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Optimizing Peptide Ionizable Lipids Enables Efficient and Low-Toxicity mRNA Delivery for In Vivo Prime Editing and Protein Replacement Therapy 优化多肽可电离脂质,为体内先导编辑和蛋白质替代治疗提供高效、低毒的mRNA递送
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1002/adma.202522552
Qiu Wang, Yi Lin, Jiahui Xiao, Keqing Xu, Zijin Luo, Hongyu Ren, Fan Liu, Lu Jia, Tuo Wei, Qiang Cheng
Highly efficient mRNA lipid nanoparticle (LNP) often presents potential safety risks. Here, we establish a structure–activity relationship framework for peptide ionizable lipids (PILs) to facilitate the rational design of safe and effective mRNA-LNPs. The PIL structure comprises three modular components: building block, side-chain length, and hydrophobic tail. Through systematic optimization, a lead compound (Dab4) with four building blocks and a moderate side chain length was identified, demonstrating minimized hepatotoxicity while maintaining superior delivery performance. Leveraging this framework, a series of Dab4-derived PILs with three tail types, including alkyl (a-tail), ester (aat-tail), and hydroxyl (e-tail), were synthesized. This tail chemistry determined organ tropism, with B12-a13Dab4 (a-tail) showing optimal performance in the liver. The B12-a13Dab4 LNP exhibited significantly higher hepatic delivery efficiency and markedly improved biosafety compared with the FDA-approved SM-102 formulation. Moreover, B12-a13Dab4 LNP efficiently triggers in vivo prime editing by co-delivering PE7 mRNA and epegRNA, and achieves significant therapeutic effects in a Hereditary Tyrosinemia Type 1 (HT-1) model through repeated delivery fumarylacetoacetate hydrolase (FAH) mRNA. This study establishes rational design principles for PILs that strike a balance between efficacy and safety, offering a versatile mRNA-LNP platform for the advancement of gene editing and protein replacement therapies.
高效的mRNA脂质纳米颗粒(LNP)往往存在潜在的安全风险。在此,我们建立了肽离子脂质(pil)的构效关系框架,以促进安全有效的mRNA-LNPs的合理设计。PIL结构由三个模块组成:构建块、侧链长度和疏水尾部。通过系统优化,确定了具有四个构建块和中等侧链长度的先导化合物(Dab4),该化合物在保持优异的给药性能的同时具有最小的肝毒性。利用这一框架,合成了一系列由dab4衍生的具有三种尾部类型的PILs,包括烷基(a-tail)、酯(aat-tail)和羟基(e-tail)。这种尾部化学决定了器官趋向性,其中B12-a13Dab4 (a-tail)在肝脏中表现最佳。与fda批准的SM-102制剂相比,B12-a13Dab4 LNP具有更高的肝脏递送效率和显著改善的生物安全性。此外,B12-a13Dab4 LNP通过共同递送PE7 mRNA和epegRNA有效触发体内引物编辑,并通过重复递送富马酰乙酸水解酶(FAH) mRNA在遗传性酪氨酸血症1型(HT-1)模型中获得显著的治疗效果。本研究建立了在疗效和安全性之间取得平衡的合理设计原则,为基因编辑和蛋白质替代疗法的发展提供了一个多功能的mRNA-LNP平台。
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引用次数: 0
Tip-Induced Self-Enhanced Concentration Gradients Catalyst for Sustainable Electrocatalytic Urea Synthesis 尖端诱导自增强浓度梯度催化剂的可持续电催化尿素合成
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1002/adma.202518547
Mingyu Chen, Xupeng Qin, Nannan Guo, Zhou Chen, Chu Zhang, Lipan Luo, Kaizhi Gu, Chade Lv, Luxiang Wang, Qinghua Liu, Zhong Cheng, Ze Wu, Han Li, Yidan Huo, Dawei Chen, Guobin Wen, Chen Chen, Shuangyin Wang
Electrocatalytic C─N coupling via the co-reduction of CO2 and NO3 represents a promising route for sustainable urea synthesis under ambient conditions, simultaneously addressing critical challenges in energy sustainability and environmental remediation. However, its practical implementation is hindered by sluggish C─N coupling kinetics and the competing hydrogen evolution reaction (HER), which severely restricts energy conversion efficiency. Herein, we propose a tip-induced local electric field strategy that generates a self-enhanced concentration gradient to promote electrocatalytic C─N coupling. By constructing densely aligned Co3O4 nanoneedles on carbon cloth, an outstanding electrocatalytic performance was achieved, requiring only an ultra-low potential of −0.60 V versus reversible hydrogen electrode (RHE) while delivering a high urea yield rate of 49.63 umol h−1 cm−2 and a Faradic efficiency of 21.37%. Finite element simulations reveal that the nanoscale high-curvature tip generates an intensified local electric field, enriching potassium ions (K+) at the electrode-electrolyte interface to stabilize key intermediates and direct the reaction pathway toward C─N coupling. Moreover, a series of operando spectroscopic characterizations provide direct evidence for enhanced C─N coupling process under an intensified local electric field. This work offers a generalizable strategy for energy-efficient C─N coupling, paving the way for sustainable utilization of nitrogen and carbon resources.
通过CO2和NO3−的共还原,电催化C─N偶联为环境条件下可持续尿素合成提供了一条有前途的途径,同时解决了能源可持续性和环境修复方面的关键挑战。然而,它的实际实施受到缓慢的C─N耦合动力学和竞争性析氢反应(HER)的阻碍,严重制约了能量转换效率。在此,我们提出了一种尖端诱导的局部电场策略,该策略可以产生自增强的浓度梯度,以促进电催化C─N耦合。通过在碳布上构建密集的Co3O4纳米针,获得了出色的电催化性能,与可逆氢电极(RHE)相比,只需要−0.60 V的超低电位,就可以获得49.63 umol h−1 cm−2的尿素产率和21.37%的Faradic效率。有限元模拟表明,纳米级高曲率尖端产生了一个增强的局部电场,在电极-电解质界面富集了钾离子(K+),稳定了关键中间体,并引导了反应途径向C─N耦合方向发展。此外,一系列的operando光谱表征为局域电场增强下的C─N耦合过程提供了直接证据。这项工作为节能碳氮耦合提供了一种可推广的策略,为氮和碳资源的可持续利用铺平了道路。
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引用次数: 0
Engineering Bilayer Tandem Catalysts on Si-Based Photocathodes for High-performance CO2 Reduction to Produce Methane 硅基光电阴极上的工程双层串联催化剂用于高效CO2还原制甲烷
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1002/adma.202518249
Hao Wu, Shenghe Si, Haitao Wang, Changlai Wang, Rongchi Dai, Jianuo Li, Shohei Fukaya, Zhenhua Pan, Yujie Xiong, Noritaka Usami, Koyo Norinaga, Yasuyoshi Kurokawa, Suchada Sirisomboonchai, Dong Liu, Qian Wang
Solar-powered CO2 reduction through photoelectrochemical (PEC) approaches to produce hydrocarbon fuels, such as methane (CH4), is one of the most promising paths for supplying sustainable fuels. However, the limited light absorption capability and sluggish kinetics restrict the photocatalytic rate and selectivity for hydrocarbon production. Here, we introduce tandem catalysts on photocathodes designed to enhance controlled sequential reactions involving intermediates and thus the selectivity of CO2 reduction. Specifically, when mounted on Cu/Ag-Cu bilayer catalysts, the p-type Si photocathode with a pyramid-structured surface dramatically improves CO2-to-CH4 conversion, achieving a selectivity of 60.2 ± 3.4% and a working current density of −32.9 ± 1.9 mA cm−2 at −1.1 V vs. RHE. As identified by operando Raman and synchrotron-radiation Fourier transform infrared spectroscopy and Density Functional Theory, the bottom layer of the Cu/Ag-Cu catalysts comprises Ag and Cu nanoparticles, which catalyse the initial reduction of CO2 to form *CO and the creation of *H species dissociated from H2O, respectively. The top Cu layer subsequently enables the protonation of *CO to *CHO, ultimately yielding CH4. This design of tandem catalysts, coupled with a thorough investigation of the reaction mechanisms, offers a powerful approach toward high-performance and selective pathways for solar-powered CO2 reduction to targeted products.
通过光电化学(PEC)方法减少太阳能二氧化碳以生产碳氢化合物燃料,如甲烷(CH4),是供应可持续燃料最有前途的途径之一。然而,有限的光吸收能力和缓慢的动力学限制了光催化产烃的速率和选择性。在这里,我们在光电阴极上引入串联催化剂,旨在增强涉及中间体的可控顺序反应,从而提高CO2还原的选择性。具体来说,当安装在Cu/Ag-Cu双层催化剂上时,具有金字塔结构表面的p型Si光电阴极显著提高了co2到ch4的转化率,在−1.1 V下,与RHE相比,其选择性为60.2±3.4%,工作电流密度为−32.9±1.9 mA cm−2。通过Raman和同步辐射傅里叶变换红外光谱以及密度泛函理论鉴定,Cu/Ag-Cu催化剂的底层由Ag和Cu纳米颗粒组成,它们分别催化CO2的初始还原生成*CO和生成*H。顶部Cu层随后使*CO质子化成*CHO,最终生成CH4。这种串联催化剂的设计,加上对反应机制的深入研究,为太阳能二氧化碳减排目标产品的高性能和选择性途径提供了强有力的途径。
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引用次数: 0
Topology-Optimized Stretchable Piezoelectric Sensors With Tailored Liquid-Metal Circuits for Anisotropic Stress-Adaptive Motion Monitoring. 面向各向异性应力自适应运动监测的定制液态金属电路拓扑优化可拉伸压电传感器。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202518168
Hanmin Zeng, Qianqian Xu, Jianxun Zhang, Peiqiong Zhou, Jiachen Zhang, Jinlan Li, Senfeng Zhao, Kechao Zhou, Dou Zhang, Chris Bowen, Yan Zhang

The design of high-sensitivity stretchable piezoelectric sensors remains challenging due to the inherent trade-off between the ability to achieve high levels of mechanical deformation while maintaining efficient stress transduction. Here, we propose a new topology-optimization strategy to construct stretchable piezoelectric sensors that efficiently utilize the spatial stress distribution and are able to adapt to a range of anisotropic mechanical stress states. By exploiting computer-aided topology optimization, the distribution of piezoelectric ceramic units within the sensor was tailored to maximize the degree of stress transfer, resulting in an increase of 103.5% and 59.7% in the maximum piezoelectric potential when subject to tension and torsion, respectively. To ensure structural stretchability and adaptability of the topology optimized sensors when subject to complex loading environments, a direct ink writing process was developed to create stretchable eutectic gallium-indium liquid alloy (EGaIn) electrodes. Based on a shear-driven mechanism of printing, new predictive theoretical equations governing printing performance were developed that could predict the printed state (with 94.7% accuracy) and enable trace width control (relative error < 15%). The final optimized sensor exhibited excellent sensitivity, achieving 14.0 V per strain and 0.10 V per degree when subject to tensile and torsional loads, exceeding the unoptimized device by 59.2% and 92.4%, respectively. Finally, inspired by the morphological characteristics of butterflies and guided by the topology-optimized layout, a multi-channel sensor was constructed to accurately identify the pattern and amplitude of a complex range of neck movements, demonstrating the significant potential of the new design and manufacturing approach for wearable electronics.

高灵敏度可拉伸压电传感器的设计仍然具有挑战性,因为在实现高水平机械变形的同时保持有效的应力传导的能力之间存在固有的权衡。在此,我们提出了一种新的拓扑优化策略来构建有效利用空间应力分布并能够适应各种各向异性机械应力状态的可拉伸压电传感器。通过计算机辅助拓扑优化,对传感器内压电陶瓷单元的分布进行了定制,使应力传递程度最大化,在拉伸和扭转作用下,最大压电电位分别提高了103.5%和59.7%。为了确保拓扑优化传感器在复杂负载环境下的结构可拉伸性和适应性,开发了一种直接墨水写入工艺来制备可拉伸共晶镓铟液体合金(EGaIn)电极。基于剪切驱动的打印机制,建立了新的控制打印性能的预测理论方程,该方程可以预测打印状态(准确率为94.7%)并实现迹宽控制(相对误差< 15%)。最终优化后的传感器具有优异的灵敏度,在拉伸和扭转载荷下,其灵敏度分别达到14.0 V /应变和0.10 V /度,分别比未优化的器件高59.2%和92.4%。最后,受蝴蝶形态特征的启发,在拓扑优化布局的指导下,构建了一个多通道传感器,以准确识别复杂范围的颈部运动模式和幅度,展示了新设计和制造方法在可穿戴电子产品中的巨大潜力。
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引用次数: 0
Electrostatic Enhanced Dual-Mode Electronic Skin for Multifunctional Robotic Hands Capable of Object Shape and Material Recognition. 具有物体形状和材料识别能力的多功能机械手静电增强双模电子皮肤。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202521409
Kunwei Bao, Yaguang Guo, Nan Li, Liwu Liu, Yanju Liu, Jinsong Leng

Owing to the increasing requirement for robotic systems to interact intelligently in unstructured and dynamic environments, multimodal perception has become an essential and challenging task. In this study, we introduce a multifunctional robotic hand that can distinguish the shape and material properties of objects using a dual-mode electronic skin (e-skin) capable of non-contact and contact sensing. The e-skin is composed of a polarized expanded polytetrafluoroethylene electret embedded in Ecoflex, thus enabling non-contact sensing via the electrostatic-field effect and contact sensing based on the triboelectric effect. The embedded electret architecture facilitates a high internal charge density, thereby significantly enhancing the intensity and range of non-contact sensing, an advantage not achievable using conventional approaches. Integrating the dual-mode e-skin into a robotic arm endows it with multifunctional capabilities; furthermore, with the assistance of a long short-term memory neural network, the robotic hand achieves 100% and 97.35% accuracies in object-shape and object-material recognition, respectively. This study demonstrates the potential of the proposed e-skin as a versatile multimodal sensing interface for robotic platforms, thereby advancing autonomous and intelligent robotic interactions.

由于对机器人系统在非结构化和动态环境中进行智能交互的要求越来越高,多模态感知已成为一项重要而具有挑战性的任务。在这项研究中,我们介绍了一种多功能机器人手,它可以使用具有非接触式和接触式传感的双模电子皮肤(e-skin)来区分物体的形状和材料特性。电子皮肤由嵌入在Ecoflex中的极化膨胀聚四氟乙烯驻极体组成,从而通过静电场效应实现非接触传感,并基于摩擦电效应实现接触传感。嵌入式驻极体结构促进了高内部电荷密度,从而显着增强了非接触式传感的强度和范围,这是使用传统方法无法实现的优势。将双模电子皮肤集成到机械臂中,使其具有多功能功能;此外,在长短期记忆神经网络的辅助下,机器人手在物体形状和物体材料识别方面的准确率分别达到100%和97.35%。这项研究证明了所提出的电子皮肤作为机器人平台的多功能多模态传感接口的潜力,从而促进了自主和智能机器人的交互。
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引用次数: 0
Bioinspired Thermal Armor Enables Perovskite Meta-Aerogels with Spectrally Tailored Luminescence up to 600 K. 生物启发热装甲使钙钛矿元气凝胶具有光谱定制发光高达600k。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202523117
Yu Jia, Hongxing Wang, Xuan Zhang, Jianyong Yu, Yang Si

High-temperature flexible luminescent materials-enabling information transmission, safety monitoring, and operational reliability at extreme temperatures-have great potential for demanding applications such as metallurgy, petrochemical engineering, and fire protection. However, developing luminescent materials that integrate multicolor emission, high color purity, and mechanical flexibility at high temperatures remains an appealing yet formidable challenge. Herein, inspired by the multilevel architecture protecting pigments in the vividly colored butterfly's wing, we present a multiscale self-confinement strategy to fabricate flexible perovskite luminescent nanofibrous meta-aerogels with bioinspired thermal armor. Benefiting from multidimensional encapsulation to shield perovskite from extrinsic environmental perturbations and directional confinement to suppress ion migration and particle agglomeration, the biomimetic flexible meta-aerogels achieve stable luminescence up to 600 K. The resulting meta-aerogels exhibit tunable emission from blue to red and narrow-band emission (full width at half maximum < 45 nm). Furthermore, the meta-aerogels demonstrate excellent recovery after 500 compression cycles and temperature-invariant superelasticity. These advancements highlight the significant potential of these materials for next-generation flexible lighting and display applications under extreme conditions.

高温柔性发光材料能够在极端温度下实现信息传输、安全监测和运行可靠性,在冶金、石化工程和消防等要求苛刻的应用中具有巨大的潜力。然而,开发集多色发射、高色纯度和高温下机械灵活性于一体的发光材料仍然是一个吸引人但艰巨的挑战。在此,受蝴蝶翅膀中保护色素的多层结构的启发,我们提出了一种多尺度自约束策略来制造柔性钙钛矿发光纳米纤维超气凝胶,并具有生物激发热盔甲。得益于多维包封保护钙钛矿免受外部环境扰动和定向约束抑制离子迁移和颗粒团聚,仿生柔性元气凝胶可实现高达600 K的稳定发光。所得的元气凝胶表现出从蓝色到红色的可调发射和窄带发射(最大半宽< 45 nm)。此外,超气凝胶在500次压缩循环后表现出优异的恢复性能和温度不变的超弹性。这些进步突出了这些材料在极端条件下用于下一代柔性照明和显示应用的巨大潜力。
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引用次数: 0
Sensitive Shortwave Infrared Organic Photodetectors Enabled by Nonfullerene Acceptor Featuring an Ultralow Optical Bandgap of Less than 1.0 eV. 具有小于1.0 eV的超低带隙的非富勒烯受体实现的灵敏短波红外有机光电探测器。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202520509
Yingqi Zheng, Lixiang Wang, Yongjie Chen, Zhong-Ze Qu, Yanjun Fang, Yi Lin, Zheng Tang, Wuyue Liu, Yunlong Guo, Thuc-Quyen Nguyen, Xiaozhang Zhu

Shortwave infrared (SWIR) photodetectors are in high demand in modern applications, including night surveillance, biological imaging, and optical communication. Emerging organic semiconductors, featuring a tailorable spectral response and solution processability, open new avenues for SWIR light detection. However, SWIR organic photodetectors (OPDs) suffer from a scarcity of ultralow-bandgap organic semiconductors and low responsivity above 1000 nm. Here, we report a new electron-rich building block, thieno[3',2':4,5]cyclopenta[1,2-b]thieno[2,3-d]pyrrole (SNCS), that exhibits strong electron-donating ability. By applying acceptor-donor-acceptor and acceptor-quinoidal-donor-quinoidal-acceptor strategy, we developed two new nonfullerene acceptors: SNCS-4F and SNCSTT-4F. The latter, with thieno[3,4-b]thiophene moiety, exhibits strong SWIR absorption up to 1400 nm in thin films. The best-performing PTB7-Th:SNCSTT-4F-based OPD exhibits a record external quantum efficiency of 50.2%, a responsivity of 0.49 A W-1 and remarkable specific detectivity of 4.47 × 1012 Jones at 1200 nm under zero bias. This is the highest performance among reported SWIR organic photodiodes and is comparable with commercial InGaAs photodetectors. Ultraviolet photoelectron spectra, Mott-Schottky analysis and trap density of states analysis were applied to evaluate the OPDs' performances. Finally, we demonstrate that the OPDs can detect SWIR light with high sensitivity in photoplethysmography measurements and infrared audio communication applications.

短波红外(SWIR)光电探测器在现代应用中有很高的需求,包括夜间监视,生物成像和光通信。新兴的有机半导体具有可定制的光谱响应和溶液可加工性,为SWIR光检测开辟了新的途径。然而,SWIR有机光电探测器(opd)受到超低带隙有机半导体的缺乏和1000 nm以上的低响应率的困扰。在这里,我们报道了一种新的富电子构建块-噻吩[3',2':4,5]环penta[1,2-b]噻吩[2,3-d]吡咯(SNCS),它具有很强的给电子能力。采用受体-供体-受体和受体-喹酮-供体-喹酮-受体策略,我们开发了两个新的非富勒烯受体:SNCS-4F和SNCSTT-4F。后者具有噻吩[3,4-b]部分,在薄膜中表现出强烈的SWIR吸收,最高可达1400 nm。性能最好的基于PTB7-Th: sncstt - 4f的OPD具有创纪录的50.2%的外量子效率,0.49 a W-1的响应率和4.47 × 1012 Jones的零偏置下1200 nm比检出率。这是目前报道的SWIR有机光电二极管中性能最高的,与商用InGaAs光电探测器相当。应用紫外光电子能谱、Mott-Schottky分析和阱态密度分析对opd的性能进行了评价。最后,我们证明了opd可以在光体积脉搏波测量和红外音频通信应用中以高灵敏度检测SWIR光。
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引用次数: 0
Dynamic Electron-Hole Shuttle at Atomic Interfaces for Solar-Driven H2O2 and Benzaldehyde Coproduction. 太阳能驱动H2O2和苯甲醛协同生产的原子界面动态电子-空穴穿梭。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202522711
Jugong Shi, Xunlu Wang, Molly Meng-Jung Li, Jiacheng Wang, J Paul Attfield, Ye Zhu, Minghui Yang

Harnessing solar energy to produce value-added chemicals simultaneously requires the critical step of spatially separating redox processes. However, conventional photocatalysts remain fundamentally constrained by sluggish charge dynamics and irreversible recombination. Here, we propose an atomic-level interfacial shuttle mechanism in sub-nanometer gold cluster-anchored nickel manganite (H-NiMn2O4-β/Au0.5 NCs), which couples dynamic electron-hole separation with Ni3+/Ni2+ redox cycling. Ultrafast transient absorption spectroscopy indicates electron transfer occurring within 3.06 ps, mediated by an Au-O-Ni coordination interface. In this system, Ni3+ functions as a transient electron trap, undergoing rapid reduction to Ni2+ and subsequently transferring electrons to adjacent Au clusters, accelerating charge kinetics by 22.16-fold. This atomic-scale electron relay selectively steers 2e- oxygen reduction by balancing *OOH intermediate stabilization and desorption, yielding H2O2 at 1.00 mmol g-1 h-1. Simultaneously, hole accumulation on lattice oxygen drives α-H abstraction, enabling photooxidation of benzyl alcohol to benzaldehyde (14.59 mmol g-1 h-1). This work presents a dynamic dual-site catalysis model, offering atomic-level insight into interfacial charge management for solar-driven redox transformations.

利用太阳能同时生产增值化学品需要空间分离氧化还原过程的关键步骤。然而,传统的光催化剂仍然受到缓慢的电荷动力学和不可逆重组的限制。在这里,我们提出了亚纳米金簇锚定镍锰矿(H-NiMn2O4-β/Au0.5 NCs)中原子水平的界面穿梭机制,该机制将动态电子空穴分离与Ni3+/Ni2+氧化还原循环耦合在一起。超快瞬态吸收光谱表明,电子转移发生在3.06 ps内,由Au-O-Ni配位界面介导。在该体系中,Ni3+作为一个瞬态电子陷阱,快速还原为Ni2+,随后将电子转移到相邻的Au团簇,将电荷动力学加速22.16倍。这种原子级电子继电器通过平衡OOH中间体稳定和解吸,选择性地控制2e-氧还原,产生1.00 mmol g-1 h-1的H2O2。同时,晶格氧上的空穴积累驱动α-H萃取,使苯甲醇光氧化生成苯甲醛(14.59 mmol g-1 h-1)。这项工作提出了一个动态的双位点催化模型,为太阳能驱动的氧化还原转化的界面电荷管理提供了原子水平的见解。
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引用次数: 0
Ultrafast Vertical Organic Electrochemical Transistors With Ion-Permeable Conductive Polymer Top Electrodes. 具有离子渗透导电聚合物顶电极的超快垂直有机电化学晶体管。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202518126
Han-Yan Wu, Yingxue An, Luigi Fabiano, Qifan Li, Qingqing Wang, Feng Zhang, Wenlong Jin, Miao Xiong, Junpeng Ji, Ugo Bruno, Grzegorz Greczynski, Grazia Maria Lucia Messina, Xianjie Liu, Chi-Yuan Yang, Simone Fabiano

Organic electrochemical transistors (OECTs) combine mixed ionic-electronic transport with bulk electrochemical doping to enable high transconductance and low-voltage operation in aqueous environments, making them attractive for bioelectronics and neuromorphic computing. Vertical OECTs (vOECTs), with channel lengths reduced to tens of nanometers, offer high current densities and compact device footprints, but their performance is fundamentally constrained by ion-impermeable metal top electrodes that restrict ion injection to slow lateral diffusion pathways. Here, we show that electrochemically stable, ion-permeable conductive polymers such as poly(benzodifurandione) (PBFDO) offer a powerful alternative to metal top electrodes in vOECTs. By enabling direct vertical ion injection into poly(benzimidazobenzophenanthroline) (BBL) channels, PBFDO yields devices with high current densities (>400 A cm-2), large on/off ratios (>106), and ultrafast switching down to 28 µs, nearly two orders of magnitude faster than equivalent gold-based vOECTs and among the fastest accumulation-mode OECTs reported to date. These results establish a new benchmark for OECT speed and underscore the role of ion-permeable electrodes in overcoming the coupling between electronic and ionic transport in vertical architectures.

有机电化学晶体管(OECTs)结合了混合离子电子输运和大量电化学掺杂,在水环境中实现了高跨导和低电压操作,使其在生物电子学和神经形态计算中具有吸引力。垂直OECTs (vOECTs)的通道长度减少到几十纳米,具有高电流密度和紧凑的器件尺寸,但其性能从根本上受到离子不渗透金属顶部电极的限制,这些电极限制了离子注入到缓慢的横向扩散路径。在这里,我们展示了电化学稳定、离子渗透的导电聚合物,如聚(苯二呋喃二酮)(pbdo),为vOECTs中的金属顶部电极提供了强大的替代品。通过将直接垂直离子注入到聚苯并咪唑苯并菲罗啉(BBL)通道中,pbdo产生的器件具有高电流密度(bbb400 A cm-2)、大开/关比(>06)和超快切换至28µs,比同等的金基vOECTs快近两个数量级,并且是迄今为止报道的最快的积累模式OECTs之一。这些结果建立了OECT速度的新基准,并强调了离子渗透电极在克服垂直结构中电子和离子传输之间耦合方面的作用。
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引用次数: 0
Self-Assembled Monolayers in p-i-n Perovskite Solar Cells: Molecular Design, Interfacial Engineering, and Machine Learning-Accelerated Material Discovery. p-i-n钙钛矿太阳能电池中的自组装单层:分子设计、界面工程和机器学习加速材料发现。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202520220
Asmat Ullah, Ying Luo, Stefaan De Wolf

Self-assembled monolayers (SAMs) have precipitated a paradigm shift in the design of hole transport layers (HTLs) for p-i-n perovskite solar cells, emerging as the cornerstone of modern, high-efficiency devices. This review comprehensively charts the evolution of SAM-based HTLs from fundamental molecular-level insights to their pivotal role in commercial-scale applications and record-breaking perovskite/silicon tandem cells. We delve into the intricate structure-property-performance relationships that govern SAMs' function, examining how meticulous engineering of anchoring groups, π-bridges, and functional headgroups dictates critical features such as energy level alignment, interfacial defect passivation, and perovskite crystallization control. The discussion extends beyond champion efficiencies to critically assess the scalability of deposition techniques, the limitations of operational stability under real-world conditions, and the pathways for integration into tandem architectures. Furthermore, we highlight the transformative potential of machine learning in accelerating the discovery and optimization of next-generation SAM materials. Finally, we provide a forward-looking perspective on molecular design strategies required to overcome existing challenges and fully unlock SAM potential for stable, high-performance photovoltaics.

自组装单层(sam)已经促成了p-i-n钙钛矿太阳能电池空穴传输层(HTLs)设计的范式转变,成为现代高效设备的基石。本文全面回顾了基于sam的HTLs的发展,从基本的分子水平的见解到它们在商业规模应用和破纪录的钙钛矿/硅串联电池中的关键作用。我们深入研究了控制sam功能的复杂结构-性能-性能关系,研究了锚定基团,π桥和功能头基团的细致工程如何决定了诸如能级排列,界面缺陷钝化和钙钛矿结晶控制等关键特性。讨论超越了冠军效率,批判性地评估了沉积技术的可扩展性,实际条件下操作稳定性的局限性,以及集成到串联架构中的途径。此外,我们强调了机器学习在加速发现和优化下一代SAM材料方面的变革潜力。最后,我们提供了前瞻性的分子设计策略,以克服现有的挑战,并充分释放稳定,高性能光伏电池的SAM潜力。
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Advanced Materials
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