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Grain size control in quasi-two-dimensional perovskite thin film via intermediate phase engineering for efficient bound exciton generation 通过中间相工程控制准二维过氧化物薄膜的晶粒尺寸,实现高效的束缚激子生成
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-29 DOI: 10.1007/s40843-024-3127-5
Guohui Li  (, ), Wenhui Zhao  (, ), Kai Lin  (, ), Kefan Zhao  (, ), Yujing Wang  (, ), Aohua Niu  (, ), Rong Weng  (, ), Kaibo Zheng  (, ), Yanxia Cui  (, )

Quasi-two dimensional (2D) perovskites have emerged as a promising class of materials due to their remarkable photoluminescence efficiency, which stems from their exceptionally high exciton binding energies. The spatial confinement of excitons within smaller grain sizes could enhance the formation of biexcitons leading to higher radiative recombination efficiency. However, the synthesis of high-quality quasi-2D perovskite thin films with controllable grain sizes remains a challenging task. In this study, we present a facile method for achieving quasi-2D perovskite thin films with controllable grain sizes ranging from 500 to 900 nm. This is accomplished by intermediate phase engineering during the film fabrication process. Our results demonstrate that quasi-2D perovskite films with smaller grain sizes exhibit more efficient bound exciton generation and a reduced stimulated emission threshold down to 15.89 µJ cm−2. Furthermore, femtosecond transient absorption measurements reveal that the decay time of bound excitons is shorter in quasi-2D perovskites with smaller grain sizes compared to that of those with larger grains at the same pump density, which is 230.5 ps. This observation suggests a more efficient exciton recombination process in the smaller grain size regime. Our findings would offer a promising approach for the development of efficient bound exciton lasers.

准二维(2D)过氧化物晶体因其卓越的光致发光效率而成为一类前景广阔的材料,这种效率源于其极高的激子结合能。激子在较小晶粒尺寸内的空间束缚可促进双激子的形成,从而提高辐射重组效率。然而,合成晶粒尺寸可控的高质量准二维包晶薄膜仍然是一项具有挑战性的任务。在本研究中,我们提出了一种简便的方法来实现晶粒尺寸可控的 500 到 900 nm 的准二维包光体薄膜。这是通过薄膜制造过程中的中间相工程来实现的。我们的研究结果表明,晶粒尺寸更小的准二维包光体薄膜能更有效地产生束缚激子,并将受激发射阈值降低到 15.89 µJ cm-2。此外,飞秒瞬态吸收测量显示,在相同泵浦密度下,晶粒尺寸较小的准二维包光体与晶粒尺寸较大的准二维包光体相比,束缚激子的衰减时间更短(230.5 ps)。这一观察结果表明,在晶粒尺寸较小的情况下,激子重组过程的效率更高。我们的发现将为开发高效的束缚激子激光器提供一种可行的方法。
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引用次数: 0
Liquid metal catalyst for ammonia synthesis at low pressure
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-29 DOI: 10.1007/s40843-024-3161-x
Ziyue Zeng, Chenyang Wang, Lei Fu
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引用次数: 0
Floatable Fe-TiO2/hydrogel composite for photodegradation of water pollutants 用于光降解水污染物的可浮 Fe-TiO2/ 水凝胶复合材料
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1007/s40843-024-3150-2
Ying-Ying Jiao  (, ), Zhi-Yong Cheng  (, ), Hao Luo  (, ), Qiu-Ping Zhao  (, ), Xue-Yan Xiang  (, ), Zhi-Ming Zhang  (, )

The development of highly efficient and low-cost photocatalysts for degradation of organic pollutants become an effective approach for environmental remediation. However, the practical application of traditional powder catalyst in photocatalytic technology is limited due to its low recycling capacity, agglomeration and secondary pollution risk. Herein, a floating Fe-doped TiO2 and hydrogel (FTH) composite was synthesized for the photodegradation of Rhodamine B via a facile impregnation method. The photodegradation results show that the FTH composite exhibits a higher photocatalytic efficiency with degradation percentage (95.6%) compared with pure TiO2 (41.2%). The enhanced photocatalytic performance is attributed to its excellent flotation performance, providing a large number of active sites for pollutant degradation, contact with O2 and photons at the air/water interface. Remarkably, the adsorbed Rhodamine B in FTH can still be removed by exposing to light in the air alone, demonstrating strong recovery ability of the FIH composite catalyst. The floatable hydrogel nanocomposites offer a promising solution for scalable solar-drive degradation of water pollutants, paving the way for sustainable water treatment technologies.

开发高效、低成本的光催化剂来降解有机污染物已成为一种有效的环境修复方法。然而,由于传统粉末催化剂的回收能力低、团聚和二次污染风险等问题,其在光催化技术中的实际应用受到了限制。本文通过简便的浸渍法合成了一种漂浮的掺铁 TiO2 和水凝胶(FTH)复合材料,用于罗丹明 B 的光降解。光降解结果表明,与纯 TiO2(41.2%)相比,FTH 复合材料具有更高的光催化效率和降解率(95.6%)。光催化性能的提高归功于其出色的浮选性能,为污染物降解提供了大量的活性位点,并在空气/水界面与氧气和光子接触。值得注意的是,FTH 中吸附的罗丹明 B 仍然可以仅通过在空气中暴露于光而被去除,这表明 FIH 复合催化剂具有很强的回收能力。可浮水凝胶纳米复合材料为可扩展的太阳能驱动水污染物降解提供了一种前景广阔的解决方案,为可持续水处理技术铺平了道路。
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引用次数: 0
Sulfur and nitrogen dual-doped graphdiyne as a highly efficient metal-free electrocatalyst for the Zn-air battery 硫氮双掺杂石墨二炔作为锌-空气电池的高效无金属电催化剂
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1007/s40843-024-3126-1
Mengtian Huo  (, ), Jianhang Sun  (, ), Wei Liu  (, ), Qianyu Li  (, ), Jinfa Chang  (, ), Zihao Xing  (, )

Sulfur and nitrogen dual-doped graphdiyne (NSGD) has been found to be a promising catalyst for oxygen reduction reaction (ORR) through a combination of density functional theory (DFT) calculation and the application of oxygen evolution reaction (OER) experiments. The DFT analysis suggests that adsorption characteristics are significantly altered by resulting nitrogen and sulfur doping, which in turn affect the ORR activity. In particular, the NSGD-800 catalyst exhibits an increased ORR half-wave potential of 0.754 V, with enhanced stability due to the synergy effect of N and S. Meanwhile, thanks to the unique acetylene-rich structure of graphdiyne to anchor metal oxides with strong d-π interactions, the activity and stability of com-RuO2 for OER were significantly enhanced by mixing with NSGD-800. The zinc-air battery (ZAB) with NSGD shows a much higher peak power density (87.3 mW cm−2) and longer charge-discharge cycle stability compared with the ZAB with Pt/C, making it an excellent candidate air electrode for ZAB and other energy storage and conversion devices.

通过结合密度泛函理论(DFT)计算和氧进化反应(OER)实验,发现硫氮双掺杂石墨二炔(NSGD)是一种很有前景的氧还原反应(ORR)催化剂。DFT 分析表明,氮和硫的掺杂会显著改变吸附特性,进而影响 ORR 活性。同时,由于石墨炔独特的富乙炔结构可以锚定具有强 d-π 相互作用的金属氧化物,与 NSGD-800 混合后,com-RuO2 在 OER 中的活性和稳定性显著提高。与使用 Pt/C 的锌-空气电池(ZAB)相比,使用 NSGD 的锌-空气电池(ZAB)显示出更高的峰值功率密度(87.3 mW cm-2)和更长的充放电循环稳定性,使其成为锌-空气电池及其他能量存储和转换设备的理想候选空气电极。
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引用次数: 0
Advancements in dental hard tissue restorative materials and challenge of clinical translation 牙科硬组织修复材料的进步与临床转化的挑战
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1007/s40843-024-3137-4
Bowen Hu  (, ), Yanyun Pang  (, ), Xiaoxue Yang  (, ), Kun Xuan  (, ), Xu Zhang  (, ), Peng Yang  (, )

Dental hard tissues, primarily enamel and dentin, serving essential functions such as cutting, chewing, speaking, and maintaining facial aesthetics, mainly composed well-aligned hydroxyapatite (HAp) nanocrystals interlaced with a protein matrix. These tissues exhibit remarkable mechanical and aesthetic behaviors. However, once damaged, its ability to self-repair is extremely limited, often accompanied by dentin hypersensitivity (DH). Currently, although dental restorations using synthetic materials and remineralization techniques have made clinical progress, these methods still have limitations that affect their widespread use in clinical applications. Therefore, understanding the formation mechanisms of dental hard tissues and developing high-performance restorative technologies that can mimic natural teeth and meet clinical needs are crucial. This review focuses on the current strategies and research advancements in enamel regeneration and dentin desensitization, and challenges of clinical translation. We emphasize that scientific research should start with clinical needs, and these studies, through translation, ultimately serve the clinic to form a mutually reinforcing virtuous cycle. This review aims to provide a new perspective on the prevention and treatment of dental hard tissues, promote innovation in restorative materials and techniques, and bring better clinical translation products and services to patients.

牙齿硬组织,主要是牙釉质和牙本质,具有切割、咀嚼、说话和保持面部美观等基本功能,主要由排列整齐的羟基磷灰石(HAp)纳米晶体与蛋白质基质交错组成。这些组织具有卓越的机械和美学特性。然而,一旦受损,其自我修复能力就极为有限,并经常伴有牙本质过敏症(DH)。目前,虽然使用合成材料和再矿化技术进行的牙科修复在临床上取得了进展,但这些方法仍然存在局限性,影响了其在临床上的广泛应用。因此,了解牙体硬组织的形成机制,开发能模拟天然牙并满足临床需求的高性能修复技术至关重要。本综述将重点介绍釉质再生和牙本质脱敏的当前策略和研究进展,以及临床转化所面临的挑战。我们强调,科学研究应以临床需求为出发点,这些研究通过转化最终服务于临床,形成相互促进的良性循环。本综述旨在为牙科硬组织的预防和治疗提供新的视角,促进修复材料和技术的创新,为患者带来更好的临床转化产品和服务。
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引用次数: 0
Ultramicroporous carbon molecular sieve membrane derived from hyper-crosslinked ionic polymers for efficient H2/CO2 separation
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-28 DOI: 10.1007/s40843-024-3133-1
Jiaao Yao  (, ), Jingjie Bi  (, ), Hongyu Zuo  (, ), Yuren Peng  (, ), Liwei Wu  (, ), Zixuan Zhang  (, ), Xuelong He  (, ), Baokang Lyu  (, ), Nanwen Li  (, ), Yaozu Liao  (, ), Weiyi Zhang  (, )

Carbon molecular sieve membranes (CMSMs) are a class of porous membranes inherited with excellent thermal stability, high tolerance and superior mechanical strength. Owing to their nanoporous structures, CMSMs usually hold significant potential for gas separation applications. Specifically, hyper-crosslinked ionic polymer (HIP) membranes possess a highly crosslinked nitrogen-rich framework, high thermal stability together with exceptional mechanical strength, making them excellent precursors for the CMSMs fabrication. Upon pyrolysis of HIP membranes, the resulting CMSMs featured with nitrogen functional sites exhibit strong interactions with CO2, which significantly reduces the CO2 permeability while other gas molecules continue to flow through the nanoporous membrane. The resultant CMSMs exhibited excellent H2/CO2 selectivity with values of 10.75 and 7.09, together with ultra-high H2 permeability of 3052 and 9181 barrer, respectively, surpassing the Robeson upper bound. The preparation route towards CMSMs with high nitrogen content from HIP can significantly enrich the rational design and synthesis strategies of high-performance gas separation CMSM materials.

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引用次数: 0
Lattice distortion enhanced self-trapped excitons emission in antimony halide crystalline clusters 晶格畸变增强卤化锑晶体团簇中的自俘获激子发射
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-25 DOI: 10.1007/s40843-024-3128-5
Da Liu  (, ), Jingjing He  (, ), Yuting Sun  (, ), Xinyi Liu  (, ), Yu Peng  (, ), Qing Li  (, ), Hua Gui Yang  (, ), Qiang Niu  (, ), Shuang Yang  (, ), Yu Hou  (, )

Zero-dimensional perovskite materials, characterized by broadband emission caused by self-trapped excitons, are promising materials for stimuli-responsive and photo-writeable encryption. However, existing research is focused on the effects of structural phase transitions on photophysical properties, and lacks in-depth understanding of the mechanisms of self-trapped excitons emission. Here, we demonstrate that the dehydration reaction in zero-dimensional antimony halide clusters significantly enhances the self-trapped excitons emission without inducing structural phase transition, resulting in a substantial increase in photoluminescence (PL) quantum yield from 3.5% to 91.4%. In-situ X-ray diffraction and PL techniques were employed to shed light on the relationship between the crystal structure and radiative recombination, demonstrating the introduction of rich lattice distortion during the dehydration process. Temperature-dependent PL spectra and transient absorption spectra suggest that the lattice distortion causes the moderate electron-phonon coupling strength and high exciton binding energy, facilitating self-trapped excitons to relax from the non-radiative recombination singlet state to the radiative recombination triplet state, corresponding to the enhanced emission intensity. As a proof of concept, several switchable PL applications have been established in scenarios such as anti-counterfeiting, rewritable luminescent paper, and humidity sensing. This finding elucidates the emission mechanism of self-trapped excitons and provides a novel avenue for designing switchable luminescent materials.

零维钙钛矿材料具有自捕获激子引起宽带发射的特点,是一种很有前途的刺激响应和光可写加密材料。然而,现有的研究主要集中在结构相变对光物理性质的影响上,缺乏对自俘获激子发射机制的深入了解。在这里,我们证明了零维卤化锑团簇中的脱水反应在不诱导结构相变的情况下显著增强了自捕获激子的发射,导致光致发光(PL)量子产率从3.5%大幅提高到91.4%。利用原位x射线衍射和PL技术揭示了晶体结构与辐射复合之间的关系,证明了在脱水过程中引入了丰富的晶格畸变。温度相关的PL光谱和瞬态吸收光谱表明,晶格畸变导致电子-声子耦合强度适中,激子结合能较高,有利于自困激子从非辐射复合单重态弛豫到辐射复合三重态,对应于增强的发射强度。作为概念验证,已经在防伪、可重写发光纸和湿度传感等场景中建立了几个可切换的PL应用程序。这一发现阐明了自俘获激子的发射机制,为设计可切换发光材料提供了新的途径。
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引用次数: 0
Memristor-based in-situ convolutional strategy for accurate braille recognition 基于 Memristor 的原位卷积策略,实现准确的盲文识别
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-25 DOI: 10.1007/s40843-024-3122-7
Xianghong Zhang  (, ), Congyao Qin  (, ), Wenhong Peng  (, ), Ningpu Qin  (, ), Enping Cheng  (, ), Jianxin Wu  (, ), Yuyang Fan  (, ), Qian Yang  (, ), Huipeng Chen  (, )

Signal processing has entered the era of big data, and improving processing efficiency becomes crucial. Traditional computing architectures face computational efficiency limitations due to the separation of storage and computation. Array circuits based on multi-conductor devices enable full hardware convolutional neural networks (CNNs), which hold great potential to improve computational efficiency. However, when processing large-scale convolutional computations, there is still a significant amount of device redundancy, resulting in low computational power consumption and high computational costs. Here, we innovatively propose a memristor-based in-situ convolutional strategy, which uses the dynamic changes in the conductive wire, doping area, and polarization area of memristors as the process of convolutional operations, and uses the time required for conductance switching of a single device as the computation result, embodying convolutional computation through the unique spiked digital signal of the memristor. Our strategy reasonably encodes complex analog signals into simple digital signals through a memristor, completing the convolutional computation at the device level, which is essential for complex signal processing and computational efficiency improvement. Based on the implementation of device-level convolutional computing, we have achieved feature recognition and noise filtering for braille signals. We believe that our successful implementation of convolutional computing at the device level will promote the construction of complex CNNs with large-scale convolutional computing capabilities, bringing innovation and development to the field of neuromorphic computing.

信号处理已进入大数据时代,提高处理效率变得至关重要。由于存储和计算分离,传统计算架构面临着计算效率的限制。基于多导器件的阵列电路实现了全硬件卷积神经网络(CNN),在提高计算效率方面具有巨大潜力。然而,在处理大规模卷积计算时,仍存在大量器件冗余,导致计算功耗低、计算成本高。在此,我们创新性地提出了一种基于忆阻器的原位卷积策略,它以忆阻器的导电线、掺杂面积和极化面积的动态变化作为卷积运算过程,以单个器件电导切换所需的时间作为计算结果,通过忆阻器独特的尖峰数字信号体现卷积计算。我们的策略通过忆阻器将复杂的模拟信号合理地编码为简单的数字信号,在器件级完成卷积计算,这对于复杂信号的处理和计算效率的提高至关重要。在实现设备级卷积计算的基础上,我们实现了盲文信号的特征识别和噪声过滤。我们相信,我们在设备级卷积计算的成功实现,将推动具有大规模卷积计算能力的复杂 CNN 的构建,为神经形态计算领域带来创新和发展。
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引用次数: 0
Advancing toward the commercial viability threshold of smart windows utilizing thermochromic polymer blends 利用热致变色聚合物混合物的智能窗户迈向商业可行性门槛
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1007/s40843-024-3160-9
Lin Yao, Yiming Liu, Wei Li
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引用次数: 0
Graph neural network guided design of novel deep-ultraviolet optical materials with high birefringence 图神经网络引导的高双折射新型深紫外光学材料设计
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-22 DOI: 10.1007/s40843-024-3114-4
Ivan A. Kruglov  (, ), Liudmila A. Bereznikova  (, ), Congwei Xie  (, ), Dongdong Chu  (, ), Ke Li  (, ), Evgenii Tikhonov  (, ), Abudukadi Tudi  (, ), Arslan Mazitov  (, ), Min Zhang  (, ), Shilie Pan  (, ), Zhihua Yang  (, )

Finding crystals with high birefringence (Δn), especially in deep-ultraviolet (DUV) regions, is important for developing polarization devices such as optical fiber sensors. Such materials are usually discovered using experimental techniques, which are costly and inefficient for a large-scale screening. Herein, we collected a database of crystal structures and their optical properties and trained atomistic line graph neural network to predict their Δn. To estimate the level of confidence of the trained model on new data, D-optimality criterion was implemented. Using trained graph neural network, we searched for novel materials with high Δn in the Materials Project database and discovered two new DUV birefringent candidates: NaYCO3F2 and SClO2F, with high Δn values of 0.202 and 0.101 at 1064 nm, respectively. Further analysis reveals that strongly anisotropic units with various anions and π-conjugated planar groups are beneficial for high Δn.

寻找具有高双折射(Δn)的晶体,尤其是在深紫外(DUV)区域,对于开发光纤传感器等偏振设备非常重要。这类材料通常是通过实验技术发现的,而实验技术对于大规模筛选来说成本高、效率低。在此,我们收集了晶体结构及其光学特性数据库,并训练原子线图神经网络来预测它们的Δn。为了估算训练模型对新数据的置信度,我们采用了 D-optimality 准则。利用训练有素的图神经网络,我们在材料项目数据库中搜索了具有高Δn 的新型材料,并发现了两种新的 DUV 双折射候选材料:NaYCO3F2 和 SClO2F,在 1064 纳米波长处的Δn 值分别高达 0.202 和 0.101。进一步的分析表明,带有各种阴离子和 π 共轭平面基团的强各向异性单元有利于获得高 Δn。
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引用次数: 0
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Science China Materials
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