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Removal of Crystal Violet Dye from Aqueous Solutions through Adsorption onto Activated Carbon Fabrics 通过活性碳织物的吸附作用去除水溶液中的水晶紫染料
C
Pub Date : 2024-02-20 DOI: 10.3390/c10010019
Batuhan Mulla, Kyriacos Ioannou, Gkerman Kotanidis, Ioannis Ioannidis, Georgios Constantinides, M. Baker, S. Hinder, Christian Mitterer, Ioannis Pashalidis, Nikolaos Kostoglou, Claus Rebholz
The removal of contaminants from aqueous solutions by adsorption onto carbonaceous materials has attracted increasing interest in recent years. In this study, pristine and oxidized activated carbon (AC) fabrics with different surface textures and porosity characteristics were used for the removal of crystal violet (CV) dye from aqueous solutions. Batch adsorption experiments were performed to investigate the CV adsorption performance of the AC fabrics in terms of contact time, temperature, adsorbate concentration and adsorbent amount. Evaluation of the thermodynamic parameters and the adsorption performance of the AC fabrics in ground water and sea water solutions were also carried out. Langmuir isotherm model, pseudo first and pseudo second order kinetics models were utilized to analyze and fit the adsorption data. The introduction of oxygen-based functional groups on the surface of AC fabrics was carried out through a nitric acid treatment. This oxidation process resulted in a significant reduction in the surface area and pore volume, along with a small increase in the average pore size and a significant enhancement in the CV adsorption capacity, indicating that the dye molecules are mainly adsorbed on the external surface of the carbon fabrics. The herein evaluated 428 mg/g adsorption capacity at 55 °C for the oxidized non-woven AC fabric is one of the highest adsorption capacity values reported in the literature for CV removal using AC materials. Thermodynamic studies showed that the adsorption occurs spontaneously and is an endothermic and entropy-driven reaction. Furthermore, pristine and oxidized non-woven AC fabrics displayed more than 90% CV uptake from sea water samples, underlining the great potential these fabrics possess for the removal of dyes from natural/multicomponent waters.
近年来,通过碳质材料吸附去除水溶液中污染物的研究越来越受到关注。本研究利用具有不同表面纹理和孔隙率特征的原始活性炭和氧化活性炭织物去除水溶液中的结晶紫(CV)染料。批量吸附实验研究了活性炭织物在接触时间、温度、吸附剂浓度和吸附剂用量方面的 CV 吸附性能。此外,还对 AC 织物在地下水和海水溶液中的热力学参数和吸附性能进行了评估。利用 Langmuir 等温线模型、伪一阶和伪二阶动力学模型来分析和拟合吸附数据。通过硝酸处理,在 AC 织物表面引入了氧官能团。这一氧化过程导致表面积和孔隙率显著减少,平均孔径略有增加,CV 吸附能力显著提高,表明染料分子主要吸附在碳织物的外表面。经评估,氧化无纺 AC 织物在 55 °C 时的吸附容量为 428 mg/g,是文献报道的使用 AC 材料去除 CV 的最高吸附容量值之一。热力学研究表明,吸附是自发发生的,是一种内热和熵驱动反应。此外,原始无纺布和氧化无纺布对海水样本中 CV 的吸附率超过 90%,凸显了这些无纺布在去除天然/多组分水体中的染料方面所具有的巨大潜力。
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引用次数: 0
Effects of Polydopamine Incorporation on the Nanostructure and Electrochemical Performance of Electrodeposited Polypyrrole Films 多多巴胺掺杂对电沉积聚吡咯薄膜的纳米结构和电化学性能的影响
C
Pub Date : 2024-02-20 DOI: 10.3390/c10010020
James A. Behan, Frédéric Barrière
Polypyrrole films are commonly prepared as conductive electrode surfaces for a variety of applications. Recently, there has been increasing interest in improving the adhesive properties and biocompatibility of polypyrrole electrodes via the incorporation of bioinspired polydopamine within the polymer scaffold. However, very little is currently known about the structural effects of polydopamine incorporation during the electropolymerisation of hybrid films. In this work, we combine electrochemical quartz crystal microbalance studies, fundamental electrochemical characterisation, atomic force microscopy, and a suite of spectroscopic techniques in order to correlate changes in the structure and performance of polypyrrole–polydopamine films to the structural modifications of the nanostructure induced by polydopamine incorporation. The results indicate that polydopamine incorporation greatly increases the rate of hybrid film deposition, as well as improving adhesion, surface homogeneity, and wettability, with no compromise in charge transfer properties. Polydopamine incorporation is strongly suggested to occur in non-connected domains within a predominantly polypyrrole-like scaffold. We propose a two-step model of co-polymerisation and the subsequent surface adhesion of hybrid films. Results are expected to be of broad general interest to researchers utilizing polypyrrole and polydopamine to prepare tailor-made electrodes for biosensing and catalysis.
聚吡咯薄膜通常被制备成导电电极表面,用于多种应用领域。最近,人们越来越关注通过在聚合物支架中加入生物启发聚多巴胺来改善聚吡咯电极的粘合性能和生物相容性。然而,目前人们对混合薄膜电聚合过程中加入多巴胺的结构影响知之甚少。在这项工作中,我们结合了电化学石英晶体微天平研究、基本电化学表征、原子力显微镜和一系列光谱技术,以便将聚吡咯-聚多巴胺薄膜的结构和性能变化与加入聚多巴胺引起的纳米结构改变联系起来。结果表明,聚多巴胺的加入大大提高了混合薄膜的沉积速率,并改善了附着力、表面均匀性和润湿性,同时电荷转移性能也没有受到影响。我们强烈建议多聚多巴胺的掺入发生在以聚吡咯为主的支架内的非连接域中。我们提出了共聚和随后混合薄膜表面粘附的两步模型。研究结果有望引起利用聚吡咯和聚多巴胺制备用于生物传感和催化的定制电极的研究人员的广泛兴趣。
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引用次数: 0
Introducing Corrections to the Reflectance of Graphene by Light Emission 通过光发射对石墨烯的反射率进行修正
C
Pub Date : 2024-02-15 DOI: 10.3390/c10010018
Ken-ichi Sasaki, Kenichi Hitachi, Masahiro Kamada, Takamoto Yokosawa, T. Ochi, Tomohiro Matsui
Monolayer graphene absorbs 2.3 percent of the incident visible light. This “small” absorption has been used to emphasize the visual transparency of graphene, but it in fact means that multilayer graphene absorbs a sizable fraction of incident light, which causes non-negligible fluorescence. In this paper, we formulate the light emission properties of multilayer graphene composed of tens to hundreds of layers using a transfer matrix method and confirm the method’s validity experimentally. We quantitatively explain the measured contrasts of multilayer graphene on SiO2/Si substrates and find sizable corrections, which cannot be classified as incoherent light emissions, to the reflectance of visible light. The new component originates from coherent emission caused by absorption at each graphene layer. Multilayer graphene thus functions as a partial coherent light source of various wavelengths, and it may have surface-emitting laser applications.
单层石墨烯吸收入射可见光的 2.3%。这种 "小 "吸收率一直被用来强调石墨烯的视觉透明度,但实际上这意味着多层石墨烯吸收了相当一部分入射光,从而导致不可忽略的荧光。在本文中,我们用转移矩阵法计算了由数十到数百层石墨烯组成的多层石墨烯的光发射特性,并通过实验证实了该方法的有效性。我们定量解释了在二氧化硅/硅衬底上测量到的多层石墨烯的对比度,并发现了对可见光反射率的相当大的修正,这不能归类为非相干光发射。新的成分来自于每个石墨烯层的吸收所引起的相干发射。因此,多层石墨烯可作为各种波长的部分相干光源,并可应用于表面发射激光。
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引用次数: 0
Introducing Corrections to the Reflectance of Graphene by Light Emission 通过光发射对石墨烯的反射率进行修正
C
Pub Date : 2024-02-15 DOI: 10.3390/c10010018
Ken-ichi Sasaki, Kenichi Hitachi, Masahiro Kamada, Takamoto Yokosawa, T. Ochi, Tomohiro Matsui
Monolayer graphene absorbs 2.3 percent of the incident visible light. This “small” absorption has been used to emphasize the visual transparency of graphene, but it in fact means that multilayer graphene absorbs a sizable fraction of incident light, which causes non-negligible fluorescence. In this paper, we formulate the light emission properties of multilayer graphene composed of tens to hundreds of layers using a transfer matrix method and confirm the method’s validity experimentally. We quantitatively explain the measured contrasts of multilayer graphene on SiO2/Si substrates and find sizable corrections, which cannot be classified as incoherent light emissions, to the reflectance of visible light. The new component originates from coherent emission caused by absorption at each graphene layer. Multilayer graphene thus functions as a partial coherent light source of various wavelengths, and it may have surface-emitting laser applications.
单层石墨烯吸收入射可见光的 2.3%。这种 "小 "吸收率一直被用来强调石墨烯的视觉透明度,但实际上这意味着多层石墨烯吸收了相当一部分入射光,从而导致不可忽略的荧光。在本文中,我们用转移矩阵法计算了由数十到数百层石墨烯组成的多层石墨烯的光发射特性,并通过实验证实了该方法的有效性。我们定量解释了在二氧化硅/硅衬底上测量到的多层石墨烯的对比度,并发现了对可见光反射率的相当大的修正,这不能归类为非相干光发射。新的成分来自于每个石墨烯层的吸收所引起的相干发射。因此,多层石墨烯可作为各种波长的部分相干光源,并可应用于表面发射激光。
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引用次数: 0
Pristine and Coated Carbon Nanotube Sheets—Characterization and Potential Applications 原始和涂层碳纳米管片--表征和潜在应用
C
Pub Date : 2024-02-09 DOI: 10.3390/c10010017
Prakash Giri, Irwin Gill, Morgan Swensgard, Alexandra Kaiser, Audrey Rust, Brian Stuparyk, Andrew Fisher, Justice Williams, Katie Renoit, Eleanor Kreeb, Corentin Lavenan, Mark J. Schulz
A carbon nanotube (CNT) sheet is a nonwoven fabric that is being evaluated for use in different textile applications. Several properties of pristine CNT sheets and CNT sheets coated with a polysilazane sealant and coating were measured and compared in the paper. The polysilazane coating is used to reduce the shedding of CNT fibers from the sheet when the sheet is in contact with surfaces. Most fabrics show some shedding of fibers during the washing or abrasion of the fabric. This study showed that the coating reduces the shedding of fibers from CNT fabric. The coating also increased the flame resistance of the fabric. The pristine and coated sheets both have low strength but high strain to failure. The pristine and coated CNT sheet densities are 0.48 g/cc and 0.65 g/cc, respectively. The pristine CNT sheet is approximately 27 μ thick. The coated sheet is approximately 24 μ thick. The coating may have densified the sheet, making it thinner. The thickness of the compliant sheets was difficult to measure and is a source of error in the properties. Characterization results are given in this paper. The results are for comparison purposes and not to establish material properties data. Possible applications for CNT sheets are briefly discussed.
碳纳米管(CNT)薄片是一种无纺布,目前正在对其在不同纺织品中的应用进行评估。本文测量并比较了原始 CNT 片材和涂有聚硅氧烷密封剂和涂层的 CNT 片材的几种特性。聚硅氧烷涂层用于减少碳纳米管纤维在板材与表面接触时的脱落。大多数织物在洗涤或磨损过程中都会出现一些纤维脱落。这项研究表明,涂层可减少 CNT 织物上纤维的脱落。涂层还提高了织物的阻燃性。原始板材和涂层板材的强度都较低,但破坏应变较大。原始和涂层碳纳米管薄片的密度分别为 0.48 g/cc 和 0.65 g/cc。原始碳纳米管薄片厚度约为 27 μ。涂层薄片的厚度约为 24 μ。涂层可能使薄片致密化,从而变薄。顺应性薄片的厚度很难测量,这也是特性误差的一个来源。本文给出了表征结果。这些结果仅用于比较,而非确定材料特性数据。本文简要讨论了碳纳米管薄片的可能应用。
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引用次数: 0
Pristine and Coated Carbon Nanotube Sheets—Characterization and Potential Applications 原始和涂层碳纳米管片--表征和潜在应用
C
Pub Date : 2024-02-09 DOI: 10.3390/c10010017
Prakash Giri, Irwin Gill, Morgan Swensgard, Alexandra Kaiser, Audrey Rust, Brian Stuparyk, Andrew Fisher, Justice Williams, Katie Renoit, Eleanor Kreeb, Corentin Lavenan, Mark J. Schulz
A carbon nanotube (CNT) sheet is a nonwoven fabric that is being evaluated for use in different textile applications. Several properties of pristine CNT sheets and CNT sheets coated with a polysilazane sealant and coating were measured and compared in the paper. The polysilazane coating is used to reduce the shedding of CNT fibers from the sheet when the sheet is in contact with surfaces. Most fabrics show some shedding of fibers during the washing or abrasion of the fabric. This study showed that the coating reduces the shedding of fibers from CNT fabric. The coating also increased the flame resistance of the fabric. The pristine and coated sheets both have low strength but high strain to failure. The pristine and coated CNT sheet densities are 0.48 g/cc and 0.65 g/cc, respectively. The pristine CNT sheet is approximately 27 μ thick. The coated sheet is approximately 24 μ thick. The coating may have densified the sheet, making it thinner. The thickness of the compliant sheets was difficult to measure and is a source of error in the properties. Characterization results are given in this paper. The results are for comparison purposes and not to establish material properties data. Possible applications for CNT sheets are briefly discussed.
碳纳米管(CNT)薄片是一种无纺布,目前正在对其在不同纺织品中的应用进行评估。本文测量并比较了原始 CNT 片材和涂有聚硅氧烷密封剂和涂层的 CNT 片材的几种特性。聚硅氧烷涂层用于减少碳纳米管纤维在板材与表面接触时的脱落。大多数织物在洗涤或磨损过程中都会出现一些纤维脱落。这项研究表明,涂层可减少 CNT 织物上纤维的脱落。涂层还提高了织物的阻燃性。原始板材和涂层板材的强度都较低,但破坏应变较大。原始和涂层碳纳米管薄片的密度分别为 0.48 g/cc 和 0.65 g/cc。原始碳纳米管薄片厚度约为 27 μ。涂层薄片的厚度约为 24 μ。涂层可能使薄片致密化,从而变薄。顺应性薄片的厚度很难测量,这也是特性误差的一个来源。本文给出了表征结果。这些结果仅用于比较,而非确定材料特性数据。本文简要讨论了碳纳米管薄片的可能应用。
{"title":"Pristine and Coated Carbon Nanotube Sheets—Characterization and Potential Applications","authors":"Prakash Giri, Irwin Gill, Morgan Swensgard, Alexandra Kaiser, Audrey Rust, Brian Stuparyk, Andrew Fisher, Justice Williams, Katie Renoit, Eleanor Kreeb, Corentin Lavenan, Mark J. Schulz","doi":"10.3390/c10010017","DOIUrl":"https://doi.org/10.3390/c10010017","url":null,"abstract":"A carbon nanotube (CNT) sheet is a nonwoven fabric that is being evaluated for use in different textile applications. Several properties of pristine CNT sheets and CNT sheets coated with a polysilazane sealant and coating were measured and compared in the paper. The polysilazane coating is used to reduce the shedding of CNT fibers from the sheet when the sheet is in contact with surfaces. Most fabrics show some shedding of fibers during the washing or abrasion of the fabric. This study showed that the coating reduces the shedding of fibers from CNT fabric. The coating also increased the flame resistance of the fabric. The pristine and coated sheets both have low strength but high strain to failure. The pristine and coated CNT sheet densities are 0.48 g/cc and 0.65 g/cc, respectively. The pristine CNT sheet is approximately 27 μ thick. The coated sheet is approximately 24 μ thick. The coating may have densified the sheet, making it thinner. The thickness of the compliant sheets was difficult to measure and is a source of error in the properties. Characterization results are given in this paper. The results are for comparison purposes and not to establish material properties data. Possible applications for CNT sheets are briefly discussed.","PeriodicalId":9397,"journal":{"name":"C","volume":"37 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139849428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Comprehensive Study on Carbon-Coated Silver for Improved Tribo-Electrical and Wetting Performance 关于碳包银改善三电性能和润湿性能的综合研究
C
Pub Date : 2024-02-04 DOI: 10.3390/c10010016
Bruno Alderete, F. Mücklich, S. Suárez
The rise in electrification has considerably increased the demand for high-efficiency and durable electrical contact materials. Carbon nanoparticles (CNP) are a promising coating material due to their intrinsic transport properties (thus minimizing the impact on conductivity), their proven solid lubricity (potentially improving tribological performance), and their hydrophobic wetting behavior (potentially providing atmospheric protection). In this study, carbon nanotube and nanohorn coatings are produced via electrophoretic deposition on silver-plated surfaces, followed by tribo-electrical and wetting characterization. The proposed coatings do not negatively affect the conductivity of the substrate, showing resistance values on par with the uncoated reference. Tribo-electrical characterization revealed that the coatings reduce adhesive wear during fretting tests while maintaining stable and constant electrical contact resistance. Furthermore, CNP-coated surfaces show a hydrophobic wetting behavior toward water, with graphite and carbon nanotube (CNT) coatings approaching super-hydrophobicity. Prolonged exposure to water droplets during sessile drop tests caused a reduction in contact angle (CA) measurement; however, CNT coatings’ CA reduction after five minutes was only approximately 5°. Accordingly, CNP (specifically CNT) coatings show auspicious results for their application as wear and atmospheric protective barriers in electrical contacts.
电气化程度的提高大大增加了对高效耐用电接触材料的需求。碳纳米颗粒(CNP)是一种很有前途的涂层材料,因为它们具有固有的传输特性(从而最大限度地减少对导电性的影响)、经证实的固体润滑性(可能改善摩擦学性能)和疏水润湿行为(可能提供大气保护)。在本研究中,通过在镀银表面电泳沉积碳纳米管和纳米角涂层,然后进行三电和润湿表征。所提出的涂层不会对基底的导电性产生负面影响,其电阻值与未涂层的参考值相当。三电特性分析表明,涂层可减少摩擦测试中的粘合剂磨损,同时保持稳定恒定的电接触电阻。此外,CNP 涂层表面对水具有疏水性润湿行为,石墨和碳纳米管 (CNT) 涂层接近超疏水性。在无柄水滴测试中,长时间接触水滴会导致接触角(CA)测量值减小;但 CNT 涂层在五分钟后的 CA 值减小仅约为 5°。因此,CNP(特别是 CNT)涂层在用作电气触点的磨损和大气保护屏障方面显示出良好的应用效果。
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引用次数: 0
Comprehensive Study on Carbon-Coated Silver for Improved Tribo-Electrical and Wetting Performance 关于碳包银改善三电性能和润湿性能的综合研究
C
Pub Date : 2024-02-04 DOI: 10.3390/c10010016
Bruno Alderete, F. Mücklich, S. Suárez
The rise in electrification has considerably increased the demand for high-efficiency and durable electrical contact materials. Carbon nanoparticles (CNP) are a promising coating material due to their intrinsic transport properties (thus minimizing the impact on conductivity), their proven solid lubricity (potentially improving tribological performance), and their hydrophobic wetting behavior (potentially providing atmospheric protection). In this study, carbon nanotube and nanohorn coatings are produced via electrophoretic deposition on silver-plated surfaces, followed by tribo-electrical and wetting characterization. The proposed coatings do not negatively affect the conductivity of the substrate, showing resistance values on par with the uncoated reference. Tribo-electrical characterization revealed that the coatings reduce adhesive wear during fretting tests while maintaining stable and constant electrical contact resistance. Furthermore, CNP-coated surfaces show a hydrophobic wetting behavior toward water, with graphite and carbon nanotube (CNT) coatings approaching super-hydrophobicity. Prolonged exposure to water droplets during sessile drop tests caused a reduction in contact angle (CA) measurement; however, CNT coatings’ CA reduction after five minutes was only approximately 5°. Accordingly, CNP (specifically CNT) coatings show auspicious results for their application as wear and atmospheric protective barriers in electrical contacts.
电气化程度的提高大大增加了对高效耐用电接触材料的需求。碳纳米颗粒(CNP)是一种很有前途的涂层材料,因为它们具有固有的传输特性(从而最大限度地减少对导电性的影响)、经证实的固体润滑性(可能改善摩擦学性能)和疏水润湿行为(可能提供大气保护)。在本研究中,通过在镀银表面电泳沉积碳纳米管和纳米角涂层,然后进行三电和润湿表征。所提出的涂层不会对基底的导电性产生负面影响,其电阻值与未涂层的参考值相当。三电特性分析表明,涂层可减少摩擦测试中的粘合剂磨损,同时保持稳定恒定的电接触电阻。此外,CNP 涂层表面对水具有疏水性润湿行为,石墨和碳纳米管 (CNT) 涂层接近超疏水性。在无柄水滴测试中,长时间接触水滴会导致接触角(CA)测量值减小;但 CNT 涂层在五分钟后的 CA 值减小仅约为 5°。因此,CNP(特别是 CNT)涂层在用作电气触点的磨损和大气保护屏障方面显示出良好的应用效果。
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引用次数: 0
Carbon Capture, Utilization, and Storage Risks from Supply Chain Perspective: A Review of the Literature and Conceptual Framework Development 从供应链角度看碳捕集、利用和封存风险:文献综述与概念框架开发
C
Pub Date : 2024-01-31 DOI: 10.3390/c10010015
Md Ainul Kabir, S. Khan, G. Kabir
The technology called carbon capture, utilization, and storage (CCUS) is important for capturing CO2 emissions before they enter the air. Because everyone wants to stop global warming by reducing CO2 emissions, CCUS is an important and emerging technology that can help slow down climate change, lower emissions in many areas, and support the move toward a sustainable and carbon-neutral future. As CCUS technology and its adaptation increases, it is very important to pay attention to the CCUS risks from a supply chain (SC) point of view. The goal of this study was to identify CCUS supply chain risks and develop a conceptual framework (CF) that provides a structured approach to ensure safe and reliable CCUS supply chain operations. Therefore, this study analyzed the literature related to the SCs of different sectors and identified the SC risks, which was the foundation for CCUS SC risk identification. This study demonstrates that there is no research article that provides a comprehensive CCUS SC risk management framework that connects with risk management strategies. The conceptual framework that is proposed in this study connects CCUS SC functions, risks, and risk management strategies to construct a complete CCUS supply chain risk management system. Moreover, the CF provides guidelines for future research, which will enrich the CCUS supply chain risk management system as well as fight climate change.
被称为碳捕集、利用和封存(CCUS)的技术对于在二氧化碳排放进入空气之前将其捕获非常重要。由于每个人都希望通过减少二氧化碳排放来阻止全球变暖,CCUS 是一项重要的新兴技术,有助于减缓气候变化,降低许多领域的排放,支持迈向可持续发展和碳中和的未来。随着 CCUS 技术及其适应性的提高,从供应链(SC)的角度关注 CCUS 风险非常重要。本研究的目标是识别 CCUS 供应链风险,并开发一个概念框架(CF),为确保 CCUS 供应链的安全可靠运营提供结构化方法。因此,本研究分析了与不同行业供应链相关的文献,确定了供应链风险,为 CCUS 供应链风险识别奠定了基础。本研究表明,目前还没有研究文章提供与风险管理战略相联系的全面的 CCUS SC 风险管理框架。本研究提出的概念框架将 CCUS SC 功能、风险和风险管理策略联系起来,构建了一个完整的 CCUS 供应链风险管理系统。此外,该框架还为今后的研究提供了指导,这将丰富 CCUS 供应链风险管理系统,并应对气候变化。
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引用次数: 0
Metal-Free Catalytic Conversion of Veratryl and Benzyl Alcohols through Nitrogen-Enriched Carbon Nanotubes 通过富氮碳纳米管实现藜芦醇和苄醇的无金属催化转化
C
Pub Date : 2024-01-26 DOI: 10.3390/c10010013
Neeraj Gupta, Ilaria Barlocco, O. Khavryuchenko, Alberto Villa
Nitrogen-rich carbon nanotubes NCNT700 and NCNT800 were prepared using the chemical vapor deposition method (CVD). The catalysts were characterized via high-resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS) analysis. Both the catalysts were found to have an inverted cup-stack-like morphology. The XPS analysis revealed that the catalysts are rich in pyridinic sites with variable amounts of nitrogen on their surface. The NCTN700, with a higher nitrogen content and more pyridinic sites on its surface, was found to be a good catalyst for the oxidation of benzyl and veratryl alcohols into respective aldehydes. It was observed that toluene and 4-methyl veratrole were also produced in this reaction. The amount of toluene produced was as high as 21%, with 99% conversion of benzaldehyde in the presence of NCNTs-700. The mechanistic pathway was revealed through DFT studies, where the unusual product formation of aromatic alkanes such as toluene and 4-methyl veratrole was explained during the reaction. It was astonishing to observe the reduced product in the reaction that proceeds in the forward direction in presence of a peroxide (tert-butyl hydroperoxide, TBHP). During the computational analysis, it was revealed that the reduced product observed in the reaction did not appear to proceed through a direct disproportionation reaction. Rather, the benzyl alcohol (the reactant) used in the reaction may undergo oxidation by releasing the hydrogen radicals. The hydrogen atoms released during the oxidation reaction appear to have been trapped on pyrrolic sites on the surface of catalyst and later transferred to the reactant molecules to produce toluene as a side product.
采用化学气相沉积法(CVD)制备了富氮碳纳米管 NCNT700 和 NCNT800。通过高分辨率透射电子显微镜(HRTEM)和 X 射线光电子能谱(XPS)分析对催化剂进行了表征。结果发现,两种催化剂都具有倒杯叠层状形态。XPS 分析表明,催化剂表面富含不同数量氮的吡啶位点。发现氮含量较高且表面吡啶位点较多的 NCTN700 是苯甲醇和藜芦醇氧化成相应醛类的良好催化剂。据观察,在这一反应中还产生了甲苯和 4-甲基藜芦。在 NCNT-700 的存在下,苯甲醛的转化率为 99%,甲苯的生成量高达 21%。通过 DFT 研究揭示了机理途径,解释了反应过程中形成甲苯和 4-甲基藜芦等芳香烃的不寻常产物。令人惊讶的是,在过氧化物(叔丁基过氧化氢,TBHP)存在的情况下,在反应中观察到了正向进行的还原产物。在计算分析过程中发现,在反应中观察到的还原产物似乎并不是通过直接歧化反应进行的。相反,反应中使用的苯甲醇(反应物)可能通过释放氢自由基而发生氧化。氧化反应中释放出的氢原子似乎被截留在催化剂表面的吡咯啉位点上,随后转移到反应物分子中,生成副产品甲苯。
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引用次数: 0
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C
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