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Reveal and correlate working geometry and surface chemistry of Ni nanocatalysts in CO2 reforming of methane 揭示并关联镍纳米催化剂在甲烷二氧化碳转化过程中的工作几何形状和表面化学性质
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-10 DOI: 10.1016/j.mattod.2024.07.006
Zichun Wang , Qian Lv , Ang Li , Ping Wu , Lizhuo Wang , Wei Li , Yijiao Jiang , Catherine Stampfl , Xiaozhou Liao , Jun Huang , Xiaodong Han

The commercialization of Ni-based catalysts in CO2 dry reforming of methane (DRM) suffers from their quick deactivation. Here, we reveal each reaction pathway for DRM based on the Ni catalyst composition and geometry under working conditions, through one working platform combining in situ high resolution Cs corrected environmental transmission electron microscopy and electron energy-loss spectroscopy coupled with mass spectroscopy. The formation of Ni3C has been found to inhibit the decomposition of CO2 and CH4, and to promote the formation of onion-like carbon to encapsulate the Ni catalysts, leading to the deactivation of the Ni-based catalysts. Designing the suitable supports or promoters to keep the Ni surface structure under Ni-NiO cycle can drive the simultaneously amorphous carbon deposition-consumption cycle and minimise the coke formation. This research is not only for developing coke resistance Ni catalysts in the DRM, but also significant for investigating many catalysis challenges both in research and engineering.

镍基催化剂在二氧化碳甲烷干法重整(DRM)中的商业化受到其快速失活的影响。在此,我们通过结合原位高分辨率铯校正环境透射电子显微镜和电子能量损失光谱与质谱的工作平台,根据工作条件下 Ni 催化剂的组成和几何形状,揭示了 DRM 的各个反应途径。研究发现,Ni3C 的形成会抑制 CO2 和 CH4 的分解,并促进洋葱状碳的形成以包裹 Ni 催化剂,从而导致 Ni 基催化剂失活。设计合适的支撑物或促进剂以保持 Ni-NiO 循环下的 Ni 表面结构,可同时推动无定形碳的沉积-消耗循环,并最大限度地减少焦炭的形成。这项研究不仅有助于开发 DRM 中的抗焦化镍催化剂,而且对研究和工程领域的许多催化挑战也具有重要意义。
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引用次数: 0
Design of metal ion-catecholate complexes towards advanced materials 设计金属离子-邻苯二酚复合物,开发先进材料
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-08 DOI: 10.1016/j.mattod.2024.07.010
Yuan Zou , Xianheng Wang , Yiwen Li , Yiyun Cheng

Metal ion-catecholate complexes (MCCs) extensively exist in plants and animals, which are in charge of versatile biological functions, such as constructing organs, controlled releasing metal ions and antibacterial. Inspired by this, researchers have exploited various kinds of artificial MCCs, which can serve as structural and functional synthons to construct advanced materials. In terms of the structural contribution, these complexes exhibit not only physical interactions, including metal-coordination, hydrogen bonding, π-π stacking and cation-π interactions, but also rich chemical reactions, including radical polymerization, Schiff base reaction and Michael addition. In terms of functional contribution, the complexes can endow the materials with the intrinsic properties of polyphenols and metal ions, including antioxidant, adhesion, antibacterial, bioimaging and catalyst. In addition, some emerging and fantastic functions are also originally from the complexes, such as tunable mechanical property, self-healing, controlled release and photothermal effect. In this review paper, we comprehensively discuss the recent development of MCC-based materials, including coatings, particles, metallogels and metal–organic frameworks (MOFs). Perspectives in this field has also been put forward as well.

金属离子-儿茶酚复合物(MCCs)广泛存在于动植物体内,具有构建器官、控制释放金属离子和抗菌等多种生物功能。受此启发,研究人员开发了各种人工 MCC,它们可以作为结构和功能合成物来构建先进材料。在结构贡献方面,这些配合物不仅表现出物理相互作用,包括金属配位、氢键、π-π堆叠和阳离子-π相互作用,还表现出丰富的化学反应,包括自由基聚合、席夫碱反应和迈克尔加成反应。在功能贡献方面,配合物可以赋予材料多酚和金属离子的固有特性,包括抗氧化、粘附、抗菌、生物成像和催化剂。此外,复合物还具有一些新兴的奇妙功能,如可调机械性能、自愈、控释和光热效应。在这篇综述论文中,我们全面讨论了基于 MCC 材料的最新发展,包括涂层、颗粒、金属凝胶和金属有机框架(MOFs)。同时还提出了该领域的展望。
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引用次数: 0
Carbon nanotube materials for future integrated circuit applications 未来集成电路应用中的碳纳米管材料
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-06 DOI: 10.1016/j.mattod.2024.07.008
Yumeng Ze , Yifan Liu , Bo Wang , Huimin Yin , Chuanhong Jin , Zhiyong Zhang

Aligned carbon nanotubes (A-CNTs) have been demonstrated to be promising materials for constructing advanced complementary metal–oxide–semiconductor (CMOS) field-effect transistors (FETs) for future integrated circuits (ICs). However, the requirements of A-CNT materials from the perspective of IC applications, such as the distributions of length, alignment, diameter and density of CNTs, have not been explicitly researched or mentioned before. In this article, we review the progress on CNT electronics and electronic-grade materials and establish material criteria for A-CNTs applicable to advanced electronics according to the developing roadmap of CNT-based ICs. Specifically, electrical performance predictions for A-CNT CMOS FETs at various technology nodes are built based on a theoretical model and experimental results, and then, the criteria for ideal A-CNTs are outlined by evaluating the energy-delay product (EDP) advantage of CNT FETs over similar node commercial silicon (Si)-based CMOS transistors. The fine requirements for A-CNT materials are estimated for 90 nm, 22 nm, 7 nm, and 3 nm node CNT CMOS FETs, which present significant advantages in terms of energy efficiency over Si CMOS transistors. The criteria will guide the development of CNT materials for future ICs and provide a comprehensive assessment of the opportunities and challenges in CNT electronics.

有序排列的碳纳米管(A-CNT)已被证明是一种很有前途的材料,可用于构建未来集成电路(IC)中的先进互补金属氧化物半导体(CMOS)场效应晶体管(FET)。然而,从集成电路应用的角度来看,对 A-CNT 材料的要求,如 CNT 的长度、排列、直径和密度分布等,以前还没有明确的研究或提及。在本文中,我们回顾了 CNT 电子学和电子级材料的研究进展,并根据 CNT 集成电路的发展路线图,建立了适用于先进电子学的 A-CNT 材料标准。具体来说,我们基于理论模型和实验结果,对不同技术节点的 A-CNT CMOS FET 的电气性能进行了预测,然后通过评估 CNT FET 相对于类似节点商用硅 (Si) 基 CMOS 晶体管的能量延迟积 (EDP) 优势,概述了理想 A-CNT 的标准。估计了 90 nm、22 nm、7 nm 和 3 nm 节点 CNT CMOS FET 对 A-CNT 材料的精细要求,与硅 CMOS 晶体管相比,这些器件在能效方面具有显著优势。这些标准将指导未来集成电路中 CNT 材料的开发,并对 CNT 电子技术的机遇和挑战进行全面评估。
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引用次数: 0
An efficient construction of nano-interfaces for excellent coking tolerance of cermet anodes 高效构建纳米界面,提高金属陶瓷阳极的结焦耐受性
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-03 DOI: 10.1016/j.mattod.2024.07.007
Kang Xu , Hua Zhang , Yangsen Xu , Feng Zhu , Fan He , Ying Liu , Kotaro Sasaki , YongMan Choi , Yu Chen

Solid oxide fuel cells (SOFCs) are promising energy conversion devices for the effective and convenient utilization of hydrocarbons (for example, methane) to electricity. However, the development of direct methane SOFCs is primarily hindered by the poor coking tolerance of the state-of-the-art Ni-based cermet anodes. Herein, we efficiently construct nano-interfaces in the anode by infiltrating a Ni0.6Y0.064Zr0.336O2-δ (NYZ) catalyst onto the traditional Ni-based cermet anode to effectively enhance the coking tolerance. After being reduced in H2, Ni and Y0.16Zr0.84O2-δ (YSZ) nanoparticles (NPs) are in situ formed on the surface of the Ni-YSZ substrate. The roughened anode demonstrates significantly improved fuel oxidation activity and coking tolerance, due likely to the formation of nano-interfaces. Specifically, when applied in the Ni-YSZ-based anode-supported SOFCs, a high peak power density of 1.785 W cm−2 and a stable operation of ∼ 240 h with no observable degradation is achieved at 750 °C in nearly dry methane (3 % H2O). A density functional theory study suggests that the excellent coking tolerance is attributed to the formation of OH species on Ni/YSZ nano-interfaces, which would further interact with intermediate carbon species to generate COH intermediates.

固体氧化物燃料电池(SOFC)是一种很有前途的能量转换设备,可有效、方便地将碳氢化合物(如甲烷)转化为电能。然而,最先进的镍基金属陶瓷阳极结焦耐受性差是阻碍直接甲烷 SOFC 发展的主要原因。在此,我们通过在传统的镍基金属陶瓷阳极上渗入镍0.6Y0.064Zr0.336O2-δ(NYZ)催化剂,在阳极中有效地构建了纳米界面,从而有效地提高了结焦耐受性。在 H2 中还原后,Ni 和 Y0.16Zr0.84O2-δ (YSZ)纳米颗粒(NPs)在 Ni-YSZ 基质表面原位形成。由于形成了纳米界面,粗化阳极的燃料氧化活性和结焦耐受性得到显著提高。具体来说,当应用于基于 Ni-YSZ 的阳极支撑 SOFC 时,在 750 °C 的近干甲烷(3 % H2O)中可达到 1.785 W cm-2 的高峰值功率密度,并可稳定运行 ∼ 240 h,且无明显降解。密度泛函理论研究表明,Ni/YSZ 纳米界面上形成的 OH 物种具有出色的结焦耐受性,这些 OH 物种将进一步与中间碳物种相互作用,生成 COH 中间产物。
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引用次数: 0
PDGFR-targeted nanovesicles for restraining breast cancer hepatic metastasis via hepatic stellate cell regression and NK cell activation 通过肝星状细胞消退和 NK 细胞激活抑制乳腺癌肝转移的 PDGFR 靶向纳米颗粒
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-03 DOI: 10.1016/j.mattod.2024.07.005
Mengjie Kong , Yan Peng , Yujie Miao , Liyan Qiu

Preventing breast cancer liver metastasis presents formidable challenges with multifaceted obstacles. In the case of acute and chronic liver injury, the disrupted liver microenvironment induced by activated hepatic stellate cells (aHSCs) would suppress immune surveillance and license the re-multiplication of disseminated tumor cells (DTCs). Herein, a cyclic peptide pPB modified nanovesicle with aHSCs targeting capability was constructed as CP-SB-siRNA to co-deliver hydrophobic SB431542 and nucleic acid drug CXCL12 siRNA. Due to the TGF-β signaling inhibition of SB431542, CP-SB-siRNA significantly suppressed the expression levels of genes coding the uppermost fibrosis-associated proteins including α-sma, Col-1 and Col-3 in aHSCs. On the other hand, the gene and protein expression level of metastasis-associated chemokine CXCL12 was significantly decreased. In addition, CP-SB-siRNA could regain the function of NK cells and attenuate the breast cancer proliferation through CXCL12-CXCR4 axis. On both breast cancer spontaneous metastasis with fibrosis mouse model and breast cancer via hematogenous metastasis with fibrosis mouse model, CP-SB-siRNA successfully reversed hepatic fibrosis by regressing aHSCs, and thereby restored the liver microenvironment, ultimately inhibiting breast cancer hepatic metastasis. This nanomaterial vector, featuring targeting and drug co-delivery functionalities, exhibited a great potential to restrain breast cancer hepatic metastasis based on the relationship among aHSCs, NK cells and DTCs.

预防乳腺癌肝转移是一项艰巨的挑战,面临着多方面的障碍。在急性和慢性肝损伤的情况下,活化的肝星状细胞(aHSCs)诱导的肝脏微环境破坏会抑制免疫监视,并允许播散性肿瘤细胞(DTCs)的再次繁殖。在此,我们构建了一种具有aHSCs靶向能力的环肽pPB修饰纳米囊泡,即CP-SB-siRNA,用于共同递送疏水性SB431542和核酸药物CXCL12 siRNA。由于SB431542对TGF-β信号传导的抑制作用,CP-SB-siRNA显著抑制了α-sma、Col-1和Col-3等最上层纤维化相关蛋白编码基因在aHSCs中的表达水平。另一方面,转移相关趋化因子 CXCL12 的基因和蛋白表达水平明显下降。此外,CP-SB-siRNA 还能恢复 NK 细胞的功能,并通过 CXCL12-CXCR4 轴抑制乳腺癌的增殖。在乳腺癌自发转移伴肝纤维化小鼠模型和乳腺癌经血行转移伴肝纤维化小鼠模型上,CP-SB-siRNA 都能通过抑制 aHSCs 成功逆转肝纤维化,从而恢复肝脏微环境,最终抑制乳腺癌的肝转移。基于造血干细胞、NK细胞和DTC之间的关系,这种具有靶向和药物协同递送功能的纳米材料载体显示出抑制乳腺癌肝转移的巨大潜力。
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引用次数: 0
4D printing: The spotlight for 3D printed smart materials 4D 打印:3D 打印智能材料的焦点
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.mattod.2024.06.004
Jia Chen , Christian Virrueta , Shengmin Zhang , Chuanbin Mao , Jianglin Wang

4D printing combines the typical 3D printing with “smart materials”, allowing 3D printed materials to undergo a structural change over time. Since its original concept was first introduced in 2013, 4D printing became an innovative research that has received more attention from scientists in different fields. This review summarizes the progress achieved in 4D printing technologies and their associated materials. First, the technology and process of 4D printing are overviewed, and then the structure and properties of smart materials utilized in 4D printing are analyzed in depth, including metamaterials, shape memory materials, hydrogels, and self-healing polymers. We systematically illustrate the morphing mechanisms of the 4D printed smart materials, and then critically discuss the stimuli that can trigger transformation in the 4D printed smart materials, including heat, light, moisture, pH, electric current, and magnetic field. For 4D printed smart materials, all the changes programmed in the materials follow a mathematical model that allows scientists to predict and design the desired behaviors of the structures, using parameters such as the material distribution and the spatial gradients of the metric tensor. We finally conclude with the discussion of future challenges and opportunities for this ever-growing technology. Overall, 4D printing can create dynamic structures programmed to be responsive to external stimuli in the environment, widening its use in a myriad of applications such as rapid prototyping, electronics, biomedicine, soft robotics, self-assembly structures, smart sensors, and dynamic actuators.

4D 打印将典型的 3D 打印与 "智能材料 "相结合,使 3D 打印材料随着时间的推移发生结构变化。自 2013 年首次提出其最初概念以来,4D 打印已成为一项创新研究,受到不同领域科学家的更多关注。本综述总结了 4D 打印技术及其相关材料所取得的进展。首先概述了 4D 打印的技术和过程,然后深入分析了 4D 打印中使用的智能材料的结构和性能,包括超材料、形状记忆材料、水凝胶和自愈合聚合物。我们系统地阐述了 4D 打印智能材料的变形机理,然后批判性地讨论了能引发 4D 打印智能材料变形的刺激因素,包括热、光、湿度、pH 值、电流和磁场。对于 4D 打印智能材料来说,材料中的所有变化都遵循一个数学模型,科学家可以利用材料分布和度量张量的空间梯度等参数来预测和设计结构的预期行为。最后,我们讨论了这项不断发展的技术未来面临的挑战和机遇。总之,4D 打印可以创建动态结构,通过编程对环境中的外部刺激做出响应,从而扩大其在快速原型、电子、生物医学、软机器人、自组装结构、智能传感器和动态致动器等众多领域的应用。
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引用次数: 0
Overview of high-entropy oxide ceramics 高熵氧化物陶瓷概述
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.mattod.2024.06.005
Yitao Jiao , Jian Dai , Zhenhao Fan , Junye Cheng , Guangping Zheng , Lawan Grema , Junwen Zhong , Hai-Feng Li , Dawei Wang

In 2004, Yeh and Cantor introduced high-entropy alloys (HEAs), which maximize configurational entropy by utilizing nearly equal elemental molar ratios. These HEAs are valuable for exploring the central regions of phase diagrams. Building on this concept, Rost et al. proposed entropy-stabilized oxides in 2015, revealing that high-entropy oxides (HEOs) exhibit structural stability driven by entropy. This article provides a comprehensive overview of HEOs, with a specific focus on high-entropy oxide ceramics (HEOCs). The paper explores the origins of the high-entropy concept and the fundamental effects of high-entropy materials. It examines entropy from its basic definition and investigates microscopic atomic distribution, crystal-level distortions, and electronic structures. Additionally, the article introduces theoretical prediction methods applied to high-entropy materials. Furthermore, this review systematically summarizes HEOCs, encompassing three key aspects: crystal structure, preparation methods, and performance applications. Finally, the review concludes by proposing future research directions based on the current progress in HEOCs.

2004 年,Yeh 和 Cantor 提出了高熵合金 (HEA),这种合金通过利用几乎相等的元素摩尔比来最大化构型熵。这些高熵合金对于探索相图的中心区域非常有价值。基于这一概念,Rost 等人于 2015 年提出了熵稳定氧化物,揭示了高熵氧化物(HEOs)在熵驱动下表现出的结构稳定性。本文全面概述了高熵氧化物,并特别关注高熵氧化物陶瓷(HEOC)。本文探讨了高熵概念的起源和高熵材料的基本效应。文章从熵的基本定义出发,研究了微观原子分布、晶体畸变和电子结构。此外,文章还介绍了应用于高熵材料的理论预测方法。此外,这篇综述系统地总结了高熵材料,包括三个关键方面:晶体结构、制备方法和性能应用。最后,本综述根据目前 HEOC 的研究进展提出了未来的研究方向。
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引用次数: 0
Bio-inspired mechanical metamaterial with ultrahigh load-bearing capacity for energy dissipation 具有超高承载能力的生物启发机械超材料,用于消散能量
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.mattod.2024.06.003
Sen Yan , Wenlong Liu , Xiaojun Tan , Zhiqiang Meng , Weijia Luo , Hang Jin , Yongzheng Wen , Jingbo Sun , Lingling Wu , Ji Zhou

Mechanical metamaterials with energy-dissipating properties can provide impact mitigation in the field of engineering. However, current energy-dissipating metamaterials frequently face a tradeoff between energy-dissipation performance and load-bearing capability, severely limiting their practicality in high-intensity impact scenarios. Here, inspired by mushroom gills, we propose a mechanism for the snap-through buckling induced by geometric frustration, and we construct a snap-through metamaterial (STM) to address this problem. By analyzing the bifurcation buckling phenomenon, the STM is improved with higher energy-dissipation efficiency. Experiments demonstrate that the STM adaptively dissipates energy and mitigates impacts, achieving up to 33% reduction, in a reusable, self-recoverable, and rate-independent manner, leading to comprehensive performance. Employing a preloading strategy further enhances its impact mitigation capability as required. Notably, the STM exhibits a remarkable load-bearing capacity of up to 55 times higher than those of previous designs. The proposed design strategy of STMs paves the way for the development of interaction-based metamaterials, enabling applications in advanced dampers, mechanical waveguides, soft robotics, and low-frequency energy harvesters.

具有能量耗散特性的机械超材料可在工程领域提供冲击缓解功能。然而,目前的能量耗散超材料经常面临能量耗散性能和承载能力之间的权衡,严重限制了其在高强度冲击场景中的实用性。在此,我们受蘑菇伞的启发,提出了一种由几何挫折引起的快穿屈曲机制,并构建了一种快穿超材料(STM)来解决这一问题。通过分析分叉屈曲现象,我们改进了 STM,使其具有更高的能量耗散效率。实验证明,STM 以可重复使用、可自我恢复和与速率无关的方式,自适应地耗散能量并减轻冲击,最多可减少 33%,从而实现综合性能。采用预加载策略可根据需要进一步增强其冲击缓解能力。值得注意的是,STM 的承载能力比以前的设计高出 55 倍。所提出的 STM 设计策略为开发基于相互作用的超材料铺平了道路,可应用于高级阻尼器、机械波导、软机器人和低频能量收集器。
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引用次数: 0
Resolving the early-stage nucleus structure and evolution in atomic systems 解析原子系统中早期阶段的核结构与演化
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.mattod.2024.06.002
Yun Li , Hubin Luo , Fang Wang , Yinhang Yang , Cuimeng Song , J. Ping Liu , Izabela Szlufarska , Jian Zhang , Baogen Shen

Nucleation underpins a vast range of phase-transition phenomena in many disciplines. Critical to revealing nucleation thermodynamics and kinetics is the understanding of the nucleus structure at its early stage. Typically, it is assumed that nucleation is a sudden local structural transition from one phase to another. Here, we are able to access fundamental steps in the nucleation from amorphous phase by a combination of molecular simulations and experimental observation. We discover a surprising pathway of semicrystalline nucleation where one of the materials components crystallizes and another remains amorphous between the crystalline planes in the nuclei. The early-stage crystallization nucleus is robustly evidenced to undergo a gradual ordering and densification, originating from the presence of diffuse interfaces, and renders an ultralow interfacial energy that is orders of magnitude lower than those typically used in various formulations of nucleation. Our study provides critical information and insight for the early stages of nucleation that determine how crystallization is initiated and benefits controllable synthesis of materials.

成核是许多学科中大量相变现象的基础。要揭示成核热力学和动力学,关键在于了解成核初期的结构。通常,人们认为成核是从一个相到另一个相的突然局部结构转变。在这里,我们通过分子模拟和实验观察相结合的方法,了解了从非晶相成核的基本步骤。我们发现了一种令人惊讶的半结晶成核途径,其中一种材料成分结晶,而另一种材料成分在晶核的晶面之间保持非晶状态。早期阶段的结晶核被有力地证明经历了逐渐的有序化和致密化,这源于扩散界面的存在,并产生了超低的界面能,比各种成核公式中通常使用的界面能低几个数量级。我们的研究为决定如何开始结晶的成核早期阶段提供了重要信息和见解,并有利于材料的可控合成。
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引用次数: 0
Corrigendum to “Oxygen-dislocation interaction-mediated nanotwinned nanomartensites in ultra-strong and ductile titanium alloys” [Mater. Today 75 (2024) 85–96] 对 "超强韧性钛合金中氧-位错相互作用介导的纳米细化纳米敏化物 "的更正 [Mater. Today 75 (2024) 85-96]
IF 21.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.mattod.2024.06.014
Chongle Zhang, Xuanzhe Li, Suzhi Li, Jinyu Zhang, Jiao Li, Gang Liu, Jun Sun
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引用次数: 0
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