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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Green synthesis of low-silica CHA zeolite without organic structural directing agents, fluoride media and seeds

Xiaojun Deng,Ping Zhou,Xiayan Yan,Renjin Xiong,Huaqin Kou,Wenhua Luo

To spare the use of OSDA and fluorides, for the sake of reducing cost and environmental conservation, a green and efficient synthesis recipe of low-silica CHA zeolites has been demonstrated, without using seeds or any other zeolites. The main factors that determine the formation of CHA zeolites have been investgated systemmatically, and several rules are obtained. (i) just considering simple memallic cations acting as the SDA , K + is indispensable for the formation of CHA framework, with noting that K + can also direct to MER topology. (ii) working as catalyst or minerization agent, OH − and F − function almost identically, but when the concentration of F − has reached a really high level or even only F − was used, CHA framework can not form because the intermediate fluoride complexes are inclined to produce small melecules of fluoride salts with morderate solubility over to enter the zeolite framework. (iii) at conditions of this work, the second stirring after the RT aging should be adopted since the contrastive tests have showed the benifits of the second stirring in making fewer or smaller impurity grains. (iv) when the concentration of K + is too high in reactive gels, with the other same conditions, MER over CHA framework is preferentially to form. (v) it is reasonable to consider the as-synthesized K-CHA materials can be used to research the novel “trapdoor” effect later. The authors considered the discussions and conclusions would offer some beneficial references to the green synthesis of zeolites and further understanding of the mechanism of hydrothermal treatment .

研究领域: 材料科学 · 环境化学 · 无机化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Highly steam-stable CHA-type zeolite imidazole framework ZIF-302 membrane for hydrogen separation

Haiqian Lian,Eryue Song,Bin Bao,Wenhe Yang,Yu Yang,Yichang Pan,Shengui Ju

Metal-organic frameworks (MOFs) as molecular sieve membrane materials have received extensive attention on the gas separation application. However, the membrane separation performance is extremely limited by its intrinsic stability of frameworks. The successful preparation of high-quality gas separation membranes with excellent stability remains a grand challenge. ZIF-302 is based on hydrophobic ligand in-situ design with a high-stabile chabazite (CHA) topology. Herein, we synthesized uniform ZIF-302 nanocrystals with exceptional stability by introducing a modulator. Correspondingly, the continuous dense ZIF-302 polycrystalline membranes were also prepared for the separation of H 2 , N 2 , CO 2 , CH 4 and other gases. The permeance of H 2 and separation factor for H 2 /CH 4 mixtures at 35 °C and 1 bar were 2.8 × 10 -8 mol m −2 s −1 Pa −1 and 51.5, respectively, exceeding the Robeson upper bound in 2008. Furthermore, the separation performance of the super-hydrophobic ZIF-302 membranes for humidified mixed gases can maintain more than 168 h at 35 °C, indicating reliable long-term operational stability. Therefore, the CHA-type ZIF-302 polycrystalline membrane is promising for actual industrial gas separation.

研究领域: 材料科学 · 化学工程 · 膜技术
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Journal of Materials Chemistry B · 2024 · IF 6.1

Sensitive detection of dipeptidyl peptidase based on DNA–peptide conjugates and double signal amplification of CHA and DNAzymes

Yan Chen,Miao He,Feifan Yin,Wenting Cheng,Zhongyun Wang,Yang Xiang

Dipeptidyl peptidase IV (DPPIV) is an enzyme belonging to the type II transmembrane serine protease family that has gained wide interest in the fields of hematology, immunology, and cancer biology. Moreover, DPPIV has emerged as a promising target for therapeutic intervention in type II diabetes. Due to its biological limitations, traditional strategies cannot meet the requirements of low abundance DPPIV analysis in complex environments. In this work, combining the high programmability of DNA and the chemical diversity of peptides, we designed DNA–peptide conjugates that can be specifically recognized, polypeptides as specific substrates for target DPPIV and DNA probes as primers for catalytic hairpin assembly (CHA), recycling a large amount of DNAzymes by triggering CHA amplification. The DNAzyme substrate modified with the FAM fluorescent group was immobilized on the surface of gold nanoparticles by S–Au chemical bonds to form a signal output probe. The DNAzymes enzyme cleaved the substrate of the signal outputs probe, yielding a double-amplified fluorescence signal. This method has a detection limit as low as 0.18 mU mL−1 and a linear range of 0–5 mU mL−1 in serum samples, showing high stability and good potential for practical applications.

研究领域: 生物化学 · 分子生物学 · 分析化学 · 糖尿病研究 · 癌症生物学
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

A reagentless triplex DNA junctions-based electrochemical DNA sensor using signal amplification strategy of CHA and tetraferrocene

Mei Wang,Hanfeng Cui,Nian Hong,Qingxia Shu,Xinru Wang,Yuping Hu,Guobing Wei,Hao Fan,Jing Zhang

In this paper, we first synthesized a novel tetraferrocene signal marker. Then a reagentless triplex DNA junctions-based electrochemical DNA sensor using signal amplification strategy of CHA and tetraferrocene was constructed. Tetraferrocene labeled hairpin probes (H1 and H2) were integrated together to form triplex DNA junctions through connecting chain (C1). It enabled catalytic hairpin assembly (CHA) reaction to be initiated without the addition of exogenous probe during the detection process, and the conformational change of the target caused the change of electrochemical signal. Combined with tetraferrocene and CHA strategies, the sensor achieved double signal amplification with a detection limit as low as 0.085pM. In addition, the sensor was successfully applied to mRNA detection in cells with high sensitivity and reagentless operation, providing possibilities for in vivo testing.

研究领域: 生物化学 · 分子生物学 · 分析化学 · 生物技术
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

A reproducible electrochemical biosensor for tobramycin highly sensitive detection based on ExoIII-assisted nucleic acid circulation and CHA reaction

Chi Zhang,Gaiping Li,Baoxian Ye,Lina Zou,Weihang Wang,Yanli Ji

Based on ExoIII-assisted nucleic acid circulation and catalytic hairpin assembly (CHA) reaction, a dual-amplification electrochemical biosensors strategy for sensitive detection of tobramycin was presented. When the target was present, the trigger 1 (T1) was released to unfold hairpin DNA (H1), which allowed the ExoIII-assisted nucleic acid circulation to proceed smoothly and create a lot of trigger 2(T2). Following that, the CHA reaction between H2 and H3 proceeded under the catalysis of T2 and produced plenty of H2-H3 complex. Signal probe labeled with ferrocene was immobilized on the electrode ahead by adenine (PolyA). Finally, the H2-H3 complex combined with the probe and the DNA strand labeled with ferrocene (C2) fell off the electrode surface. The above process significantly reduced the electrochemical signal, so the biosensor has a low detection limit of 0.11 nM. Moreover, this biosensor has a satisfactory regenerability.

CAS / MDL: 32986-56-4
研究领域: 生物化学 · 分析化学 · 生物技术
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Efficient SERS substrate HOF@Au synergistically CHA-mediated double-end DNA walker as high-efficient signal amplification strategy to achieve ultra-sensitive detection of roxithromycin

Yi He,Xiaoyu Yang,Shunbi Xie,Runzi Zhang,Yao Liu,Mengjun Wang

Roxithromycin (ROX) is an effective antibiotic, but its prolonged administration may lead to hepatotoxicity and other side effects. To address this concern, the present study introduced a novel strategy that integrated a CHA-mediated dual-end DNA walker with hydrogen-bonded organic frameworks (HOFs) combined with Au nanoparticles (NPs) as efficient SERS substrates, enabling highly sensitive detection of ROX in food. Notably, HOF possessed a large specific surface area and strong adsorption properties that making it excellent platforms for the in-situ synthesis of abundant Au NPs and contributed to robust and uniform SERS signals. When ROX was present, it can trigger the activation of CHA and resulting the formation of a dual-end DNAzyme structure. Meanwhile, under the catalytic action of Mg 2+ , DNAzyme initiated the DNA walker mechanism and generated a substantial amount of Output DNA. Moreover, the Au@4-NTP@Ag core-shell structure generated numerous SERS “hot spots” and combined with the signal-amplifying capability of HOF@Au, leading to a remarkable improvement in SERS sensitivity. Based on this mechanism, the developed sensor employs a “signal-on” strategy for ultra-sensitive detection of ROX, achieving a detection range from 1.0 × 10 −6 to 1.0 × 10 −13  mol/L with a detection limit of 3.72 × 10 −14  mol/L. Furthermore, the method had been successfully applied to the detection of ROX in real food samples, including milk and honey, offering a promising and innovative framework for the development of next-generation SERS biosensors. This approach demonstrated significant potential for highly selective and sensitive antibiotic monitoring in food safety applications.

研究领域: 分析化学 · 生物传感器 · 纳米技术 · 食品安全 · 抗生素检测
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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

Sensitive electrochemical detection of oxytetracycline based on target triggered CHA and poly adenine assisted probe immobilization

Weihang Wang,Chi Zhang,Jiaxin Guo,Gaiping Li,Baoxian Ye,Lina Zou

Here, we developed a homogeneous electrochemical biosensor for the sensitive determination of antibiotic by the CHA reaction and the consecutive adenine mediated probe fixation. The binding of target to the target recognition sequences in the triple-helix DNA can release the trigger. It can initiate the catalytic hairpin assembly (CHA) to generate lots of mimic targets, which were labeled with electroactive substance ferrocene (Fc). Because the generated mimic target has consecutive sequence of adenines (PolyA), they can be self-assembled on the AuNPs modified electrode and finally realize electrochemical detection . Under optimal conditions, this developed biosensor achieved a satisfactory limit of detection of 0.089 nM (S/N = 3) and a linear range from 0.1 nM to 100 nM for sensitive detection of oxytetracycline with good specificity. The whole process is carried out in homogeneous solution, not only realizes signal amplification, but also avoids the complex modification process of electrode surface. Compared with some reported electrochemical sensors , the method is easier to operate and has good precision.

CAS / MDL: 79-57-2
研究领域: 分析化学 · 生物传感器 · 电化学 · 纳米技术
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Chemistry-An Asian Journal · 2023 · IF 4.1

Ultrasensitive miRNA detection by AuNP-based 3D DNA walker and catalytic hairpin assembly (CHA) cascade amplification for early cancer diagnosis

Junyou Li,Hung-Wing Li

By combining exquisitely designed hairpins with the catalytic hairpin assembly to form tripedal DNA walkers driven by enzyme, we constructed a 3D DNA walker with accordingly complementary hairpins attached on gold nanoparticles (AuNPs) and sensitive fluorescence sensing system for the sensitive detection of target miRNA-21. The presence of miR-21 triggers the CHA among three hairpins, which lead to the formation of the tripedal DNA walkers. For the walking trajectories, FAM-labeled hairpins were attached to the surface of AuNPs, the fluorescence of which was initially quenched due to its close proximity to AuNPs. After the binding/cleaving/moving process of tripedal DNA walkers with HP4 driven by Exonuclease III (Exo III), a number of single-stranded DNAs (ssDNAs) will be released with FAM fluorescence recovered. Benefiting from the DNA walker and CHA cascade amplification, the proposed sensing strategy showed remarkable improvement in sensitivity with the LOD of 46 aM. Also, the system was practically applied in human serum samples, demonstrating satisfactory outcome. Owing to the precise design of the system, this method exhibited excellent specificity to distinguish miR-21 from its single-, double-mismatched sequences and non-complementary sequences, showing great versatility and potential for the biological analysis and early disease diagnosis.

研究领域: 生物技术 · 纳米技术 · 癌症诊断 · 分子生物学 · 分析化学
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BIOSENSORS & BIOELECTRONICS · 2021 · IF 10.618

Dual CHA-mediated high-efficient formation of a tripedal DNA walker for constructing a novel proteinase-free dual-mode biosensing strategy

Wan Huang,Danyan Zhan,Yiming Xie,Xin Li,Guosong Lai

DNA walkers have been recognized as a type of powerful signal amplification tool for biosensors, but how to adopt a proper strategy to increase their amplification efficiency is still highly desirable. Herein we design a dual-catalytic hairpin assembly (CHA)-mediated strategy for the high-efficient formation of a tripedal Mg 2+ -dependent DNAzyme (MNAzyme)-DNA walker, and thus develop a novel proteinase-free dual-mode biosensing method for the kanamycin (Kana) antibiotic assay. The first CHA is initiated by a target-biorecognition reaction, which can produce the DNA walker and also induce the target recycling. The second CHA is initiated by a special base sequence designed as a one-half substrate of the MNAzyme. Upon the first CHA-triggered DNA walking at a magnetic bead (MB) track, this “pseudo-target” sequence can be released to induce another CHA-cycle for the formation of the same DNA walker. Meanwhile, the other one-half substrate strand exposed on the MB surface will trigger the quantitative hybridization chain reaction (HCR)-assembly of a G-quadruplex DNAzyme (G-DNAzyme)-enriched double-stranded DNA polymer. So the enzymatic reaction of G-DNAzymes enabled the convenient colorimetric and photoelectrochemical dual-mode signal transduction of the method. Due to the dual-CHA facilitation to the tripedal and three-dimensional DNA walking and synergetic signal amplification of HCR, this method exhibits very low detection limits of 9.4 and 0.55 fg mL −1 , respectively. In combination with its wide linear range, automated manipulation, and excellent selectivity , repeatability and reliability, the proposed method is expected to be used for the convenient semiquantitative screening and accurate determination of possible antibiotic residues in complicated matrices.

研究领域: 生物化学 · 分析化学 · 生物传感器 · 纳米技术
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JOURNAL OF POROUS MATERIALS · 2025 · IF 3.2

Template-free synthesis of low-silica chabazite zeolite aggregates in K+/Sr2+ system by in situ hydrothermal growth

Qian Yi,Jiang Qingqing,Xiang Shimeng,Lu Zhenhao,Xu Xiaowen,Yang Jing,Dai Guoliang,Song Ruifeng,Jiang Ji

Separating CO 2 and N 2 from CH 4 is crucial for energy production and environmental protection. This study showed the rapid synthesis of CHA zeolites with different morphologies using an in situ growth method, without the assistance of organic structure directing agents (OSDA) or fluoride media. The crystallization behavior of CHA zeolites was studied in terms of synthesis gel composition (including water content, silicon and aluminum content, alkalinity and Sr 2+ concentration), synthesis temperature and duration. The results suggested that pure phase CHA zeolite nano-aggregates could be synthesized with broad precursor conditions at 150 °C for only 4 h. Then, K-CHA zeolite was ion-exchanged to Na-CHA and Ca-CHA and the adsorption properties of CHA zeolites with different morphologies and ions were studied. The results suggested that Na-CHA exhibited highest CH 4 , CO 2 and N 2 adsorption capacity and showed higher ideal selectivity for N 2 /H 2 ; Although Ca-CHA zeolites exhibited relative lower CO 2 and CH 4 adsorption capacity, it exhibited the highest ideal selectivity for CO 2 /CH 4 ; Simultaneously, K-CHA zeolite exhibited high CH 4 adsorption capacity and high adsorption separation ability of CH 4 /N 2 . Furthermore, breakthrough experiments have confirmed the practical feasibility of separating CO 2 from CH 4 .

CAS / MDL: 10042-76-9
研究领域: 材料科学 · 化学工程 · 吸附与分离 · 分子筛合成 · 气体分离
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RSC Advances · 2021 ·Vol. 11 ·期 10 ·5506-5511 · IF 3.361

Highly sensitive and selective detection of PCB 77 using an aptamer-catalytic hairpin assembly in an aquatic environment

Lin Yuan,Qiang Fu,Maojuan Zhou,Yunqian Ma,Lihua Zang,Yingjian Qin,Dandan Ji,Fengshan Zhang

Polychlorinated biphenyls (PCBs) are synthetic organic compounds that are extremely difficult to break down in water and can accumulate in human fat and organisms. However, methods that can be used to detect large amounts of PCBs remain unsatisfactory, as they are generally overly sensitive and involve complex operations. An aptamer-based catalytic hairpin assembly (aptamer-CHA) reaction for the selective detection of 3,3′,4,4′-tetrachlorobiphenyl (PCB 77) was developed. It combines the advantages of aptamers and signal amplification reactions. The aptamer selectivity recognizes the target, PCB 77, which triggers the sensitive CHA reaction to produce a fluorescence signal. CHA is a sensitive enzyme-free signal amplification method suitable for on-site detection. Therefore, the identification aptamer is the basis for the quantitative detection of PCB 77, with a detection range of 0.01 μg L−1 to 500 μg L−1 and a detection limit of 0.01 μg L−1. In this study, the aptamer was used to improve the selectivity of the reaction, and the CHA reaction improved the sensitivity of the detection system. Such high-sensitivity PCB detection capabilities with simplified procedures may be useful for real-time field detection and other monitoring tasks. This method can be used as a rapid fluorescence detection strategy for other targets in aquatic environments.

研究领域: 环境科学 · 分析化学 · 分子生物学
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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 27 ·9398-9405 · IF 4

Facile synthesis of aluminosilicate zeolites with STT, CHA and MWW topology structures

Yuliang Guo,Peilun Li,Zhengchang Wei,Guangjun Wu,Landong Li

Efficient synthesis of zeolites with different topologies is of great significance for both fundamental research and industrial application. Herein, the SSZ-23 zeolite, an odd zeolite containing 7-membered ring (7-MR) and 9-MR channels, has been synthesized under fluorine-free conditions via the route of pre-aging and pH regulation. By this novel synthesis route, the crystallization time can be significantly shortened to 3 days, nearly half as that by the conventional route in fluoride media. The pH value of the aging gel, i.e., the basicity, is found to play a key role in the synthesis, as SSZ-13 and SSZ-25 zeolites can be synthesized simply by changing the basicity of the same aging gel. Characterization results indicate that decreasing the basicity can promote the condensation between Si and Si/Al species and thus increase the framework density of the resulting zeolites. Finally, the dimethyl ether (DME) carbonylation reaction is employed to evaluate the catalytic properties of the above three zeolites with an identical chemical composition, and to reveal the unique confinement effect in various zeolite topologies.

研究领域: 材料科学 · 催化化学
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