Advanced Powder Materials最新文献_第6页

High-loading inducing Fe-dimer on carbon nitride promotes the generation of ·O2− 氮化碳上高负荷诱导铁二聚体促进了·O2−的生成

Advanced Powder Materials

Pub Date : 2025-06-18 DOI: 10.1016/j.apmate.2025.100308

Xinran Zheng , Yuchao Wang , Jianping Guan , Xu Liu , Yu Bai , Yingbi Chen , Peiyao Yang , Jing Zhang , Houzheng Ou , Meng Wang , Yu Xiong , Haozhi Wang , Yongpeng Lei

The research on metal dimer clusters is of great importance, owing to the potential in modulating the adsorption behavior towards reaction intermediates. Here, we develop a loading heightening strategy to obtain a 32.5 wt% Fe-dimer catalyst (Fe-32.5). The co-anchoring of two Fe atoms in a single triazine ring of carbon nitride with an atomic spacing of ∼0.23 nm is proved. Fe atoms occupy the pores of the triazine ring in the lower iron content sample (Fe-12.9 and Fe-17.1). However, with the increase of iron content to 32.5 wt%, two Fe atoms simultaneously occupy one triazine ring. For Fe-32.5, besides the main peak located at ∼1.5 Å corresponding to the Fe–N interaction, a peak attributed to Fe–Fe bonding is observed at ∼2.2 Å in Fourier-transformed k³-weithted extended X-ray absorption fine structure. Density functional theoretical calculations reveal that Fe-dimer in Fe-32.5 induces a charge redistribution compared with that in Fe-12.9 and Fe-17.1. H₂O∗ is adsorbed on O∗ via hydrogen bonding in Fe-12.9 and Fe-17.1. However, H₂O∗and O∗ in Fe-32.5 are adsorbed on Fe–Fe dimer, resulting in a decrease in the total energy of the reaction process. For the two former, O₂⁻∗ adsorbs on individual Fe atoms. Fe-dimer in Fe-32.5 adsorbs O₂⁻∗ in the form of bridge bonds, which facilitates the ·O₂⁻ release. Furthermore, an enhanced affinity for the substrate 3,3′,5,5′-tetramethylbenzidine and higher peroxidase-like activity were displayed. This work provides an effective mean to synthesize metal dimer clusters through high loading.

金属二聚体簇具有调节反应中间体吸附行为的潜力，其研究具有重要意义。在这里，我们开发了一种负载增强策略，以获得32.5 wt%的铁二聚体催化剂（Fe-32.5）。证明了两个铁原子在原子间距为0.23 nm的氮化碳单三嗪环上共锚定。在铁含量较低的样品（Fe-12.9和Fe-17.1）中，铁原子占据了三嗪环的孔。然而，当铁含量增加到32.5 wt%时，两个铁原子同时占据一个三嗪环。对于Fe-32.5，除了位于~ 1.5 Å对应于Fe-N相互作用的主峰外，在傅里叶变换k3-加权扩展x射线吸收精细结构中，在~ 2.2 Å观察到一个归因于Fe-Fe键合的峰。密度泛函理论计算表明，与Fe-12.9和Fe-17.1相比，Fe-32.5中的fe -二聚体引起了电荷重分布。H2O *在Fe-12.9和Fe-17.1中通过氢键吸附在O *上。然而，Fe-32.5中的H2O∗和O∗被Fe-Fe二聚体吸附，导致反应过程的总能量降低。对于前两种，O2−*吸附在单个铁原子上。Fe-32.5中的铁二聚体以桥键的形式吸附O2−*，促进了·O2−的释放。此外，对底物3,3 ',5,5 ' -四甲基联苯胺的亲和力增强，并显示出更高的过氧化物酶样活性。本研究为高负载合成金属二聚体簇提供了有效手段。

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引用次数: 0

Tailored fluoroborate-based electrolyte with fast interphase formation kinetics toward stable Ah-level zinc batteries 具有快速相形成动力学的定制氟硼酸盐基电解质用于稳定的ah级锌电池

Advanced Powder Materials

Pub Date : 2025-06-16 DOI: 10.1016/j.apmate.2025.100306

Jiangtao Huang , Yunpeng Zhong , Najla AlMasoud , Taghrid S. Alomar , Yiman Xie , Bingan Lu , Shuquan Liang , Zeinhom M. El-Bahy , Siyu Tian , Jiang Zhou

Solid electrolyte interphase (SEI) plays a critical role in stabilizing zinc batteries, yet insufficient attention has been given to its in-situ growth kinetics and the post-stripping morphology of zinc anodes, both affecting the SEI-forming quality. Herein, we showcase a synergistic effect between uniform Zn stripping and rapid SEI formation through introducing tetramethylurea (TMU) into Zn(BF₄)₂-based electrolytes. TMU participates in the Zn²⁺ solvation structure and reshapes the electrolyte hydrogen-bond network, enabling a water-poor electric double layer that mitigates the corrosion-induced stripping inhomogeneity. Subsequently, a multi-component and inorganic-rich SEI with high uniformity is rapidly deposited during the plating process. This SEI with abundant zincophilic sites activates instantaneous nucleation and hence guides dense and uniform Zn deposition. With enhanced Zn stripping/plating symmetry, the long-term effectiveness of SEI is guaranteed, contributing to the high reversibility over 3200 h at 1 mA cm⁻²/2 mAh cm⁻². Impressively, the Zn//NaV₃O₈ full cell (4.43 mAh cm⁻²) can be steadily cycled at 0.1 A g⁻¹ under an intermittent-rest protocol. The stable operation of an Ah-level pouch cell over 100 cycles further demonstrates the scalability of this strategy and highlights the significance of achieving high stripping/plating symmetry and a long-term effective SEI toward practical zinc batteries.

固体电解质界面相（SEI）在稳定锌电池中起着至关重要的作用，但其原位生长动力学和锌阳极剥离后的形貌影响SEI形成质量的研究一直不够重视。在此，我们通过将四甲基脲（TMU）引入Zn(BF4)2基电解质中，展示了均匀锌剥离和快速SEI形成之间的协同效应。TMU参与了Zn2+的溶剂化结构，重塑了电解质的氢键网络，形成了一个缺水的双电层，减轻了腐蚀引起的剥离不均匀性。随后，在电镀过程中快速沉积出一种多组分、高均匀性、富无机的SEI。这种具有丰富亲锌位点的SEI激活瞬时成核，从而引导致密均匀的锌沉积。由于锌剥离/电镀对称性增强，保证了SEI的长期有效性，有助于在1ma cm−2/ 2mah cm−2下超过3200小时的高可逆性。令人印象深刻的是，在间歇休息协议下，Zn//NaV3O8电池（4.43 mAh cm−2）可以在0.1 A g−1下稳定循环。ah级袋状电池超过100次循环的稳定运行进一步证明了该策略的可扩展性，并强调了实现高剥离/镀对称性和长期有效的SEI对实用锌电池的重要性。

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引用次数: 0

Rare earth-rich sublayer tuned Pd-skin for methanol and CO tolerance oxygen reduction and hydrogen oxidation reaction 富稀土亚层调谐Pd-skin用于甲醇和CO耐受氧还原和氢氧化反应

Advanced Powder Materials

Pub Date : 2025-06-14 DOI: 10.1016/j.apmate.2025.100305

Felix Kwofie , Jinfan Chen , Yujing Liu , Ying Zhang , Junsong Zhang , Yang Yang , Quentin Meyer , Chuan Zhao , Zhenjiang He , Yunjiao Li , Yi Cheng

Storing hydrogen in green methanol is a well-known and cost-effective way for long-term energy storage. However, using green methanol in fuel cell technologies requires electrocatalysts with superior resistance to poisoning induced by intermediate species. This study introduces a new class of palladium-based rare earth (RE) alloys with exceptional resistance to methanol for the oxygen reduction reaction (ORR) and outstanding resistance to carbon monoxide poisoning for the hydrogen oxidation reaction (HOR). The PdEr catalyst achieved unparalleled ORR activity amongst the Pd-based rare earth alloys and demonstrated remarkable resistance to methanol poisoning, which is two orders of magnitude higher than commercial Pt/C catalysts. Furthermore, the PdEr catalyst shows high hydrogen oxidation activity under 100 ppm CO. Comprehensive analysis demonstrates that the RE element-enriched sublayer tuning of the Pd-skin's surface strain is responsible for the enhanced ORR and HOR capabilities. This modification allows for precise control over the adsorption strength of critical intermediates while concurrently diminishing the adsorption energy of methanol and CO on the PdEr surface.

在绿色甲醇中储存氢是一种众所周知且经济有效的长期储能方法。然而，在燃料电池技术中使用绿色甲醇需要具有优异的抗中间物质中毒能力的电催化剂。本研究介绍了一类新的钯基稀土（RE）合金，该合金在氧还原反应（ORR）中具有优异的抗甲醇性能，在氢氧化反应（HOR）中具有优异的抗一氧化碳中毒性能。PdEr催化剂在钯基稀土合金中具有无与伦比的ORR活性，并表现出显著的抗甲醇中毒能力，比商用Pt/C催化剂高出两个数量级。此外，PdEr催化剂在100 ppm CO下表现出较高的氢氧化活性。综合分析表明，Pd-skin表面应变的富RE亚层调整是ORR和HOR能力增强的原因。这种修饰可以精确控制关键中间体的吸附强度，同时降低甲醇和CO在PdEr表面的吸附能。

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引用次数: 0

Ultrafast piezocatalytic organic pollutant degradation enabled by dynamic spin state regulation of cobalt in nano-ferroelectrics 纳米铁电体中钴的动态自旋态调控使超快压电催化有机污染物降解成为可能

Advanced Powder Materials

Pub Date : 2025-06-14 DOI: 10.1016/j.apmate.2025.100307

Yu Mo , Jiyue Wu , Wei Liu , Yizheng Bao , Zimeng Hu , Nan Meng , Haitao Huang , Genshui Wang

Ferroelectric materials are gaining increasing attention for the development of advanced catalytic technologies due to their field-responsive polarization states. However, achieving dynamic optimization of catalytic activity using ferroelectrics remains a fundamental challenge. Inspired by the force-adaptive mechanisms of fish scales, we introduce an intracrystalline force regulation strategy to dynamically control cobalt spin states and enhance peroxymonosulfate (PMS) activation in Fenton-like processes. This approach utilizes BaTi_0.92Co_0.08O_3-δ (BTC-8) nano-ferroelectrics, where ultrasound irradiation generates a built-in electric field that drives electrons towards cobalt sites. This electron transfer is further facilitated by electronegativity differences between cobalt and barium/titanium ions. The resulting piezo-driven electron flow promotes continuous regeneration of high-spin Co²⁺, enhancing PMS adsorption and SO₄-OH bond cleavage, leading to increased production of ·SO₄⁻ and singlet oxygen (¹O₂) for organic pollutant degradation. Consequently, BTC-8 achieves a reaction rate (k=1.7960 min⁻¹) 28.93 times higher than that of pure barium titanate, surpassing previously reported PMS activation and piezocatalytic systems. This work represents a shift from static electronic structure design to dynamic electronic engineering in the development of advanced catalytic strategies for water remediation.

铁电材料由于具有场响应极化态，在先进催化技术的发展中受到越来越多的关注。然而，利用铁电体实现催化活性的动态优化仍然是一个根本性的挑战。受鱼鳞的力适应机制的启发，我们引入了一种晶体内力调节策略来动态控制钴的自旋状态，并增强芬顿样过程中过氧单硫酸盐（PMS）的激活。该方法利用bati0.92 co0.080 o3 -δ (BTC-8)纳米铁电体，其中超声照射产生内置电场，将电子驱动到钴位点。钴和钡/钛离子之间的电负性差异进一步促进了这种电子转移。由此产生的压电驱动电子流促进了高自旋Co2+的连续再生，增强了PMS吸附和SO4- oh键的裂解，从而增加了用于有机污染物降解的·SO4−和单线态氧（1O2）的产量。因此，BTC-8的反应速率（k=1.7960 min−1）比纯钛酸钡高28.93倍，超过了先前报道的PMS活化和压电催化体系。这项工作代表了从静态电子结构设计到动态电子工程在发展先进的水修复催化策略的转变。

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引用次数: 0

Advancements in flexible Perovskite solar cells and their integration into self-powered wearable optoelectronic systems 柔性钙钛矿太阳能电池及其与自供电可穿戴光电系统集成的进展

Advanced Powder Materials

Pub Date : 2025-05-27 DOI: 10.1016/j.apmate.2025.100304

Ghazanfar Nazir , Adeela Rehman , Jagadis Gautam , Muhammad Ikram , Sajjad Hussain , Sikandar Aftab , Kwang Heo , Seul-Yi Lee , Soo-Jin Park

Driven by rapid advancements in smart wearable technologies and perovskite photovoltaics, flexible perovskite solar cells (FPSCs) have emerged as highly promising autonomous power sources, poised to transform the next generation of mobile energy systems, portable electronics, and integrated wearable devices. For successful deployment in real-world scenarios, FPSCs must exhibit a combination of key attributes, including high power conversion efficiency, lightweight architecture, environmental robustness, and mechanical adaptability—encompassing flexibility, stretchability, and twistability. This review provides a detailed examination of the evolution, current state, and practical deployment of FPSCs, emphasizing their potential as efficient, portable energy solutions. It investigates advanced strategies for improving environmental resilience and mechanical recoverability, including the engineering of flexible substrates, deposition of high-quality perovskite films, and optimization of charge-selective interfaces. Additionally, it offers a systematic analysis of device design, fabrication protocols, scalable printing techniques, and standardized performance evaluation methods tailored for wearable FPSCs. Recent progress in enhancing the optoelectronic properties and mechanical durability of FPSCs is also critically reviewed. Ultimately, this work delivers a comprehensive perspective on FPSCs from both optoelectronic and mechanical viewpoints, identifies key challenges, and outlines future research pathways toward the seamless integration of FPSCs into multifunctional, next-generation wearable systems.

在智能可穿戴技术和钙钛矿光伏技术快速发展的推动下，柔性钙钛矿太阳能电池（FPSCs）已经成为非常有前途的自主电源，有望改变下一代移动能源系统、便携式电子设备和集成可穿戴设备。为了在实际场景中成功部署，fpsc必须具备一系列关键属性，包括高功率转换效率、轻量级架构、环境稳健性和机械适应性，包括灵活性、可拉伸性和可扭转性。这篇综述详细介绍了fpsc的发展、现状和实际部署，强调了它们作为高效便携式能源解决方案的潜力。它研究了提高环境弹性和机械可恢复性的先进策略，包括柔性衬底的工程设计、高质量钙钛矿薄膜的沉积和电荷选择界面的优化。此外，它还为可穿戴式fpsc提供了设备设计、制造协议、可扩展打印技术和标准化性能评估方法的系统分析。本文还评述了近年来在提高FPSCs光电性能和机械耐久性方面的研究进展。最后，这项工作从光电和机械的角度提供了FPSCs的全面视角，确定了关键挑战，并概述了将FPSCs无缝集成到多功能下一代可穿戴系统中的未来研究路径。

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引用次数: 0

Electronic structure regulation inducing robust solid electrolyte interphase for stable anode-free sodium metal batteries 稳定无阳极钠金属电池中诱导坚固固体电解质界面的电子结构调控

Advanced Powder Materials

Pub Date : 2025-05-19 DOI: 10.1016/j.apmate.2025.100303

Peng Xu , Yinghan Liu , Mulan Qin , Fei Huang , Shuquan Liang , Guozhao Fang

Anode-free sodium metal batteries (AFSMBs) have gained attention as next-generation storage systems with high energy density and cost-effectiveness. However, non-uniform sodium (Na) deposition and an unsteady solid electrolyte interphase (SEI) lead to dendrite-related issues and severe irreversible Na⁺ plating/stripping, greatly aggravating their cycle deterioration. In this study, we effectively modified the 3D current collector's electronic structure by introducing Zn-N_x active sites (Zn-CNF), which enhances lateral Na⁺ diffusion and the Na planar growth, enabling uniform deep Na deposition at an exceptionally high capacity of 10 mA h cm⁻². Furthermore, the Zn-N_x bonds enhance the adsorption capacity of PF₆⁻ and contribute to forming a stable inorganic-rich SEI layer. Consequently, Zn-CNF with the electronic structure regulation endows an ultra-low nucleation overpotential (8 mV) and ultra-high Coulombic efficiency of 99.94% over 1,600 cycles. Symmetric cells demonstrate stable Na⁺ plating/stripping behavior for more than 4,400 h at 1 mA cm⁻². Moreover, under high cathode loading (7.97 mg cm⁻²), the AFSMBs achieve a high energy density of 374 W h kg⁻¹ and retain a high discharge capacity of 82.49 mA h g⁻¹ with a capacity retention of 80.4% after 120 cycles. This work proposes a viable strategy to achieving high-energy-density AFSMBs.

无阳极金属钠电池（AFSMBs）作为具有高能量密度和高性价比的新一代储能系统受到了广泛关注。然而，不均匀的钠（Na）沉积和不稳定的固体电解质界面（SEI）导致了与枝晶相关的问题和严重的不可逆的Na+镀/剥离，大大加剧了它们的循环退化。在这项研究中，我们通过引入Zn-Nx活性位点（Zn-CNF）有效地修饰了3D集流器的电子结构，从而增强了Na+的横向扩散和Na的平面生长，从而在10 mA h cm−2的超高容量下实现了均匀的深Na沉积。此外，Zn-Nx键增强了PF6 -的吸附能力，有助于形成稳定的富无机SEI层。因此，具有电子结构调控的Zn-CNF具有超低的成核过电位（8 mV）和超高的库仑效率（超过1600次循环），达到99.94%。对称电池在1ma cm−2下表现出稳定的Na+镀/剥离行为，持续时间超过4400小时。此外，在高阴极负载（7.97 mg cm−2）下，AFSMBs的能量密度达到374 W h kg−1，放电容量为82.49 mA h g−1,120次循环后容量保持率为80.4%。这项工作提出了实现高能量密度afsmb的可行策略。

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引用次数: 0

Enhancing dipole polarization loss in conjugated metal-organic frameworks via coordination symmetry breaking under electromagnetic field 电磁场下配位对称性破缺增强共轭金属有机骨架中偶极子极化损耗

Advanced Powder Materials

Pub Date : 2025-05-19 DOI: 10.1016/j.apmate.2025.100302

Weize Wang , Rong Liu , Jiaqi Tao , Tinglei Yu , Yijie Liu , Lvtong Duan , Zifu Zhang , Zhihao He , Shuang Chen , Jintang Zhou , Ping Chen , Peijiang Liu , Zhengjun Yao

Modulating the dipole polarization loss in the single-atom region and establishing its direct relationship with the electromagnetic wave absorption (EWA) performance remain an unmet challenge. Here, a dual-ligand modulation strategy, i.e., partially changing coordination atoms in the single-metal region (sMr), is introduced to effectively break the coordination symmetry of conjugated metal-organic frameworks (cMOFs), finally enhancing EWA property of cMOFs materials. Further, the asymmetrical sMr is experimentally found to elicit the dipole polarization loss, overcoming the handicaps of other electromagnetic wave loss mechanisms, which directly contribution to enhance EWA performance of this series of cMOFs. This strategy is further confirmed by replacing metal centers. Among studied series of cMOFs, Cu_2.25/Co_0.75(HHTP_1.67HITP_0.33) achieves excellent EWA performance with an effective absorption bandwidth of 5.00 GHz and a reflection loss of −66.03 dB. We introduce a dual-ligand modulation strategy targeting single-metal regions within cMOFs here, aiming to achieve superior EWA performance through atomic-scale dipole polarization loss modulation. We hope our study can inspire more exploration to realize high-performance EWA materials.

调制单原子区域的偶极极化损耗并建立其与电磁波吸收性能的直接关系仍然是一个未解决的难题。本文引入双配体调制策略，即部分改变单金属区（sMr）的配位原子，有效打破共轭金属有机骨架（cMOFs）的配位对称性，最终提高cMOFs材料的EWA性能。此外，实验还发现，不对称的sMr引起了偶极子极化损耗，克服了其他电磁波损耗机制的缺陷，这直接有助于提高该系列cmos的EWA性能。更换金属中心进一步证实了这一策略。在所研究的cMOFs系列中，Cu2.25/Co0.75（htp1.67 - hitp0.33）具有优异的EWA性能，有效吸收带宽为5.00 GHz，反射损耗为- 66.03 dB。本文介绍了一种针对cMOFs内单金属区域的双配体调制策略，旨在通过原子尺度的偶极极化损耗调制来实现优越的EWA性能。我们希望我们的研究能够激发更多的探索，实现高性能的EWA材料。

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引用次数: 0

Recent progress on high-precision construction of nanoarchitectured SERS substrates for ultrasensitive bio-medical sensors 超灵敏生物医学传感器用纳米结构SERS基板的高精度构建研究进展

Advanced Powder Materials

Pub Date : 2025-05-15 DOI: 10.1016/j.apmate.2025.100300

Heguang Liu , Ben Mou , Jinxin Li , Na Tian , Yiming Feng , Xiaodong Cui , Yury Kapitonov , Huageng Liang , Caiyin You , Yuan Li , Tianyou Zhai

Surface-enhanced Raman spectroscopy (SERS) has evolved from a laboratory technique to a practical tool for ultra-sensitive detection, particularly in the biomedical field, where precise molecular identification is crucial. Despite significant advancements, a gap remains in the literature, as no comprehensive review systematically addresses the high-precision construction of SERS substrates for ultrasensitive biomedical detection. This review fills that gap by exploring recent progress in fabricating high-precision SERS substrates, emphasizing their role in enabling ultrasensitive bio-medical sensors. We carefully examine the key to these advancements is the precision engineering of substrates, including noble metals, semiconductors, carbon-based materials, and two-dimensional materials, which is essential for achieving the high sensitivity required for ultrasensitive detection. Applications in biomedical diagnostics and molecular analysis are highlighted. Finally, we address the challenges in SERS substrate preparation and outline future directions, focusing on improvement strategies, design concepts, and expanding applications for these advanced materials.

表面增强拉曼光谱（SERS）已经从实验室技术发展成为超灵敏检测的实用工具，特别是在生物医学领域，精确的分子鉴定至关重要。尽管取得了重大进展，但文献中仍然存在空白，因为没有全面的综述系统地解决了用于超灵敏生物医学检测的SERS底物的高精度构建。本文通过探索制造高精度SERS衬底的最新进展来填补这一空白，强调它们在实现超灵敏生物医学传感器中的作用。我们仔细研究了这些进步的关键是衬底的精密工程，包括贵金属，半导体，碳基材料和二维材料，这对于实现超灵敏检测所需的高灵敏度至关重要。强调了生物医学诊断和分子分析方面的应用。最后，我们解决了SERS基板制备中的挑战，并概述了未来的发展方向，重点关注这些先进材料的改进策略，设计概念和扩展应用。

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引用次数: 0

Integrating luminescence with triboelectricity: Meticulously designed hybrid nanogenerator for multipurpose applications 集成发光与摩擦电：精心设计的混合纳米发电机多用途应用

Advanced Powder Materials

Pub Date : 2025-05-15 DOI: 10.1016/j.apmate.2025.100301

Mandar Vasant Paranjape , Punnarao Manchi , Harishkumarreddy Patnam , Anand Kurakula , Venkata Siva Kavarthapu , Jae Su Yu

A seamless combination of mechanical energy-harvesting triboelectric nanogenerators with other technologies is the key to widening their applicability. Combining luminescent and triboelectric materials can develop hybrid nanogenerators (HNGs) which can be utilized for energy-harvesting, optical thermometry, and lighting applications. In this study, we designed an Er³⁺ and Eu³⁺ co-doped Sr_1.85Ca_0.15NaNb₅O₁₅ (SCNNO:EE) green-yellow-emitting phosphor with excellent temperature-sensing capabilities. SCNNO:EE possessed a high dielectric constant and was thus utilized as a filler inside the polydimethylsiloxane polymer to fabricate composite films. The composite films were employed to fabricate various HNG devices and the filler concentration was optimized to attain the highest electrical output of 170 V, 5.05 μA, and 75 μC/m². The piezoelectric-structured energy-harvesting device (PSEHD) was fabricated and further modified to fabricate a self-activated PSEHD (SAPSEHD) for solid-state lighting applications. Different engraved aluminum electrodes were attached to the composite films to obtain different glowing words and patterns. The electrical signals generated by the PSEHD, when the pressure was applied, were fed into the processing unit, which further flowing into the SAPSEHD. The SAPSEHD can generate electrical signals when pressure is applied and automatically produce light by activating the phosphor in the composite film. This type of devices could attract attention at the places where pressure-activated automatic lighting is required. Also, owing to the promising properties of the proposed devices, they can be utilized for various applications on a large scale.

机械能量收集摩擦电纳米发电机与其他技术的无缝结合是扩大其适用性的关键。结合发光材料和摩擦电材料可以开发混合纳米发电机（HNGs），可用于能量收集，光学测温和照明应用。在这项研究中，我们设计了一种Er3+和Eu3+共掺杂的Sr1.85Ca0.15NaNb5O15 （SCNNO:EE）绿黄发光荧光粉，具有优异的温度传感能力。SCNNO:EE具有较高的介电常数，因此被用作聚二甲基硅氧烷聚合物内部的填料来制备复合薄膜。利用复合薄膜制备了各种HNG器件，并对填料浓度进行了优化，获得了最高电输出为170 V、5.05 μA和75 μC/m2。制备了压电结构能量收集装置（PSEHD），并对其进行了进一步改进，以制造用于固态照明应用的自激活PSEHD （SAPSEHD）。将不同的雕刻铝电极附着在复合薄膜上，得到不同的发光字和图案。当施加压力时，PSEHD产生的电信号被送入处理单元，处理单元进一步流入SAPSEHD。当施加压力时，SAPSEHD可以产生电信号，并通过激活复合膜中的荧光粉自动发光。这种类型的设备可以在需要压力激活自动照明的地方引起注意。此外，由于所提出的器件的有前途的性质，它们可以大规模地用于各种应用。

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引用次数: 0

Single bond regulated 1O2 and ‧O2− selective generation of heptazine-based conjugated polymers for high-selectivity photocatalysis 单键调控的1O2和·O2−选择性生成用于高选择性光催化的七嗪基共轭聚合物

Advanced Powder Materials

Pub Date : 2025-05-03 DOI: 10.1016/j.apmate.2025.100299

Guobang Li , Mengkai Wang , Dan Yang , Ziwen Yu , Tianyu Qiu , Tonghui Wang , Qing Jiang , Yangguang Li , Huaqiao Tan

In conjugated polymers (CPs) photocatalytic system, the generation of reactive oxygen species (ROS) is regulated by cross-scale factors involving active site, excitonic behavior, and O₂ activation process on the surface. However, research on exploring the domino effect of “structure → excitonic behavior → O₂ activation → photocatalytic reaction” through structural modification at the atomic scale remains at its early stages. Herein, two heptazine-based CPs, CP-DPA, and CP-CZ were successfully prepared by polymerization of precursors formed by reacting diphenylamine (DPA) and carbazole (CZ) with cyameluric chloride, respectively. The minute difference in single bond between DPA and CZ endows the polymers with distinct physicochemical properties. Owing to the rotation between benzene rings, CP-DPA exhibits relatively lower conjugation, resulting in increased exciton binding energy (E_b) and inhibited exciton dissociation. Meanwhile, its more triplet state excitons facilitate energy transfer to generate singlet oxygen. Therefore, CP-DPA shows excellent activity for phenylboronic acid oxidation. Conversely, CP-CZ possesses relatively higher conjugation, minimal E_b and intensified exciton dissociation, which promotes charge transfer to produce superoxide radical. Consequently, CP-CZ displays optimal activity for phenylacetylene oxidation and [3 + 2] cycloaddition. This work provides new insights into regulating ROS generation by modulating the composition and structure of photocatalysts at the atomic scale.

在共轭聚合物（CPs）光催化体系中，活性氧（ROS）的生成受活性位点、激子行为和表面O2活化过程等跨尺度因素的调控。然而，在原子尺度上通过结构修饰探索“结构→激子行为→O2活化→光催化反应”多米诺骨牌效应的研究仍处于早期阶段。以二苯胺（DPA）和咔唑（CZ）与氯氰尿酸分别反应形成的前驱体为原料，成功地聚合制备了CP-DPA和CP-CZ两种以七嗪为基础的CPs。DPA和CZ之间单键的微小差异赋予了聚合物不同的物理化学性质。由于苯环之间的旋转，CP-DPA表现出相对较低的共轭作用，从而增加了激子结合能（Eb），抑制了激子解离。同时，它的三重态激子较多，有利于能量转移生成单线态氧。因此，CP-DPA对苯硼酸具有良好的氧化活性。相反，CP-CZ具有较高的共轭性，Eb最小，激子解离加剧，促进电荷转移产生超氧自由基。因此，CP-CZ表现出最佳的苯乙炔氧化活性和[3 + 2]环加成活性。这项工作为通过在原子尺度上调节光催化剂的组成和结构来调节ROS的产生提供了新的见解。

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