CHINESE JOURNAL OF CHEMISTRY
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2022
·Vol. 40
·期 12
·1437-1446
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IF 5.56
Xinshuang Chu,Qinghong Shi
Comprehensive Summary Inspired by nature, precise spatial organization of enzyme cascades of interest is crucial to the improvement of catalytic performance. Herein, DNA scaffolds were introduced to construct a toolkit for versatile immobilization of enzyme pairs on dextran-coated magnetic nanoparticles (MNPs). After the glucose oxidase (GOx) and horseradish peroxidase (HRP) pair was immobilized through random covalent, DNA-directed and DNA tile-directed strategies, the immobilized GOx/HRP pair on the MNP-based carrier assembled with DNA tile (TD@MNPs) exhibited the highest activity due to rational spatial organization and less conformational change of constituent enzymes. With a decrease in interenzyme distance on TD@MNPs, furthermore, the catalytic efficiency of the HRP/GOx pair increased further for both substrates, 2,2’-azinobis(3-ethyl-benzthiazoline-6-sulfonate) (ABTS) and 3,3',5,5'-tetramethyl benzidine (TMB). As the assembled HRP was closer to the carrier surface, the catalytic efficiency of the GOx/HRP pair increased by 6.2-fold for positively charged TMB and only by 62% for negatively charged ABTS compared with the free GOx/HRP pair. Moreover, a reversal of catalytic efficiency was found after the GOx/HRP pair was assembled on a positively charged carrier (TD@pMNPs). This research demonstrated that MNP-based carriers had the potential to become a versatile toolkit for shedding an insight into catalytic performance and the development of new biocatalysts.
研究领域:
生物化学
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纳米生物学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Xin Shang,Jiayang He,Chunli Yang,Siyu Zuo,Ruo Yuan,Wenju Xu
Development of logic AND-gated multivariate assay systems of DNA-scaffolded green- and red-fluorescent Ag nanoclusters ( g- AgNC and r- AgNC) is promising and remains challenging. By using two DNA segments ( T o and T r) as dual-targeting inputs, herein we report an innovative strategy that utilizes targets-recycled amplification to create a sensitive AND-gated light-up ratiometric sensor with reversely changed fluorescence of g- AgNC and r- AgNC. The design is based on that: two hairpins ( H o and H r) are individually recognizable to T o and T r, and two hybridized duplexes are resultantly implemented for transient dissipative base pairing, i.e. H o· H r, releasing T o and T r for repeated recycling. In an original stem-loop hairpin reporter (HR), one exposed overhang is to host g -AgNC. When HR is unfolded by the cooperative sticky toeholds in H o∙ H r, its liberated stem merging with the g -AgNC template is for r- AgNC clustering. Only when meeting simultaneously the overexpressed T o and T r in SARS-CoV-2, the AND-gated ratio fluorescence of r- AgNC over g- AgNC can be lighted-up in a typical assay, enabling highly specific-inputs binding and sensitive dose-dependence down to 0.29 pM. This enzyme-free and label-free AND-logic ratiometirc strategy illustrates the potential of using multicolor AgNCs emitters for more accurate multivariate assay.
研究领域:
生物化学
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分子生物学
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分析化学
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DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
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2025
·
IF 11.5
Shiyi Bi,Jieyu Shen,Yu Zhu,Lei Fan,Huangxian Ju,Ying Liu
Choosing appropriate delivery system for chemotherapeutic drugs as well as arranging the time spots for adoptive cells administrations is the key to achieve efficient combined chemo-adoptive cell therapy. Tumor-homing character makes adoptive immune cells appropriate targeting delivery carriers, but they are rarely used for chemtoxic payloads considering payloads internalization during administration which impairs adoptive cells. Herein, we frame adoptive NK cells using DNA scaffold with chemotherapeutic payloads fastened exterior, and achieves time-programmed drugs release and NK cell decapsulation to minimize side effects and enhance therapeutic effect. IL-21 nanoparticles are prepared by conjugating cytokine IL-21 with a GSH cleavable linker and act as anchor points for DNA scaffold assembly. Chemotherapeutic payloads are prepared by loading DOX/verapamil drugs to PLGA nanoparticles (PLGA drugs NPs), and connected to the exterior of DNA scaffold with a ROS cleavable linker. Porous DNA scaffold protects NK cells functions from impairing by chemotherapeutic payloads, while guarantees efficient communication of NK cells with exterior environment to keep tumor homing capability. Reactive oxygen species (ROS) in tumor microenvironment releases PLGA drugs NPs to perform chemotherapy, which subsequently generates a reductive environment to detach DNA scaffold for NK cell and IL-21 release to achieve combined chemo-adoptive cell therapy with enhanced therapeutic efficiency.
研究领域:
生物医学工程
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肿瘤学
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纳米医学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiayi Song,Wenting He,Hao Shen,Zixin Zhou,Mengqi Li,Ping Su,Yi Yang
The encapsulated enzyme system by metal–organic frameworks exhibited great potential in pharmaceuticals, enzyme fuel cells, and biocatalysis. However, the enzymatic activity and overall catalytic efficiency are severely hampered due to their enzyme leaching and causal enzyme location. Herein, for the first time, horseradish peroxidase (HRP) and glucose oxidase (GOx) used as model enzymes were cross-linked by rationally designed DNA scaffold network, and the multienzyme system has been successfully encapsulated into zeolite imidazolate framework-8 (ZIF-8). The prepared encapsulation multienzyme can efficiently suppress enzyme leaching from the MOFs skeleton, and the leaching amount was more than 10-times lower than the traditional MOFs encapsulation strategy. The well-tailored proximity and colocalization of cascade enzymes by the DNA scaffold network obviously improved the overall catalytic efficiency, enzymatic activity, and kinetic performance. The K m and k cat / K m for encapsulation multienzyme was 13.8 mM and 3.47 s −1 mM −1 , which was 0.27-fold lower and 9.9-fold higher than those of free enzymes, respectively, indicating a better substrate affinity. Furthermore, the multienzyme system exhibited excellent stability and reusability compared with free enzymes and control groups, which could preserve 95% initial activity at 50 °C after 75 min incubation and more than 87% of the original activity after 14 cycles. Finally, the immobilized multienzyme exhibited enhanced performance to detect low concentration of glucose (0.4 µM) with excellent selectivity. The outcome indicated that the encapsulated multienzyme could be extended for broad practical applications in biotechnology, biocatalysis, and biomedical engineering.
研究领域:
生物技术
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生物催化
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生物医学工程
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产品关联
DOI
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
·
2025
·
IF 6.6
Shanglin Li,Ziyang He,Yonghong Meng,Baoxin Li,Mei Liu
Aflatoxin B1 contamination poses severe threats to food safety, vitally requiring reliable assays. Biosensors are effective but subject to unsatisfactory signal conversion efficiency owing to their usage of the monovalent probes with redundant materials and procedures. Herein, we developed a photothermal aptasensor, which combined multifunctional polyvalent DNA scaffolds with thermal imaging for the portable detection of aflatoxin B1. The aptasensor was conferred with favorable properties of specific recognition, surface modification and signal amplification by the polyvalent DNA scaffolds, thereby showed enhanced analytical performance with simplified procedures. Moreover, the detection potential of the aptasensor was further improved by introducing Cu x S nanoparticles to provide intuitive temperature output for portable devices analysis. Consequently, AFB1 could be quantified in a wide range of 1–500 ng/mL with the detection limit of 0.75 ng/mL, merely using common thermometer. For food samples, the spiked recoveries of the proposed method ranged from 93.5 % to 108.7 % with relative standard deviation from 2.9 % to 6.3 %. These results were in agreement with the high-performance liquid chromatography method, demonstrating the good accuracy of this method. Therefore, this method is expected to be extended as a universal detection strategy for food hazards analysis.
研究领域:
食品科学
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生物传感技术
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分析化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Zhenzhen Zhang,Yu Han,Jing-Jing Cao,Li-xia Yuwen,Liu Zhang,Xiao-Xia Han,Dong-Hao Zhang
In traditional multienzyme random co-immobilization, it is difficult to precisely locate and regulate the relative positions between two enzyme molecules, resulting in low cascade efficiency between the two enzymes and limiting the application of multienzyme cascade catalysis technology. This study prepared PVAC@Y-dsDNA@GOD/HRP magnetic co-immobilized multienzyme by constructing a three-pronged DNA scaffold for co-coupling glucose oxidase (GOD) and horseradish peroxidase (HRP), which achieved directional co-immobilization of dual enzymes and precise regulation of inter-enzyme distance. Compared with traditional random co-immobilization of multienzyme, PVAC@Y-dsDNA@GOD/HRP could shorten the distance between GOD and HRP to the nanoscale and form substrate channeling, which greatly improved the cascade activity between the two enzymes. The inter-enzyme spacing between GOD and HRP could be precisely regulated by changing the length of DNA strands. When the inter-enzyme spacing was 10.08 nm, PVAC@Y-dsDNA@GOD/HRP exhibited high cascade activity of 707 U/mg. The inter-enzyme spacing that was too large or too small would reduce the cascade activity, indicating a distance-dependence of multienzyme cascade activity. PVAC@Y-dsDNA@GOD/HRP showed good reusability, indicating that the three-pronged DNA scaffold constructed by DNA double strands hybridization could firmly immobilize enzyme on carrier, with less enzyme leakage.
研究领域:
生物化学
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分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2025
·
IF 4.6
Wen Yun,Youwei Chen,Ruiqi Wang,Nana Xie,Xingmin Wang
A novel spatially constrained dual pincer DNA scaffold was developed for Bisphenol A (BPA) detection. The dumbbell-shaped aptamer hairpin could be opened by target BPA. The two tails of opened aptamer-hairpin separately triggered the catalytic hairpin assembly between the two hairpins at both ends of DNA scaffold through the proximity effect. The effective concentration of the hairpins on dual pincer DNA scaffold greatly increased about 2800 fold due to the spatial constraint design. A good dynamic correlation was shown from 10 pM to 300 pM. The limit of detection was as low as 3 pM according to the 3σ/slope protocol. Real sample detection confirmed that dual pincer DNA scaffold could be effectively used for food and environmental monitoring with accurate sensing.
研究领域:
分析化学
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生物化学
·
环境科学
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食品安全
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生物传感器
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核酸工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yunlong Wang,Jie Zhou,Yan Dong,Peng Wang,Ruiyang Zi,Honglan Zhang,Yingqiang Luo,Yan Zhang,Teng Wang,Yuhan Chen,Biao Hu,Houjie Liang,Zhihao Wei,Xiang Zhao
Constructing precise delivery systems to enhance the antitumor efficacy of drugs represents a pressing clinical practice need. The characteristics of suitable physiological stability, flexible tunable size, and highly programmable architecture make functional DNA scaffolds an ideal solution to this requirement. Here, we designed DNA oligonucleotide probes Y 1 , Y 2 and Y 3 to construct a smart-responsive Y-shaped DNA scaffold drug conjugate (sYDD). This sYDD incorporates two AS1411 aptamers, an apurinic/apyrimidinic (AP) site, a B-cell lymphoma-2 (Bcl-2) antisense oligonucleotide (ASO) and a doxorubicin (DOX)-carrying sequence. The Bcl-2 ASO and DOX within sYDD could be responsively released in tumor cells that exhibited high expression of apurinic/apyrimidinic endonuclease 1 (APE1) and microRNA-21 (miR-21). And the in vitro and in vivo experiments demonstrated that sYDD exhibited substantial antitumor efficiency. Moreover, the flow cytometry and RNA sequencing results proved that the proposed sYDD effectively activated immune responses. This strategy provides an alternative approach for designing synergistic chemo-gene drug conjugates, which facilitates the development of precision tumor treatment modalities.
研究领域:
药学
·
生物技术
·
癌症研究
·
分子生物学
·
纳米医学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）