Harnessing a simple ratiometric fluorescent probe for albumin recognition and beyond.

A commercially available naphthalene fluorophore serves as a ratiometric indicator for albumin, showcasing its applications in albumin-based supramolecular recognition.

Anti-cancer drug axitinib: a unique tautomerism-induced dual-emissive probe for protein analysis.

A commercial anti-cancer drug, axitinib, exhibits very stable dual emissions for discrimination of human serum albumin.

Ratiometric determination of etomidate based on an albumin-based indicator displacement assay (IDA).

The first fluorescent sensor based on the indicator displacement assay (IDA) for on-site determination of etomidate.

Kinetic Process with Anti-Frenkel Disorder in a CsPbI3 Perovskite.

Halide perovskites are rich in ionic diffusion phenomena due to their low activation energy. The soft lead iodide lattice can, in theory, endow the system with more complex defect collaborative motions. In this work, we systematically investigated the hopping mechanics of iodide interstitials with respect to various defect behaviors, such as anti-Frenkel disorder creation and annihilation. We found that the existence of iodide vacancies and interstitials can effectively lower the creation barrier of additional anti-Frenkel disorder in the halide perovskite. The free energy barriers for generating additional Frenkel defect pairs vary from 0.25 to 0.43 eV, in the proximity of those of the original iodide defects at 300 K. This finding suggests that the spontaneous creation of a specific level of anti-Frenkel disorder facilitates long-range annihilation and defect hopping processes.

Toward stabilization of formamidinium lead iodide perovskites by defect control and composition engineering.

Phase instability poses a serious challenge to the commercialization of formamidinium lead iodide (FAPbI3)-based solar cells and optoelectronic devices. Here, we combine density functional theory and machine learning molecular dynamics simulations, to investigate the mechanism driving the undesired α-δ phase transition of FAPbI3. Prevalent iodine vacancies and interstitials can significantly expedite the structural transition kinetics by inducing robust covalency during transition states. Extrinsically, the detrimental roles of atmospheric moisture and oxygen in degrading the FAPbI3 perovskite phase are also rationalized. Significantly, we discover the compositional design principles by categorizing that A-site engineering primarily governs thermodynamics, whereas B-site doping can effectively manipulate the kinetics of the phase transition in FAPbI3, highlighting lanthanide ions as promising B-site substitutes. A-B mixed doping emerges as an efficient strategy to synergistically stabilize α-FAPbI3, as experimentally demonstrated by substantially higher initial optoelectronic characteristics and significantly enhanced phase stability in Cs-Eu doped FAPbI3 as compared to its Cs-doped counterpart. This study provides scientific guidance for the design and optimization of long-term stable FAPbI3-based solar cells and other optoelectronic devices through defect control and synergetic composition engineering.

Rational design of a FA1-targeting anti-interference fluorescent probe for the point-of-care testing of albuminuria.

Albuminuria is a crucial urine biomarker of human unhealthy events such as kidney diseases, cardiovascular diseases, and diabetes. However, the accurate diagnosis of albuminuria poses a significant challenge owing to the severe interference from urine fluorescence and urine drugs. Here, we report a novel flavone-based fluorescent probe, DMC, by incorporating the FA1-targeting methylquinazoline group into a flavone skeleton with the extend π-conjugation. DMC exhibited a rapid response time, high sensitivity, and selectivity towards human serum albumin (HSA) in urine. Moreover, the red-shifted fluorescence and the FA1-targeted HSA-binding of DMC efficiently mitigated the interference from both urine fluorescence and urine drug metabolites. Furthermore, the establishment of a portable testing system highlighted the potential for point-of-care testing, offering a user-friendly and accurate approach to diagnose A2-level and A3-level albuminuria. We expect that the success of this DMC-based diagnostic platform in real urine samples can signify a significant advancement in early clinical diagnosis of albuminuria and its associated diseases.

A dual-emissive supramolecular sensor for fast and ratiometric determination of carprofen in meat.

Carprofen (CPF) is a non-steroidal anti-inflammatory drug that has been widely used in livestock for the treatment of fever and inflammation. Yet the massive use of CPF comes at the cost of its residue ubiquitous in the environment thus leading to a huge risk to human health. Therefore, development of a convenient analytical method for monitoring CPF is of considerable importance. In this study, a dual-emissive supramolecular sensor was facilely constructed using bovine serum albumin as the host and an environmentally sensitive dye as the guest. This sensor, for the first time, successfully realized the fluorescent detection of CPF with a rapid response, high sensitivity and selectivity. More importantly, this sensor exhibited a very unique ratiometric response to CPF, which endowed this method with satisfactory detection accuracy for food analysis. To the best of our knowledge, this is the first fluorescent method for fast determination of CPF in food.

A portable paper-based testing device for fast and on-site determination of nitroxynil in food.

Nitroxynil (NTX) is a common anthelmintic veterinary drug for the management of fascioliasis in food-producing sheep and cattle. Since excessive NTX residue in food can lead to several adverse side effects, such as allergic skin reaction and respiratory irritation, it is of great importance to develop an efficient analytical method for NTX determination. Herein, we report a simple fluorescent detection method based on a novel supramolecular probe capable of detecting NTX with a fast response (5 s), high sensitivity (107 nM), high selectivity, and acceptable anti-interference property. Moreover, the portable paper-based test strips were facilely prepared and successfully realized on-site determination of NTX in real edible animal products simply with the aid of a smartphone. To the best of our knowledge, this is the very first report on the portable detection of NTX. This study also provides a promising strategy for the fast and portable detection of analyte based on the host-guest system, which will lead to improved fluorescent probe design for food analysis.

The first fluorescent sensor for the detection of closantel in meat.

Closantel is widely used in the management of parasitic infestation in livestock, but is contraindicated in humans due to its high toxic to human retina. Thus, development of a fast and selective method for the detection of closantel residues in animal products is highly needed yet still challenging. In the present study, we report a supramolecular fluorescent sensor for closantel detection through a two-step screening process. The fluorescent sensor can detect closantel with a fast response (<10 s), high sensitivity, and high selectivity. The limit of detection is 0.29 ppm, which is much lower than the maximum residue level set by government. Moreover, the applicability of this sensor has been demonstrated in commercial drugs tablets, injection fluids, and real edible animal products (muscle, kidney, and liver). This work provides the first fluorescence analytical tool for accurate and selective determination of closantel, and may inspire more sensor design for food analysis.

Dual-mode supramolecular fluorescent probe for rapid and on-site detection of chlorpyrifos in the environment.

Chlorpyrifos (CPF) as a classic organophosphorus pesticide has been widely used in agricultural applications to control insects and worms. CPF in the environment can cause deaths of diverse kinds of aquatic organism and bring a high risk to human health. Therefore, the development of effective analytical method for CPF is of great importance. In this work, a novel dual-mode albumin (ALB)-based supramolecular probe FD@ALB was designed and prepared for rapid detection of CPF in the environment. The limit of detection is 0.57 µM (∼ 0.2 ppm) with a wider detection range up to 200 µM, which is satisfactory for application. The sensing mechanism can be ascribed to CPF-induced phosphorylation of ALB, thus leading to a change in the binding microenvironment of FD dye. Moreover, the paper-based test strips were used in conjunction with the FD@ALB, realizing the portable detection of CPF. This method was demonstrated to be suitable for on-site detection of CPF in various kinds of environmental samples, including water, soil, and food samples, with the aid of a smartphone. To the best of our knowledge, this is the first analytical method achieving a combination of the rapid and ratiometric detection of CPF in the environment.

Smartphone-based on-site detection of hydrogen peroxide in milk by using a portable ratiometric fluorescent probe.

The on-site detection of hydrogen peroxide (H2O2) is important for maintaining food safety as the ingestion of H2O2 can lead to serious pathological conditions. However, most reported fluorescent probes require a fluorometer to ensure readable signal output and reliable detection result. Consequently, the fluorescent detection of H2O2 can be realized only within a standard laboratory setting. Herein, we report a novel supramolecular strategy that can successfully convert the typical off-on response to H2O2 into a ratiometric response, which allows the on-site detection of H2O2 when used in conjunction with a smartphone-based 3D-printed miniaturized testing system. This method has acceptable sensitivity, good anti-interference ability, and desirable accuracy compared to a standard detection method. More importantly, this portable ratiometric method can be used to detect H2O2 residue in commercial milk samples with the simple testing apparatuses.

General Method for Pesticide Recognition Using Albumin-Based Host-Guest Ensembles.

The massive use of pesticides nowadays has led to serious consequences for the environment and public health. Fluorescence analytical methods for pesticides are particularly advantageous with respect to simplicity and portability; however, currently available fluorescence methods (enzyme-based assays and indicator displacement assays) with poor universality are only able to detect few specific pesticides (e.g., organophosphorus). Making use of the multiple flexible and asymmetrical binding sites in albumin, we herein report a set of multicolor albumin-based host-guest ensembles. These ensembles exhibit a universal but distinctive fluorescent response to most of the common pesticides and allow array-based identification of pesticides with high accuracy. Furthermore, the simplicity, portability, and visualization of this method enable on-site determination of pesticides in a practical setting. This albumin host strategy largely expands the toolbox of traditional indicator displacement assays (synthetic macrocycles as hosts), and we expect it to inspire a series of sensor designs for pesticide detection.

Fluorescence discrimination of HSA from BSA: A close look at the albumin-induced restricted intramolecular rotation of flavonoid probe.

Discrimination of human serum albumin (HSA) from bovine serum albumin (BSA) based on the fluorescence probe technique is still challenging due to similar chemical structures. In this work, a novel flavonoid-based fluorescent probe AF is reported for successful discrimination of HSA from BSA. The sensing performances of probe, including sensing dynamic, sensitivity and selectivity, have been carefully studied. Moreover, sensing mechanism was elucidated by Job's plot, displacement experiment, and molecular docking, suggesting that the specific response to HSA originated from the albumin-induced restricted intramolecular rotation (RIR) of probe. This work may provide a simple way for designing of novel probes for HSA with high selectivity.

A DS2-specific flavonoid-based probe with a unique dual-emissive response to human serum albumin.

The hydroxyl substituent in flavonoids can cause the binding site to change from DS1 to DS2 and restore the ESIPT process of flavonoids, thereby leading to a unique dual-emissive response towards human serum albumin.

Paper-Based Ratiometric Fluorescence Analytical Devices towards Point-of-Care Testing of Human Serum Albumin.

Monitoring of human serum albumin (HSA) in a point-of-care fashion is urgently needed in particular for elderly or chronically ill patients. Herein, a dual-state emissive chalcone probe having the feature of aggregation-induced emission was designed and synthesized. The concentration of HSA can be evaluated by the ratios of emission from probes in aggregated and monomeric state, which gives a visually discernible red-to-green color change. A simple, portable paper-based analytical device have been fabricated by integration of the recognition probe in the detection pad and employed for HSA test using the whole blood samples. This paper-based assay shows the analytical capability comparable to the standard testing methods but is in a point-of-care fashion, providing a promising tool for at-home HSA detection and HSA-related disease diagnosis.

A flavonoid-based fluorescent probe enables the accurate quantification of human serum albumin by minimizing the interference from blood lipids.

We herein provide a simple design strategy to improve the sensing specificity towards human serum albumin by incorporating a nitrobenzene quencher into a traditional polarity-sensitive probe in responding to the interference from blood lipids.