High Activity Retention Research Articles

Chitin membrane for efficient laccase immobilization and synergistic removal of 17α-ethynylestradiol from water-based solutions

A unique chitin–laccase membrane was fabricated as an environmentally friendly biocatalytic platform, utilizing 1-butyl-3-methylimidazolium acetate as the solvent for chitin. Observations using scanning electron microscopy showed that the chitin-laccase membrane possessed a uniform and densely packed structure. Based on the presence of FT-IR signals at 1020 cm−1 and changes in the intensity of signals at 1540 cm−1 and 1645 cm−1, the effectiveness of laccase immobilization was confirmed. FT-IR mapping revealed that the enzyme is evenly distributed on the surface of the membrane. The catalytic activity of the native enzyme and laccase immobilized using the membrane was determined based on a model reaction, and the retention of high activity was confirmed using real solutions. Laccase immobilized using the chitinous membrane retained over 60 % of its initial activity after 30 days of storage at 4 °C. By contrast, the free enzyme retained <40 % of its initial activity. Moreover, the activity of chitin-laccase system remained at 85 % after 5 cycles. This novel chitin–laccase combination was tested in the 17α-ethynylestradiol (EE2) removal from water-based solutions. It was found that EE2 underwent synergistic degradation through concurrent adsorption and biocatalytic transformation, with enzymatic conversion as the dominant mechanism.

Enhancing Performances of Enzyme/Metal-Organic Polyhedra Composites by Mixed-Protein Co-Immobilization.

Protein immobilization using water-soluble ionic metal-organic polyhedra (MOPs) acting as porous spacers has recently been demonstrated as a potent strategy for the preparation of biocatalysts. In this article, we describe a mixed-protein approach to achieve biocomposites with adjustable enzyme contents and excellent immobilization efficiencies, in a systematic and well-controlled manner. Self-assembly of either cationic or anionic MOPs with bovine serum albumin or egg white lysozyme combined with enzymes (alkaline phosphatase, laccase or cytochrome c) led to solid-state catalysts with a high retention of enzyme activity. Furthermore, for all these systems, the dilution of enzymes within the solid-state composite led to noticeably improved catalytic performances, with both higher specific activity and affinity for substrate.

Single stage bi-substrate transglycosylation reaction for the synthesis of ascorbic acid 2 glucoside using immobilized α-glucosidase

Alpha glucosidases are multifunctional glycoside hydrolases with hydrolysis and transglycosylation ability. It can be utilized for the glycosidic bond synthesis or glycosylation of Ascorbic acid/Vitamin C to its stable analogue, Ascorbic acid 2 glucoside (AA2G), a compound with wide applications in cosmetics and pharma. The application of α-glucosidases for industrial scale transglycosylation is limited due to the low transglycosylation yield of free enzymes. Enzyme immobilization techniques could enable the development of efficient, reusable catalysts. Only a few glycoside hydrolases have been studied in immobilized form for transglycosylation reactions, and α-glucosidases are probably the least explored in this form. Transglycosylation activity of immobilized α-glucosidase from Aspergillus carbonarius BTCF 5 was studied for AA2G synthesis, where different immobilization techniques like calcium alginate encapsulation, adsorption on chitosan beads, covalent cross-linking on magnetic nanoparticles, and cross-linked enzyme aggregates (CLEA) were employed for the immobilization. The immobilization yield of calcium alginate encapsulated enzyme, enzyme immobilized on Fe-MNP support, enzyme immobilized on chitosan beads and as CLEA were 107%, 99%, 46% and 486%, respectively. CLEA was identified as the best immobilization technique for this bi-substrate reaction due to the high immobilization yield and activity retention (30% activity retained after 5 consecutive cycles). Enzyme immobilization increased the transglycosylation activity by 38%, yielding 118 mM AA2G against 72 mM by the free enzyme. This indicates the potential of immobilized α-glucosidase as a catalyst for synthesizing AA2G at an industrial scale.

Pickering emulsion co-delivery system: Stimuli-responsive biomineralized particles act as particulate emulsifiers and bioactive carriers

Pickering emulsions provide a promising platform for the efficient delivery of bioactive. However, co-delivery of fragile bioactives with different physicochemical properties for comprehensive effects still faces practical challenges due to the limited protection for bioactives and the lack of stimuli-responsive property for on-demand release. Herein, a stimuli-responsive co-delivery system is developed based on biomineralized particles stabilized Pickering emulsions. In this tailor co-delivery system, hydrophilic bioactive (pepsin) with the fragile structure is encapsulated and immobilized by biomineralization, the obtained biomineralized particles (PPS@CaCO3) are further utilized as emulsifiers to form O/W Pickering emulsions, in which the hydrophobic oxidizable bioactive (curcumin) is stably trapped into the dispersed phase. The results show that two bioactives are successfully co-encapsulated in Pickering emulsions, and benefiting from the protection capacities of biomineralization and Pickering emulsions, the activity of pepsin and curcumin shows a 7.33-fold and 144.83-fold enhancement compared to the free state, respectively. Moreover, In vitro study demonstrates that Pickering emulsions enable to co-release of two bioactives with high activity retention by the acid-induced hydrolyzation of biomineralized particles. This work provides a powerful stimuli-responsive platform for the co-delivery of multiple bioactive compounds, enabling high activity of bioactives for the comprehensive health effects.

High activity retention Al–Bi–Zn-base composite powder with mild hydrogen generation

Al–10Bi–7Zn and Al–10Bi–7Zn–1.5X (X: Cu, Fe, Ni, in wt.%) composite powders were designed and prepared through phase diagram calculation and gas atomization method. The effects of Cu, Fe, and Ni on the hydrolysis of Al–Bi–Zn-base composite powders for hydrogen production were investigated respectively. The composition and morphology of powders were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM) with energy disperse spectroscopy (EDS) analyses. Hydrolysis performance test results indicate that the additions of Cu, Fe, or Ni can modify the hydrogen production rate and enhance oxidation resistance in Al–10Bi–7Zn ternary alloy composite powder. In the quaternary composite powder system, Al–10Bi–7Zn–1.5Ni (wt.%) exhibits the best performance with the hydrogen generation yield of 75.3% (954.1 mL/g) within 500 min when reacting with distilled water at 60 °C and maintains a hydrogen yield of 57.9% (733.7 mL/g) within 1500 min after being stored (30 °C, relative humidity of 60%) for 7 d. In addition, the mechanism investigation suggested that the additions of Cu, Fe, or Ni in Al–Bi–Zn-base composite powders can stabilize the Al matrix to retain the high activity of powders resulting from inhibiting the cracking of composite powders in the air.

3-[18F]Fluoro-para-hydroxyphenethylguanidine (3-[18F]pHPG) PET-A Novel Imaging Modality for Paraganglioma.

Functional positron emission tomography (PET) imaging for the characterization of pheochromocytoma and paraganglioma (PCC/PGL) and for detection of metastases in malignant disease, offers valuable clinical insights that can significantly guide patient treatment. This work aimed to evaluate a novel PET radiotracer, 3-[18F]fluoro-para-hydroxyphenethylguanidine (3-[18F]pHPG), a norepinephrine analogue, for its ability to localize PCC/PGL. 3-[18F]pHPG PET/CT whole-body scans were performed on 16 patients (8 male:8 female; mean age 47.6 ± 17.6 years; range, 19-74 years) with pathologically confirmed or clinically diagnosed PCC/PGL. After intravenous administration of 304 to 475 MBq (8.2-12.8 mCi) of 3-[18F]pHPG, whole-body PET scans were performed at 90 minutes in all patients. 3-[18F]pHPG PET was interpreted for abnormal findings consistent with primary tumor or metastasis, and biodistribution in normal organs recorded. Standardized uptake value (SUV) measurements were obtained for target lesions and physiological organ distributions. 3-[18F]pHPG PET showed high radiotracer uptake and trapping in primary tumors, and metastatic tumor lesions that included bone, lymph nodes, and other solid organ sites. Physiological biodistribution was universally present in salivary glands (parotid, submandibular, sublingual), thyroid, heart, liver, adrenals, kidneys, and bladder. Comparison [68Ga]DOTATATE PET/CT was available in 10 patients and in all cases showed concordant distribution. Comparison [123I]meta-iodobenzylguanidine [123I]mIBG planar scintigraphy and SPECT/CT scans were available for 4 patients, with 3-[18F]pHPG showing a greater number of metastatic lesions. We found the kinetic profile of 3-[18F]pHPG PET affords high activity retention within benign and metastatic PCC/PGL. Therefore, 3-[18F]pHPG PET imaging provides a novel modality for functional imaging and staging of malignant paraganglioma with advantages of high lesion affinity, whole-body coregistered computed tomography, and rapid same-day imaging.

Novel seamless shell-core microbead for probiotics encapsulation: Influence of gel structure on storage stability and gastrointestinal activity

Probiotics have poor stability in storage and gastrointestinal digestion, resulting in low biological activity. Therefore, we have innovatively designed a shell-core microbead that can place probiotics in an independent lipid environment as a core, with an outer layer coated with a shell film composed of gelatin and/or pectin. Addition of 3% pectin to the shell layer and cross-linking with calcium ions significantly improved the physicochemical properties of the shell film of the microbeads, including water vapor permeability (WVP), water contact angle (WCA), and gel characteristics. The microbeads have spherical structure, uniform size and low moisture content (<5%). The water solubility of gelatin microbeads (Gel-Mb, 69.62%), gelatin-pectin microbeads (Gel-Pec-Mb, 61.06%) and shell cross-linked microbeads (Cro-Pec-Mb, 52.97%) decreased gradually. Cryo-scanning electron microscopy (Cryo-SEM) showed an evident shell core structure, and an apparent gel network was observed in the surface layer of shell of Cro-Pec-Mb. SEM analysis also showed the same porous network structure on the surface of Cro-Pec-Mb. The probiotic activities of Gel-Mb, Gel-Pec-Mb and Cro-Pec-Mb were 6.87, 6.76 and 6.74 log CFU/g after 4 months storage at 4 °C, respectively. This indicates that microbead encapsulation has a high retention of probiotic activity due to the effective insulation of the lipid environment from oxygen, moisture, etc. Cro-Pec-Mb can maintain the integrity of the structure and resist the enzymatic hydrolysis of digestive enzymes, reducing probiotic inactivation during the gastrointestinal digestion, with only a decrease 1.85 log CFU/g. This study show that microbeads were a promising platform for intestinal probiotic delivery.

In Situ Anchoring of Small-Sized Silver Nanoparticles on Porphyrinic Triazine-Based Frameworks for the Conversion of CO2 into α-Alkylidene Cyclic Carbonates with Outstanding Catalytic Activities under Ambient Conditions.

The preparation of catalytic hybrid materials by introducing highly dispersed metallic nanoparticles into porous organic polymers (POPs) may be an ideal and promising strategy for integrated CO2 capture and conversion. In terms of the carboxylative cyclization of propargyl alcohols with CO2, the anchoring of silver nanoparticles (AgNPs) on functional POPs to fabricate efficient heterogeneous catalysts is considered to be quite intriguing but remains challenging. In the contribution, well-dispersed AgNPs were successfully anchored onto the porphyrinic triazine-based frameworks by a simple "liquid impregnation and in situ reduction" strategy. The presence of N-rich dual active sites, porphyrin and triazine, which acted as the electron donor and acceptor, respectively, offered a huge opportunity for the nucleation and growth of metal nanoparticles. Significantly, the as-prepared catalyst Ag/TPP-CTF shows excellent catalytic activity (up to 99%) toward the carboxylative cyclization of propargyl alcohols with CO2 at room temperature, achieving record-breaking activities (TOF up to 615 h-1 at 1 bar and 3077 h-1 at 10 bar). Moreover, the catalyst can be easily recovered and reused at least 10 times with retention of high catalytic activity. The possible mechanism involves small-sized AgNP-mediated alkyne activation, which may promote highly efficient and green conversion of CO2. This work paves the way for immobilizing metal nanoparticles onto functional POPs by surface structure changes for enhanced CO2 catalysis.

Biomimetic Metal-Pyrimidine Nanoflowers: Enzyme Immobilization Platforms with Boosted Activity.

For the enzyme immobilization platform, enhancing enzyme activity retention while improving enzyme stability remains a challenge for sensitive sensing analysis. Herein, an in situ biomimetic immobilized enzyme carrier (metal-pyrimidine nanoflowers, MPNFs) synthesized by the coordination of DNA base derivative (2-aminopyrimidine) with Zn2+ in the aqueous phase at room temperature is developed. The biocompatibility of 2-aminopyrimidine and the hydrophilicity and green synthetic conditions of MPNFs allows the immobilized enzymes to retain above 91.2% catalytic activity. On this basis, a cascade catalytic platform is constructed by simultaneously immobilizing acetylcholinesterase (AChE), choline oxidase (CHO), and horseradish peroxidase (HRP) in MPNFs (AChE/CHO/HRP@MPNFs) for organophosphorus pesticides (OPs) colorimetric biosensing detection. The assay could specifically detect parathion-methyl within 13min with a wider linear range (0.1-1000.0nm) and a lower limit of detection (LOD) (0.032nm). The remarkable stability of the immobilized enzymes is also achieved under harsh environments, room temperature storage, and recycling. Furthermore, a portable and cost-effective biosensing platform is developed by integrating AChE/CHO/HRP@MPNFs with a smartphone-assisted paper device for the on-site detection of OPs. Overall, the high catalytic activity retention and the enhanced detection performance demonstrate that MPNF is a robust carrier in enzyme immobilization and holds great promise in biosensing and other field applications.

Stability of Phenolic Compounds, Antioxidant Activity and Color Parameters in Colored-Flesh Potato Chips.

Potato (Solanum tuberosum) chips are the most consumed snacks worldwide today. Colored potato chips prepared from potato cultivars with red and purple flesh are a novel alternative to traditional potato chips because of their higher phenolic compound content, such as anthocyanins and hydroxycinnamic acid derivatives (HCADs), which might make these chips healthier compared with traditional chips. There is little information on the stability of these compounds. In this study, the nutritional value of these chips was evaluated by determining phenolic profiles, antioxidant activity and color parameters with liquid chromatography diode array and mass spectrometry detection (HPLC-DAD-ESI-MS/MS) and spectrophotometric methods during storage for four months. Five anthocyanins and three HCADs were detected, with the latter compounds being the most abundant, with concentrations on average between the first (97.82 mg kg-1) and the last (31.44 mg kg-1) week of storage. Similar trends were observed in antioxidant activity and stability, with the CUPRAC method showing the highest response among all the methods employed. The color indices were stable throughout the storage time. Based on these results, colored-flesh potato chips are an optimal alternative for consumption because of their high retention of phenolic compounds and antioxidant activity during storage, providing potential benefits to human health.

Isolation and Identification of β-Glucosidases-Producing Non-Saccharomyces Yeast Strains and Its Influence on the Aroma of Fermented Mango Juice.

The cultivation and enrichment of different soils in a vineyard yielded 95 yeast species. Among them, seven strains capable of producing β-glucosidases were identified using the aescin colorimetric method. One non-Saccharomyces yeast strain was isolated from a plate containing lysine and identified using internal transcription (ITS) as Candida cf. sorbosivorans (C. cf. sorbosivorans), which was named Candida cf. sorbosivorans X1. Additionally, the enzymatic characteristics of the β-glucosidases produced by this strain were investigated. The β-glucosidases generated by C. cf. sorbosivorans X1 displayed high enzymatic activity and enzyme-activity retention in a pH range of 3.0 to 5.4 and at temperatures of 30 °C to 35 °C. Using non-targeted metabolomics methods, we investigated the alterations in metabolites during the fermentation of mango juice. The strain C. cf. sorbosivorans X1 demonstrated activity against phenols and terpenes. In the fermented mango juice (X1FMJ), we identified 41 differential metabolites. These included 14 esters, 4 hydrocarbons, 3 aldehydes, 5 ketones, 4 terpenoids, 4 alcohols, 1 aromatic hydrocarbon, 2 amines, 1 acid, and 3 heterocyclic compounds. The metabolic pathways of these differential metabolites were analyzed, revealing four key pathways: tyrosine metabolism, phenylpropanoid biosynthesis, monoterpene biosynthesis, and α-linolenic acid metabolism, which promoted the formation of aroma compounds in the fermented mango juice.

Acetylcholinesterase Adsorption on Modified Gold: Effect of Surface Chemistry on Enzyme Binding and Activity.

Surface chemistry plays a crucial role in the performance of biosensors and biocatalysts, where enzymes directly interact with a solid support. In this work, we investigated the effect of surface charge and hydrophobicity on the binding and activity of acetylcholinesterase (AChE) following direct adsorption to modified gold surfaces. Surface modifications included self-assembled monolayers (SAMs) terminated with -COO-, -NH3+, -OH, and -CH3 functional groups at varying mole %. We also investigated the effects of positively and negatively charged helical peptides covalently coupled to the SAM. Using spectroscopic ellipsometry, we measured the surface concentration of AChE on each modified surface after 1 h of adsorption. We found that surface concentration was directly proportional to surface hydrophobicity (r = 0.76). The highest binding was observed on the more hydrophobic surfaces. We also measured the specific activity of AChE on each surface using a colorimetric assay and found that activity was inversely proportional to surface hydrophobicity (r = -0.71). The highest activity was observed on the more hydrophilic surfaces. Plotting specific activity versus surface concentration showed a similar relationship, with the highest activity observed at low AChE densities (∼20% of a monolayer) on surfaces terminated with 50% -COO- or -NH3+ and 50% -CH3 functional groups. Interestingly, this is similar to the approximate composition of hydrophobic versus hydrophilic amino acid residues on the surface of AChE. These surfaces also exhibited the highest total activity: a ∼100% improvement over bare gold due to a combination of moderate binding and high activity retention. This work highlights the importance of developing new attachment strategies beyond direct adsorption that promote, tune, and optimize both high binding and high activity retention.

Immobilization of Cellulolytic Enzymes in Accurel® MP1000

Cellulases are a class of enzymes of great industrial interest that present several strategic applications. However, the high cost of enzyme production, coupled with the instabilities and complexities of proteins required for hydrolytic processes, still limits their use in several protocols. Therefore, enzyme immobilization may be an essential tool to overcome these issues. The present work aimed to evaluate the immobilization of cellulolytic enzymes of the commercial enzyme cocktail Celluclast® 1.5 L in comparison to the cellulolytic enzyme cocktail produced from the wild strain Trichoderma harzianum I14-12 in Accurel® MP1000. Among the variables studied were temperature at 40 °C, ionic strength of 50 mM, and 72 h of immobilization, with 15 m·L −1 of proteins generated biocatalysts with high immobilization efficiencies (87% for ACC-Celluclast biocatalyst and 95% for ACC-ThI1412 biocatalyst), high retention of activity, and specific activities in the support for CMCase (DNS method), FPase (filter paper method) and β-glucosidase (p-nitrophenyl-β-D-glucopyranoside method). Presenting a lower protein concentration (0.32 m·L−1) than the commercial Celluclast® 1.5 L preparation (45 m·L−1), the ACC-ThI1412-derived immobilized biocatalyst showed thermal stability at temperatures higher than 60 °C, maintaining more than 90% of the residual activities of FPase, CMCase, and β-glucosidase. In contrast, the commercial-free enzyme presented a maximum catalytic activity at only 40 °C. Moreover, the difference in molecular weight between the component enzymes of the extract was responsible for different hydrophobic and lodging interactions of proteins on the support, generating a robust and competitive biocatalyst.

Amorphous TiOx Stabilized Intermetallic Pt3Ti Nanocatalyst for Methanol Oxidation Reaction.

Intermetallic compounds, featuring atomically ordered structures, have emerged as a class of promising electrocatalysts for fuel cells. However, it remains a formidable challenge to controllably synthesize Pt-based intermetallics during the essential high-temperature annealing process as well as stabilize the nanoparticles (NPs) during the electrocatalytic process. Herein, we demonstrated a Ketjen black supported intermetallic Pt3Ti nanocatalyst coupled with amorphous TiOx species (Pt3Ti-TiOx/KB). The TiOx can not only confine Pt3Ti NPs during the synthesis and electrocatalytic process by a strong metal-oxide interaction but also promote the water dissociation for generating more OH species, thus facilitating the conversion of COad. The Pt3Ti-TiOx/KB showed a significantly enhanced mass activity (2.15 A mgPt-1) for the methanol oxidation reaction, compared with Pt3Ti/KB and Pt/C, and presented an impressively high mass activity retention (∼71%) after the durability test. This work provides an effective strategy of coupling Pt-based intermetallics with functional oxides for developing highly performed electrocatalysts.

Water-Soluble Ionic Metal-Organic Polyhedra as a Versatile Platform for Enzyme Bio-immobilization.

Metal-organic polyhedra (MOPs) can act as elementary structural units for the design of modular porous materials; however, their association with biological systems remains greatly restricted by their typically low stabilities and solubilities in water. Herein, we describe the preparation of novel MOPs bearing either anionic or cationic groups and exhibiting a high affinity for proteins. Simple mixing of the protein bovine serum albumin (BSA) and ionic MOP aqueous solutions resulted in the spontaneous formation of MOP-protein assemblies, in a colloidal state or as solid precipitates depending on the initial mixing ratio. The versatility of the method was further illustrated using two enzymes, catalase and cytochrome c, with different sizes and isoelectric points (pI's) below and above 7. This mode of assembly led to the high retention of catalytic activity and enabled recyclability. Furthermore, the co-immobilization of cytochrome c with highly charged MOPs resulted in a substantial 44-fold increase of its catalytic activity.

Carbonic Anhydrase Enhanced UV-Crosslinked PEG-DA/PEO Extruded Hydrogel Flexible Filaments and Durable Grids for CO2 Capture.

In this study, poly (ethylene glycol) diacrylate/poly (ethylene oxide) (PEG-DA/PEO) interpenetrating polymer network hydrogels (IPNH) were extruded into 1D filaments and 2D grids. The suitability of this system for enzyme immobilization and CO2 capture application was validated. IPNH chemical composition was verified spectroscopically using FTIR. The extruded filament had an average tensile strength of 6.5 MPa and elongation at break of 80%. IPNH filament can be twisted and bent and therefore is suitable for further processing using conventional textile fabrication methods. Initial activity recovery of the entrapped carbonic anhydrase (CA) calculated from esterase activity, showed a decrease with an increase in enzyme dose, while activity retention of high enzyme dose samples was over 87% after 150 days of repeated washing and testing. IPNH 2D grids that were assembled into spiral roll structured packings exhibited increased CO2 capture efficiency with increasing enzyme dose. Long-term CO2 capture performance of the CA immobilized IPNH structured packing was tested in a continuous solvent recirculation experiment for 1032 h, where 52% of the initial CO2 capture performance and 34% of the enzyme contribution were retained. These results demonstrate the feasibility of using rapid UV-crosslinking to form enzyme-immobilized hydrogels by a geometrically-controllable extrusion process that uses analogous linear polymers for both viscosity enhancement and chain entanglement purposes, and achieves high activity retention and performance stability of the immobilized CA. Potential uses for this system extend to 3D printing inks and enzyme immobilization matrices for such diverse applications as biocatalytic reactors and biosensor fabrication.

Reactive Adsorption Desulfurization of Fluid Catalytic Cracking Gasoline: The Effect of Promoters (Fe, Mo, and W) on the Structural and Catalytic Properties of Ni/ZnO Adsorbents

A series of Ni/ZnO adsorbents containing promoters (Fe, Mo, and W) were prepared for reducing the loss of the octane number because of olefin saturation during the reactive adsorption desulfurization (RADS) process. The bimetallic adsorbents synthesized by a two-step impregnation method were analyzed by a series of characterization methods to evaluate the effect of additional metal on the structural and catalytic properties of the traditional Ni/ZnO adsorbent. Hydrogen temperature-programmed reduction (H2-TPR) results showed that the addition of promoter Fe enhanced the reduction performance of NiO, while W hindered the reduction of NiO. The electron density of Ni was modified following the introduction of Fe and W, as analyzed by X-ray photoelectron spectroscopy (XPS), which weakened the adsorption of π complexation between olefins and Ni. Experimental results showed that the desulfurization performance of Ni–Mo was improved but aggravated the loss of the octane number. Ni–W effectively attenuated the olefin saturation reaction but seriously shortened the breakthrough time. The adsorbent modified by Fe can reduce the saturation reaction of olefins and improve the desulfurization performance. In addition, multicycle regeneration experiments proved the excellent regeneration performance of the adsorbent modified by an appropriate amount of Fe. Therefore, the Ni–Fe bimetallic adsorbent may become a novel adsorbent for reactive adsorption desulfurization, which achieves high desulfurization activity and olefin retention ability to satisfy the requirements of fluid catalytic cracking (FCC) gasoline refining.

Atomic hydrogen provision by cobalt sites in a bimetallic Ni/Co(OH)x and trimetallic Ni/Cu2O/Co(OH)x configurations for superior ammonia production

Electrochemical reduction of nitrate provides a green alternative for decentralized ammonia production by selectively transforming a pollutant in an added-value product. Electrocatalysts containing platinum group metals (PGM) present a high selectivity and stability for ammonia production. However, these cost-prohibitive elements motivate the design of catalysts based on earth-abundant elements with comparable performance. Herein, Ni/Co(OH)x and Ni/Cu2O/Co(OH)x interfaces illustrate high competitiveness as PGM-free substitutive electrocatalyst. Evaluation of synergistic effects and mechanisms suggest co-existing direct charge transfer reduction and catalytic hydrogenation by atomic hydrogen provision over Co(OH)x sites. Trimetallic configuration reached high nitrate conversion (90.3 %) in less than 120 min when treating solutions at environmental-relevant concentration of 30 mg L−1 NO3--N. Meanwhile, electrode stability evaluation demonstrated high activity retention (>90 %) and negligible metal leaching after 12 h of sustained use. These results motivate the exploration of electrocatalyst based on earth-abundant materials for electrochemically driven N-resource recovery.

A Systematic Investigation into the Influence of Net Charge on the Biological Distribution of Radiometalated Peptides Using [68Ga]Ga-DOTA-TATE Derivatives.

Recently, several radiometalated peptides have been approved for clinical imaging and/or therapy (theranostics) of several types of cancer; nonetheless, the primary challenge that most of these peptides confront is significant renal uptake and retention, which is often dose limiting and can cause nephrotoxicity. In response to this, numerous methods have been employed to reduce the uptake of radiometalated peptides in the kidneys, and among these is adding a linker to modulate polarity and/or charge. To better understand the influence of net charge on the biodistribution of radiometalated peptides, we selected the clinically popular construct DOTA-TATE (NETSPOT/LUTATHERA) as a model system. We synthesized derivatives using manual solid-phase peptide synthesis methods including mechanical and ultrasonic agitation to effectively yield the gold standard DOTA-TATE and a series of derivatives with different net charges (+2, +1, 0, -1, -2). Dynamic PET imaging from 0 to 90 min in healthy female mice (CD1) revealed high accumulation and retention of activity in the kidneys for the net-neutral (0) charged [68Ga]Ga-DOTA-TATE and even higher for positively charged derivatives, whereas negatively charged derivatives exhibited low accumulation and fast renal excretion. Ex vivo biodistribution at 2 h post injection demonstrated a significant retention of [68Ga]Ga-DOTA-TATE (∼74 %ID/g) in the kidneys, which increased as the net positive charge per molecule increased to +1 and +2 (∼272 %ID/g and ∼333 %ID/g, respectively), but the -1 and -2 net charged molecules exhibited lower renal uptake (∼15 %ID/g and 16 %ID/g, respectively). Interestingly, the net -2 charged [68Ga]Ga-DOTA-(Glu)2-PEG4-TATE was stable in blood serum but had much higher healthy organ uptake (lungs, liver, spleen) than the net -1 compound, suggesting instability in vivo. Although the [68Ga]Ga-DOTA-PEG4-TATE derivative with a net charge of 0 also showed a decrease in kidney uptake, it also showed instability in blood serum and in vivo. Despite the superior pharmacokinetics of the net -1 charged [68Ga]Ga-DOTA-Glu-PEG4-TATE in healthy mice with respect to kidney uptake and overall profile, dynamic PET images and ex vivo biodistribution in male mice (NSG) bearing AR42J (SSTR2 overexpressing) subcutaneous tumor xenografts showed significantly diminished tumor uptake when compared to the gold standard [68Ga]Ga-DOTA-TATE. Taken together, these findings indicate unambiguously that kidney uptake and retention are significantly influenced by the net charge of peptide-based radiotracers. In addition, it was illustrated that the negatively charged peptides had substantially decreased kidney uptake, but in this instantiation the tumor uptake was also impaired.

Effectiveness of Opuntia ficus-indica mucilage as a carrier agent in microencapsulation of bioactive compounds of Amaranthus hypochondriacus var. Nutrisol

The effectiveness of maltodextrin (10%) and cactus mucilage (CM) (0%, 0.25%, 0.50%, 0.75%, and 1%) as carrier agents was evaluated in the encapsulation of bioactive amaranth compounds. Spray drying, an efficient encapsulation method, achieved high yields (62.9%–68%). The increase in CM concentration significantly augmented the water absorption index (WAI), bulk density, and hygroscopicity of the encapsulated amaranth powders. Conversely, it significantly decreased the moisture content, water activity, and water solubility index (WSI). The glass transition temperatures (>40 °C), Hausner ratio (HR), and Carr's index (CI) values indicated the suitability of powders for handling and processing. Moreover, no cracks were observed in the microcapsules surface, which favoured the bioactive amaranth compounds retention and stability. Thus, low degradation rate constants and long half-life time values were determined for the encapsulated amaranth powders, indicative of its storage appropriateness. Incorporation of 0.75% CM was an efficient concentration to achieve high percentage retention of betacyanins (55.5%), betaxanthins (58%), total polyphenols (73.3%), amaranthine (56.8%), isoamaranthine (62.7%), individual polyphenols (44.6%–81%), and antioxidant activity (79.6%). These results demonstrated the efficiency of CM as an encapsulating agent in the food industry.