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On-Chip Construction of Hierarchically Macro-/Mesoporous Cerium Oxide/Pt Gas Sensitive Film for Ultrasensitive Detection of Trace Oxygen 级联宏/介孔氧化铈/铂气敏膜超灵敏检测痕量氧的片上构建
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1002/idm2.12254
Yu Deng, Keyu Chen, Wenhe Xie, Xin-Yu Huang, Fengluan Jiang, Lingxiao Xue, Ziling Zhang, Qin Yue, Limin Wu, Wei Luo, Yonghui Deng

Hierarchically porous structure is extremely favorable for many applications, including heterogeneous catalysis, chemical sensing, and energy conversion and storage. In these applications, controllable synthesis and assembly of transition metal oxide materials with tailored hierarchically porous structure and chemical microenvironments are highly desired but challenging. Herein, uniform mesoporous cerium oxide (mCeO2) microspheres functionalized with Pt nanoparticles (NPs) were designed via efficient nanoemulsion approach and used to construct hierarchical macro-/mesoporous CeO2/Pt film on micro-electromechanical system (MEMS) chips. The resultant functional chip-based devices have controllable porous structure and rich highly accessible active Pt–CeO2 interfaces, and thus they exhibit outstanding performance as oxygen sensors with an unprecedented low limit of detection (LOD, 7.16 ppm), high sensitivity at a relatively low working temperature (250°C). Finite element analysis, density functional theory calculations, and in situ characterizations reveal that, such an excellent performance is mainly due to the favorable mass transfer and gas–solid interface interaction, the oxygen spillover effect enabled by the nanosized Pt, and the enhanced catalytic reaction causing the dramatic change of electronic resistance of the sensing layer in oxygen atmosphere. Finally, a smart gas sensing module capable of real-time precise detection of oxygen was fabricated, demonstrating the possibility for commercial application.

分层多孔结构在多相催化、化学传感、能量转换和存储等领域具有广泛的应用前景。在这些应用中,具有定制层次多孔结构和化学微环境的过渡金属氧化物材料的可控合成和组装是非常需要的,但也是具有挑战性的。本文采用高效纳米乳液的方法,设计了均匀介孔氧化铈(mCeO2)微球,并将其功能化Pt纳米粒子(NPs),用于在微机电系统(MEMS)芯片上构建宏观/介孔CeO2/Pt薄膜。由此产生的基于功能芯片的器件具有可控的多孔结构和丰富的高可达活性Pt-CeO2界面,因此它们在相对较低的工作温度(250°C)下具有前所未有的低检测限(LOD, 7.16 ppm)和高灵敏度,表现出出色的氧传感器性能。有限元分析、密度泛函理论计算和原位表征表明,这种优异的性能主要是由于良好的传质和气固界面相互作用、纳米Pt的氧溢出效应以及催化反应的增强导致传感层在氧气环境中的电子电阻发生了巨大变化。最后,制作了一个能够实时精确检测氧气的智能气体传感模块,展示了商业应用的可能性。
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引用次数: 0
Efficient Inverted Perovskite Solar Cells Enabled by Sequential Passivation Using Two-Dimensional Perovskites 利用二维钙钛矿序贯钝化实现高效倒置钙钛矿太阳能电池
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1002/idm2.12256
Bingcan Ke, Jing Li, Zewei Zhu, Siqi Zhang, Ruixuan Jiang, Chengkai Jin, Chang Hu, Qi Zhang, Jie Su, Sai Bai, Fuzhi Huang, Yi-Bing Cheng, Tongle Bu

Refining the process in which two-dimensional (2D) perovskites passivate three-dimensional (3D) perovskites is vital for improving the performance of perovskite solar cells (PSCs), yet is frequently overlooked. Herein, a novel sequential passivation process that initially employs phenethylamine iodide (PEAI) on the 3D perovskite surface, followed by treatment with 4-trifluoromethylphenylethylamine iodide (CF3PEAI) is presented. A comprehensive comparison of the intrinsic molecular structures and their impact on the perovskites reveals that the small-sized, low-polarized PEA molecule induces minimal lattice strain and a negative shift of the vacuum energy level of perovskite surface, whereas the large-sized, high-polarized CF3PEA molecule leads to larger lattice strain and a positive shift of the vacuum energy level. By leveraging the opposing properties of these molecules through our tailored sequential passivation strategy, optimal passivation effects and efficient interface charge transfer are obtained, outperforming the posttreatment with mixed ligands and greatly surpassing posttreatment with a single ligand. Consequently, a champion efficiency of 26.27% is achieved for the inverted PSCs, along with outstanding operational stability featuring a T80 lifetime exceeding 1000 h under continuous light illumination at the maximum power point tracking.

改进二维(2D)钙钛矿钝化三维(3D)钙钛矿的工艺对于提高钙钛矿太阳能电池(PSCs)的性能至关重要,但经常被忽视。本文提出了一种新的顺序钝化工艺,首先在三维钙钛矿表面使用苯乙胺碘化(PEAI),然后用4-三氟甲基苯乙胺碘化(CF3PEAI)处理。综合比较了其固有分子结构及其对钙钛矿的影响,发现小尺寸、低极化的PEA分子导致钙钛矿表面晶格应变最小,真空能级负移,而大尺寸、高极化的CF3PEA分子导致较大的晶格应变和真空能级正移。通过我们量身定制的顺序钝化策略,利用这些分子的相反性质,获得了最佳的钝化效果和高效的界面电荷转移,优于混合配体后处理,大大超过了单一配体后处理。因此,倒置PSCs实现了26.27%的冠军效率,以及出色的运行稳定性,在最大功率点跟踪的连续光照下,T80寿命超过1000小时。
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引用次数: 0
Manipulating Anti-Site Defects in α-MgAgSb for Thermoelectric Cooling Enhancement 控制α-MgAgSb的反位缺陷用于热电冷却增强
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1002/idm2.12252
Juan Li, Guijuan Li, Qiyong Chen, Jianghe Feng, Tao Feng, Lili Xi, Weishu Liu, Wenqing Zhang, Ruiheng Liu, Rong Sun

α-MgAgSb is one of the few high-performance thermoelectric materials near room temperature, thanks to its inherently suppressed lattice thermal conductivity. However, conventional approaches to optimizing electrical properties often inadvertently degrade carrier mobility, adversely impacting thermoelectric performance at lower temperatures. In this study, we discovered in an experiment that Mg-Ag anti-site defects exist in the lattice and create staggered nanoscale anti-site zones in the matrix. This unique structure significantly scatters phonons while having a negligible influence on carrier transport due to the preservation of carrier transport channels. By fine-tuning the formation energy of Mg-Ag anti-sites through Zn doping, both carrier transport and phonon scattering were successfully bolstered. Consequently, a high figure of merit (zT) of ~0.45 at 200 K and an average zT of ~0.75 within the low-temperature range of 200–400 K can be achieved. Furthermore, a single-pair device constructed using the obtained α-MgAgSb and commercial Bi2Te3 legs exhibited a temperature difference of ~56 K at 325 K, showcasing promise for thermoelectric cooling applications. This demonstration underscores the efficiency of anti-site manipulation as a means to enhance the thermoelectric cooling performance of α-MgAgSb.

α-MgAgSb由于其固有的抑制晶格热导率,是为数不多的室温附近的高性能热电材料之一。然而,传统的优化电学性能的方法往往会无意中降低载流子的迁移率,对低温下的热电性能产生不利影响。在本研究中,我们在实验中发现Mg-Ag反位缺陷存在于晶格中,并在基体中形成交错的纳米级反位区。这种独特的结构显著散射声子,但由于保留了载流子输运通道,对载流子输运的影响可以忽略不计。通过Zn掺杂微调Mg-Ag反位的形成能,成功地增强了载流子输运和声子散射。因此,在200 K时可以获得~0.45的高品质系数(zT),在200 - 400 K的低温范围内可以获得~0.75的平均zT。此外,使用α-MgAgSb和商用Bi2Te3支腿构建的单对器件在325 K时的温差为~56 K,显示了热电冷却应用的前景。这一演示强调了反位操作作为提高α-MgAgSb热电冷却性能的一种手段的效率。
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引用次数: 0
Creating Biomimetic Bouligand Architectures for Biomedical and Healthcare Applications 为生物医学和医疗保健应用创建仿生Bouligand建筑
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1002/idm2.12260
Hongye Yang, Xinyu Zhang, Shilei Wang, Yize Wang, Rui Xiong, Cui Huang

The hierarchical Bouligand structure, ubiquitous in organisms and endowing natural creatures with exceptional performance attributes, stands as a prime example of nature's evolutionary prowess. Following the example of nature, the construction of biomimetic Bouligand structures will significantly propel advancements and innovations within the domain of biomedical and healthcare applications. In this review, we summarize cutting-edge research progress of biomimetic Bouligand architectures. Firstly, the natural Bouligand structures in animals, plants, and humans are introduced. On this basis, the relationship between properties and Bouligand structure is briefly discussed, including toughening mechanism, optical characteristics, and biological properties. Subsequently, the review details the construction strategies of the biomimetic Bouligand architectures, covering a variety of methods such as self-assembly, biomimetic mineralization, shear brushing, electrostatic spinning, and 3D printing. Finally, the utilization of biomimetic Bouligand architectures in biomedical and healthcare fields, especially for bone regeneration, tooth repair, body protection, and biosensor transmission, is discussed in detail. Despite the significant theoretical advantages of Bouligand structure, its feasibility in biomedical and healthcare applications still remains in its infancy. We eagerly anticipate the future development of biomimetic Bouligand architectures with superior performance, tailored to clinical scenarios and health needs, thereby fulfilling the grand vision of “inspiration from nature and giving back to life.”

分层的布利甘结构在生物体中无处不在,赋予自然生物非凡的性能属性,是大自然进化能力的一个主要例子。以自然为例,仿生Bouligand结构的建设将极大地推动生物医学和医疗保健应用领域的进步和创新。本文综述了仿生Bouligand建筑的最新研究进展。首先,介绍了动物、植物和人类的天然布利根结构。在此基础上,简要讨论了性能与Bouligand结构之间的关系,包括增韧机理、光学特性和生物学特性。随后,综述了仿生Bouligand建筑的构建策略,包括自组装、仿生矿化、剪切刷、静电纺丝和3D打印等多种方法。最后,详细讨论了仿生Bouligand结构在生物医学和医疗保健领域的应用,特别是在骨再生、牙齿修复、身体保护和生物传感器传输方面的应用。尽管Bouligand结构具有显著的理论优势,但其在生物医学和医疗保健方面的可行性仍处于起步阶段。我们热切期待未来仿生Bouligand建筑的发展,以卓越的性能,为临床场景和健康需求量身定制,从而实现“灵感来自自然,回馈生活”的宏伟愿景。
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引用次数: 0
Ultrathin Nanocomposite Membrane With Robust Anti-Wettability for Stable Membrane Distillation 用于稳定膜蒸馏的超强抗润湿性超薄纳米复合膜
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1002/idm2.12253
Zhongao Chen, Yongxuan Wang, Xiao Chen, Cheng Huang, Shiqing Xu, Quanwei Xu, Shuaifei Zhao, Wojciech Kujawski, Pengchao Zhang

Hydrophobic porous membrane is the key to the desalination performance of membrane distillation (MD). However, traditional MD membranes suffer from poor hydrophobicity of pore surfaces, leading to pore wetting and causing the loss of desalination stability. In this study, we present an ultrathin polyvinylidene fluoride (PVDF) nanocomposite membrane with robust anti-wetting properties and high permeability for stable MD desalination. The improved anti-wetting properties are achieved by enhancing the hydrophobicity of membrane pore surfaces via introducing hydrophobic silica nanoparticles to build nanostructures on the pore surfaces. The hydrophobic nanostructured pore surfaces induce the formation of the nano-Cassie state upon contact with water, thereby enhancing the specific liquid entry pressure of water (LEPw) with 788% compared to commercial PVDF membranes. The resulted porous structure and 10 μm membrane thickness (i.e., 20 times thinner than commercial PVDF membranes) enable the stable desalination flux of 20.30 kg m−2 h−1 and high salt rejection of > 99.9% with 60°C seawater. Our ultrathin nanocomposite membranes provide a promising solution for long-term MD seawater desalination.

疏水多孔膜是膜蒸馏脱盐性能的关键。然而,传统的MD膜由于孔表面疏水性差,导致孔湿润,失去脱盐稳定性。在这项研究中,我们提出了一种超薄聚偏氟乙烯(PVDF)纳米复合膜,具有强大的抗湿性能和高渗透性,用于稳定的MD脱盐。通过在膜孔表面引入疏水性二氧化硅纳米粒子构建纳米结构来增强膜孔表面的疏水性,从而提高了膜的抗湿性能。疏水纳米结构孔表面与水接触后诱导纳米cassie态的形成,从而使水的比入液压力(LEPw)比商用PVDF膜提高了788%。所得到的多孔结构和10 μm的膜厚度(即比商用PVDF膜薄20倍)使得在60°C海水中脱盐通量稳定为20.30 kg m−2 h−1,盐去除率高达99.9%。我们的超薄纳米复合膜为长期MD海水淡化提供了很有前景的解决方案。
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引用次数: 0
Synergistic Chemical and Physical Encapsulation Strategies Enable Highly Stable and Lead Leakage-Suppressed Perovskite Solar Cells 协同化学和物理封装策略使高稳定和铅泄漏抑制钙钛矿太阳能电池
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-02 DOI: 10.1002/idm2.12255
Yumeng Xu, Qingrui Wang, Zhenhua Lin, Siyu Zhang, Xing Guo, Zhaosheng Hu, Juanxiu Xiao, Yue Hao, Liming Ding, Jingjing Chang

Although outstanding power conversion efficiency has been achieved in perovskite solar cells (PSCs), poor stability and lead (Pb) toxicity are still the key challenges limiting the commercial application of PSCs. Herein, we adopted both chemical encapsulation and physical encapsulation to address these problems. Via strong chemical interaction between dibutyl phthalate (DBP) and perovskite, the chemical encapsulation strategy results in higher perovskite film quality with reduced trap density, and the device efficiency enhances from 22.07% to 24.36%. Physical encapsulation polymer with high film robustness and self-healing properties could effectively isolate external risks and restore protection after physical damage. Furthermore, both chemical and physical encapsulation materials could trap Pb ions leaking from the perovskite materials by forming coordination interactions. We simulated realistic scenarios in which PSCs encapsulated by different methods suffered water immersion and mechanical damage, and quantitatively measured Pb leakage rates under different conditions. Higher device stability and greater Pb leakage reduction were achieved, confirming the excellent encapsulation effect of the synergy of chemical and physical encapsulation. This study provides an effective strategy to realize safe and environmentally friendly PSCs to promote their commercialization.

尽管钙钛矿太阳能电池(PSCs)已经取得了优异的功率转换效率,但稳定性差和铅(Pb)毒性仍然是限制其商业应用的主要挑战。为了解决这些问题,我们采用了化学封装和物理封装两种方法。通过邻苯二甲酸二丁酯(DBP)与钙钛矿之间的强化学相互作用,化学包封策略使钙钛矿膜质量提高,陷阱密度降低,器件效率从22.07%提高到24.36%。物理封装聚合物具有较高的膜坚固性和自愈性,可以有效隔离外部风险,在物理损伤后恢复保护。此外,化学和物理封装材料都可以通过形成配位作用来捕获从钙钛矿材料中泄漏的Pb离子。模拟不同封装方法下pccs的浸水和机械损伤情况,定量测量不同条件下的Pb泄漏率。器件稳定性更高,Pb泄漏减少幅度更大,证实了化学和物理封装协同作用的优异封装效果。本研究为实现安全环保的psc提供了有效的策略,以促进其商业化。
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引用次数: 0
Inside Front Cover: Volume 4 Issue 3 内封面:第4卷第3期
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-05-26 DOI: 10.1002/idm2.12257

Inside Front Cover: The review of doi:10.1002/idm2.12245 provides a comprehensive summary and discussion of the emerging research frontier Engineered Living Energy Materials (ELEMs). These materials represent a novel paradigm that integrates biological and artificial systems to enable sustainable energy conversion. By identifying key technical hurdles, this review provides a roadmap for future directions.

内页封面:回顾doi:10.1002/idm2.12245提供了一个全面的总结和新兴研究前沿工程生活能源材料(ELEMs)的讨论。这些材料代表了一种新的范例,它整合了生物和人工系统,以实现可持续的能源转换。通过确定关键的技术障碍,本综述为未来的发展方向提供了路线图。
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引用次数: 0
Outside Front Cover: Volume 4 Issue 3 外封面:第4卷第3期
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-05-26 DOI: 10.1002/idm2.12187

Outside Front Cover: The article of doi:10.1002/idm2.12249 explores how machine learning–driven activity prediction, energy barrier optimization, and data-guided materials design accelerate the discovery of a new generation of electrocatalysts, and discusses their applications in water electrolysis, fuel cells, and carbon dioxide reduction, thereby advancing innovation in sustainable energy solutions.

外封面:文章doi:10.1002/idm2.12249探讨了机器学习驱动的活动预测,能量障碍优化和数据指导材料设计如何加速新一代电催化剂的发现,并讨论了它们在水电解,燃料电池和二氧化碳减排中的应用,从而推进可持续能源解决方案的创新。
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引用次数: 0
Inside Back Cover: Volume 4 Issue 3 封底内:第4卷第3期
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-05-26 DOI: 10.1002/idm2.12258

Inside Back Cover: This image of doi:10.1002/idm2.12250 vividly illustrates the role of Mg-based materials in the field of gas separation and purification. In the figure, NeZha, a hero in Chinese traditional myth representing magnesium, is combating exhaust gas from factories including CO2, SO2 and NOx, etc., which is represented by a dark dragon. The weapons are designed according to the molecular structure of Mg-based materials such as MgH2, Mg-MOF-74, MgO and Mg(OH)2, which are discussed in the article. The figure encapsulates the article's core focus on utilizing Mg-based compounds to develop cost-effective and efficient gas separation technologies for environment protection and clean energy.

内页封底:这张doi:10.1002/idm2.12250的图片生动地说明了镁基材料在气体分离和净化领域的作用。在图中,代表镁的中国传统神话中的英雄哪吒正在与工厂排放的二氧化碳、二氧化硫、氮氧化物等气体作斗争,这些气体由一条黑龙代表。根据MgH2、Mg- mof -74、MgO和Mg(OH)2等镁基材料的分子结构进行了武器设计,并对其进行了讨论。这个数字概括了文章的核心重点,即利用镁基化合物开发具有成本效益和高效的气体分离技术,以保护环境和清洁能源。
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引用次数: 0
Outside Back Cover: Volume 4 Issue 3 封底外:第4卷第3期
IF 24.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-05-26 DOI: 10.1002/idm2.12259

Outside Back Cover: The cover image of doi:10.1002/idm2.12243 illustrates the diverse applications of fiber-shaped supercapacitors (FSCs), including their integration into wearable power fabrics for modular energy storage, coupling with specific devices, forming composite fibers, and combining with energy-harvesting fibers to develop integrated fabrics with both energy-harvesting and energy-storage functions.

封底外:doi:10.1002/idm2.12243的封面图像说明了纤维形超级电容器(FSCs)的各种应用,包括将其集成到可穿戴动力织物中用于模块化储能,与特定设备耦合,形成复合纤维,并与能量收集纤维结合开发具有能量收集和能量存储功能的集成织物。
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引用次数: 0
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Interdisciplinary Materials
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