Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Xihong Guo,Ying Li,Huan Huang,Dongmei Wang,Rongli Cui,Jialiang Li,Yidong Zhao,Dan Wang,Hui Yuan,Jinquan Dong,Baoyun Sun
Graphdiyne-based materials are promising candidates for the adsorption and detection of heavy metal ions (HMIs) as the acetylenic links in graphdiyne strongly interact with some metal ions. To improve the sensing performance of graphdiyne-based materials and further understand their detection mechanism, we prepared N-substituted graphdiyne (TGDY) through bottom-up method as electrode modified materials, which contained position-fixed and content-controlled alkynyl bonds and pyridine N atoms. By comparing with the H-substituted graphdiyne (HGDY), which was roughly the same in structure as TGDY except that the benzene ring without N atoms, we found that the introduction of N in TGDY greatly improves the electrochemical performance and the signal intensity is closely related to the number of detection sites. Furthermore, the performance of TGDY-based electrochemical sensor was also explored, which showed satisfactory selectivity , reproducibility, stability and applicability for the detection of Cd 2+ and Pb 2+ in water. Our work provided an important reference for rational design and synthesis of electrode materials through bottom-up method to improve the detection performance and explore the detection mechanism.
研究领域:
材料科学
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环境科学
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分析化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Tao Wang,Qiang Bai,Zhiling Zhu,Hailian Xiao,Fuyi Jiang,Fanglin Du,William W. Yu,Manhong Liu,Ning Sui
Multifunctional enzymatic nanomaterials (nanozymes) with good biocompatibility, strong enzymatic activity, and substrate specificity are the desired alternatives to natural enzymes. Here, the design of a peroxidase mimetic nanozyme capable of detecting and depleting glutathione (GSH) in the bacterial cells is presented. The nanozyme palladium-iron nanostructure decorated graphdiyne nanosheet (PdFe/GDY) was prepared by a facile hydrothermal approach. It can efficiently catalyze the decomposition of H 2 O 2 to produce •OH by a peroxidase-like mechanism. Surprisingly, the PdFe/GDY nanozymes can detect GSH in bacteria with excellent specificity and ultra-low detection limit of 24.45 nM. Moreover, the PdFe/GDY nanozymes can consume GSH for bacterial disinfection with killing efficacy > 99.99%, promote wound healing and do not cause significant toxicity in vitro and in vivo . To our knowledge, this is the first example of a GDY-based nanozyme biosensor and antibacterial agent. Collectively, this work would be indicative to construct GDY-based nanozymes in clinical diagnosis and sterilization.
研究领域:
生物化学
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纳米技术
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生物医学工程
✓ 已验证
DOI
高影响因子
CARBON
·
2020
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IF 8.821
Yan Lv,Xueyan Wu,Wei Jia,Jixi Guo,Hongbo Zhang,Huibiao Liu,Dianzeng Jia,Fenglian Tong
Structural and interface engineering enable the optimization of electrocatalysts in terms of both activity and durability. Herein, the three-dimensional (3D) architecture graphdiyne nanowall (GDY) serving as scaffolds anchor metal cations to form the NiFe layered double hydroxide (LDH) nanodots/graphdiyne (NiFe ND/GDY) heterojunction electrocatalysts for water oxidation in alkaline solution. After tuning the loading amount of NiFe-LDH carefully, the NiFe ND displays ultrasmall nanometer size of 2.7 nm and intimate interfacial coupling with GDY. Owing to the optimized 0D/3D structure, strong interfacial forces and the unique properties of GDY, the resulting NiFe ND/GDY requires an overpotential of only 252 mV to deliver current density of 10 mA cm −2 and shows favorable kinetics with a small Tafel slope of 39.70 mV dec −1 . Notably, the mass activity of NiFe ND/GDY heterojunction is 70 times higher than that of the commercial RuO 2 (631 A g −1 vs. 9 A g −1 to RuO 2 , at η = 300 mV), and it exhibits a superior long-term stability (only 10% degradation during continuous electrolysis of 100 h). This work indicates that GDY can serve as a promising substrate to anchor the ultrafine nanoparticle catalysts for water oxidation or beyond.
研究领域:
材料科学
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电化学
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纳米技术
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催化
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2020
·
IF 3.594
Jing Xiao,Hao Wang,Chunxiang Li,Keqin Deng,Xiaofang Li
High-quality tremella-like graphdiyne (GDY) nanotubes composed of intertwined ultrathin nanosheets were acidified. Shortened and acidified multi-walled carbon nanotubes (S-MWCNTs) were simply blended with GDY in a certain proportion to modify glassy carbon electrode (GCE). Electrochemical behavior of DA was studied on different modified electrodes . GDY showed high preconcentration to DA. S-MWCNTs facilitated the electron transport and promoted the oxidation of DA. Differential pulse voltammetry (DPV) was applied to determine low concentrations of DA. It exhibited a linear response in the concentration range of 0.02 to 20.0 μM with an estimated detection limit of 8.6 nM (S/N = 3). This sensor showed excellent performances for detection of DA in biological fluids.
研究领域:
分析化学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2018
·Vol. 31
·期 6
·1806272
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IF 21.95
Fan Wang,Zicheng Zuo,Liang Li,Feng He,Fushen Lu,Yuliang Li
The structural and interfacial stabilities of metal oxides (MOs) are key issues while facing the volumetric variation and intensive interfacial polarization in electrochemical applications, including lithium-ion batteries (LIBs), supercapacitors, and catalysts. The growth of a seamless all-carbon interfacial layer on MOs with complex dimensions is not only a scientific problem, but also a practical challenge in these fields. Here, the growth of graphdiyne under ultramild condition is successfully implemented in situ for coating MOs of complex dimensions. The seamless all-carbon interface and conductive network are formed at the same time. This method cleverly avoids the structural degradation of MOs at a high temperature in the presence of traditional carbon materials. Under the protection of the high-quality graphdiyne layer, the samples as LIB anodes deliver high performances in terms of Coulomb efficiency, capacity, long-term retention, and structural and interfacial stabilities. Both experimental achievements and theoretical calculations demonstrate that the graphdiyne is a particular protection layer for MOs and plays a crucial role for preventing the structural and interfacial degradation of the electrode. Furthermore, the universality of this method will promote the potential applications of many promising MOs in other electrochemical fields.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2022
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IF 6.911
Yang-Yang Hou,Wan-Zhen Xie,Ke-Jing Huang,Jing Xu
A novel self-powered biosensor is engineered by the integration of DNAzyme walker and AuNPs/graphdiyne biosensing interface, realizing sensitive detection of target microRNA . The cleverly constructed DNAzyme walker with outstanding signal transduction ability to obtain an amplified signal response. In addition, the AuNPs/graphdiyne significantly improves electron transport speed of biosensing interface for improving the sensitivity of biosensor. A dynamic linear range of 0.05 fM-10 pM with a low detection limit of 0.015 fM (S/N = 3) is obtained by utilizing the self-powered biosensor. Meanwhile, the developed self-powered biosensor is capable of assaying miRNA-21 in human serum samples with satisfactory recoveries. This strategy provides a valid method for the sensitive microRNA detection, and shows great potential in point-care detection of tumor biomarker.
研究领域:
生物传感器
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分子生物学
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纳米技术
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2023
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IF 7.1
Chao Zhang,Huike Zhang,Xin Wan,Yue Xie,Michael J. Bentel,Zhanjiang Yu,Zhenguo Chen,Jiaan He,Junlang Li,Xuezhu Xiang,Xinzhi Wang,Zhaoli Wang,Guang-Guo Ying,Dionysios D. Dionysiou,Mingzhi Huang
Pollution removal via peroxymonosulfate (PMS)-mediated advanced oxidation processes provides an effective approach for water remediation. Although numerous carbon allotropes have been applied in PMS activation, the application of graphdiyne-based catalysts has been practically unexplored in this process despite their excellent electronic properties. In this study, the first instance of exploiting N-doped graphdiyne nanotubes (NGNTs) for metal-free PMS activation is presented to remove recalcitrant heterocyclic contaminants in aqueous environments. This mechanistic study demonstrates that the NGNT–PMS system decomposes heterocyclic contaminants via electron-transfer-mediated nonradical oxidation, where metastable NGNT–PMS* complexes were the primary oxidants. The apparent reaction rate constant for the NGNT–PMS system is 2.4 and 3.1 times higher than those for the counterpart systems by N-doped carbon nanotubes (NCNTs) and graphene oxide (NGO) systems, respectively. The NGNT exhibits excellent N-doping potential, demonstrated by a 7-fold increase in atomic nitrogen compared to NCNT in an identical N-doping procedure. The possible N-doping sites in NGNT were determined as mainly sp-N-1, sp-N-2, pyridinic-N, amino-N, and graphitic-N atoms by the N K-edge X-ray absorption near-edge structure spectra and X-ray photoelectron spectroscopy. Theoretical calculations demonstrate the relatively obvious electron transfer between PMS and different N-sites in NGNT, indicating the possible formation of NGNT–PMS* complexes. Additionally, the NGNT–PMS system plays an important role in the cleavage of pyridine heterocycles and C–Cl bonds as demonstrated by the destruction of nitenpyram. This study provides mechanistic insights into the roles of NGNT in the metal-free activation of PMS for the remediation of recalcitrant heterocyclic contaminants.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 11
·3072-3083
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IF 7.3
Chuanqi Pan,Biluan Zhang,Tingyu Pan,Hui Huang,Siyi Song,Xitong Cai,Yuhang Wang,Hongwei Sun,Zhu Luo,Lizhi Zhang,Yanbing Guo
The dual activation mechanism of molecular oxygen (O2) and water (H2O) in the local structure of catalysts has not been elucidated yet. Herein, we report a strategy for manufacturing fully exposed Ag4 sites in nano silver/graphdiyne (Ag/GDY) composites for activating O2 and H2O. The synthesized nano Ag was uniformly anchored on the surface of GDY without any surfactant added, with an average particle size of 2.5 nm. The unique sp-hybrid C and triangular pore structure of GDY not only regulate the stable geometric structure of nano Ag, but also enhance the adsorption ability of Ag4 sites for O2 and H2O molecules in nano Ag/GDY. Electron spin resonance spectroscopy and density functional theory calculation results proved that O2 is more favorable to synergistically promote the activation of H2O to generate reactive ·O2− and ·OH radicals on the nano Ag/GDY surfaces, leading to outstanding antibacterial activity. This work provides a simple strategy for the preparation of stable nano Ag and proposes to improve the catalytic oxidation activity by adjusting the local electronic structure of catalysts to activate O2 and H2O.
研究领域:
材料科学
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催化化学
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微生物学
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2022
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IF 12.545
Kai Niu,Zicheng Zuo,Xianbo Lu,Lili Zou,Jiping Chen
There is an urgent need for developing electrochemical biosensor based on the acetylcholinesterase (AChE) inhibition to real-time analysis of organophosphorus pesticides (OPs), but it is suffered from the sluggish electrode kinetics and high oxidation potential toward signal species. Herein, a nanocomposite of ultrafine Cu quantum dots (QD) uniformly loaded on three-dimensional ultrathin graphdiyne (GDY) nanosheets (denoted as Cu@GDY) was synthesized via a one-step strategy, which showing high-density of active sites with persistent stability. Then an AChE biosensor based on Cu@GDY was fabricated to detect OPs, and the results revealed that the Cu@GDY nanocomposite can significantly amplifies electrochemical signal and reduces the oxidation potential for OPs. The strong interaction between active site of Cu@GDY and thiocholine signal species caused rapid analyte aggregation and decreased the reaction activation energy of thiocholine electro-oxidation. Benefiting from the excellent catalytic activity of Cu@GDY nanocomposite and reasonable regulation of enzyme inhibition kinetics , the biosensor achieved rapid and sensitive detection of OPs with a detection limit of 1 μg L −1 for paraoxon . Furthermore, the biosensor demonstrated great reproducibility, good stability and high recovery rate for OPs detection in real samples. Cu@GDY based sensor also displayed high catalytic activities and good selectivity to the non-enzymatic detection of glucose in alkaline medium . Cu@GDY offers a versatile and promising platform for sensors and biosensors featuring remarkably enhanced activity and stability, and can be applied to many other fields as desirable electrocatalyst .
研究领域:
分析化学
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生物传感
·
电催化
✓ 已验证
DOI
PubMed
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 5
·1999-2014
·
IF 9.6
Li Mei,Wang Jing-Zhi,Jin Zhi-Liang
In the process of photocatalytic water cracking, the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the catalyst. In this paper, a carbon isotope superconducting material graphdiyne (GDY) is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn 0.5 Co 0.5 S/MoS 2 inorganic system. In terms of hydrogen evolution kinetics, GDY acts as an electron bridge, not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated charges. Morphologically, the large two-dimensional layer provides more loading and anchoring points for Zn 0.5 Co 0.5 S/MoS 2 , which increases the number of active sites. The ternary composite catalyst 20%GDY/Zn 0.5 Co 0.5 S/Mo 2 S (20-GCSM) generates 69.94 μmol of hydrogen (5 h) in triethanolamine solution. It is 2.97 and 1.80 times higher than Zn 0.5 Co 0.5 S and Zn 0.5 Co 0.5 S/MoS 2 , respectively. After the cyclic experiment, it still has stable hydrogen evolution performance after standing for 24 h (under dark conditions). In addition, the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron spectroscopy. This work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges. Graphical abstract
研究领域:
材料科学
·
催化
·
纳米技术
·
能量转换
·
固体物理
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 5
·1-9
·
IF 5.3
Li Rui,Que Wenzhong,Han Haiyan,Shi Honghui,Wang Rongfeng,Qiu Bin
IL-17 (interleukin-17) is a common proinflammatory cytokine and can be adopted as an important biomarker for several diseases; it is thus very necessary to design an effective method for monitoring IL-17. Herein, by preparing silver nanoparticles/graphdiyne (Ag/GDY) with simple electroless deposition as the sensing platform and methylene blue/UiO-66-NH 2 MOFs (MB/MOFs) as the signaling-amplifier, a highly efficient sandwich-like electrochemical immunosensing (SLEI) platform was designed for IL-17 detection. The superior electrical property, easy preparation, large surface area, and high stability of Ag/GDY make it a desirable substrate to immobilize primary antibody of IL-17. Meanwhile, the unique structure of UiO-66-NH 2 is beneficial to immobilize MB probe and secondary antibody. By optimizing experimental conditions, the MB current obtained at the as-designed SLEI platform increases along with IL-17 increase, and the related linearity is 1.0 pg mL −1 –1.0 ng mL −1 coupled with a low detection limit of 0.3 pg mL −1 . It is expected that the SLEI platform based on Ag/GDY and MB/MOFs shows some potential application for IL-17 detection. Graphical abstract
研究领域:
生物医学工程
·
免疫学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
International Journal of Nanomedicine
·
2024
·
IF 6.6
Wenjie Xie,Yixun Zhang,Qianfeng Xu,Guowei Zhong,Jundong Lin,Huichan He,Qiuling Du,Huijing Tan,Muqi Chen,Zhenjie Wu,Yulin Deng,Zhaodong Han,Jianming Lu,Jianheng Ye,Fen Zou,Yangjia Zhuo,Weide Zhong
Purpose Current treatment approaches for Prostate cancer (PCa) often come with debilitating side effects and limited therapeutic outcomes. There is urgent need for an alternative effective and safe treatment for PCa.Methods We developed a nanoplatform to target prostate cancer cells based on graphdiyne (GDY) and a copper-based metal-organic framework (GDY-CuMOF), that carries the chemotherapy drug doxorubicin (DOX) for cancer treatment. Moreover, to provide GDY-CuMOF@DOX with homotypic targeting capability, we coated the PCa cell membrane (DU145 cell membrane, DCM) onto the surface of GDY-CuMOF@DOX, thus obtaining a biomimetic nanoplatform (DCM@GDY-CuMOF@DOX). The nanoplatform was characterized by using transmission electron microscope, atomic force microscope, X-ray diffraction, etc. Drug release behavior, antitumor effects in vivo and in vitro, and biosafety of the nanoplatform were evaluated.Results We found that GDY-CuMOF exhibited a remarkable capability to load DOX mainly through π-conjugation and pore adsorption, and it responsively released DOX and generated Cu+ in the presence of glutathione (GSH). In vivo experiments demonstrated that this nanoplatform exhibits remarkable cell-killing efficiency by generating lethal reactive oxygen species (ROS) and mediating cuproptosis. In addition, DCM@GDY-CuMOF@DOX effectively suppresses tumor growth in vivo without causing any apparent side effects.Conclusion The constructed DCM@GDY-CuMOF@DOX nanoplatform integrates tumor targeting, drug-responsive release and combination with cuproptosis and chemodynamic therapy, offering insights for further biomedical research on efficient PCa treatment.
研究领域:
肿瘤学
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纳米技术
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药学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）