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Development of Double-Side Ordered Membrane Electrode Assembly Based on Titanium Nitride Nanoarrays 开发基于氮化钛纳米阵列的双面有序膜电极组件
Pub Date : 2024-03-21 DOI: 10.1039/d4im00008k
Lingfeng Xuan, Deqing Mei, Caiying Zhou, Wenze Mao, Yancheng Wang
The membrane electrode assembly (MEA) plays a crucial role in the functionality of proton exchange membrane fuel cells (PEMFCs). The channels present within the catalyst layer of MEAs exhibit a disordered configuration, which consequently give rise to low efficiency in mass transportation. This paper presents a novel double-side ordered MEA to improve its both mass transport performance and durability. Using seed-assisted hydrothermal reaction and nitriding treatment, TiN nanorods array was synthesized on ITO surface and the catalyst was uniformly coated onto the TiN support by ultrasonic spraying. After that the double-side ordered MEA was fabricated employing a transfer printing process. The electrochemical testing was conducted to evaluate the MEA’s performance, and results showed that the double-side ordered MEA can generate a peak power of 678.30 mW/cm2 with platinum loading of 0.2 mg/cm2. After chemical accelerated stress test operation, the peak performance degradation was 5%. These results provide substantial evidence for the effectiveness of our developed double-side ordered MEA can mitigate catalyst polarization corrosion. Thus, this study reveals the immense potential of the TiN nanorod array-based double-side ordered MEA could advance the development of efficient and stable MEAs.
膜电极组件(MEA)在质子交换膜燃料电池(PEMFC)的功能中起着至关重要的作用。质子交换膜燃料电池催化剂层内的通道呈现出无序配置,因此在大规模运输中效率较低。本文介绍了一种新型双面有序 MEA,以改善其质量传输性能和耐用性。利用种子辅助水热反应和氮化处理,在 ITO 表面合成了 TiN 纳米棒阵列,并通过超声喷涂将催化剂均匀涂覆在 TiN 支承上。然后采用转移印刷工艺制作了双面有序 MEA。电化学测试评估了 MEA 的性能,结果表明,在铂负载为 0.2 mg/cm2 的情况下,双面有序 MEA 可产生 678.30 mW/cm2 的峰值功率。经过化学加速应力测试操作后,峰值性能衰减为 5%。这些结果充分证明了我们开发的双面有序 MEA 能够有效缓解催化剂极化腐蚀。因此,这项研究揭示了基于 TiN 纳米棒阵列的双面有序 MEA 的巨大潜力,可推动高效、稳定 MEA 的发展。
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引用次数: 0
Improvement of Octane Number in FCC Gasoline Through the Extraction with Urea/Thiourea Complex based on Property Analysis 基于性能分析的尿素/硫脲复合物萃取法改善催化裂化汽油的辛烷值
Pub Date : 2024-03-16 DOI: 10.1039/d4im00005f
Lin Gao, Chunyu Geng, Botao Teng, Hongwei Xiang, Xiaodong Wen, Yong Yang, Yongwang Li
In this paper, the uses urea/thiourea complexation approach was employed to enhance octane number of FCC gasoline by extracting n-alkanes. It was observed that adding thiourea improved the removal of n-alkanes from the gasoline, and matching results were obtained through the experiments using model samples. Molecular dynamics simulation revealed that the stability of urea complexes increased with raising carbon number of n-alkanes, while lighter n-alkane molecules exhibited lower propensity for complex formation with urea. This finding is in line with the results of DSC measurement at decomposition temperature. Furthermore, infrared spectrum analysis, XRD characterization, and reaction heat measurements indicated that although thiourea was introduced into the reaction system, it did not actively participate in the complexation reaction. In summary, the introduction of thiourea resulted in an increased solubility of urea in ethanol solution and enhanced reaction heat, suggesting its beneficial role in promoting urea complex formation and facilitating n-alkane removal from FCC gasoline.
本文采用尿素/硫脲络合方法,通过萃取正构烷烃来提高催化裂化汽油的辛烷值。研究发现,添加硫脲可提高汽油中正烷烃的去除率,并通过使用模型样品进行实验获得了与之匹配的结果。分子动力学模拟显示,尿素复合物的稳定性随着正构烷烃碳数的增加而增加,而较轻的正构烷烃分子与尿素形成复合物的倾向性较低。这一发现与分解温度下的 DSC 测量结果一致。此外,红外光谱分析、XRD 表征和反应热测量结果表明,虽然反应体系中引入了硫脲,但硫脲并没有积极参与络合反应。总之,硫脲的引入增加了尿素在乙醇溶液中的溶解度并提高了反应热,这表明硫脲在促进尿素络合物的形成和促进催化裂化汽油中正烷烃的脱除方面发挥了有益的作用。
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引用次数: 0
Cross-polymerization between bio-oil and polyaniline: synergistic effects on pore development in subsequent activation and adsorption of phenol 生物油与聚苯胺之间的交叉聚合:对随后活化和吸附苯酚过程中孔隙发育的协同效应
Pub Date : 2024-03-07 DOI: 10.1039/d4im00001c
Baihong Li, Chao Li, Dianqiang Li, Lijun Zhang, Shu Zhang, Yi Wang, Song Hu, Jun Xiang, Mortaza Gholizadeh, Xun Hu
Bio-oil is a major product from pyrolysis of biomass which serves as a carbon source to produce carbon material due to its high reactivity towards polymerization itself or cross-polymerization with other organic feedstocks. In this study, activation of polyaniline (PANI) mixed with wheat straw-derived bio-oil and K2C2O4 at 800 °C was conducted, aiming to understand the effect of potential interactions of bio-oil with PANI on pore development of resulting activated carbon (AC). The results revealed cross-polymerization reactions between PANI and bio-oil during direct activation, which increased the yield of AC from 13.0% (calculated average) to 15.0%, the specific surface area from 1677.9 m2 g−1 (calculated average) to 1771.3 m2 g−1, and the percentage of micropores from 94.3% to 97.1%. In addition, pre-polymerization of PANI and bio-oil at 200 °C before activation was also conducted. Such pretreatment could increase the AC yield from 13.0% to 23.3%, but the specific surface area decreased to 1381.8 m2 g−1. The pre-polymerization formed the organics that were more resistant towards cracking/gasification, but introduced oxygen-rich functionalities. This made AC highly hydrophilic, rendering a much higher capability for adsorption of phenol despite the smaller specific surface area. Additionally, the AC with developed pore structures facilitated dispersion of nickel in Ni/AC and enhanced the catalytic activity for hydrogenation of o-chloronitrobenzene and vanillin.
生物油是生物质热解的主要产物,由于其本身具有高聚合反应活性或与其他有机原料发生交叉聚合反应,因此可作为生产碳材料的碳源。本研究在 800 °C 下对混合了小麦秸秆生物油和 K2C2O4 的聚苯胺(PANI)进行了活化,旨在了解生物油与 PANI 的潜在相互作用对生成的活性炭(AC)孔隙发育的影响。结果表明,在直接活化过程中,PANI 和生物油之间发生了交叉聚合反应,使活性炭的产率从 13.0%(计算平均值)提高到 15.0%,比表面积从 1677.9 m2 g-1(计算平均值)提高到 1771.3 m2 g-1,微孔百分比从 94.3% 提高到 97.1%。此外,还在活化前对 PANI 和生物油进行了 200 °C 的预聚合。这种预处理可将交流电收率从 13.0% 提高到 23.3%,但比表面积降至 1381.8 m2 g-1。预聚合形成的有机物更耐开裂/气化,但引入了富氧官能团。这使得 AC 具有很强的亲水性,尽管比表面积较小,但吸附苯酚的能力却大大提高。此外,具有发达孔隙结构的 AC 还有利于镍在 Ni/AC 中的分散,并提高了邻氯硝基苯和香兰素氢化的催化活性。
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引用次数: 0
Liquid-based electronic materials for bioelectronics: current trends and challenges 用于生物电子学的液基电子材料:当前趋势与挑战
Pub Date : 2024-03-05 DOI: 10.1039/D3IM00122A
Kijun Park, Sangwoo Park, Yejin Jo, Soo A. Kim, Tae Young Kim, Sangwon Kim and Jungmok Seo

Liquid-based materials have emerged as promising soft materials for bioelectronics due to their defect-free nature, conformability, robust mechanical properties, self-healing, conductivity, and stable interfaces. A liquid is infiltrated into a structuring material endowing the material with a liquid-like behavior. Liquid-based electronics with favorable features are being designed and engineered to meet requirements of practical applications. In this review, various types of liquid-based electronic materials and the recent progress on bioelectronics in multiple applications are summarized. Liquid-based electronic materials include ionic liquid hydrogel, nanomaterial-incorporated hydrogel, liquid metal, liquid-infused encapsulation, and liquid-based adhesive. These materials are demonstrated via electronic applications, including strain sensor, touch sensor, implantable stimulator, encapsulation, and adhesive as necessary components comprising electronics. Finally, the current challenges and future perspective of liquid-based electronics are discussed.

Keywords: Bioelectronics; Liquid metal; Soft electronics; Hydrogel electronics; Lubricant-infused.

液基材料因其无缺陷、保形性、坚固的机械性能、自愈性、导电性和稳定的界面,已成为生物电子学领域前景广阔的软材料。液体渗透到结构材料中,使材料具有类似液体的特性。目前正在设计和制造具有这些优点的液基电子器件,以满足实际应用的要求。本综述概述了各种类型的液基电子材料及其在生物电子学多种应用中的最新进展。液基电子材料包括离子液体水凝胶、纳米材料融入水凝胶、液态金属、液体注入封装和液基粘合剂。这些材料通过电子应用进行了展示,包括应变传感器、触摸传感器、植入式刺激器、封装和粘合剂等电子产品的必要组成部分。最后,还讨论了液基电子学当前面临的挑战和未来展望。
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引用次数: 0
Enhancing conversion using diffusio-osmosis from patterned catalytic surfaces 利用图案化催化表面的扩散渗透作用提高转化率
Pub Date : 2024-03-01 DOI: 10.1039/D3IM00130J
Aura Visan, Jeffery A. Wood and Rob G. H. Lammertink

An inhomogeneous catalyst surface leads to concentration gradients along this surface, which can generate diffusio-osmotic flows. The magnitude of this surface flow and the extent to which it impacts the catalytic conversion is numerically investigated and depends foremost on the reaction kinetics of the system and the surface-species interactions expressed via the diffusio-osmotic mobility. We present general scaling laws based on the reaction kinetics and interaction potential between chemical species and the catalytic surface, captured in a single parameter. We further investigate the optimal catalyst coverage in order to maximize the benefit of these surface flows.

Keywords: Diffusio-osmosis; Catalysis; Transport; Enhancement.

不均匀的催化剂表面会导致沿该表面的浓度梯度,从而产生扩散渗流。我们对这种表面流动的大小及其对催化转化的影响程度进行了数值研究,研究结果主要取决于系统的反应动力学以及通过扩散渗透流动性表现出来的表面-物种相互作用。我们提出了基于反应动力学和化学物种与催化表面之间相互作用势的一般缩放定律,并以单一参数加以体现。我们进一步研究了催化剂的最佳覆盖范围,以便最大限度地发挥这些表面流动的优势。
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引用次数: 0
Multi-component liquid-infused systems: a new approach to functional coatings 多组分液体注入系统:功能涂料的新方法
Pub Date : 2024-02-23 DOI: 10.1039/D4IM00003J
Zachary Applebee and Caitlin Howell

Antifouling liquid-infused surfaces have generated interest in multiple fields due to their diverse applications in industry and medicine. In nearly all reports to date, the liquid component consists of only one chemical species. However, unlike traditional solid surfaces, the unique nature of liquid surfaces holds the potential for synergistic and even adaptive functionality simply by including additional elements in the liquid coating. In this work, we explore the concept of multi-component liquid-infused systems, in which the coating liquid consists of a primary liquid and a secondary component or components that provide additional functionality. For ease of understanding, we categorize recently reported multi-component liquid-infused surfaces according to the size of the secondary components: molecular scale, in which the secondary components are molecules; nanoscale, in which they are nanoparticles or their equivalent; and microscale, in which the additional components are micrometer size or above. We present examples at each scale, showing how introducing a secondary element into the liquid can result in synergistic effects, such as maintaining a pristine surface while actively modifying the surrounding environment, which are difficult to achieve in other surface treatments. The review highlights the diversity of fabrication methods and provides perspectives on future research directions. Introducing secondary components into the liquid matrix of liquid-infused surfaces is a promising strategy with significant potential to create a new class of multifunctional materials.

Keywords: Active surfaces; Antimicrobial; Antifouling; Interfaces; Sensing surfaces.

注入液体的防污表面因其在工业和医学领域的多种应用而在多个领域引起了人们的兴趣。在迄今为止的几乎所有报告中,液体成分都只包含一种化学物质。然而,与传统的固体表面不同,液体表面的独特性质蕴含着协同甚至自适应功能的潜力,只需在液体涂层中加入额外的元素即可。在这项工作中,我们探索了多组分液体注入系统的概念,其中涂层液体由一种主要液体和一种或多种提供附加功能的次要成分组成。为了便于理解,我们根据次要成分的大小对最近报道的多组分液体注入表面进行了分类:分子级,其中次要成分为分子;纳米级,其中次要成分为纳米颗粒或等效物;微米级,其中附加成分为微米或以上大小。我们介绍了每种尺度的实例,展示了在液体中引入辅助元素如何产生协同效应,例如在保持原始表面的同时积极改变周围环境,而这是其他表面处理方法难以实现的。综述强调了制造方法的多样性,并对未来的研究方向提出了展望。在液体注入表面的液体基质中引入辅助成分是一种前景广阔的策略,具有创造新型多功能材料的巨大潜力。
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引用次数: 0
Triphase photocatalytic water-gas-shift reaction for hydrogen production with enhanced interfacial diffusion at gas–liquid–solid interfaces† 三相光催化水气变换反应制氢,增强气-液-固界面的界面扩散能力
Pub Date : 2024-02-20 DOI: 10.1039/D3IM00135K
Huige Chen, Zhenhua Li, Chao Zhou, Run Shi and Tierui Zhang

The exothermic characteristic of the water-gas-shift (WGS) reaction, coupled with the thermodynamic constraints at elevated temperatures, has spurred a research inclination towards conducting the WGS reaction at reduced temperatures. Nonetheless, the challenge of achieving efficient mass transfer between gaseous CO and liquid H2O at the photocatalytic interface under mild reaction conditions hinders the advancement of the photocatalytic WGS reaction. In this study, we introduce a gas–liquid–solid triphase photocatalytic WGS reaction system. This system facilitates swift transportation of gaseous CO to the photocatalyst's surface while ensuring a consistent water supply. Among various metal-loaded TiO2 photocatalysts, Rh/TiO2 nanoparticles positioned at the triphase interface demonstrated an impressive H2 production rate of 27.60 mmol g−1 h−1. This rate is roughly 2 and 10 times greater than that observed in the liquid–solid and gas–solid diphase systems. Additionally, finite element simulations indicate that the concentrations of CO and H2O at the gas–liquid–solid interface remain stable. This suggests that the triphase interface establishes a conducive microenvironment with sufficient CO and H2O supply to the surface of photocatalysts. These insights offer a foundational approach to enhance the interfacial mass transfer of gaseous CO and liquid H2O, thereby optimizing the photocatalytic WGS reaction's efficiency.

Keywords: Water-gas-shift; Photocatalysis; Triphase interface; Hydrogen evolution; TiO2.

水气变换(WGS)反应的放热特性,加上高温下的热力学限制,促使研究人员倾向于在较低温度下进行 WGS 反应。然而,在温和的反应条件下实现气态 CO 和液态 H2O 在光催化界面上的高效传质这一难题阻碍了光催化 WGS 反应的发展。在本研究中,我们介绍了一种气液固三相光催化 WGS 反应系统。该系统有助于将气态 CO 迅速输送到光催化剂表面,同时确保稳定的水供应。在各种负载金属的二氧化钛光催化剂中,位于三相界面的 Rh/TiO2 纳米粒子的 H2 产率高达 27.60 mmol g-1 h-1。这一速率比在液固和气固二相体系中观察到的速率分别高出约 2 倍和 10 倍。此外,有限元模拟表明,气-液-固界面的 CO 和 H2O 浓度保持稳定。这表明三相界面建立了一个有利的微环境,为光催化剂表面提供了充足的 CO 和 H2O。这些见解为加强气态 CO 和液态 H2O 的界面传质,从而优化光催化 WGS 反应的效率提供了一种基础方法。
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引用次数: 0
Strategies to enable microsized alloy anodes for high-energy and long-life alkali-ion batteries 为高能量、长寿命碱性离子电池实现微尺寸合金阳极的策略
Pub Date : 2024-02-16 DOI: 10.1039/d3im00126a
Amine Daali, Rachid Amine, Wilkistar A Otieno, Gui-Liang Xu, Khalil Amine
Micro-sized anode materials demonstrate greater potential for practical applications than nanomaterials in the aspects of volumetric energy density, Coulombic efficiency, fabrication process, and cost. However, the huge volume changes of alloy anodes (up to ~ 500%) during repeated charge/discharge has led to a series of challenging issues including pulverization of active material particles and delamination from current collectors, formation of thick anf fragile solid-electrolyte interphase (SEI) and depletion of electrolytes, eventually leading to rapid cell degradation. Herein, we review recent progress of rational strategies to enable the use of microsized alloy anodes (Si, P, Sb, Sn, etc.) including electrolyte modulation, binder design and architecture engineering. We also provide perspectives on future directions and remaining challenges of microsized anodes towards practical applications.
与纳米材料相比,微尺寸阳极材料在体积能量密度、库仑效率、制造工艺和成本等方面具有更大的实际应用潜力。然而,合金阳极在反复充放电过程中的巨大体积变化(高达约 500%)导致了一系列具有挑战性的问题,包括活性材料颗粒的粉碎和与集流器的分层、厚而脆弱的固电解质相(SEI)的形成以及电解质的耗竭,最终导致电池的快速降解。在此,我们回顾了使用微尺寸合金阳极(Si、P、Sb、Sn 等)的合理策略的最新进展,包括电解质调节、粘合剂设计和结构工程。我们还展望了微尺寸阳极走向实际应用的未来方向和仍然面临的挑战。
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引用次数: 0
Theoretical Investigation of Carbon Dioxide on MgH2 with Cobalt Catalyst 钴催化剂在 MgH2 上的二氧化碳理论研究
Pub Date : 2024-01-26 DOI: 10.1039/d3im00096f
Sara Rozas Azcona, Fabiana C. Gennari, Mert Atilhan, Alfredo Bol, Santiago Aparicio
This research paper presents a theoretical investigation of carbon dioxide (CO2) methanation using MgH2 as a hydrogen source with cobalt (Co) as a catalyst. The focus of this study is on the properties and mechanisms involved in the CO2 adsorption on clean MgH2 surfaces and the role of Co catalysts in enhancing the adsorption process. Density functional theory (DFT) calculations were performed to examine different CO2 adsorption sites on the MgH2 surface, including adsorption distances, binding energies, and geometric parameters. The results indicate that physical adsorption of CO2 occurs on MgH2, with similar adsorption energies observed across the different adsorption sites. The coverage effect of CO2 molecules on MgH2 was also investigated, revealing an increased affinity of CO2 with higher surface coverage. However, excessive coverage led to a decrease in adsorption efficiency due to competing surface adsorption and intermolecular interactions. The orientation of adsorbed CO2 molecules shifted from parallel to pseudo-perpendicular arrangements upon adsorption, with notable deformations observed at higher coverage. Furthermore, the study explores the CO2 adsorption capacity of MgH2 in comparison to other materials reported in the literature, showcasing its medium to strong affinity for CO2. Additionally, the effectiveness of Co single atoms and Co clusters as catalysts for CO2 adsorption on MgH2 was examined. Overall, this theoretical investigation provides insights into the CO2 adsorption properties of MgH2 and highlights the potential of Co catalysts in enhancing the efficiency of the methanation process.
本研究论文介绍了以 MgH2 为氢源、钴 (Co) 为催化剂进行二氧化碳 (CO2) 甲烷化的理论研究。本研究的重点是二氧化碳在洁净 MgH2 表面的吸附特性和机理,以及 Co 催化剂在增强吸附过程中的作用。通过密度泛函理论(DFT)计算,研究了 MgH2 表面不同的二氧化碳吸附位点,包括吸附距离、结合能和几何参数。结果表明,二氧化碳在 MgH2 上发生了物理吸附,不同吸附位点的吸附能相似。此外,还研究了二氧化碳分子在 MgH2 上的覆盖效应,发现表面覆盖率越高,二氧化碳的亲和力越强。然而,由于表面吸附和分子间相互作用的竞争,过高的覆盖率会导致吸附效率下降。吸附后,被吸附的二氧化碳分子的取向从平行排列转变为假垂直排列,在较高的覆盖率下观察到明显的变形。此外,该研究还探讨了 MgH2 对二氧化碳的吸附能力,并与文献报道的其他材料进行了比较,结果表明 MgH2 对二氧化碳具有中等至较强的亲和力。此外,研究还考察了 Co 单原子和 Co 簇作为催化剂在 MgH2 上吸附二氧化碳的有效性。总之,这项理论研究深入揭示了 MgH2 的二氧化碳吸附特性,并强调了 Co 催化剂在提高甲烷化过程效率方面的潜力。
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引用次数: 0
Recent progress in nickel single-atom catalysts for the electroreduction of CO2 to CO 将 CO2 电还原为 CO 的镍单原子催化剂的最新进展
Pub Date : 2024-01-09 DOI: 10.1039/d3im00109a
Ziyan Yang, Rongzhen Chen, Ling Zhang, Yuhang Li, Chunzhong Li
The electrocatalytic reduction of carbon dioxide (CO2) is considered an effective strategy for mitigating the energy crisis and the greenhouse effect. Nickel is widely used in single-atom catalysts (SACs) owing to its special electronic structure. In this minireview, the basic principles of Ni SACs in the electrocatalytic reduction of CO2 to CO are first described. Subsequently, Ni SACs are divided into three categories depending on different strategies used to improve properties. The synthesis, morphology, performance and theoretical calculations of the catalysts are also described. Finally, an overview of the existing challenges and perspectives of Ni SACs for CO2 reduction is presented.
电催化还原二氧化碳(CO2)被认为是缓解能源危机和温室效应的有效策略。镍因其特殊的电子结构而被广泛应用于单原子催化剂(SAC)中。在本小视图中,首先介绍了镍单原子催化剂在电催化将 CO2 还原成 CO 的过程中的基本原理。随后,根据改善性能的不同策略,Ni SACs 被分为三类。此外,还介绍了催化剂的合成、形态、性能和理论计算。最后,概述了用于二氧化碳还原的 Ni SACs 目前面临的挑战和前景。
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引用次数: 0
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Industrial Chemistry & Materials
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