IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-10-09 DOI: 10.1016/j.carbon.2024.119689

Akash Bhimrao Shirsath , Manas Mokashi , Reihaneh Pashminehazar , Ahmet Çelik , Patrick Lott , Steffen Tischer , Jan-Dierk Grunwaldt , Olaf Deutschmann

Methane pyrolysis is a promising method for eco-friendly hydrogen production, but soot formation and carbon interaction pose challenges for scaling up. Therefore, understanding the dynamics of soot formation and carbon deposition is crucial. This study delves into the intricacies of soot formation in methane pyrolysis under industrially relevant conditions, namely operations at atmospheric pressure, employing a H₂:CH₄ ratio of 2 and exploring a range of hot zone temperatures (1473 K, 1573 K, 1673 K, and 1773 K) with a 5 s residence time. Utilizing a detailed gas-phase kinetic model with direct carbon deposition reactions, the research adopts the method of moments coupled with a one-dimensional plug flow reactor model to simulate soot formation. The model is validated by characterizing soot particles that were produced in a pyrolysis reactor by means of transmission electron microscopy, Dynamic light scattering (DLS), and Raman spectroscopy. Results show that lower temperatures lead to nucleation-dominated growth, whereas higher temperatures significantly restrain particle growth due to carbon deposition. DLS data indicate a complex balance between particle growth and deposition processes. These findings provide insights into operational parameters that can enhance reactor performance and sustainability in hydrogen production processes by mitigating soot and carbon deposition.

甲烷热解是一种很有前景的环保型制氢方法，但烟尘的形成和碳的相互作用给扩大规模带来了挑战。因此，了解煤烟形成和碳沉积的动态至关重要。本研究深入探讨了在工业相关条件下甲烷热解过程中烟尘形成的复杂性，即在常压下操作，采用 2 的 H2:CH4 比率，并探索一系列热区温度（1473 K、1573 K、1673 K 和 1773 K）和 5 秒停留时间。该研究利用详细的气相动力学模型与直接碳沉积反应，采用矩法结合一维塞流反应器模型模拟烟尘的形成。通过透射电子显微镜、动态光散射（DLS）和拉曼光谱对热解反应器中产生的烟尘颗粒进行表征，验证了该模型。结果表明，较低的温度会导致以成核为主的生长，而较高的温度则会由于碳沉积而明显抑制颗粒的生长。DLS 数据表明，颗粒生长和沉积过程之间存在复杂的平衡关系。这些发现为通过减少烟尘和碳沉积来提高反应器性能和制氢过程可持续性的操作参数提供了启示。

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引用次数: 0

Enhancing bond performance of carbon fiber reinforced plastic bars in concrete structures: Insights and guidelines 提高混凝土结构中碳纤维增强塑料条的粘结性能：启示与指南

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-10-05 DOI: 10.1016/j.carbon.2024.119685

Haksung Lee , Kwan-Woo Kim , Man Kwon Choi , Byung-Joo Kim , Young Chul Choi , Mauricio Terrones

This study examines the adhesion characteristics of fiber reinforced plastic (FRP) bars, specifically focusing on carbon fiber reinforced plastic (CFRP), within concrete matrices. Key findings underscore the significant influence of the concrete compressive strength values such as embedment length, surface treatment, and environmental conditions. Enhanced concrete compressive strength positively impacts interfacial strength, while longer embedment lengths result in weak interfaces within the composites. Surface treatment, particularly sand coating, is crucial when promoting higher interfacial bond strengths and adhesion. Comparisons with international design codes reveal discrepancies, with ACI 440.1R-15 closely matching test results. The study also highlights the advantages of using epoxy resins for FRP strengthening. In chloride environments, CFRP results in superior corrosion resistance when compared to basalt fiber reinforced polymer (BFRP) and glass fiber reinforced polymer (GFRP). However, interfacial bond strength retention decreases over prolonged exposure, exacerbated by wet-dry cycles and exposure to temperature fluctuations. Overall, this research provides valuable insights for selecting and designing robust concrete structures within FRP reinforcements, considering their advantages.

本研究探讨了纤维增强塑料（FRP）棒材，特别是碳纤维增强塑料（CFRP）棒材在混凝土基体中的粘附特性。主要发现强调了混凝土抗压强度值（如嵌入长度、表面处理和环境条件）的重要影响。混凝土抗压强度的提高会对界面强度产生积极影响，而较长的预埋长度则会导致复合材料内部的界面变得脆弱。表面处理，尤其是砂涂层，对于提高界面粘结强度和粘附力至关重要。与国际设计规范的比较显示出差异，ACI 440.1R-15 与测试结果非常吻合。研究还强调了使用环氧树脂进行玻璃钢加固的优势。在氯化物环境中，与玄武岩纤维增强聚合物（BFRP）和玻璃纤维增强聚合物（GFRP）相比，CFRP 具有更强的耐腐蚀性。然而，界面粘接强度保持率会随着长期暴露而降低，干湿循环和暴露于温度波动会加剧这种情况。总之，考虑到玻璃纤维增强聚合体的优势，这项研究为选择和设计使用玻璃纤维增强聚合体的坚固混凝土结构提供了有价值的见解。

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引用次数: 0

Magnetic biochar-doped g-C3N4/Fe2O3 S-scheme heterojunction with enhanced photocatalytic degradation of tetracycline by addition of persulfate 磁性生物炭掺杂 g-C3N4/Fe2O3 S 型异质结通过添加过硫酸盐增强四环素的光催化降解能力

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-10-01 DOI: 10.1016/j.carbon.2024.119681

Huijuan Yu , Jing Zhang , Ruiqi Zhai , Cuiping Gao , Yingjie Zhang , Chunmei Tian , Qiang Ma

Graphitic carbon nitride (g-C₃N₄) exhibits remarkable thermal and chemical stability, enabling effective activation of molecular oxygen and generation of superoxide radicals for photocatalytic pollutant degradation. However, its low surface area and poor photocatalytic activity have limited its development, and the reaction mechanism of pollutant degradation remains unclear. In this study, we synthesized g-C₃N₄/BC/Fe₂O₃ catalysts by combining g-C₃N₄, biochar (BC), and Fe₂O₃ in intimate contact. The highest photocatalytic degradation efficiency of tetracycline (TC) reached 94.9 % in the g-C₃N₄/BC/Fe₂O₃-2/PDS system, which was 3.01, 1.53, and 2.35 times higher than that of pure g-C₃N₄, BC, and BC/Fe₂O₃, respectively. The addition of persulfate (PDS) accelerated the formation of reactive oxygen species (ROS), providing more active species and improving photocatalytic performance, thereby enhancing TC degradation. LC-MS analysis and density functional theory (DFT) calculations were used to elucidate possible TC degradation pathways in the g-C₃N₄/BC/Fe₂O₃-2/PDS system. Electron paramagnetic resonance (EPR) confirmed the generation of multiple ROS in the reaction system, including h⁺, •OH, SO₄^•−, •O₂⁻, and ¹O₂. This work provides mechanistic insights into TC degradation and offers a theoretical foundation for future studies on advanced oxidation processes for water treatment.

氮化石墨（g-C3N4）具有显著的热稳定性和化学稳定性，可有效激活分子氧并生成超氧自由基，从而实现光催化降解污染物。然而，g-C3N4 的比表面积低、光催化活性差，限制了其发展，而且污染物降解的反应机理尚不清楚。本研究将 g-C3N4、生物炭（BC）和 Fe2O3 紧密接触，合成了 g-C3N4/BC/Fe2O3 催化剂。在 g-C3N4/BC/Fe2O3-2/PDS 体系中，四环素（TC）的最高光催化降解效率达到 94.9%，分别是纯 g-CN4、BC 和 BC/Fe2O3 的 3.01 倍、1.53 倍和 2.35 倍。过硫酸盐（PDS）的加入加速了活性氧（ROS）的形成，提供了更多的活性物种，改善了光催化性能，从而提高了 TC 的降解能力。LC-MS 分析和密度泛函理论（DFT）计算用于阐明 g-C3N4/BC/Fe2O3-2/PDS 系统中可能的 TC 降解途径。电子顺磁共振 (EPR) 证实了反应体系中生成了多种 ROS，包括 h+、-OH、SO4--、-O2- 和 1O2。这项研究从机理上揭示了三氯甲烷的降解过程，为今后研究用于水处理的高级氧化过程奠定了理论基础。

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引用次数: 0

High-strength and toughness CNT films from microwaving-promoted purification and structural reconstruction 微波促进纯化和结构重构的高强度和韧性 CNT 薄膜

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-30 DOI: 10.1016/j.carbon.2024.119680

Li Yan Zhang , Yu Ting Chen , Hang Zhan , Jian Nong Wang

Carbon nanotube (CNT) films can now be prepared by catalytic floating chemical vapor deposition (CVD) with low cost and high yield. However, their performance deteriorates drastically due to the presence of impurities and structural defects all over the films. In this study, we report a simple and fast heating and quenching approach to tackle this issue by using a household microwave oven. Experimental results show that the strong interaction between CNTs and low-power microwaves within 10 s not only triggered the diffusion of Fe particles from the interior to the surface of the film for easy purification but also improved the graphitic structure of CNTs and their inter-tube binding for mechanical strengthening and electrical conduction. After a sequential treatment of microwaving-acid washing-microwaving, followed by additional rolling, the final CNT film exhibited a tensile strength of 7.45 GPa, an elongation at break of 11.33 %, and an electrical conductivity of 1.85 × 10⁶ S m⁻¹. The combination of such mechanical and electrical properties is superior to previous fibers and films reported in open literature. Considering its efficient and environment-friendly features, the present approach is suitable for the large-scale production of high-performance CNT films, thereby meeting the requirements for practical applications in many fields.

碳纳米管（CNT）薄膜现在可以通过催化浮动化学气相沉积（CVD）法制备，成本低、产量高。然而，由于薄膜中存在杂质和结构缺陷，其性能急剧下降。在本研究中，我们利用家用微波炉报告了一种简单快速的加热和淬火方法来解决这一问题。实验结果表明，在 10 秒钟内，CNT 与低功率微波之间的强烈相互作用不仅引发了铁颗粒从薄膜内部向表面的扩散，便于提纯，而且改善了 CNT 的石墨化结构及其管间结合，增强了机械强度和导电性能。经过微波-酸洗-微波的连续处理，再经过滚压，最终的 CNT 薄膜显示出 7.45 GPa 的拉伸强度、11.33 % 的断裂伸长率和 1.85 × 106 S m-1 的导电率。这种机械和电气性能的结合优于以往公开文献中报道的纤维和薄膜。考虑到其高效、环保的特点，本方法适用于大规模生产高性能 CNT 薄膜，从而满足许多领域的实际应用要求。

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引用次数: 0

Controllable photoexfoliation of monolayer graphene quantum dots using temporally and spatially shaped femtosecond laser 利用时间和空间成形飞秒激光实现单层石墨烯量子点的可控光剥离

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-28 DOI: 10.1016/j.carbon.2024.119667

Junrui Wu , Le Ma , Lan Jiang , Xin Li , Shaoqian Wang , Mengyao Tian , Sumei Wang , Pei Zuo

Graphene quantum dots (GQDs) have displayed significant momentum in numerous fields due to their unique electronic properties. However, how to obtain uniformly monolayer quantum dots and explain the synthesis mechanism are still a key technical problem. Here, a rapid and controllable photoexfoliation rate of monolayer graphene quantum dots of up to 80 % was achieved by using temporally and spatially shaped femtosecond laser to ablate bulk highly oriented pyrolytic graphite targets in liquid. Theoretical calculations suggested that the temporally shaped laser can minimize the spatial range of electron excitation, maximize the Coulomb repulsion between the outer layers and Coulomb explosion within the topmost layer through multi-level electron excitation. The above multilevel photoexfoliations lead to the formation of monolayer GQDs. These findings demonstrate a perfect theoretical explanation of controllable and rapid preparation of monolayer quantum dots, accelerating its industrialization in energy storage devices.

石墨烯量子点（GQDs）因其独特的电子特性而在众多领域显示出巨大的发展潜力。然而，如何获得均匀的单层量子点并解释其合成机理仍是一个关键技术问题。在此研究中，利用时间和空间成形飞秒激光烧蚀液体中的块状高取向热解石墨靶，实现了单层石墨烯量子点的快速可控光剥离，其剥离率高达80%。理论计算表明，时间成形激光可使电子激发的空间范围最小化，通过多级电子激发使外层之间的库仑斥力和最上层内的库仑爆炸最大化。上述多级光致发光导致了单层 GQD 的形成。这些发现为单层量子点的可控和快速制备提供了完美的理论解释，加速了其在储能设备中的产业化进程。

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引用次数: 0

The role of carbon textile surface functionalities in reactive adsorption of vapor and liquid 2-chloroethyl ethyl sulfide: Evaluating interactions at the interface 碳织物表面功能性在反应吸附蒸汽和液体 2-氯乙基硫醚中的作用：评估界面上的相互作用

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-28 DOI: 10.1016/j.carbon.2024.119673

Paola S. Pauletto, Dimitrios A. Giannakoudakis, Marc Florent, Teresa J. Bandosz

A carbon textile (CT) was chemically modified to increase its surface activity and promote the adsorption and degradation of 2-chloroethyl ethyl sulfide (CEES) - a surrogate for mustard gas. CT was initially subjected to oxidation (CTO), and then heated under ammonia (CTON) or hydrogen sulfide (CTOS) atmosphere to incorporate nitrogen or sulfur functionalities, respectively. Detoxification experiments were performed in closed vials using either vapor or liquid forms of CEES. The maximum vapor weight uptakes on CT, CTO, CTOS, and CTON were 399, 372, 434, and 489 mg/g, respectively. All textiles were able to prevent the vaporization of CEES liquid droplets. Although similar reaction products were detected in both vapor and liquid systems, the marked differences in the extent of CEES chemical transformation on the surfaces of the textiles indicate distinct detoxification pathways influenced by surface chemistry. Even though the heterogeneous surface of CTO, enriched with oxygen surface groups, facilitated various reactions, hydrolysis was the predominant pathway. The thermal treatment, regardless of the atmosphere, reduced the oxygen content, decreasing the extent of hydrolysis. However, incorporating basic surface groups such as pyridines, amines, or weak acids such as thiols promoted dehydrohalogenation as the main detoxification pathway on these samples.

对一种碳织物（CT）进行了化学改性，以提高其表面活性，促进芥子气的代用品--2-氯乙基硫醚（CEES）的吸附和降解。首先对 CT 进行氧化（CTO），然后在氨气（CTON）或硫化氢（CTOS）气氛下加热，分别加入氮或硫的官能团。解毒实验在封闭的小瓶中进行，使用的是蒸汽或液体形式的 CEES。CT、CTO、CTOS 和 CTON 的最大蒸气重量吸收率分别为 399、372、434 和 489 mg/g。所有纺织品都能阻止 CEES 液滴的汽化。虽然在气态和液态系统中都检测到了类似的反应产物，但纺织品表面 CEES 化学转化程度的明显差异表明，受表面化学影响的解毒途径各不相同。尽管 CTO 的异质表面富含氧表面基团，促进了各种反应，但水解是最主要的途径。无论在何种气氛下进行热处理，氧含量都会减少，从而降低水解程度。然而，加入吡啶、胺等碱性表面基团或硫醇等弱酸性基团会促进脱氢卤化，成为这些样品的主要解毒途径。

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引用次数: 0

Oxygen-reduced surface-terminated MXenes as cathodes for enhanced reversible Li–CO2 batteries 氧还原表面封端 MXenes 作为增强型可逆二氧化碳锂电池的阴极

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-27 DOI: 10.1016/j.carbon.2024.119676

Huan Liu , Hongjuan Lai , Bin Cao , Xue Tian , Di Zhang , Razium Ali Soomro , Yi Wu

Li–CO₂ batteries have garnered global attention due to their dual attributes of high energy density and effective CO₂ capture. However, they still face a formidable challenge in decomposing the discharge products Li₂CO₃, resulting in subpar battery performance. MXene has been proposed as a promising candidate owing to its high electrical conductivity and effective CO₂ activation performance. Nevertheless, unavoidable surface terminations (such as –O and –OH) during synthesis strongly influence their catalytic properties, posing a significant hurdle for high-performance Li–CO₂ batteries. Herein, a thermal annealing approach is proposed to control the surface termination groups of MXene to reduce the generation of lithium hydroxide byproducts, thereby accelerating Li₂CO₃ decomposition kinetics and enhancing the reversibility of the battery. The systematic annealing of MXene in the range of 500–800 °C confirmed optimal surface terminations at 500 °C (TC500). The TC500, when tested as a catalyst in a Li–CO₂ battery, exhibited enhanced performance metrics, such as low voltage gap (1.98 V), high specific capacity (15,740.38 mA h g⁻¹ at 100 mA g⁻¹), and prolonged cycle stability (700 h at 200 mA g⁻¹). The proposed work offers an effective strategy for regulating MXene surface termination groups via simple annealing treatments to achieve high-performance Li–CO₂ batteries.

锂-二氧化碳电池因其高能量密度和有效捕获二氧化碳的双重特性而备受全球关注。然而，它们在分解放电产物 Li2CO3 方面仍面临着巨大挑战，导致电池性能不佳。由于具有高导电性和有效的二氧化碳活化性能，MXene 被认为是一种很有前途的候选材料。然而，在合成过程中不可避免的表面终止（如 -O 和 -OH）会严重影响其催化性能，从而对高性能锂-CO2 电池构成重大障碍。本文提出了一种热退火方法来控制 MXene 的表面终止基团，以减少氢氧化锂副产物的生成，从而加速 Li2CO3 的分解动力学并提高电池的可逆性。在 500-800 °C 范围内对 MXene 进行的系统退火确认了 500 °C 时的最佳表面端接（TC500）。在锂-CO2 电池中作为催化剂进行测试时，TC500 表现出更高的性能指标，如低电压间隙（1.98 V）、高比容量（100 mA g-1 时为 15,740.38 mA h g-1）和更长的循环稳定性（200 mA g-1 时为 700 h）。这项工作提供了一种有效的策略，通过简单的退火处理调节 MXene 表面的终止基团，从而实现高性能的锂-二氧化碳电池。

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引用次数: 0

Macroscopic superlubricity achieved by hydrolysis reaction of ethyl lactate on silicon-doped diamond-like carbon film 通过乳酸乙酯在掺硅类金刚石碳薄膜上的水解反应实现宏观超润滑性

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-27 DOI: 10.1016/j.carbon.2024.119675

Jinyan Chen , Wei Song , Jinjin Li

Superlubricity between steel/diamond-like carbon (DLC) film could be achieved at vacuum or nitrogen condition, but it would be failed at ambient conditions. In this work, the macroscale superlubricity was achieved at ambient conditions by introducing ethyl lactate into ethylene glycol as lubricant additive for the friction pairs of silicon-doped diamond-like carbon (Si-DLC)/steel. Stable friction coefficient (μ = 0.002) and wear rate of friction pairs with the introduction of ethyl lactate could be respectively reduced by 99 % and 35 %. The characterization tests and density functional theory (DFT) calculation both demonstrated that the partial ethyl lactate was hydrolyzed into lactic acid due to the catalysis effect of steel surfaces. The molecular dynamics (MD) simulation result showed that the lactic acid molecules could be chemically adsorbed on the surfaces of friction pairs, forming a tribofilm through hydrogen bond with ethylene glycol molecules, which led to a significant reduction in the friction coefficient. This work presents a novel approach to achieve superlubricity on Si-DLC film with liquid, providing a great support for industrial application of superlubricity on DLC film.

钢/类金刚石碳（DLC）薄膜之间的超润滑性可在真空或氮气条件下实现，但在环境条件下则会失效。在这项研究中，通过在乙二醇中引入乳酸乙酯作为掺杂硅的类金刚石碳（Si-DLC）/钢摩擦副的润滑添加剂，在环境条件下实现了宏观超润滑性。引入乳酸乙酯后，摩擦副的稳定摩擦系数（μ = 0.002）和磨损率分别降低了 99% 和 35%。表征试验和密度泛函理论（DFT）计算均表明，由于钢表面的催化作用，部分乳酸乙酯被水解为乳酸。分子动力学（MD）模拟结果表明，乳酸分子可化学吸附在摩擦副表面，通过氢键与乙二醇分子形成三膜，从而显著降低摩擦系数。这项研究提出了一种新的方法来实现 Si-DLC 薄膜与液体的超润滑性，为 DLC 薄膜超润滑性的工业应用提供了有力支持。

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引用次数: 0

Preparation of multi-element doped carbon nanospheres with core-shell structure derived from polystyrene as lubricating additives for improving tribological behavior 制备多元素掺杂的聚苯乙烯核壳结构碳纳米球，作为润滑添加剂改善摩擦学性能

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-27 DOI: 10.1016/j.carbon.2024.119677

Yixin Wang , Sha Liu , Tiantian Wang , Shujuan Liu , Qian Ye , Feng Zhou , Weimin Liu

In this study, the multi-element doped carbon nanospheres with core-shell structure (N,P,S-PCNs) have been successfully synthesized through the carbonization of hyper-cross-linked polystyrene nanospheres (HPSs) encapsulated with poly(cyclotriphosphazene-co-4,4′-sulfonyldiphenol) (PZS). The phosphonitrilic chloride trimer can in-situ assemble on HPSs surface, forming a poly(phosphonitrilic chloride trimer) film via sulfonyldiphenol as cross-linking agent to obtain HPSs@PZS. Subsequently, the HPSs@PZS undergoes high-temperature calcination under N₂ atmosphere, and PZS with a well-preserved encapsulation capability efficiently incorporated N, P and S into carbon nanospheres to gain multi-element (N,P,S) co-doped carbon nanospheres (N,P,S-PCNs) with core-shell structure. The prepared N,P,S-PCNs exhibit exceptional dispersibility and stability as lubricant additives, effectively mitigating friction (reduced to 0.106) and wear (decreased by 84.0 %). The lubrication performance of N,P,S-PCNs is exceptional due to the nanospheres' remarkable ability to enter the gaps between friction pairs and form a deposition film on the surfaces. Moreover, the nanospheres can undergo a chemical reaction with the matrix surface, resulting in the formation of a chemical protective film. The composite protective film (deposition film and chemical protective film) significantly enhances the lubricants' ability to reduce friction and resist wear.

本研究通过对包覆有聚（环三膦-4,4′-磺基二苯酚）（PZS）的超交联聚苯乙烯纳米球（HPSs）进行碳化，成功合成了多元素掺杂的核壳结构碳纳米球（N,P,S-PCNs）。通过磺酰二苯酚作为交联剂，磷酰氯三聚体可在 HPSs 表面原位组装，形成聚（磷酰氯三聚体）膜，得到 HPSs@PZS。随后，将 HPSs@PZS 在 N2 气氛下进行高温煅烧，具有良好封装能力的 PZS 将 N、P、S 有效地掺入到碳纳米球中，得到具有核壳结构的多元素（N、P、S）共掺杂碳纳米球（N、P、S-PCNs）。制备的 N,P,S-PCNs 作为润滑油添加剂具有优异的分散性和稳定性，可有效降低摩擦（降低至 0.106）和磨损（降低 84.0%）。N,P,S-氯化萘的润滑性能之所以出众，是因为纳米球具有进入摩擦对之间的间隙并在表面形成沉积膜的卓越能力。此外，纳米球还能与基体表面发生化学反应，形成化学保护膜。复合保护膜（沉积膜和化学保护膜）大大增强了润滑剂减少摩擦和抗磨损的能力。

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引用次数: 0

Metal-doped amorphous microporous carbon for isotope separation: Pore size modulation and selective deuterium adsorption 用于同位素分离的金属掺杂无定形微孔碳：孔径调节和选择性氘吸附

IF 10.5 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2024-09-27 DOI: 10.1016/j.carbon.2024.119674

Hyunlim Kim , Minji Jung , Jaewoo Park , Taeung Park , Jonghyeok Park , Hyerin Lee , Balaji G. Ghule , Ji-Hyun Jang , Raeesh Muhammad , Sandeep Kumar , Hyunchul Oh

Efficient hydrogen isotope separation is crucial for applications in energy production and advanced scientific research, but separation of these poses significant challenges. In this study, we developed amorphous microporous carbon (AMC) derived from a zeolite template and explored hydrogen isotope separation using quantum sieving. Thermal desorption spectroscopy (TDS) technique was used to evaluate the selectivity of hydrogen (H₂) and deuterium (D₂) isotope separation. The doping of metal ions, such as Ca²⁺, Mg²⁺, Ni²⁺, and Cu²⁺, in the porous carbon modulates the physicochemical properties of the pores. The metal-doped carbon samples demonstrated D₂ vs H₂ selectivity (S_D2/H2) of over 10, compared to the pristine carbon's S_D2/H2 of less than 8. Density functional theory (DFT) calculation infers that pore modulation through metal doping enhanced the binding affinity of materials towards D₂ resulting in increased separation selectivity compared to pristine carbon samples. This approach not only boosts separation efficiency but also provides a scalable and cost-effective solution for industrial applications.

高效的氢同位素分离对于能源生产和先进科学研究中的应用至关重要，但分离氢同位素却面临巨大挑战。在这项研究中，我们开发了源自沸石模板的无定形微孔碳（AMC），并利用量子筛分技术探索了氢同位素分离。热解吸光谱（TDS）技术用于评估氢（H2）和氘（D2）同位素分离的选择性。在多孔碳中掺入 Ca2⁺、Mg2⁺、Ni2⁺ 和 Cu2⁺等金属离子可调节孔隙的物理化学性质。密度泛函理论（DFT）计算推断，通过掺杂金属调节孔隙增强了材料与 D2 的结合亲和力，从而提高了与原始碳样品相比的分离选择性。这种方法不仅提高了分离效率，还为工业应用提供了一种可扩展且具有成本效益的解决方案。

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引用次数: 0

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