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Functionalization of separator with two-dimensional anionic nanosheets for interfacial regulation of lithium deposition in lithium metal batteries. 二维阴离子纳米片功能化隔膜对锂金属电池中锂沉积界面调控的研究。
IF 9.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2027-01-15 Epub Date: 2026-09-01 DOI: 10.1016/j.jcis.2026.141500
Ying Zhang, Yuqin Wang, Xiaoyang Zheng, Guanyao Wang, Jinlong Jiang, Sikandar Iqbal, Xianzhong Yang, Haoxuan Liu, Chao Wu

Lithium metal anodes suffer from dendrite growth, low coulombic efficiency, and safety concerns, limiting their practical application in rechargeable batteries. Herein, polypropylene (PP) separators are functionalized with ultrathin 2D anionic (H3Sb3P2O14) HSPO nanosheets to construct a negatively charged interfacial layer. The HSPO layer improves electrolyte affinity, increases the Li+ transference number from 0.5 to 0.8, and guides a more homogeneous Li+ flux toward the lithium metal surface. Density functional theory calculations indicate stronger interactions between HSPO and Li/electrolyte species than those on pristine PP, while finite-element simulations and in situ optical microscopy reveal a more uniform electric-field distribution and regulated lithium deposition process. As a result, Li||Cu cells show improved plating/stripping stability over 250 cycles, and the Li||Li symmetric cell achieves a sevenfold increase in lifespan. Notably, the interfacial regulation strategy enables exceptional full-cell durability, delivering 2000 cycles for Li||LiFePO4 at 1C and 12,000 cycles for Li||I2 at 5C. This work highlights charged two-dimensional nanosheets as interfacial modifiers for separator-mediated regulation of ion transport and lithium deposition.

锂金属阳极存在枝晶生长、库仑效率低和安全性问题,限制了其在可充电电池中的实际应用。本文采用超薄二维阴离子(H3Sb3P2O14) HSPO纳米片功能化聚丙烯(PP)隔板,构建带负电荷的界面层。HSPO层提高了电解质亲和力,将Li+转移数从0.5提高到0.8,并引导更均匀的Li+通量向锂金属表面移动。密度泛函数理论计算表明HSPO与Li/电解质之间的相互作用比原始PP更强,而有限元模拟和原位光学显微镜显示HSPO与Li/电解质之间的电场分布更均匀,锂沉积过程更有规律。结果表明,Li||Cu电池在250次循环中表现出更好的镀/剥离稳定性,而Li||Li对称电池的寿命延长了7倍。值得注意的是,这种界面调节策略可以实现出色的全电池耐久性,在1C条件下,Li b| |LiFePO4循环2000次,在5C条件下,Li||I2循环12000次。这项工作强调带电的二维纳米片作为离子传输和锂沉积的分离器介导调节的界面调节剂。
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引用次数: 0
Preparation of an organic-copper composite modified layer via displacement reaction on zinc anode. 锌阳极上置换反应制备有机铜复合改性层。
IF 9.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2027-01-15 Epub Date: 2026-09-04 DOI: 10.1016/j.jcis.2026.141536
Teng Yu, Meiting Fu, Mengyu Liu, Zhen Hong, Wenxiang Sun, Haojie Liang, Lei Wang, Qi Sun, Caixia Li

Aqueous zinc-ion batteries face severe challenges in practical cycling, mainly including irregular zinc dendrite growth and unstable interfacial reactions, which greatly degrade the cycling performance. Herein, via a facile immersion method relying on a one-step in-situ spontaneous displacement reaction, an organic-inorganic composite layer composed of organic components and copper nanoparticles are fabricated on the surface of the zinc metal anode. The upper layer is enriched with carboxyl groups and Cu2+, constructing the upper layer by coordination interactions. Acting as migration sites and transport pathways for Zn2+, the as-formed SEI layer induces the uniform and ordered deposition of zinc. The bottom layer is composed of zincophilic copper clusters, which can form a compact physical shielding layer on the zinc anode surface and effectively inhibit interfacial corrosion. Benefiting from the synergistic effect, the symmetric cell achieves an ultra-long cycle life of over 4000 h at 3 mA cm-2, and still maintains a cycle life exceeding 2000 h even at a high current density of 10 mA cm-2. Meanwhile, the Cu-BTC@Zn//MVO full battery exhibits a 57% increase in capacity retention compared with bare Zn anode after 700 cycles. Meanwhile, this work reveals the synergistic regulation mechanism of the organic-inorganic composite layer toward Zn deposition, and provides a facile and practical strategy to construct stable artificial SEI layers for high performance zinc-metal anodes.

水性锌离子电池在实际循环中面临着严峻的挑战,主要是锌枝晶生长不规则和界面反应不稳定,大大降低了循环性能。本研究通过依靠一步原位自发位移反应的易浸法,在锌金属阳极表面制备了由有机组分和铜纳米颗粒组成的有机-无机复合层。上层富含羧基和Cu2+,通过配位相互作用构建上层。形成的SEI层作为Zn2+的迁移位点和运输通道,诱导锌均匀有序的沉积。底层由亲锌铜团簇组成,可在锌阳极表面形成致密的物理屏蔽层,有效抑制界面腐蚀。得益于协同效应,对称电池在3ma cm-2下可实现超过4000 h的超长循环寿命,即使在10ma cm-2的高电流密度下仍能保持超过2000 h的循环寿命。与此同时,Cu-BTC@Zn//MVO电池经过700次循环后,其容量保持率比裸锌阳极提高了57%。同时,本研究揭示了有机-无机复合层对锌沉积的协同调控机制,为构建稳定的人工SEI层制备高性能锌金属阳极提供了一种简便实用的策略。
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引用次数: 0
A ratiometric fluorescence sensor based on integrated bimetallic Zr/Eu-MOF for rapid and visual detection of glyphosate. 基于集成双金属Zr/Eu-MOF的比例荧光传感器用于草甘膦的快速和视觉检测。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-07-15 DOI: 10.1016/j.talanta.2026.130308
Haojie Shi, Wei Wang, Haoyu Shi, Liangang Mao, Lan Zhang, Lizhen Zhu, Chi Wu, Xingang Liu

The widespread use of glyphosate in agriculture has raised concerns about environmental contamination and associated health risks, creating an urgent need for rapid, sensitive, and field-deployable analytical tools. In this work, Zr/Eu-metal-organic framework (Zr/Eu-MOFs) as an integrated bimetallic ratiometric fluorescent hydrogel sensor for fast and highly sensitive visual detection of glyphosate has been developed. By doping Eu3+ into a robust Zr-based MOF framework, Zr/Eu-MOFs exhibit dual-emission bands at 445 and 618 nm, enabling an intrinsic self-referenced signal without multicomponent assembly. Upon glyphosate addition, the sensor responds within 10 s. Zr/Eu-MOFs display a reliable ratiometric response over 0.05 - 10.0 mg/L with a low detection limit of 0.03 mg/L (0.2 μmol/L), which is far below the permissible maximum residue limit (MRL) for drinking water by the US EPA and China (4.1 μmol/L). Mechanistic evidence indicates that glyphosate forms P-O-Zr coordination linkages and interfacial interactions which modulate the ligand-to-metal charge transfer (LMCT) process, resulting in an enhanced ratiometric fluorescence response at 445 nm, while the Eu3+ emission at 618 nm remains essentially unchanged. Moreover, an agarose hydrogel format coupled with smartphone image analysis enables rapid visual detection. A spraying-enabled fluorescence imaging strategy further allows rapid screening of glyphosate contamination on leaves, apple surfaces, and soil-water matrices under UV illumination. Overall, this work provides a facile, integrated, and visually readable ratiometric platform for on-site glyphosate monitoring.

草甘膦在农业中的广泛使用引起了人们对环境污染和相关健康风险的关注,迫切需要快速、敏感和可在现场部署的分析工具。Zr/Eu-metal-organic framework (Zr/Eu-MOFs)是一种集成的双金属比例荧光水凝胶传感器,用于快速、高灵敏度的草甘膦视觉检测。通过将Eu3+掺杂到稳健的Zr基MOF框架中,Zr/ eu -MOF在445和618 nm处呈现双发射带,实现了无需多组件组装的内在自参考信号。添加草甘膦后,传感器在10 s内响应。Zr/Eu-MOFs在0.05 ~ 10.0 mg/L范围内具有可靠的比例响应,低检出限为0.03 mg/L(0.2 μmol/L),远低于美国EPA和中国饮用水允许的最大残留限量(4.1 μmol/L)。机理证据表明,草甘膦形成P-O-Zr配位键和界面相互作用,调节了配体到金属的电荷转移(LMCT)过程,导致445 nm处的比例荧光响应增强,而618 nm处的Eu3+发射基本保持不变。此外,琼脂糖水凝胶格式与智能手机图像分析相结合,可实现快速视觉检测。喷雾荧光成像策略进一步允许在紫外线照射下快速筛选叶片、苹果表面和土壤-水基质上的草甘膦污染。总的来说,这项工作为现场草甘膦监测提供了一个方便、综合、直观可读的比率测量平台。
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引用次数: 0
Autocatalytic DNA cascade circuits via split-triggered recombination for ultrasensitive programmable nucleic acid detection. 自催化DNA级联电路通过分裂触发重组超灵敏的可编程核酸检测。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-07-07 DOI: 10.1016/j.talanta.2026.130262
Shanshan Tao, Suqin Wang, Songbai Zhang, Hongbo Li, Ruqin Yu

Accurate detection of microRNAs is of great significance for the clinical diagnosis and therapeutic guidance of cancer. Herein, we have established an isothermal self-catalytic DNA circuit that can combine an autocatalytic hairpin assembly (ACHA) converter with autocatalytic hybridization chain reaction (AHCR) amplification for the sensitive detection of miRNA-21. HCR is initiated by the recognition of the target analyte, generating new trigger strands that subsequently activate the CHA amplifier. One terminus of the CHA amplifier is engineered to expose the identical HCR initiator sequence, thereby enabling sustained HCR propagation. The DNAzyme moiety at the opposite terminus functions as a fluorescent signal reporter, efficiently cleaving the fluorogenic reporter probe. Therefore, the self-catalytic feedback loop between the HCR and CHA systems allows trace targets to produce fluorescence signals with exponential amplification. This circuit conducted a sensitive, reliable and universal analysis of miRNA-21, with a detection limit of 33.4 fM. Self-feedback cascade circuits provide a promising tool for molecular sensing in complex biological environments, this cascaded circuit can be used for the analysis of miRNA-21 in human serum samples. It has broad application prospects in low-abundance biomolecular sensing and early diagnosis of diseases.

microrna的准确检测对癌症的临床诊断和治疗指导具有重要意义。在此,我们建立了一个等温自催化DNA电路,该电路可以将自催化发夹组装(ACHA)转换器与自催化杂交链反应(AHCR)扩增相结合,以灵敏地检测miRNA-21。HCR由目标分析物的识别开始,产生新的触发链,随后激活CHA放大器。CHA放大器的一个末端设计为暴露相同的HCR启动器序列,从而使持续的HCR传播成为可能。相反末端的DNAzyme片段作为荧光信号报告者,有效地切割荧光报告者探针。因此,HCR和CHA系统之间的自催化反馈回路允许痕量目标产生具有指数放大的荧光信号。该电路对miRNA-21进行了灵敏、可靠、通用的分析,检测限为33.4 fM。自反馈级联电路为复杂生物环境中的分子传感提供了一种很有前途的工具,这种级联电路可用于分析人血清样品中的miRNA-21。在低丰度生物分子传感和疾病早期诊断方面具有广阔的应用前景。
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引用次数: 0
Synchronous modulation of fluorescence and oxidase-mimicking activity in a Mn-based MOF nanozyme via post-synthetic metal exchange for Cu2+ sensing. 基于合成后金属交换的锰基MOF纳米酶的荧光和氧化酶模拟活性同步调制
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-07-11 DOI: 10.1016/j.talanta.2026.130300
Linying Cheng, Xiang Liu, Zixin Zhang, Jing Liu, Jianru Tang, Xiaohua Zhu, Youyu Zhang, Meiling Liu

Copper ions (Cu2+) are essential micronutrients but become hazardous when accumulated in excess, necessitating reliable, sensitive, and field-deployable detection methods. Herein, we report a fluorescent Mn-based MOF nanozyme (Mn-TCPP) that exhibits intrinsic oxidase-like activity, capable of catalyzing the oxidation of non-fluorescent o-phenylenediamine (OPD) to fluorescent 2,3-diaminophenazine (DAP) with an emission peak at 560 nm, while the Mn-TCPP itself displays characteristic fluorescence at 655 nm. Upon exposure to Cu2+, the stronger affinity of Cu2+ toward the porphyrinic TCPP ligand displaces Mn2+ from the framework, forming Cu-TCPP. This metal-exchange process simultaneously quenches the 655 nm fluorescence of the MOF and attenuates its oxidase-mimicking activity, whereas free Cu2+ in solution independently catalyzes OPD oxidation, further enhancing the 560 nm emission. Leveraging this dual-response mechanism, we develop a ratiometric fluorescence sensing strategy for Cu2+ detection based on the intensity ratio F560/F655. The calibration curve follows a linear equation: F560/F655 = 0.201x-0.001 (0.2-10 μM, R2 = 0.985) and y = 0.002x+2.061 (10-100 μM, R2 = 0.994) with the limit of detection (LOD) of 81 nM (S/N = 3). The sensor exhibits excellent selectivity over competing metal ions, and the method reliability is validated by standard addition recovery experiments in real water and rice samples. Furthermore, the Mn-TCPP nanozyme is embedded into an agarose hydrogel matrix, enabling visual, instrument-free monitoring of Cu2+ contamination: increasing Cu2+ concentrations induce a discernible fluorescence color transition from orange to yellow under 365 nm illumination. This work presents a tunable MOF platform that exploits competitive targets synchronous modulation of fluorescence and enzyme-mimicking activity, providing a robust, selective, and field-deployable ratiometric sensor for Cu2+.

铜离子(Cu2+)是必需的微量营养素,但当积累过量时就会变得危险,因此需要可靠、敏感和可现场部署的检测方法。本文中,我们报道了一种荧光锰基MOF纳米酶(Mn-TCPP),它具有内在的类似氧化酶的活性,能够催化非荧光邻苯二胺(OPD)氧化为荧光2,3-二氨基苯二嗪(DAP),其发射峰位于560 nm,而Mn-TCPP本身在655 nm处显示特征荧光。暴露于Cu2+后,Cu2+对卟啉型TCPP配体的亲和力较强,从框架中取代Mn2+,形成Cu-TCPP。这种金属交换过程同时淬灭了MOF的655 nm荧光,并减弱了其模拟氧化酶的活性,而溶液中的游离Cu2+独立催化OPD氧化,进一步增强了560 nm的发射。利用这种双响应机制,我们开发了一种基于强度比F560/F655的Cu2+检测比例荧光传感策略。校准曲线遵循线性方程:F560 / F655 = 0.201 x - 0.001(0.2 -10 μM, R2 = 0.985) x和y = 0.002 + 2.061(10 - 100 μM, R2 = 0.994)的检测极限(LOD) 81 海里 (S / N = 3)。该传感器对竞争金属离子具有良好的选择性,并通过实际水和大米样品的标准添加回收率实验验证了该方法的可靠性。此外,Mn-TCPP纳米酶被嵌入琼脂糖水凝胶基质中,实现了对Cu2+污染的可视化、无仪器监测:在365 nm照明下,增加Cu2+浓度可诱导从橙色到黄色的可识别荧光颜色转变。这项工作提出了一个可调的MOF平台,该平台利用荧光和酶模拟活性的竞争性靶标同步调制,为Cu2+提供了一个强大的、选择性的、可现场部署的比率传感器。
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引用次数: 0
Triphase interface engineering in bilayer aerogels for highly efficient water evaporation and photothermal-photocatalytic hydrogen peroxide production. 用于高效水蒸发和光热-光催化过氧化氢生产的双层气凝胶三相界面工程。
IF 9.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2027-01-01 Epub Date: 2026-09-05 DOI: 10.1016/j.jcis.2026.141523
Yuancheng Ji, Yan Zhu, Yang Yang, Yijie Xu, Chunyu Qi, Yan Li, Shuangjiang Yu, Junqiu Liu, Hongcheng Sun

Solar-driven photocatalytic oxygen reduction offers a sustainable route for hydrogen peroxide (H2O2) production. However, this process is often limited by the high energy barrier for hydrogen extraction from water, low oxygen solubility and diffusion, and poor selectivity for the two-electron oxygen reduction reaction (ORR), especially under alkaline conditions. Herein, we reported a synergistic photothermal-photocatalytic bilayer aerogel constructed with konjac glucomannan to integrate a photothermal lower layer of reduced graphene oxide (rGO) and a catalytic upper layer of keto-form anthraquinone covalent organic framework (Kf-AQ-COF). Owing to its hydrophobic mesoporous structure, the bilayer aerogel forms a robust gas-liquid-solid triphase interface on a porous substrate. Under alkaline conditions, the hydroxide clusters adsorbed onto ketone moieties can drive the anthraquinone-anthrahydroquinone cycle of Kf-AQ-COF for enabling electron transfer and H2O2 production. Meanwhile, the underlying rGO layer functions primarily as a localized photothermal converter and lightweight structural matrix, raising the interfacial temperature to accelerate reaction kinetics and driving rapid vapor escape without altering the intrinsic band structure of the top photocatalyst. As a result, this photothermal-synergistic triphase interface achieves an H2O2 production rate of 15.0 mmol m-2∙h-1 under air without sacrificial agents within 60 min, which is 1.43 times that of the conventional solid-liquid diphase system. This work demonstrates a new photocatalytic strategy integrating molecular reaction regulation with interfacial engineering.

太阳能驱动的光催化氧还原为过氧化氢(H2O2)的生产提供了一条可持续的途径。然而,该工艺往往受到从水中提取氢的高能垒、低氧溶解度和低氧扩散以及双电子氧还原反应(ORR)选择性差的限制,特别是在碱性条件下。本文中,我们报道了一种由魔芋葡甘露聚糖构建的协同光热-光催化双层气凝胶,该气凝胶集成了光热下层的还原氧化石墨烯(rGO)和催化上层的酮型蒽醌共价有机框架(Kf-AQ-COF)。由于其疏水介孔结构,双层气凝胶在多孔基底上形成坚固的气-液-固三相界面。在碱性条件下,吸附在酮基上的氢氧化物团簇可以驱动Kf-AQ-COF的蒽醌-蒽对苯二酚循环,从而实现电子转移和H2O2的生成。同时,底层氧化石墨烯层主要作为局部光热转换器和轻质结构基质,在不改变顶部光催化剂固有能带结构的情况下,提高界面温度以加速反应动力学和驱动快速蒸汽逸出。结果表明,该光热-协同三相界面在无牺牲剂的空气条件下,60 min内H2O2产率达到15.0 mmol m-2∙h-1,是常规固液两相体系的1.43倍。这项工作展示了一种结合分子反应调控和界面工程的光催化新策略。
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引用次数: 0
A gelatinase-responsive cascade microfluidic chemiluminescence assay for ultrasensitive detection of drug-resistant bacteria and antibiotic susceptibility. 明胶酶反应级联微流控化学发光试验用于耐药细菌和抗生素敏感性的超灵敏检测。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-07-11 DOI: 10.1016/j.talanta.2026.130291
Xueming Zhu, Wenchao Zhu, Bing Fan, Meng Gao, Dan Gao

Antibiotic-resistant bacterial infections pose a global health crisis, driving the need for innovative diagnostic approaches. Conventional methods for detecting resistant strains and antibiotic susceptibility testing (AST) are often limited by long assay times, low sensitivity, and operational complexity. Herein, a novel gelatinase-responsive cascade microfluidic chemiluminescence (CL) biosensor was developed for ultrasensitive detection of gelatinase-producing bacteria, with phenotypic AST validated using Staphylococcus aureus (S. aureus) as the model pathogen. Peptide-DNA probes were designed to respond to gelatinase secreted by bacteria remain metabolically active following antibiotic exposure. Bacterial gelatinase cleaves peptides to release initiator single-stranded DNA (ssDNA), triggering hybridization chain reaction (HCR) amplification in micropillar-structured microchannels. Through streptavidin-biotin interaction, poly-horseradish peroxidase (poly-HRP) is anchored in the channel to catalyze luminol based CL. This biosensor achieves high specificity and sensitivity, with a detection limit of 15 CFU/mL, which is better or comparable to previously reported biosensors. Moreover, the potential clinical applicability of this platform is further verified by testing four clinical S. aureus strains against five antibiotics, yielding 95% categorical agreement rate with standard AST methods. The area under the receiver operating characteristic ROC curve (AUC) was 0.944, close to the ideal value of 1, indicating excellent diagnostic performance for AST. The assay time from isolated colonies to AST result takes approximately 4-5 h. Featuring portability and low cost, the platform enables universal bacterial AST, providing a reliable tool for precise antimicrobial therapy and antimicrobial resistance control.

耐抗生素细菌感染构成了全球健康危机,推动了对创新诊断方法的需求。检测耐药菌株和抗生素敏感性试验(AST)的传统方法通常受测定时间长、灵敏度低和操作复杂性的限制。本研究开发了一种新型的明胶酶反应级联微流控化学发光(CL)生物传感器,用于明胶酶产生菌的超灵敏检测,并以金黄色葡萄球菌(S. aureus)为模型病原体对AST进行了表型验证。肽- dna探针被设计用于响应细菌分泌的明胶酶,在抗生素暴露后保持代谢活性。细菌明胶酶裂解多肽,释放引发单链DNA (ssDNA),在微柱结构的微通道中触发杂交链反应(HCR)扩增。通过链亲和素-生物素相互作用,多辣根过氧化物酶(polyhrp)锚定在通道中催化鲁米诺基CL。该生物传感器具有较高的特异性和灵敏度,检测限为15 CFU/mL,优于或可与先前报道的生物传感器相媲美。此外,通过对4种临床金黄色葡萄球菌菌株对5种抗生素的检测,进一步验证了该平台的潜在临床适用性,与标准AST方法的分类符合率为95%。受试者工作特征ROC曲线下面积(AUC)为0.944,接近理想值1,表明AST诊断效果良好。从分离菌落到AST结果的检测时间约为4-5 h。该平台具有便携性和低成本的特点,可实现通用细菌AST,为精确抗菌治疗和抗菌药物耐药性控制提供可靠的工具。
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引用次数: 0
Corrigendum to "Magnetic nanoparticles amplification-based terahertz and fluorescence dual-mode assays for efficient isolation and sensitive detection of circulating tumor cells" [Talanta 298 (2026) 128894]. “基于磁性纳米粒子扩增的太赫兹和荧光双模式检测用于有效分离和敏感检测循环肿瘤细胞”的更正[Talanta 298(2026) 128894]。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-08-22 DOI: 10.1016/j.talanta.2026.130463
Yi Zhou, Mei Xin, Ling Liang, Fengxin Xie, Huiyan Tian, Weidong Jin, Yitong Ren, Jia Shi, Ke Yang, Xiang Yang
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引用次数: 0
Ce-doped ZnO upconversion nanoparticles for optical thermometry, antibacterial therapy, and cardiac biomarker detection. 用于光学测温、抗菌治疗和心脏生物标志物检测的ce掺杂ZnO上转换纳米颗粒。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2027-01-01 Epub Date: 2026-07-08 DOI: 10.1016/j.talanta.2026.130277
Yuemei Li, Yongmei Li

Lanthanide-doped upconversion nanoparticles (UCNPs) due to their unique optical properties are promising for applications ranging from bioimaging to biosensing. However, their practical implementation remains challenging owing to relatively low luminescence efficiency. Herein, we synthesize a series of Ce-doped Yb/Eu/ZnO, Yb/Er/ZnO and Yb/Tm/ZnO UCNPs via a hydrothermal method. Ce ions incorporation promotes anisotropic growth, which increases surface roughness and modulates the local coordination environment. Electrochemical impedance spectroscopy and Tafel plot analyses reveal that Ce doping significantly enhances charge separation and transfer kinetics. Ce ion doping markedly increases the emission intensities of Eu3+, Er3+ and Tm3+, attributed to the formation of Yb3+ dimers and efficient energy transfer under 980 nm excitation. Benefiting from these improvements, the Ce-doped ZnO UCNPs exhibit three distinct bio-applications: (i) superior low-temperature optical thermometry with a maximum relative sensitivity of 4.81% K-1 at 80 K; (ii) excellent antibacterial activity against S. aureus and E. coli (up to 82.16% and 87.64% inhibition at 8 mol% Ce); and (iii) successful employment as luminescent probes in a multiplex immunoassay for the cardiac markers BNP (detection range 10-100 pg/mL) and ST2 (5-25 ng/mL), with high specificity and sensitivity. These findings underscore the potential of Ce-doped ZnO UCNPs as multifunctional platforms for optical thermometry, antibacterial therapy and biomedical diagnostics.

镧系掺杂上转换纳米粒子(UCNPs)由于其独特的光学特性,在从生物成像到生物传感等领域有着广阔的应用前景。然而,由于相对较低的发光效率,它们的实际实施仍然具有挑战性。本文采用水热法合成了一系列ce掺杂的Yb/Eu/ZnO、Yb/Er/ZnO和Yb/Tm/ZnO UCNPs。Ce离子的加入促进了各向异性生长,增加了表面粗糙度并调节了局部配位环境。电化学阻抗谱和Tafel图分析表明,Ce掺杂显著提高了电荷分离和转移动力学。Ce离子掺杂显著提高了Eu3+、Er3+和Tm3+的发射强度,这是由于Yb3+二聚体的形成和980 nm激发下的高效能量转移。得益于这些改进,ce掺杂ZnO UCNPs表现出三种不同的生物应用:(i)优越的低温光学测温性能,在80 K时的最大相对灵敏度为4.81% K-1;(ii)对金黄色葡萄球菌和大肠杆菌具有良好的抑菌活性(8 mol% Ce时抑菌率分别为82.16%和87.64%);(iii)作为发光探针成功应用于心脏标志物BNP(检测范围10-100 pg/mL)和ST2(5-25 ng/mL)的多重免疫分析,具有高特异性和敏感性。这些发现强调了ce掺杂ZnO UCNPs作为光学测温、抗菌治疗和生物医学诊断的多功能平台的潜力。
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引用次数: 0
Coupling lattice distortion with electronic states in highly crystalline LDHs for efficient piezocatalytic conversion of low-concentration CO2. 高结晶LDHs中晶格畸变与电子态的耦合用于低浓度CO2的高效压催化转化。
IF 9.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2027-01-01 Epub Date: 2026-09-06 DOI: 10.1016/j.jcis.2026.141537
Dingyu Qiu, Yaning Gong, Xingchen He, Junhui Shao, Najun Li, Dongyun Chen, Hua Li, Qingfeng Xu, Jianmei Lu

The restricted conversion of low-concentration CO2 in industrial flue gas and the structural degradation inherent in traditional defect engineering remain key challenges in piezocatalysis. In this work, highly crystalline Co-substituted MgAl-LDH nanosheets were constructed via isomorphous substitution. The atomic-level incorporation breaks the structural centrosymmetry through local lattice distortion. Consequently, it bolsters the piezoelectric built-in electric field to accelerate charge carrier separation. Simultaneously, the Co active sites optimize the interfacial d-band center, strengthen the specific adsorption of CO2, and substantially lower the energy barrier for the rate-determining step (⁎COOH formation). The strong coupling between the polarization-induced electric field and interfacial reaction kinetics lets 5% Co-MgAl-LDH outperform pristine MgAl-LDH by roughly 5.7-fold. At 25 °C under a 10% CO2 atmosphere, 5%Co-MgAl-LDH achieves CO and H2 production rates of 5542.8 and 3266.2 μmol g-1 h-1, respectively, corresponding to a CO/H2 molar ratio of approximately 1.7:1. Together, local lattice distortion and interfacial electronic-state modulation account for this performance within an otherwise highly crystalline framework, pointing to a workable route for catalysts aimed at low-concentration CO2 conversion.

工业烟气中低浓度CO2转化受限以及传统缺陷工程固有的结构退化问题仍然是压电催化的主要挑战。在这项工作中,通过同构取代构建了高结晶性的MgAl-LDH纳米片。原子水平的掺入通过局部晶格畸变破坏了结构的中心对称性。因此,它增强了压电内置电场来加速载流子的分离。同时,Co活性位点优化了界面d带中心,增强了对CO2的比吸附,并大大降低了速率决定步骤(COOH形成)的能垒。极化诱导电场和界面反应动力学之间的强耦合使得5% Co-MgAl-LDH的性能比原始MgAl-LDH高出约5.7倍。在25℃、10% CO2气氛下,5%Co-MgAl-LDH的CO和H2产率分别为5542.8和3266.2 μmol g-1 h-1, CO/H2的摩尔比约为1.7:1。局部晶格畸变和界面电子态调制共同解释了在高度结晶框架内的这种性能,为低浓度二氧化碳转化的催化剂指明了一条可行的途径。
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