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SENSORS AND ACTUATORS B-CHEMICAL · 2025 · IF 7.7

Target-responsive DNAzyme hydrogel reinforced by click reaction for surface enhanced Raman scattering detection of okadaic acid

Ming Wang,Lizhen Zhao,Yuling Hu,Gongke Li

Shellfish toxins are common marine toxins that have attracted worldwide attention due to their serious threats to food safety and human health. In this work, DNA hydrogel based on rolling circle amplification (RCA) and click reaction was developed for surface enhanced Raman scattering (SERS) detection of okadaic acid (OA) combined with target-responsive DNAzyme signal amplification. The RCA strands containing azido-dCTP were combined with cross-linked strands with ethynyl groups via click reaction to form a DNA hydrogel framework. The click reaction strengthened the DNA hydrogel network, making it more rigid and easier to manipulate during the detection process. The aptamer and DNAzyme were introduced into the DNA hydrogel as functionalized DNA components. Upon the specific recognition of OA by the aptamer, the DNAzyme released via the displacement reaction would continuously cleave the enzyme cutting site within the substrate strand to liberate the SERS signal tag. The functionalized DNA hydrogel concurrently achieved the functions of target recognition, signal conversion and signal amplification. Under optimal conditions, this strategy could detect OA with limits of detection as low as 0.2 nmol/L within 30 min. The SERS signal intensity showed good linear relationship with OA concentration in the range of 1.0–300.0 nmol/L. The practical application was validated for detecting trace amounts of OA in aquatic product samples. The stable DNA hydrogel combined with target-responsive DNAzyme signal amplification offers a universal strategy for rapid detection of trace toxins in complex matrixes.

研究领域: 生物化学 · 分析化学 · 毒理学
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Self-Assembled DNA Hydrogel Based on Enzymatically Polymerized DNA for Protein Encapsulation and Enzyme/DNAzyme Hybrid Cascade Reaction

Binbin Xiang,Kaiyu He,Rong Zhu,Zhuoliang Liu,Shu Zeng,Yan Huang,Zhou Nie,Shouzhuo Yao

DNA hydrogel is a promising biomaterial for biological and medical applications due to its native biocompatibility and biodegradability. Herein, we provide a novel, versatile, and cost-effective approach for self-assembly of DNA hydrogel using the enzymatically polymerized DNA building blocks. The X-shaped DNA motif was elongated by terminal deoxynucleotidyl transferase (TdT) to form the building blocks, and hybridization between dual building blocks via their complementary TdT-polymerized DNA tails led to gel formation. TdT polymerization dramatically reduced the required amount of original DNA motifs, and the hybridization-mediated cross-linking of building blocks endows the gel with high mechanical strength. The DNA hydrogel can be applied for encapsulation and controllable release of protein cargos (for instance, green fluorescent protein) due to its enzymatic responsive properties. Moreover, this versatile strategy was extended to construct a functional DNAzyme hydrogel by integrating the peroxidase-mimicking DNAzyme into DNA motifs. Furthermore, a hybrid cascade enzymatic reaction system was constructed by coencapsulating glucose oxidase and β-galactosidase into DNAzyme hydrogel. This efficient cascade reaction provides not only a potential method for glucose/lactose detection by naked eye but also a promising modular platform for constructing a multiple enzyme or enzyme/DNAzyme hybrid system.

研究领域: 生物材料学 · 分子生物学
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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

A chemiluminescent biosensor for ultrasensitive detection of adenosine based on target-responsive DNA hydrogel with Au@HKUST-1 encapsulation

Yanna Lin,Xueying Wang,Yuanling Sun,Yuxue Dai,Weiyan Sun,Xiaodong Zhu,Hao Liu,Rui Han,Dandan Gao,Chuannan Luo

In this work, target-responsive DNA hydrogel with high loading and good biocompatibility was used to construct chemiluminescent biosensor for specific detection of adenosine. Acrydite-modified adenosine aptamer (Acry-A-Apt), acrydite-modified single-strand DNA (Acry-ssDNA) and hemin aptamer (H-Apt) were used to prepared the DNA hydrogel, and the three single-strand DNA were partially complementary to each other. Thus, the DNA hydrogel only dissolved when adenosine and hemin were present simultaneously. HKUST-1 is a Cu-based MOFs with peroxidase-like activity. Au NPs were coated into cavities of HKUST-1 to obtain [email protected] , and the [email protected] had a stronger peroxidase-like activity than HKUST-1. [email protected] was coated in the DNA hydrogel. When only hemin was present, hemin bound to the H-Apt to form the G-quadruplex/hemin and the DNA hydrogel remained in the gel state. Therefore, the G-quadruplex/hemin was formed in the hydrogel and the excess hemin can be removed, avoiding background signal interference. Adenosine was then added and the preferential interaction between adenosine and adenosine aptamer resulted in complete dissolution of the DNA hydrogel. Subsequently, G-quadruplex/hemin and [email protected] were released simultaneously, enabling dual signal amplification of chemiluminescent biosensor, yielding a “signal on” readout. As a result, the biosensor could quantify adenosine from 4 × 10 −13 – 1.5 × 10 -10 mol/L with a detection limit as low as 1.04 × 10 −13 mol/L. The DNA hydrogel system provides a simple, sensitive and biocompatible method for the detection of adenosine which is useful in the field of biotechnology.

研究领域: 生物技术 · 分析化学 · 材料科学
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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Highly Stable and Multiemissive Silver Nanoclusters Synthesized in Situ in a DNA Hydrogel and Their Application for Hydroxyl Radical Sensing

Jing Li,Jiantao Yu,Yishun Huang,Haoran Zhao,Leilei Tian

Oligonucleotide-stabilized silver nanoclusters (AgNCs) show promising applications in bioimaging and bio-/chemo-sensing. However, their unsatisfactory photostability limits their practical applications. In this work, fluorescent AgNCs were synthesized in situ in a DNA hydrogel, consisting of cross-linked enzymatically amplified polymeric DNAs with cytosine-rich sequences in the presence of Ag+. The fluorescence property of the resultant AgNCs was optimized by a rational design of the DNA sequences to cover a broad spectrum with comparable green and red emissions. Under the protection of the DNA hydrogel, the AgNCs showed significantly improved photostability in an ambient oxygen environment, as well as low cytotoxicity even at a high concentration. Therefore, these properties show the rolling-circle-amplification-stabilized AgNCs to be a promising possible fluorescent probe for the detection of reactive oxygen/nitrogen species (ROS/RNS) in live cells because red-emitting species are susceptible to oxidation and consequently convert to green-emitting species. Finally, the as-prepared AgNCs were demonstrated to be a sensitive and specific probe for cellular imaging and the monitoring of ROS/RNS levels, which broadens the applications of AgNCs and provides a new tool for related biological investigations.

研究领域: 生物化学 · 纳米生物学 · 分析化学
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BIOSENSORS & BIOELECTRONICS · 2022 · IF 12.545

CRISPR/Cas12a-derived sensitive electrochemical biosensing of NF-κB p50 based on hybridization chain reaction and DNA hydrogel

Feng Qiu,Xiaoyan Gan,Jianglong Yao,Bingying Jiang,Ruo Yuan,Yun Xiang

Transcription factors (TFs) are key substances in regulating the transcription, replication and expression of genes, and the detection of TFs can provide valuable information to diagnose a variety of diseases. By integrating hybridization chain reaction (HCR)-activated Cas12a enzyme with bio-responsive DNA hydrogels, we propose a dual amplification and label-free homogeneous electrochemical detection method to realize sensitive nuclear factor-kappa B p50 (NF-κB p50) detection. The presence of the target molecules protects the DNA duplex probes from digesting by exonuclease III and initiates HCR to generate long double stranded DNAs that can activate the activity of RNA-guided Cas12a enzymes. The single-stranded region of the DNA linkers that crosslink the DNA hydrogels can be cleaved by the activated Cas12a to release a large number of electroactive substances embedded in the gels, which exhibit highly enhanced electrochemical signals for detecting target molecules at the detection limit of 54.1 fM. In addition, the successful interrogation of NF-κB p50 spiked into lysate of HeLa cells by such method is also verified. The established method thus shows new opportunities for sensitive and convenient monitoring of other transcription factors and biomarkers.

CAS / MDL: 79-06-1
研究领域: 生物化学 · 分子生物学 · 医学诊断
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TALANTA · 2024 · IF 5.6

Portable T-2 toxin biosensor based on target-responsive DNA hydrogel using water column height as readout

Meixiang Xue,Shuangxi Cai,Ye Deng,Fang Luo,Jianhui Huang,Zhenyu Lin

T-2 toxin, a hazardous mycotoxin often present in cereals and products based on cereals, poses a substantial risk to humans and animals due to its high toxicity. The development of uncomplicated, quick and highly sensitive methods for detecting T-2 toxin is imperative. In this work, a portable sensing system was constructed using water column height as a readout device in combination with a controlled release system, which allows for an accurate quantitative analysis of T-2 toxin without the need for expensive instrumentation or skilled technicians. Hyaluronic acid (HA) hydrogel was constructed by double cross-linked DNA/aptamer hybrids with polyethyleneimine (PEI) and embedded with platinum nanoparticles (Pt NPs). The aptamer specifically bound to T-2 toxin in its presence, resulting in the disruption of the hydrogel and subsequent release of the Pt NPs. These Pt NPs were later mixed with a solution of H 2 O 2 in a confined reaction flask, leading to the decomposition of H 2 O 2 into O 2 . A glass capillary tube containing a column of red water had been inserted into the cap of the reaction flask, and the low solubility of O 2 led to an increase in pressure within the reaction unit, causing the red water column to rise. There is a good linear correlation between the height of the capillary liquid level and the T-2 toxin concentration in the range of 20 ng/mL to 6 μg/mL. The system has been successfully used to detect T-2 toxin in samples of barley tea and corn.

研究领域: 生物传感技术 · 食品安全检测
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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

A responsive pure DNA hydrogel for label-free detection of lead ion

Jian Chu,Chun Chen,Xijian Li,Libing Yu,Wenjing Li,Mengxi Cheng,Wei Tang,Zhonghua Xiong

It is of great significance to develop facile and economical strategies for on-site detection and treatment of toxic metal ions . Stimulus-responsive DNA hydrogel materials have been increasingly used for convenient detection of metal ions due to their advantages such as simplicity, portability, and ease of storage. However, these methods still require encapsulation of signal tags by labeling or embedding. In this paper, a one-step preparation of Pb 2+ -responsive pure DNA hydrogel material was designed to realize a new label-free strategy for Pb 2+ biosensing. The Pb 2+ -dependent DNAzyme strand and substrate strand were introduced to fabricate the DNA hydrogel. The presence of Pb 2+ in the sample activates the enzyme strand in the hydrogel skeleton and triggers the cleavage of the substrate, thereby destroy the hydrogel structure. DNA fragments released by the collapsed hydrogel were readily measured as signal output for quantifying Pb 2+ concentrations with a minimum detection limit of 7.7 nM. We successfully eliminated the need for embedding or labeling of signal molecules by using the DNA molecules that construct hydrogels as the signal output. And the newly developed method for label-free detection of Pb 2+ based on pure DNA hydrogel is simple, easy readout, and cost-effective. By adjusting the DNAzyme and substrate sequences, label-free analysis of other metal ions can also be achieved. We expect that our strategy can be applied to the field detection of toxic metal ions.

CAS / MDL: 7365-45-9
研究领域: 环境科学 · 材料科学 · 生物传感
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TALANTA · 2023 · IF 6.1

The development of a paper-based distance sensor for the detection of Pb2+ assisted with the target-responsive DNA hydrogel

Jinpeng Liu,Yanhui Bi,Wenjun Tai,Yong Wei,Qiang Zhang,Anna Liu,Qiongzheng Hu,Li Yu

Due to the serious risks of lead pollution to human health, it plays a great role in constructing a simple, inexpensive, portable, and user-friendly strategy for Pb 2+ detection in environmental samples. Herein, a paper-based distance sensor is developed to detect Pb 2+ assisted with the target-responsive DNA hydrogel. Pb 2+ can activate DNAzyme to cleave its substrate strand, which results in the hydrolysis of the DNA hydrogel. The released water molecules trapped in the hydrogel can flow along the patterned pH paper due to the capillary force. The water flow distance (WFD) is significantly influenced by the amount of water released from the collapsed DNA hydrogel triggered by the addition of various Pb 2+ concentrations. In this way, Pb 2+ can be quantitatively detected without using specialized instruments and labeled molecules, and the limit of detection (LOD) of Pb 2+ is 3.0 nM. Additionally, the Pb 2+ sensor works well in lake water and tap water. Overall, this simple, inexpensive, portable, and user-friendly method is very promising for quantitative and in-field detection of Pb 2+ with excellent sensitivity and selectivity .

研究领域: 生物化学 · 环境科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

A portable visual capillary sensor based on functional DNA crosslinked hydrogel for point-of-care detection of lead ion

Chao Jiang,Yansheng Li,Hui Wang,Desheng Chen,Yongqiang Wen

We proposed a facile DNA-based hydrogel capillary sensor (DHCS) for sensitive detection of Pb 2+ . This proposed biosensor took advantage of the capillary action of the capillary tube controlled by the hydrogel film and the mesh size of the hydrogel based on target-responsive DNA. In the presence of Pb 2+ , the crosslinker substrate strand was cleaved leading the hydrogel fractured partly, and the mesh size of the hydrogel film plugging the end of the capillary tube changed. Owing to this, the behavior of the solution flowing through the capillary controlled by the hydrogel film was affected by the concentration of Pb 2+ . Therefore, through reading the distance and duration time by the naked eye, quantitative detection of Pb 2+ was achieved without any equipment. Additionally, and importantly, the tiny Pb 2+ responsive DNA hydrogel (0.02 μL) can be directly applied to analysis without encapsulation operations of nanoparticles or enzymes. Benefiting from the DNAzyme merits of high sensitivity and selectivity, in the range of 0.01 –50 μM, the developed method was able to detect as low as 10 nM Pb 2+ in less 1 h with the distance under 20 mm, meanwhile, the signals of blank and other high concentration metal ions were negligible. This sensor could be utilized to detect Pb 2+ in tap water with good reliability. Therefore, this proposed strategy provided a miniature, portable, sensitive and highly selective, visual platform for the detection of Pb 2+ in situ measurement.

研究领域: 生物化学 · 环境科学 · 分析化学
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ACS Nano · 2022 · IF 18.027

Microneedle Array Encapsulated with Programmed DNA Hydrogels for Rapidly Sampling and Sensitively Sensing of Specific MicroRNA in Dermal Interstitial Fluid

Qiqi Yang,Yeyu Wang,Tengfei Liu,Chaoxiong Wu,Jinze Li,Jiale Cheng,Wei Wei,Fan Yang,Liping Zhou,Yufan Zhang,Shuangshuang Yang,Haifeng Dong

Author: Please verify that the changes made to improve the English still retain your original meaning.Detection of microRNA (miRNA) in dermal interstitial fluid (ISF) has emerged as clinically useful in health status monitoring. However, it remains a great challenge owing to the difficult sampling and low abundance. Here, we report a DNA hydrogel microneedles (MNs) array to realize rapid enrichment and sensitive detection of miRNA in ISF. The MNs’ patch consists of methacrylate hyaluronic acid (MeHA) equipped with a smart DNA circuit hydrogels’ system (MeHA/DNA), in which an appropriate miRNA input enables triggering a cascading toehold-mediated DNA displacement reaction to catalytically cleave cross-linking points to generate amplified fluorescence (FL) for miRNA detection. The MeHA/DNA-MNs patch with high mechanical strength can extract adequate ISF in a short time (0.97 ± 0.2 mg in 5 min) in vivo because of its supreme water affinity. Additionally, the cascading toehold-mediated DNA displacement signal amplification reaction allows for sensitive detection of the low-abundant miRNAs down to 241.56 pM. The DNA hydrogels’ MNs present potential for minimally invasive personalized diagnosis and real-time health monitoring in clinical applications.

CAS / MDL: 68-12-2
研究领域: 生物医学工程 · 分子生物学 · 纳米技术 · 临床诊断
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ACS Sensors · 2021 · IF 7.711

Distance-Based Biosensor for Ultrasensitive Detection of Uracil-DNA Glycosylase Using Membrane Filtration of DNA Hydrogel

Chao Jiang,Fangfang Wang,Kexin Zhang,Tiantian Min,Desheng Chen,Yongqiang Wen

In the deoxyribonucleic acid (DNA) repair pathways, DNA repair enzymes have great significance for genomic integrity. As one important initiator of the base-excision repair pathway, the aberrant activity of uracil-DNA glycosylase (UDG) is closely associated with many diseases. Herein, we developed a simple distance-based device for visual detection of UDG activity using a load-free DNA hydrogel. The DNA hydrogel consists of polyacrylamide–DNA chains being bridged by a single-stranded DNA crosslinker containing a responsive uracil base site. UDG can recognize and remove the uracil, resulting in the cleavage effect of the DNA crosslinker strand with the assistance of endonuclease IV (Endo IV). Plugging one end of the capillary tube, the DNA hydrogel acting as a filter membrane separator would control molecules to flow into the tube. The integrity of the DNA hydrogel networks is affected by the excision of UDG. Therefore, taking full advantage of membrane filtration of the DNA hydrogel, the activity of UDG can be quantitatively detected via reading the distance of the red indicator solution in the capillary tube. Without any instruments and complicated procedures, this method realizes high sensitivity and specificity for the detection of UDG as low as 0.02 mU/mL and can even measure UDG in complex cell samples. Additionally, this method is simple, universal, and can be used to screen inhibitors, which shows great potential for point-of-care testing, clinical diagnosis, and drug discovery.

CAS / MDL: 1390-65-4
研究领域: 生物化学 · 分子生物学 · 医学诊断
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Bioactive Materials · 2025 · IF 20.3

Multifunctional DNA hydrogels with light-triggered gas-therapy and controlled G-Exos release for infected wound healing

Yuyun Ye,Yan Liu,Shengchao Ma,Xipeng Li,Wei Wang,Xu Chen,Judun Zheng,Zhijin Fan,Yideng Jiang,Yuhui Liao

Infectious wound healing remains a significant medical challenge due to chronic inflammation and bacterial colonization. Effective antimicrobial and anti-inflammatory therapies are essential to facilitate wound recovery. Herein, we introduce a highly biocompatible, ROS-responsive DNA hydrogel (LGAH), modified with aggregation-induced emission luminogens (AIEgen) and incorporating ginseng-derived exosomes (G-Exos) and nitric oxide (NO) donor-L-arginine (L-Arg) to promote healing of infected wounds. The hydrogel degrades in response to elevated ROS levels, releasing therapeutic agents. Upon laser irradiation, AIEgen generates 1 O 2 , which activates L-Arg to produce NO, leading to a synergistic antimicrobial effect. NO is particularly effective at inhibiting bacterial growth and promoting angiogenesis, supporting wound healing. G-Exos modulate immune responses, reduce inflammation, and promote the transition from the inflammatory to the proliferative phase. They also enhance cell proliferation, migration, and collagen production, which are key to tissue regeneration. In vivo experiments demonstrated that LGAH significantly accelerates S. aureus -infected wound healing by modulating the wound microenvironment and promoting tissue regeneration. Transcriptomic analysis revealed that LGAH down-regulates gene expression in inflammation and immune response signaling pathways while up-regulating genes related to energy metabolism. Biosafety evaluations at cellular and animal levels have demonstrated that LGAH possesses excellent biocompatibility and biodegradability, making it ideal for tissue repair and regeneration. This multifunctional DNA hydrogel system offers a safe and promising strategy for the clinical treatment of infected wounds.

CAS / MDL: 6066-82-6 74-79-3
研究领域: 生物医学工程 · 药理学 · 组织修复与再生
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