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Disrupting the Senescence-Associated Secretory Phenotype–M1Macrophage Feedback Loop in Synovitis Using Dual Nano-Switches To Restore Joint Homeostasis 利用双纳米开关破坏滑膜炎中衰老相关分泌表型- m1巨噬细胞反馈回路以恢复关节稳态
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsnano.5c15543
Jing Zhang,Xinghua Li,Ping Wang,Xin Liu,Wuqi Guo,Jia Si,Qiang Huo,Ming Xu,Yang Liu,Yimin Niu
Osteoarthritis (OA), a leading cause of disability worldwide, impacts over 300 million people through progressive joint degeneration marked by chronic pain and functional impairment. A key driver of osteoarthritis progression is synovitis, characterized by inflamed synovial tissue harboring senescent fibroblasts and pro-inflammatory macrophages. These senescent cells secrete senescence-associated secretory phenotype (SASP) components, includining cytokines and proteases, which drive macrophage polarization toward a pro-inflammatory M1 state. Simultaneously, M1 macrophages release reactive oxygen species (ROS) and inflammatory mediators, amplifying cellular senescence and establishing a pathological feedback loop. Unfortunately, conventional single-target therapies, such as senolytics or macrophage modulators, fail to address this interdependence vicious cycle. Herein, guided by bioinformatics analysis integrated with clinical and murine specimen data, we developed an easy-to-produce combinatorial nanomedicine platform comprising: (i) synovium-targeting liposomes delivering senolytics to clear senescent fibroblasts and suppress SASP, and (ii) M2 macrophage-derived exosomes to convert M1 macrophages into regenerative M2 phenotypes. In rat OA models, this dual approach combined disrupted the senescence-inflammation cascade, achieving 73.53% synovitis index reduction and 75.00% OARSI score reduction. In summary, by concurrently clearing SASP-producing senescent cells and pro-inflammatory M1 macrophages, our strategy restores joint homeostasis and presents a translatable framework for treating age-related inflammatory disorders.
骨关节炎(OA)是全球致残的主要原因之一,它通过以慢性疼痛和功能损伤为特征的进行性关节变性影响着3亿多人。骨性关节炎进展的一个关键驱动因素是滑膜炎,其特征是滑膜组织炎症窝藏衰老成纤维细胞和促炎巨噬细胞。这些衰老细胞分泌衰老相关分泌表型(SASP)成分,包括细胞因子和蛋白酶,它们驱动巨噬细胞向促炎M1状态极化。同时,M1巨噬细胞释放活性氧(ROS)和炎症介质,放大细胞衰老,建立病理反馈回路。不幸的是,传统的单靶点治疗,如抗衰老药或巨噬细胞调节剂,无法解决这种相互依赖的恶性循环。在此,在结合临床和小鼠标本数据的生物信息学分析的指导下,我们开发了一个易于生产的组合纳米药物平台,该平台包括:(i)滑膜靶向脂质体提供抗衰老药物,以清除衰老的成纤维细胞并抑制SASP,以及(ii) M2巨噬细胞来源的外泌体将M1巨噬细胞转化为再生的M2表型。在大鼠OA模型中,这种双重方法联合破坏了衰老-炎症级联,使滑膜炎指数降低了73.53%,OARSI评分降低了75.00%。总之,通过同时清除产生sasp的衰老细胞和促炎M1巨噬细胞,我们的策略恢复了关节稳态,并为治疗与年龄相关的炎症性疾病提供了一个可翻译的框架。
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引用次数: 0
Active Colloid Phase Transitions and Living Binary Crystal Formation 活性胶体相变和活性二元晶体的形成
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsnano.5c19183
Jingyuan Chen,Shaobin Zhuo,Binglin Zeng,Zhigang Li,Jinyao Tang
Colloids can be utilized as model “meta-atoms” to emulate phase behaviors at the atomic scale for easy observation and slower dynamics. Photoactive colloids have recently been demonstrated with on-demand directional interactions as well as tunable dynamics, which are particularly suitable to emulate the phase transition of atomic lattices due to their excellent tunability. In this study, we demonstrate that the photochemical reaction on active colloids can induce an optically tunable hydrodynamic interaction field. By spontaneously controlling the directional interaction and omnidirectional repulsion with two sets of illumination, the phase transition between the zigzag band, chains, and dispersed phase, distinguished by their 2-fold bond orientational order, can be realized. Furthermore, the addition of passive colloids, analogous to reactant atoms with different chemical natures and sizes, causes a “chemical reaction” between the colloid species, forming colloid compounds with well-defined stoichiometric ratios, while the phase transition of the colloid compound can also be emulated with external illumination. By bridging active matter physics and solid-state chemistry, our platform provides a versatile tool for studying phase diagrams and optically encoding “reaction pathways” in colloidal alloys.
胶体可以作为模型“元原子”来模拟原子尺度上的相行为,以方便观察和较慢的动力学。光活性胶体最近被证明具有按需定向相互作用以及可调动力学,由于其优异的可调性,特别适合模拟原子晶格的相变。在这项研究中,我们证明了活性胶体上的光化学反应可以诱导光学可调的水动力相互作用场。通过两组光照自发控制定向相互作用和全向排斥,可以实现以2重键取向顺序区分的之字形带、链和分散相之间的相变。此外,被动胶体的加入,类似于具有不同化学性质和大小的反应物原子,引起胶体物种之间的“化学反应”,形成具有明确定义的化学计量比的胶体化合物,而胶体化合物的相变也可以用外部照明来模拟。通过连接活性物质物理和固态化学,我们的平台为研究相图和光学编码胶体合金中的“反应途径”提供了一个多功能工具。
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引用次数: 0
circTNIK Promotes Carbon Nanotubes-Induced Lung Carcinogenesis via GRP78-Mediated Endoplasmic Reticulum Stress and Suppression of Type I Interferon Signaling circTNIK通过grp78介导的内质网应激和抑制I型干扰素信号传导促进碳纳米管诱导的肺癌发生
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsnano.5c16536
Wenlong Peng,Kexin Chen,Yi Hu,Ziyao Xiao,Zhenyu Pan,Xiliang Yang,Yuqing Tang,Wei Xue,Hongxing Liu,Wen Liu
Circular RNAs (circRNAs) play an important role in tumorigenesis induced by carbon nanotubes (CNTs) exposure, but the specific mechanism remains unclear. Here, we demonstrate for the first time that circTNIK promotes CNTs-induced malignant transformation by regulating the endoplasmic reticulum (ER) chaperone GRP78, thereby disrupting ER homeostasis and inhibiting type I interferon (IFN-I)-mediated antitumor immunity. Mechanistically, circTNIK interacts with GRP78 and interferes with its interaction with UPR sensors, thereby activating the ER stress response and promoting the transformation of cells toward a malignant phenotype. Meanwhile, circTNIK upregulates the expression of GRP78 and promotes its partial translocation into the nucleus. In the nucleus, GRP78 competitively binds to ID2, preventing its interaction with p65, a subunit of nuclear factor-κB (NF-κB), thereby inhibiting the phosphorylation of both NF-κB and IRF3, attenuating the IFN-I-mediated antitumor immune response and accelerating malignant transformation. Animal experiments showed that overexpression of circTNIK aggravated lung lesions in CNTs-exposed mice, accompanied by increased recruitment of M2 macrophages and decreased infiltration of CD8+ T cells. In clinical lung cancer tissue samples, circTNIK expression was positively correlated with GRP78 expression and negatively correlated with IFN-I signaling intensity, further supporting its oncogenic role in vivo. In summary, this study reveals that circTNIK plays a key role in CNTs-induced lung cancer development by regulating GRP78-mediated ER stress and IFN-I immunosuppression, providing a potential biomarker and therapeutic target for the early diagnosis and treatment of environmental-exposure-related lung cancer.
环状rna (circRNAs)在碳纳米管(CNTs)暴露诱导的肿瘤发生中发挥重要作用,但具体机制尚不清楚。在这里,我们首次证明了circTNIK通过调节内质网(ER)伴侣GRP78促进碳纳米管诱导的恶性转化,从而破坏内质网稳态并抑制I型干扰素(IFN-I)介导的抗肿瘤免疫。从机制上讲,circTNIK与GRP78相互作用,干扰GRP78与UPR传感器的相互作用,从而激活内质网应激反应,促进细胞向恶性表型转化。同时,circTNIK上调GRP78的表达,促进其部分易位进入细胞核。在细胞核中,GRP78与ID2竞争性结合,阻止其与核因子-κB (NF-κB)亚基p65的相互作用,从而抑制NF-κB和IRF3的磷酸化,减弱ifn - i介导的抗肿瘤免疫反应,加速恶性转化。动物实验表明,在cnts暴露的小鼠中,circTNIK的过表达加重了肺部病变,同时伴有M2巨噬细胞募集增加和CD8+ T细胞浸润减少。在临床肺癌组织样本中,circTNIK表达与GRP78表达呈正相关,与IFN-I信号强度负相关,进一步支持其在体内的致癌作用。综上所述,本研究揭示了circTNIK通过调节grp78介导的内质网应激和IFN-I免疫抑制在碳纳米管诱导的肺癌发展中发挥关键作用,为环境暴露相关肺癌的早期诊断和治疗提供了潜在的生物标志物和治疗靶点。
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引用次数: 0
Precursor Stabilization Strategies via Vapor–Solid Reaction for Reproducible and High-Efficiency Vapor-Deposited Perovskite Solar Cells 可再生高效气相沉积钙钛矿太阳能电池的气固反应前驱体稳定策略
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsnano.5c18423
Shenghan Hu,Peiran Hou,Yichen Dou,Changyu Duan,Xinyu Deng,Yong Peng,Yi-Bing Cheng,Guijie Liang,Xiong Li,Zhiliang Ku
The stability of perovskite precursors significantly impacts the performance of perovskite solar cell (PSCs). Notably, in the vapor–solid reaction perovskite fabrication process, both organic amine salt precursors and inorganic lead halide precursors are involved. Consequently, the long-term stability of these precursor materials plays a critical role in enabling the industrial-scale production of PSCs. Our observations revealed that the inherent instability of iodide ions (I–) in formamidinium iodide (FAI) precursor solutions accelerates solution aging. Additionally, the photoinstability of lead iodide (PbI2) promotes I– loss, generating iodine vacancies in the material. To address these issues, we introduced l-ascorbic acid (LAA) into the organic amine salt precursor solution to create an acidic and reducing environment, thereby reducing side reactions of the amine salt. Additionally, we effectively enhanced the stability of the PbI2 film by performing a surface dimensional regulation strategy on the PbI2 precursor film with 2-thiophenethylammonium iodide (2-ThEAI) vapor, inhibiting the formation of Pb0. As a result, PSCs fabricated by the optimized precursors achieve a power conversion efficiency (PCE) of 22.51% (@0.16 cm2) and 20.02% (@10 cm2). Remarkably, the four-terminal tandem photovoltaic device integrated with silicon solar cells achieves a PCE of 29.39%, demonstrating exceptional performance potential for next-generation solar technologies.
钙钛矿前驱体的稳定性对钙钛矿太阳能电池(PSCs)的性能有重要影响。值得注意的是,在气固反应制备钙钛矿的过程中,有机胺盐前驱体和无机卤化铅前驱体都有涉及。因此,这些前驱体材料的长期稳定性在实现psc的工业规模生产中起着关键作用。我们的观察结果表明,碘离子(I -)在碘化甲脒(FAI)前驱体溶液中的固有不稳定性加速了溶液的老化。此外,碘化铅(PbI2)的光不稳定性促进了I -损失,在材料中产生碘空位。为了解决这些问题,我们将l-抗坏血酸(LAA)引入到有机胺盐前体溶液中,以创造酸性和还原环境,从而减少胺盐的副反应。此外,我们通过使用2-噻吩乙基碘化铵(2-ThEAI)蒸气对PbI2前驱体膜进行表面尺寸调节策略,有效地增强了PbI2薄膜的稳定性,抑制了Pb0的形成。结果表明,采用优化前驱体制备的PSCs的功率转换效率(PCE)分别为22.51% (@0.16 cm2)和20.02% (@10 cm2)。值得注意的是,与硅太阳能电池集成的四端串联光伏器件的PCE达到29.39%,显示出下一代太阳能技术的卓越性能潜力。
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引用次数: 0
Mid-infrared Intraband Transitions in InAs Colloidal Quantum Dots InAs胶体量子点的中红外带内跃迁
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsnano.5c20445
Shraman Kumar Saha,Philippe Guyot-Sionnest
III–V Colloidal quantum dots (CQDs) have been widely studied for their applications as detectors and emitters from visible to short-wave infrared. They might also be used in the mid-infrared if they can be stably n-doped to access their intraband transitions. Mid-infrared intraband transitions are therefore studied for InAs, InAs/InP, and InAs/ZnSe CQDs with an energy gap of 1.4 μm. Using electrochemistry, the quantum dot films show state-resolved mobility, state-resolved electron filling, and intraband absorption in the 3–8 μm range. The InAs/ZnSe films need a more reducing potential than the InAs, but the InAs/InP films need a lower reduction potential. As a result, we found that dry films of InAs/InP dots show stable n-doping of the 1Se state, with a steady-state intraband absorption in the 3–5 μm range and intraband luminescence at 5 μm. With low toxicity, high thermal stability, and stable n-doping, InAs quantum dots become an interesting material for mid-infrared applications.
胶体量子点(CQDs)作为可见光到短波红外波段的探测器和发射体得到了广泛的研究。如果它们可以稳定地掺杂氮以获得其带内跃迁,它们也可能用于中红外。因此,研究了能隙为1.4 μm的InAs、InAs/InP和InAs/ZnSe CQDs的中红外带内跃迁。电化学分析表明,该量子点薄膜在3 ~ 8 μm范围内具有态分辨迁移率、态分辨电子填充和带内吸收特性。InAs/ZnSe薄膜比InAs需要更大的还原电位,而InAs/InP薄膜需要更小的还原电位。结果表明,InAs/InP点的干膜表现出稳定的1Se态n掺杂,在3 ~ 5 μm波段有稳定的带内吸收,在5 μm波段有稳定的带内发光。由于低毒性、高热稳定性和稳定的n掺杂,InAs量子点成为中红外应用的有趣材料。
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引用次数: 0
Quantitative Stimulated Emission Depletion (STED) Microscopy with DNA-Fluorophore Labels 定量受激辐射损耗(STED)显微镜与dna荧光标记
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c21411
Laurell F. Kessler, Yunqing Li, Ashwin Balakrishnan, Mike Heilemann
Stimulated emission depletion (STED) microscopy enables super-resolution imaging of complex biological samples in 3D, in large volumes, and live. However, molecular quantification with STED has remained underexplored. Here, we present a straightforward approach for quantitative STED that enables molecule counting. For this purpose, we designed DNA-fluorophore labels that enable signal amplification and allow for reliable intensity-based quantitative imaging. We demonstrate accurate molecule counting on DNA origami. Furthermore, we visualized and quantified EGF receptor monomers and dimers in cells. In summary, we introduce a robust, fast, and easy-to-implement tool for quantitative STED microscopy with single-protein resolution.
受激发射损耗(STED)显微镜能够在3D、大体积和活体中对复杂的生物样品进行超分辨率成像。然而,STED的分子定量研究仍未得到充分的探索。在这里,我们提出了一种简单的定量STED方法,可以进行分子计数。为此,我们设计了dna荧光团标签,使信号放大,并允许可靠的基于强度的定量成像。我们在DNA折纸上展示了精确的分子计数。此外,我们可视化和定量细胞中的EGF受体单体和二聚体。总之,我们介绍了一种强大,快速,易于实施的工具,用于单蛋白分辨率的定量STED显微镜。
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引用次数: 0
Strain-Induced Giant Topological Rashba Splitting 菌株诱导的巨型拓扑Rashba分裂
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c16503
Hongwei Wang,Gan Jin,Mingyang Du,Yuxin Li,Xu Li,Xudong Zhu,Yurong Yang,Baomin Wang,Xiaohui Liu,Chengwang Niu,Lixin He,Tian Cui,Karin M. Rabe,Feng Liu
Rashba-type spin–orbit coupling is an important physical phenomenon for spintronic device applications. The size of Rashba splitting is generally enhanced by increasing inversion symmetry breaking, typically by increasing the spontaneous polarization of ferroelectric materials. Here, we identify an intriguing mechanism to enhance Rashba splitting by topological band inversion induced by strain. Using density functional theory, we show that monolayer quasi-1D ferroelectric chalcogenides BaTiSe3 and BaZrSe3 exhibit in-plane polarization, giving rise to Rashba splitting in the valence and conduction band edges with a persistent spin texture. Remarkably, under 1% compressive biaxial strain, the Rashba parameter and splitting energy of monolayer BaZrSe3 are enhanced to ∼3.0 eV Å and ∼60 meV, respectively, among the highest in 2D materials, and concurrently, a giant Berry curvature is induced, which is ∼1400 Å2 in magnitude. Our analysis shows that these enhancements result from a generic mechanism of strain-induced phase transition from semiconductor to topological insulator, which in turn changes interband transitions. Our findings manifest a unique strain-induced interplay between topology and ferroelectricity, and the integration of topological bands with Rashba splitting may provide promising applications to advancing spintronics technology.
rashba型自旋轨道耦合是自旋电子器件应用中的重要物理现象。Rashba分裂的大小通常通过增加反转对称性破缺来增强,特别是通过增加铁电材料的自发极化来增强。在这里,我们确定了一个有趣的机制,以增强Rashba分裂由应变引起的拓扑能带反转。利用密度泛函理论,我们发现单层准一维铁电硫族化合物BaTiSe3和BaZrSe3表现出面内极化,在价带和导带边缘产生Rashba分裂,并具有持续的自旋织体。值得注意的是,在1%的双轴压缩应变下,单层BaZrSe3的Rashba参数和分裂能分别提高到~ 3.0 eV Å和~ 60 meV,是二维材料中最高的,同时产生了一个巨大的Berry曲率,其量级为~ 1400 Å2。我们的分析表明,这些增强来自于从半导体到拓扑绝缘体的应变诱导相变的一般机制,这反过来又改变了带间转变。我们的发现表明了一种独特的应变诱导的拓扑和铁电性之间的相互作用,并且拓扑带与Rashba分裂的集成可能为推进自旋电子学技术提供有前途的应用。
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引用次数: 0
Correction to “Biomimetic Nanoparticles Simultaneously Targeting Modulation of Lipid Metabolism and Phenotype of Macrophages for Programmed Atherosclerosis Management” 对“同时靶向调节脂质代谢和巨噬细胞表型的仿生纳米颗粒用于程序性动脉粥样硬化管理”的修正
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c20273
Xiaoyan Dong,Yaoyu Suo,Jie Yu,Feifei Yu,Feng Li,Judun Zheng,Guizhong Li,Shengchao Ma,Yinju Hao,Huiping Zhang,Bin Liu,Yideng Jiang
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引用次数: 0
Nanofluidic Confined DNA Aptamers for Neuromorphic Multiplex Discrimination 纳米流体约束DNA适体用于神经形态多重识别
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c16862
Yonghuan Chen,Xinru Yue,Yixin Ling,Yang Liu,Weihua Yu,Qi Zhu,Zilong He,Minrui Long,Xin-Qi Hao,Xu Hou,Fengyu Li
Bioinspired nanofluidic systems that utilize ions as signal carriers hold great promise for emulating neural processing in biochemical sensing and neuromorphic computing. However, achieving parallel, brain-like processing of multiple biochemical signals remains a significant challenge. Herein, we present a nanofluidic artificial postsynaptic membrane (APM) functionalized with confined DNA aptamers to construct a neuromorphic signal processing platform. Target-induced conformational switching of DNA aptamers dynamically modulates ionic transport through nanochannels, effectively mimicking synaptic information transmission. The integration of cross-responsive aptamer-based APM units into a cascaded logic system enables signal processing without relying on the physical series network of nanochannels. By independently addressing and reading each unit, dendritic multi-input integration and brain-like information fusion are achieved at the signal-algorithm level, and 100% accurate discrimination of multiple targets is reached. This approach marks a conceptual shift from the traditional “one-probe-one-target” model toward a brain-inspired, multitarget recognition architecture. The fusion of DNA probes with nanofluidic logic and their cascade at the signal level enables the development of neuromorphic biochips with integrated processing capabilities for multiplexed signals.
利用离子作为信号载体的生物启发纳米流体系统在模拟生化传感和神经形态计算中的神经处理方面具有很大的前景。然而,实现多个生化信号的并行、类脑处理仍然是一个重大挑战。在此,我们提出了一种纳米流体人工突触后膜(APM),用受限的DNA适体功能化,以构建一个神经形态信号处理平台。靶诱导的DNA适体构象转换动态调节离子通过纳米通道的传输,有效地模拟突触信息传递。基于适配体的交叉响应APM单元集成到级联逻辑系统中,使信号处理不依赖于纳米通道的物理系列网络。通过对每个单元的独立寻址和读取,在信号算法层面实现了树突多输入集成和类脑信息融合,实现了对多个目标的100%准确识别。这种方法标志着从传统的“一个探针-一个目标”模型向大脑启发的多目标识别体系结构的概念转变。DNA探针与纳米流体逻辑的融合及其在信号水平上的级联使得具有多路信号综合处理能力的神经形态生物芯片的发展成为可能。
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引用次数: 0
Salt-Free Glycine Electrosynthesis via Carbon–Nitrogen Coupling Boosted by the Lattice Strain in Atomically Thin p-Block Bismuthene 原子薄p-嵌段铋晶格应变促进碳氮耦合电合成无盐甘氨酸
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c19472
Minghong Huang,Sheng-Hua Zhou,Cheng-Jie Yang,Chung-Li Dong,Lei Jiao,Dong-Dong Ma,Qi-Long Zhu,Zhenguo Huang
Electrochemical carbon–nitrogen (C–N) coupling using simple inorganic feedstocks offers a sustainable route to valuable organonitrogen compounds such as amino acids. Herein, we present an atomically thin and acid-resistant p-block bismuthene (Bi-ene) derived via the reconstruction of a Bi-based metal–organic framework, where the enriched atomic misarrangement induces significant lattice strain that modulates the local electronic structure of the resultant Bi-ene, significantly boosting its electrocatalytic activity. Such defective Bi-ene exhibits an exceptional electrocatalytic performance for reductive C–N coupling in a salt-free acidic system, achieving a Faradaic efficiency (FE) of 95.7% and an ultrahigh yield rate of 1161 μmol cm–2 h–1 for NH2OH generation via the nitrate reduction reaction (NtrRR). Further, the efficient coreduction of HNO3 and oxalic acid (OA) over Bi-ene simultaneously generates NH2OH and glyoxylic acid (GX) respectively, which undergo effective C–N coupling to produce glycine with a high yield of 455.4 μmol cm–2 h–1. Moreover, the Bi-ene demonstrates stable performance for over 120 h at an industrial-relevant current density of 200 mA cm–2. Operando spectroscopy and calculations reveal that the strain in lattice-distorted Bi-ene optimizes the intermediate adsorption through modulating local electronic structure and thus enhances the efficacy for glycine electrosynthesis.
电化学碳氮(C-N)偶联使用简单的无机原料提供了一个可持续的途径有价值的有机氮化合物,如氨基酸。在此,我们提出了一种原子薄且耐酸的p-嵌段铋(Bi-ene),通过重建bi基金属有机框架,其中富集的原子错排引起显著的晶格应变,从而调节所得Bi-ene的局部电子结构,显著提高其电催化活性。该缺陷双烯在无盐酸性体系中对还原性C-N偶联具有优异的电催化性能,通过硝酸盐还原反应(NtrRR)生成NH2OH的法拉第效率(FE)达到95.7%,产率高达1161 μmol cm-2 h-1。此外,HNO3和草酸(OA)在双烯上有效共还原,分别生成NH2OH和乙醛酸(GX),并通过有效的C-N偶联生成甘氨酸,产率高达455.4 μmol cm-2 h-1。此外,在工业相关的200 mA cm-2电流密度下,Bi-ene表现出超过120小时的稳定性能。Operando光谱和计算结果表明,晶格畸变双烯中的应变通过调节局部电子结构来优化中间吸附,从而提高了甘氨酸电合成的效率。
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引用次数: 0
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