165 results on '"Yi-Tao Long"'
Search Results
2. Pore confined time-of-flight secondary ion electrochemical mass spectrometry
- Author
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Jun-Gang Wang, Ru-Jia Yu, Xin Hua, and Yi-Tao Long
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General Chemistry - Abstract
This review highlights the important historical and technological developments of in situ ToF-SIEMS technique, especially, the challenges encountered when extending ToF-SIMS from a high vacuum condition to a liquid electrochemical environment.
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- 2023
3. Profiling the chemistry- and confinement-controlled sensing capability of an octameric aerolysin-like protein
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Xue-Yuan Wu, Jie Jiang, Jun-Ge Li, Meng-Yin Li, and Yi-Tao Long
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Materials Chemistry ,Metals and Alloys ,Ceramics and Composites ,General Chemistry ,Catalysis ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials - Abstract
Octameric Aep1 shows unique suitability for the gamma-cyclodextrin (γ-CD) adapter with 8 subunits, enabling the discrimination for β-nicotinamide mononucleotide.
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- 2023
4. Identification of Single Amino Acid Chiral and Positional Isomers Using an Electrostatically Asymmetric Nanopore
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Jiajun Wang, Jigneshkumar Dahyabhai Prajapati, Fan Gao, Yi-Lun Ying, Ulrich Kleinekathöfer, Mathias Winterhalter, and Yi-Tao Long
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Nanopores ,Amyloid beta-Peptides ,Colloid and Surface Chemistry ,Isomerism ,Static Electricity ,Escherichia coli ,Amino Acid Sequence ,General Chemistry ,Amino Acids ,Biochemistry ,Catalysis - Abstract
Chirality is essential in nearly all biological organization and chemical reaction but is rarely considered due to technical limitations in identifying L/D isomerization. Using OmpF, a membrane channel from E. coli with an electrostatically asymmetric constriction zone, allows discriminating chiral amino acids in a single peptide. The heterogeneous distribution of charged residues in OmpF causes a strong asymmetric electrostatic field at the constriction. This asymmetry forces the sidechains of the peptides to specific orientations within OmpF, causing distinct ion current fluctuations. Using a statistical analysis of the respective ion current variations allows distinguishing the presence and position of each chiral amino acid. To explore potential applications, the disease-related peptide β-Amyloid, and its D-Asp1 isoform, as well as a mixture of the Icatibant peptide drug (HOE 140) and its D-Ser7 mutant, have been discriminated. Both chiral isomers were not applicable to be distinguished by mass spectrum approaches. These findings highlight a novel sensing mechanism for identifying single amino acids in single peptides and even for achieving single-molecule protein sequencing.
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- 2022
5. Observing Confined Local Oxygen‐induced Reversible Thiol/Disulfide Cycle with a Protein Nanopore
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Wei Liu, Chao‐Nan Yang, Zhong‐Lin Yang, Ru‐Jia Yu, Yi‐Tao Long, and Yi‐Lun Ying
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General Medicine ,General Chemistry ,Catalysis - Published
- 2023
6. Controlled Genetic Encoding of Unnatural Amino Acid in Protein Nanopore
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Xue-Yuan Wu, Meng-Yin Li, Shao-Jun Yang, Jie Jiang, Yi-Lun Ying, Peng R. Chen, and Yi-Tao Long
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General Medicine ,General Chemistry ,Catalysis - Published
- 2023
7. Editorial: Nanopore Electrochemistry
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Yi‐Tao Long, Meni Wanunu, and Mathias Winterhalter
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Organic Chemistry ,General Chemistry ,Biochemistry - Published
- 2023
8. Monitoring Photoinduced Interparticle Chemical Communication In Situ
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Mengjie Chen, Si‐Min Lu, Hao‐Wei Wang, and Yi‐Tao Long
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General Chemistry ,General Medicine ,Catalysis - Published
- 2023
9. SmartImage: A Machine Learning Method for Nanopore Identifying Chemical Modifications on RNA
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Shijia Li, Xinyi Li, Yong‐Jing Wan, Yi‐Lun Ying, Ru‐Jia Yu, and Yi‐Tao Long
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Organic Chemistry ,General Chemistry ,Biochemistry - Abstract
RNA modifications modulate essential cellular functions. However, it is challenging to quantitatively identify the differences in RNA modifications. To further improve the single-molecule sensing ability of nanopores, we propose a machine-learning algorithm called SmartImage for identifying and classifying nanopore electrochemical signals based on a combination of improved graph conversion methods and deep neural networks. SmartImage is effective for nearly all ranges of signal duration, which breaks the limitation of the current nanopore algorithm. The overall accuracy (OA) of our proposed recognition strategy exceeded 90% for identifying three types of RNAs. Prediction experiments show that the SmartImage owns the ability to recognize one modified RNA molecule from 1000 normal RNAs with OA90%. Thus our proposed model and algorithm hold the potential application in clinical applications.
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- 2022
10. 3D Blockage Mapping for Identifying Familial Point Mutations in Single Amyloid‐β Peptides with a Nanopore
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Kai‐Li Xin, Zheng‐Li Hu, Shao‐Chuang Liu, Xin‐Yi Li, Jun‐Ge Li, Hongyan Niu, Yi‐Lun Ying, and Yi‐Tao Long
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Nanopores ,Amyloid beta-Peptides ,Alzheimer Disease ,Mutation ,Humans ,Point Mutation ,General Medicine ,General Chemistry ,Peptide Fragments ,Catalysis - Abstract
Accurate discrimination of amyloid-β (Aβ) peptides containing familial point mutations would advance the knowledge of their roles in early-onset Alzheimer's disease. Herein, we simultaneously identified the mutant A21G, E22G, E22Q, and the wild-type (WT) Aβ
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- 2022
11. Single‐Molecule Frequency Fingerprint for Ion Interaction Networks in a Confined Nanopore
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Yong-Jing Wan, Xi-Xin Fu, Yi-Lun Ying, Xinyi Li, and Yi-Tao Long
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Physics::Biological Physics ,Quantitative Biology::Biomolecules ,Materials science ,Nanoelectrochemistry ,General Medicine ,General Chemistry ,Electrochemistry ,Catalysis ,Characterization (materials science) ,Ion ,Quantitative Biology::Subcellular Processes ,Nanopore ,Amplitude ,Physics::Plasma Physics ,Chemical physics ,Fingerprint ,Molecule ,Physics::Chemical Physics - Abstract
The transport of molecules and ions through biological nanopores is governed by interaction networks among restricted ions, transported molecules, and residue moieties at pore inner walls. However, identification of such weak ion fluctuations from only few tens of ions inside nanopore is hard to achieve owing to electrochemical measurement limitations. Here, we developed an advanced frequency method to achieve qualitative and spectral analysis of ion interaction networks inside a nanopore. The peak frequency fm reveals the dissociation rate between nanopore and ions; the peak amplitude am depicts the amount of combined ions with the nanopore after interaction equilibrium. A mathematical model for single-molecule frequency fingerprint achieved the prediction of interaction characteristics of mutant nanopores. This single-molecule frequency fingerprint is important for classification, characterization, and prediction of synergetic interaction networks inside nanoconfinement.
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- 2021
12. Understanding the Dynamic Potential Distribution at the Electrode Interface by Stochastic Collision Electrochemistry
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Jianfu Chen, Yi-Tao Long, Hui Ma, Yue-Yi Peng, Haifeng Wang, Wei Ma, Peijun Hu, and Si-Min Lu
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Distribution (number theory) ,Chemistry ,Nanoparticle ,General Chemistry ,Electrode interface ,Electrochemistry ,Collision ,Biochemistry ,Catalysis ,Colloid and Surface Chemistry ,Chemical physics ,Electrode ,Nanoscopic scale ,Electrode potential - Abstract
The potential distribution at the electrode interface is a core factor in electrochemistry, and it is usually treated by the classic Gouy-Chapman-Stern (G-C-S) model. Yet the G-C-S model is not applicable to nanosized particles collision electrochemistry as it describes steady-state electrode potential distribution. Additionally, the effect of single nanoparticles (NPs) on potential should not be neglected because the size of a NP is comparable to that of an electrode. Herein, a theoretical model termed as Metal-Solution-Metal Nanoparticle (M-S-MNP) is proposed to reveal the dynamic electrode potential distribution at the single-nanoparticle level. An explicit equation is provided to describe the size/distance-dependent potential distribution in single NPs stochastic collision electrochemistry, showing the potential distribution is influenced by the NPs. Agreement between experiments and simulations indicates the potential roles of the M-S-MNP model in understanding the charge transfer process at the nanoscale.
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- 2021
13. An Envelope Algorithm for Single Nanoparticle Collision Electrochemistry †
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Chun-Yu Xu, Yong-Jing Wan, Ru-Jia Yu, Yi-Tao Long, Xi-Xin Fu, Su-Wen Xu, Xue Ni, and Yi-Lun Ying
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Savitzky–Golay filter ,Chemistry ,Nanoparticle ,General Chemistry ,Electrochemistry ,Collision ,Molecular physics ,Envelope (waves) - Published
- 2021
14. Biological Nanopore Approach for Single‐Molecule Protein Sequencing
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Yi-Tao Long, Yi-Lun Ying, Ming-Zhu Huo, and Zheng-Li Hu
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Models, Molecular ,chemistry.chemical_classification ,010405 organic chemistry ,Chemistry ,Proteins ,Peptide ,General Medicine ,General Chemistry ,Computational biology ,010402 general chemistry ,Proteomics ,01 natural sciences ,Catalysis ,DNA sequencing ,0104 chemical sciences ,Amino acid ,Nanopores ,Nanopore ,Protein sequencing ,Sequence Analysis, Protein ,Native protein ,Molecule - Abstract
Proteins are responsible for the occurrence and treatment of many diseases, and therefore protein sequencing will revolutionize proteomics and clinical diagnostics. Biological nanopore approach has proved successful for single-molecule DNA sequencing, which resolves the identities of 4 natural deoxyribonucleotides based on the current blockages and duration times of their translocations across the nanopore confinement. However, open challenges still remain for biological nanopores to sequentially identify each amino acid (AA) of single proteins due to the inherent complexity of 20 proteinogenic AAs in charges, volumes, hydrophobicity and structures. Herein, we focus on recent exciting advances in biological nanopores for single-molecule protein sequencing (SMPS) from native protein unfolding, control of peptide translocation, AA identification to applications in disease detection.
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- 2021
15. A Course of Hands-On Nanopore Experiments for Undergraduates: Single-Molecule Detection with Portable Electrochemical Instruments
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Yi-Tao Long, Xiao-Dong Yu, Xuan-Feng Kong, Jian-Rong Zhang, Zheng-Li Hu, Ming-Zhu Huo, and Yi-Lun Ying
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Science instruction ,010405 organic chemistry ,05 social sciences ,050301 education ,General Chemistry ,01 natural sciences ,0104 chemical sciences ,Education ,Nanopore ,Human–computer interaction ,Laboratory education ,ComputingMilieux_COMPUTERSANDEDUCATION ,0503 education ,Sensing system - Abstract
The prompt introduction of single-molecule science into undergraduates’ curricula is an urgent but challenging task. However, the research experiments are often too complicated and the instruments are too expensive to be widely transferred into a compulsory course of undergraduate students. Herein, we introduce a recently developed nanopore technique into an accessible laboratory course for students with the advantages of simple operation, high repeatability, and low cost. The nanopore course serves to help undergraduates in practice to understand single-molecule behaviors, think at a single molecule level, and gradually develop single-molecule solutions for scientific issues. The learning activities for undergraduate students include setup of the instrument, fabrication of a biological nanopore on an artificial lipid bilayer membrane, detection of individual oligonucleotides, and data analysis. An experiment example is single-molecule detection of the model DNA sample poly(dA)n (n = 4, 5) using the aerolysin nanopore. As our developed nanopore sensing system is simple, portable, and easy to handle, the experiment course could be implemented and popularized in undergraduates’ laboratory education. For the undergraduate students who have taken general chemistry and/or biochemistry courses, this hands-on experience of nanopore experiments would benefit them with a better understanding of the chemical world at a single-molecule level and further using single-molecule tools in various applications including DNA and/or protein sequencing.
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- 2020
16. Single-entity electrochemistry at confined sensing interfaces
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Rui Gao, Wei Wang, Yi-Lun Ying, Yi-Tao Long, Connor K. Terry Weatherly, Jiajun Wang, Lanqun Mao, Ying Jiang, Henry S. White, Anna Rose Leach, Hang Ren, Cong Xu, Paolo Actis, Andrew D. Pendergast, and Martin A. Edwards
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Chemical process ,Analyte ,Materials science ,Chemical measurement ,Interface (Java) ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,0104 chemical sciences ,Single entity ,0210 nano-technology - Abstract
Measurements at the single-entity level provide more precise diagnosis and understanding of basic biological and chemical processes. Recent advances in the chemical measurement provide a means for ultra-sensitive analysis. Confining the single analyte and electrons near the sensing interface can greatly enhance the sensitivity and selectivity. In this review, we summarize the recent progress in single-entity electrochemistry of single molecules, single particles, single cells and even brain analysis. The benefits of confining these entities to a compatible size sensing interface are exemplified. Finally, the opportunities and challenges of single entity electrochemistry are addressed.
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- 2020
17. Direct Quantification of Damaged Nucleotides in Oligonucleotides Using an Aerolysin Single Molecule Interface
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Yi-Tao Long, Yi-Lun Ying, Jiajun Wang, Jie Yang, Xue-Yuan Wu, Ya-Qian Wang, Meng-Yin Li, and Jin Huang
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chemistry.chemical_classification ,010405 organic chemistry ,Chemistry ,Oligonucleotide ,General Chemical Engineering ,Mutant ,Aerolysin ,General Chemistry ,010402 general chemistry ,01 natural sciences ,DNA sequencing ,0104 chemical sciences ,Lesion ,Nanopore ,chemistry.chemical_compound ,Biophysics ,medicine ,Nucleotide ,medicine.symptom ,QD1-999 ,DNA ,Research Article - Abstract
DNA lesions such as metholcytosine(mC), 8-OXO-guanine (OG), inosine (I), etc. could cause genetic diseases. Identification of the varieties of lesion bases are usually beyond the capability of conventional DNA sequencing which is mainly designed to discriminate four bases only. Therefore, lesion detection remains a challenge due to massive varieties and less distinguishable readouts for structural variations at the molecular level. Moreover, standard amplification and labeling hardly work in DNA lesion detection. Herein, we designed a single molecule interface from the mutant aerolysin (K238Q), whose sensing region shows high compatibility to capture and then directly convert a minor lesion into distinguishable electrochemical readouts. Compared with previous single molecule sensing interfaces, the temporal resolution of the K238Q aerolysin nanopore is enhanced by two orders, which has the best sensing performance in all reported aerolysin nanopores. In this work, the novel K238Q could discriminate directly at least three types of lesions (mC, OG, I) without labeling and quantify modification sites under the mixed heterocomposition conditions of the oligonucleotide. Such a nanopore electrochemistry approach could be further applied to diagnose genetic diseases at high sensitivity., Herein, we designed a single molecule interface from the mutant aerolysin (K238Q), whose sensing region shows high compatibility to capture and then directly convert a minor DnA lesion into distinguishable electrochemical readouts.
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- 2020
18. Single molecule sensing of amyloid-β aggregation by confined glass nanopores† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c9sc03260f
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Su-Wen Xu, Ru-Jia Yu, Si-Min Lu, Yi-Lun Ying, Yuan-Jie Li, Qun Xu, and Yi-Tao Long
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Amyloid β ,Amyloid ,010405 organic chemistry ,Chemistry ,General Chemistry ,010402 general chemistry ,01 natural sciences ,Oligomer ,0104 chemical sciences ,chemistry.chemical_compound ,Nanopore ,Adsorption ,Molecular size ,Biophysics ,Molecule ,Surface charge - Abstract
We have employed glass nanopore as a single molecule technique for direct sensing amyloidosis process of Aβ1–42 peptide, which of great significance in Alzheimer's disease., We have developed a glass nanopore based single molecule tool to investigate the dynamic oligomerization and aggregation process of Aβ1–42 peptides. The intrinsic differences in the molecular size and surface charge of amyloid aggregated states could be distinguished through single molecule induced characteristic current fluctuation. More importantly, our results reveal that the neurotoxic Aβ1–42 oligomer tends to adsorb onto the solid surface of nanopores, which may explain its instability and highly neurotoxic features.
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- 2019
19. Profiling single-molecule reaction kinetics under nanopore confinement
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Yi-Lun Ying, Chaonan Yang, Yi-Tao Long, Zhonglin Yang, and Wei Liu
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Chemical kinetics ,Nanopore ,Materials science ,Chemical physics ,Kinetics ,Molecular mechanism ,Dynamic covalent chemistry ,Molecule ,General Chemistry ,Chemical reaction ,Confined space - Abstract
The study of a single-molecule reaction under nanoconfinement is beneficial for understanding the reactive intermediates and reaction pathways. However, the kinetics model of the single-molecule reaction under confinement remains elusive. Herein we engineered an aerolysin nanopore reactor to elaborate the single-molecule reaction kinetics under nanoconfinement. By identifying the bond-forming and non-bond-forming events directly, a four-state kinetics model is proposed for the first time. Our results demonstrated that the single-molecule reaction kinetics inside a nanopore depends on the frequency of individual reactants captured and the fraction of effective collision inside the nanopore confined space. This insight will guide the design of confined nanopore reactors for resolving the single-molecule chemistry, and shed light on the mechanistic understanding of dynamic covalent chemistry inside confined systems such as supramolecular cages, coordination cages, and micelles.
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- 2021
20. An engineered third electrostatic constriction of aerolysin to manipulate heterogeneously charged peptide transport
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Hongyan Niu, Meng-Ying Li, Yi-Lun Ying, and Yi-Tao Long
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General Chemistry - Abstract
Reading the primary sequence directly using nanopores remains challenging due to the complex building blocks of 20 proteinogenic amino acids and the corresponding sophisticated structures. Compared to the uniformly negatively charged polynucleotides, biological nanopores hardly provide effective ionic current responses to all heterogeneously charged peptides under nearly physiological pH conditions. Herein, we precisely design a N226Q/S228K mutant aerolysin which creates a new electrostatic constriction named R3 in-between two natural sensing regions for controlling the capture and translocation of heterogeneously charged peptides. At nearly physiological pH, the decoration of positive charges at this constriction gives a large velocity of electroosmotic flow (EOF), leading to a maximum 8-fold increase in frequency for the heterogeneously charged peptides with the net charge from +1 to -3. Even the duration time of the negatively charged peptide Aβ35-25D4 in N226Q/S228K AeL also rises from 0.07 ± 0.01 ms to 0.63 ± 0.01 ms after introducing the third electrostatic constriction. Therefore, the N226Q/S228K aerolysin nanopore with three electrostatic constrictions realizes the dual goals of both capturing and decelerating heterogeneously charged peptides without labelling, even for the folded peptides.
- Published
- 2021
21. Snapshotting the transient conformations and tracing the multiple pathways of single peptide folding using a solid-state nanopore
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Weihua Li, Yong-Jing Wan, Yi-Lun Ying, Yi-Tao Long, and Shao-Chuang Liu
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chemistry.chemical_classification ,Time evolution ,Non-equilibrium thermodynamics ,Peptide ,02 engineering and technology ,General Chemistry ,Tracing ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Folding (chemistry) ,Nanopore ,Chemistry ,chemistry ,Biophysics ,Protein folding ,Transient (oscillation) ,0210 nano-technology - Abstract
A fundamental question relating to protein folding/unfolding is the time evolution of the folding of a protein into its precisely defined native structure. The proper identification of transition conformations is essential for accurately describing the dynamic protein folding/unfolding pathways. Owing to the rapid transitions and sub-nm conformation differences involved, the acquisition of the transient conformations and dynamics of proteins is difficult due to limited instrumental resolution. Using the electrochemical confinement effect of a solid-state nanopore, we were able to snapshot the transient conformations and trace the multiple transition pathways of a single peptide inside a nanopore. By combining the results with a Markov chain model, this new single-molecule technique is applied to clarify the transition pathways of the β-hairpin peptide, which shows nonequilibrium fluctuations among several blockage current stages. This method enables the high-throughput investigation of transition pathways experimentally to access previously obscure peptide dynamics, which is significant for understanding the folding/unfolding mechanisms and misfolding of peptides or proteins., A solid-state nanopore based method is described for resolving protein-folding-related problems via snapshotting the folding intermediates and characterizing the kinetics of a single peptide.
- Published
- 2021
22. Tracking the Electrocatalytic Activity of a Single Palladium Nanoparticle for the Hydrogen Evolution Reaction
- Author
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Zhifeng Ding, Yue-Yi Peng, Si-Min Lu, Yi-Tao Long, and Mengjie Chen
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Chemistry ,Organic Chemistry ,Palladium nanoparticles ,chemistry.chemical_element ,Nanoparticle ,Metal Nanoparticles ,Nanotechnology ,General Chemistry ,Electrochemistry ,Tracking (particle physics) ,Catalysis ,Electrode ,Hydrogen evolution ,Electrodes ,Palladium ,Hydrogen - Abstract
The nanoparticle-based electrocatalysts' performance is directly related to their working conditions. In general, a number of nanoparticles are uncontrollably fixed on a millimetre-sized electrode for electrochemical measurements. However, it is hard to reveal the maximum electrocatalytic activity owing to the aggregation and detachment of nanoparticles on the electrode surface. To solve this problem, here, we take the hydrogen evolution reaction (HER) catalyzed by palladium nanoparticles (Pd NPs) as a model system to track the electrocatalytic activity of single Pd NPs by stochastic collision electrochemistry and ensemble electrochemistry, respectively. Compared with the nanoparticle fixed working condition, Pd NPs in the nanoparticle diffused working condition results in a 2-5 orders magnitude enhancement of electrocatalytic activity for HER at various bias potential. Stochastic collision electrochemistry with high temporal resolution gives further insights into the accurate study of NPs' electrocatalytic performance, enabling to dramatically enhance electrocatalytic efficiency.
- Published
- 2021
23. Rapid ultrasensitive monitoring the single-particle surface-enhanced Raman scattering (SERS) using a dark-field microspectroscopy assisted system
- Author
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Yi-Tao Long, Yi-Lun Ying, and Shao-Chuang Liu
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Materials science ,Nanoparticle ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Dark field microscopy ,0104 chemical sciences ,Characterization (materials science) ,Nanomaterials ,symbols.namesake ,symbols ,Particle ,0210 nano-technology ,Spectroscopy ,Raman spectroscopy ,Raman scattering - Abstract
The observation of single-particle surface-enhanced Raman scattering (SERS) has generated considerable interest both in the nanomaterials filed and in the single-particle spectroscopy community. It is a challenge to realize rapid, facile, and high throughput SERS at single nanoparticle level. Here, without the complex experimental device and difficult experimental operations, a general single-particle SERS technique has been achieved by using dark-field-assisted surface-enhanced Raman spectroscopy (DFSERS). This advanced method provides in-situ characterization of the chemical reaction performance at single gold nanorod.
- Published
- 2020
24. Recent advances in nanocollision electrochemistry
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Mahmoud Elsayed Hafez, Wei Ma, Yi-Tao Long, and Ze-Hui Sun
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Computer science ,Single entity ,Ensemble averaging ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,0210 nano-technology ,Electrochemistry ,01 natural sciences ,0104 chemical sciences - Abstract
Ensemble averaging measurements obscure the link between the electrochemical performance and the specific properties of an individual because of the interplay of inhomogeneity and heterogeneity. Nanocollision electrochemistry has attracted increasing interest because of its extremely high sensitivity, revealing the intrinsic properties of individual entities that are masked in the traditional ensemble measurements. In this perspective review, we summarized the recent developments in nanocollision-based single entity electrochemistry and photoelectrochemistry, the combined nanocollision electrochemistry with the other complementary techniques, as well as accurate data process. In closing, future challenges, opportunities, and destinations related to nanocollison electrochemistry were discussed.
- Published
- 2019
25. Unveiling the Intrinsic Catalytic Activities of Single‐Gold‐Nanoparticle‐Based Enzyme Mimetics
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Wei Ma, Hui Ma, Mahmoud Elsayed Hafez, and Yi-Tao Long
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biology ,010405 organic chemistry ,Chemistry ,Nanoparticle ,Ultramicroelectrode ,General Medicine ,General Chemistry ,010402 general chemistry ,Electrocatalyst ,01 natural sciences ,Combinatorial chemistry ,Catalysis ,0104 chemical sciences ,Enzyme catalysis ,Nanomaterials ,Colloidal gold ,biology.protein ,Glucose oxidase - Abstract
Gold nanoparticles (AuNPs) have been demonstrated to serve as effective nanomaterial-based enzyme mimetics (nanozymes) for a number of enzymatic reactions under mild conditions. The intrinsic glucose oxidase and peroxidase activities of single AuNPs and Ag-Au nanohybrids, respectively, were investigated by single NP collision electrochemical measurements. A significantly high turnover number of nanozymes was obtained from individual catalytic events compared with the results from the classical, ensemble-averaged measurements. The unusual enhancement of catalytic activity of single nanozymes is believed to originate from the high accessible surface area of monodispersed NPs and the high activities of carbon-supported NPs during single-particle collision at a carbon ultramicroelectrode. This work introduces a new method for the precise characterization of the intrinsic catalytic activities of nanozymes, giving further insights to the design of high-efficiency nanomaterial catalysts.
- Published
- 2019
26. Simultaneous Removal of Multiple Heavy Metal Ions from River Water Using Ultrafine Mesoporous Magnetite Nanoparticles
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Yi-Tao Long, Li-Jun Zhao, Da-Wei Li, Tano Patrice Fato, and Kaipei Qiu
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Pollutant ,Pollution ,Materials science ,General Chemical Engineering ,Metal ions in aqueous solution ,media_common.quotation_subject ,General Chemistry ,River water ,Article ,Nanomaterials ,lcsh:Chemistry ,Magnetite Nanoparticles ,lcsh:QD1-999 ,Environmental chemistry ,Mesoporous material ,media_common - Abstract
The exploration of simultaneous removal of co-existing or multiple pollutants from water by the means of nanomaterials paves a new avenue that is free from secondary pollution and inexpensive. In the aquatic environment, river water contains a mixture of ions, which can influence the adsorption process. In this respect, removing heavy metal ions becomes a true challenge. Here, four heavy metal ions, namely, Pb2+, Cd2+, Cu2+, and Ni2+, have been successfully removed simultaneously from river water using ultrafine mesoporous magnetite (Fe3O4) nanoparticles (UFMNPs) based on the affinity of these metal ions toward the UFMNP surfaces as well as their unique mesoporous structure, promoting the easy adsorption. The individual removal efficiencies of Pb2+, Cd2+, Cu2+, and Ni2+ ions from river water were 98, 87, 90, and 78%, respectively, whereas the removal efficiencies of the mixed Pb2+, Cd2+, Cu2+, and Ni2+ ions were 86, 80, 84, and 54%, respectively, in the same river water. Thus, the data clearly indicate the complex removal of heavy metal ions in multi-ion systems. This study has demonstrated the huge potential of UFMNPs to be effective for their use in wastewater treatment, especially to simultaneously remove multiple heavy metal ions from aqueous media.
- Published
- 2019
27. Revisiting a classical redox process on a gold electrode by operando ToF-SIMS: where does the gold go?
- Author
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Xin Hua, Hai-Lun Xia, and Yi-Tao Long
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Materials science ,010405 organic chemistry ,General Chemistry ,010402 general chemistry ,Electrochemistry ,01 natural sciences ,Redox ,0104 chemical sciences ,Electrochemical cell ,Chemistry ,chemistry.chemical_compound ,Electron transfer ,chemistry ,Electrode ,Physical chemistry ,Ferricyanide ,Cyclic voltammetry ,Ferrocyanide - Abstract
Our results indicated that a gold electrode participates in the redox reaction of [Fe(CN)6]3/4– by competing with it to form Au(CN)2–., Electrochemical redox conversion between ferricyanide and ferrocyanide on a gold electrode is one of the most classical reactions in electrochemistry. In textbooks, the gold electrode is seen as chemically inert, on which only the adsorption/desorption of [Fe(CN)6]3/4– and electron transfer take place. Here, the electrochemical process of [Fe(CN)6]3/4– on a gold electrode was revisited using a vacuum-compatible microfluidic electrochemical cell in combination with operando liquid ToF-SIMS. An intermediate, Au(CN)2–, was observed in the cyclic voltammetry of ferricyanide with an interesting periodic potential-dependent variation trend. It was demonstrated that the gold electrode participated in the redox reaction of [Fe(CN)6]3/4– by competing with it to form Au(CN)2–, since the formation constant was Fe(CN)63– > Au(CN)2– > Fe(CN)64–. The formation and evolution of Au(CN)2– depends on the ratio of Fe(iii) and Fe(ii) on the surface of the gold electrode, which was determined by the redox conversion between Fe(iii) and Fe(ii) as well as the electric field force-based attraction or repulsion between the gold electrode and [Fe(CN)6]3/4–. Both of these factors were potential-dependent, resulting in the periodic change of Au(CN)2– in the dynamic potential scan of [Fe(CN)6]3/4–. These results provided solid molecular evidence for the participation of the gold electrode in the [Fe(CN)6]3/4– redox system, which will deepen mechanistic understandings of related electrochemical applications.
- Published
- 2019
28. A lithium-ion-active aerolysin nanopore for effectively trapping long single-stranded DNA
- Author
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Shao-Chuang Liu, Yi-Tao Long, Zheng-Li Hu, Yi-Lun Ying, and Meng-Yin Li
- Subjects
chemistry.chemical_classification ,Oligonucleotide ,Aerolysin ,chemistry.chemical_element ,General Chemistry ,Ion ,Molecular dynamics ,chemistry.chemical_compound ,Nanopore ,chemistry ,Biophysics ,Nucleotide ,Lithium ,DNA - Abstract
Wild-type aerolysin (AeL) nanopores allow direct single nucleotide discrimination of very short oligonucleotides (≤10 nt) without labelling, which shows great potential for DNA sensing. To achieve real applications, one major obstacle of AeL is its poor capture ability of long single-stranded DNA (ssDNA, >10 nt). Here, we have proposed a novel and robust strategy for the electrostatic focusing of long ssDNA into a lithium-chloride (LiCl)-active AeL. By using this method, for the first time we have demonstrated AeL detection of ssDNA longer than 100 nt. Due to screening more negative charges, LiCl improves AeL capture ability of long ssDNA (i.e. 60 nt) by 2.63- to 10.23-fold compared to KCl. Further calculations and molecular dynamics simulations revealed that strong binding between Li+ and the negatively charged residue neutralized the AeL, leading to a reduction in the energy barrier for ssDNA capture. These findings facilitate the future high-throughput applications of AeL in genetic and epigenetic diagnostics.
- Published
- 2019
29. Muscle-like Artificial Molecular Actuators for Nanoparticles
- Author
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He Tian, Si-Jia Rao, Da-Hui Qu, Yi-Tao Long, Xin Li, Qi Zhang, Tian-Yi Xu, Da-Wei Li, and Tao Xie
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Materials science ,Quantitative Biology::Tissues and Organs ,General Chemical Engineering ,Physics::Medical Physics ,Biochemistry (medical) ,Supramolecular chemistry ,Nanoparticle ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Biochemistry ,Molecular machine ,0104 chemical sciences ,Computer Science::Robotics ,Chemical energy ,Colloidal gold ,Materials Chemistry ,Environmental Chemistry ,0210 nano-technology ,Actuator ,Biological system ,Nanoscopic scale ,Plasmon - Abstract
Summary Muscle tissue performs crucial contraction/extension motions that generate mechanical force and work by consuming chemical energy. Inspired by this naturally created biomolecular machine, artificial molecular muscles are designed and synthesized to undertake linear actuation functions. However, most of these muscle-like actuators are performed at large ensembles, while to realize the nanoscale actuation at the single- to few-molecule level remains challenging. Herein, we developed an artificial muscle-like molecular actuator that can reversibly control the proximity of the attached nano-objects, gold nanoparticles, within the single-molecule length level by its stimuli-responsive muscle-like linear contraction/extension motion. The molecular actuation motion is accompanied by an optical signal output resulting from the plasmonic resonance properties of gold nanoparticles. Meanwhile, the thermal noise of the muscle-like molecular actuator can be overcome by integrating the optical signal over a sufficiently long period.
- Published
- 2018
30. Correction: An engineered third electrostatic constriction of aerolysin to manipulate heterogeneously charged peptide transport
- Author
-
Hongyan Niu, Meng-Yin Li, Yi-Lun Ying, and Yi-Tao Long
- Subjects
General Chemistry - Abstract
Correction for ‘An engineered third electrostatic constriction of aerolysin to manipulate heterogeneously charged peptide transport’ by Hongyan Niu et al., Chem. Sci., 2022, 13, 2456–2461, https://doi.org/10.1039/D1SC06459B.
- Published
- 2022
31. pH-Dependent Water Clusters in Photoacid Solution: Real-Time Observation by ToF-SIMS at a Submicropore Confined Liquid-Vacuum Interface
- Author
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Ying-Ya Liu, Xin Hua, Zhiwei Zhang, Junji Zhang, Shaoze Zhang, Ping Hu, and Yi-Tao Long
- Subjects
Work (thermodynamics) ,Proton ,hydrogen-bonding network ,Protonation ,liquid-vacuum interface ,02 engineering and technology ,Electrolyte ,010402 general chemistry ,01 natural sciences ,lcsh:Chemistry ,in-situ liquid ToF-SIMS ,Water cluster ,Original Research ,chemistry.chemical_classification ,water cluster ,Aqueous solution ,Chemistry ,Hydrogen bond ,General Chemistry ,photoacid ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,lcsh:QD1-999 ,Chemical engineering ,0210 nano-technology ,Organic acid - Abstract
Water clusters are ubiquitously formed in aqueous solutions by hydrogen bonding, which is quite sensitive to various environment factors such as temperature, pressure, electrolytes, and pH. Investigation of how the environment has impact on water structure is important for further understanding of the nature of water and the interactions between water and solutes. In this work, pH-dependent water structure changes were studied by monitoring the changes for the size distribution of protonated water clusters by in-situ liquid ToF-SIMS. In combination with a light illumination system, in-situ liquid ToF-SIMS was used to real-time measure the changes of a light-activated organic photoacid under different light illumination conditions. Thus, the proton transfer and pH-mediated water cluster changes were analyzed in real-time. It was found that higher concentration of free protons could lead to a strengthened local hydrogen bonding network as well as relatively larger protonated water clusters in both organic acid and inorganic acid. Besides, the accumulation of protons at the liquid-vacuum interface under light illumination was observed owing to the affinity of organic molecules to the low-pressure gas phase. The application of in-situ liquid ToF-SIMS analysis in combination with in-situ light illumination system opened up an avenue to real-time investigate light-activated reactions. Besides, the results regarding water structure changes in acidic solutions showed important insights in related atmospheric and physiochemical processes.
- Published
- 2020
32. Exploring dynamic interactions of single nanoparticles at interfaces for surface-confined electrochemical behavior and size measurement
- Author
-
Wei Ma, Hui Ma, Yi-Tao Long, P. Hu, Haifeng Wang, and Jianfu Chen
- Subjects
Surface (mathematics) ,Work (thermodynamics) ,Materials science ,Chemistry(all) ,Interface (Java) ,Science ,General Physics and Astronomy ,Nanoparticle ,Ultramicroelectrode ,Nanotechnology ,02 engineering and technology ,Size measurement ,Physics and Astronomy(all) ,010402 general chemistry ,Electrochemistry ,01 natural sciences ,Characterization and analytical techniques ,General Biochemistry, Genetics and Molecular Biology ,Article ,lcsh:Science ,Scaling ,Multidisciplinary ,Biochemistry, Genetics and Molecular Biology(all) ,General Chemistry ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Nanoparticles ,lcsh:Q ,0210 nano-technology ,Analytical chemistry - Abstract
With the development of new instruments and methodologies, the highly dynamic behaviors of nanoparticle at the liquid-solid interface have been studied. However, the dynamic nature of the electrochemical behavior of individual nanoparticles on the electrode interface is still poorly understood. Here, we generalize scaling relations to predict nanoparticle-electrode interactions by examining the adsorption energy of nanoparticles at an ultramicroelectrode interface. Based on the theoretical predictions, we investigate the interaction-modulated dynamic electrochemical behaviors for the oxidation of individual Ag nanoparticles. Typically, significantly distinct current traces are observed owing to the adsorption-mediated motion of Ag nanoparticles. Inspired by restraining the stochastic paths of particles in the vicinity of the electrode interface to produce surface-confined current traces, we successfully realize high-resolution size measurements of Ag nanoparticles in mixed-sample systems. This work offers a better understanding of dynamic interactions of nanoparticles at the electrochemical interface and displays highly valuable applications of single-entity electrochemistry., Single-entity electrochemistry has been proposed for studying properties of single nanoparticles (NPs). Here, the authors make use of adsorption-mediated motion of Ag NPs to take individual NP size measurements using electrochemical impacts with excellent agreement to standard imaging techniques.
- Published
- 2020
33. Manipulating and visualizing the dynamic aggregation-induced emission within a confined quartz nanopore
- Author
-
Yuan-Jie Li, He Tian, Yi-Lun Ying, Yong-Xu Hu, Ju Mei, Rui Gao, and Yi-Tao Long
- Subjects
Multidisciplinary ,Materials science ,Science ,General Physics and Astronomy ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,General Biochemistry, Genetics and Molecular Biology ,Article ,0104 chemical sciences ,Nanopore ,Optical sensing ,lcsh:Q ,Aggregation-induced emission ,lcsh:Science ,0210 nano-technology ,Quartz ,Confined space - Abstract
Aggregation-induced emission (AIE) as a unique photophysical process has been intensively explored for their features in fields from optical sensing, bioimaging to optoelectronic devices. However, all AIE luminogens (AIEgens) hardly recover into the initial dispersed state after illuminating at the ultimate aggregated state, which limits AIEgens to achieve reversible sensing and reproducible devices. To real-time manipulate the emission of AIEgen, here we take the advantage of confined space in the quartz nanopore to achieve a nanopore-size-dependent restriction of AIEgens for reversible conversions of “on-to-off” and “off-to-on” emission. By electrochemically manipulating 26 fL AIEgen solution inside nanopore confinement, AIE illuminates while moves along nanopore from the constricted tip to inside cavity at a velocity of 1.4–2.2 μm s−1, and vice versa. We further apply this dynamic manipulation for a target delivery of AIEgen into single cells, which opens up new possibility to design powerful and practical AIE applications., The difficulty in recovering the aggregation-induced emission fluorogens (AIEgens) to the initial dispersed state upon illuminating has limited their applications. Here, the authors employ the confined space in the quartz nanopore to achieve a nanopore-size dependent restriction of AIEgens.
- Published
- 2018
34. Nanochannels of Covalent Organic Frameworks for Chiral Selective Transmembrane Transport of Amino Acids
- Author
-
Yan Liu, Yong Cui, Rui Gao, Xing Han, Xiaowei Wu, Yi-Tao Long, and Chen Yuan
- Subjects
chemistry.chemical_classification ,Aldehydes ,Molecular Structure ,Chemistry ,Surface Properties ,Biological Transport ,General Chemistry ,Membrane transport ,Diamines ,010402 general chemistry ,01 natural sciences ,Biochemistry ,Combinatorial chemistry ,Catalysis ,0104 chemical sciences ,Amino acid ,Colloid and Surface Chemistry ,Covalent bond ,Nanotechnology ,Imines ,Amino Acids ,Particle Size ,human activities ,Porosity ,ComputingMethodologies_COMPUTERGRAPHICS - Abstract
Mimicking cellular transport mechanisms to make solid-state smart nanochannels has long been of great interest for their diverse applications, but it poses a critical synthetic challenge. Covalent organic frameworks (COFs) are porous crystalline materials with tailor-made nanochannels and hold great potential for ion and molecule transport. We demonstrate here for the first time that 2D COFs possess the necessary merits to be promising solid-state nanochannels for selective transport of amino acids, which are the basis for life. By imine condensations of a
- Published
- 2019
35. A Time-Resolved Single-Molecular Train Based on Aerolysin Nanopore
- Author
-
Yi-Tao Long, Fu-Na Meng, Zheng-Li Hu, He Tian, Yi-Lun Ying, Junji Zhang, Chan Cao, and Ziyuan Li
- Subjects
Physics ,education.field_of_study ,General Chemical Engineering ,Biochemistry (medical) ,Population ,Aerolysin ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Biochemistry ,Molecular machine ,0104 chemical sciences ,Nanopore ,Temporal resolution ,Materials Chemistry ,Environmental Chemistry ,0210 nano-technology ,Biological system ,education - Abstract
Summary An aerolysin nanopore interface was introduced as a molecular machine to electrically read out the real-time photo-controlled motion of an azobenzene-geared DNA train with high spatial and temporal resolution. Under alternating UV and visible irradiation, each DNA train performed two regulated speeds of 1.9 and 6.3 bases/s corresponding to trans and cis states, respectively, with readily identified current signals. Each train type fell into the ultra-narrow current population with a full-width half maximum of 0.2–0.4 pA. The combination of a model molecular machine system and powerful aerolysin interface enabled the motions of every artificial molecular machine to be followed in real time.
- Published
- 2018
36. Monitoring disulfide bonds making and breaking in biological nanopore at single molecule level
- Author
-
Chan Cao, Yi-Tao Long, Da-Wei Li, Ya-Qian Wang, and Bing Zhou
- Subjects
DTNB ,Chemistry ,Aerolysin ,Ionic bonding ,02 engineering and technology ,General Chemistry ,Nanoreactor ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Reversible reaction ,0104 chemical sciences ,Nanopore ,Chemical bond ,Biophysics ,Molecule ,0210 nano-technology - Abstract
Monitoring subtle changes in ionic current flow through a nanopore could be applied to observe single molecule reaction. Here, we introduced cysteine to substitute for lysine at position 238 constructing a mutant aerolysin K238C. It could be regarded as a nanoreactor to efficiently visualize chemical bonds making and breaking. The compound 5,5′-dithiobis-(2-nitrobenzoic acid) (DTNB) was selected as a reactant coming into collisions on the interface of the pore to occur a reversible reaction. Our results showed that the mutant aerolysin could respond to three molecules of DTNB simultaneously and reflect corresponding levels with distinguishable current signals. Therefore, this method constitutes a simple, generic tool for monitoring single molecule reaction, which evokes a guidance for the mutant aerolysin towards the application of tracking other more reactions at single molecule level.
- Published
- 2018
37. Quantifying Visible-Light-Induced Electron Transfer Properties of Single Dye-Sensitized ZnO Entity for Water Splitting
- Author
-
Wei Ma, Yi-Tao Long, Yue-Yi Peng, Hui Ma, Zhe-Yao Yang, He Tian, Jianfu Chen, and Xiao-Yuan Liu
- Subjects
Photocurrent ,Chemistry ,business.industry ,Ultramicroelectrode ,02 engineering and technology ,General Chemistry ,Electron ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Biochemistry ,Electron transport chain ,Catalysis ,Photoinduced electron transfer ,0104 chemical sciences ,Electron transfer ,Colloid and Surface Chemistry ,Optoelectronics ,Water splitting ,0210 nano-technology ,business ,Photocatalytic water splitting - Abstract
Quantifying the photoinduced electron transfer properties of a single entity is of paramount importance for clarifying the link between the photoelectrochemical performance and the specific properties of an individual. Here, we successfully monitored the photoelectrochemical behavior of a single dye-sensitized ZnO entity on a Au ultramicroelectrode with different TiO2 film thicknesses. Due to a trap-limited electron diffusion in TiO2 film, a sub-millisecond photocurrent transient was observed for an individual N719@ZnO associated with single-particle photocatalytic water splitting. Furthermore, a Monte Carlo random walk numerical simulation model was developed to simulate the photoinjected electron transport dynamics and recombination in a nanoparticulate TiO2 film. Our approach allowed the photocatalytic properties of N719 at the single-molecule level to be quantified, and electron diffusivity and electron collection efficiency as a function of the film thickness were estimated by simulation analyses. Ex...
- Published
- 2018
38. Single-Nanoparticle Photoelectrochemistry at a Nanoparticulate TiO2 -Filmed Ultramicroelectrode
- Author
-
Yue-Yi Peng, Yi-Tao Long, He Tian, Hui Ma, and Wei Ma
- Subjects
Photocurrent ,Materials science ,business.industry ,Photoelectrochemistry ,Nanoparticle ,Ultramicroelectrode ,General Medicine ,02 engineering and technology ,General Chemistry ,Electron ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Thermal diffusivity ,01 natural sciences ,Catalysis ,Photoinduced electron transfer ,0104 chemical sciences ,Diffusion process ,Optoelectronics ,0210 nano-technology ,business - Abstract
An ultrasensitive photoelectrochemical method for achieving real-time detection of single nanoparticle collision events is presented. Using a micrometer-thick nanoparticulate TiO2-filmed Au ultra-microelectrode (TiO2@Au UME), a sub-millisecond photocurrent transient was observed for an individual N719-tagged TiO2 (N719@TiO2) nanoparticle and is due to the instantaneous collision process. Owing to a trap-limited electron diffusion process as the rate-limiting step, a random three-dimensional diffusion model was developed to simulate electron transport dynamics in TiO2 film. The combination of theoretical simulation and high-resolution photocurrent measurement allow electron-transfer information of a single N719@TiO2 nanoparticle to be quantified at single-molecule accuracy and the electron diffusivity and the electron-collection efficiency of TiO2@Au UME to be estimated. This method provides a test for studies of photoinduced electron transfer at the single-nanoparticle level.
- Published
- 2018
39. Electrochemically generated green-fluorescent N-doped carbon quantum dots for facile monitoring alkaline phosphatase activity based on the Fe3+-mediating ON-OFF-ON-OFF fluorescence principle
- Author
-
Yi-Tao Long, Yuanhong Xu, Fushuang Niu, Xin Hua, Yi-Lun Ying, and Yusheng Niu
- Subjects
Detection limit ,Quantum yield ,Ethylenediamine ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,Fluorescence ,Pyrophosphate ,0104 chemical sciences ,chemistry.chemical_compound ,Hydrolysis ,chemistry ,Biochemistry ,Alkaline phosphatase ,General Materials Science ,0210 nano-technology ,Nuclear chemistry - Abstract
Herein, green-fluorescent N-doped carbon quantum dots (N-CQDs) with quantum yield of 30.6% were prepared via a simple bottom-up electrochemical (EC) method using the mixtures of pyrocatechol and ethylenediamine as both precursors and electrolytes. The ON-OFF fluorescence (FL) principle that the FL intensity of the N-CQDs was quenched in the presence of Fe3+ was further extended to the ON-OFF-ON and ON-OFF-ON-OFF ones for pyrophosphate anions (PPi) and alkaline phosphatase (ALP) detection, respectively, based on the specific competitive interaction of N-CQDs with Fe3+ and PPi and the hydrolysis of PPi in the presence ALP. Under the optimized conditions, limit of detection (LOD) of 1.2 μM and 0.5 μM were achieved for assays of Fe3+ and PPi, respectively. Meanwhile, measurable evaluation of ALP activity was reached in a wide range from 5 to 360 U/L with a LOD of 1.1 U/L. The as-proposed sensors showed many advantages including label free, rapid, simple, low-cost, high sensitive, which has great promising application potential in vivo and in vitro clinical diagnosis and will promote the application of EC derived carbon nanomaterials.
- Published
- 2018
40. Reversible redox inter-conversion of biologically active NAD+/NADH derivatives bound to a gold electrode: ToF-SIMS evidence
- Author
-
Ruo-Can Qian, Xin Hua, Yi-Tao Long, Jian Lv, and Li-Jun Zhao
- Subjects
Nad nadh ,Chemistry ,Metals and Alloys ,Biological activity ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,Combinatorial chemistry ,Redox ,Catalysis ,0104 chemical sciences ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Secondary ion mass spectrometry ,Electrode ,Materials Chemistry ,Ceramics and Composites ,Surface modification ,NAD+ kinase ,0210 nano-technology - Abstract
The realization of the reversible inter-conversion between NADH and NAD+ is a long-term challenge in biological and energy-related chemistry. Here, we achieve the electrochemical reversible redox of NAD+/NADH derivatives by the functionalization of a gold electrode with a specially designed NAD+ derivative, and the electrochemical redox products are characterized by time-of-flight secondary ion mass spectrometry (ToF-SIMS).
- Published
- 2018
41. Quaternary two dimensional Zn–Ag–In–S nanosheets for highly efficient photocatalytic hydrogen generation
- Author
-
Xianyuan Jiang, Jianxi Ke, Fei Wang, Hao Chen, Xiao-Yuan Liu, Youqi Ke, Xu Wang, Yi-Tao Long, Qiong Zhang, Kaimin Xu, Qi Wei, Shizhuo Wang, Zhijun Ning, and Qian Gao
- Subjects
Materials science ,Passivation ,Renewable Energy, Sustainability and the Environment ,business.industry ,Graphene ,chemistry.chemical_element ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Oxygen ,0104 chemical sciences ,law.invention ,Semiconductor ,Chemical engineering ,chemistry ,law ,Photocatalysis ,General Materials Science ,0210 nano-technology ,business ,Absorption (electromagnetic radiation) ,Photocatalytic water splitting ,Hydrogen production - Abstract
Hydrogen generation based on photocatalytic water splitting is a promising strategy for renewable energy production. Significant efforts have been made to improve the photocatalytic efficiency. However, the light harvesting ability of photocatalytic systems in the visible region still needs to be significantly improved to enable them to be a competitive technology for hydrogen generation. Herein, for the first time, we synthesized 2D Zn–Ag–In–S (ZAIS) nanosheets with strong absorption in the visible region and applied them for photocatalytic hydrogen generation. The exploration of oxygen passivation (O-ZAIS) reduced the defect concentration and nonradiative decay. The hydrogen generation rate is up to 25.2 mmol g−1 h−1, which is 14.7 times higher than that of pristine ZAIS nanosheets. Furthermore, by introducing 2D Co3O4 as the co-catalyst, carrier separation is accelerated, giving rise to a hydrogen generation efficiency of 43.6 mmol g−1 h−1. To the best of our knowledge, this is the highest efficiency reported among all kinds of 2D photocatalysts.
- Published
- 2018
42. In situ and real-time ToF-SIMS analysis of light-induced chemical changes in perovskite CH3NH3PbI3
- Author
-
Duo Xu, Yi-Tao Long, Hongwei Qiao, He Tian, Hua Gui Yang, Xin Hua, and Shao-Chuang Liu
- Subjects
In situ ,Materials science ,Metals and Alloys ,Analytical chemistry ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Catalysis ,0104 chemical sciences ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Secondary ion mass spectrometry ,Material Degradation ,Materials Chemistry ,Ceramics and Composites ,Light induced ,0210 nano-technology ,Perovskite (structure) - Abstract
A hybrid light/ToF-SIMS system was used to analyze the dynamic chemical changes of perovskite CH3NH3PbI3 films under light illumination, in order to reveal the mechanism of light instability for perovskite materials. Real-time material degradation and quasi-reversible iodine migration were successfully observed.
- Published
- 2018
43. Cover Picture: Single‐Molecule Frequency Fingerprint for Ion Interaction Networks in a Confined Nanopore (Angew. Chem. Int. Ed. 46/2021)
- Author
-
Yi-Lun Ying, Yi-Tao Long, Yong-Jing Wan, Xi-Xin Fu, and Xinyi Li
- Subjects
Nanopore ,Materials science ,Nanoelectrochemistry ,Chemical physics ,Fingerprint (computing) ,Molecule ,Cover (algebra) ,General Chemistry ,Catalysis ,Ion - Published
- 2021
44. In-situ discrimination of the water cluster size distribution in aqueous solution by ToF-SIMS
- Author
-
Yi-Lun Ying, Xin Hua, Ying-Ya Liu, and Yi-Tao Long
- Subjects
In situ ,Heavy water ,Range (particle radiation) ,Aqueous solution ,Materials science ,Analytical chemistry ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Mass spectrometry ,01 natural sciences ,0104 chemical sciences ,Secondary ion mass spectrometry ,chemistry.chemical_compound ,chemistry ,Molecule ,Water cluster ,0210 nano-technology ,Physics::Atmospheric and Oceanic Physics - Abstract
The size distribution and molecular structure of water clusters play a critical role in the chemical, biological and atmospheric process. The common experimental study of water clusters in aqueous solution is challenged due to the influence of local H-bonding environments on vibration spectroscopies or vacuum requirements for most mass spectrometry technologies. Here, the time-of-flight secondary ion mass spectrometry (ToF-SIMS) combining with a microfluidic chip has been applied to achieve the in-situ discrimination of the size distribution for water clusters in liquid water at room temperature. The results demonstrated that the presented method is highly system stable, reproducible and accurate. The comparison of heavy water with pure water was made to further demonstrate the accuracy of this technique. These results showed that (H2O)3H+ and (D2O)4D+ are the most dominant clusters in pure and heavy water, respectively. This one water molecule difference in the dominant cluster size may due to the nuclear quantum effects on water’s hydrogen bonded network. It is the first time to experimentally show the size distribution of water clusters over a wide range ( n =1–30) for pure (H2O) and heavy (D2O) water from molecular level. This technique provides an achievable method for liquid water, which offers a bridge to close the gap between theoretical and experimental study of water cluster in aqueous solution.
- Published
- 2017
45. A 30 nm Nanopore Electrode: Facile Fabrication and Direct Insights into the Intrinsic Feature of Single Nanoparticle Collisions
- Author
-
Rui Gao, Yong-Xu Hu, Yuan-Jie Li, Yi-Tao Long, Ru-Jia Yu, Yi-Lun Ying, and Yao Lin
- Subjects
Materials science ,Nanoelectrochemistry ,business.industry ,010405 organic chemistry ,Nanoparticle ,02 engineering and technology ,General Chemistry ,General Medicine ,021001 nanoscience & nanotechnology ,010402 general chemistry ,Capacitance ,01 natural sciences ,Catalysis ,0104 chemical sciences ,Nanopore ,Collision frequency ,Temporal resolution ,Electrode ,Optoelectronics ,0210 nano-technology ,business ,Order of magnitude - Abstract
Clarifying the hidden but intrinsic feature of single nanoparticles by nanoelectrochemistry could help understand its potential for diverse applications. The uncontrolled interface and bandwidth limitation in the electrochemical measurement put the obstacle in single particle collision. Here, we demonstrate a well-defined 30 nm nanopore electrode with a rapid chemical-electrochemical fabrication method which provides a high reproducibility in both size and performance. A capacitance-based detection mechanism is demonstrated to achieve a high current resolution of 0.6 pA ±0.1 pA (RMS) and a high the temporal resolution of 0.01 ms. By utilizing this electrode, the dynamic interactions of every single particle in the mixture could be directly read during the collision process. The collision frequency is two orders of magnitude higher than previous reports, which helps reveal the hidden features of nanoparticles during the complex and multidimensional interaction processes.
- Published
- 2017
46. Wearable Chemosensors: A Review of Recent Progress
- Author
-
Yi-Tao Long and Ruo-Can Qian
- Subjects
Computer science ,010401 analytical chemistry ,electronic healthcare ,Wearable computer ,Minireviews ,02 engineering and technology ,General Chemistry ,021001 nanoscience & nanotechnology ,Human motion ,biosensors ,sensors ,01 natural sciences ,0104 chemical sciences ,analytical methods ,Human–computer interaction ,Fabrication methods ,Minireview ,0210 nano-technology ,Healthcare system ,wearable chemosensors - Abstract
In recent years, there has been growing demand for wearable chemosensors for their important potential applications in mobile and electronic healthcare, patient self‐assessment, human motion monitoring, and so on. Innovations in wearable chemosensors are revolutionizing the modern lifestyle, especially the involvement of both doctors and patients in the modern healthcare system. The facile interaction of wearable chemosensors with the human body makes them favorable and convenient tools for the detection and long‐term monitoring of the chemical, biological, and physical status of the human body at a low cost with high performance. In this Minireview, we give a brief overview of the recent advances and developments in the field of wearable chemosensors, summarize the basic types of wearable chemosensors, and discuss their main functions and fabrication methods. At the end of this paper, the future development direction of wearable chemosensors is prospected. With continued interest and attention to this field, new exciting progress is expected in the development of innovative wearable chemosensors.
- Published
- 2017
47. Detection of single oligonucleotide with an electrochemical confined solid-state nanopore
- Author
-
Shao-Chuang Liu, Yao Lin, Yi-Tao Long, Yi-Lun Ying, and Qiao Li
- Subjects
Nanopore ,Materials science ,Dielectric strength ,Oligonucleotide ,General Chemical Engineering ,Materials Chemistry ,Solid-state ,Molecule ,Nanotechnology ,General Chemistry ,Electrochemistry ,Biochemistry ,Confined space - Abstract
Solid-state nanopore has been widely used for a variety of single-molecule analysis due to its advantage of size control, high stability, adjustable surface properties, and the potential of further integration. Therefore, the insensitive studies have applied for the nanopore analysis of DNA, RNA and proteins. In order to detect an oligonucleotide at single-molecule level, here, we fabricated two SiN X solid-state nanopores with diameter of 3.1 and 8.5 nm by controlled dielectric breakdown. The weak interaction between the solid-state nanopore and the oligonucleotide could be efficiently enhanced by electrochemical confined space effect of nanopore. We employed a 67-nt oligonucleotide as a model which could be electrochemically driven into a nanopore. The model ssDNA in nanopore with confined diameter of 3.1 nm could result in two kinds of electrochemical behaviors which assign to bumping and translocation. Our findings pave the path for a better understanding of the electrochemical behavior of the single molecule in a confined space.
- Published
- 2017
48. Single-molecule analysis in an electrochemical confined space
- Author
-
Yi-Tao Long and Yi-Lun Ying
- Subjects
chemistry.chemical_classification ,Chemistry ,Biomolecule ,Repeat sequence ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Electrochemistry ,01 natural sciences ,0104 chemical sciences ,Nanopore ,Chemical physics ,Metastability ,Molecule ,High temporal resolution ,0210 nano-technology ,Confined space - Abstract
Electrochemical analysis of single molecules is a method with the strong ability of the enhanced efficiency and ultra-sensitivity. Here, we demonstrate that the electrochemical confined space could efficiently convert single molecule characteristics into measurable electrochemical signatures with high temporal resolution. The human telomere repeat sequence T8 was used as a probe to determine the electrochemical confined effect in a nanopore. Our results show that the nanopore with comparable confined space of the telomere repeat sequence exhibits the most distinguishable single-molecule signals which suggest the folded conformation of T8. This method will greatly extend the lifetime of a metastable conformation for a single biomolecule by strong analyte-nanopore interactions, which brings the new insight into the understanding of the biomolecule’s function at single-molecule level.
- Published
- 2017
49. A Two-Stage Dissociation System for Multilayer Imaging of Cancer Biomarker-Synergic Networks in Single Cells
- Author
-
Ruo-Can Qian, Yi-Tao Long, Yue Cao, Zhen Gu, and Li-Jun Zhao
- Subjects
Indoles ,Polymers ,Metal Nanoparticles ,Breast Neoplasms ,Nanotechnology ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,Catalysis ,Dissociation (chemistry) ,Biomarkers, Tumor ,medicine ,Humans ,Biomarker Analysis ,Stage (cooking) ,Chemistry ,Optical Imaging ,Cancer ,General Medicine ,General Chemistry ,021001 nanoscience & nanotechnology ,medicine.disease ,0104 chemical sciences ,Biomarker (cell) ,MicroRNAs ,Microscopy, Fluorescence ,Colloidal gold ,Cytoplasm ,MCF-7 Cells ,Sialic Acids ,Cancer research ,Female ,Cancer biomarkers ,Gold ,Single-Cell Analysis ,Tumor Suppressor Protein p53 ,0210 nano-technology - Abstract
The monitoring of cancer biomarkers is crucial to the early detection of cancer. However, a limiting factor in biomarker analysis is the ability to obtain the multilayered information of various biomarker molecules located at different parts of cells from the plasma membrane to the cytoplasm. A two-stage dissociation nanoparticle system based on multifunctionalized polydopamine-coated gold nanoparticles (Au@PDA NPs) is reported, which allows for the two-stage imaging of cancer biomarkers in single cells. We demonstrate the feasibility of this strategy on sialic acids (SAs), p53 protein, and microRNA-21 (miRNA-21) in MCF-7 breast cancer cells by two custom-built probes. Furthermore, the multicolor fluorescence information extracted is used for the monitoring of biomarker expression changes under different drug combinations, which allows us to investigate the complex interactions between various cancer biomarkers and to describe the cancer biomarker-synergic networks in single cells.
- Published
- 2017
50. Advanced electroanalytical chemistry at nanoelectrodes
- Author
-
Dongping Zhan, Zhifeng Ding, Yi-Lun Ying, and Yi-Tao Long
- Subjects
Chemistry ,High spatial resolution ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,0210 nano-technology ,01 natural sciences ,0104 chemical sciences ,Characterization (materials science) - Abstract
In this perspective, we discuss the challenges, advances and opportunities in electroanalytical chemistry at nanoelectrodes, including nanoelectrode fabrication, real-time characterizations, and high-performance electrochemical instrumentation., Nanoelectrodes, with dimensions below 100 nm, have the advantages of high sensitivity and high spatial resolution. These electrodes have attracted increasing attention in various fields such as single cell analysis, single-molecule detection, single particle characterization and high-resolution imaging. The rapid growth of novel nanoelectrodes and nanoelectrochemical methods brings enormous new opportunities in the field. In this perspective, we discuss the challenges, advances, and opportunities for nanoelectrode fabrication, real-time characterizations and high-performance electrochemical instrumentation.
- Published
- 2017
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