ACS Omega
·
2026
·
IF 5.2
Zhaobo Hu,Yan Guo,Peishuo Cao,Keyan Wei,Zongjie Ma,Boxin Li,Dong Li,Liang Zhou,Chang-ye Hui
Abstract This work presents an engineered single-plasmid, dual-pigment whole-cell biosensor for simultaneous colorimetric detection of Pb(II) and Hg(II). To address the challenge of signal interference in cocontaminated environmental samples, a Pb(II)-responsive PbrR regulatory module driving indigo biosynthesis (blue, 620 nm) and an Hg(II)-responsive MerR module driving deoxyviolacein biosynthesis (purple, 570 nm) were integrated into Escherichia coli TOP10. The orthogonal decoupling of the two pigment pathways, combined with a unified 10 h induction protocol, enables independent chromogenic readout of both metals from a single cultivation. Dose-response assays afforded a broad linear dynamic range for Pb(II) of 0.977–2000 μM (R2 = 0.9503) with a limit of detection (LOD) of 0.977 μM, alongside nanomolar sensitivity for Hg(II) with a linear range of 0.244–250 nM (R2 = 0.9800) and an LOD of 0.244 nM. A two-dimensional cross-concentration matrix experiment further demonstrated that the two detection channels maintain distinguishable dose-dependent responses under coexposure conditions, with crosstalk remaining within an acceptable range. Robust performance was retained in spiked surface water and seawater matrices, yielding Pb(II) LODs of 0.244 μM (surface water) and 0.488 μM (seawater), and Hg(II) LODs of 0.488 nM (surface water) and 0.977 nM (seawater). These detection limits approach or fall below relevant environmental regulatory thresholds, including the Class III surface-water standard for Hg(II). This self-contained, instrument-free pigment-based approach enables naked-eye discrimination of both metals in a standard microplate assay, offering a low-cost, high-throughput screening platform that complements standard instrumental methods for on-site environmental monitoring and emergency pollution response.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Huihui Yang,Jun Chen,Yuling Liang,Yanfei Zhang,Wen Yin,Yuzhi Xu,Si-Yang Liu,Zong Dai,Xiaoyong Zou
Dynamic imaging of cell surface pH is extremely challenging due to the slight changes in pH and the fast diffusion of secreted acid to the extracellular environment. In this work, we construct a novel metal–organic framework (MOF)-shell-confined i-motif-based pH probe (MOFC-i) strategy that enables sensitive and dynamic imaging of cell surface pH. The CY3- and CY5-labeled i-motif, which is hybridized via its short complementary chain with two-base mismatches, is optimized for sensing at physiological pH. After efficiently anchoring the optimized pH probes onto the cell membrane with the aid of cholesterol groups, a biocompatible microporous MOF shell is then formed around the cell by cross-linking ZIF-8 nanoparticles via tannic acid. The microporous MOF shell can confine secreted acid without inhibiting the normal physiological activities of cells; thus, the MOFC-i strategy can be used to monitor dynamic changes in the cell surface pH of living cells. Furthermore, this method can not only clearly distinguish the different metabolic behaviors of cancer cells and normal cells but also reveal drug effects on the cell surface pH or metabolism, providing promising prospects in pH-related diagnostics and drug screening.
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 3
·2006839
·
IF 16.836
Bingbing Gao,Maoze Guo,Kai Lyu,Tianshu Chu,Bingfang He
Wounds, especially those caused by chronic diseases, are severe threats to human health. To facilitate their recovery, considerable efforts have been devoted to the generation of wound tissues and the detection of wound biomarkers. Here, an intelligent origami silk fibroin microneedle-structured dressing (i-SMD) with a smart drug release system, biochemical sensing, and physiological monitoring ability for epidermal sensing and wound healing, is presented. By utilizing temperature-responsive N -isopropylacrylamide (NIPAM) hydrogel and inverse opal (IO) photonic crystals (PCs) as a smart drug release system, controllable drug release is achieved on the i-SMD. The patterned microfluidic channels on the i-SMD and IO PCs enable the liquid to flow spontaneously in the channels, thereby achieving sensitive multiple biochemical analysis of inflammatory factors; meanwhile, microelectronic circuits integrated on the i-SMD enable sensitive motion monitoring. Notably, the performance of i-SMD in facilitating wound healing is demonstrated by treating full-thickness cutaneous wounds in a diabetic mouse model, indicating the remarkable prospects of i-SMD in wound management and other related biomedical fields.
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NUCLEIC ACIDS RESEARCH
·
2025
·Vol. 53
·期 12
·
IF 13.1
Luo Tengshuo,Guan Ziyue,Liu Yunlong,Zhou Jun,Mergny Jean-Louis,Cheng Mingpan
A molecular beacon (MB) is an oligonucleotide probe with a stem-loop structure designed to fluoresce upon hybridization with a specific target nucleic acid. Herein, we introduce a novel i-motif DNA-based molecular beacon (iMB) designed for nucleic acid detection. DNA chemical sequencing showed that the iMB can be selectively opened when its target is present, thanks to the formation of a duplex between this target and the iMB recognition loop. Phase diagrams were introduced to analyze the binding properties between the iMB and its target, and to optimize the detection conditions with different combinations of pH and temperature. Benefiting from the environment-sensitive stability and special structural feature inherent to the i-motif, this iMB exhibits a controllable sensitivity and specificity through choosing appropriate temperature/pH combination and recognition loop position in the i-motif probe. Leveraging the duplex-specific nuclease (DSN) resistance of the i-motif, we significantly enhanced the sensitivity by more than four orders of magnitude through the implementation of a DSN-assisted amplification strategy. Finally, miRNAs in cell lines and patient plasma were detected by the iMBs, as validated via quantitative reverse transcription polymerase chain reaction (RT-qPCR). This research successfully broadens the structural repertoire of MB stems to include a pH- and temperature-responsive i-motif stem.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2026
·
IF 6.7
Jiawen Yu,Kunying Chen,Yujing Zhang,Xujie Wang,Yangchun Shen,Yu Deng,Xingtao Zhou
Abstract Modulating intestinal macrophage polarization is critical for maintaining intestinal barrier integrity. Our previous study demonstrated that glucomannan from Aloe vera gel (AGP) improved the intestinal barrier, yet its direct impact on intestinal macrophages remained undefined. Here, we demonstrated that AGP reduced M1 macrophage infiltration in colonic tissue. Integrated serum untargeted metabolomics identified lactic acid as a key AGP-induced metabolite, with 16S rRNA sequencing pointing to the gut microbiota as its potential source. Mechanistically, lactic acid suppressed M1 polarization by inhibiting the mechanosensitive cation channel Piezo1, thereby attenuating calcium influx, concurrently dampening STAT3 activation and ROS production─core drivers of M1 commitment. Critically, these effects were abrogated by a Piezo1 agonist, confirming the centrality of the lactic acid–Piezo1–Ca2+ axis. Collectively, our study defines a novel immunometabolic pathway wherein AGP fortifies the intestinal barrier through microbiota-derived lactic acid, which restrains macrophage M1 polarization via the lactic acid–Piezo1–calcium axis.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaoyu Hu,Fengyun Ding,Renjin Xiong,Yongtao An,Xingwen Feng,Jiangfeng Song,Linsen Zhou,Peilong Li,Changlun Chen
Realizing ideal deuterium separation from isotopic mixtures remains a daunting challenge because of their almost identical sizes, shapes, and physicochemical properties. Using the quantum sieving effect in porous materials with suitable pore size and open metal sites (OMSs) enables efficient hydrogen isotope separation. Herein, synthetic HKUST-1-derived microporous mixed-valence Cu(I)Cu(II)-BTC (BTC = benzene-1,3,5-tricarboxylate), featuring a unique network of distinct Cu(I) and Cu(II) coordination sites, can remarkably boost the D2/H2 isotope separation, which has a high selectivity (SD2/H2) of 37.9 at 30 K, in comparison with HKUST-1 and other porous materials. Density functional theory (DFT) calculations indicate that the introduction of Cu(I) macrocycles in the framework decreases the pore size and further leads to relatively enhanced interaction of H2/D2 molecules on Cu(II) sites. The significantly enhanced selectivity of Cu(I)Cu(II)-BTC at 30 K can be mainly attributed to the synergistic effect of kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS). The results reveal that Cu(I) OMSs exhibit counterintuitive behaviors and play a crucial role in tuning quantum sieving without a complex structural design, which provides a deeper insight into quantum sieving mechanisms and a new strategy for the intelligent design of highly efficient isotope systems.
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Advanced Materials Technologies
·
2026
·
IF 6
Wen Huang,Qishuo Li,Xin Zhang,Hengru Fei,Zhengjian Lin,Qifu Yao,Yong Yan,Xing'ao Li,Lei Wang,Xuegong Yu
The emerging vertically two-terminal optoelectronic synaptic devices have attracted significant attention due to their structural and performance advantages. However, most existing devices are limited to optically unidirectional modulation and suffer from restricted synaptic weight ranges and poor rectification characteristics, hindering their integration into neuromorphic systems. Here, a novel type-I two-terminal optoelectronic synaptic architecture based on an iodinated two-dimensional/three-dimensional (I-2D/3D) perovskite heterostructure is proposed. The devices demonstrate electrical-assisted monochromatic optically stimulated bidirectional synaptic behavior, enabled by ion migration, carrier trapping, and recombination effects. The incorporation of the I-2D perovskite layer yields an exceptional rectification ratio of 1 × 10 6 and significantly enhances the synaptic weight range to 34.4, outperforming previously reported perovskite-based counterparts. Bidirectional synaptic functions and their excellent performance metrics arise from the unique design of type-I I-2D/3D heterojunction that improves the carrier separation capability to an optimal balance state. Furthermore, the YOLOv8 model, constructed based on synaptic devices, achieves accuracy comparable to pure software models when recognizing the VOC2012 dataset and demonstrates real-time moving object detection in video streams, with average accuracies of 91%, 90%, and 89% for bicycles, persons, and cars, respectively. This work presents a novel strategy for bidirectional optoelectronic synapses, advancing their application in neuromorphic dynamic visual systems.
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Journal of Physical Chemistry Letters
·
2026
·Vol. 17
·期 33
·9746-9755
·
IF 4.5
Lan Zhineng,Wan Meng,Yan Huilin,Huang Hao,Liu Benyu,Lu Yi,Yang Yingying,Suo Yi,Zhang Guanzheng,Du Shuxian,Zhang Qiang,Wang Zhiwei,Jiang Tongtong,Sun Changxu,Qu Shujie,Yan Luyao,Cui Peng,Li Meicheng
Stability degradation plagues both
regular n-i-p and inverted p-i-n
perovskite solar cells (PSCs), with the organic hole transport layer
(HTL) constituting a key restricting factor. Poly(triarylamine) (PTAA)
possesses intrinsic polymer characteristics and excellent thermal
stability, rendering it a competitive candidate for high-performance
PSCs applicable to both device structures. However, challenging p-doping
procedures and vulnerability to humidity restrict its utilization.
Herein, we introduced a hydrophobic dilauroyl peroxide (DP) with oxidation
ability and a long-chain alkanes structure into the PTAA. Upon cleavage
of the peroxide bond (−O–O−) of DP, two decanoyl
free radicals are generated. These radicals seize the lone pair of
electrons on the N atom of the triarylamine in PTAA, oxidizing PTAA
into a positively charged radical PTAA •+ , thereby
achieving p-type doping of PTAA. This doping process enhances the
electrical properties and transport characteristics of PTAA. Besides,
the introduction of long-chain alkyl groups enhances the hydrophobicity
of the PTAA film, increasing the water contact angle from 60.18 °
to 80.39 ° . As a result, the champion PCE of n-i-p PSCs increased
from 23.49% to 24.82%, while that of p-i-n PSCs increased from 25.26%
to 26.04%. Moreover, the humidity stability and thermal stability
of the PSCs are enhanced. As a result, after the PSC aged for approximately
4752 h at 25 ° C and 45% relative humidity, it still maintained
97% of its initial PCE.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhongzhong Jia,Song Yin,Xudong Liu,Mingxuan Liu,Hua Zhong,Shi Chen,Luozheng Zhang,Shaopeng Yang,Weiguang Kong
The p-i heterojunction imbedded underneath the perovskite layer plays a vital role in determining the efficiency and stability of inverted perovskite solar cells (PSCs). We found that poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] (PTAA) suffers from the severely chain entanglement resulting in poor contact with perovskite. In this work, PTAA layer was treated by poly[(2,6-(4,8-bis(5-(2-ethylhexylthio)-4-fluorothiophen-2-yl)-benzo[1,2-b:4,5-b′] dithiophene))- alt -(5,5-(1′,3′-di-2-thienyl-5′,7′-bis(2-ethylhexyl) benzo[1′,2′-c:4′,5′-c′] dithiophene-4,8-dione)] (PBDB- T -SF) diluted solution in chlorobenzene . PBDB- T -SF, which contains dual carbonyl groups in its backbones and suitable electronic levels, can spontaneously fill the voids in chlorobenzene-washed PTAA (nano-PTAA). This not only promotes the work function of the substrate but also strengthens the coherence between perovskite and the substrate. Blade coated PSC (0.09 cm 2 ) containing PBDB- T -SF (s-PSCs) realized a power conversion efficiency (PCE) of 21.83 %. After aging for more than 2000 h, s-PSCs maintains 88 % of the initial efficiency which is only 59 % for the control devices.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 67
·e202201968
·
IF 5.02
Shujue Xu,Shen Zhang,Yang Yu,Shengrui Zhang,Minjie Li
Graphical Au(I)-thiolate nanosheets with closely-packed multiple surface functional groups have been synthesized via a one-pot co-assembly strategy. The easy but powerful strategy addresses the surface engineering problem for 2D materials and paves the way for their wider applications in sensing and biomaterials. Two-dimensional (2D) Au(I)-thiolate assemblies are a special type of material that can balance high structural stability and rich surface functionality, which shows promising prospects in both fundamental research and applications. Co-assembly of multiple ligands is a facile way to further enrich the surface properties and functions, and expand their application potentials. In this work, taking 3-mercaptopropionic acid (MPA), cysteine (Cys) and 1-thioglycerol (TGO) as example ligands, we studied in detail the possibility to co-assemble them into one nanosheet. Although the three ligands have significantly different controllability and pathways when self-assembling individually with Au(I), they can still be effectively co-assembled by reacting with HAuCl 4 together to obtain three-ligand nanosheets with good colloidal stability. The key points for successful co-assembly are also revealed by comparing single- and three-ligand self-assembly processes, laying a solid foundation for co-assembly of even more ligands. The easy but powerful strategy for 2D materials with closely-packed and multiple tunable surface functional groups addresses the surface engineering problem for 2D materials and paves the way for their wider applications in sensing and biomaterials.
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Nature Plants
·
2024
·
IF 15.8
Zhang Aihong,Tian Lin,Zhu Tong,Li Mengyu,Sun Mengwei,Fang Ying,Zhang Yi,Lu Congming
Photosystem I (PSI) is one of two large pigment–protein complexes responsible for converting solar energy into chemical energy in all oxygenic photosynthetic organisms. The PSI supercomplex consists of the PSI core complex and peripheral light-harvesting complex I (LHCI) in eukaryotic photosynthetic organisms. However, how the PSI complex assembles in land plants is unknown. Here we describe PHOTOSYSTEM I BIOGENESIS FACTOR 8 (PBF8), a thylakoid-anchored protein in Arabidopsis thaliana that is required for PSI assembly. PBF8 regulates two key consecutive steps in this process, the building of two assembly intermediates comprising eight or nine subunits, by interacting with PSI core subunits. We identified putative PBF8 orthologues in charophytic algae and land plants but not in Cyanobacteria or Chlorophyta. Our data reveal the major PSI assembly pathway in land plants. Our findings suggest that novel assembly mechanisms evolved during plant terrestrialization to regulate PSI assembly, perhaps as a means to cope with terrestrial environments.
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ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Ru Ma,Zhihao Zhao,Qian Wu,Ziqin Lu,Yuanxia Lv,Shijiao Chen,Hongmei Lu
Abstract Single-cell mass spectrometry (MS) faces significant challenges in covering low-abundance and poorly ionizable metabolites, hindering comprehensive single-cell metabolomics studies of disease and life processes. Herein, we proposed a new single-cell MS method based on a pulled flowprobe that enables online static-zone metabolite enrichment and derivatization of cis-diol metabolites, thereby greatly enhancing metabolite coverage. A stationary sample band was observed within the continuously flowing liquid microjunction of the pulled flowprobe when the inner capillary was substantially retracted inside the outer capillary. A larger retraction distance and lower solvent flowrate were found to benefit band formation, and the band served as a static zone to enrich analytes, achieving up to 50-fold signal enhancement. Then, a benzylboronic acid derivatization reagent was introduced into this band, where both the reagent and cis-diol metabolites were enriched to achieve static derivatization, yielding faster reaction kinetics (< 1/4 the time to reach maximum yield) and greatly reduced band diffusion/dilution (peak width: 30 s vs > 100 s) compared with the traditional dynamic online derivatization. Then, the new single-cell MS method with online enrichment and static-zone derivatization was established and enhanced overall metabolite coverage more than two-fold (53 vs 24), and specifically three-fold for cis-diol metabolites from a single cell, compared to the traditional method using dynamic derivatization. Finally, the new single-cell MS method was applied to the neuronal injury study, and six metabolites involved in oxidative stress, myelin damage, and DNA damage pathways were found to be significantly altered between injured and normal cells. These results highlight the advances of our method in expanding the molecular understanding at the single-cell level to uncover disease mechanisms.
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