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Exploring a New Class of PVDF/3‐Aminopropyltriethoxysilane (core) and 2,2‐Bis(hydroxymethyl)butyric Acid (monomer)‐Based Hyperbranched Polyester Hybrid Fibers by Electrospinning Technique for Enhancing Triboelectric Performance 利用电纺丝技术探索一种新型 PVDF/3-氨基丙基三乙氧基硅烷(芯材)和 2,2-双(羟甲基)丁酸(单体)基超支化聚酯杂化纤维,以提高三电性能
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-10 DOI: 10.1002/adsu.202400311
Vadakkaveedu Subramanian Niranjana, Jae Uk Yoon, Insun Woo, Prasad Gajula, Jin Woo Bae, Arun Anand Prabu
With the rapid advancement in sensor technologies, triboelectric nanogenerators (TENGs) have emerged as a promising sustainable power source for intelligent electronics. Herein, fabricated a novel 3‐aminopropyltriethoxysilane (core) and 2,2‐bis(hydroxymethyl)butyric acid (monomer)‐based hyperbranched polyester by facile single‐step polycondensation technique generation 2 (Si‐HBP‐G2). Further, a new class of polyvinylidene fluoride (PVDF) and different weight percentages (0, 5, 10, 15, and 20 wt%) of Si‐HBP‐G2 hybrid fiber blends are prepared by traditional electrospinning technique. The as‐prepared Si‐HBP‐G2 and its blends are well characterized using SEM/EDS, FTIR, NMR, and XRD studies. The influence of Si‐HBP‐G2 content on triboelectric performance in terms of the open circuit potential (VOC) and short circuit current (ISC) is evaluated using aluminum (Al) as a counter electrode. Among them, 15 wt% of Si‐HBP‐G2/PVDF hybrid fiber mat (PG2‐15) exhibits superior electrical performance. Which is almost increased 5.9 times (22–130 V) of VOC and 4.9 times (0.71–3.5 µA) of ISC than PVDF fiber mate. These results reveal the significance of Si‐HBP‐G2 in the triboelectric performance. The optimized TENG device (PG2‐15/Al‐TENG) exhibits a peak power density of 0.2 Wm−2 at 100 MΩ external load. Finally, the PG2‐15/Al‐TENG practically demonstrates real‐time application energy harvesting applications such as powering 100 LEDs and a stopwatch.
随着传感器技术的飞速发展,三电纳米发电机(TENGs)已成为智能电子领域一种前景广阔的可持续电源。本文通过简单的单步缩聚技术第二代(Si-HBP-G2)制备了一种新型的 3-氨丙基三乙氧基硅烷(芯材)和 2,2-双(羟甲基)丁酸(单体)基超支化聚酯。此外,还采用传统的电纺丝技术制备了新型聚偏二氟乙烯(PVDF)和不同重量百分比(0、5、10、15 和 20 wt%)的 Si-HBP-G2 混合纤维。利用 SEM/EDS、FTIR、NMR 和 XRD 研究对制备的 Si-HBP-G2 及其混合物进行了表征。以铝(Al)为反电极,评估了 Si-HBP-G2 含量对开路电势(VOC)和短路电流(ISC)等三电性能的影响。其中,15 wt% 的 Si-HBP-G2/PVDF 混合纤维毡(PG2-15)表现出卓越的电气性能。与 PVDF 纤维垫相比,其 VOC 值几乎提高了 5.9 倍(22-130 V),ISC 值提高了 4.9 倍(0.71-3.5 µA)。这些结果揭示了 Si-HBP-G2 在三电性能中的重要作用。优化后的 TENG 器件(PG2-15/Al-TENG)在 100 MΩ 外部负载下的峰值功率密度为 0.2 Wm-2。最后,PG2-15/Al-TENG 实际演示了实时应用能量收集应用,如为 100 个 LED 和秒表供电。
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引用次数: 0
Synthesis of Poly‐Pyrrole Nanotubes/Chromium Vanadate Composite as Wired Interlocks to Achieve an Asymmetric Supercapacitor Device with Scaled Electrochemical Energy Parameters 合成聚吡咯纳米管/钒酸铬复合材料作为有线互锁物,实现具有规模化电化学能量参数的不对称超级电容器装置
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-09 DOI: 10.1002/adsu.202400271
Neeru Jhanjhariya, Suman Lata
Herein, a novel combination with a focused morphology is designed after synthesizing CrVO4 (CV) nanoparticles and poly‐pyrrole nanotubes (PNT or P) to prepare the interlocks of the composites of PNT and CrVO4 as 1PCV1, 1PCV2, 2PCV1, and 2PCV2 to study the supercapacitor application. Structural and spectral characterizations are perpetuated to confirm the synthesis of the samples. Results furnishing best energy storage are obtained for the intercalated composite 2PCV1 examined for three‐probe and two‐probe set‐up. The excel values for specific capacitance (Cs) for 2PCV1 concerning the Cyclic voltammetry (CV) cycle and Galvanostatic Charge Discharge (GCD) curve are 1745.60 F g−1 at 10 mV s−1 rate and 1545.62 F g−1 at 0.625 A g−1 current density studied along with interface controlled and transport‐controlled Cs with a contribution of 55.13% interface part and 44.87% transport part at 5 mV s−1 scan rate. Electrochemical Impedance Spectroscopy (EIS) study has provided 0.86 n‐factor with solution resistance Rs of 1.48 Ω, and a charge transfer resistance of 0.166 Ω. The respective specific power and specific energy values obtained through the two‐probe set‐up are also interestingly high 416.68 W kg−1 and 45.14 Wh kg−1 at 0.83 A g−1 current density. Also, the retention % in Cs values is studied by running 5000 continuous voltammetric cycles with 96.23% retention in supercapacitor device.
本文设计了一种具有聚焦形态的新型组合,在合成了 CrVO4 (CV) 纳米粒子和聚吡咯纳米管(PNT 或 P)之后,制备了 PNT 和 CrVO4 的互锁复合材料 1PCV1、1PCV2、2PCV1 和 2PCV2,以研究超级电容器的应用。为了证实样品的合成,对其进行了结构和光谱表征。对插层复合材料 2PCV1 进行了三探针和双探针设置测试,结果表明其储能效果最佳。在循环伏安法(CV)周期和伽马静电荷放电(GCD)曲线上,2PCV1 的比电容(Cs)卓越值分别为:10 mV s-1 速率下 1745.60 F g-1 和 0.625 A g-1 电流密度下 1545.62 F g-1;在 5 mV s-1 扫描速率下,界面控制和传输控制的 Cs 占界面部分的 55.13%,传输部分的 44.87%。电化学阻抗谱(EIS)研究提供了 0.86 n 因子,溶液电阻 Rs 为 1.48 Ω,电荷转移电阻为 0.166 Ω。在 0.83 A g-1 电流密度下,通过双探针设置获得的比功率和比能量值也分别高达 416.68 W kg-1 和 45.14 Wh kg-1。此外,通过连续运行 5000 次伏安循环,研究了铯值的保留率,超级电容器装置中的保留率为 96.23%。
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引用次数: 0
High Performance Flexible Supercapacitor Based on Single Precursor Derived NiFe2O4 Spinel with Tailored Cationic Distribution and Oxygen Vacancies in Acidic Medium 基于单一前驱体衍生的具有定制阳离子分布和酸性介质中氧空位的 NiFe2O4 尖晶石的高性能柔性超级电容器
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-09 DOI: 10.1002/adsu.202400244
Ajay, Vaishali Tanwar, Aditi Ashok Gujare, Pravin Popinand Ingole
Spinel metal oxides are extensively studied for supercapacitors (SCs) in alkaline electrolytes, where charge storage capacity is limited by surface site availability due to surface reconstruction forming metal hydroxides/oxyhydroxides. The use of an acidic medium, which can boost the charge storage capacity of spinel oxides offering an additional channel of intercalation-deintercalation of protons, is underexplored. Moreover, the impact of chemical compositions and the cationic distributions is crucial on the electrocatalysis performance of spinel oxides, however, such a correlation is first time reported for charge storage properties of spinel ferrite NiFe2O4 nanoparticles (NFO NPs). Besides, a low-cost and scalable synthesis of NFO NPs involving the thermal decomposition of Ni-Fe glycolate, followed by controlled air-calcination is reported. Thus crafted NFO NPs-based device shows impressive specific capacitance (2112 F g−1 at 10 A g−1) in half-cell configuration. A flexible all-solid-state asymmetric device (full-cell) configuration depicts impressive energy density (20.7 Wh kg−1), power density (4000 W kg−1), gravimetric capacitance (140 F g−1 at 2 A g−1), and retention of its performance (≈75% after 10,000 charging/discharging cycles). The results depict a new insight toward the tuning of electronic and charge storage properties in NFO, which otherwise are predominately attributed to only the crystallite size and morphological effects.
人们对碱性电解质中的尖晶石金属氧化物超级电容器(SC)进行了广泛的研究,在碱性电解质中,电荷存储容量受表面位点可用性的限制,这是由于表面重构形成了金属氢氧化物/氧氢氧化物。使用酸性介质可以提高尖晶石氧化物的电荷存储容量,为质子的插层-插层提供额外的通道,但目前对酸性介质的研究还很欠缺。此外,化学成分和阳离子分布对尖晶石氧化物的电催化性能也有至关重要的影响,然而,这种相关性在尖晶石铁氧体 NiFe2O4 纳米粒子(NFO NPs)的电荷存储特性方面尚属首次报道。此外,还报道了一种低成本、可扩展的 NFO NPs 合成方法,该方法涉及乙二酸镍铁合金的热分解,然后是受控的空气煅烧。因此,基于 NFO NPs 制作的器件在半电池配置下显示出惊人的比电容(10 A g-1 时为 2112 F g-1)。灵活的全固态非对称器件(全电池)配置显示出令人印象深刻的能量密度(20.7 Wh kg-1)、功率密度(4000 W kg-1)、重力电容(2 A g-1 时为 140 F g-1)和性能保持率(10,000 次充电/放电循环后≈75%)。这些结果为调整 NFO 的电子和电荷存储特性提供了新的视角,而这些特性主要归因于晶体尺寸和形态效应。
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引用次数: 0
Biobased Polyethylene Furanoate: Production Processes, Sustainability, and Techno‐Economics 生物基聚呋喃乙烯:生产工艺、可持续性和技术经济学
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-09 DOI: 10.1002/adsu.202400074
John H. Sanders, Julia Cunniffe, Edgar Carrejo, Cullen Burke, Autumn M. Reynolds, Shaikat Chandra Dey, Md. Nazrul Islam, Owen Wagner, Dimitris Argyropoulos
Polyethylene furanoate (PEF) is a biobased plastic, similar to synthetic polyethylene terephthalate (PET), which is produced from the platform chemical 2,5‐hydroxymethylfurfural (HMF). Much of the literature surrounding PEF is focused on unit processes, with little regard for their sustainability and economic viability. In this comprehensive critical review, the entire process of PEF production, from the feedstock to polymerization and upstream applications, is critically examined. Identification of individual pathways capable of producing PEF efficiently and with favorable properties while considering economic viability and environmental sustainability are presented. For each unit operation, recent technological developments are summarized, and recommendations are made based on process efficiency. The collection of the findings from both life cycle assessments (LCA) and techno‐economic analyses (TEA) facilitated the identification of pathways with the greatest potential for environmental sustainability and economic viability of PEF production.
聚呋喃乙烯(PEF)是一种生物基塑料,类似于合成聚对苯二甲酸乙二醇酯(PET),由平台化学品 2,5-羟甲基糠醛(HMF)生产。有关 PEF 的许多文献都集中在单元工艺上,很少考虑其可持续性和经济可行性。在这篇综合评论中,对全氟乙烯生产的整个过程,从原料到聚合再到上游应用,都进行了严格的审查。在考虑经济可行性和环境可持续性的同时,还确定了能够高效生产 PEF 并具有良好特性的各个途径。对每个单元操作的最新技术发展进行了总结,并根据工艺效率提出了建议。通过收集生命周期评估(LCA)和技术经济分析(TEA)的结果,确定了具有最大环境可持续性潜力和经济可行性的全氟聚醚生产途径。
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引用次数: 0
Revealing the Electrocatalytic Reaction Mechanism of Water Splitting by In Situ Raman Technique 利用原位拉曼技术揭示水分离的电催化反应机理
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-05 DOI: 10.1002/adsu.202400387
Weifeng Hu, Yixiang Luo, Enchi Zhu, Anlei Zhang, Longlu Wang
Using renewable energy for water splitting to produce hydrogen is a crucial step toward achieving the dual carbon goals. However, due to the lack of a clear understanding of the precise localization of catalytic active sites and the complex structural evolution of catalysts during actual reaction conditions, there is still a challenge to reveal the electrocatalytic reaction mechanism of water splitting. In situ electrochemical Raman characterization technique can dynamically monitor the structural evolution of catalysts in real time, reveal the dynamic structure‐performance relationship of catalysts during the reaction process, and explore the catalytic reaction mechanism. This paper focuses on reviewing the latest developments in in situ electrochemical Raman characterization technology in terms of active sites on catalyst surfaces, the behavior of interfacial water molecules, and the structure evolution of electrocatalysts. The future development prospect of advanced in situ electrochemical Raman technology is also prospected.
利用可再生能源进行水分离制氢是实现双碳目标的关键一步。然而,由于对催化活性位点的精确定位和实际反应条件下催化剂复杂的结构演化缺乏清晰的认识,揭示水分离的电催化反应机理仍是一项挑战。原位电化学拉曼表征技术可以实时动态监测催化剂的结构演变,揭示催化剂在反应过程中的动态结构-性能关系,探索催化反应机理。本文重点从催化剂表面活性位点、界面水分子行为和电催化剂结构演化等方面综述了原位电化学拉曼表征技术的最新发展。同时还展望了先进原位电化学拉曼技术的未来发展前景。
{"title":"Revealing the Electrocatalytic Reaction Mechanism of Water Splitting by In Situ Raman Technique","authors":"Weifeng Hu, Yixiang Luo, Enchi Zhu, Anlei Zhang, Longlu Wang","doi":"10.1002/adsu.202400387","DOIUrl":"https://doi.org/10.1002/adsu.202400387","url":null,"abstract":"Using renewable energy for water splitting to produce hydrogen is a crucial step toward achieving the dual carbon goals. However, due to the lack of a clear understanding of the precise localization of catalytic active sites and the complex structural evolution of catalysts during actual reaction conditions, there is still a challenge to reveal the electrocatalytic reaction mechanism of water splitting. In situ electrochemical Raman characterization technique can dynamically monitor the structural evolution of catalysts in real time, reveal the dynamic structure‐performance relationship of catalysts during the reaction process, and explore the catalytic reaction mechanism. This paper focuses on reviewing the latest developments in in situ electrochemical Raman characterization technology in terms of active sites on catalyst surfaces, the behavior of interfacial water molecules, and the structure evolution of electrocatalysts. The future development prospect of advanced in situ electrochemical Raman technology is also prospected.","PeriodicalId":7294,"journal":{"name":"Advanced Sustainable Systems","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141568056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Utilization of High Entropy Alloy (Co–Cu–Fe–Mn–Ni) and Support (CeO2) Interaction for CO2 Conversion into Syngas 利用高熵合金(Co-Cu-Fe-Mn-Ni)和支持物(CeO2)的相互作用将二氧化碳转化为合成气
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-05 DOI: 10.1002/adsu.202400219
Bhanu P. Gangwar, Rahul Mitra, Arko Parui, Pooja Gakhad, Pradeep Kumar Yadav, Abhishek Kumar Singh, Chandra Sekhar Tiwary, Krishanu Biswas, Sudhanshu Sharma
Here metal support interaction (MSI) is demonstrated in a high entropy alloy (HEA: CoCuFeMnNi) supported CeO2. The HEA behaves as an active dry reforming catalyst only when it is supported over CeO2 oxide, clearly demonstrating MSI. Based on spectroscopic and microscopic observations, it is envisaged that the substitutional effect is the one that causes the lattice oxygen activation, an important active species during DRM reaction. Transient studies are performed to understand the surface chemistry of the interaction between methane and CO2 in the presence of a catalyst, which results in a methane decomposition first to generate hydrogen and carbon and followed by a CO2 reaction to give CO using deposited carbon. The experimental observations are further proven by mechanistic study with DFT calculations which show a major contribution of H‐assisted CO2 dissociation and pre‐H2 releasing carbon depositing CH4 dissociation and a minor contribution of pre‐CO releasing H2 formation. This MSI moves the d‐band center of the Co atoms of CoCuFeMnNi/CeO2 to the closest position of the Fermi level as compared to the isolated nanoparticles. This study can be taken as a proof of concept to demonstrate that MSI can be generated in the HEA/CeO2 catalysts for a generic heterogeneous gas phase reaction.
在此,我们展示了以 CeO2 为载体的高熵合金(HEA:CoCuFeMnNi)中的金属载体相互作用(MSI)。只有当 HEA 被 CeO2 氧化物支撑时,它才表现为活性干重整催化剂,这清楚地证明了 MSI。根据光谱和显微镜观察,我们认为置换效应是导致晶格氧活化的原因,而晶格氧是 DRM 反应过程中的重要活性物种。瞬态研究旨在了解甲烷和二氧化碳在催化剂作用下的表面化学反应,其结果是甲烷首先分解生成氢和碳,然后与二氧化碳反应,利用沉积碳生成一氧化碳。通过 DFT 计算进行的机理研究进一步证实了实验观察结果,该计算显示,H 辅助 CO2 解离和 H2 释放前碳沉积 CH4 解离起主要作用,CO 释放前 H2 形成起次要作用。与孤立的纳米粒子相比,这种 MSI 将 CoCuFeMnNi/CeO2 中 Co 原子的 d 波段中心移到了费米级的最近位置。这项研究可以作为概念验证,证明在 HEA/CeO2 催化剂中可以产生 MSI,用于一般的异相气相反应。
{"title":"Utilization of High Entropy Alloy (Co–Cu–Fe–Mn–Ni) and Support (CeO2) Interaction for CO2 Conversion into Syngas","authors":"Bhanu P. Gangwar, Rahul Mitra, Arko Parui, Pooja Gakhad, Pradeep Kumar Yadav, Abhishek Kumar Singh, Chandra Sekhar Tiwary, Krishanu Biswas, Sudhanshu Sharma","doi":"10.1002/adsu.202400219","DOIUrl":"https://doi.org/10.1002/adsu.202400219","url":null,"abstract":"Here metal support interaction (MSI) is demonstrated in a high entropy alloy (HEA: CoCuFeMnNi) supported CeO<jats:sub>2</jats:sub>. The HEA behaves as an active dry reforming catalyst only when it is supported over CeO<jats:sub>2</jats:sub> oxide, clearly demonstrating MSI. Based on spectroscopic and microscopic observations, it is envisaged that the substitutional effect is the one that causes the lattice oxygen activation, an important active species during DRM reaction. Transient studies are performed to understand the surface chemistry of the interaction between methane and CO<jats:sub>2</jats:sub> in the presence of a catalyst, which results in a methane decomposition first to generate hydrogen and carbon and followed by a CO<jats:sub>2</jats:sub> reaction to give CO using deposited carbon. The experimental observations are further proven by mechanistic study with DFT calculations which show a major contribution of H‐assisted CO<jats:sub>2</jats:sub> dissociation and pre‐H<jats:sub>2</jats:sub> releasing carbon depositing CH<jats:sub>4</jats:sub> dissociation and a minor contribution of pre‐CO releasing H<jats:sub>2</jats:sub> formation. This MSI moves the d‐band center of the Co atoms of CoCuFeMnNi/CeO<jats:sub>2</jats:sub> to the closest position of the Fermi level as compared to the isolated nanoparticles. This study can be taken as a proof of concept to demonstrate that MSI can be generated in the HEA/CeO<jats:sub>2</jats:sub> catalysts for a generic heterogeneous gas phase reaction.","PeriodicalId":7294,"journal":{"name":"Advanced Sustainable Systems","volume":null,"pages":null},"PeriodicalIF":7.1,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141568054","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Advancing Sustainable Building Materials: Reducing Formaldehyde Emissions in Medium Density Fiber Boards with Lignin Nanoparticles 推进可持续建筑材料:用木质素纳米颗粒降低中密度纤维板的甲醛释放量
IF 6.5 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-05 DOI: 10.1002/adsu.202400102
Ali Dorieh, Farideh Pahlavan, Kateřina Hájková, Štěpán Hýsek, Mohammad Farajollah Pour, Elham H. Fini

The pressing need to develop eco-friendly polymer materials for building applications has led to increased interest in modifying existing polymer systems. In this study, a sustainable approach to augmenting urea-formaldehyde (UF) resins, widely employed in wood-based panels is introduced. Addressing this, formaldehyde-scavenger demethylated lignin nanoparticles into UF resins, aiming to produce a green and enhanced medium-density-fiberboard (MDF) with minimal formaldehyde emissions is incorporated. The results indicate that increasing concentrations of demethylated lignin nanoparticles in the UF adhesive, there is not only a reduction in formaldehyde emissions from MDF composites but also a significant decrease in thickness swelling. The highest reduction in formaldehyde emission is observed in the MDF composite prepared with UF resin containing 7% lignin nanoparticles (UF-7NL), with an emission of 2.9 mg/100 g, marking a substantial decrease of 74% compared to emission of 11.2 mg/100 g from neat resin. Importantly, this reduction does not compromise physical and mechanical properties of the MDF; they remain comparable to boards bonded with unmodified UF. Molecular modeling revealed that lignin effectively traps formaldehyde, incorporating it as -CH2OH groups, leading to a notable decrease in formaldehyde emission from MDF. This approach offers an eco-friendly modification to a common polymer, showcasing lignin nanoparticles as innovative additives. 

由于急需为建筑应用开发生态友好型聚合物材料,人们对改良现有聚合物体系的兴趣与日俱增。在本研究中,介绍了一种可持续的方法来增强广泛用于人造板的脲醛(UF)树脂。为了解决这个问题,在 UF 树脂中加入了甲醛清除剂脱甲基木质素纳米粒子,旨在生产出甲醛释放量最小的绿色增强型中密度纤维板(MDF)。结果表明,随着超滤粘合剂中去甲基化木质素纳米粒子浓度的增加,中密度纤维板复合材料的甲醛释放量不仅会减少,而且厚度膨胀也会显著降低。使用含 7% 木质素纳米颗粒的 UF 树脂(UF-7NL)制备的中密度纤维板复合材料的甲醛释放量降低幅度最大,释放量为 2.9 毫克/100 克,与纯树脂的 11.2 毫克/100 克释放量相比,大幅降低了 74%。重要的是,这种减少并没有影响中密度纤维板的物理和机械性能;它们仍然与未改性 UF 粘合的板材相当。分子建模显示,木质素能有效捕获甲醛,并将其转化为 -CH2OH 基团,从而显著降低了中密度纤维板的甲醛释放量。这种方法对普通聚合物进行了环保改性,展示了作为创新添加剂的木质素纳米颗粒。
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引用次数: 0
Disproportionation and Transalkylation of Phenol and Dimethylphenol on Zeolite Catalysts 苯酚和二甲基苯酚在沸石催化剂上的歧化和反烷基化反应
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-02 DOI: 10.1002/adsu.202400276
Junyu Mao, Naiwang Liu, Xuan Meng, Li Shi
Substantial amounts of phenolic compounds are present in medium‐low temperature coal tar (MLCT), of which dimethylphenol (DMP) is not as valuable to be utilized as the more abundant cresol due to its complex composition and difficulty in isolation. In this study, the disproportionation and transalkylation reactions of MLCT‐related model compound, i.e., 2,6‐DMP, in phenol over zeolite catalysts are investigated using a fixed‐bed reactor for sustainable new option to utilize MLCT‐derived phenolic mixtures. Reactivity is promoted at high temperatures and associated with zeolite acidity and pore structure. Since disproportionation and transalkylation reactions have certain spatial requirements, the micropores of MFI‐type zeolite may cause spatial barriers that make it difficult to carry out the reactions. MCM‐22, characterized by MWW‐type zeolite, maximized the conversion of 2,6‐DMP due to its strong Bronsted acidity and large mesopore volume. FAU‐type zeolite HY with a 3D large 12‐ring through‐channel shows relatively small spatial confinement and certain molecular sieving ability, which enables bimolecular reactions while allowing cresols to flow out of the pores efficiently to obtain the highest cresol selectivity. The addition of phenol significantly inhibits the spontaneous disproportionation of 2,6‐DMP to tricresol. Besides, o‐cresol dominate the cresol products, suggesting that the selectivity of o‐cresol is kinetically controlled.
中低温煤焦油(MLCT)中含有大量酚类化合物,其中二甲基苯酚(DMP)由于成分复杂且难以分离,其利用价值不如含量更高的甲酚。本研究使用固定床反应器研究了 MLCT 相关模型化合物(即 2,6-DMP)在沸石催化剂上与苯酚的歧化和反烷基化反应,为利用 MLCT 衍生的酚类混合物提供了可持续的新选择。反应活性在高温下得到促进,并与沸石的酸度和孔结构有关。由于歧化和反烷基化反应有一定的空间要求,MFI 型沸石的微孔可能会造成空间障碍,使反应难以进行。以 MWW 型沸石为特征的 MCM-22 由于具有强勃朗斯特酸性和较大的中孔体积,最大限度地提高了 2,6-DMP 的转化率。具有三维大 12 环通孔的 FAU 型沸石 HY 显示出相对较小的空间限制和一定的分子筛分能力,在实现双分子反应的同时,还能使甲酚有效地流出孔道,从而获得最高的甲酚选择性。苯酚的加入明显抑制了 2,6-DMP 与三甲酚的自发歧化反应。此外,邻甲酚在甲酚产物中占主导地位,这表明邻甲酚的选择性是受动力学控制的。
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引用次数: 0
Nitrogen‐Doped Carbon‐Encapsulated Nickel Nanoparticle Catalysts Using Covalent Organic Frameworks as Templates for Electrochemical CO2 Conversion 以共价有机框架为模板的掺氮碳包封镍纳米粒子催化剂用于电化学二氧化碳转化
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-02 DOI: 10.1002/adsu.202400284
Yuzhen Zhao, Xinxin Yu, Zhuangzhuang Wu, Yongpeng Li, Wenxin Wang, Lijuan Feng, Zhuyin Sui, Qi Chen
Electrochemical CO2 reduction (ECR) reactions, powered by cleaner energy, possess significant promise in mitigating CO2 emissions and achieving carbon recycling. Herein, Ni@N‐C electrocatalysts with encapsulated structures are prepared using covalent organic frameworks (COFs) as templates, where COF‐derived nitrogen‐doped carbon (N‐C) is utilized to wrap Ni nanoparticles. At the potential of −0.97 V vs. RHE, 2Ni@N‐C‐800 is characterized by a high current density (j = 24.2 mA cm‐2) and relatively high CO Faraday efficiency (FECO = 72%), reflecting its good catalytic activity. The ECR performance of 2Ni@N‐C‐800 is due to the cooperative interaction between Ni nanoparticles and the N‐C structure, which is inferred from control and poisoning measurements. This study provides a new idea for finding efficient and stable ECR catalysts.
以清洁能源为动力的电化学二氧化碳还原(ECR)反应在减少二氧化碳排放和实现碳循环方面前景广阔。本文以共价有机框架(COF)为模板,制备了具有封装结构的 Ni@N-C 电催化剂,其中利用 COF 衍生的掺氮碳(N-C)来包裹 Ni 纳米粒子。在相对于 RHE 的 -0.97 V 电位下,2Ni@N-C-800 具有高电流密度(j = 24.2 mA cm-2)和相对较高的一氧化碳法拉第效率(FECO = 72%),反映了其良好的催化活性。2Ni@N-C-800 的 ECR 性能得益于镍纳米颗粒与 N-C 结构之间的协同作用,这是从控制和中毒测量中推断出来的。这项研究为寻找高效稳定的 ECR 催化剂提供了新思路。
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引用次数: 0
Effective Liquid Electrolytes for Enabling Room‐Temperature Sodium–Sulfur Batteries 实现室温钠硫电池的有效液态电解质
IF 7.1 3区 材料科学 Q2 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY Pub Date : 2024-07-02 DOI: 10.1002/adsu.202400268
Vittorio Marangon, Edoardo Barcaro, Francesco De Boni, Mirko Prato, Dominic Bresser, Jusef Hassoun
Glyme‐based electrolytes for sodium‐sulfur (Na–S) batteries are proposed for advanced cell configuration. Solutions of NaClO4 or NaCF3SO3 in tetraglyme are investigated in terms of thermal stability, ionic conductivity, Na+‐transference number, electrochemical stability, stripping‐deposition ability, and chemical stability in Na‐cells. Subsequently, versions of the electrolytes doped with fluoroethylene carbonate (FEC) are prepared using 0.5, 1, 2, or 3% additive weight concentrations, and evaluated by adopting the same approach used for the bare solutions. Scanning electron microscopy (SEM) provides morphological details of the passivation layer formed on the Na electrodes, while X‐ray photoelectron spectroscopy (XPS) sheds light on its composition. The most relevant achievement of the FEC‐added electrolyte is the suppression of the polysulfide shuttle in Na–S cells using a cathode with 70 wt.% of sulfur in the composite. This result appears even more notable considering the low amount of the additive requested for enabling the reversible cell operation. The solutions using 1% of FEC show the best compromise between cell performance and stability. Cyclic voltammetry (CV) displays the potential region related to the FEC electrochemical process responsible for Na–S cell operation. The understanding of the electrolyte features enables additional cycling tests using sulfur cathode with an optimized current collector, increased specific capacity, and coulombic efficiency.
针对钠硫(Na-S)电池的先进电池配置,提出了基于甘油的电解质。研究了 NaClO4 或 NaCF3SO3 在四聚乙二醇中的溶液在钠电池中的热稳定性、离子电导率、Na+ 传递数、电化学稳定性、剥离沉积能力和化学稳定性。随后,使用 0.5、1、2 或 3% 的添加剂重量浓度制备了掺有氟碳酸乙烯酯 (FEC) 的电解质,并采用与裸溶液相同的方法进行了评估。扫描电子显微镜 (SEM) 提供了在 Na 电极上形成的钝化层的形态细节,而 X 射线光电子能谱 (XPS) 则揭示了其成分。添加了 FEC 的电解质最重要的成果是抑制了使用含硫量为 70 wt.% 的复合阴极的 Na-S 电池中的多硫穿梭现象。考虑到实现电池可逆运行所需的添加剂量较低,这一结果显得更为显著。使用 1% FEC 的溶液显示出电池性能和稳定性之间的最佳折衷。循环伏安法 (CV) 显示了与 Na-S 电池运行的 FEC 电化学过程有关的电位区域。了解了电解质的特性后,就可以使用硫阴极进行更多循环测试,从而优化集流器,提高比容量和库仑效率。
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Advanced Sustainable Systems
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