Wastewater treatment has become a great concern of this century owing to the advent of different types of refractory pollutants, which needs to be effectively treated with state-of-the-art catalysts and techniques. Layered double hydroxides (LDHs), as two-dimensional (2D) layered materials, are deemed to be promising candidates for environmental remediation due to outstanding advantages, such as high surface area, unique exchangeability of intercalated anions, porous, and stable layered structure. Fenton-based processes have been demonstrated their ability in removal of recalcitrant contaminants even in low quantities. Recently, LDHs and their derivatives have emerged as an important class of Fenton-based catalysts to overcome conventional Fenton process drawbacks, including narrow working pH, potential for secondary contamination, and sludge production. This review aims to summarize the current knowledge about LDHs, different synthesis procedure, and properties of LDHs materials. A systematical investigation on the recent progress in application of multi-metals LDH-based catalysts in Fenton, Fenton-like, photo-Fenton (PF), and electro-Fenton (EF) processes and the corresponding reaction mechanisms were provided. Furthermore, key strategies (oxygen vacancies, carbon materials, incorporation of different metals, magnetic materials) to increase active sites, electron transfer rates, and hydroxyl radicals (•OH) generation, were also described, which thereby lead to improvement in the LDHs performance. The role of LDHs in the design of electrodes and EF membranes were discussed in detail. This study also summarized the applications of LDHs materials as catalysts in Fenton-based processes for elimination of different organic pollutants. Finally, this review focuses on challenges, some crucial issues of current research, and future prospects of LDH-based Fenton catalysts in environmental remediation to achieve excellent catalytic performance. It is believed that this work provides valuable insights into the efficacious applications of LDH materials in the field of Fenton-based processes. 

State-of-the-art recent applications of layered double hydroxides (LDHs) material in Fenton-based oxidation processes for water and wastewater treatment

The world today is witnessing the significant role and huge demand for molecular detection and screening in healthcare and medical diagnosis, especially during the outbreak of COVID-19. Surface-enhanced spectroscopy techniques, including Surface-Enhanced Raman Scattering (SERS) and Infrared Absorption (SEIRA), provide lattice and molecular vibrational fingerprint information which is directly linked to the molecular constituents, chemical bonds, and configuration. These properties make them an unambiguous, nondestructive, and label-free toolkit for molecular diagnostics and screening. However, new issues in molecular diagnostics, such as increasing molecular species, faster spread of viruses, and higher requirements for detection accuracy and sensitivity, have brought great challenges to detection technology. Advancements in artificial intelligence and machine learning (ML) techniques show promising potential in empowering SERS and SEIRA with rapid analysis and automatic data processing to jointly tackle the challenge. This review introduces the combination of ML and SERS/SEIRA by investigating how ML algorithms can be beneficial to SERS/SEIRA, discussing the general process of combining ML and SEIRA/SERS, highlighting the molecular diagnostics and screening applications based on ML-combined SEIRA/SERS, and providing perspectives on the future development of ML-integrated SEIRA/SERS. In general, this review offers comprehensive knowledge about the recent advances and the future outlook regarding ML-integrated SEIRA/SERS for molecular diagnostics and screening.

/pdf/machine-learning-augmented-surface-enhanced-spectroscopy-16tbd1e8.pdf

Machine learning-augmented surface-enhanced spectroscopy toward next-generation molecular diagnostics

Cells and their derived extracellular vesicles (EVs) or exosomes contain unique molecular signatures that could be used as biomarkers for the detection of severe diseases such as cancer, as well as monitoring the treatment response. Revealing these molecular signatures requires developing non-invasive ultrasensitive tools to enable single molecule/cell-level detection using a small volume of sample with low signal-to-noise ratio background and multiplex capability. Surface-enhanced Raman scattering (SERS) can address the current limitations in studying cells and EVs through two main mechanisms: plasmon-enhanced electric field (the so-called electromagnetic mechanism (EM)), and chemical mechanism (CM). In this review, we first highlight these two SERS mechanisms and then discuss the nanomaterials that have been used to develop SERS biosensors based on each of the aforementioned mechanisms as well as the combination of these two mechanisms in order to take advantage of the synergic effect between electromagnetic enhancement and chemical enhancement. Then, we review the recent advances in designing label-aided and label-free SERS biosensors in both colloidal and planar systems to investigate the surface biomarkers on cancer cells and their derived EVs. Finally, we discuss perspectives of emerging SERS biosensors in future biomedical applications. We believe this review article will thus appeal to researchers in the field of nanobiotechnology including material sciences, biosensors, and biomedical fields.

Emerging SERS biosensors for the analysis of cells and extracellular vesicles.

Designing good compatibility factor in segmented Bi0.5Sb1.5Te3 – GeTe thermoelectrics for high power conversion efficiency

The use of biomass and waste to produce adsorbent reduces the cost of water treatment. The bio-char of Sargassum oligocystum (BCSO) was modified with MnFe2O4 magnetic particles and La-metal organic framework (MOF) to generate an efficient adsorbent (BCSO/MnFe2O4@La-MOF) for fluoride ions (F-) removal from aqueous solutions. The performance of BCSO/MnFe2O4@La-MOF was compared with BCSO/MnFe2O4 and BCSO. The characteristics of the adsorbents were investigated using various techniques, which revealed that the magnetic composites were well-synthesized and exhibited superparamagnetic properties. The maximum adsorption efficiencies (BCSO: 97.84%, BCSO/MnFe2O4: 97.85%, and BCSO/MnFe2O4@La-MOF: 99.36%) were achieved under specific conditions of pH 4, F- concentration of 10 mg/L, and adsorbent dosage of 3, 1.5, and 1 g/L for BCSO, BCSO/MnFe2O4, and BCSO/MnFe2O4@La-MOF, respectively. The results demonstrated that the experimental data adheres to a pseudo-second-order kinetic model. The enthalpy, entropy, and Gibbs free energy were determined to be negative; thus, the F- adsorption was exothermic and spontaneous in the range of 25-50 °C. The equilibrium data of the process exhibited conformity with the Langmuir model. The maximum adsorption capacities of F- ions were determined as 10.267 mg/g for BCSO, 14.903 mg/g for the BCSO/MnFe2O4, and 31.948 mg/g for BCSO/MnFe2O4@La-MOF. The KF and AT values for the F- adsorption were obtained at 21.03 mg/g (L/mg)1/n and 100 × 10+9 L/g, indicating the pronounced affinity of the BCSO/MnFe2O4@La-MOF towards F- than other samples. The significant potential of the BCSO/MnFe2O4@La-MOF magnetic composite for F- removal from industrial wastewater, makes it suitable for repeated utilization in the adsorption process. 

Amendment of Sargassum oligocystum bio-char with MnFe2O4 and lanthanum MOF obtained from PET waste for fluoride removal: A comparative study.

Cold-Sintered Bi2Te3-Based Materials for Engineering Nanograined Thermoelectrics

Efficient removal of heavy metal ions from wastewater and fixation of heavy metals in soil by manganese dioxide nanosorbents with tailored hollow mesoporous structure

Circulating tumor cells (CTCs) usually shed from primary and metastatic tumors serve as an important tumor marker, and easily cause fatal distant metastasis in cancer patients. Accurately and effectively detecting CTCs in a peripheral blood sample is of great significance in early tumor diagnosis, efficacy evaluation, and postoperative condition monitoring. In this work, a TiO2@Ag nanostructure is structured as a SERS substrate, rhodamine 6G (R6G) is used as a Raman signal molecule, the reduced bovine serum protein (rBSA) acts as a protective agent, and folic acid (FA) acts as a target molecule to specifically recognize cancer cells. A TiO2@Ag-based SERS bioprobe is successfully prepared with the feature of ultrahigh sensitivity, good specificity, low toxicity, and high accuracy in CTC detection. The remarkable SERS activity of the TiO2@Ag nanostructure is synergistically contributed by surface plasmon resonance and photon-induced charge transfer mechanism. The limit of detection for rhodamine 6G (R6G) molecules adsorbed on the TiO2@Ag SERS substrate is 5 × 10-14 M, and the corresponding SERS enhancement factor can reach 7.61 × 107. The designed TiO2@Ag-R6G-rBSA-FA SERS bioprobe is effectively utilized in detecting various cancer cells in rabbit blood, and the limit of detection (LOD) for the target cancer cell is 1 cell per mL. Notably, CTCs in peripheral blood of six clinical liver cancer patients are successfully recognized via the TiO2@Ag-based SERS bioprobe. Accurately recognizing CTCs in peripheral blood based on the TiO2@Ag-R6G-rBSA-FA SERS bioprobe is also carefully verified by in situ immunofluorescence staining experiments, which directly supports the CTC detection accuracy of the SERS strategy. These results demonstrate that the TiO2@Ag-based SERS bioprobe has great application potential in early screening and diagnosis of tumors.

Ultrahigh SERS activity of the TiO2@Ag nanostructure leveraged for accurately detecting CTCs in peripheral blood.

Synthesis of hollow mesoporous manganese dioxide nanoadsorbents with strong negative charge and their ultra-efficient adsorption for cationic dyes

Endo/exo-genous dual-stimuli responsive gold nanotetrapod-based nanoprobe for magnetic resonance imaging and enhanced multimodal therapeutics by amplifying·OH generation.

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