Schiff Base Reaction in a Living Cell: In Situ Synthesis of a Hollow Covalent Organic Polymer To Regulate Biological Functions.

Artificially performing chemical reactions in living biosystems to attain various physiological aims remains an intriguing but very challenging task. In this study, the Schiff base reaction was conducted in cells using Sc(OTf) as a catalyst, enabling the in situ synthesis of a hollow covalent organic polymer (HCOP) without external stimuli. The reversible Schiff base reaction mediated intracellular Oswald ripening endows the HCOP with a spherical, hollow porous structure and a large specific surface area.

Dual-Modal Apoptosis Assay Enabling Dynamic Visualization of ATP and Reactive Oxygen Species in Living Cells.

ATP and reactive oxygen species (ROS) are considered significant indicators of cell apoptosis. However, visualizing the interplay between apoptosis-related ATP and ROS is challenging. Herein, we developed a metal-organic framework (MOF)-based nanoprobe for an apoptosis assay using duplex imaging of cellular ATP and ROS.

AuNPs-COFs Core-Shell Reversible SERS Nanosensor for Monitoring Intracellular Redox Dynamics.

The redox homeostasis in living cells is greatly crucial for maintaining the redox biological function, whereas accurate and dynamic detection of intracellular redox states still remains challenging. Herein, a reversible surface-enhanced Raman scattering (SERS) nanosensor based on covalent organic frameworks (COFs) was prepared to dynamically monitor the redox processes in living cells. The nanosensor was fabricated by modifying the redox-responsive Raman reporter molecule, 2-Mercaptobenzoquione (2-MBQ), on the surface of gold nanoparticles (AuNPs), followed by the in situ coating of COFs shell.

Label-free detection of DNA methylation by surface-enhanced Raman spectroscopy using zirconium-modified silver nanoparticles.

DNA methylation is an important feature of gene epigenetics that affects the metabolic process of organisms. Although surface-enhanced Raman spectroscopy (SERS) has demonstrated great potential in label-free DNA detection, discriminating the various processes involved in DNA methylation remains a challenge. DNA molecules fold themselves, wrapping the hydrophobic bases, thus making it difficult for traditional methods to detect single-base signals.

Revealing the Catalytic Activities of Single-Dispersed Pd Clusters Embedded on Hollow Nanoparticles toward the Hydrogen Evolution Reaction.

Hydrogen evolution reaction (HER) is one of the revolutionary aspects that grab lots of attention for the production of clean energy sources, increasing the demands of revealing the intrinsic activities of HER catalysts for designing efficient candidates. Based on using only surface active sites on solid nanoparticles (SNPs), catalysts with high atom dispersion are immensely desirable to magnify their efficiency through maximum atom utilization. Herein, we employed hollow mesoporous silica nanoparticles (HMSNPs) as an insulating nanoplatform for engineering single-dispersed Pd clusters on their surface, assuring high dispersion of the Pd clusters.

Reversible polymerization of carbon dots based on dynamic covalent imine bond.

Carbon dots (CDs), as new type of carbon-based nanoparticles, are considered to be an aggregate with irreversible polymerization. Achieving the reversible tunability of CDs luminescence based on their reversible polymerization is a challenging subject. Herein, we, for the first time, design and construct the blue-emitting CDs with reversible polymerization by a room-temperature Schiff base reaction between tannic acid and ethylenediamine.

Dynamic Visualization of Endoplasmic Reticulum Stress in Living Cells via a Two-Stage Cascade Recognition Process.

The endoplasmic reticulum (ER) is crucial for the regulation of multiple cellular processes, such as cellular responses to stress and protein synthesis, folding, and posttranslational modification. Nevertheless, monitoring ER physiological activity remains challenging due to the lack of powerful detection methods. Herein, we built a two-stage cascade recognition process to achieve dynamic visualization of ER stress in living cells based on a fluorescent carbon dot (CD) probe, which is synthesized by a facile one-pot hydrothermal method without additional modification.

Dual-Emitting Carbonized Polymer Dots Synthesized at Room Temperature for Ratiometric Fluorescence Sensing of Vitamin B12.

Ratiometric fluorescence (FL) probes are highly desirable for highly sensitive and reliable assays. Dual-emitting carbonized polymer dots (CPDs) have great application prospects in building ratiometric FL sensors. However, dual-emitting CPDs are usually synthesized at high temperatures and high pressures, which not only increases the cost but also complicates the structure of CPDs.

In Situ Monitoring of Hydrogen Peroxide Released from Living Cells Using a ZIF-8-Based Surface-Enhanced Raman Scattering Sensor.

Hydrogen peroxide (HO) widely involves in intracellular and intercellular redox signaling pathways, playing a vital role in regulating various physiological events. Nevertheless, current analytical methods for the HO assay are often hindered by relatively long response time, low sensitivity, or self-interference. Herein, a zeolitic imidazolate framework-8 (ZIF-8)-based surface-enhanced Raman scattering (SERS) sensor has been developed to detect HO released from living cells by depositing ZIF-8 over SERS active gold nanoparticles (AuNPs) grafted with HO-responsive probe molecules, 2-mercaptohydroquinone.

Electrochemically renewable SERS sensor: A new platform for the detection of metabolites involved in peroxide production.

The accurate detection of hydrogen peroxide (HO)-involved metabolites plays a significant role in the early diagnosis of metabolism-associated diseases, whereas most of current metabolite-sensing systems are often hindered by low sensitivity, interference of coexisting species, or tedious preparation. Herein, an electrochemistry-regenerated surface-enhanced Raman scattering (SERS) sensor was developed to serve as a universal platform for detecting HO-involved metabolites. The SERS sensor was constructed by modifying newly synthesized 2-mercaptohydroquinone (2-MHQ) molecules on the surface of gold nanoparticles (AuNPs) that were electrochemically predeposited on an ITO electrode.

Facile route for C-N/NbO nanonet synthesis based on 2-methylimidazole for visible-light driven photocatalytic degradation of Rhodamine B.

Herein, we fabricated a C and N co-modified NbO nanonet structure (C-N/NbONNs) from niobium oxalate using 2-methylimidazole (Hmim) as a source for C and N a simple hydrothermal route. The obtained nanonets are robust and cost-effective with excellent recycling stability. Compared with N-doped TiO (N-TiO) and a NbO control sample (NbO-CS), the resulting nanonets exhibited the highest performance toward the photocatalytic degradation of Rhodamine B (RhB) upon visible light irradiation ( > 420 nm).

Correlated Anodic-Cathodic Nanocollision Events Reveal Redox Behaviors of Single Silver Nanoparticles.

We reported a novel method to real-time monitor the redox behaviors of single Ag nanoparticles (AgNPs) at a Au ultramicroelectrode between oxidizing and reducing pulse potentials using the nanocollision electrochemical method. At fast pulse potentials, the instantaneous anodic-cathodic current transients of a single AgNP were observed for the electrooxidation of AgNP, followed by the electroreduction of the newborn silver oxide (AgO) NP in alkaline media via switching of redox potentials; however, only anodic oxidation signals of individual AgNPs were observed in neutral solution. Through this study, we have revealed the substantial different dynamic nanocollision electrochemical behaviors of single AgNPs on the electrode surface in various media.

Electrochemistry-Regulated Recyclable SERS Sensor for Sensitive and Selective Detection of Tyrosinase Activity.

Tyrosinase (TYR) which can catalyze the oxidation of catechol is recognized as a significant biomarker of melanocytic lesions, thus developing powerful methods for the determination of TYR activity is highly desirable for the early diagnosis of melanin-related diseases, including melanoma. Herein, we develop a novel portable and recyclable surface-enhanced Raman scattering (SERS) sensor, prepared by assembling gold nanoparticles and p-thiol catechol ( p-TC) on an ITO electrode, for detecting TYR activity via the SERS spectral variation caused by the conversion of p-TC into its corresponding quinone under TYR catalysis. The developed SERS sensor has a rapid response to TYR within 1 min under the optimized conditions and shows high selectivity for TYR with the detection limit at 0.

Unveiling the Intrinsic Catalytic Activities of Single-Gold-Nanoparticle-Based Enzyme Mimetics.

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.

Detection of leucine aminopeptidase activity in serum using surface-enhanced Raman spectroscopy.

Leucine aminopeptidase (LAP), an important proteolytic enzyme, is closely associated with diverse physiological and pathological disorders such as liver injury and cancers. Hence, it is imperative to develop an effective method to detect LAP activity for early diagnosis of diseases. In this work, we report a novel SERS probe bis-s-s'-[(s)-2-amino-N-(3-thiophenyl)-Leu].