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High-performance thermal interface materials enabled by vertical alignment of lightweight and soft graphene foams 通过垂直排列轻质软石墨烯泡沫实现高性能热界面材料
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-27 DOI: 10.1007/s12274-024-6985-7
Huaqiang Fu, Renqiang Fang, Chao Tian, Wei Qian, Shiya Cao, Ziran Zhang, Xiaoxi Xu, Chuang Yao, Zhe Wang, Daping He

High-performance thermal interface materials (TIMs) are highly sought after for modern electronics. Two-dimensional (2D) materials as vertical aligned fillers can optimize the out-plane thermal conductivity (k), but their excessively high content or intrinsic rigidness deteriorate TIMs softness, leading to worsening for thermal contact resistance (Rcontact). In this study, 2D graphene materials are fabricated into lightweight and soft graphene foams (GFs) with high-orientation, acting as vertical filler frameworks to optimize the k and Rcontact for vertical GF (VGF) TIMs. The VGF-TIM has a high k of 47.9 W·m−1·K−1 at a low graphene content of 15.5 wt.%. Due to the softness and low filler contents of GFs, the VGF-TIM exhibits a low compressive module (4.2 MPa), demonstrating excellent compressibility. The resulting TIM exhibit a low contact resistance of 24.4 K·mm2·W−1, demonstrating 185.1% higher cooling efficiency in practical heat dissipating scenario compared to commercial advanced TIMs. This work provides guidelines for the design of advanced TIMs and their applications in thermal management.

高性能热界面材料(TIMs)是现代电子产品所孜孜以求的。二维(2D)材料作为垂直排列的填充物可以优化平面外热导率(k⊥),但其含量过高或固有的刚性会降低热界面材料的柔软性,导致热接触电阻(Rcontact)恶化。在本研究中,二维石墨烯材料被制成轻质柔软的高取向石墨烯泡沫 (GF),作为垂直填充框架,以优化垂直 GF (VGF) TIM 的 k⊥ 和 Rcontact。在石墨烯含量较低的 15.5 wt.% 条件下,VGF-TIM 的 k⊥ 高达 47.9 W-m-1-K-1。由于石墨烯的柔软性和较低的填料含量,VGF-TIM 显示出较低的压缩模量(4.2 兆帕),表现出优异的可压缩性。由此产生的 TIM 具有 24.4 K-mm2-W-1 的低接触电阻,与商用先进 TIM 相比,在实际散热情况下冷却效率提高了 185.1%。这项研究为先进 TIM 的设计及其在热管理中的应用提供了指导。
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引用次数: 0
Liquid-encapsulated quantum dot for enhanced UV and thermal stability of quantum dot color conversion films 液态封装量子点可增强量子点色彩转换薄膜的紫外线和热稳定性
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-17 DOI: 10.1007/s12274-024-6971-0
Ronghuan Liu, Fan Fang, Pai Liu, Xijian Duan, Kai Wang, Xiao Wei Sun

Encapsulation is a widely recognized method for enhancing the stability of colloidal quantum dots (CQDs). However, traditional encapsulation methods for solid-state materials expose encapsulated CQDs to risks such as ligand loss and poor dispersion. Additionally, these encapsulated CQDs still face the risk of aging due to surface ligand bond breakage under high-energy radiation. In this study, we found that quantum dots in solution exhibited enhanced ultraviolet (UV) tolerance compared to their counterparts in solid form under an inert atmosphere. We attribute this enhancement to improved ligand retention and self-healing of quantum dots in solution. Herein, we introduce a novel method for fabricating liquid-encapsulated quantum dot (LEQD) color conversion films. This technique leverages the self-healing capability of ligands in liquid-state quantum dots to enhance the UV and thermal stability of the quantum dot color conversion films. Experimental results demonstrate that LEQD films exhibit better resistance to UV radiation and high temperatures than solid-encapsulated quantum dot (SEQD) color conversion films. After 400 h of exposure to 100 mW blue light-emitting device (LED) light at 60 °C and 90% humidity, the brightness of LEQD film retained 90% of its initial level. This liquid-state quantum dot encapsulation approach offers a promising pathway for developing more durable quantum dot color conversion films.

封装是一种公认的提高胶体量子点(CQDs)稳定性的方法。然而,固态材料的传统封装方法会使封装的 CQDs 面临配体损失和分散性差等风险。此外,这些封装的 CQDs 还面临着在高能辐射下因表面配体键断裂而老化的风险。在这项研究中,我们发现在惰性气氛下,溶液中的量子点与固体形式的量子点相比,表现出更强的紫外线(UV)耐受性。我们将这种增强归因于溶液中量子点的配体保留和自我修复能力的提高。在此,我们介绍了一种制造液态封装量子点(LEQD)色彩转换薄膜的新方法。该技术利用液态量子点中配体的自修复能力,提高了量子点色彩转换薄膜的紫外线和热稳定性。实验结果表明,与固态封装量子点(SEQD)色彩转换薄膜相比,液态量子点薄膜具有更好的抗紫外线辐射和耐高温性能。在 60 °C 和 90% 湿度条件下,将 LEQD 薄膜置于 100 mW 蓝色发光器件 (LED) 灯光下 400 小时后,其亮度仍保持在初始水平的 90%。这种液态量子点封装方法为开发更耐用的量子点色彩转换薄膜提供了一条前景广阔的途径。
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引用次数: 0
Precise synthesis of dual atom sites for electrocatalysis 电催化双原子位点的精确合成
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-17 DOI: 10.1007/s12274-024-6940-7
Yao Wang, Fengya Ma, Guoqing Zhang, Jiawei Zhang, Hui Zhao, Yuming Dong, Dingsheng Wang

Single atom sites are widely applied in various electrocatalytic fields due to high atom utilization, mass activity, and selectivity. They are limited in catalyzing multi-electron reactions due to their intrinsic mono-metal center feature. Dual atom sites (DASs) as promising candidate have received enormous attentions because adjacent active sites can accelerate their catalytic performance via synergistic effect. Herein, the fundamental understandings and intrinsic mechanism underlying DASs and corresponding electrocatalytic applications are systemically summarized. Different synergy dual sites are presented to disclose the structure-performance relationship with engineering the well-defined DASs on the basis of theoretical principle. An overview of the electrocatalytic applications is showed, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. Finally, a conclusion and future prospective are provided to reveal the current challenges for rational designing, synthesizing, and modulating the advanced DASs toward electrocatalytic reactions.

单原子位点具有原子利用率高、质量活性高和选择性高的特点,因此被广泛应用于各种电催化领域。由于其固有的单金属中心特性,单原子位点在催化多电子反应方面受到限制。双原子位点(DASs)作为一种有前途的候选材料受到了广泛关注,因为相邻的活性位点可以通过协同效应提高催化性能。本文系统地总结了对双原子位点的基本认识、其内在机理以及相应的电催化应用。在理论原理的基础上,介绍了不同的协同双位点,揭示了定义明确的 DASs 的工程结构-性能关系。还概述了电催化应用,包括氧气还原反应、氢气进化反应、氧气进化反应、二氧化碳还原反应和氮气还原反应。最后,还给出了结论和未来展望,揭示了当前合理设计、合成和调控先进 DASs 以实现电催化反应所面临的挑战。
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引用次数: 0
Exploring the potential of simple automation concepts for quantifying functional groups on nanomaterials with optical assays 探索利用光学测定法量化纳米材料上功能基团的简单自动化概念的潜力
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-14 DOI: 10.1007/s12274-024-6970-1
Isabella Tavernaro, Anna Matiushkina, Kai Simon Rother, Celina Mating, Ute Resch-Genger

Until now, automation in nanomaterial research has been largely focused on the automated synthesis of engineered nanoparticles (NPs) including the screening of synthesis parameters and the automation of characterization methods such as electron microscopy. Despite the rapidly increasing number of NP samples analyzed due to increasing requirements on NP quality control, increasing safety concerns, and regulatory requirements, automation has not yet been introduced into workflows of analytical methods utilized for screening, monitoring, and quantifying functional groups (FGs) on NPs. To address this gap, we studied the potential of simple automation tools for the quantification of amino surface groups on different types of aminated NPs, varying in size, chemical composition, and optical properties, with the exemplarily chosen sensitive optical fluorescamine (Fluram) assay. This broadly applied, but reportedly error-prone assay, which utilizes a chromogenic reporter, involves multiple pipetting and dilution steps and photometric or fluorometric detection. In this study, we compared the influence of automated and manual pipetting on the results of this assay, which was automatically read out with a microplate reader. Special emphasis was dedicated to parameters like accuracy, consistency, achievable uncertainties, and speed of analysis and to possible interferences from the NPs. Our results highlight the advantages of automated surface FG quantification and the huge potential of automation for nanotechnology. In the future, this will facilitate process and quality control of NP fabrication, surface modification, and stability monitoring and help to produce large data sets for nanomaterial grouping approaches for sustainable and safe-by-design, performance, and risk assessment studies.

迄今为止,纳米材料研究中的自动化主要集中在工程纳米粒子(NPs)的自动化合成,包括合成参数筛选和电子显微镜等表征方法的自动化。尽管由于对 NP 质量控制的要求不断提高、对安全性的关注日益增加以及监管要求,分析的 NP 样品数量迅速增加,但用于筛选、监测和量化 NP 上官能团 (FG) 的分析方法的工作流程尚未引入自动化。为了填补这一空白,我们研究了简单自动化工具的潜力,这些工具可用于定量不同类型胺化 NPs 上的氨基表面基团,这些 NPs 的尺寸、化学成分和光学性质各不相同,我们选择了灵敏的光学荧光胺 (Fluram) 检测法作为范例。这种检测方法应用广泛,但据说容易出错,它利用一种发色性报告物,涉及多个移液和稀释步骤以及光度或荧光检测。在本研究中,我们比较了自动移液和手动移液对该检测结果的影响,该检测使用微孔板阅读器自动读取。我们特别强调了准确性、一致性、可实现的不确定性、分析速度等参数以及 NPs 可能产生的干扰。我们的研究结果凸显了自动化表面 FG 定量的优势,以及自动化在纳米技术中的巨大潜力。未来,这将促进对 NP 制备、表面改性和稳定性监测的过程和质量控制,并有助于为可持续和安全设计、性能和风险评估研究中的纳米材料分组方法生成大型数据集。
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引用次数: 0
Colloidal II–VI nanoplatelets for optoelectronic devices: Progress and perspectives 用于光电器件的胶体 II-VI 纳米片:进展与前景
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-14 DOI: 10.1007/s12274-024-6965-y
An Hu, Li Ma, Xiaoyu Yang, Yige Yao, Yunke Zhu, Jingjing Qiu, Shuang Wang, Changjun Lu, Yunan Gao

Colloidal II–VI nanoplatelets (NPLs) are solution-processable two-dimensional (2D) quantum dots that have vast potential in high-performance optoelectronic applications, including light-emitting diodes, sensors, and lasers. Superior properties, such as ultrapure emission, giant oscillator strength transition, and directional dipoles, have been demonstrated in these NPLs, which can improve the efficiency of light-emitting diodes and lower the threshold of lasers. In this review, we present an overview of the current progress and propose perspectives on the most well-studied II–VI NPLs that are suitable for the optoelectronic applications. We emphasize that the control of the symmetrical shell growth of NPLs is critical for the practical utilization of the advantages of NPLs in these devices.

胶体 II-VI 纳米颗粒(NPLs)是一种可溶液加工的二维量子点,在高性能光电应用(包括发光二极管、传感器和激光器)中具有巨大潜力。这些 NPL 具有超纯发射、巨振子强度转变和定向偶极子等优异特性,可以提高发光二极管的效率并降低激光器的阈值。在这篇综述中,我们概述了当前的研究进展,并对适合光电应用的研究最深入的 II-VI NPL 提出了展望。我们强调,控制 NPL 的对称壳生长对于在这些器件中实际利用 NPL 的优势至关重要。
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引用次数: 0
Rational design and structural regulation of near-infrared silver chalcogenide quantum dots 近红外卤化银量子点的合理设计与结构调控
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-14 DOI: 10.1007/s12274-024-6958-x
Zhen-Ya Liu, Wei Zhao, Li-Ming Chen, Yan-Yan Chen, Zhi-Gang Wang, An-An Liu, Dai-Wen Pang

Silver chalcogenides (Ag2E; E = S, Se, or Te) quantum dots (QDs) have emerged as promising candidates for near-infrared (NIR) applications. However, their narrow bandgap and small exciton Bohr radius render the optical properties of Ag2E QDs highly sensitive to surface and size variations. Moreover, the propensity for the formation of silver impurities and their low solubility product constants pose challenges in their controllable synthesis. Recent advancements have deepened our understanding of the relationship between the multi-hierarchical structure of Ag2E QDs and their optical properties. Through rational design and precise structural regulation, the performance of Ag2E QDs has been significantly enhanced across various applications. This review provides a comprehensive overview of historical and current progress in the synthesis and structural regulation of Ag2E QDs, encompassing aspects such as size control, crystal structure engineering, and surface/interface engineering. Additionally, it discusses outstanding challenges and potential opportunities in this field. The aim of this review is to promote the custom synthesis of Ag2E QDs for applications in biological imaging, and optoelectronics applications.

铬化银(Ag2E;E = S、Se 或 Te)量子点(QDs)已成为近红外(NIR)应用的理想候选材料。然而,由于其带隙窄和激子玻尔半径小,Ag2E 量子点的光学特性对表面和尺寸变化非常敏感。此外,银杂质的形成倾向和它们的低溶度积常数也给它们的可控合成带来了挑战。最近的研究进展加深了我们对 Ag2E QDs 的多层结构与其光学特性之间关系的理解。通过合理的设计和精确的结构调整,Ag2E QDs 的性能在各种应用中得到了显著提高。本综述全面概述了 Ag2E QDs 的合成和结构调控方面的历史和当前进展,包括尺寸控制、晶体结构工程和表面/界面工程等方面。此外,本综述还讨论了这一领域的突出挑战和潜在机遇。本综述旨在促进 Ag2E QDs 的定制合成,以应用于生物成像和光电应用。
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引用次数: 0
Thermodynamically induced crystal restructuring to make CsPbCl3 single crystal films for weak light detection 利用热力学诱导晶体重组制造用于弱光探测的 CsPbCl3 单晶薄膜
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-13 DOI: 10.1007/s12274-024-6967-9
Xiyan Pan, Tai An, Jie Sun, Hua Dong, Zhu Ma, Guangxing Liang, Yongbo Yuan, Yang Li, Wuqiang Wu, Yong Ding, Liming Ding

CsPbCl3 perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice energy and low polarizability result in extremely low solubility in conventional solvents, making the synthesis of CsPbCl3 single crystals a significant challenge. In this study, we propose a novel thermodynamically induced crystal restructuring (TICR) process that can transform microcrystalline films (MCFs) into single crystal films (SCFs) within a short period. This method, for the first time, has successfully achieved the synthesis of centimeter-sized CsPbCl3 SCFs and the mechanism has been explored in depth using in-situ techniques. Furthermore, we report the first instance of a CsPbCl3 SCF UV photodiode, which exhibits a record-breaking on/off ratio of 3.32 × 107 and a detectivity of up to 1.15 × 1014 Jones under 0 V bias. It demonstrates excellent response even under weak light conditions of 10 nW·cm−2 and maintains outstanding stability with almost no performance degradation after 15 months. This study provides a novel approach for the synthesis of perovskite single crystals and holds significant potential for advancing the development of high-performance optoelectronic devices.

CsPbCl3 包晶因其卓越的热稳定性和出色的短波长光响应,被认为是一种极有前途的紫外线(UV)光电探测器材料。然而,它的高晶格能和低极化性导致其在传统溶剂中的溶解度极低,从而使 CsPbCl3 单晶的合成成为一项重大挑战。在本研究中,我们提出了一种新型热力学诱导晶体重组(TICR)工艺,可在短时间内将微晶薄膜(MCF)转化为单晶薄膜(SCF)。这种方法首次成功合成了厘米级的 CsPbCl3 SCFs,并利用原位技术对其机理进行了深入探讨。此外,我们还首次报告了 CsPbCl3 SCF 紫外光二极管的实例,该二极管在 0 V 偏置下的开/关比达到了破纪录的 3.32 × 107,探测率高达 1.15 × 1014 Jones。即使在 10 nW-cm-2 的弱光条件下,它也能表现出卓越的响应能力,并且在 15 个月后仍能保持出色的稳定性,几乎没有性能衰减。这项研究为合成包光体单晶体提供了一种新方法,为推动高性能光电器件的发展提供了巨大潜力。
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引用次数: 0
Advanced emerging ambient energy harvesting technologies enabled by transition metal dichalcogenides: Opportunity and challenge 过渡金属二卤化物带来的先进新兴环境能量采集技术:机遇与挑战
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1007/s12274-024-6959-9
Ning Sun, Yan Wang, Xianya Liu, Jianmin Li, Shiyan Wang, Yixiang Luo, Zhe Feng, Jie Dong, Mengyang Zhang, Fengshun Wang, Yang Li, Longlu Wang

Environmental pollution and global warming caused by fossil fuels have become increasingly serious issues. Therefore, it is urgent to explore novel strategies to obtain sustainable, renewable and clean energy. Fortunately, ambient energy harvesting technologies, which are receiving increasing attention, provide an optimal solution. Additionally, the investigation of two-dimensional (2D) materials represented by transition metal dichalcogenides (TMDs) significantly facilitates the advancement of ambient energy harvesting technologies due to their unique properties, enabling the application of ambient energy harvesting. Herein, we summarized recent advances in the application of TMDs in thermal energy harvesting, osmotic energy harvesting, mechanical energy harvesting, water energy harvesting and radiofrequency energy harvesting respectively. In the meanwhile, we listed some representative structure and device optimization strategies for enhancing the energy conversion performance of these ambient energy harvesters, aiming to provide valuable insights for future investigations towards further optimization. Finally, we highlight the pressing issues currently faced in the application of the TMDs ambient energy harvesting technologies and propose some potential solutions to these challenges. We aimed to provide a comprehensive review in the applications of the energy harvesting technologies, in order to provide innovative insights for optimizing existing TMDs-based technologies.

化石燃料造成的环境污染和全球变暖问题日益严重。因此,迫切需要探索新的战略,以获得可持续、可再生的清洁能源。幸运的是,日益受到关注的环境能量采集技术提供了一个最佳解决方案。此外,以过渡金属二掺杂物(TMDs)为代表的二维(2D)材料因其独特的性能,大大促进了环境能量收集技术的发展,使环境能量收集技术得以应用。在此,我们分别总结了 TMDs 在热能收集、渗透能收集、机械能收集、水能收集和射频能收集方面的最新应用进展。同时,我们列举了一些具有代表性的结构和器件优化策略,以提高这些环境能量收集器的能量转换性能,从而为今后的进一步优化研究提供有价值的见解。最后,我们强调了目前在应用 TMDs 环境能量收集技术时所面临的紧迫问题,并针对这些挑战提出了一些潜在的解决方案。我们的目标是对能量收集技术的应用进行全面回顾,以便为优化基于 TMDs 的现有技术提供创新见解。
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引用次数: 0
Hierarchical porous molybdenum carbide synergic morphological engineering towards broad multi-band tunable microwave absorption 分层多孔碳化钼协同形貌工程实现宽泛的多波段可调微波吸收
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1007/s12274-024-6938-1
Tianbao Zhao, Di Lan, Zirui Jia, Zhenguo Gao, Guanglei Wu

With the accelerating development of electronic technology, how to effectively eliminate electromagnetic radiation pollution has become a critical issue. Electromagnetic wave (EMW) absorption materials have an irreplaceable position in the field of military stealth as well as in the field of electromagnetic pollution control. In order to cope with the complicated electromagnetic environment, the design of multifunctional and multiband high-efficiency EMW absorbers remains a daunting challenge. In this work, a hierarchical porous molybdenum carbide matrix with a three-dimensional porous structure was designed by salt melt synthesis (SMS) strategy. Furthermore, the relationship between the structure and the impedance matching performance was explored by stepwise modification via ultrathin layered MoS2 nanoflakes. Analysis indicates that the extent of modification of hierarchical porous molybdenum carbide by MoS2 nanoflakes modulates the dielectric performance due to differences in morphology and the introduction of heterogeneous structures, along with a dramatic impact on the impedance matching performance. In particular, the prepared MS/MC/PNC-2 composite exhibits a reflection loss (RL) of -55.30 dB at 2.4 mm, and an ultra-broad effective absorption bandwidth (EAB) of 7.60 GHz is obtained at 2.0 mm. The coordination of structure and component enables the absorber to exhibit strong absorption, wide bandwidth, thin thickness, and multi-band absorption characteristics. Noticeably, the effective absorption performance in the broadband for X and Ku is also satisfying, as well as possessing moderate marine anti-corrosion performance. This study contributes to an in-depth understanding of the relationship between impedance matching and EMW absorber performance and provides a reference for the design of multifunctional, multiband microwave absorbing materials.

随着电子技术的加速发展,如何有效消除电磁辐射污染已成为一个关键问题。电磁波吸收材料在军事隐身领域和电磁污染控制领域都有着不可替代的地位。为了应对复杂的电磁环境,设计多功能、多频段的高效电磁波吸收材料仍然是一项艰巨的挑战。在这项工作中,采用盐熔合成(SMS)策略设计了一种具有三维多孔结构的分层多孔碳化钼基体。此外,通过对超薄层状 MoS2 纳米片进行逐步改性,探索了结构与阻抗匹配性能之间的关系。分析表明,MoS2 纳米片对分层多孔碳化钼的修饰程度会改变介电性能,这是因为形态的差异和异质结构的引入会对阻抗匹配性能产生巨大影响。其中,制备的 MS/MC/PNC-2 复合材料在 2.4 mm 时的反射损耗 (RL) 为 -55.30 dB,在 2.0 mm 时的有效吸收带宽 (EAB) 为 7.60 GHz。结构和元件的协调使吸收器表现出强吸收、宽带宽、薄厚度和多波段吸收特性。值得注意的是,X 和 Ku 波段的有效吸收性能也令人满意,同时还具有适度的海洋抗腐蚀性能。这项研究有助于深入理解阻抗匹配与电磁波吸收器性能之间的关系,并为多功能、多频带微波吸收材料的设计提供参考。
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引用次数: 0
On the role of Zn and Fe doping in nitrogen-carbon electrocatalysts for oxygen reduction 氮碳氧还原电催化剂中锌和铁掺杂的作用
IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1007/s12274-024-6962-1
Yanan Zou, Yuanyuan Su, Yongchao Yu, Jinliang Luo, Xiaomin Kang, Jun Zhang, Linghan Lan, Tianshi Wang, Jun Li

Zn is a frequently used and sometimes even an inevitably involved element (when zeolitic imidazolate framework-8 (ZIF-8) is adopted as the precursor) for preparing high-performance Fe-N-C oxygen reduction reaction (ORR) catalysts. However, how the Zn element affects the physicochemical architecture of the catalysts, how it enhances the catalytic activity and whether Zn atoms serve as the active centers remain unclear. Herein, we proposed a novel route that adopted pyrrole as the precursor and flexibly controlled the addition of exogenous Zn and Fe dopants before pyrrole polymerization. In this way, a series of nitrogen-carbon catalysts with or without Zn or Fe doping were synthesized. The detailed characterization revealed the role of Zn and Fe doping in the catalyst morphology, pore structure, active site configurations, ORR catalytic activity and fuel cell performance. Importantly, the findings revealed that Zn doping has little effect on the ORR mechanism and pathway. It enhances ORR activity primarily by increasing the number of active sites via introducing more micro- and meso-pores, rather than by creating new active sites. While Fe doping participated in forming both pores and active site centers. Moreover, the catalyst that co-doped with Zn and Fe atoms (Zn-FeNC), synthesized via this simple and template-free route we proposed, presented a unique hollow and hierarchical pore structure with highly boosted ORR activity. It exhibited a 40 mV higher E1/2 value than Pt/C in alkaline media, along with a rapid current response in air-cathode of the direct formate fuel cell. These results are valuable in guiding the synthesis of high-performance Fe-N-C catalysts.

在制备高性能 Fe-N-C 氧还原反应(ORR)催化剂时,锌是一种常用元素,有时甚至是一种不可避免的元素(当采用沸石咪唑盐酸盐框架-8(ZIF-8)作为前驱体时)。然而,Zn 元素如何影响催化剂的物理化学结构、如何提高催化活性以及 Zn 原子是否作为活性中心等问题仍不清楚。在此,我们提出了一种以吡咯为前驱体,并在吡咯聚合前灵活控制外源锌和铁掺杂剂添加的新型路线。通过这种方法,我们合成了一系列掺杂或不掺杂锌或铁的氮碳催化剂。详细的表征揭示了锌和铁掺杂在催化剂形态、孔结构、活性位点构型、ORR 催化活性和燃料电池性能中的作用。重要的是,研究结果表明,锌掺杂对 ORR 机制和途径的影响很小。它主要是通过引入更多的微孔和中孔增加活性位点的数量,而不是通过创造新的活性位点来提高 ORR 活性。而铁的掺杂既参与了孔隙的形成,也参与了活性位点中心的形成。此外,通过我们提出的这种简单的无模板路线合成的共掺杂锌和铁原子的催化剂(Zn-FeNC)呈现出独特的中空和分层孔隙结构,具有极高的 ORR 活性。在碱性介质中,它的 E1/2 值比 Pt/C 高 40 mV,同时在直接甲酸燃料电池的空气阴极中具有快速的电流响应。这些结果对于指导高性能 Fe-N-C 催化剂的合成具有重要价值。
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引用次数: 0
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Nano Research
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