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Precise Detection, Control and Synthesis of Chiral Compounds at Single-Molecule Resolution 单分子分辨率手性化合物的精确检测、控制和合成。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-09-12 DOI: 10.1007/s40820-023-01184-5
Chen Yang, Weilin Hu, Xuefeng Guo

Chirality, as the symmetric breaking of molecules, plays an essential role in physical, chemical and especially biological processes, which highlights the accurate distinction among heterochiralities as well as the precise preparation for homochirality. To this end, the well-designed structure-specific recognizer and catalysis reactor are necessitated, respectively. However, each kind of target molecules requires a custom-made chiral partner and the dynamic disorder of spatial-orientation distribution of molecules at the ensemble level leads to an inefficient protocol. In this perspective article, we developed a universal strategy capable of realizing the chirality detection and control by the external symmetry breaking based on the alignment of the molecular frame to external stimuli. Specifically, in combination with the discussion about the relationship among the chirality (molecule), spin (electron) and polarization (photon), i.e., the three natural symmetry breaking, single-molecule junctions were proposed to achieve a single-molecule/event-resolved detection and synthesis. The fixation of the molecular orientation and the CMOS-compatibility provide an efficient interface to achieve the external input of symmetry breaking. This perspective is believed to offer more efficient applications in accurate chirality detection and precise asymmetric synthesis via the close collaboration of chemists, physicists, materials scientists, and engineers.

手性作为分子的对称断裂,在物理、化学特别是生物过程中起着至关重要的作用,这就突出了对杂手性的准确区分以及对同手性的精确制备。为此,需要精心设计结构特异性识别器和催化反应器。然而,每一种靶分子都需要一个定制的手性伴侣,并且分子在集成水平上的空间取向分布的动态无序导致了低效的方案。在这篇前瞻性文章中,我们开发了一种通用策略,能够实现手性检测和控制的外部对称破缺基于分子框架对外部刺激的对齐。具体来说,结合对手性(分子)、自旋(电子)和极化(光子)之间的关系,即三种自然对称性破缺的讨论,提出了单分子结来实现单分子/事件分辨的检测和合成。分子取向的固定和cmos的兼容性为实现对称破缺的外部输入提供了有效的接口。通过化学家、物理学家、材料科学家和工程师的密切合作,这一观点被认为在精确手性检测和精确不对称合成方面提供了更有效的应用。
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引用次数: 0
Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel 双掺杂硫化镍电升级聚对苯二甲酸乙二醇酯为有价化学品和氢燃料。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-09-11 DOI: 10.1007/s40820-023-01181-8
Zhijie Chen, Renji Zheng, Teng Bao, Tianyi Ma, Wei Wei, Yansong Shen, Bing-Jie Ni

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management. Recently, electrocatalytically converting polyethylene terephthalate (PET) into formate and hydrogen has aroused great interest, while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol (PET monomer) oxidation reaction (EGOR) remains a challenge. Herein, a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy. Benefiting from the interconnected ultrathin nanosheet architecture, dual dopants induced up-shifting d band centre and facilitated in situ structural reconstruction, the Co and Cl co-doped Ni3S2 (Co, Cl-NiS) outperforms the single-doped and undoped analogues for EGOR. The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency (> 92%) and selectivity (> 91%) at high current densities (> 400 mA cm−2). Besides producing formate, the bifunctional Co, Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h−1 in 2 M KOH, at 1.7 V. This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes, but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

电子升级回收塑料废物为增值化学品/燃料是塑料废物管理的一种有吸引力和可持续的方式。近年来,电催化将聚对苯二甲酸乙二醇酯(PET)转化为甲酸酯和氢引起了人们的极大兴趣,但开发高效、低成本、高选择性的中心乙二醇(PET单体)氧化反应催化剂仍然是一个挑战。本文采用钴和氯化物共掺杂策略,设计了一种用于塑料垃圾电升级回收的高性能硫化镍催化剂。Co和Cl共掺Ni3S2 (Co, Cl- nis)的EGOR性能优于单掺杂和未掺杂的类似物,得益于相互连接的超薄纳米片结构,双掺杂诱导d带中心上移并促进原位结构重建。在高电流密度(> 400 mA cm-2)下,自进化的sulfide@oxyhydroxide异质结构具有高的Faradic效率(> 92%)和选择性(> 91%)。除产甲酸外,双官能团Co, cl - ni辅助的PET水解产物电解槽在2 M KOH、1.7 V条件下的产氢率可达50.26 mmol h-1。该研究不仅展示了双掺杂策略,为电化学转化过程设计具有成本效益的双功能催化剂,而且为塑料废物升级回收和同时节能制氢提供了绿色可持续的途径。
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引用次数: 0
Zinc–Bromine Rechargeable Batteries: From Device Configuration, Electrochemistry, Material to Performance Evaluation 锌-溴可充电电池:从设备配置,电化学,材料到性能评估。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-31 DOI: 10.1007/s40820-023-01174-7
Norah S. Alghamdi, Masud Rana, Xiyue Peng, Yongxin Huang, Jaeho Lee, Jingwei Hou, Ian R. Gentle, Lianzhou Wang, Bin Luo

Zinc–bromine rechargeable batteries (ZBRBs) are one of the most powerful candidates for next-generation energy storage due to their potentially lower material cost, deep discharge capability, non-flammable electrolytes, relatively long lifetime and good reversibility. However, many opportunities remain to improve the efficiency and stability of these batteries for long-life operation. Here, we discuss the device configurations, working mechanisms and performance evaluation of ZBRBs. Both non-flow (static) and flow-type cells are highlighted in detail in this review. The fundamental electrochemical aspects, including the key challenges and promising solutions, are discussed, with particular attention paid to zinc and bromine half-cells, as their performance plays a critical role in determining the electrochemical performance of the battery system. The following sections examine the key performance metrics of ZBRBs and assessment methods using various ex situ and in situ/operando techniques. The review concludes with insights into future developments and prospects for high-performance ZBRBs.

锌溴可充电电池(zbrb)具有材料成本低、深度放电能力强、电解质不可燃、使用寿命长、可逆性好等优点,是下一代储能技术的有力候选者之一。然而,提高这些电池的效率和稳定性以实现长寿命运行仍有许多机会。本文讨论了zbrb的器件结构、工作机理和性能评价。非流动(静态)和流动型细胞在本综述中都有详细介绍。讨论了基本的电化学方面,包括主要挑战和有希望的解决方案,特别关注锌和溴半电池,因为它们的性能在决定电池系统的电化学性能方面起着关键作用。下面几节将研究zbrb的关键性能指标,以及使用各种非原位和原位/操作技术的评估方法。最后对高性能zbrb的未来发展和前景进行了展望。
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引用次数: 0
Recent Advances in Structural Optimization and Surface Modification on Current Collectors for High-Performance Zinc Anode: Principles, Strategies, and Challenges 高性能锌阳极集流器结构优化与表面改性研究进展:原理、策略与挑战。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-31 DOI: 10.1007/s40820-023-01177-4
Yuxin Gong, Bo Wang, Huaizheng Ren, Deyu Li, Dianlong Wang, Huakun Liu, Shixue Dou

Highlights

  • The mechanisms of the surface modification and structure design of zinc anode current collectors were summarized.

  • The recent advances of high-performance zinc anode current collectors were reviewed and categorized according to their working mechanisms.

  • The possible prospects and directions of zinc anode research were discussed.

近年来,锌离子电池(zib)以其低成本和高安全性被认为是储能系统的有力竞争者。然而,该体系的可逆性和可用性受到枝晶生长不可控、析氢和阳极侧腐蚀钝化等问题的影响。一种功能和结构设计良好的阳极集流器(CCs)被认为是解决这些问题的可行方案,但缺乏对其工作机制的总结。本文综述了锌阳极面临的挑战,以及改性阳极CCs的机理,可分为亲锌改性、结构设计和优选晶面取向。最后提出了锌阳极研究和设计的可能前景和方向,以期促进锌阳极的实际应用。
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引用次数: 0
Progress and Challenges Toward Effective Flexible Perovskite Solar Cells 高效柔性钙钛矿太阳能电池的进展与挑战。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-31 DOI: 10.1007/s40820-023-01165-8
Xiongjie Li, Haixuan Yu, Zhirong Liu, Junyi Huang, Xiaoting Ma, Yuping Liu, Qiang Sun, Letian Dai, Shahzada Ahmad, Yan Shen, Mingkui Wang

The demand for building-integrated photovoltaics and portable energy systems based on flexible photovoltaic technology such as perovskite embedded with exceptional flexibility and a superior power-to-mass ratio is enormous. The photoactive layer, i.e., the perovskite thin film, as a critical component of flexible perovskite solar cells (F-PSCs), still faces long-term stability issues when deformation occurs due to encountering temperature changes that also affect intrinsic rigidity. This literature investigation summarizes the main factors responsible for the rapid destruction of F-PSCs. We focus on long-term mechanical stability of F-PSCs together with the recent research protocols for improving this performance. Furthermore, we specify the progress in F-PSCs concerning precise design strategies of the functional layer to enhance the flexural endurance of perovskite films, such as internal stress engineering, grain boundary modification, self-healing strategy, and crystallization regulation. The existing challenges of oxygen-moisture stability and advanced encapsulation technologies of F-PSCs are also discussed. As concluding remarks, we propose our viewpoints on the large-scale commercial application of F-PSCs.

基于柔性光伏技术(如钙钛矿)的建筑集成光伏和便携式能源系统的需求是巨大的,这些光伏技术具有卓越的灵活性和优越的功率质量比。光活性层,即钙钛矿薄膜,作为柔性钙钛矿太阳能电池(f - psc)的关键组成部分,当遇到温度变化导致变形时,仍然面临长期稳定性问题,而温度变化也会影响其固有刚度。本文献综述了导致F-PSCs快速破坏的主要因素。我们专注于f - psc的长期机械稳定性,以及最近改善这种性能的研究方案。此外,我们详细介绍了f- psc在功能层的精确设计策略方面的进展,以提高钙钛矿薄膜的弯曲耐久性,如内应力工程、晶界修饰、自修复策略和结晶调节。讨论了f - psc在氧湿稳定性和先进封装技术方面存在的挑战。最后,我们对f - psc的大规模商业应用提出了自己的观点。
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引用次数: 0
Achieving Tunable Cold/Warm White-Light Emission in a Single Perovskite Material with Near-Unity Photoluminescence Quantum Yield 用接近统一的光致发光量子产率在单一钙钛矿材料中实现可调冷/暖白光发射。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-31 DOI: 10.1007/s40820-023-01168-5
Bo Zhou, Aixuan Du, Dong Ding, Zexiang Liu, Ye Wang, Haizhe Zhong, Henan Li, Hanlin Hu, Yumeng Shi

Single materials that exhibit efficient and stable white-light emission are highly desirable for lighting applications. This paper reports a novel zero-dimensional perovskite, Rb4CdCl6:Sn2+, Mn2+, which demonstrates exceptional white-light properties including adjustable correlated color temperature, high color rendering index of up to 85, and near-unity photoluminescence quantum yield of 99%. Using a co-doping strategy involving Sn2+ and Mn2+, cyan-orange dual-band emission with complementary spectral ranges is activated by the self-trapped excitons and d-d transitions of the Sn2+ and Mn2+ centers in the Rb4CdCl6 host, respectively. Intriguingly, although Mn2+ ions doped in Rb4CdCl6 are difficult to excite, efficient Mn2+ emission can be realized through an ultra-high-efficient energy transfer between Sn2+ and Mn2+ via the formation of adjacent exchange-coupled Sn–Mn pairs. Benefiting from this efficient Dexter energy transfer process, the dual emission shares the same optimal excitation wavelengths of the Sn2+ centers and suppresses the non-radiative vibration relaxation significantly. Moreover, the relative intensities of the dual-emission components can be modulated flexibly by adjusting the fraction of the Sn2+ ions to the Sn–Mn pairs. This co-doping approach involving short-range energy transfer represents a promising avenue for achieving high-quality white light within a single material.

单一材料表现出高效和稳定的白光发射是非常理想的照明应用。本文报道了一种新型的零维钙钛矿Rb4CdCl6:Sn2+, Mn2+,它具有特殊的白光性能,包括可调的相关色温,高达85的显色指数和99%的近统一光致发光量子产率。采用Sn2+和Mn2+共掺杂策略,Rb4CdCl6主体中Sn2+和Mn2+中心的自捕获激子和d-d跃迁分别激活了具有互补光谱范围的青橙色双带发射。有趣的是,虽然在Rb4CdCl6中掺杂的Mn2+离子很难激发,但通过形成相邻的交换偶联Sn-Mn对,Sn2+和Mn2+之间的超高效率能量转移可以实现Mn2+的高效发射。得益于这种高效的Dexter能量传递过程,双发射具有相同的Sn2+中心的最佳激发波长,显著抑制了非辐射振动的弛豫。此外,通过调整Sn-Mn对中Sn2+离子的比例,可以灵活地调节双发射组分的相对强度。这种涉及短距离能量转移的共掺杂方法代表了在单一材料内实现高质量白光的有希望的途径。
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引用次数: 0
Synergistic “Anchor-Capture” Enabled by Amino and Carboxyl for Constructing Robust Interface of Zn Anode 氨基和羧基协同“锚捕获”构建锌阳极坚固界面。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-28 DOI: 10.1007/s40820-023-01171-w
Zhen Luo, Yufan Xia, Shuang Chen, Xingxing Wu, Ran Zeng, Xuan Zhang, Hongge Pan, Mi Yan, Tingting Shi, Kai Tao, Ben Bin Xu, Yinzhu Jiang

Highlights

  • The synergistic “anchor-capture” mechanism of polar groups on Zn stripping/plating process is firstly proposed.

  • The amino group firmly anchors on Zn surface and the carboxyl group strongly captures Zn2+, constructing a robust anode–electrolyte interface and inducing uniform Zn deposition.

  • The ultra-stable cycle lifespan of Zn–Zn symmetric cell (over 2800 h) and high utilization rate of Zn anode (the depth of discharge up to 68% for 200 h) are achieved under the proposal of synergistic “anchor-capture.”

水溶液锌离子电池(AZIBs)已被公认为是最具应用前景的电池之一,但锌阳极-电解质界面的不稳定性极大地制约了其进一步发展。在这里,我们利用氨基酸甘氨酸(Gly)作为电解质添加剂来稳定锌阳极-电解质界面。这种独特的界面化学是由Gly分子中极性基团的协同“锚-捕获”效应促成的,表现为同时偶联氨基在Zn阳极表面锚定,羧基在局部区域捕获Zn2+。因此,这种坚固的阳极-电解质界面抑制了Zn2+的无序迁移,并有效地抑制了副反应和枝晶的生长。在1 mA cm-2和0.5 mAh cm-2循环500次后,锌阳极的可逆性显著提高,平均库仑效率达到99.22%。在高锌利用率(放电深度,DODZn)为68%的情况下,超薄锌箔(20 μm)的稳定循环寿命可达200 h。Zn- mno2电池优异的倍率性能和长期循环稳定性进一步证明了Gly在稳定Zn阳极方面的有效性。这项工作从azib的极性基团的具体作用揭示了增材设计。
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引用次数: 0
Integration of Multiple Heterointerfaces in a Hierarchical 0D@2D@1D Structure for Lightweight, Flexible, and Hydrophobic Multifunctional Electromagnetic Protective Fabrics 多异质界面在层次化0D@2D@1D结构中的集成用于轻质、柔性、疏水性多功能电磁防护织物。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-25 DOI: 10.1007/s40820-023-01179-2
Shuo Zhang, Xuehua Liu, Chenyu Jia, Zhengshuo Sun, Haowen Jiang, Zirui Jia, Guanglei Wu

The development of wearable multifunctional electromagnetic protective fabrics with multifunctional, low cost, and high efficiency remains a challenge. Here, inspired by the unique flower branch shape of “Thunberg’s meadowsweet” in nature, a nanofibrous composite membrane with hierarchical structure was constructed. Integrating sophisticated 0D@2D@1D hierarchical structures with multiple heterointerfaces can fully unleash the multifunctional application potential of composite membrane. The targeted induction method was used to precisely regulate the formation site and morphology of the metal–organic framework precursor, and intelligently integrate multiple heterostructures to enhance dielectric polarization, which improves the impedance matching and loss mechanisms of the electromagnetic wave absorbing materials. Due to the synergistic enhancement of electrospinning-derived carbon nanofiber “stems”, MOF-derived carbon nanosheet “petals” and transition metal selenide nano-particle “stamens”, the CoxSey/NiSe@CNSs@CNFs (CNCC) composite membrane obtains a minimum reflection loss value (RLmin) of -68.40 dB at 2.6 mm and a maximum effective absorption bandwidth (EAB) of 8.88 GHz at a thin thickness of 2.0 mm with a filling amount of only 5 wt%. In addition, the multi-component and hierarchical heterostructure endow the fibrous membrane with excellent flexibility, water resistance, thermal management, and other multifunctional properties. This work provides unique perspectives for the precise design and rational application of multifunctional fabrics.

开发多功能、低成本、高效率的可穿戴多功能电磁防护织物仍然是一个挑战。在这里,灵感来自于自然界中独特的“通贝里绣线菊”的花枝形状,构建了一种具有层次结构的纳米纤维复合膜。将复杂的0D@2D@1D层次结构与多个异质界面相结合,可以充分释放复合膜的多功能应用潜力。利用定向感应方法精确调控金属-有机骨架前驱体的形成部位和形态,智能整合多种异质结构增强介质极化,改善电磁波吸收材料的阻抗匹配和损耗机制。由于电纺丝衍生的碳纳米纤维“茎”、mof衍生的碳纳米片“花瓣”和过渡金属硒化纳米颗粒“雄花”的协同增强,CoxSey/NiSe@CNSs@CNFs (CNCC)复合膜在2.6 mm处的最小反射损失值(RLmin)为-68.40 dB,在2.0 mm薄层处的最大有效吸收带宽(EAB)为8.88 GHz,填充量仅为5 wt%。此外,多组分和分层异质结构赋予纤维膜优异的柔韧性、耐水性、热管理等多功能性能。这项工作为多功能织物的精确设计和合理应用提供了独特的视角。
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引用次数: 0
Nanoengineering Metal–Organic Frameworks and Derivatives for Electrosynthesis of Ammonia 电合成氨的纳米工程金属有机框架及其衍生物。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-24 DOI: 10.1007/s40820-023-01169-4
Daming Feng, Lixue Zhou, Timothy J. White, Anthony K. Cheetham, Tianyi Ma, Fengxia Wei

Highlights

  • Recent advances in the metal–organic framework (MOF)-related catalysts for electrochemical ammonia synthesis protocols under ambient reaction conditions are summarized and discussed.

  • The design and fabrication of efficient electrocatalysts from MOF for the reduction of N2 and NO3 are systematically analyzed.

  • Based on the current advances, the ongoing challenges and promising perspectives are highlighted.

温和条件下的电催化合成作为工业应用的一种实用替代方法,特别是在绿色氨(NH3)工业中已变得越来越重要。设计合理的电催化剂对实现优异的催化性能起着至关重要的作用。在各种有前景的纳米材料中,金属有机框架(mof)是开发高效电催化NH3合成的有竞争力的候选材料,可以从简单的含氮分子或离子,如N2和NO3-。综述了近年来mof电催化剂在NH3电合成中的研究进展,并对其在N2还原反应(NRR)和NO3-还原反应(NO3RR)中的应用进行了分类和讨论。首先,阐述了该工艺的基本原理,包括N2和NO3-生成NH3的可能机理、相应的电催化装置、反应效率评价参数以及NH3产率的检测方法。然后,详细讨论了NRR过程的电催化剂,包括原始mof, mof杂化,mof衍生的n掺杂多孔碳,mof热解的单原子催化剂以及其他mof相关材料。随后,还列出并讨论了mof相关的NO3RR工艺。最后,提出了合理设计和制造mof电催化剂用于电化学NH3合成的挑战和前景,如人工智能研究方法的发展、mof相关催化剂合成方法的创新、表征技术的进步以及电催化反应的扩展。
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引用次数: 0
Cerium Methacrylate Assisted Preparation of Highly Thermally Conductive and Anticorrosive Multifunctional Coatings for Heat Conduction Metals Protection 甲基丙烯酸铈辅助制备高导热防腐蚀多功能热传导金属防护涂料。
IF 26.6 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-08-18 DOI: 10.1007/s40820-023-01163-w
Fei Xu, Peng Ye, Jianwen Peng, Haolei Geng, Yexiang Cui, Di Bao, Renjie Lu, Hongyu Zhu, Yanji Zhu, Huaiyuan Wang

Preparing polymeric coatings with well corrosion resistance and high thermal conductivity (TC) to prolong operational life and ensure service reliability of heat conductive metallic materials has long been a substantive and urgent need while a difficult task. Here we report a multifunctional epoxy composite coating (F-CB/CEP) by synthesizing cerium methacrylate and ingeniously using it as a novel curing agent with corrosion inhibit for epoxy resin and modifier for boron nitride through "cation-π" interaction. The prepared F-CB/CEP coating presents a high TC of 4.29 W m−1 K−1, which is much higher than other reported anti-corrosion polymer coatings and thereby endowing metal materials coated by this coating with outstanding thermal management performance compared with those coated by pure epoxy coating. Meanwhile, the low-frequency impedance remains at 5.1 × 1011 Ω cm2 even after 181 days of immersion in 3.5 wt% NaCl solution. Besides, the coating also exhibits well hydrophobicity, self-cleaning properties, temperature resistance and adhesion. This work provides valuable insights for the preparation of high-performance composite coatings with potential to be used as advanced multifunctional thermal management materials, especially for heat conduction metals protection.

制备具有良好耐蚀性和高导热性的聚合物涂层,以延长导热金属材料的使用寿命和保证其使用可靠性,是一项现实而迫切的任务,也是一项艰巨的任务。本文报道了合成甲基丙烯酸铈并巧妙地将其作为新型固化剂,通过阳离子-π相互作用对环氧树脂具有抑制作用,并对氮化硼具有改性作用,制备了多功能环氧复合涂层(F-CB/CEP)。制备的F-CB/CEP涂层具有4.29 W m-1 K-1的高TC,远高于已有报道的其他防腐聚合物涂层,因此与纯环氧涂层相比,该涂层涂层的金属材料具有出色的热管理性能。同时,在3.5 wt% NaCl溶液中浸泡181天后,其低频阻抗仍保持在5.1 × 1011 Ω cm2。此外,该涂层还具有良好的疏水性、自洁性、耐温性和附着力。该研究为高性能复合涂层的制备提供了有价值的见解,具有作为先进多功能热管理材料的潜力,特别是在导热金属保护方面。
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引用次数: 0
期刊
Nano-Micro Letters
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