A unique method for determining chlorophyll content in microalgae is devised employing a gold interdigitated electrode (G-IDE) with a 10-µm gap, augmented by a nano-molecularly imprinted polymer (nano-MIP) and a titanium dioxide/multiwalled carbon nanotube (TiO2/MWCNT) nanocomposite. The nano-MIP, produced using chlorophyll template voids, successfully trapped chlorophyll, while the TiO2/MWCNT nanocomposite, synthesized by the sol-gel technique, exhibited a consistent distribution and anatase crystalline structure. The rebinding of procured chlorophyll powder, which was used as a template for nano-MIP synthesis, was identified with a high determination coefficient (R2 = 0.9857). By combining the TiO2/MWCNT nanocomposite with nano-MIP, the G-IDE sensing method achieved a slightly better R2 value of 0.9892 for detecting chlorophyll in microalgae. The presented G-IDE sensor showed a significant threefold enhancement in chlorophyll detection compared with commercially available chlorophyll powder. It had a detection limit of 0.917 mL (v/v) and a linear range that spanned from 10-6 to 1 mL. The effectiveness of the sensor in detecting chlorophyll in microalgae was confirmed through validation of its repeatability and reusability.

The present study elucidates the effectiveness of a molecularly imprinted polyacrylonitrile-imbued graphite-base electrode (MAN@G) for the selective detection of folic acid (FA) in food samples. The prime objective of the recognition and quantification of vitamin compounds like FA is the overall quality assessment of vegetables and fruits. The cost-effective, reproducible, and durable MAN@G electrode has been fabricated using acrylonitrile (AN) as the monomer and FA as the template over graphite-base. The characterization of the synthesized MAN@G electrode material has been accomplished by utilizing UV-visible (UV-vis) spectroscopy and scanning electron microscopy (SEM). A tri-electrode system based on differential pulse voltammetry (DPV) and cyclic voltammetry (CV) techniques was employed to explore the analytical performance of the synthesized electrode. Rigorous analyses divulged that a widespread linearity window could be exhibited by the electrode under an optimized experimental environment, ranging from 20 μM to 400 μM concentrations with an acceptable lower limit of detection (LOD) and limit of quantification (LOQ) of 18 nM, and 60 nM respectively. Additionally, this electrode exhibits high reproducibility, good stability, and high repeatability, with RSD values of 1.72 %, 1.32 %, and 1.19 %, respectively. The detection efficacy of the proposed electrode has been further examined in food extracts, namely orange, spinach, papaya, soybean, and cooked rice, which endorsed high accuracy compared to the high-performance liquid chromatography (HPLC) method. Moreover, the statistical results obtained from the t-test analysis were also satisfactory for the FA concentrations present in those five samples.

In the field of sensing, the development of sensors with high sensitivity, accuracy, selectivity, sustainability, simplicity, and low cost remains a key focus. Over the past decades, optical and electrochemical sensors based on molecular imprinting techniques have garnered significant attention due to the above advantages. Molecular imprinting technology utilizes molecularly imprinted polymers (MIPs) to mimic the specific recognition capabilities of enzymes or antibodies for target molecules. Recently, MIP-based sensors rooting in signal amplification techniques have been employed to enhance molecular detection level and the quantitative ability for environmental pollutants, biomolecules, therapeutic compounds, bacteria, and viruses. The signal amplification techniques involved in MIP-based sensors mainly cover nucleic acid chain amplification, enzyme-catalyzed cascade, introduction of high-performance nanomaterials, and rapid chemical reactions. The amplified analytical signals are centered around electrochemical, fluorescence, colorimetric, and surface-enhanced Raman techniques, which can effectively realize the determination of some low-abundance targets in biological samples. This review highlights the recent advancements of electrochemical/optical sensors based on molecular imprinting integrated with various signal amplification strategies and their dedication to the study of trace biomolecules. Finally, future research directions on developing multidimensional output signals of MIP-based sensors and introducing multiple signal amplification strategies are proposed.

In this study, covalent organic frameworks (COFs) were grown in situ on magnetic nitrogen-doped graphene foam (MNGF), and the resulting composite of COFs-modified MNGF (MNC) was wrapped by molecularly imprinted polymers (MNC@MIPs) for specifically capturing SAs. A magnetic solid phase extraction (MSPE) method for SAs was established using MNC@MIPs with good magnetic responsiveness. The adsorption performance of MNC@MIPs was superior to that of non-molecularly imprinted polymers (MNC@NIPs), with shorter adsorption/desorption time and higher imprinting factors. A high-efficiency SAs analytical method was developed by fusing HPLC and MNC@MIPs-based MSPE. This approach provides excellent precision, a low detection limit, and wide linearity. By analyzing fish samples, the feasibility of the approach was confirmed, with SAs recoveries and relative standard deviations in spiked samples in the ranges of 77.2-112.7 % and 2.0-7.2 %, respectively. This study demonstrated the potential use of MNC@MIPs-based MSPE for efficient extraction and quantitation of trace hazards in food.

Concerns regarding the hazard of the carcinogenic ethyl carbamate (EC) have driven attempts to exploit efficient, timely, straightforward, and economic assays for warning early food safety. Here, we proposed a novel molecularly imprinted polymer Co@MOF-MIP, with a high peroxidase (POD)-like activity and a bright blue fluorescence emission, to develop a versatile visual assay for colorimetric, fluorescent, and photothermal trimodal detection and logic gate outputting of EC. Briefly, the POD-like activity of Co@MOF-MIP made it to decompose H2O2 into ·OH for oxidizing colorless 3,3\',5,5\'-tetramethylbenzidine (TMB) into a blue oxTMB, resulting in a 660 nm irradiated photothermal effect and bursting the blue fluorescence of Co@MOF-MIP via inner filter effect, observing a decreased fluorescence signal together with an increased colorimetric and 660 nm irradiated photothermal signals. However, EC could specifically fill the imprinted cavities of Co@MOF-MIP to block the catalytic substrates TMB and H2O2 out of Co@MOF-MIP for further reacting with the inside catalytic center of Co2+, resulting in the transformation suppressing of TMB into oxTMB, yielding an EC concentration-dependent trimodal responses in fluorescence signal enhancement, colorimetric, and 660 nm irradiated photothermal signal decreases. Assisted by the portable devices such as smartphones and hand-held thermal imagers, a visual onsite portable trimodal analytical platform was proposed for EC fast and accurate detection with the low detection limits of 1.64, 1.24, and 1.78 μg/L in colorimetric, fluorescent, and photothermal modes, respectively. Interestingly, these reactive events could be programmed by the classical Boolean logic gate analysis to offer a novel promising avenue for the big data Internet of Things monitoring and warning early residual EC in a more intelligent, dynamical, fast, and accurate manner, safeguarding food safety.

Molecular imprinting is a promising approach for developing polymeric materials as artificial receptors. However, only a few types of molecularly imprinted polymers (MIPs) are commercially available, and most research on MIPS is still in the experimental phase. The significant limitation has been a challenge for screening imprinting systems, particularly for weak functional target molecules. Herein, a combined method of quantum mechanics (QM) computations and molecular dynamics (MD) simulations was employed to screen an appropriate 2,4-dichlorophenoxyacetic acid (2,4-D) imprinting system. QM calculations were performed using the Gaussian 09 software. MD simulations were conducted using the Gromacs2018.8 software suite. The QM computation results were consistent with those of the MD simulations. In the MD simulations, a realistic model of the \'actual\' pre-polymerisation mixture was obtained by introducing numerous components in the simulations to thoroughly investigate all non-covalent interactions during imprinting. This study systematically examined MIP systems using computer simulations and established a theoretical prediction model for the affinity and selectivity of MIPs. The combined method of QM computations and MD simulations provides a robust foundation for the rational design of MIPs.

The misuse of chloramphenicol (CAP) has jeopardized environmental safety. It is critical to create an effective and sensitive CAP detection technique. In this paper, a composite of chitosan (CS)-derived carbon material modified hollow spherical hydroxylated poly(3,4-propylenedioxythiophene) (PProDOT-2CH2OH) was designed, which innovatively used o-phenylenediamine and p-aminobenzoic acid as bi-functional monomers to prepare molecular imprinting polymer (MIP) sensors for highly sensitive analysis and determination of CAP. It was found that the hollow spherical structure of PProDOT-2CH2OH significantly enhanced the rapid electron migration. When combined with the CS-derived carbon material, which has multi-functional sites, it improved the electrical activity and stability of the sensor. It also provided more active centers for the MIP layer to specifically recognize CAP. Therefore, this MIP sensor had a wide linear response (0.0001 ∼ 125 μM), a low limit of detection (LOD, 6.6 pM), excellent selectivity and stability. In addition, studies showed that the sensor has potential practical value. ENVIRONMENTAL IMPLICATION: Chloramphenicol (CAP) is one of the most widely used antibiotics with the highest dosage due to its low price and broad-spectrum antimicrobial properties. Due to its incomplete metabolism in living organisms and its difficulty in degrading in the environment, contamination caused by it can pose a threat to public health. In this study, a novel molecularly imprinted sensor (MIP/PC2C1/GCE) was designed to provide a new idea for rapid and precise removal of CAP by adsorption. The detection of CAP in pharmaceutical, water quality, and food fields was realized.

The development of a highly specific recognition electrospray ionization source presents a major challenge for achieving rapid ambient mass spectrometry (AMS) detection of trace harmful substances in complex samples. In this study, we constructed a molecular imprinting nanofiber electrospinning membrane-coated steel substrate (MINMCS) based on the electrospinning strategy. This was designed as a highly specific recognition and enrichment electrospray ionization source module for AMS, where the molecular imprinting nanofiber membrane served as an excellent extraction and enrichment layer. The prepared ionization source demonstrated a sufficient loading capacity for three bioamines (BAs): histamine (HIS), tyramine (TYR), and tryptamine (TRY). With simplified sample pretreatment, this ionization source exhibited sensitivity comparable to that of high performance liquid chromatography-mass spectrometry (HPLC-MS/MS). Moreover, the entire analysis process could be completed within 1 min with acceptable recoveries (83.21-101.80%). In brief, this study introduces a new integrated recognition and enrichment electrospray ionization source for the detection of harmful substances such as bioamines, showcasing significant commercial potential for the rapid detection of foodborne harmful compounds.

The urgent need for real-time and noninvasive monitoring of health-associated biochemical parameters has motivated the development of wearable sweat sensors. Existing electrochemical sensors show promise in real-time analysis of various chemical biomarkers. These sensors often rely on labels and redox probes to generate and amplify the signals for the detection and quantification of analytes with limited sensitivity. In this study, we introduce a molecularly imprinted polymer (MIP)-based biochemical sensor to quantify a molecular biomarker in sweat using electrochemical impedance spectroscopy, which eliminates the need for labels or redox probes. The molecularly imprinted biosensor can achieve sensitive and specific detection of cortisol at concentrations as low as 1 pM, 1000-fold lower than previously reported MIP cortisol sensors. We integrated multimodal electrochemical sensors with an iontophoresis sweat extraction module and paper microfluidics for real-time sweat analysis. Several parameters can be simultaneously quantified, including sweat volume, secretion rate, sodium ion, and cortisol concentration. Paper microfluidic modules not only quantify sweat volume and secretion rate but also facilitate continuous sweat analysis without user intervention. While we focus on cortisol sensing as a proof-of-concept, the molecularly imprinted wearable sensors can be extended to real-time detection of other biochemicals, such as protein biomarkers and therapeutic drugs.

Generally, molecularly imprinted (MIP) electrochemical sensors for amino acids operate in a \"label-like\" mode. That is, after an amino acid is specifically recognized by an imprinted cavity at the sensing interface, the amino acid itself provides the sensing signal for quantitative detection. However, poorly electroactive amino acids impede electron transfer at the sensing interface and require high potentials to drive the reaction; thus, more interfering reactions tend to be triggered in practical applications, causing enhanced background noise in the detection. To address these issues, a \"label-free\" mode of the MIP sensor based on the ferrocene (Fc)/PEDOT:PSS-polypyrrole (PPy) composite was designed for the first time. The Fc/PEDOT:PSS-PPy is drop coated on the electrode surface as a substrate, and MIP polymers with specific recognition ability are immobilized on the substrate via electrostatic adsorption. As a proof of concept, l-tyrosine (l-Tyr) was selected as a model analyte and the \"label-free\" mode MIP/Fc/PEDOT:PSS-PPy sensor was constructed. The limit of detection (LOD) and linearity range of the MIP/Fc/PEDOT:PSS-PPy sensor were 2.31 × 10-11 M and from 100 pM to 5 mM, respectively. Compared with the label-like mode, the LOD was three orders of magnitude lower, the linear range was increased by three orders of magnitude, and the sensitivity was improved by more than four times. This work provides a universal and effective concept for MIP electrochemical sensing of amino acids.