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Gradient Thermal Annealing Assisted Perovskite Film Crystallization Regulation for Efficient and Stable Photovoltaic-Photodetection Bifunctional Device. 梯度热退火辅助包光体薄膜结晶调节,实现高效稳定的光伏-光电探测双功能器件。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1002/smtd.202401098
Zhiyu Wang, Peng Chen, Jianwen Luo, Zexian Ouyang, Mulin Sun, Qin Hu, Weiguang Xie, Pengyi Liu, Ke Chen

Perovskite crystallization regulation is essential to obtain excellent film optoelectronic properties and device performances. However, rapid crystallization during annealing always results in poor perovskite film and easy formation of trap, thereby greatly restricting device performance due to severe non-radiative recombination. Here, an easy and reproducible gradient thermal annealing (GTA) approach is used to regulate the perovskite crystallization. Through a low-temperature initial annealing of GTA, the solvent evaporation is slowed down, thus extending nucleation time and providing a buffer for the rapid crystallization of perovskite grains in the subsequent high-temperature stage. As a result, completely converted and highly crystalline perovskite is obtained with 1.6 times larger grain size, reduced trap density and suppressed non-radiative recombination of photo-generated carriers. The film crystallinity is also enhanced with more advantageous (100) and (111) lattice facets which are favorable for carrier transport. Consequently, the perovskite photodetectors exhibit a large linear dynamic range of 174 dB and an excellent response even under ultra-weak light of 303 pW. Meanwhile, perovskite solar cells achieved increased PCE and maintained 85% of original efficiency after heating at 65 °C for nearly 1000 h under unencapsulated conditions. To the knowledge, this represents the best performance reported for a perovskite photovoltaic-photodetection bifunctional device.

要获得优异的薄膜光电特性和器件性能,必须对包晶石结晶进行调节。然而,退火过程中的快速结晶总是会导致包晶体薄膜变差,并容易形成陷阱,从而由于严重的非辐射重组而极大地限制了器件的性能。在这里,我们采用了一种简单且可重复的梯度热退火(GTA)方法来调节包晶石的结晶。通过 GTA 的低温初始退火,减缓了溶剂蒸发,从而延长了成核时间,并为随后的高温阶段中包晶石晶粒的快速结晶提供了缓冲。因此,获得了完全转化和高度结晶的包晶体,其晶粒大小增加了 1.6 倍,阱密度降低,光生载流子的非辐射重组受到抑制。此外,薄膜的结晶度也得到了提高,具有更多有利于载流子传输的(100)和(111)晶格面。因此,包晶石光电探测器的线性动态范围高达 174 dB,即使在 303 pW 的超微弱光下也能做出出色的响应。同时,在未封装的条件下,在 65 °C 下加热近 1000 小时后,包晶体太阳能电池的 PCE 得到提高,并保持了 85% 的原始效率。据了解,这是目前所报道的包晶体光伏-光电检测双功能器件的最佳性能。
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引用次数: 0
Fusing Allosteric Ribozymes with CRISPR-Cas12a for Efficient Diagnostics of Small Molecule Targets. 用 CRISPR-Cas12a 融合异构胰蛋白酶,实现小分子靶标的高效诊断。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1002/smtd.202401236
Lichuan Guo, Shu Zhang, Xinyu Du, Mo Zhou, Hongzhou Gu

The CRISPR-Cas systems are adopted as powerful molecular tools for not only genetic manipulation but also point-of-care diagnostics. However, methods to enable diagnostics of non-nucleic-acid targets with these systems are still limited. Herein, by fusing ligand-dependent allosteric ribozymes with CRISPR-Cas12a, a derived CRISPR-Cas system is created for efficient quantitative analysis of non-nucleic-acid targets in 1-2 h. On two different small molecules, the system's generality, reliability and accuracy is demonstrated, and show that the well operability of this system can enable high-throughput detection of a small molecule in blood samples. The system can be further converted to rely on allosteric deoxyribozyme instead of allosteric ribozyme to recognize non-nucleic-acid targets and transduce the signal to CRISPR-Cas12a for amplification, likely making it easier for storage and more consistent in data generation as DNA possess a stability advantage over RNA. This (deoxy)ribozyme-assisted CRISPR-Cas12a system anticipates that it can facilitate bioanalysis in various scientific and clinical settings and further drive the development of clinical translation.

CRISPR-Cas 系统是一种强大的分子工具,不仅可用于遗传操作,还可用于护理点诊断。然而,利用这些系统对非核酸靶标进行诊断的方法仍然有限。本文通过将配体依赖性异位核酶与CRISPR-Cas12a融合,创建了一种衍生的CRISPR-Cas系统,可在1-2小时内对非核酸靶标进行高效定量分析。在两种不同的小分子上,展示了该系统的通用性、可靠性和准确性,并表明该系统的良好可操作性可实现血液样本中小分子的高通量检测。由于 DNA 比 RNA 具有稳定性优势,该系统可进一步转换为依靠异位脱氧核糖核酸酶而不是异位核糖核酸酶来识别非核酸靶标,并将信号转导至 CRISPR-Cas12a 进行扩增,从而使其更易于储存,数据生成也更加一致。这种(脱氧)核酸酶辅助 CRISPR-Cas12a 系统有望促进各种科学和临床环境中的生物分析,并进一步推动临床转化的发展。
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引用次数: 0
Homogeneous Integration of Polyoxometalates and Titania into Crumpled Layers. 将聚氧化金属盐和二氧化钛均匀集成到皱褶层中。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1002/smtd.202401377
Bilal Akram, Syeda Sundas Musawar, Sanam Mumtaz, Fozia Nazir, Palwisha Umer, Qingda Liu

The crumpling and buckling in nanosheets are anticipated to provide new characteristics that could not be observed in ideal flat layers. However, the rigid lattice structure of inorganic metal oxides limits their assembly into well-defined crumpled layers. Here, this study demonstrates that at the sub-nm scale, polyoxometalates (POMs) clusters having well-defined structures can intercede during the nucleation process of titania and co-assemble with nuclei to form uniform, large-sized crumpled binary 2D layers with a thickness of 2 nm. The obtained crumpled layers are then used as a support material to immobilize Pd nanoclusters with an average size of 2 nm. Pd-immobilized crumpled layers are employed as heterogeneous catalysts for the partial hydrogenation of acetylene. This structurally and compositionally unique heterogeneous catalyst manifests exceptional selectivity to cis-alkene with almost 100% yield as compared to commercially available titania which only exhibits 10% diphenylacetylene conversion and 42% selectivity in the given period of time.

纳米片中的皱缩和屈曲预计将提供在理想平面层中无法观察到的新特性。然而,无机金属氧化物的刚性晶格结构限制了它们组装成定义明确的皱缩层。本研究在此证明,在亚纳米尺度上,具有明确结构的聚氧化金属(POMs)团簇可以在二氧化钛成核过程中介入,并与核共同组装形成厚度为 2 纳米的均匀、大尺寸皱缩二元二维层。获得的皱缩层可用作固定平均尺寸为 2 纳米的钯纳米团簇的支撑材料。固定了钯的皱缩层被用作乙炔部分氢化的异相催化剂。这种结构和组成独特的异相催化剂对顺式烯烃的选择性极高,收率几乎达到 100%,而市售的二氧化钛在给定时间内的二苯基乙炔转化率仅为 10%,选择性仅为 42%。
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引用次数: 0
Boosting the Performance and Durability of Fe-N-C Fuel Cell Catalysts via Integrating Mo2C Clusters. 通过整合 Mo2C 簇提升 Fe-N-C 燃料电池催化剂的性能和耐用性。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1002/smtd.202401270
Liming Guo, Xin Wan, Xiaofang Liu, Jiaxiang Shang, Ronghai Yu, Jianglan Shui

Carbon-supported nitrogen-coordinated iron single-atom (Fe-N-C) catalysts have been regarded among the most promising platinum-group-metal-free catalysts for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). Nevertheless, their limited intrinsic activity and unsatisfactory stability have hindered their practical applications. Here, it is reported that the integration of Mo2C clusters effectively enhances the ORR activity and stability of Fe-N-C catalysts. The composite catalyst of Fe single atoms and Mo2C clusters co-embedded on nitrogen-doped carbon (FeSA/Mo2C-NC) exhibits an excellent ORR activity with a half-wave potential of 0.82 V in acidic media and a high peak power density of 0.5 W cm-2 in an H2-air PEMFC. Moreover, improved stability is achieved with nearly no decay under H2-air conditions for 80 h at 0.4 V. Experiments with theoretical calculations elucidate that the etching effect of the phosphomolybdic acid precursor optimizes the pore size distribution of the composite catalyst, thereby exposing more active sites. The Mo2C clusters modulate the electronic configuration of the Fe-N4 sites, optimizing adsorption energy for ORR intermediates and strengthening the Fe-N bond to mitigate demetalation. This work provides valuable insights into the construction of single-atom/nanoaggregate hybrid catalysts for efficient energy-related applications.

碳支撑氮配位铁单原子(Fe-N-C)催化剂一直被认为是质子交换膜燃料电池(PEMFC)中最有前途的氧还原反应(ORR)无铂族金属催化剂之一。然而,它们有限的内在活性和不尽人意的稳定性阻碍了它们的实际应用。据报道,Mo2C 团簇的加入有效提高了 Fe-N-C 催化剂的 ORR 活性和稳定性。在掺氮碳(FeSA/Mo2C-NC)上共嵌铁单原子和 Mo2C 团簇的复合催化剂表现出优异的 ORR 活性,在酸性介质中的半波电位为 0.82 V,在 H2-air PEMFC 中的峰值功率密度高达 0.5 W cm-2。此外,稳定性也得到了提高,在 0.4 V 的氢空气条件下,80 小时内几乎没有衰减。实验和理论计算阐明,磷钼酸前驱体的蚀刻效应优化了复合催化剂的孔径分布,从而暴露出更多的活性位点。Mo2C 团簇调节了 Fe-N4 位点的电子构型,优化了 ORR 中间体的吸附能,并加强了 Fe-N 键以减轻脱金属现象。这项工作为构建单原子/纳米团聚体混合催化剂以实现高效的能源相关应用提供了宝贵的见解。
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引用次数: 0
Platinum Nanozyme-Loaded Dissolving Microneedles Scavenge ROS and Promote Lineage Progression for Androgenetic Alopecia Treatment. 铂纳米酶载体溶解微针清除 ROS 并促进雄激素性脱发治疗的血统发展
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-18 DOI: 10.1002/smtd.202401176
Weitong Hu, Shuhan Shi, Yihua Xu, Yunting Zhang, Jingyi Hu, Qiong Bian, Xiaolu Ma, Yuxian Ye, Shengfei Yang, Xiaoxia Sheng, Guang Liang, Tianyuan Zhang, Haibin Wu, Jianqing Gao

Androgenetic alopecia (AGA) is a prevalent issue affecting the physical and mental health of individuals but with fewer current treatments. Platinum nanozymes (PtNZs) are known for their excellent ability to reduce and modulate the high oxidative stress environment in AGA pathology. And microneedles are used to overcome the skin barrier due to the poor permeability of PtNZs. Herein, dissolving microneedles loaded with PtNZs (Pt-MNs) are designed and successfully induced hair regeneration in the AGA model. Pt-MNs possessed adequate mechanical strength to breach the skin barrier for effective PtNZs delivery. In vivo, PtNZs first reduced reactive oxygen species (ROS) to oxygen, which recovered the AGA pathological environment. And the oxygen then increased oxidative phosphorylation, promoting the differentiation of hair follicle stem cells to achieve hair regeneration. The group treated with Pt-MNs with a dosing frequency of once every three days achieved faster hair growth than the daily application of the positive drug minoxidil. Further safety experiments showed that the application of Pt-MNs locally opened temporary and recoverable skin channels, with no retention of Pt in major organs, indicating high safety. In conclusion, this study indicated the potential of Pt-MNs as an effective method for treating AGA.

雄激素性脱发(AGA)是一个影响个人身心健康的普遍问题,但目前的治疗方法较少。众所周知,铂纳米酶(PtNZs)具有降低和调节 AGA 病理学中高氧化应激环境的卓越能力。由于 PtNZs 的渗透性较差,微针可用于克服皮肤屏障。本文设计了负载铂氮化合物的可溶解微针(Pt-MNs),并成功诱导了AGA模型中的毛发再生。Pt-MNs具有足够的机械强度,可突破皮肤屏障,有效输送PtNZs。在体内,PtNZs 首先将活性氧(ROS)还原成氧气,恢复了 AGA 的病理环境。然后,氧气增加了氧化磷酸化,促进了毛囊干细胞的分化,实现了毛发再生。与每天服用阳性药物米诺西地相比,每三天服用一次铂-锰的治疗组头发生长速度更快。进一步的安全性实验表明,在局部应用铂族金属络氨酸可打开暂时的、可恢复的皮肤通道,主要器官中没有铂的残留,这表明铂族金属络氨酸具有很高的安全性。总之,这项研究表明,铂-金属萘有可能成为治疗 AGA 的一种有效方法。
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引用次数: 0
Electric Field Mediated Unclogging of Angstrom-Scale Channels. 电场介导的埃级通道疏通。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-17 DOI: 10.1002/smtd.202400961
Solleti Goutham, Raj Kumar Gogoi, Hiran Jyothilal, Gwang-Hyeon Nam, Abdulghani Ismail, Siddhi Vinayak Pandey, Ashok Keerthi, Boya Radha

Angstrom-scale fluidic channels offer immense potential for applications in areas such as desalination, molecular sieving, biomolecular sequencing, and dialysis. Inspired by biological ion channels, nano- and angstrom (Å)-scale channels are fabricated that mimic these molecular or atomic-scale dimensions. At the Å-scale, these channels exhibit unique phenomena, including selective ion transport, osmotic energy generation, fast water and gas flows, and neuromorphic ion memory. However, practical utilization of Å-scale channels is often hindered by contamination, which can clog these nanochannels. In this context, a promising technique is introduced here for unclogging 2D channels, particularly those with sub-nanometre dimensions (≈6.8 Å). The voltage-cycling method emerges as an efficient and reliable solution for this challenge. The electric field effectively dislodges contaminants from the clogged Å-scale channels, facilitating ion and molecular transport. This study provides practical guidelines for reviving clogged nano- and Å-scale channels, thereby enhancing their applicability in various ion and molecular transport applications.

埃级流体通道在海水淡化、分子筛分、生物分子测序和透析等领域具有巨大的应用潜力。受生物离子通道的启发,人们制造出纳米和埃级(Å)通道,模拟这些分子或原子尺度的尺寸。在埃尺度上,这些通道表现出独特的现象,包括选择性离子传输、渗透能生成、快速水流和气流以及神经形态离子记忆。然而,埃级通道的实际利用往往受到污染的阻碍,污染会堵塞这些纳米通道。在此背景下,本文介绍了一种前景广阔的技术,用于疏通二维通道,尤其是那些亚纳米尺寸(≈6.8 Å)的通道。电压循环法是应对这一挑战的高效可靠的解决方案。电场能有效地将污染物从堵塞的埃级通道中排出,促进离子和分子的传输。这项研究为恢复堵塞的纳米级和埃级通道提供了实用指南,从而提高了它们在各种离子和分子传输应用中的适用性。
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引用次数: 0
An Integrated Microcurrent Delivery System Facilitates Human Parathyroid Hormone Delivery for Enhancing Osteoanabolic Effect. 集成微电流传输系统促进人甲状旁腺激素的传输,增强骨合成代谢效应
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-17 DOI: 10.1002/smtd.202401144
Xiaoyi Mo, Keyu Meng, Zehui Li, Shanwei Lan, Zhengda Ren, Xihong Fu, Chenglin Li, Tiancheng Sun, Denghui Xie, Zhongmin Zhang, Hui-Jiuan Chen

Human parathyroid hormone (1-34) (PTH) exhibits osteoanabolic and osteocatabolic effects, with shorter plasma exposure times favoring bone formation. Subcutaneous injection (SCI) is the conventional delivery route for PTH but faces low delivery efficiency due to limited passive diffusion and the obstruction of the vascular endothelial barrier, leading to prolonged drug exposure times and reduced osteoanabolic effects. In this work, a microcurrent delivery system (MDS) based on multimicrochannel microneedle arrays (MMAs) is proposed, achieving high efficiency and safety for PTH transdermal delivery. The internal microchannels of the MMAs are fabricated using high-precision 3D printing technology, providing a concentrated and safe electric field that not only accelerates the movement of PTH but also reversibly increases vascular endothelial permeability by regulating the actin cytoskeleton and interendothelial junctions through Ca2+-dependent cAMP signaling, ultimately promoting PTH absorption and shortening exposure times. The MDS enhances the osteoanabolic effect of PTH in an osteoporosis model by inhibiting osteoclast differentiation on the bone surface compared to SCI. Moreover, histopathological analysis of the skin and organs demonstrated the good safety of PTH delivered by MDS in vivo. In addition to PTH, the MDS shows broad prospects for the high-efficiency transdermal delivery of macromolecular drugs.

人甲状旁腺激素(1-34)(PTH)具有促骨合成和骨合成作用,较短的血浆暴露时间有利于骨形成。皮下注射(SCI)是 PTH 的传统给药途径,但由于被动扩散受限和血管内皮屏障阻塞,给药效率较低,导致药物暴露时间延长,骨合成作用降低。本研究提出了一种基于多微通道微针阵列(MMA)的微电流给药系统(MDS),可实现高效、安全的 PTH 经皮给药。MMAs 的内部微通道采用高精度三维打印技术制造,可提供一个集中而安全的电场,不仅能加速 PTH 的移动,还能通过 Ca2+ 依赖性 cAMP 信号调节肌动蛋白细胞骨架和内皮间连接,从而可逆地增加血管内皮的通透性,最终促进 PTH 的吸收并缩短暴露时间。与 SCI 相比,在骨质疏松症模型中,MDS 通过抑制骨表面破骨细胞的分化,增强了 PTH 的骨合成代谢作用。此外,皮肤和器官的组织病理学分析表明,MDS 在体内输送的 PTH 具有良好的安全性。除 PTH 外,MDS 还为大分子药物的高效透皮给药展示了广阔的前景。
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引用次数: 0
Lubricin-Inspired Nanozymes Reconstruct Cartilage Lubrication System with an “In-Out” Strategy (Small Methods 10/2024) 受润滑蛋白启发的纳米酶通过 "进-出 "策略重建软骨润滑系统(小方法 10/2024)
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1002/smtd.202470059
Chengcheng Du, Zhuolin Chen, Senrui Liu, Jiacheng Liu, Jingdi Zhan, Jing Zou, Junyi Liao, Wei Huang, Yiting Lei

Inside Front Cover

In article number 2400757, Liao, Huang, Lei, and co-workers developed a novel nanozyme which employs an “In-Out” strategy to restore the cartilage lubrication system. The “Out” aspect aims to decrease friction and minimize the wear and tear on cartilage, while the “In” aspect is focused on alleviating oxidative stress to facilitate the production and secretion of lubricin, thereby enhancing the natural lubrication capacity of cartilage.

封面内页在编号为 2400757 的文章中,Liao、Huang、Lei 及其合作者开发了一种新型纳米酶,它采用 "进-出 "策略来恢复软骨润滑系统。出 "的目的是减少摩擦,将软骨的磨损降至最低,而 "入 "的重点是减轻氧化应激,促进润滑蛋白的产生和分泌,从而增强软骨的天然润滑能力。
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引用次数: 0
Hyaluronic Acid Receptor-Mediated Nanomedicines and Targeted Therapy (Small Methods 10/2024) 透明质酸受体介导的纳米药物和靶向治疗(小方法 10/2024)
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1002/smtd.202470062
Qiuhong Ouyang, Ying Zhao, Kunyao Xu, Yuechen He, Meng Qin

Inside Back Cover

In article number 2400513, Qin and co-workers review the hyaluronic acid (HA) receptor-mediated nanomedicines and targeted therapy. HA exhibits multiple endogenous cellular receptors. Based on ligand-receptor interactions, HA-modified nanomedicines can target and bind to overexpressed cellular receptors, which are widely used in the treatment of diseases such as tumors and inflammation.

封底内页在编号为 2400513 的文章中,Qin 及其合作者回顾了透明质酸(HA)受体介导的纳米药物和靶向治疗。透明质酸具有多种内源性细胞受体。基于配体与受体之间的相互作用,HA修饰的纳米药物可以靶向并结合过表达的细胞受体,广泛应用于肿瘤和炎症等疾病的治疗。
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引用次数: 0
Revealing the Structural Intricacies of Biomembrane-Interfaced Emulsions with Small- and Ultra-Small-Angle Neutron Scattering (Small Methods 10/2024) 利用小角和超小角中子散射揭示生物膜界面乳液的复杂结构(小方法 10/2024)
IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-16 DOI: 10.1002/smtd.202470063
Mark Louis P. Vidallon, Ashley P. Williams, Mitchell J. Moon, Haikun Liu, Sylvain Trépout, Alexis I. Bishop, Boon Mian Teo, Rico F. Tabor, Karlheinz Peter, Liliana de Campo, Xiaowei Wang

Back Cover

Unlocking the mysteries of cell membranes with advanced neutron scattering techniques like Kookaburra USANS and Bilby SANS. These powerful technologies provide super lenses, revealing the hidden complexities of cell-inspired materials. This breakthrough opens exciting possibilities to understand and design cell-inspired and biomimetic materials. More in article number 2400348, Vidallon, de Campo, Wang, and co-workers.

封底 利用 Kookaburra USANS 和 Bilby SANS 等先进的中子散射技术揭开细胞膜的神秘面纱。这些强大的技术提供了超级透镜,揭示了细胞启发材料隐藏的复杂性。这一突破为了解和设计细胞启发材料和仿生材料提供了令人兴奋的可能性。更多信息请参见文章编号 2400348,Vidallon、de Campo、Wang 及合作者。
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引用次数: 0
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