One-pot Reaction System Research Articles

Silica gel supported Cu nanoparticles for selective reductive etherification of furfural into isopropyl furfuryl ether

Furfural (FF) is one of the important platform molecules of biomass, which can be obtained by hydrolysis from lignocellulose and can produce many high value-added chemicals. In this study, a new 4.5 wt% Cu-supported silica gel (SG) catalyst with dual functions of metal and acid site was prepared by acid-base adsorption impregnation method. Isopropyl furfuryl ether (IPFE) with 80.4 % yield was obtained by one-pot reductive etherification of FF in 2-propanol at 150 °C under 2 MPa H2. The characterization of the catalyst proved that the Cu synthesized by this method was well dispersed, and the average size of Cu NPs was 3.34 nm. The reduction of FF to IPFE in a one-pot reaction system is deduced as follows: the existence of a hydrogenation-etherification pathway (main path) and an acetalization-hydrogenolysis pathway. The study in this paper provides a reference for the development of non-noble metal hydroetherification catalysts.

Co-upcycling of Plastic Waste and Biowaste via Tandem Transesterification Reactions.

Polyethylene terephthalate (PET) and glycerol are prevalent forms of plastic and biowaste, necessitating facile and effective strategies for their upcycling treatment. Herein, we present an innovative one-pot reaction system for the concurrent depolymerization of PET plastics and the transesterification of glycerol into dimethyl terephthalate (DMT), a valuable feedstock in polymer manufacturing. This process occurs in the presence of methyl acetate (MA), a byproduct of the industrial production of acetic acid. The upcycling of biowaste glycerol into glycerol acetates renders them valuable additives for application in both the biofuel and chemical industries. This integrated reaction system enhances the conversion of glycerol to acetins compared with the singular transesterification of glycerol. In this approach, cost-effective catalysts, based on perovskite-structured CaMnO3, were employed. The catalyst undergoes in situ reconstruction in the tandem PET/glycerol/MA system due to glycerolation between the metal oxides and glycerol/acetins. This process results in the formation of small metal oxide nanoparticles confined in amorphous metal glycerolates, thereby enhancing the PET depolymerization efficiency. The optimized coupled reaction system can achieve a product yield exceeding 70% for glycerol acetates and 68% for PET monomers. This research introduces a tandem pathway for the simultaneous upcycling of PET plastic waste and biowaste glycerol with minimal feedstock input and maximal reactant utilization efficiency, promising both economic advantages and positive environmental impacts.

Acid-catalyzed transformation of orange waste into furfural: the effect of pectin degree of esterification

The transformation of biomasses from agro-industrial waste can significantly impact the production of green chemicals from sustainable resources. Pectin is a biopolymer present in lignocellulosic biomass as Orange Peel Waste (OPW) and has possibilities for making platform compounds such as furfural for sustainable chemistry. In this work, we studied the transformation to furfural of OPW, pectins, and d-galacturonic acid (D-GalA), which is the main component (65 wt%) of pectin. We analyzed pectins with different degrees of esterification (45, 60 and 95 DE) in a one-pot hydrolysis reaction system and studied the differences in depolymerization and dehydration of the carbohydrates. The results show that the production of furfural decreases as the DE value increases. Specifically, low DE values favor the formation of furfural since the decarboxylation reaction is favored over deesterification. Interestingly, the furfural concentration is dependent upon the polysaccharide composition of pentoses and uronic acid. The obtained concentrations of furfural (13 and 14 mmol/L), d-xylose (6.2 and 10 mmol/L), and L-arabinose (2.5 and 2.7 mmol/L) remained the same when the galacturonic acid was fed either as a polymer or a monomer under the same reaction conditions (0.01 M SA, 90 min and 433 K). OPW is proposed as a feedstock in a biorefinery, in which on a per kg OPW dry basis, 90 g of pectin and 15 g of furfural were produced in the most favorable case. We conclude that the co-production of pectin and furfural from OPW is economically feasible.Graphical

Bench-stable oxidant sodium percarbonate for functional group transformation of arylboronic acids

Sodium percarbonate (2Na2CO3·3H2O2, sodium carbonate-hydrogen peroxide, SPC), an easily accessible and bench-stable hydrogen peroxide-solid adduct based on inorganic salt, was efficiently used as a solid hydroxylating reagent for the ipso-hydroxylation of arylboronic acids under mild conditions, affording the corresponding phenols in an excellent manner at a fast rate. Moreover, a solvent-free solid-state reaction system using SPC for the oxidative hydroxylation of arylboronic acids was also demonstrated. Furthermore, subsequent treatment with benzyl halide was successfully performed, providing an alternative synthetic route for preparing benzyl phenyl ethers in a one-pot tandem reaction system.

Covalent organic frameworks

The dream to prepare well-defined materials drives the methodological evolution for molecular synthesis, structural control and materials manufacturing. Among various methods, chemical approaches to design, synthesize, control and engineer small molecules, polymers and networks offer the fundamental strategies. Merging covalent bonds and non-covalent interactions into one method to establish a complex structural composition for specific functions, mimicking biological systems such as DNA, RNA and proteins, is at the centre of chemistry and materials science. Covalent organic frameworks (COFs) are a class of crystalline porous polymers that enable the integration of organic units into highly ordered structures via polymerization. This polymerization system is unique as it deploys covalent bonds to construct the primary order structures of polymeric backbones via polycondensation and leverages on non-covalent interactions to create the high order structures of polymeric networks via supramolecular polymerization in a one-pot reaction system. This Primer covers all aspects of the field of COFs from chemistry to physics, materials and applications, and outlines the design principle, experimental methods, characterization and applications, with an aim to show a concise yet full picture of the field. The key fundamental issues to be addressed are analysed with an outlook on the future major directions from different perspectives. Covalent organic frameworks (COFs) are a class of crystalline porous polymers consisting of highly ordered organic structures formed by polymerization. In this Primer, Tan et al. discuss the design principle, experimental methods, characterization and applications of COFs.

One-pot preparation of amphoteric cellulose polymers for simultaneous recovery of ammonium and dihydrogen phosphate from wastewater and reutilizing as slow-release fertilizer

In this paper, a simple approach was developed to prepare amphoteric cellulose adsorbent (EAC) through etherification of cellulose with glycidyl trimethyl ammonium chloride (ETA) and glycidylsulfonoic acid sodium salt (SEP) in a one-pot reaction system. The effect of the molar ratio of cellulose to ETA and SEP on the contents of sulfur and nitrogen elements in the EAC was evaluated with the aim of deriving the adsorbents with amounts of ionic functional groups. The EAC was examined for adsorption to NH4+ and H2PO4- ions. Meanwhile, the effect of adsorption parameters, including dosage of EAC, pH value of solution, contact time and ionic strength, on its adsorption capacity was also analyzed. The EAC displayed excellent affinity to the targeted ions, with an adsorption capacity of 40.38 mg/g for NH4+ and 30.42 mg/g for H2PO4-. The adsorption of EAC for NH4+ and H2PO4- reached equilibrium within 30 min and was fitted by second-order and Langmuir models well. More importantly, the EAC after adsorption could be recovered and recycled as a slow-release fertilizer, which could release approximately 95.5% of NH4+ and 92.5% of H2PO4− within 30 days. The results demonstrated that the EAC after adsorption would be reutilized as a slow-release fertilizer, which would give highlights on cost-effective and eco-friendly development in agriculture.

A thermostable Cas12b from Brevibacillusleverages one-pot discrimination of SARS-CoV-2 variants of concern.

SummaryBackgroundCurrent SARS-CoV-2 detection platforms lack the ability to differentiate among variants of concern (VOCs) in an efficient manner. CRISPR/Cas (Clustered Regularly Interspaced Short Palindromic Repeats/CRISPR-associated) based detection systems have the potential to transform the landscape of COVID-19 diagnostics due to their programmability; however, most of these methods are reliant on either a multi-step process involving amplification or elaborate guide RNA designs.MethodsThree Cas12b proteins from Alicyclobacillus acidoterrestris (AacCas12b), Alicyclobacillus acidiphilus (AapCas12b), and Brevibacillus sp. SYP-B805 (BrCas12b) were expressed and purified, and their thermostability was characterised by differential scanning fluorimetry, cis-, and trans-cleavage activities over a range of temperatures. The BrCas12b was then incorporated into a reverse transcription loop-mediated isothermal amplification (RT-LAMP)-based one-pot reaction system, coined CRISPR-SPADE (CRISPR Single Pot Assay for Detecting Emerging VOCs).FindingsHere we describe a complete one-pot detection reaction using a thermostable Cas12b effector endonuclease from Brevibacillus sp. to overcome these challenges detecting and discriminating SARS-CoV-2 VOCs in clinical samples. CRISPR-SPADE was then applied for discriminating SARS-CoV-2 VOCs, including Alpha (B.1.1.7), Beta (B.1.351), Gamma (P.1), Delta (B.1.617.2), and Omicron (B.1.1.529) and validated in 208 clinical samples. CRISPR-SPADE achieved 92·8% sensitivity, 99·4% specificity, and 96·7% accuracy within 10–30 min for discriminating the SARS-CoV-2 VOCs, in agreement with S gene sequencing, achieving a positive and negative predictive value of 99·1% and 95·1%, respectively. Interestingly, for samples with high viral load (Ct value ≤ 30), 100% accuracy and sensitivity were attained. To facilitate dissemination and global implementation of the assay, a lyophilised version of one-pot CRISPR-SPADE reagents was developed and combined with an in-house portable multiplexing device capable of interpreting two orthogonal fluorescence signals.InterpretationThis technology enables real-time monitoring of RT-LAMP-mediated amplification and CRISPR-based reactions at a fraction of the cost of a qPCR system. The thermostable Brevibacillus sp. Cas12b offers relaxed primer design for accurately detecting SARS-CoV-2 VOCs in a simple and robust one-pot assay. The lyophilised reagents and simple instrumentation further enable rapid deployable point-of-care diagnostics that can be easily expanded beyond COVID-19.

Novel dTDP-l-Rhamnose Synthetic Enzymes (RmlABCD) From Saccharothrix syringae CGMCC 4.1716 for One-Pot Four-Enzyme Synthesis of dTDP-l-Rhamnose.

Deoxythymidine diphospho-l-rhamnose (dTDP-l-rhamnose) is used by prokaryotic rhamnosyltransferases as the glycosyl donor for the synthesis of rhamnose-containing polysaccharides and compounds that have potential in pharmaceutical development, so its efficient synthesis has attracted much attention. In this study, we successfully cloned four putative dTDP-l-rhamnose synthesis genes Ss-rmlABCD from Saccharothrix syringae CGMCC 4.1716 and expressed them in Escherichia coli. The recombinant enzymes, Ss-RmlA (glucose-1-phosphate thymidylyltransferase), Ss-RmlB (dTDP-d-glucose 4,6-dehydratase), Ss-RmlC (dTDP-4-keto-6-deoxy-glucose 3,5-epimerase), and Ss-RmlD (dTDP-4-keto-rhamnose reductase), were confirmed to catalyze the sequential formation of dTDP-l-rhamnose from deoxythymidine triphosphate (dTTP) and glucose-1-phosphate (Glc-1-P). Ss-RmlA showed maximal enzyme activity at 37°C and pH 9.0 with 2.5mMMg2+, and the Km and kcat values for dTTP and Glc-1-P were 49.56μM and 5.39s−1, and 117.30μM and 3.46s−1, respectively. Ss-RmlA was promiscuous in the substrate choice and it could use three nucleoside triphosphates (dTTP, dUTP, and UTP) and three sugar-1-Ps (Glc-1-P, GlcNH2-1-P, and GlcN3-1-P) to form nine sugar nucleotides (dTDP-GlcNH2, dTDP-GlcN3, UDP-Glc, UDP-GlcNH2, UDP-GlcN3, dUDP-Glc, dUDP-GlcNH2, and dUDP-GlcN3). Ss-RmlB showed maximal enzyme activity at 50°C and pH 7.5 with 0.02mM NAD+, and the Km and kcat values for dTDP-glucose were 98.60μM and 11.2s−1, respectively. A one-pot four-enzyme reaction system was developed by simultaneously mixing all of the substrates, reagents, and four enzymes Ss-RmlABCD in one pot for the synthesis of dTDP-l-rhamnose and dUDP-l-rhamnose with the maximal yield of 65% and 46%, respectively, under the optimal conditions. dUDP-l-rhamnose was a novel nucleotide-activated rhamnose reported for the first time.

A Highly Efficient Three-Liquid-Phase-Based Enzymatic One-Pot Multistep Reaction System with Recoverable Enzymes for the Synthesis of Biodiesel.

A three-liquid-phase system (TLPS) was developed and used as a novel enzymatic one-pot multistep reaction (EOMR) system. In this system, lipase and phospholipase were enriched in a single liquid phase with a high recovery (ca. 98%) and then used for the simultaneous catalysis of mutually inhibiting and interfering reactions (hydrolysis of phospholipids and glyceride in crude oil). A novel emulsion containing the two dispersed droplets (W2/O/W2 and W1/W2 emulsion structures) could be the key reason for this phenomenon because the emulsion system not only provided a new catalytic interface but also relieved the product inhibition. As a result, the content of free fatty acid (main hydrolysate of the glyceride) and the removal of phospholipid from the crude oil could be increased to 96 and 95%, respectively, within 1 h. The product obtained from the EOMR was directly used in the production of biodiesel via enzymatic esterification, and the content of fatty acid methanol ester could be increased to 93% within 2 h. Furthermore, the enzymes in the middle phase could also be reused, at least for eight rounds without significant loss in catalytic efficiency. Therefore, the TLPS could be considered as an ideal catalytic platform for the EOMR.

Novel aggregation induced emission based 7-(diethylamino)-3-(4-nitrophenyl)-2H-chromen-2-one for forensic and OLEDs applications

In this report, a novel solvatochromism, aggregation induced emission (AIE) based 7-(diethylamino)-3-(4-nitrophenyl)-2H-chromen-2-one fluorescent probe (CFP) was synthesizes via one-pot multi-component reaction system under ultrasonication method. The synthesized CFP was characterized using different instrumental techniques namely, Fourier transform infrared spectroscopy (FTIR), Proton nuclear magnetic resonance spectroscopy (1H NMR), Mass spectrometer, Scanning electron microscope (SEM), Energy dispersive X-ray analysis (EDAX), Thermal gravimetric analysis (TGA), Transmission electron microscopy (TEM), UV−Vis spectrometry and Fluorescence spectrophotometer. The synthesized CFP produces red emission in solid as well as in liquid state. The synthesized CFP was investigated as a new labeling mediator for the visualization of latent fingerprints (LFPs) on the different non-porous materials surface. The obtained CIE result proves that the organic moiety was extremely helpful for the fabrication of red-light emitting diodes in the display device. The synthesized CFP will play a crucial role in visualizing the LFPs on various materials surface, organic light emitting diodes (OLEDs) and anti-counterfeiting applications.

Catalytic Process Development of Bio-BTX from Lignocellulose Derived Product: Preliminary Study Using Transition Metal Catalysts

Lately, the increase in biofuel production has simultaneously led to lignocellulose material disposal activities. As a waste produced by the biofuel industry, lignocellulose materials are not utilized fully yet due to their complex polymeric structure. As one compound of lignocellulose, lignin possesses the lowest economic value due to its recalcitrant nature. In this work, guaiacol as one of monomeric substance originated from lignin is used as a representative molecule to be valorized due to the existence of both hydroxyl and methoxy moiety groups in it. One important reaction of lignin monomeric substance (phenolic compounds) valorization is oxygen removal. Aromatic substances such as Benzene and Toluene are produced through oxygen removal from the guaiacol molecule. Hydrodeoxygenation of guaiacol is aimed to remove oxygen atoms from it. Though conventionally hydrogen for the Hydrodeoxygenation process is supplied by external molecular hydrogen, in this work it is supplied from hydrogen atom abstraction of methylcyclohexane. Therefore, in a one-pot catalytic reaction system, methylcyclohexane dehydrogenation is the sole hydrogen provider for subsequent hydrodeoxygenation of guaiacol and this novel concept of a circular hydrogen economy has been proven its feasibility through heterogeneous catalytic reaction schemes conducted in this work. Metal supported on zeolite beta is selected as heterogeneous catalysts to evaluate the feasibility of one-pot hydrodeoxygenation and dehydrogenation reaction. Of every catalytic reaction attempt, multiple products consist of alkylated phenol, phenol itself, and toluene are observed proofing the feasibility of this concept. Possible interaction of catalyst surface acidity and metal contents are also probed through the distribution of byproducts. Overall, sequential dehydrogenation and hydrodeoxygenation have been proven through a catalytic reaction catalyzed by metal-supported zeolite beta catalyst and this work can potentially pave the way for further application.

A Hybrid Catalytic Conversion of Corncob to Furfurylamine in Tandem Reaction with Aluminium-Based Alkaline-Treated Graphite and ω-Transaminase Biocatalyst in γ-Valerolactone–Water

Furfurylamine is an important furfural-upgrading biobased chemical for the production of pharmaceuticals, biofuels, fibers, additives, polymers, etc. In one-pot reaction system, biomass was tandemly catalyzed to furfurylamine with aluminium-based alkaline-treated graphite (Al-AG) catalyst and recombinant ω-transaminase biocatalyst. Al-AG (3.6 wt%) catalyzed corncob (75.0 g/L) to 110.0 mM furfural at 56.8% yield (based on xylan in corncob) in γ-valerolactone–water (1:4, v:v; pH 1.0) for 40 min at 180 °C. The pH-adjusted corncob-slurry (pH 7.5) containing furfural were catalyzed to furfurylamine at high yield with γ-valerolactone-tolerant Aspergillus terreus ω-transaminase biocatalyst at 35 °C using isopropylamine (3 mol isopropylamine/mol furfural) as amine donor. Such an efficient and sustainable approach for catalytic conversion of biomass to high-value-added biobased furfurylamine was successfully established in tandem reaction with Al-AG and ω-transaminase biocatalyst.

Production of levulinic acid from wet microalgae in a biphasic one-pot reaction process

This work addresses the conversion of wet microalgae to levulinic acid (LA) using a one-pot reaction system. Utilizing moisture in microalgae forms a biphasic system with an organic solvent of 1, 2-dichloroethane (DCE) is formed. This system enhances the LA yield by making an acidic environment through the decomposition of DCE in a small quantity and the recovery of products in each aqueous and organic phase. With lipid-rich Nannochloropsis gaditana and carbohydrate-rich Chlorella species, the effects of reaction variables of temperature, water content, and DCE dosage on the LA production were investigated. The LA yield was 30.13 wt% and 28.15 wt% based on the mass of total hexoses (43–47 wt% of convertible hexoses) for the two types of microalgae at 160 °C, while the yield of free fatty acids reached 90.13 w/w% at 180 °C based on the esterifiable lipid. This biphasic system facilitates the forward reaction and the product recovery for concurrent reaction and separation.

Solvent free and green synthesis of efficient solvochromism based coumarin moieties for quick visualization of LFPs and OLEDs applications

We report a novel solvochromism based coumarin thiophene fluorescent tags (CTFTs) namely, 3-(thiophen-2-yl)-2H-chromen-2-one (3a) and 6, 8-dichloro-3-(thiophen-2-yl)-2H-chromen-2-one (3b) via solvent free, eco-friendly, low-cost and one-pot multicomponent reaction system under microwave irradiation protocol. The synthesized CTFTs derivatives were characterized by different analytical techniques namely, Fourier transform infrared spectroscopy (FTIR), Proton nuclear magnetic resonance spectroscopy (1H NMR), Mass spectrometer, Powder X-ray diffraction (PXRD), Scanning electron microscope (SEM), Energy dispersive X-ray analysis (EDAX), Ultraviolet-visible (UV−vis) and Photoluminescence spectrometer (PL). The CTFTs show strong excitation peaks at 407 nm (3a) and 431 nm (3b) due to π-π* and n-π* transitions in the aromatic core and CTFTs show strong emission peaks at 456 nm (3a) and 501 nm (3b) due to σ-π* and π-π* transitions. The CTFTs derivatives exhibit cyan blue (3a) and greenish blue (3b) luminescence in liquid and solid-state. The CTFTs are investigated as an innovative category for the visualization of latent fingerprints on various non-porous material surfaces. The obtained results prove that the CTFTs can be served as promising small organic fluorescent tags for flat-panel display and latent fingerprint applications.

One-pot production of d-allulose from inulin by a novel identified thermostable exoinulinase from Aspergillus piperis and Dorea sp. d-allulose 3-epimerase

Inulin has been widely used as a cheap bioresource for producing many valuable products by enzymatic hydrolysis or microbial fermentation, such as high-fructose syrup and fructooligosaccharides. In this work, a one-pot two-enzyme reaction system was developed to produce d-allulose from inulin using A. piperis exoinulinase and Dorea sp. d-Allulose 3-epimerase. The exoinulinase that was identified from Aspergillus piperis CBS 112811 was cloned and intracellularly expressed in Escherichia coli. The enzyme displayed the maximal activity as 3750 U mg−1 at pH 6.0 and 55 °C. For the effects of different cations, Mn2+ simulated the enzyme activity by 41 %. When 10 g L−1 inulin was hydrolyzed by A. piperis exoinulinase, the conversion rate reached 98 % within 6 h. Furthermore, the optimum pH, temperature and the ratio of the two enzymes loaded for one-pot reaction were measured to be pH 6.0, 60 °C and 15/15 U mL−1, respectively. The conversion rate of inulin to d-allulose reached 23.3 % after reaction for 4 h with 10 g L−1 inulin. When adding 100 g L−1 as a substrate, 21.4 g L−1d-allulose was produced using the two-enzyme system.

Fabrication of a superhydrophilic PVDF-g-PAA@FeOOH ultrafiltration membrane with visible light photo-fenton self-cleaning performance

A self-cleaning surface can effectively solve the accumulation problem of irreversible contamination of ultrafiltration membranes. In this work, a (polyvinylidene fluoride)-g-(polyacrylic acid) (PVDF-g-PAA) ultrafiltration membrane, hereafter denoted as FAS, was prepared by a one-pot method. A superhydrophilic self-cleaning ultrafiltration membrane, hereafter denoted as FASF, was then obtained based on the strong complexation of Fe3+ with the abundant carboxyl groups at the FAS surface, which then mineralized Fe3+ into β-FeOOH nanoparticles and deposited them onto the FAS surface. This deposition was confirmed by Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray diffraction, and X-ray photoelectron spectroscopy. Bovine serum albumin (BSA) cross-flow filtration experiments confirmed the high ultrafiltration performance of FAS and FASF. FASF exhibited highly efficient degradation of methylene blue (MB) solution under visible light photo-Fenton conditions. The optimum amount of acrylic acid was 6 wt% in the one-pot reaction system, and the alkaline coagulation bath enhanced the wettability of FAS. The β-FeOOH nanoparticle content of the surface-mineralized FASF tended to be saturated after 24 h. β-FeOOH can significantly enhance the hydrophilicity and wettability of FASF and further enhance the antifouling performance of BSA. After four cycles of cleaning operation under visible light photo-Fenton conditions, the flux recovery rate of BSA-contaminated FASF reached 96.2%, and the rejection rate remained stable. FASF had superhydrophilicity, high antifouling, and fast photocatalytic self-cleaning performances, indicating good application prospects in organic wastewater treatment.

An Effective Hybrid Strategy for Conversion of Biomass into Furfurylamine by Tandem Pretreatment and Biotransamination.

In this work, an effective hybrid strategy was developed for tandem conversion of biomass to furfurylamine with tin-based solid acid Sn-Maifanitum stone and recombinant Escherichia coli whole cells harboring ω-transaminase. 90.3mM furfural was obtained from corncob (75g/L) at 170°C for 0.5h over Sn-Maifanitum stone catalyst (3.5wt%) in the aqueous media (pH 1.0), which could be further bioconverted into furfurylamine at 74.0% yield (based on biomass-derived furfural) within 20.5h. Finally, an efficient recycling and reuse of Sn-Maifanitum stone catalyst and immobilized Escherichia coli AT2018 whole-cell biocatalyst was developed for the synthesis of furfurylamine from biomass in the one-pot reaction system.

One-pot cascade catalysis at neutral pH driven by CuO tandem nanozyme for ascorbic acid and alkaline phosphatase detection

During the past decades, most reported nanozymes have been confined to limited species of enzyme-like activities and only few examples were reported to mimic tandem enzyme-like activities. To fill gaps in expanding the species and improving catalytic efficiency of nanozymes, exploring nanozymes as tandem nanozymes has turned out to be an effective method. Herein, we have presented the cupric oxide nanoparticles (CuO NPs) as tandem nanozymes, which is expected to simultaneously catalyze the cascade reaction coupling ascorbate oxidase with peroxidase like activities at temperature (45 °C) and neutral pH (pH = 7). This one-pot cascade reaction system included the oxidation of ascorbic acid (AA) to yield H2O2 and terephthalic acid (TA) oxidation reaction mediated by H2O2 to generate a fluorescence product (λex = 315 nm, λem =422 nm). More significantly, fluorescent sensors are respectively fabricated for AA, alkaline phosphatase (ALP) and l-phenylalanine (ALP inhibitor) detection coupling the catalysis of CuO tandem nanozymes with ALP enzymatic reaction. Base on these findings, this work shows high selectivity/sensitivity and low limit of detection (2.92 × 10−8 M for AA, 0.058 U/L for ALP) properly due to an in-situ reaction. CuO tandem nanozymes expand the species of nanozymes and these CuO tandem nanozymes based fluorescent sensors can be applied for one-pot nonenzymatic biomolecular sensing in clinical diagnostics, biological or pharmaceutical analysis.

Techno-economic analysis of an integrated biorefinery strategy based on one-pot biomass fractionation and furfural production

This study evaluates the techno-economic feasibility of an integrated biorefinery for the co-production of furfural, lignin, and ethanol from lignocellulosic biomass (i.e., switchgrass as a model feedstock). The proposed biorefinery is based on a novel one-pot biomass fractionation and furfural production, which is integrated into ethanol production. The one-pot reaction system uses a biphasic solvent comprising aqueous choline chloride (ChCl) and methyl isobutyl ketone (MIBK). Aqueous ChCl is the reaction medium for simultaneous pretreatment and hemicellulose conversion, while MIBK is the organic phase for in situ furfural extraction. Aspen Plus simulation indicates that 49% of total carbon in the feedstock is converted to the target products (i.e., 17.9% to furfural, 16.0% to lignin, and 15.1% to ethanol). The base case has a minimum furfural selling price (MFSP) of 625 $/t, which is about 37% lower than furfural market price. Sensitivity analysis shows that the technical parameters (e.g., reaction temperature, solid loading) have a larger effect on MFSP than the economic parameters (e.g., material cost, installation cost). The techno-economic analysis results suggest that the proposed system is cost-competitive and has low economic risk.

Biodegradation of 1,2,3-Trichloropropane to Valuable (S)-2,3-DCP Using a One-Pot Reaction System

1,2,3-trichloropropane (TCP) being one of the important environmental pollutants, has drawn significant concern due to its highly toxic and carcinogenic effects. In this study, we built a one-pot reaction system in which immobilized haloalkane dehalogenase (DhaA31) and halohydrin dehalognase (HheC) were used to catalyze the recalcitrant TCP to produce 2,3-dichloro-1-propanol (2,3-DCP) by removing epichlorohydrin (ECH). Since HheC displays a high R enantiopreference toward 2,3-DCP, the production of enantiopure (S)-2,3-DCP was expected. However, the enantioselective resolution of (R,S)-2,3-DCP by HheC was greatly inhibited by the circular reaction occurring between the product ECH and 1,3-dichloro-2-propanol (1.3-DCP). To resolve this problem, HZD-9 resin-based in situ product removal was implemented. Under the optimized conditions, TCP was completely consumed, resulting in optically pure (S)-2,3-DCP with enantiomer excess (e.e) > 99% and 40% yield (out of the 44% theoretical maximum). The scale-up resin-integrated reaction system was successfully carried out in 0.5 L batch reactor. Moreover, the system could be reused for 6 rounds with 64% of original activity retained, showing that it could be applied in the treatment of large volumes of liquid waste and producing enantiopure (S)-2,3-DCP.