A novel red-to-near-infrared AIE fluorescent probe for detection of Hg2+ with large Stokes shift in plant and living cells.

Due to the highly toxic nature of mercury ions to living organisms, accurately detecting Hg2+ in water samples and biological systems is of great significance. In this study, we designed and synthesized a novel red-to-near-infrared Aggregation-Induced Emission (AIE) fluorescent probe (named as DS) based Fluorene derivatives on specifically for Hg2+ detection. Probe DS can visually identify Hg2+ through an red-to-near-infrared fluorescence enhancement change, characterized by a large Stokes shift (130 nm) and AIE feature. This probe offers a fast response, high selectivity and sensitivity. The Hg2+-induced deprotection reaction of the thioketal mechanism was thoroughly investigated using nuclear magnetic resonance spectroscopy (NMR), mass spectrometry (MS) and density functional theory (DFT) calculation. Additionly, dynamic light scattering (DLS) results indicated that the aggregation states changes of the molecular play a crucial role in the AIE fluorescence response of probe DS toward Hg2+. The red-to-near-infrared response with AIE feature not only avoids the interference of auto-fluorescence signals in complex environments, but also reduces the fluorescence quenching caused by probe molecular aggregation. This makes probe DS highly suitable for high-quality imaging detection of Hg2+ in aqueous environments. Furthermore, probe DS demonstrates the capability for visual fluorescence detection of Hg2+ concentrations in water sample, plant roots and living cells.

Effect of separation pretreatment on environmental and economic performance of sludge resource utilization.

As a new technology for accurate utilization of sludge resources, sludge inorganic-organic matter separation (IOMS) has attracted wide attention. This study examined the impact of this pretreatment on environmental and economic performance of sludge composting and incineration using life cycle assessment (LCA) and whole life costing (WLC). LCA results indicated that IOMS pretreatment reduced the energy conservation and emission reduction (ECER) values of composting and incineration by 56 % and 76 %, respectively. Meanwhile, WLC exhibited that IOMS pretreatment could cut the break-even year of incineration from 11 years to 4 years. The combination of organic sludge incineration/composting with inorganic sludge sintering ceramsite reveals excellent environmental and economic performance. The application optimization hypothesis analysis of these two routes in various provinces of China indicates that Jiangsu has the greatest development potential and should become a major promotion region.

Environmental and economic analysis of the transformation of paper mill sludge treatment technologies in China.

Paper mill sludge (PMS) is featured with a high content of cellulose and hemicellulose, and using its characteristics to make paperboard can achieve a high-value utilization of PMS, which has attracted growing interest. In this study, currently prevalent landfill, incineration technologies (generating heat and electricity by incineration), and three paperboard technologies (medium density fiberboard, pulp board, and corrugated paper) were evaluated and compared via life cycle assessment (LCA) and life cycle costing (LCC) methods. LCA results show that the PMS-to-pulp board outperforms others with an energy conservation and emission reduction (ECER) value of - 2.86 × 10-8, while the landfill exhibits the highest overall environmental impact with an ECER value of 4.80 × 10-9. LCC results reveal that the PMS-to-pulp board delivers the highest economic profit with $257.357, while the landfill is the lowest with $ - 35.63. The PMS paperboard technologies are more economically friendly than the incineration technologies due to additional electricity/steam consumption during the PMS pre-drying process in incineration. In addition, different scenarios were set up to explore national GHG emission reduction potential by increasing paperboard technologies application rate and reducing the proportion of landfill and incineration. The scenario analysis suggests that replacing 90% of landfill and incineration ratio with PMS paperboard technologies could tremendously improve the overall emission reduction performance with - 9.08 × 1010 kg CO2 eq. This result indicates that the PMS treatment technology transformation has a significant favorable impact on the achievement of the "carbon neutrality" target.

An activated near-infrared mitochondrion-targetable fluorescent probe for rapid detection of NADH.

A novel NIR fluorescent probe based on quinoline-conjugated benzo[cd]indol dual-salt for NADH was developed. This probe swiftly detects and responds sensitively to both endogenous and exogenous NADH alterations, enabling imaging of NADH fluctuations in type II diabetic and AD model cells.

NIR-II Fluorescence Sensor Based on Steric Hindrance Regulated Molecular Packing for In Vivo Epilepsy Visualization.

Fluorescence sensing is crucial to studying biological processes and diagnosing diseases, especially in the second near-infrared (NIR-II) window with reduced background signals. However, it's still a great challenge to construct "off-on" sensors when the sensing wavelength extends into the NIR-II region to obtain higher imaging contrast, mainly due to the difficult synthesis of spectral overlapped quencher. Here, we present a new fluorescence quenching strategy, which utilizes steric hindrance quencher (SHQ) to tune the molecular packing state of fluorophores and suppress the emission signal. Density functional theory (DFT) calculations further reveal that large SHQs can competitively pack with fluorophores and prevent their self-aggregation. Based on this quenching mechanism, a novel activatable "off-on" sensing method is achieved via bio-analyte responsive invalidation of SHQ, namely the Steric Hindrance Invalidation geNerated Emission (SHINE) strategy. As a proof of concept, the ClO--sensitive SHQ lead to the bright NIR-II signal release in epileptic mouse hippocampus under the skull and high photon scattering brain tissue, providing the real-time visualization of ClO- generation process in living epileptic mice.

Chitosan-based fluorescent probe for the detection of Fe3+ in real water and food samples.

Iron ions play a crucial role in the environment and the human body. Therefore, developing an effective detection method is crucial. In this paper, we report CNS2, a chitosan-based fluorescent probe utilizing naphthalimide as a fluorophore. CNS2 is designed to "quench" its own yellow fluorescence through the specific binding of compounds containing enol structures to Fe3+. Studying the fluorescence lifetime of CNS2 in the presence or absence of Fe3+ reveals that the quenching mechanism is static. The presence of multiple recognition sites on the chitosan chain bound to Fe3+ gave CNS2 rapid recognition (1 min) and high sensitivity, with a detection limit as low as 0.211 µM. Moreover, the recognition of Fe3+ by CNS2 had a good specificity and was not affected by interferences. More importantly, in this study, CNS2 was successfully utilised to prepare fluorescent composite membranes and to detect Fe3+ in real water samples and a variety of food samples. The results show that the complex sample environment still does not affect the recognition of Fe3+ by CNS2. All the above experiments obtained more satisfactory results, which provide strong support for the detection of Fe3+ by the probe CNS2 in practical applications.

Multi-source domain adaptation based tempo-spatial convolution network for cross-subject EEG classification in RSVP task.

Objective.Many subject-dependent methods were proposed for electroencephalogram (EEG) classification in rapid serial visual presentation (RSVP) task, which required a large amount of data from new subject and were time-consuming to calibrate system. Cross-subject classification can realize calibration reduction or zero calibration. However, cross-subject classification in RSVP task is still a challenge.Approach.This study proposed a multi-source domain adaptation based tempo-spatial convolution (MDA-TSC) network for cross-subject RSVP classification. The proposed network consisted of three modules. First, the common feature extraction with multi-scale tempo-spatial convolution was constructed to extract domain-invariant features across all subjects, which could improve generalization of the network. Second, the multi-branch domain-specific feature extraction and alignment was conducted to extract and align domain-specific feature distributions of source and target domains in pairs, which could consider feature distribution differences among source domains. Third, the domain-specific classifier was exploited to optimize the network through loss functions and obtain prediction for the target domain.Main results.The proposed network was evaluated on the benchmark RSVP dataset, and the cross-subject classification results showed that the proposed MDA-TSC network outperformed the reference methods. Moreover, the effectiveness of the MDA-TSC network was verified through both ablation studies and visualization.Significance.The proposed network could effectively improve cross-subject classification performance in RSVP task, and was helpful to reduce system calibration time.

Synthesis and application of hypochlorite ratiometric fluorescence probe based on cellulose.

Cellulose is the most abundant natural polymer with good biocompatibility and easy modification characteristics. In this paper, a novel cellulose fluorescence probe CNS for detecting ClO- was prepared by modifying microcrystalline cellulose (MCC). The fluorescence detection results indicate that CNS exhibits a highly specific "ratiometric" and "colorimetric" fluorescence response to ClO-. In the presence of ClO-, the fluorescence color changes from green to cyan. In addition, the color of the solution changes from yellow to colorless, which can be observed with the "naked eye". Considering the good selectivity and anti-interference ability of CNS, the probe can be used for the detection of ClO- in real water samples. Importantly, CNS composite films and test papers were prepared and showed practicability in the detection of ClO-, highlighting its broad application potentials.

A flavonol-labelled cellulose fluorescent probe combined with composite fluorescent film imaging and smartphone technology for the detection of Fe3.

Fe3+ is one of the most widely distributed and abundant elements on earth. Realizing efficient and real-time monitoring of Fe3+ is of great significance for the natural environment and the health of living organisms. In this paper, a flavonol-labelled cellulose-based fluorescent probe (ACHM) was synthesized by using dialdehyde cellulose (DAC) as the backbone and combining with flavonol derivatives (AHM - 1). The mechanism of recognizing Fe3+ was verified by characterizing the structure of ACHM by NMR, HRMS (High Resolution Mass Spectrometry), FTIR (Fourier Transform Infrared Spectroscopy), XRD (X-ray Diffraction), TG (Thermogravimetry) and SEM (Scanning Electron Microscopy). The H2O solution of the probe ACHM showed good fluorescence properties. It has quenching fluorescence properties for Fe3+, with a low limit of detection (LOD) of 0.10 µM and a fast response time of only 20 s. In addition, in order to expand the application range of the probe, ACHM was prepared as a fluorescent composite film with an average tensile strength of 32.9 MPa and an average elongation at break of 3.39 %. It shows its superiority in mechanical properties. The probe also demonstrated its practical application value for detecting Fe3+ in smartphone imaging applications.

Single-Trial EEG Classification Using Spatio-Temporal Weighting and Correlation Analysis for RSVP-Based Collaborative Brain Computer Interface.

OBJECTIVE: Since single brain computer interface (BCI) is limited in performance, it is necessary to develop collaborative BCI (cBCI) systems which integrate multi-user electroencephalogram (EEG) information to improve system performance. However, there are still some challenges in cBCI systems, including effective discriminant feature extraction of multi-user EEG data, fusion algorithms, time reduction of system calibration, etc. Methods: This study proposed an event-related potential (ERP) feature extraction and classification algorithm of spatio-temporal weighting and correlation analysis (STC) to improve the performance of cBCI systems. The proposed STC algorithm consisted of three modules. First, source extraction and interval modeling were used to overcome the problem of inter-trial variability. Second, spatio-temporal weighting and temporal projection were utilized to extract effective discriminant features for multi-user information fusion and cross-session transfer. Third, correlation analysis was conducted to match target/non-target templates for classification of multi-user and cross-session datasets. RESULTS: The collaborative cross-session datasets of rapid serial visual presentation (RSVP) from 14 subjects were used to evaluate the performance of the EEG classification algorithm. For single-user/collaborative EEG classification of within-session and cross-session datasets, STC had significantly higher performance than the existing state-of-the-art machine learning algorithms. CONCLUSION: It was demonstrated that STC was effective to improve the classification performance of multi-user collaboration and cross-session transfer for RSVP-based BCI systems, and was helpful to reduce the system calibration time.

Exploring the Interactions of Soybean 7S Globulin with Gallic Acid, Chlorogenic Acid and (-)-Epigallocatechin Gallate.

In this study, the noncovalent interaction mechanisms between soybean 7S globulin and three polyphenols (gallic acid (GA), chlorogenic acid (CA) and (-)-epigallocatechin gallate (EGCG)) were explored and compared using various techniques. Fluorescence experiments showed that GA and EGCG had strong static quenching effects on 7S fluorescence, and that of CA was the result of multiple mechanisms. The interactions caused changes to the secondary and tertiary structure of 7S, and the surface hydrophobicity was decreased. Thermodynamic experiments showed that the combinations of polyphenols with 7S were exothermic processes. Hydrogen bonds and van der Waals forces were the primary driving forces promoting the binding of EGCG and CA to 7S. The combination of GA was mainly affected by electrostatic interaction. The results showed that the structure and molecular weight of polyphenols play an important role in their interactions. This work is helpful for developing products containing polyphenols and soybean protein.

A Chitosan-Based Fluorescent Probe Combined with Smartphone Technology for the Detection of Hypochlorite in Pure Water.

Using chitosan as a raw material, 1,8-naphthimide as the fluorescent chromophore, and sulfur-containing compounds as the recognition groups, a novel naphthimide-functionalized chitosan probe, CS-BNS, for the detection of ClO- was successfully synthesized. The modification of chitosan was verified by SEM, XRD, FTIR, mapping, 13C-NMR, TG and the structure of the probe molecule was characterized. The identification performance of the probes was studied using UV and fluorescence spectrophotometers. The results show that CS-BNS exhibits a specific response to ClO- based on the oxidative reaction of ClO- to the recognition motifs, as well as a good resistance to interference. And the probe has high sensitivity and fast response time, and can complete the detection of ClO- in a pure water system within 60 s. The probe can also quantify ClO- (y = 30.698x + 532.37, R2 = 0.9833) with a detection limit as low as 0.27 µM. In addition, the combination of the probe with smartphone technology enables the visualization and real-time monitoring of ClO-. Moreover, an identification system for ClO- was established by combining the probe with smartphone technology, which realized the visualization and real-time monitoring of ClO-.

Synthesis of sulfur-containing benzo[b]pyrrolo[2,1-c][1,4]oxazine-3,9-diones: blue light promoted radical cyclization process.

The selective and controllable construction of spio-tricyclic skeletons through visible light promoted radical cyclization still remains challenging. Herein, a general and convenient protocol for the blue light-promoted radical-mediated cascade spiro-cyclization/Michael addition of N-arylpropiolamides with thiophenols under metal-free conditions was developed. In this protocol, commercially available hydrochloric acid was employed as the cheap promoter and air as the sustainable oxidant. In addition, many functional groups tolerate the reaction conditions and produce a series of sulfur-containing benzo[b]pyrrolo[2,1-c][1,4]oxazine-3,9-diones.

A robotic arm control system with simultaneous and sequential modes combining eye-tracking with steady-state visual evoked potential in virtual reality environment.

At present, single-modal brain-computer interface (BCI) still has limitations in practical application, such as low flexibility, poor autonomy, and easy fatigue for subjects. This study developed an asynchronous robotic arm control system based on steady-state visual evoked potentials (SSVEP) and eye-tracking in virtual reality (VR) environment, including simultaneous and sequential modes. For simultaneous mode, target classification was realized by decision-level fusion of electroencephalography (EEG) and eye-gaze. The stimulus duration for each subject was non-fixed, which was determined by an adjustable window method. Subjects could autonomously control the start and stop of the system using triple blink and eye closure, respectively. For sequential mode, no calibration was conducted before operation. First, subjects' gaze area was obtained through eye-gaze, and then only few stimulus blocks began to flicker. Next, target classification was determined using EEG. Additionally, subjects could reject false triggering commands using eye closure. In this study, the system effectiveness was verified through offline experiment and online robotic-arm grasping experiment. Twenty subjects participated in offline experiment. For simultaneous mode, average ACC and ITR at the stimulus duration of 0.9 s were 90.50% and 60.02 bits/min, respectively. For sequential mode, average ACC and ITR at the stimulus duration of 1.4 s were 90.47% and 45.38 bits/min, respectively. Fifteen subjects successfully completed the online tasks of grabbing balls in both modes, and most subjects preferred the sequential mode. The proposed hybrid brain-computer interface (h-BCI) system could increase autonomy, reduce visual fatigue, meet individual needs, and improve the efficiency of the system.

ERP and Pupillometry Synchronization Analysis on Rapid Serial Visual Presentation of Words, Numbers, Pictures.

Hybrid brain-computer interfaces (HBCI) combining eye-tracker has attracted the attentions of researchers in target recognition. However, there are still many issues to be addressed in rapid sequence visual presentation (RSVP) tasks, such as the effect of presentation rates and target types on event-related potentials (ERP) and pupillometry, synchronization analysis of electroencephalography (EEG) and eye-tracking, and so on. In this study, the RSVP experiments with three different target types of pictures, words and numbers at the presentation rates of 100 and 200 ms were conducted. EEG data and pupillometry data were synchronously collected from 20 university students. The results of ERP analysis showed that, among three different target types at the presentation rate of 100 ms, the picture P300 component had the largest amplitude and the longest latency. From the 100 ms presentation rates to 200 ms one for the three target types, the P300 amplitudes became smaller, and the P300 latencies became shorter. The results of pupillometry analysis showed that, at the presentation rates of 100 and 200 ms, the pupil dilation of pictures had the smallest amplitude and the shortest latency. At the two presentation rates, no significant differences of pupil size and latency were found for the three target types. For the early pupil dilation within 1000 ms, the picture pupil size was significantly smaller than the other ones, and the picture pupil acceleration had the largest average amplitude and the shortest latency. These pupillometry features within 1000 ms combining with the P300 features could be taken as the effective ones for target classification. Through synchronization analysis of the EEG data and pupillometry data, the effects of target type and presentation rate on ERP and pupil dilation were different. These results could contribute to developing the fusion methods between EEG and eye-tracking, and provide valuable references for the multi-target recognition of hybrid BCI based on eye-tracking.

Synthesis of corn bract cellulose-based Au3+ fluorescent probe and its application in composite membranes.

To achieve real-time monitoring of Au3+, a corn bract cellulose-based fluorescent probe MAC-1 for was synthesized. MAC-1 showed good fluorescence properties in DMF-H2O (1:9, v/v, pH = 7.4) solution, showed a fluorescence emission peak at 520 nm with quenching fluorescence properties for Au3+. The structure of MAC-1 was analyzed by SEM (Sample microstructure images), XRD (X-ray diffraction), FTIR (Fourier transform infrared spectroscopy), 1H NMR, Elemental analysis, EDS, Mapping and TG (Thermogravimetry) were analyzed. The fluorescence properties of the probe were also characterized by UV spectrophotometer and fluorescence spectrophotometer. The results showed that the recognition of Au3+ by the probe MAC-1 exhibited high selectivity and high sensitivity. Moreover, it is highly resistant to interference and has a short response time, which can be rapidly responded within 1 min. In addition, to improve the practical application of the probe, the probe was prepared as a fluorescent composite film and the fluorescence effect shown by the fluorescent composite film is consistent with the fluorescence change of the probe MAC-1 itself. The fluorescent composite film also has excellent selectivity and good overall physical and mechanical properties. This study provides a meaningful reference for the detection of Au3+ and further expands the application field of agroforestry waste.

Synthesis of 3,4,5-trisubstituted phenols via Rh(III)-catalyzed alkenyl C-H activation assisted by phosphonium cations.

An efficient method for the construction of various 3,4,5-trisubstituted phenol derivatives has been achieved via the Rh(III)-catalyzed coupling of phosphonium cations with internal alkynes. This protocol shows good substrate compatibility, as an array of structurally and electronically diverse phosphonium compounds react efficiently with up to 87% yield.

Assembling global and local spatial-temporal filters to extract discriminant information of EEG in RSVP task.

Objective.Brain-computer interface (BCI) system has developed rapidly in the past decade. And rapid serial visual presentation (RSVP) is an important BCI paradigm to detect the targets in high-speed image streams. For decoding electroencephalography (EEG) in RSVP task, the ensemble-model methods have better performance than the single-model ones.Approach.This study proposed a method based on ensemble learning to extract discriminant information of EEG. An extreme gradient boosting framework was utilized to sequentially generate the sub models, including one global spatial-temporal filter and a group of local ones. EEG was reshaped into a three-dimensional form by remapping the electrode dimension into a 2D array to learn the spatial-temporal features from real local space.Main results.A benchmark RSVP EEG dataset was utilized to evaluate the performance of the proposed method, where EEG data of 63 subjects were analyzed. Compared with several state-of-the-art methods, the spatial-temporal patterns of proposed method were more consistent with P300, and the proposed method can provide significantly better classification performance.Significance.The ensemble model in this study was end-to-end optimized, which can avoid error accumulation. The sub models optimized by gradient boosting theory can extract discriminant information complementarily and non-redundantly.

A Novel Near-Infrared Ratiometric Fluorescence Probe for Hg2+ Based on Quinoline-Fused Rhodamine Dye.

As one of the most toxic metals, Mercury ions cause serious environmental pollution and threaten the health of living organisms. Hence, we designed and synthesised a new near-infrared (NIR) ratiometric fluorescent probe toward monitoring of Hg2+ based on quinoline-fused rhodamine dye. Owing to the specific spirolactam ring-opening reaction, the probe exhibits a ratiometric fluorescent change after treatment of Hg2+ with increased emission in NIR and significantly reduced emission in visible region. The specific response mechanism and dual-channel fluorescence change allow the probe to have remarkable detection selectivity, fast response and high detection sensitivity. Moreover, with the properties of excellent cell permeability and low cytotoxicity, probe can be applied as detection tool for mercury ions with dual-channel ratiometric fluorescence imaging in living cell.