Mercury Adsorption and Oxidation Performance of an Iron-Based Oxygen Carrier during Coal Chemical Looping Process.

During chemical looping combustion (CLC) and chemical looping gasification (CLG) of coal, the release, migration, and speciation of mercury in coal are significantly influenced by oxygen-carrier materials; however, the underlying mechanism remains inadequately addressed. In this work, the effect of a typical iron-based oxygen carrier on the release behavior of mercury from a bituminous coal and a lignite was investigated based on the Ontario-Hydro method. It is found that the effect of the iron-based oxygen carrier is attributed to three aspects: the enhanced release rate of mercury from coal, the adsorption of the released mercury, and the oxidization of gaseous Hg0 into Hg2+. With the increasing temperature, the adsorbance of mercury by the iron-based oxygen carrier decreases, while the oxidation of mercury enhances. Even at 900 °C, the adsorbance of mercury by the oxygen carrier remained at 0.1687 g/g, with a relative content of Hg2+ at 22.55%. Additionally, it was observed that iron-based oxygen carriers can physically absorb both Hg0 and Hg2+, while chemisorption refers to complex-compound formation between the iron-based oxygen carrier and mercury.

Gold nanoparticles-decorated peptide hydrogel for antifouling electrochemical dopamine determination.

A reliable and brief ultralow fouling electrochemical sensing system capable of monitoring targets in complex biological media was constructed and validated based on gold nanoparticles-peptide hydrogel-modified screen-printed electrode. The self-assembled zwitterionic peptide hydrogel was prepared by a newly designed peptide sequence of Phe-Phe-Cys-Cys-(Glu-Lys)3 with the N-terminal modified with a fluorene methoxycarbonyl group. The thiol groups on cysteine of the designed peptide are able to self-assemble with AuNPs to form a three-dimensional nanonetwork structure, which showed satisfactory antifouling capability in complex biological media (human serum). The developed gold nanoparticles-peptide hydrogel-based electrochemical sensing platform displayed notably sensing properties for dopamine determination, with a wide linear range (from 0.2 nM to 1.9 µM), a low limit of detection (0.12 nM), and an excellent selectivity. This highly sensitive and ultralow fouling electrochemical sensor was fabricated via simple preparation with concise components that avoid the accumulation of layers with single functional material and complex activation processes. This ultralow fouling and highly sensitive strategy based on the gold nanoparticles-peptide hydrogel with a three-dimensional nanonetwork offers a solution to the current situation of various low-fouling sensing systems facing impaired sensitivity and provides a potential path for the practical application of electrochemical sensors.

A low-fouling electrochemical biosensor for biomarker detection in serum based on designed α/ß-peptides with anti-enzymolysis and antifouling capabilities.

The zwitterionic peptides, especially those composed of glutamic (E) and lysine (K) groups have drawn enormous attention as antifouling biomaterials owing to their strong hydration capability and biocompatibility. However, the susceptibility of α-amino acid K to the proteolytic enzymes in human serum limited the broad application of such peptides in biological media. Herein, a new multifunctional peptide with favorable stability in human serum was designed, and it was composed of three sections with immobilizing, recognizing and antifouling capabilities, respectively. The antifouling section was composed of alternating E and K amino acids, but the enzymolysis-susceptive amino acid α-K was replaced by the unnatural ß-K. Compared with the conventional peptide composed of all α-amino acids, the α/ß-peptide exhibited significantly enhanced stability and longer antifouling performance in human serum and blood. The electrochemical biosensor based on the α/ß-peptide showed a favorable sensitivity to its target IgG, with a quite wide linear range from 100 pg mL-1 to 10 µg mL-1 and a low detection limit (33.7 pg mL-1, S/N = 3), and it was promising for the detection of IgG in complex human serum. The tactic of designing antifouling α/ß-peptides offered an efficient way to develop low-fouling biosensors with robust operation in complex body fluids.

Peptide nucleic acid and antifouling peptide based biosensor for the non-fouling detection of COVID-19 nucleic acid in saliva.

The electrochemical biosensor with outstanding sensitivity and low cost is regarded as a viable alternative to current clinical diagnostic techniques for various disease biomarkers. However, their actual analytical use in complex biological samples is severely hampered due to the biofouling, as they are also highly sensitive to nonspecific adsorption on the sensing interfaces. Herein, we have constructed a non-fouling electrochemical biosensor based on antifouling peptides and the electroneutral peptide nucleic acid (PNA), which was used as the recognizing probe for the specific binding of the viral RNA of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Different from the negatively charged DNA probes that will normally weaken the biosensors' antifouling capabilities owing to the charge attraction of positively charged biomolecules, the neutral PNA probe will generate no side-effects on the biosensor. The biosensor demonstrated remarkable sensitivity in detecting SARS-CoV-2 viral RNA, possessing a broad linear range (1.0 fM - 1.0 nM) and a detection limit down to 0.38 fM. Furthermore, the sensing performance of the constructed electrochemical biosensor in human saliva was nearly similar to that in pure buffer, indicating satisfying antifouling capability. The combination of PNA probes with antifouling peptides offered a new strategy for the development of non-fouling sensing systems capable of assaying trace disease biomarkers in complicated biological media.

A wearable sensor based on multifunctional conductive hydrogel for simultaneous accurate pH and tyrosine monitoring in sweat.

Flexible and wearable sweat sensors have drawn extensive attention by virtue of their continuous and real-time monitoring of molecular level information. However, current sweat-based sensors still pose several challenges, such as low accuracy for analytes detection, susceptibility to microorganism and poor mechanical performance. Herein, we demonstrated a noninvasive wearable sweat sensing patch composed of an electrochemical sensing system, and a pilocarpine-based iontophoretic system to stimulate sweat secretion. The electrochemical sensor based on tannic acid-Ag-carbon nanotube-polyaniline (TA-Ag-CNT-PANI) composite hydrogel was designed for on-body detection of pH and tyrosine (Tyr), a disease marker associated with multiple disorders, such as tyrosinemia and bulimia nervosa. The wearable sweat sensor can not only monitor the pH and Tyr in sweat simultaneously, but also further calibrate Tyr detection results with the measured pH value, so as to eliminate the effect of Tyr response variance at different pH and enhance the accuracy of the sensor. Furthermore, the presence of tannic acid chelated-Ag nanoparticles (TA-Ag NPs) and carbon nanotubes (CNTs) significantly improved the conductivity and flexibility of the hydrogel and endowed the composite hydrogel with antibacterial capability. Of note, the constructed wearable sensor was capable of monitoring Tyr with enhanced accuracy in various sweats.

Designed multifunctional peptides with two recognizing branches specific for one target to achieve highly sensitive and low fouling electrochemical protein assay in human serum.

Herein, an antifouling electrochemical biosensor based on designed multifunctional peptides with two recognizing branches specific for one target was proposed to improve the target recognition efficiency and sensitivity. The designed multifunctional peptide contains two different recognizing branches (with sequences FYWHCLDE and FYCHTIDE) for immunoglobulin G (IgG), an antifouling sequence (EKEKEK) and an anchoring sequence (CPPPP), which can be immobilized onto the gold nanoparticles (AuNPs) and poly(3,4-ethylenedioxythiophene) (PEDOT) modified electrode surface. Owing to the synergistic effect of the two recognizing branches, the dual-recognizing peptide-based biosensor exhibited significantly enhanced sensitivity. Under the optimal experimental conditions, the biosensor for IgG exhibited a linear response range of 0.1 pg/mL to 0.1 µg/mL, with a limit of detection of 0.031 pg/mL (about 2 orders of magnitude lower than that of the normal biosensor). Moreover, the biosensor was also capable of assaying IgG in real biological samples such as human serum without suffering from significant biofouling. This strategy for biosensor construction not only ensures the ultra-sensitivity for target detection, but also effectively avoids biofouling on sensing interfaces in complex biological media.

d-Amino Acid-Based Antifouling Peptides for the Construction of Electrochemical Biosensors Capable of Assaying Proteins in Serum with Enhanced Stability.

The susceptibility of peptides to proteolytic degradation in human serum significantly hindered the potential application of peptide-based antifouling biosensors for long-term assaying of clinical samples. Herein, a robust antifouling biosensor with enhanced stability was constructed based on peptides composed of d-amino acids (d-peptide) with prominent proteolytic resistance. The electrode was electropolymerized with poly(3,4-ehtylenedioxythiophene) and electrodeposited with Au nanoparticles (AuNPs), and the d-peptide was then immobilized onto the AuNPs, and a typical antibody specific for immunoglobulin M (IgM) was immobilized. Because of the effect of d-amino acids, the d-peptide-modified electrode surface showed prominent antifouling capability and high tolerance to enzymatic hydrolysis. Moreover, the d-peptide-modified electrode exhibited much stronger long-term stability, as well as antifouling ability in human serum than the electrode modified with normal peptides. The electrochemical biosensor exhibited a sensitive response to IgM linearly within the range of 100 pg mL-1 to 1.0 µg mL-1 and a very low detection limit down to 37 pg mL-1, and it was able to detect IgM in human serum with good accuracy. This work provided a new strategy to develop robust peptide-based biosensors to resist the proteolytic degradation for practical application in complex clinical samples.

Open-Source and Reduced-Expenditure Nanosystem with ROS Self-Amplification and Glutathione Depletion for Simultaneous Augmented Chemodynamic/Photodynamic Therapy.

Reactive oxygen species (ROS)-induced cell apoptosis has emerged as an efficient strategy for cancer therapy. However, tumor hypoxia and insufficient amounts of endogenous hydrogen peroxide (H2O2) in the tumor microenvironment are currently the main limitations of photodynamic therapy (PDT) and chemodynamic therapy (CDT). Moreover, the glutathione (GSH) scavenging effect on ROS further hinders the efficiency of ROS-mediated therapy. Here, a CaO2-based nanosystem (named as CF@CO@HC) with ROS self-amplification and GSH-depletion abilities was developed by a bottom-up approach. This hybrid nanoparticle consisted of a photosensitizer-doped calcium peroxide (CaO2) core (CaO2-FM), a hybrid organosilica framework (Cu-ONS) incorporated with Fenton reagents (Cu2+) and tetrasulfide groups, and a local hydrophobic cage (HC) shell. The photosensitizer was fluorescein derivative 4-FM with a thermally activated delayed fluorescence (TADF) property. The HC shell was built to protect the CaO2 and the photosensitizer from being attacked by water. Upon being internalized into cancer cells, the nanosystem was decomposed through the reduction reactions of Cu2+ and the tetrasulfide bond-doped silica shell by GSH, thus releasing Cu+ for Cu+-mediated CDT. Meanwhile, the exposed CaO2-FM can react with H2O to liberate photosensitizer 4-FM and generate H2O2 and O2 to overcome barriers in CDT and PDT. Thus, our study provided an open-source and reduced-expenditure strategy via GSH depletion and ROS self-amplification behaviors for ROS generation and significantly achieved an improved synergistic PDT/CDT for cancers.

Supported Liquid Membranes Based on Bifunctional Ionic Liquids for Selective Recovery of Gallium.

In this work, separation and recovery of gallium from aqueous solutions was examined using acid-base bifunctional ionic liquids (Bif-ILs) in both solvent extraction and supported liquid membrane (SLM) processes. The influence of a variety of parameters, such as feed acidity, extractant concentration and metal concentration on the solvent extraction behavior were evaluated. The slope method combined with FTIR spectroscopy was utilized to determine possible extraction mechanisms. The SLM containing Bif-ILs demonstrated highly selective facilitated transport of 96.2% Ga(III) from feed to stripping solution after optimization. During the evaluation of the separation performance of SLM for the transport of Ga(III), in the presence of Al(III), Mg(II), Cu(II) and Fe(II), 88.5% Ga(III) could be transported with only 6% Fe(II) and a nil quantity of other metals co-transported. SLM exhibited excellent long-time stability in five repeated transport cycles. Highly selective transport and separation performance was achieved using the SLM containing Bif-ILs, indicating considerable potential for application in Ga(III) recovery.

Human Wharton's jelly cells can be induced to differentiate into growth factor-secreting oligodendrocyte progenitor-like cells.

Human Wharton's jelly-derived mesenchymal stromal cells (hWJ-MSCs) are capable of differentiating into neural and astroglia-like cell types. However, a reliable means of inducing the selective differentiation of hWJ-MSCs into oligodendrocyte progenitor cells (OPCs) in vitro has not yet been established. In this study, the OPC-like differentiation of hWJ-MSCs was characterized using and immunoblotting. The hWJ-MSC-derived OPC-like cells were able to secrete nerve growth factors and promote neurite outgrowth in vitro. These results show that hWJ-MSCs can be induced to differentiate into cells with the morphologic, phenotypic and functional characteristics of OPC-like cells.

Biocompatible peptide hydrogels with excellent antibacterial and catalytic properties for electrochemical sensing application.

A unique electrochemical sensor was constructed based on designed peptide hydrogels loaded with ciprofloxacin and gold nanoparticles, which exhibited excellent biocompatibility, antibacterial capability and electrochemical catalytic property. The peptide hydrogel was prepared base on the self-assembly of a designed short peptide sequence of Phe-Glu-Lys-Phe (FEKF) with the N-terminal modified with a fluorene methoxycarbonyl (Fmoc) group. The peptide hydrogel possessed nanofibrous network structure and exhibited good shear-thinning behavior and excellent biocompatibility, and it can be easily doped with gold nanoparticles and the antibiotic drug ciprofloxacin. The loaded antibacterial drug offered remarkable antibacterial activity of the hydrogel, while the loaded gold nanoparticles rendered the hydrogel excellent electrochemical catalytic capability towards the detection of a typical neurotransmitter dopamine. The combination of the antibacterial property and the electrochemical catalytic ability within a peptide hydrogel ensured the development of sensitive and antibacterial electrochemical sensors, and this strategy was expected to promote the construction of implantable sensors without infection.

An electrochemical biosensor for alpha-fetoprotein detection in human serum based on peptides containing isomer D-Amino acids with enhanced stability and antifouling property.

The development of antifouling biosensors capable of detecting biomarkers at low concentrations in complex bio-fluids with many interference components is of great importance in the diagnosis and treatment of diseases. Certain zwitterionic peptides composed of natural L-amino acids have been used for the construction of low fouling biosensors and demonstrated excellent antifouling performances, but they are prone to enzymatic degradation in biological media, such as serum that contains a variety of enzymes. In this work, a novel antifouling peptide with the sequence of cppPPEKEKEkek was designed, and three unnatural D-amino acids were set at both ends of the peptide to enhance its tolerance to enzymatic degradation. An electrochemical biosensor was constructed by coupling the antifouling peptide with a conducting polymer polyaniline (PANI) to achieve accurate detection of alpha-fetoprotein (AFP) in clinical samples. Owing to the presence of the designed peptide with partial D-amino acids (pD-peptide), the biosensing interface showed significantly high antifouling performance and enhanced stability in human serum. Meanwhile, the pD-peptide based biosensor exhibited high sensitivity toward the target AFP, with the linear range from 0.1 fg mL-1 to 1.0 ng mL-1 and the limit of detection of 0.03 fg mL-1 (S/N = 3). This strategy of enhancing the stability (tolerance to enzymolysis) of antifouling peptides in biological samples provided an effective way to develop antifouling biosensors for practical applications.

Dietary apple pectic oligosaccharide improves reproductive performance, antioxidant capacity, and ovary function of broiler breeders.

Reproduction performance is one of the most important economic traits for the poultry industry. Intriguingly, apple pectic oligosaccharide (APO) could promote gastrointestinal function and immune function to improve performance; however, literature about APO on reproduction performance in breeders is limited. This study aimed to determine whether APO administration can improve reproduction performance and ovary function of broiler breeders with different egg laying rates. Two hundred and fifty six Arbor Acres broiler breeders (48-week-old) were used in a 2 × 2 factorial design with 2 egg laying rates (average [AR] and low [LR]) and 2 dietary levels of APO (0 and 200 mg/kg APO). Results showed that the LR breeders presented higher egg weight but lower egg laying rate, qualified egg rate, and feed efficiency than the AR breeders (P(laying) < 0.05). Also, the LR breeders had decreased serum Anti-Müllerian hormone, leptin, and antioxidant enzyme (superoxide dismutase, total antioxidant capacity) levels than the AR breeders (P(laying) ≤ 0.05). Dietary supplementation with APO improved egg weight, feed efficiency, as well as egg albumen quality (higher albumen height and Haugh unit) (P(APO) < 0.05), and decreased the concentration of pro-inflammatory cytokine levels (interleukin [IL]-1ß, IL-8) in serum (P(APO) ≤ 0.05). The apoptosis rate and pro-apoptosis-related gene expression (caspase 9 and Bax) in the ovary of LR breeders were higher, while the anti-apoptosis-related gene expression (Bcl-2, PCNA) was lower in LR compared with the AR breeders (P(laying) < 0.05). Dietary supplementation with APO decreased the caspase 9 and Bax expression in LR breeders (P(interaction) < 0.05), and increased the Bcl-2 and PCNA expression in the 2 breeders (P(APO) < 0.05). These findings indicate that breeders with a lower egg laying rate exhibit lower antioxidant capacity and high cell apoptosis in the ovary. Dietary supplementation with APO might improve albumen quality and antioxidant capacity, and decrease the inflammatory factors and ovary apoptosis-related genes expression to improve ovary function. Moreover, the effect of APO on decreasing ovarian pro-apoptosis-related gene expression was more pronounced in lower reproductive breeders.

The impact of dietary supplementation of different feed additives on performances of broiler breeders characterized by different egg-laying rate.

This study was conducted to determine the impact of different feed additives on reproductive performance, egg quality, intestinal morphology, and blood metabolic profile of broiler breeder with different egg-laying rate. A total of 512 AA broiler breeders (48 wk old) were used in a 2 × 4 factorial design which encompassed 2 egg-laying rate levels [average (AR) and low (LR)] and 4 different dietary groups [control (no additive), 6 × 108 CFU/kg Enterococcus faecium (EF), 200 mg/kg apple pectic oligosaccharide (APO), and 1,000 mg/kg tributyrin (TRI)]. As expected, the LR breeders presented higher egg weight, eggshell thickness (P < 0.05), and feed conversion ratio as well as lower egg-laying and qualified egg rate than the AR breeders (P < 0.01). Dietary supplementation with the 3 additives improved egg weight (P ≤ 0.01). Dietary APO addition improved albumen height and Haugh units (P < 0.05) in both AR and LR breeders. Compared with APO and TRI, dietary EF addition increased eggshell thickness (P ≤ 0.01). An effect of the egg-laying rate and dietary additives on eggshell thickness (P < 0.01) was noted, with the addition of EF enhancing the eggshell thickness, which is more pronounced in the AR group. The duodenum of AR breeders presented a lower crypt depth and a higher villus/crypt ratio (P < 0.05); moreover, an effect of the laying rate and dietary additives on crypt depth was noted (P < 0.05), with the addition of APO to the diet resulting in a lower crypt depth. Compared with the APO and TRI, dietary EF addition increased follicle-stimulating hormone (FSH) level in serum (P < 0.05). Overall, the results gathered in this study indicate that LR breeders have lower production performance, eggshell thickness and decreased gastrointestinal tract functionality in compared with the AR breeders. Dietary supplementation with APO might improve albumen quality and decrease duodenal morphology, while EF improved eggshell quality and FSH secretion, and the improvement was more pronounced in the breeders with an average egg-laying rate.