>·h<sup>-1</sup> and first drop collection at the 49th s, an impressively short time rarely reported. Compared to the superhydrophobic, superhydrophilic samples, and the reference, WCR increased by 180 %, 62 %, and 59 %, respectively, and the first droplet collection time decreased by 73 %, 46 %, and 62 %, respectively. This efficient water collection method has huge potential in arid regions.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105332"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552302","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}

引用次数: 0

Recent advances in flexible/stretchable sensors using laser-induced three-dimensional porous graphene: From precursor to manufacturing 使用激光诱导三维多孔石墨烯的柔性/可拉伸传感器的最新进展：从前驱体到制造

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105359

Jiyuan Sun, Ziqiang Chen, Linfeng Yuan, Junyan Xiang, Wentao Wang

Graphene is an ideal material for flexible sensors with outstanding stretchability and extensibility, but its further development is being severely hindered by the existing multi-step routes. Laser-induced graphene (LIG) is a recently emerging technology that enables industrial scale preparation with mask-free, fast-scanning speed, and high spatial resolution. In this review, the latest advances on three-dimensional porous LIG from the perspective of precursor selections to manufacturing methods are presented. First, the commonly precursors such as graphene oxide, polymers, and natural materials for photothermal/chemical transformation was classified in combined with auxiliary processing equipment. Then, three all-purpose fabrication strategies, including casting-and-peeling transfer, topology architecture and Kirigami design, are summarized for the LIG-based sensors. Next, the representative progress of flexible/stretchable LIG-based pressure, strain, liquid, and gas sensors were categorized based on sensing principles, with the aim of improving the sensing performance in practical applications. Finally, the newest developments, major challenges, and outlook in LIG-manufacturing and integrated flexible sensors are discussed, showing huge potential in future wearable electronics.

石墨烯是柔性传感器的理想材料，具有出色的拉伸性和延伸性，但现有的多步骤制备方法严重阻碍了石墨烯的进一步发展。激光诱导石墨烯（LIG）是最近兴起的一种技术，可实现无掩膜、快速扫描和高空间分辨率的工业规模制备。本综述从前驱体选择到制造方法的角度，介绍了三维多孔石墨烯的最新进展。首先，结合辅助加工设备对氧化石墨烯、聚合物、光热/化学转化天然材料等常用前驱体进行了分类。然后，总结了基于 LIG 的传感器的三种通用制造策略，包括浇铸-剥离转移、拓扑结构和 Kirigami 设计。接着，根据传感原理对基于 LIG 的柔性/可拉伸压力、应变、液体和气体传感器的代表性进展进行了分类，旨在提高实际应用中的传感性能。最后，讨论了 LIG 制造和集成柔性传感器的最新发展、主要挑战和前景，展示了未来可穿戴电子产品的巨大潜力。

{"title":"Recent advances in flexible/stretchable sensors using laser-induced three-dimensional porous graphene: From precursor to manufacturing","authors":"Jiyuan Sun, Ziqiang Chen, Linfeng Yuan, Junyan Xiang, Wentao Wang","doi":"10.1016/j.surfin.2024.105359","DOIUrl":"10.1016/j.surfin.2024.105359","url":null,"abstract":"<div><div>Graphene is an ideal material for flexible sensors with outstanding stretchability and extensibility, but its further development is being severely hindered by the existing multi-step routes. Laser-induced graphene (LIG) is a recently emerging technology that enables industrial scale preparation with mask-free, fast-scanning speed, and high spatial resolution. In this review, the latest advances on three-dimensional porous LIG from the perspective of precursor selections to manufacturing methods are presented. First, the commonly precursors such as graphene oxide, polymers, and natural materials for photothermal/chemical transformation was classified in combined with auxiliary processing equipment. Then, three all-purpose fabrication strategies, including casting-and-peeling transfer, topology architecture and Kirigami design, are summarized for the LIG-based sensors. Next, the representative progress of flexible/stretchable LIG-based pressure, strain, liquid, and gas sensors were categorized based on sensing principles, with the aim of improving the sensing performance in practical applications. Finally, the newest developments, major challenges, and outlook in LIG-manufacturing and integrated flexible sensors are discussed, showing huge potential in future wearable electronics.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105359"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552021","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}

引用次数: 0

Purification of textile wastewater by collective degradation using nanorods of cesium titanium bromide (CsTiBr3) perovskite 使用纳米棒状过磷酸盐铯钛溴化物 (CsTiBr3) 通过集体降解净化纺织废水

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105358

K A Benazeera Beegum , Suvarna Ganesh , Chinnu Sabu , Alene Sara Varghese , Aiswarya A S , Christeena Thomas , Saranya Sasi , Alex Mathew , Anumol Jose , Reshmi Raman

The present work recommends a sustainable environmentally safe method for the removal of textile dyes in an economically viable way.The wastewater expelled from the textile dying units contains a mixture of dyes. Here we address the challenge of using a single catalyst for the collective photocatalytic degradation of mixture of six dyes and two samples of textile effluents collected from a local dying unit under direct sunlight. The lead-free perovskite of CsTiBr₃ nanorods prepared via the solvothermal process is effective in the collective photocatalytic degradation of dye mixture containing toxic dyes like congo red, crystal violet, malachite green, methylene blue, rhodamine, and methyl orange. The six-dye mixture turned colorless within three hours of direct sunlight exposure. The collective photocatalytic degradation ability of CsTiBr₃ perovskite nanorods is successfully exploited for the degradation of the textile effluents. The chemical oxygen demand (COD) analysis guarantees the degradation of dye into non-toxic components. The recycling of wastewater is made possible by the removal of CsTiBr₃ catalysts through adsorption using biochar derived from invasive plants. The biochars are extracted from invasive plants such as Acrostichum Aureum, Alternanthera bettzickiana, cyclosorus interrupts, and Quisqualis indica in which Acrostichum Aureum showed maximum adsorption. The scavenger studies using isopropyl alcohol (IPA), ethylene diamine tetra acetic acid (EDTA), and silver nitrate (AgNO₃) suggest that holes control the photocatalysis mechanism.

从纺织品染色单位排出的废水中含有多种染料混合物。在这里，我们要解决的难题是使用单一催化剂在阳光直射下集体光催化降解从当地染厂收集的六种染料混合物和两种纺织废水样品。通过溶热法制备的 CsTiBr3 纳米棒无铅过氧化物能有效地对含有刚果红、水晶紫、孔雀石绿、亚甲基蓝、罗丹明和甲基橙等有毒染料的染料混合物进行集体光催化降解。六种染料混合物在阳光直射三小时内变成无色。CsTiBr3 包晶纳米棒的集体光催化降解能力被成功地用于降解纺织污水。化学需氧量（COD）分析保证了染料降解为无毒成分。利用从入侵植物中提取的生物炭，通过吸附去除 CsTiBr3 催化剂，实现了废水的循环利用。这些生物炭是从一些入侵植物中提取的，如 Acrostichum Aureum、Alternanthera bettzickiana、cyclosorus interrupts 和 Quisqualis indica，其中 Acrostichum Aureum 的吸附量最大。使用异丙醇（IPA）、乙二胺四乙酸（EDTA）和硝酸银（AgNO3）进行的清除剂研究表明，空穴控制着光催化机制。

{"title":"Purification of textile wastewater by collective degradation using nanorods of cesium titanium bromide (CsTiBr3) perovskite","authors":"K A Benazeera Beegum , Suvarna Ganesh , Chinnu Sabu , Alene Sara Varghese , Aiswarya A S , Christeena Thomas , Saranya Sasi , Alex Mathew , Anumol Jose , Reshmi Raman","doi":"10.1016/j.surfin.2024.105358","DOIUrl":"10.1016/j.surfin.2024.105358","url":null,"abstract":"<div><div>The present work recommends a sustainable environmentally safe method for the removal of textile dyes in an economically viable way.The wastewater expelled from the textile dying units contains a mixture of dyes. Here we address the challenge of using a single catalyst for the collective photocatalytic degradation of mixture of six dyes and two samples of textile effluents collected from a local dying unit under direct sunlight. The lead-free perovskite of CsTiBr<sub>3</sub> nanorods prepared via the solvothermal process is effective in the collective photocatalytic degradation of dye mixture containing toxic dyes like congo red, crystal violet, malachite green, methylene blue, rhodamine, and methyl orange. The six-dye mixture turned colorless within three hours of direct sunlight exposure. The collective photocatalytic degradation ability of CsTiBr<sub>3</sub> perovskite nanorods is successfully exploited for the degradation of the textile effluents. The chemical oxygen demand (COD) analysis guarantees the degradation of dye into non-toxic components. The recycling of wastewater is made possible by the removal of CsTiBr<sub>3</sub> catalysts through adsorption using biochar derived from invasive plants. The biochars are extracted from invasive plants such as <em>Acrostichum Aureum, Alternanthera bettzickiana, cyclosorus interrupts, and Quisqualis indica</em> in which Acrostichum Aureum showed maximum adsorption<em>.</em> The scavenger studies using isopropyl alcohol (IPA), ethylene diamine tetra acetic acid (EDTA), and silver nitrate (AgNO<sub>3</sub>) suggest that holes control the photocatalysis mechanism.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105358"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571674","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}

引用次数: 0

Morphological evolution mechanism of microstructures involved in shaping micro-pillar arrays into microlens arrays on fused silica surfaces by CO2 laser polishing 通过二氧化碳激光抛光将熔融石英表面的微柱阵列塑造成微透镜阵列的微结构形态演变机制

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105333

Zixiao Zhang , Qiang Zhao , Zhaoyang Yin , Jian Cheng , Hongqin Lei , Xinxin He , Linjie Zhao , Mingjun Chen , Jinghe Wang , Tianhao Zhang

The periodic micro-pillars on the hard-brittle fused silica surface can be shaped into the smooth and defect-free microlens arrays (MLA) by CO₂ laser polishing, which can be applied in imaging and beam-shaping. However, the morphology evolution mechanism of the micro-pillars is not clear during polishing, which seriously affects the rapid preparation of high-quality MLAs. Herein, a multi-physics coupling model is established to investigate the interaction between CO₂ lasers and micro-pillars on the fused silica surface, and is verified from the perspectives of temporal and spatial temperature. The steady surface temperature evolution law with laser power and spot radius is explored, based on which, the parameter ‘Window’ for polishing is determined to make the material melt and flow without ablation removal. The morphology evolution of micro-pillars is investigated as well as laser-material interaction. It is found that under laser irradiation, the micro-pillar height first increases and then decreases, and its top curvature radius increases. The surface tension makes the dominant contributions to the melting and flow of the micro-pillar materials, while the Marangoni effect and the gravity have little effect. Furthermore, to fabricate the target MLAs with the specific dimensions, the influence of micro-pillar aspect ratio (φ) on microlens surface morphology is investigated. It is found that there are two critical φ for the target MLAs. For the required MLA with the target period of 200 μm and the target height of 40 μm, when the φ is larger than 5.1, the micro-pillar array fails to be shaped into the target MLA by CO₂ laser polishing. As the φ decreases, the junction of micro-pillar and the substrate sags downwards significantly, and the deviation between the shaped- and the ideal spherical contours increases. To successfully prepared the target MLA and guarantee the geometry accuracy, the minimum φ is selected to be 0.71. This work has important theoretical significance for obtaining the smooth and defect-free target fused silica MLAs with the specific dimensions by CO₂ laser non-evaporative polishing.

硬脆熔融石英表面上的周期性微柱可通过二氧化碳激光抛光形成光滑无缺陷的微透镜阵列（MLA），从而应用于成像和光束整形。然而，抛光过程中微柱的形貌演变机制并不清晰，这严重影响了高质量微透镜阵列的快速制备。本文建立了一个多物理场耦合模型来研究 CO2 激光与熔融石英表面微柱之间的相互作用，并从时间和空间温度的角度进行了验证。探究了表面温度随激光功率和光斑半径的稳定演变规律，并据此确定了抛光参数 "Window"，使材料熔化并流动而不被烧蚀去除。研究了微柱的形态演变以及激光与材料的相互作用。研究发现，在激光照射下，微柱高度先增大后减小，其顶部曲率半径增大。微柱材料的熔化和流动主要受表面张力的影响，而马兰戈尼效应和重力的影响很小。此外，为了制造具有特定尺寸的目标 MLA，还研究了微柱长宽比（φ）对微透镜表面形态的影响。研究发现，目标 MLA 有两个临界 φ。对于目标周期为 200 μm、目标高度为 40 μm 的所需 MLA，当 φ 大于 5.1 时，微柱阵列无法通过 CO2 激光抛光成型为目标 MLA。随着 φ 的减小，微柱与基板的交界处明显向下凹陷，成型轮廓与理想球形轮廓之间的偏差增大。为了成功制备目标 MLA 并保证几何精度，选择最小 φ 为 0.71。这项工作对于通过 CO2 激光非蒸发抛光获得光滑、无缺陷、具有特定尺寸的目标熔融石英 MLA 具有重要的理论意义。

{"title":"Morphological evolution mechanism of microstructures involved in shaping micro-pillar arrays into microlens arrays on fused silica surfaces by CO2 laser polishing","authors":"Zixiao Zhang , Qiang Zhao , Zhaoyang Yin , Jian Cheng , Hongqin Lei , Xinxin He , Linjie Zhao , Mingjun Chen , Jinghe Wang , Tianhao Zhang","doi":"10.1016/j.surfin.2024.105333","DOIUrl":"10.1016/j.surfin.2024.105333","url":null,"abstract":"<div><div>The periodic micro-pillars on the hard-brittle fused silica surface can be shaped into the smooth and defect-free microlens arrays (MLA) by CO<sub>2</sub> laser polishing, which can be applied in imaging and beam-shaping. However, the morphology evolution mechanism of the micro-pillars is not clear during polishing, which seriously affects the rapid preparation of high-quality MLAs. Herein, a multi-physics coupling model is established to investigate the interaction between CO<sub>2</sub> lasers and micro-pillars on the fused silica surface, and is verified from the perspectives of temporal and spatial temperature. The steady surface temperature evolution law with laser power and spot radius is explored, based on which, the parameter ‘Window’ for polishing is determined to make the material melt and flow without ablation removal. The morphology evolution of micro-pillars is investigated as well as laser-material interaction. It is found that under laser irradiation, the micro-pillar height first increases and then decreases, and its top curvature radius increases. The surface tension makes the dominant contributions to the melting and flow of the micro-pillar materials, while the Marangoni effect and the gravity have little effect. Furthermore, to fabricate the target MLAs with the specific dimensions, the influence of micro-pillar aspect ratio (<em>φ</em>) on microlens surface morphology is investigated. It is found that there are two critical <em>φ</em> for the target MLAs. For the required MLA with the target period of 200 μm and the target height of 40 μm, when the <em>φ</em> is larger than 5.1, the micro-pillar array fails to be shaped into the target MLA by CO<sub>2</sub> laser polishing. As the <em>φ</em> decreases, the junction of micro-pillar and the substrate sags downwards significantly, and the deviation between the shaped- and the ideal spherical contours increases. To successfully prepared the target MLA and guarantee the geometry accuracy, the minimum <em>φ</em> is selected to be 0.71. This work has important theoretical significance for obtaining the smooth and defect-free target fused silica MLAs with the specific dimensions by CO<sub>2</sub> laser non-evaporative polishing.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105333"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552362","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}

引用次数: 0

Efficient removal of Congo red from aqueous solutions using calcined and uncalcined MgZnFe ternary layered double hydroxide (LDH) 利用煅烧和未煅烧的镁锌铁三元层状双氢氧化物（LDH）高效去除水溶液中的刚果红

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105341

Amit Bar , Sanjeev Kumar , Sudarshan Sarkar , Ram Sharan Singh , Chandan Upadhyay

This study investigates the textile industries' dye Congo-red removal from aqueous solution using the calcined and uncalcined

[M g_{0.5}^{2 +} Z n_{0.25}^{2 +} F e_{0.25}^{3 +} {(O H)}_{2}] . {(C O_{3}^{2 -})}_{0.125} . H_{2} O

ternary layered double hydroxide (LDH). XRD confirms the successful formation of the crystalline structure of LDH. FTIR analysis shows that the peak position at 1108 cm⁻¹, which indicates the presence of S = O group. TEM analysis reveals the formation of a hexagonal shape morphology, whereas BET measurements demonstrate an improvement in surface area after calcination. This study analyzed dye adsorption, which is affected by interaction time, solution pH, and adsorbent dosage. The adsorption data is analyzed using the Langmuir isotherm and Freundlich isotherm, while the kinetics data is analyzed using pseudo-first-order, pseudo-second-order, and intraparticle diffusion models. The change in enthalpy (ΔH₀) being positive and the change in Gibbs free energy (ΔG₀) being negative designates that the adsorption process is endothermic and occurs spontaneously. The Langmuir isotherm model analyzed the adsorption isotherm data and calculated the amount of adsorbate adsorbed by adsorbent. The maximum amount of Congo-red adsorbed by calcined and uncalcined layered double hydroxide are 205.76 and 89.76 mg g^-1. These results suggested that calcined layered double hydroxide is a significant adsorbent for removing effluents from wastewater.

本研究利用煅烧和未煅烧的[Mg0.52+Zn0.252+Fe0.253+(OH)2].(CO32-)0.125.H2O 三元层状双氢氧化物（LDH）研究了从水溶液中去除纺织工业染料刚果红的问题。XRD 证实了 LDH 晶体结构的成功形成。傅立叶变换红外光谱（FTIR）分析表明，1108 cm-1 处出现了峰值，这表明存在 S = O 基团。TEM 分析显示形成了六角形的形态，而 BET 测量则表明煅烧后表面积有所改善。本研究分析了染料吸附受相互作用时间、溶液 pH 值和吸附剂用量的影响。吸附数据采用 Langmuir 等温线和 Freundlich 等温线进行分析，动力学数据则采用伪一阶、伪二阶和颗粒内扩散模型进行分析。焓的变化（ΔH0）为正值，吉布斯自由能的变化（ΔG0）为负值，说明吸附过程是自发的内热过程。朗缪尔等温线模型分析了吸附等温线数据，并计算出吸附剂吸附的吸附剂量。煅烧和未煅烧的层状双氢氧化物对刚果红的最大吸附量分别为 205.76 和 89.76 mg g-1。这些结果表明，煅烧过的层状双氢氧化物是一种去除废水中废水的重要吸附剂。

{"title":"Efficient removal of Congo red from aqueous solutions using calcined and uncalcined MgZnFe ternary layered double hydroxide (LDH)","authors":"Amit Bar , Sanjeev Kumar , Sudarshan Sarkar , Ram Sharan Singh , Chandan Upadhyay","doi":"10.1016/j.surfin.2024.105341","DOIUrl":"10.1016/j.surfin.2024.105341","url":null,"abstract":"<div><div>This study investigates the textile industries' dye Congo-red removal from aqueous solution using the calcined and uncalcined <span><math><mrow><mrow><mo>[</mo><mrow><mi>M</mi><msubsup><mi>g</mi><mrow><mn>0.5</mn></mrow><mrow><mn>2</mn><mo>+</mo></mrow></msubsup><mi>Z</mi><msubsup><mi>n</mi><mrow><mn>0.25</mn></mrow><mrow><mn>2</mn><mo>+</mo></mrow></msubsup><mi>F</mi><msubsup><mi>e</mi><mrow><mn>0.25</mn></mrow><mrow><mn>3</mn><mo>+</mo></mrow></msubsup><msub><mrow><mo>(</mo><mrow><mi>O</mi><mi>H</mi></mrow><mo>)</mo></mrow><mn>2</mn></msub></mrow><mo>]</mo></mrow><mo>.</mo><msub><mrow><mo>(</mo><mrow><mi>C</mi><msubsup><mi>O</mi><mn>3</mn><mrow><mn>2</mn><mo>−</mo></mrow></msubsup></mrow><mo>)</mo></mrow><mrow><mn>0.125</mn></mrow></msub><mo>.</mo><msub><mi>H</mi><mn>2</mn></msub><mi>O</mi></mrow></math></span> ternary layered double hydroxide (LDH). XRD confirms the successful formation of the crystalline structure of LDH. FTIR analysis shows that the peak position at 1108 <em>cm</em><sup>−1</sup>, which indicates the presence of <em>S</em> = <em>O</em> group. TEM analysis reveals the formation of a hexagonal shape morphology, whereas BET measurements demonstrate an improvement in surface area after calcination. This study analyzed dye adsorption, which is affected by interaction time, solution pH, and adsorbent dosage. The adsorption data is analyzed using the Langmuir isotherm and Freundlich isotherm, while the kinetics data is analyzed using pseudo-first-order, pseudo-second-order, and intraparticle diffusion models. The change in enthalpy (Δ<em>H</em><sub>0</sub>) being positive and the change in Gibbs free energy (Δ<em>G</em><sub>0</sub>) being negative designates that the adsorption process is endothermic and occurs spontaneously. The Langmuir isotherm model analyzed the adsorption isotherm data and calculated the amount of adsorbate adsorbed by adsorbent. The maximum amount of Congo-red adsorbed by calcined and uncalcined layered double hydroxide are 205.76 and 89.76 mg g<sup>-1</sup>. These results suggested that calcined layered double hydroxide is a significant adsorbent for removing effluents from wastewater.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105341"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594134","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}

引用次数: 0

Femtosecond laser-induced plasma-assisted backward deposition of robustly adherent porous carbon films on glass substrates 飞秒激光诱导等离子体辅助在玻璃基底上反向沉积牢固附着的多孔碳薄膜

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105304

Sheng Peng , Junjie Zou , Tangyang Pu , Heng Wang , Ruonan Wang , Xiaoyu Tian , Sheng Liu , Qiang Cao

The simple and rapid production and transfer of high-quality carbon materials are crucial for the flexible and efficient fabrication of carbon-based electronic devices. Recently, a laser-assisted transfer method combining laser-induced carbonization and transfer printing was demonstrated for the one-step preparation and transfer of patterned laser-induced carbon films to transparent substrates. However, this method is limited by insufficient robustness and weak adhesion of the carbon film post-transfer. Herein, we developed a non-contact laser-induced plasma-assisted deposition method to deposit robustly adherent porous carbon films on glass substrates. By well-adjusting the laser parameters and inserting spacers with adjustable thickness, laser-induced plasma ablation replaced direct laser ablation during femtosecond laser scanning of the substrate-polyimide-carrier sandwich structure, resulting in micro-channels with a carbon-glass recast layer instead of easily peelable flakes on the glass substrate. This hierarchical structure significantly enhances the adhesion between the laser-induced carbon film and the glass substrate, ensuring outstanding stability of the deposited carbon film under various adhesion tests. Furthermore, compared to carbon films prepared by the laser-assisted transfer method, the obtained carbon films are hydrophilic, low-resistance, and porous, facilitating the fabrication of energy storage devices. To demonstrate its practical application, a planar carbon-based micro-supercapacitor was fabricated on glass, exhibiting excellent electrochemical and cycling performance.

简单快速地生产和转移高质量的碳材料对于灵活高效地制造碳基电子器件至关重要。最近，一种结合了激光诱导碳化和转印的激光辅助转印方法被证明可一步制备激光诱导碳膜图案并将其转印到透明基底上。然而，这种方法受限于碳膜的不稳定性和转移后的弱附着力。在此，我们开发了一种非接触式激光诱导等离子体辅助沉积方法，可在玻璃基底上沉积牢固附着的多孔碳膜。在飞秒激光扫描基底-聚酰亚胺-载体夹层结构的过程中，通过精心调整激光参数和插入厚度可调的间隔物，激光诱导等离子体烧蚀取代了直接激光烧蚀，从而在玻璃基底上形成具有碳-玻璃重铸层的微通道，而不是容易剥离的薄片。这种分层结构大大增强了激光诱导碳膜与玻璃基底之间的粘附力，确保了沉积碳膜在各种粘附测试中的出色稳定性。此外，与激光辅助转移法制备的碳膜相比，所获得的碳膜具有亲水性、低电阻性和多孔性，有利于能量存储设备的制造。为了证明其实际应用，我们在玻璃上制作了一个平面碳基微型超级电容器，该电容器表现出优异的电化学性能和循环性能。

{"title":"Femtosecond laser-induced plasma-assisted backward deposition of robustly adherent porous carbon films on glass substrates","authors":"Sheng Peng , Junjie Zou , Tangyang Pu , Heng Wang , Ruonan Wang , Xiaoyu Tian , Sheng Liu , Qiang Cao","doi":"10.1016/j.surfin.2024.105304","DOIUrl":"10.1016/j.surfin.2024.105304","url":null,"abstract":"<div><div>The simple and rapid production and transfer of high-quality carbon materials are crucial for the flexible and efficient fabrication of carbon-based electronic devices. Recently, a laser-assisted transfer method combining laser-induced carbonization and transfer printing was demonstrated for the one-step preparation and transfer of patterned laser-induced carbon films to transparent substrates. However, this method is limited by insufficient robustness and weak adhesion of the carbon film post-transfer. Herein, we developed a non-contact laser-induced plasma-assisted deposition method to deposit robustly adherent porous carbon films on glass substrates. By well-adjusting the laser parameters and inserting spacers with adjustable thickness, laser-induced plasma ablation replaced direct laser ablation during femtosecond laser scanning of the substrate-polyimide-carrier sandwich structure, resulting in micro-channels with a carbon-glass recast layer instead of easily peelable flakes on the glass substrate. This hierarchical structure significantly enhances the adhesion between the laser-induced carbon film and the glass substrate, ensuring outstanding stability of the deposited carbon film under various adhesion tests. Furthermore, compared to carbon films prepared by the laser-assisted transfer method, the obtained carbon films are hydrophilic, low-resistance, and porous, facilitating the fabrication of energy storage devices. To demonstrate its practical application, a planar carbon-based micro-supercapacitor was fabricated on glass, exhibiting excellent electrochemical and cycling performance.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105304"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551535","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}

引用次数: 0

Optimizing the resistivity of colloidal SnO2 thin films by ion implantation and annealing 通过离子注入和退火优化二氧化锡胶体薄膜的电阻率

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105325

Abubakar Sadiq Yusuf , Martin Markwitz , Zhan Chen , Maziar Ramezani , John V. Kennedy , Holger Fiedler

Tin oxide (SnO₂) is a critical material for a wide range of applications, such as in perovskite solar cells, gas sensors, as well as for photocatalysis. For these applications the transparency to visible light, high availability, cheap fabrication process and high conductivity of SnO₂ benefits its commercial deployment. In this paper, we demonstrate that the resistivity of widely colloidal SnO₂ can be reduced by noble gas ion beam modification. After low energy argon implantation with a fluence of 4×10¹⁵ at.cm⁻² at 25keV and annealing at 200°C in air, the resistivity of as-deposited film was reduced from (178±6)μΩcm to (133±5)μΩcm, a reduction of 25%. Hall effect measurements showed that the primary cause of this is the increase in carrier concentration from (8.1±0.3)×10²⁰ cm⁻³ to (9.9±0.3)×10²⁰ cm⁻³. Annealing at 200°C resulted in the removal of defect clusters introduced by implantation, while annealing at 300°C resulted in the oxidation of the films, increasing their resistivity. The concentration of oxygen vacancy defects can be controlled by a combination of low energy noble gas ion implantation and annealing, providing promising performance increases for potential applications of SnO₂ where a low resistivity is crucial.

氧化锡（SnO2）是一种应用广泛的关键材料，如用于过氧化物太阳能电池、气体传感器以及光催化。在这些应用中，二氧化锡对可见光的透明性、高可用性、廉价的制造工艺和高导电性都有利于其商业应用。在本文中，我们证明了通过惰性气体离子束改性可以降低广泛胶体二氧化锡的电阻率。在 25keV 下以 4×1015 at.cm-2 的通量进行低能氩离子注入并在 200°C 的空气中退火后，沉积薄膜的电阻率从 (178±6)μΩcm 降低到 (133±5)μΩcm，降低了 25%。霍尔效应测量结果表明，主要原因是载流子浓度从 (8.1±0.3)×1020 cm-3 增加到 (9.9±0.3)×1020 cm-3。200°C 退火可去除植入过程中引入的缺陷簇，而 300°C 退火则会导致薄膜氧化，增加其电阻率。氧空位缺陷的浓度可通过低能惰性气体离子植入和退火相结合的方法加以控制，从而有望提高对电阻率要求较低的二氧化锡的潜在应用性能。

{"title":"Optimizing the resistivity of colloidal SnO2 thin films by ion implantation and annealing","authors":"Abubakar Sadiq Yusuf , Martin Markwitz , Zhan Chen , Maziar Ramezani , John V. Kennedy , Holger Fiedler","doi":"10.1016/j.surfin.2024.105325","DOIUrl":"10.1016/j.surfin.2024.105325","url":null,"abstract":"<div><div>Tin oxide (SnO<sub>2</sub>) is a critical material for a wide range of applications, such as in perovskite solar cells, gas sensors, as well as for photocatalysis. For these applications the transparency to visible light, high availability, cheap fabrication process and high conductivity of SnO<sub>2</sub> benefits its commercial deployment. In this paper, we demonstrate that the resistivity of widely colloidal SnO<sub>2</sub> can be reduced by noble gas ion beam modification. After low energy argon implantation with a fluence of 4×10<sup>15</sup> at.cm<sup>−2</sup> at 25keV and annealing at 200°C in air, the resistivity of as-deposited film was reduced from (178±6)μΩcm to (133±5)μΩcm, a reduction of 25%. Hall effect measurements showed that the primary cause of this is the increase in carrier concentration from (8.1±0.3)×10<sup>20</sup> cm<sup>−3</sup> to (9.9±0.3)×10<sup>20</sup> cm<sup>−3</sup>. Annealing at 200°C resulted in the removal of defect clusters introduced by implantation, while annealing at 300°C resulted in the oxidation of the films, increasing their resistivity. The concentration of oxygen vacancy defects can be controlled by a combination of low energy noble gas ion implantation and annealing, providing promising performance increases for potential applications of SnO<sub>2</sub> where a low resistivity is crucial.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105325"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571679","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}

引用次数: 0

Electrochemical corrosion behavior and passive film properties of Fe2Ni2CrV0.5Nbx (x=0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy coating prepared by laser cladding 激光熔覆制备的 Fe2Ni2CrV0.5Nbx (x=0.2, 0.4, 0.6, 0.8) 共晶高熵合金涂层的电化学腐蚀行为和被动膜特性

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105317

Hao Liu , Yingying Li , Peijian Chen , Xinhua Liu , Jingbin Hao , Haifeng Yang

The phase composition, microstructure morphology, and corrosion behavior of Fe₂Ni₂CrV_0.5Nb_x (x = 0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy (EHEA) coatings produced via laser cladding were investigated. The research delved into discerning the phase structures and microstructural variations of the EHEA coatings concerning differing Nb compositions. The findings highlighted a direct correlation between Nb content and the volume fraction of the eutectic structure, specifically the FCC/Laves phases. Electrochemical evaluations, including diverse tests such as potentiodynamic polarization, electrochemical impedance spectroscopy, cyclic polarization, Mott-Schottky measurements, and X-ray photoelectron spectroscopy, revealed distinct corrosion behaviors among the EHEA variants. Notably, the Fe₂Ni₂CrV_0.5Nb_0.2 coating exhibited relatively superior corrosion resistance compared with Fe₂Ni₂CrV_0.5Nb_x (x = 0.4,0.6,0.8) coatings, attributed to its lower corrosion current density (I_corr) and the formation of a thicker passive film with prolonged passivation duration. Conversely, the Fe₂Ni₂CrV_0.5Nb_0.8 coating, characterized by increased eutectic structures and grain boundary density, yielded a thicker yet non-uniform passive film with higher vacancy defects. This comprehensive exploration into the corrosion behavior and passive film properties of these EHEA coatings provides a reference for designing materials that hold promising implications for future corrosion-resistant material development in industrial parts repair applications.

研究了通过激光熔覆生产的 Fe2Ni2CrV0.5Nbx（x = 0.2、0.4、0.6、0.8）共晶高熵合金（EHEA）涂层的相组成、微观结构形态和腐蚀行为。研究深入探讨了不同铌成分的 EHEA 涂层的相结构和微观结构变化。研究结果表明，铌含量与共晶结构（特别是 FCC/Laves 相）的体积分数直接相关。电化学评估包括各种测试，如电位动力极化、电化学阻抗光谱、循环极化、Mott-Schottky 测量和 X 射线光电子能谱，这些评估揭示了不同 EHEA 变体之间截然不同的腐蚀行为。值得注意的是，与 Fe2Ni2CrV0.5Nbx（x = 0.4、0.6、0.8）涂层相比，Fe2Ni2CrV0.5Nb0.2 涂层表现出相对较强的耐腐蚀性，这归因于其较低的腐蚀电流密度（Icorr）和较厚的被动膜的形成以及较长的钝化持续时间。相反，Fe2Ni2CrV0.5Nb0.8 涂层的特点是共晶结构和晶界密度增加，形成的被动膜较厚但不均匀，空位缺陷较多。对这些 EHEA 涂层的腐蚀行为和被动膜特性的全面探索为设计材料提供了参考，对未来工业零部件维修应用中的耐腐蚀材料开发具有重要意义。

{"title":"Electrochemical corrosion behavior and passive film properties of Fe2Ni2CrV0.5Nbx (x=0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy coating prepared by laser cladding","authors":"Hao Liu , Yingying Li , Peijian Chen , Xinhua Liu , Jingbin Hao , Haifeng Yang","doi":"10.1016/j.surfin.2024.105317","DOIUrl":"10.1016/j.surfin.2024.105317","url":null,"abstract":"<div><div>The phase composition, microstructure morphology, and corrosion behavior of Fe<sub>2</sub>Ni<sub>2</sub>CrV<sub>0.5</sub>Nb<sub>x</sub> (<em>x</em> = 0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy (EHEA) coatings produced via laser cladding were investigated. The research delved into discerning the phase structures and microstructural variations of the EHEA coatings concerning differing Nb compositions. The findings highlighted a direct correlation between Nb content and the volume fraction of the eutectic structure, specifically the FCC/Laves phases. Electrochemical evaluations, including diverse tests such as potentiodynamic polarization, electrochemical impedance spectroscopy, cyclic polarization, Mott-Schottky measurements, and X-ray photoelectron spectroscopy, revealed distinct corrosion behaviors among the EHEA variants. Notably, the Fe<sub>2</sub>Ni<sub>2</sub>CrV<sub>0.5</sub>Nb<sub>0.2</sub> coating exhibited relatively superior corrosion resistance compared with Fe<sub>2</sub>Ni<sub>2</sub>CrV<sub>0.5</sub>Nb<sub>x</sub> (<em>x</em> = 0.4,0.6,0.8) coatings, attributed to its lower corrosion current density (I<sub>corr</sub>) and the formation of a thicker passive film with prolonged passivation duration. Conversely, the Fe<sub>2</sub>Ni<sub>2</sub>CrV<sub>0.5</sub>Nb<sub>0.8</sub> coating, characterized by increased eutectic structures and grain boundary density, yielded a thicker yet non-uniform passive film with higher vacancy defects. This comprehensive exploration into the corrosion behavior and passive film properties of these EHEA coatings provides a reference for designing materials that hold promising implications for future corrosion-resistant material development in industrial parts repair applications.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105317"},"PeriodicalIF":5.7,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142571670","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}

引用次数: 0