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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

Magnetic DNA walker-engineered electrochemical sensor for highly sensitive detection of antibiotics

Jingyi Cai,Junping Ma,Yuan Dang,Shuangli Chen,Jieli Tang,Sha Yu,Yuanzhen Zhou

Antibiotics residue pollution in food and environmental matrices has posed a serious threat to global public health. It is an urgent demand in developing highly sensitive methods for the detection of low-abundance antibiotics in real samples. Herein, we established a magnetic DNA walker-engineered electrochemical sensor by taking advantages of the distinct recognition capability of aptamer and the excellent signal amplification performance of magnetic DNA walker for the accurate detection of kanamycin (Kana). The aptamer can specifically recognize Kana, while the magnetic DNA walker can not only amplify the target signal through the cascade displacement reaction, but also effectively reduce background interference via the magnetic separation, thus ensuring the sensitivity and accuracy of Kana detection in complex samples. The proposed electrochemical sensing method possesses a good linear relationship in the range of 10 fM −1 μM, and the limit of detection is as low as 0.02 fM. Moreover, the excellent selectivity allows this sensor has the ability to specifically identify the Kana from other antibiotics and even in the milk and tap water.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

2′-Fluoro-substituted DNA-induced self-assembly strategy for engineering hybrid nanospheres

Haihui Wang,Yifan Jiang,Yichang Liu,Xiaohui Zhu,Yongfei Liu,Minle Chen,Tao Zeng,Zhaowei Chen,Jinyu Li,Chunhua Lu,Huanghao Yang

The physicochemical differences between DNA and other molecules pose a challenge to the construction of DNA-based nanostructures. Herein, we propose a straightforward approach for preparing multifunctional DNA-based nanospheres through direct self-assembly of 2′-fluoro-substituted single-stranded DNA (2′F-DNA) with various small molecules. Molecular dynamics simulation revealed that 2′F substitution in DNA can cause the repulsion of adjacent PO 4 3- group, leading to local stretching of the DNA structure. Moreover, 2′F substituent induced the regular polarization of H 2 O nearby F to form the hydration layer, which interrupts inherent interactions among bases. In this way, the bases of 2′F-DNA chain have fewer constraints and more flexibility in conformation, facilitating their non-covalent interactions with other molecules and enhancing the self-assembly capacity of 2′F-DNA. Consequently, 2′F-DNA can bind to more molecules, tending to spontaneously form hybrid DNA nanospheres. Following this approach, a chemo-gene therapy 2′F-DNA/doxorubicin model was designed, showing the significant synergistic anti-tumor therapeutic efficacy. Taken together, this study provides an expandable approach for constructing engineering hybrid nanospheres using DNA and other small molecules, which holds great potential for further biological applications.

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JOURNAL OF NANOBIOTECHNOLOGY · 2022 ·Vol. 20 ·期 1 ·1-17 · IF 9.429

Boosting cisplatin chemotherapy by nanomotor-enhanced tumor penetration and DNA adducts formation

Xu Lihua,Zhang Kaixiang,Ma Xing,Li Yingying,Jin Yajie,Liang Chenglin,Wang Yong,Duan Wendi,Zhang Hongling,Zhang Zhenzhong,Shi Jinjin,Liu Junjie,Wang Yunlong,Li Wentao

Despite many nano-based strategies devoted to delivering cisplatin for tumor therapy, its clinical benefits are compromised by poor tissue penetration and limited DNA adducts formation of the drug. Herein, a cisplatin loading nanomotor based janus structured Ag-polymer is developed for cisplatin delivery of deeper tissue and increased DNA adducts formation. The nanomotor displayed a self‐propelled tumor penetration fueled by hydrogen peroxide (H2O2) in tumor tissues, which is catalytically decomposed into a large amount of oxygen bubbles by Ag nanoparticles (NPs). Notably, cisplatin could elevate the intracellular H2O2 level through cascade reactions, further promote the degradation of Ag NPs accompanied with the Ag+ release, which could downregulate intracellular Cl− through the formation of AgCl precipitate, thereby enhancing cisplatin dechlorination and Pt–DNA formation. Moreover, polymer can also inhibit the activity of ALKBH2 (a Fe2+-dependent DNA repair enzyme) by chelating intracellular Fe2+ to increase the proportion of irreparable Pt–DNA cross-links. It is found that deep tissue penetration, as well as the increased formation and maintenance of Pt–DNA adducts induced by the nanomotor afford 80% of tumor growth inhibition with negligible toxicity. This work provides an important perspective of resolving chemotherapeutic barriers for boosting cisplatin therapy.Graphical Abstract

CAS / MDL: 7761-88-8
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Biomaterials Science · 2022 ·Vol. 11 ·期 1 ·162-169 · IF 7.59

A self-delivery photodynamic sensitizer for enhanced DNA damage by PARP inhibition

Ren-Jiang Kong,Xin-Yu Li,Jia-Qi Huang,Xiang Zhou,Fu-An Deng,Yan-Mei Li,Ling-Shan Liu,Shi-Ying Li,Hong Cheng

Tumor cells activate DNA repair pathways to combat the oxidative damage induced by reactive oxygen species (ROS), contributing to their resistance to photodynamic therapy (PDT). Herein, a self-delivery photodynamic sensitizer is developed to enhance oxidative damage by blocking the DNA repair pathway through poly(ADP-ribose) polymerase (PARP) inhibition. Specifically, the photodynamic sensitizer (CeOla) is constructed based on the self-assembly of the photosensitizer chlorine e6 (Ce6) and the PARP inhibitor olaparib (Ola). Of note is that carrier free CeOla has a high drug content and favorable water stability, which could be effectively internalized by tumor cells for robust PDT upon light irradiation. Moreover, CeOla could inhibit the activation of PARP, promote the upregulation of γ-H2AX and reduce the expression of Rad51, thereby blocking the DNA repair pathway to sensitize tumor cells for PDT. As a consequence, the self-delivery CeOla greatly promotes the tumor cell apoptosis and shows a high antitumor performance with low side effects. It serves as a novel platform for the development of self-delivery nanomedicine to overcome oxidative resistance in tumor treatment.

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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

Dual-band fluorescence detection of double-stranded DNA with QDs-Mn2+-pefloxacin

Qiang Zhang,Shengbao Duan,Yinong Huang,Jingjing Tian,Jia Hu

By integrating the fluorescence of quantum dots (QDs) and Mn 2+ -pefloxacin mesylate (Mn 2+ -pefloxacin), a new type of dual-band fluorescence biosensor for high-efficiency and sensitive determination of double-stranded DNA (dsDNA) is developed. The biosensor is based on the fluorescence "OFF-ON" mode of both QDs and QDs-Mn 2+ -pefloxacin. The Mn 2+ -pefloxacin complex can quench the QDs fluorescence via photoinduced electron transfer (PET), and its fluorescence is also quenched. Due to the specificity and strong binding affinity of dsDNA for the Mn 2+ -pefloxacin complex, it can break the low fluorescent QDs-Mn 2+ -pefloxacin and restore the fluorescence of QDs and Mn 2+ -pefloxacin complex in their respective bands. Therefore, the dual-band fluorescence quantitative detection of dsDNA by QDs-Mn 2+ -pefloxacin can be achieved, while bovine serum albumin , single-stranded DNA, and bio-related ions do not yield similar results. Furthermore, the possible reaction mechanisms are systematically discussed. The detection limits (3δ/K) of herring sperm (hs) DNA in the fluorescence recovery bands of QDs and Mn 2+ -pefloxacin complex are 0.0142 and 0.0465 μg/mL, respectively. The developed biosensor was used for dsDNA detection in synthetic samples, and desirable results are obtained.

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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

DNA self-assembled FeNxC nanocatalytic network for ultrasensitive electrochemical detection of microRNA

Yunyun Ning,Cuiling Zhang,Chunyan Wang,Chuqing Zhou,Nana Gong,Qiang Wang,Ye Zhu

Accurate detection of microRNA (miRNA) is challenging but essential for disease diagnostics and therapeutics. To meet the high demands of miRNA analysis, we proposed a highly sensitive and specific electrochemical strategy based on duplex-specific nuclease (DSN)-assisted target recycling and DNA self-assembled FeN x C nanocatalytic network for precise quantitation of miRNA-21 as a model. FeN x C nanospherical catalyst with high peroxidase-mimicking activity was synthesized through high-temperature pyrolysis and modified with DNA. The identification of miRNA-21 by elaborately designed capture probe triggered DSN-assisted target recycling. Subsequently, self-assembled FeN x C nanocatalytic network was constructed on the sensor surface through DNA hybridization reaction, whose signal response was demonstrated to be 4.272-fold higher than the single layer of FeN x C. By virtue of such cascade signal amplification, ultrasensitive electrochemical detection of miRNA-21 was realized in a dynamic range of 0.5 fM - 1 pM with a detection limit of 0.2805 fM. Additionally, the proposed strategy exhibited high specificity for miRNA-21 and practical applicability in real sample analysis, demonstrating promising potential for the reliable miRNA analysis in disease diagnosis and therapy applications.

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Advanced Materials Technologies · 2022 ·Vol. 7 ·期 10 ·2200066 · IF 8.856

Design of a DNA-Based Double Network Hydrogel for Electronic Skin Applications

Li Tang,Shaoji Wu,Yue Xu,Youwei Li,Bailin Dai,Caixia Yang,Aifeng Liu,Jianxin Tang,Liang Gong

Electronic skin (e-skin) is widely studied for its ability to detect physiological information and provide feedback through electrical signals. Biocompatible stimulus-responsive DNA-based hydrogels exhibit high sensitivity, which makes them outstanding candidates for biomedical applications. However, several disadvantages, such as weak mechanical properties, expensive manufacturing costs, cumbersome double chain design, and difficulty obtaining bulk size, seriously limit their practical application. Based on the double network (DN) strategy, a universal, low-cost, and high-toughness deoxyribonucleic acid/poly( N -hydroxyethyl acrylamide) (DNA/pHEAA) DN hydrogel is designed. The transparent hydrogel shows tensile stress/strain of 0.96 ± 0.043 MPa/2537.55 ± 23.24%, rapid self-recovery ability (peak stress/energy dissipation recovery rate of 99.72%/95.38% after 30 s resting), excellent fatigue resistance (peak stress/energy dissipation retention rate of 91.08%/81.05% after 100 loading-unloading cycles with strain of 50%), reversible adhesive ability (≈45 KPa), and good biocompatibility. Thus, the DNA/pHEAA DN hydrogel can be used as an e-skin. Sensing signals are displayed on a smartphone as images sent through wireless technology; the images change with the collected signals, achieving motion detection. The universal and low-cost design of stimulus-responsive DNA-based hydrogels with high toughness, excellent self-recovery, and anti-fatigue performance is expected to promote their application in the biomedical field.

CAS / MDL: 106797-53-9 7647-15-6
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Nanoscale · 2022 ·Vol. 14 ·期 17 ·6465-6470 · IF 8.307

An activatable DNA nanodevice for correlated imaging of apoptosis-related dual proteins

Zhixiang Li,Xueyan Feng,Wenping Hu,Lele Li

Apoptosis plays an important role in the life cycle of multicellular organisms. The development of techniques for sensitive monitoring of apoptosis-related key molecules can be used to assess not only disease progression but also its therapeutic interventions. However, there is still a lack of an imaging probe amenable for simultaneously detecting multiple biomarkers during drug-induced apoptosis. Herein, a novel activatable DNA nanodevice was designed to image apoptosis-related dual proteins in real time. The turn-on and specific recognition properties of our probe allow the spatially selective detection of apoptotic-related marker cytochrome c and apurinic/apyrimidinic endonuclease 1 in living cells. We demonstrated that the DNA nanodevice has the ability to monitor apoptosis and evaluate the efficacy of apoptosis-related drugs, which potentially can be used as a tool to evaluate the molecular mechanism of apoptosis regulation or to screen apoptotic drugs.

CAS / MDL: 70-18-8
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

Metal nanoclusters combined with CRISPR-Cas12a for hepatitis B virus DNA detection

Yu Tao,Ke Yi,Haixia Wang,Kai Li,Mingqiang Li

Since hepatitis B virus (HBV) infection can cause chronic viral hepatitis, increase the risk of liver fibrosis and cirrhosis, and ultimately result in hepatoma, it is of great significance to explore convenient, rapid, and sensitive diagnostic strategies for HBV DNA detection. In this study, we developed a novel and sensitive fluorescent biosensor for HBV detection based on the sensing system consisting of CRISPR-Cas12a enzymes and metal nanoclusters as the luminescent nanoprobes, involving gold nanoclusters (AuNCs), silver nanoclusters (AgNCs), and copper nanoclusters (CuNCs). The DNA probes could effectively be applied as the template for the preparation of fluorescent metal nanoclusters. In the presence of the HBV target, the trans-cleavage capability of Cas12a was able to be initiated to degrade DNA probes, which brought about the inhibition of metal nanoclusters formation, thereby giving minimal fluorescence signals. In comparison with AuNCs and AgNCs, the CuNCs-based nanosensor exhibited much higher sensitivity. In addition, the fluorescence response of CuNCs to HBV detection was significantly faster, which could be completed within 25 min without the requirements of sophisticated equipment or harsh reaction conditions. Moreover, the practical application of this analysis method was also demonstrated to detect HBV DNA target in human serum samples with satisfactory recovery, which was promising for simple, rapid, sensitive, and label-free HBV DNA bioanalysis .

CAS / MDL: 7447-39-4 68-04-2
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ACS Applied Nano Materials · 2022 · IF 6.14

Gold/Palladium–Polypyrrole/Graphene Nanocomposites for Simultaneous Electrochemical Detection of DNA Bases

Peng Lei,Ying Zhou,Bei Li,Yang Liu,Chuan Dong,Shaomin Shuang

The unique combination of DNA bases is essential for storing genetic information. A reliable and accurate electrochemical sensor based on a gold/palladium–polypyrrole/graphene nanocomposite (Au/Pd–PPy/GR) has been prepared to individually and simultaneously detect guanine (G), adenine (A), thymine (T), and cytosine (C). The bimetallic nanomaterial (Au/Pd–PPy) is used to enhance the sensing performance of DNA bases, and the GR could further increase the electroactive area and amplify the electrochemical response. As expected, the electrochemical sensor shows excellent electrocatalytic activity with well-separated current responses at 0.704 V (G), 0.976 (A), 1.164 (T), and 1.348 V (C). The prepared sensor exhibits the linear range of 1–350 μM for G, 5–300 μM for A, 20–900 μM for T, and 10–700 μM for C. The developed device is also demonstrated as an excellently sensitive and highly selective sensor to identify the four bases in calf thymus DNA, which provides the application of electrochemical sensors in bioscience.

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Biosensors-Basel · 2022 ·Vol. 12 ·期 3 ·162 · IF 5.743

Magnetic Immunosensor Coupled to Enzymatic Signal for Determination of Genomic DNA Methylation

Yitao Liang,Bin Zhang,Zexin Xue,Xuesong Ye,Bo Liang

Aberrations of genomic DNA methylation have been confirmed to be involved in the evolution of human cancer and have thus gained the potential to be depicted as biomarkers for cancer diagnostics and prognostic predictions, which implicates an urgent need for detection of total genomic DNA methylation. In this work, we suggested an assay for the quantification of global DNA methylation, utilizing methylation specific antibody (5mC) modified magnetic beads (MBs) for immunorecognition and affinity enrichment. Subsequently, the captured DNA on the surface of MBs interacted with the glucose oxidase-conjugated DNA antibody whose catalytic reaction product was engaged in electrochemical detection of the overall level of DNA methylation on a PB-doped screen-printed electrode. With 15 pg of input DNA, which, to our best knowledge, is the lowest required amount of DNA without sodium bisulfite treatment or amplification, this test strategy was able to perceive as low as 5% methylation level within 70 min including the preparation of anti-5mC-MBs. We believe this detection technique offers a promising option to detect global DNA methylation in both academic and clinical scenarios.Keywords:DNA methylation;magnetic beads;screen printed electrode;electrochemical

CAS / MDL: 1185-53-1
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-14 · IF 16.6

A smart pathogen detector engineered from intracellular hydrogelation of DNA-decorated macrophages

Gui Yueyue,Zeng Yujing,Chen Binrui,Yang Yueping,Ma Jiehua,Li Chao

Bacterial infection is a major threat to global public health, which urgently requires useful tools to rapidly analyze pathogens in the early stages of infection. Herein, we develop a smart macrophage (Mø)-based bacteria detector, which can recognize, capture, enrich and detect different bacteria and their secreted exotoxins. We transform the fragile native Møs into robust gelated cell particles (GMøs) using photo-activated crosslinking chemistry, which retains membrane integrity and recognition capacity for different microbes. Meanwhile, these GMøs equipped with magnetic nanoparticles and DNA sensing elements can not only respond to an external magnet for facile bacteria collection, but allow the detection of multiple types of bacteria in a single assay. Additionally, we design a propidium iodide-based staining assay to rapidly detect pathogen-associated exotoxins at ultralow concentrations. Overall, these nanoengineered cell particles have broad applicability in the analysis of bacteria, and could potentially be used for the management and diagnosis of infectious diseases.

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