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1.
Sci Data ; 11(1): 426, 2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38658574

RESUMO

Yellow-cheek carp (Elopichthys bambusa) is a typical large and ferocious carnivorous fish endemic to East Asia, with high growth rate, nutritional value and economic value. In this study, a chromosome-level genome of yellow-cheek carp was generated by combining PacBio reads, Illumina reads and Hi-C data. The genome size is 827.63 Mb with a scaffold N50 size of 33.65 Mb, and 99.51% (823.61 Mb) of the assembled sequences were anchored to 24 pseudo-chromosomes. The genome is predicted to contain 24,153 protein-coding genes, with 95.54% having functional annotations. Repeat elements account for approximately 55.17% of the genomic landscape. The completeness of yellow-cheek carp genome assembly is highlighted by a BUSCO score of 98.4%. This genome will help us understand the genetic diversity of yellow-cheek carp and facilitate its conservation planning.


Assuntos
Carpas , Cromossomos , Genoma , Animais , Carpas/genética , Tamanho do Genoma
2.
PNAS Nexus ; 3(4): pgae118, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38595803

RESUMO

Enzymatic humification plays a crucial biogeochemical role in eliminating steroidal estrogens and expanding organic carbon stocks. Estrogenic contaminants in agroecosystems can be taken up and acropetally translocated by crops, but the roles of laccase-triggered rhizospheric humification (L-TRH) in pollutant dissipation and plant uptake remain poorly understood. In this study, the laccase-induced decontamination and humification mechanisms of 17ß-estradiol (E2) in water-crop media were investigated by performing greenhouse pot experiments with maize seedlings (Zea mays L.). The results demonstrated that L-TRH effectively dissipated E2 in the rhizosphere solution and achieved the kinetic constants of E2 dissipation at 10 and 50 µM by 8.05 and 2.75 times as much as the treatments without laccase addition, respectively. The copolymerization of E2 and root exudates (i.e. phenols and amino acids) consolidated by L-TRH produced a larger amount of humified precipitates with the richly functional carbon architectures. The growth parameters and photosynthetic pigment levels of maize seedlings were greatly impeded after a 120-h exposure to 50 µM E2, but L-TRH motivated the detoxication process and thus mitigated the phytotoxicity and bioavailability of E2. The tested E2 contents in the maize tissues initially increased sharply with the cultivation time but decreased steadily. Compared with the treatment without laccase addition, the uptake and accumulation of E2 in the maize tissues were obviously diminished by L-TRH. E2 oligomers such as dimer, trimer, and tetramer recognized in the rhizosphere solution were also detected in the root tissues but not in the shoots, demonstrating that the acropetal translocation of E2 oligomers was interrupted. These results highlight a promising strategy for decontaminating estrogenic pollutants, boosting rhizospheric humification, and realizing low-carbon emissions, which would be beneficial for agroenvironmental bioremediation and sustainability.

3.
Molecules ; 28(18)2023 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-37764520

RESUMO

The functional pool of canonical amino acids (cAAs) has been enriched through the emergence of non-canonical amino acids (ncAAs). NcAAs play a crucial role in the production of various pharmaceuticals. The biosynthesis of ncAAs has emerged as an alternative to traditional chemical synthesis due to its environmental friendliness and high efficiency. The breakthrough genetic code expansion (GCE) technique developed in recent years has allowed the incorporation of ncAAs into target proteins, giving them special functions and biological activities. The biosynthesis of ncAAs and their incorporation into target proteins within a single microbe has become an enticing application of such molecules. Based on that, in this study, we first review the biosynthesis methods for ncAAs and analyze the difficulties related to biosynthesis. We then summarize the GCE methods and analyze their advantages and disadvantages. Further, we review the application progress of ncAAs and anticipate the challenges and future development directions of ncAAs.


Assuntos
Aminoácidos , Antifibrinolíticos , Código Genético
4.
J Agric Food Chem ; 71(30): 11386-11395, 2023 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-37470251

RESUMO

Exolaccase-propelled humification (E-PH) helps eliminate phenolic pollutants and produce macromolecular precipitates. Herein, we investigated the influencing mechanism of 12 humic precursors (HPs) on exolaccase-enabled bisphenol A (BPA) decontamination and humification. Catechol, vanillic acid, caffeic acid, and gentian acid not only expedited BPA removal but also created large amounts of copolymeric precipitates. These precipitates had rich functional groups similar to natural humic substances, which presented great aromatic and acidic characteristics. The releasing amounts of BPA monomer from four precipitates were 0.08-12.87% at pH 2.0-11.0, suggesting that BPA-HP copolymers had pH stability. More excitingly, certain copolymeric precipitates could stimulate the growth and development of radish seedlings. The radish growth-promotion mechanisms of copolymers were involved in two aspects: (1) Copolymers interacted with root exudates to accelerate nutrient uptake; (2) Copolymers released auxins to provoke radish growth. These results may provide an innovative strategy for decontaminating phenolic pollutants and yielding humic-like biostimulants in E-PH.


Assuntos
Poluentes Ambientais , Fenóis , Fenóis/química , Substâncias Húmicas/análise , Compostos Benzidrílicos/química , Polímeros
5.
J Cancer Res Clin Oncol ; 149(12): 9705-9720, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37233762

RESUMO

PURPOSE: This study aims to elucidate the mechanism underlying temozolomide resistance in patients with MGMT promoter hypomethylated glioblastoma, which is correlated with poor prognosis. The objective is to identify therapeutic targets and drugs suitable for temozolomide-resistant glioblastoma patients using big data analysis. METHODS: In this retrospective study, transcriptome sequencing data from 457 glioblastoma patients, multi-omics data, and single-cell sequencing data were employed to assess the expression pattern, prognostic value, and biological functions of AHR in glioblastoma. The HERB database was utilized to screen for AHR-targeted drugs for glioblastoma treatment. Validation of our findings was conducted using multiplex immunofluorescence staining of clinical samples and T cells and tumor cells co-culture models. RESULTS: Our findings demonstrated that patients with MGMT promoter unmethylation did not benefit from postoperative temozolomide chemotherapy due to resistance arising from DNA repair function and tumor immune response. AHR was found to be expressed in immune cells and exhibited an immunomodulatory role in glioblastoma with MGMT promoter unmethylation. AHR was identified as a potential novel inhibitory immune checkpoint receptor, serving as a therapeutic target for temozolomide-resistant glioblastoma. Furthermore, targeting AHR with Semen aesculi markedly enhanced the cytotoxic effect of T cells on glioma cells. CONCLUSIONS: In addition to DNA repair function, the tumor immune response plays a pivotal role in temozolomide resistance of glioblastoma. Herbal compounds targeting AHR may offer an effective treatment for temozolomide-resistant glioblastoma.


Assuntos
Neoplasias Encefálicas , Glioblastoma , Humanos , Glioblastoma/tratamento farmacológico , Glioblastoma/genética , Glioblastoma/patologia , Temozolomida , Antineoplásicos Alquilantes , Estudos Retrospectivos , Proteínas Supressoras de Tumor/metabolismo , Enzimas Reparadoras do DNA/genética , Enzimas Reparadoras do DNA/metabolismo , Metilases de Modificação do DNA/genética , Metilases de Modificação do DNA/metabolismo , Neoplasias Encefálicas/tratamento farmacológico , Neoplasias Encefálicas/genética , Neoplasias Encefálicas/patologia , Metilação de DNA
6.
Nanoscale ; 15(17): 7991-8005, 2023 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-37067249

RESUMO

Extracellular vesicles (EVs) show potential as a therapeutic tool for peripheral nerve injury (PNI), promoting neurological regeneration. However, there are limited data on the in vivo spatio-temporal trafficking and biodistribution of EVs. In this study, we introduce a new non-invasive near-infrared fluorescence imaging strategy based on glucose-conjugated quantum dot (QDs-Glu) labeling to target and track EVs in a sciatic nerve injury rat model in real-time. Our results demonstrate that the injected EVs migrated from the uninjured site to the injured site of the nerve, with an increase in fluorescence signals detected from 4 to 7 days post-injection, indicating the release of contents from the EVs with therapeutic effects. Immunofluorescence and behavioral tests revealed that the EV therapy promoted nerve regeneration and functional recovery at 28 days post-injection. We also found a relationship between functional recovery and the NIR-II fluorescence intensity change pattern, providing novel evidence for the therapeutic effects of EV therapy using real-time NIR-II imaging at the live animal level. This approach initiates a new path for monitoring EVs in treating PNI under in vivo NIR-II imaging, enhancing our understanding of the efficacy of EV therapy on peripheral nerve regeneration and its mechanisms.


Assuntos
Vesículas Extracelulares , Traumatismos dos Nervos Periféricos , Ratos , Animais , Distribuição Tecidual , Vesículas Extracelulares/metabolismo , Traumatismos dos Nervos Periféricos/diagnóstico por imagem , Traumatismos dos Nervos Periféricos/terapia , Imagem Óptica , Regeneração Nervosa
7.
Artigo em Inglês | MEDLINE | ID: mdl-36767373

RESUMO

Rice-duck and rice-crayfish co-culture patterns can increase soil productivity and sustainability and reduce the use of chemical pesticides and fertilizers, thereby reducing the resulting negative environmental impacts. However, most studies have focused on the rice-duck and rice-crayfish binary patterns and have ignored integrated systems (three or more), which may have unexpected synergistic effects. To test these effects, a paddy field experiment was carried out in the Chaohu Lake Basin, Hefei city, Southeast China. Four groups, including a rice-duck-crayfish ecological co-culture system (RDC), idle field (CK), single-season rice planting system (SSR), and double-season rice planting system (DSR), were established in this study. The results showed that the RDC improved the soil physical properties, fertility, humus content, and enzyme activity. In the RDC system, the soil total nitrogen content ranged from 8.54% to 28.37% higher than other systems in the 0-10 cm soil layer. Similar increases were found for soil total phosphorus (8.22-30.53%), available nitrogen (6.93-22.72%), organic matter (18.24-41.54%), urease activity (16.67-71.51%), and acid phosphatase activity (23.41-66.20%). Relative to the SSR treatment, the RDC treatment reduced the total losses of nitrogen and phosphorus runoff by 24.30% and 10.29%, respectively. The RDC also did not cause any harm to the soil in terms of heavy metal pollution. Furthermore, the RDC improved the yield and quality of rice, farmer incomes, and eco-environmental profits. In general, the RDC can serve as a valuable method for the management of agricultural nonpoint-source pollution in the Chaohu Lake area and the revitalization of the countryside.


Assuntos
Oryza , Solo , Animais , Solo/química , Patos , Astacoidea , Técnicas de Cocultura , Agricultura/métodos , Fósforo/análise , China , Fertilizantes , Nitrogênio/análise
8.
Environ Pollut ; 321: 121155, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36709035

RESUMO

Bisphenol A (BPA) is a ubiquitous endocrine disruptor that poses adverse human health risks. Herein, biotransformation kinetics, products, and mechanisms of BPA undergoing a laccase-producing Trametes hirsuta La-7 metabolism were for the first time reported. Strain La-7 could completely biotransform ≤0.5 mmol·L-1 BPA within 6 d in vivo. Notably, its extracellular crude laccase solution (ECLS) and intracellular homogenized mycelium (HM) only required 6 h to convert 85.71% and 84.24% of 0.5 mmol·L-1 BPA in vitro, respectively. The removal of BPA was noticeably hampered by adding a cytochrome P-450 inhibitor (piperonyl butoxide) in HM, disclosing that cytochrome P-450 monooxygenase participated in BPA oxidation and metabolism. BPA intermediates were elaborately identified by high-resolution mass spectrometry (HRMS) combined with 13C stable isotope ratios (BPA: 13C12-BPA = 0.25: 0.25, molar concentration). Based on the accurate molecular mass, isotope labeling difference, and relative intensity ratio of product peaks, 6 versatile metabolic mechanisms of BPA, including polymerization, hydroxylation, dehydration, bond cleavage, dehydrogenation, and carboxylation in vivo and in vitro, were confirmed. Germination index values revealed that inoculating strain La-7 in a BPA-contaminated medium presented no phytotoxicity to the germinated radish (Raphanus sativus L.) seeds. In vivo, Mg2+, Fe2+, Fe3+, and Mn2+ were conducive to BPA removal, but Cd2+ and Hg2+ significantly obstructed BPA elimination. Additionally, strain La-7 also exhibited high-efficiency metabolic ability toward estrone (E1), 17ß-estradiol (E2), and 17α-ethinylestradiol (EE2), with more than 96.13%, 96.65%, and 100% of E1, E2, and EE2 having been converted, respectively. Our findings provide an environmentally powerful laccase-producing fungus to decontaminate endocrine disruptor-contaminated water matrices by radical polymerization and oxidative decomposition.


Assuntos
Disruptores Endócrinos , Lacase , Humanos , Lacase/metabolismo , Trametes/metabolismo , Disruptores Endócrinos/toxicidade , Disruptores Endócrinos/metabolismo , Compostos Benzidrílicos/toxicidade , Compostos Benzidrílicos/metabolismo , Biotransformação
9.
Eco Environ Health ; 2(4): 219-226, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38435360

RESUMO

Humification plays a significant role in converting phenolic pollutants and forming heterogeneous polymers, but few studies have been performed to investigate exolaccase-started humification (ESH). Herein, the influences of lignin precursors (LPs) on exolaccase-induced bisphenol A (BPA) removal and humification were explored. In particular, the architectural features and botanical effects of the formed humification products were also tested. ESH was extremely beneficial in boosting BPA removal in the presence of LPs. Compared with LP-free (58.49%), 100% of BPA was eliminated after the reaction with ESH for 72 h. Such a process was controlled by an exolaccase-caused random assembly of radicals, which generated a large number of hydrophobic polymers through nonspecific covalent binding of C-C and/or C-O. These humified polymers were extremely stable at pH 2.0-10.0 and -20 °C to 80 °C and displayed unique functions, i.e., scavenged 2,2-diphenyl-1-picrylhydrazyl/2,2'-azino-bis3-ethylbenzothiazoline-6-sulphonic acid radicals and exerted antioxidant capacities. More importantly, the functional polymers could act as auxin analogs to increase the germination index (>100%), plant biomass, and salt tolerance of radish seedlings. Our findings disclosed that ESH could not only be optimized to mitigate the ecological risks of phenolic pollutants and sequester organic carbon in environmental bioremediation, but the resulting abundant auxin analogs also contributed to agricultural productivity.

10.
Artigo em Inglês | MEDLINE | ID: mdl-36554891

RESUMO

Complex bacteria communities that comprised Brevibacillus sp. (M1) and Achromobacter sp. (M2) with effective abilities of degrading decabromodiphenyl ether (BDE-209) were investigated for their degradation characteristics and mechanisms under aerobic conditions. The experimental results indicated that 88.4% of 10 mg L-1 BDE-209 could be degraded after incubation for 120 h under the optimum conditions of pH 7.0, 30 °C and 15% of the inoculation volume, and the addition ratio of two bacterial suspensions was 1:1. Based on the identification of BDE-209 degradation products via liquid chromatography-mass spectrometry (LC-MS) analysis, the biodegradation pathway of BDE-209 was proposed. The debromination, hydroxylation, deprotonation, breakage of ether bonds and ring-opening processes were included in the degradation process. Furthermore, intracellular enzymes had the greatest contribution to BDE-209 biodegradation, and the inhibition of piperyl butoxide (PB) for BDE-209 degradation revealed that the cytochrome P450 (CYP) enzyme was likely the key enzyme during BDE-209 degradation by bacteria M (1+2). Our study provided alternative ideas for the microbial degradation of BDE-209 by aerobic complex bacteria communities in a water system.


Assuntos
Bactérias , Éteres Difenil Halogenados , Biodegradação Ambiental , Bactérias/metabolismo , Hidroxilação
11.
J Med Chem ; 65(16): 10992-11009, 2022 08 25.
Artigo em Inglês | MEDLINE | ID: mdl-35960655

RESUMO

Receptor activator of nuclear factor-κB (RANK) and its ligand, RANKL, play pivotal roles in bone remodeling. The monoclonal antibody denosumab successfully inhibited the maturation of osteoclasts (OCs) by binding to RANKL in the clinic. We continued our efforts to develop small-molecule inhibitors of RANKL. In this work, 41 ß-carboline derivatives were synthesized based on previously synthesized compound Y1599 to improve its drug-like properties. Compound Y1693 was identified as a potent RANKL inhibitor that improved absorption-distribution-metabolism-excretion properties and effectively prevented RANKL-induced osteoclastogenesis and bone resorption. Furthermore, Y1693 also suppressed the expression of OC marker genes. Moreover, Y1693 demonstrated good tolerability and efficacy in an orally administered mouse model of osteoporosis as well as the ability to rescue alveolar bone loss in vivo caused by periodontal disease. Collectively, the above findings may provide a valuable direction for the development of novel antiresorptive therapies that target RANKL.


Assuntos
Reabsorção Óssea , Ligante RANK , Animais , Reabsorção Óssea/tratamento farmacológico , Reabsorção Óssea/prevenção & controle , Diferenciação Celular , Ligantes , Camundongos , NF-kappa B/metabolismo , Osteoclastos , Ligante RANK/metabolismo , Receptor Ativador de Fator Nuclear kappa-B/metabolismo
12.
iScience ; 25(9): 104885, 2022 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-36039291

RESUMO

Globally, phenolic contaminants have posed a considerable threat to agro-ecosystems. Exolaccase-boosted humification may be an admirable strategy for phenolic detoxification by creating multifunctional humic-like products (H-LPs). Nonetheless, the potential applicability of the formed H-LPs in agricultural production is still overlooked. This review describes immobilized exolaccase-enabled humification in eliminating phenolic pollutants and producing artificial H-LPs. The similarities and differences between artificial H-LPs and natural humic substances (HSs) in chemical properties are compared. In particular, the agronomic effects of these reproducible artificial H-LPs are highlighted. On the basis of the above summary, the granulation process is employed to prepare granular humic-like organic fertilizers, which can be applied to field crops by mechanical side-deep fertilization. Finally, the challenges and perspectives of exolaccase-boosted humification for practical applications are also discussed. This review is a first step toward a more profound understanding of phenolic detoxification, soil improvement, and agricultural production by exolaccase-boosted humification.

13.
Chemosphere ; 307(Pt 1): 135685, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35842042

RESUMO

Bisphenol A (BPA) is regarded as an endocrine disruptor associated with negative health effects in animals and humans. Laccase from white-rot fungus can enable BPA oxidation and auto-polymerization to circumvent its biotoxicity, but the work concerning the effect mechanisms of divalent and trivalent metal ions (MIs) on BPA polyreaction have rarely been reported. Herein, Trametes versicolor laccase-started BPA conversion within 1 h followed pseudo-first order kinetics, and the rate constant (kprcs) and half-life were respectively 0.61 h-1 and 1.14 h. The presence of Ca2+, Mg2+, Cu2+, Pb2+, Cd2+, Zn2+ and Al3+ exhibited insignificant impact on BPA removal, whereas Fe2+, Fe3+ and Mn2+ had a strong inhibiting effect. Compared with MI-free, the kprcs values of BPA respectively lowered 34.4%, 44.3% and 98.4% in the presence of Fe2+, Fe3+ and Mn2+. Enzymatic activity and differential absorption spectrum disclosed that the inhibitory actions were accomplished by two different mechanisms. One is Fe2+ was preferentially oxidized into Fe3+ that restrained laccase activity at the initial stage of reaction, and subsequently, the formed Fe3+ complex bound with laccase T1-Cu site and thus impeded the single-electron transfer system. The other is Mn2+ was instantly oxidized by laccase to generate Mn3+-citrate complex, which completely consumed the dissolved O2 in solution and consequently terminated BPA removal. Considering environmental bioremediation, T. versicolor laccase-enabled auto-polymerization is a simple and convenient candidate to eliminate BPA in enzymatic wastewater treatment, however the effects of Fe2+/Fe3+ and Mn2+ on BPA decontamination should be cautiously assessed.


Assuntos
Disruptores Endócrinos , Lacase , Compostos Benzidrílicos/metabolismo , Compostos Benzidrílicos/toxicidade , Cádmio , Citratos , Humanos , Íons , Lacase/metabolismo , Chumbo , Fenóis , Trametes
14.
Cell Death Dis ; 13(6): 524, 2022 06 04.
Artigo em Inglês | MEDLINE | ID: mdl-35665750

RESUMO

Transient receptor potential melastatin 8 (TRPM8) functions as a Ca2+-permeable channel in the plasma membrane (PM). Dysfunction of TRPM8 is associated with human pancreatic cancer and several other diseases in clinical patients, but the underlying mechanisms are unclear. Here, we found that lymphocyte-specific protein tyrosine kinase (LCK) directly interacts with TRPM8 and potentiates TRPM8 phosphorylation at Y1022. LCK positively regulated channel function characterized by increased TRPM8 current densities by enhancing TRPM8 multimerization. Furthermore, 14-3-3ζ interacted with TRPM8 and positively modulated channel multimerization. LCK significantly enhanced the binding of 14-3-3ζ and TRPM8, whereas mutant TRPM8-Y1022F impaired TRPM8 multimerization and the binding of TRPM8 and 14-3-3ζ. Knockdown of 14-3-3ζ impaired the regulation of TRPM8 multimerization by LCK. In addition, TRPM8 phosphotyrosine at Y1022 feedback regulated LCK activity by inhibiting Tyr505 phosphorylation and modulating LCK ubiquitination. Finally, we revealed the importance of TRPM8 phosphorylation at Y1022 in the proliferation, migration, and tumorigenesis of pancreatic cancer cells. Our findings demonstrate that the LCK-14-3-3ζ-TRPM8 axis for regulates TRPM8 assembly, channel function, and LCK activity and maybe provide potential therapeutic targets for pancreatic cancer.


Assuntos
Neoplasias Pancreáticas , Canais de Cátion TRPM , Proteínas 14-3-3/genética , Proteínas 14-3-3/metabolismo , Humanos , Proteína Tirosina Quinase p56(lck) Linfócito-Específica/genética , Proteínas de Membrana/metabolismo , Neoplasias Pancreáticas/genética , Neoplasias Pancreáticas/patologia , Fosforilação , Canais de Cátion TRPM/genética , Canais de Cátion TRPM/metabolismo , Neoplasias Pancreáticas
15.
J Hazard Mater ; 436: 129269, 2022 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-35739784

RESUMO

How humic acid (HA) modifies bisphenol A (BPA) conversion in exoenzyme-activated polyreaction is poorly understood. Herein, the influencing mechanism of HA on laccase-induced BPA self-polymerization was investigated, and the phytotoxicity of the produced BPA self/co-polymers was assessed for the first time. HA prominently boosted BPA elimination, and the rate constants of BPA conversion augmented from 0.61 to 1.43 h-1 as HA level raised from 0 to 50 mg·L-1. It is because the generated BPA-HA co-polymers promptly lowered the yields of long-chain BPA self-oligomers, consequently maintaining laccase activity through opening enzymatic substrate-binding pockets. Notably, a few BPA monomers were re-released from the loosely bound self-polymers and co-polymers, and the releasing amounts respectively were 13.9 - 22.4% and 0.3 - 0.5% at pH 2 - 11. Formation of self/co-polymers was greatly conducive to avoiding BPA biotoxicity. Compared with BPA self-polymers, the phytotoxicity of BPA co-polymers to germinated radish (Raphanus sativus L.) seeds was lower due to these covalently bound products were more complex and stable. It follows that laccase-mediated co-polymerization played a significant role in BPA conversion, contaminant detoxification, and carbon sequestration. These findings are not only beneficial to clarifying exoenzyme-activated the generation mechanism of BPA co-polymers in water, but to reusing these supramolecular aggregates in crop growth.


Assuntos
Substâncias Húmicas , Lacase , Compostos Benzidrílicos/química , Compostos Benzidrílicos/toxicidade , Substâncias Húmicas/análise , Cinética , Lacase/metabolismo , Fenóis , Polímeros/química
16.
Environ Sci Technol ; 56(12): 7412-7425, 2022 06 21.
Artigo em Inglês | MEDLINE | ID: mdl-35638921

RESUMO

Traditional composting is a well-suited biotechnology for on-farm management of livestock manure (LM) but still leads to the release of toxic micropollutants and imbalance of nutrients. One in situ exoenzyme-assisted composting has shown promise to ameliorate the agronomical quality of end products by improving humification and polymerization. The naturally occurring extracellular laccase from microorganisms belongs to a multicopper phenoloxidase, which is verified for its versatility to tackle micropollutants and conserve organics through the reactive radical-enabled decomposition and polymerization channels. Laccase possesses an indispensable relationship with humus formation during LM composting, but its potential applications for the harmless disposal and resource utilization of LM have until now been overlooked. Herein, we review the extracellular laccase-aided humification mechanism and its optimizing strategy to maintain enzyme activity and in situ production, highlighting the critical roles of laccase in treating micropollutants and preserving organics during LM composting. Particularly, the functional effects of the formed humification products by laccase-amended composting on plant growth are also discussed. Finally, the future perspectives and outstanding questions are summarized. This critical review provides fundamental insights into laccase-boosted humification that ameliorates the quality of end products in LM composting, which is beneficial to guide and advance the practical applications of exoenzyme in humification remediation, the carbon cycle, and agriculture protection.


Assuntos
Compostagem , Animais , Substâncias Húmicas/análise , Lacase , Gado , Esterco , Solo
17.
Chemosphere ; 290: 133356, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34929277

RESUMO

Humic constituents (HCs) are ubiquitous in the aquatic ecosystems, and contain various functional groups that seriously impact the conversion of 17ß-estradiol (17ß-E2) by fungal laccase. The purpose of this study was to explore the influencing mechanism of HCs on Trametes versicolor laccase-enabled 17ß-E2 oxidation and oligomerization. Herein, T. versicolor-secreted laccase could rapidly convert 99.2% of 17ß-E2 (rate constant = 3.7 × 10-2 min-1, half-life = 18.7 min) into multifarious oligomers at 25 °C and pH 5.0, by phenolic radical-caused C-C and/or C-O self-linking routes, whereas HCs with O-phenolic hydroxyl groups (O-p-OH, i.e., catechol, pyrogallol, gallic acid, and caffeic acid) dramatically suppressed 17ß-E2 oligomerization. Compared with HC-free, 17ß-E2 rate constants weakened 6.3-15.8 fold in the presence of HCs containing O-p-OH. It is largely because the O-p-OH was preferentially oxidized by T. versicolor laccase to create the electrophilic O-quinone monomers/oligomers. These unstable reactive O-quinone intermediates strongly reversed 17ß-E2 phenolic radicals to their monomeric molecules via two proton-transfer versus two electron-transfer channels, thus intercepting 17ß-E2 oxidation and oligomerization. These findings highlight new insights into the effect of HCs containing O-p-OH on T. versicolor laccase-started 17ß-E2 conversion, which is beneficial to re-understanding the fate and geochemical behavior of 17ß-E2 in water.


Assuntos
Lacase , Trametes , Ecossistema , Estradiol , Substâncias Húmicas/análise
18.
Sci Total Environ ; 802: 150005, 2022 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-34525729

RESUMO

Humification processes of phenolic pollutants may play a profound role in environment purification and plant growth. However, little literature is performed to explore exoenzyme-driven humification to polymerize 17ß-estradiol (E2) and humic constituents (HCs), and the effects of their polymeric precipitates on plant growth are usually overlooked. Herein, E2 conversion and radish (Raphanus sativus L.) growth were systematically investigated under humification mediated by extracellular laccase (EL) of Trametes versicolor. Results disclosed that EL-assisted humification achieved a wonderful E2 conversion efficiency (>99%) within 2-h, but the presence of HCs such as humic acid (HA), vanillic acid (VA), and ferulic acid (FA) impeded E2 elimination significantly. Compared with HC-free, the kinetics constants declined by 2.84-, 5.72-, and 5.22-fold with HA, VA, and FA present, respectively. Intriguingly, three close-knit self/cross-linked precipitates (i.e., E2-HA, E2-VA, and E2-FA hybrid precipitates) in dark gray, dark brown, and deep yellow were created after a continuous humification by phenolic radical-initiated polymerization mechanisms. The formation of these humified precipitates was extremely effective on circumventing phytotoxicity caused by monomeric E2, VA, or FA. Furthermore, they acted as humic-like organic fertilizers, accelerating seed germination, root elongation, and enhancing NaCl-tolerance of radish through the combination of oxygen-contained functional components and auxin structural analogues with unstable and stubborn carbon skeletons. This is the first study reporting the pollution purification and plant growth promotion in EL-activated humification. Our findings frame valuable perspectives regarding the natural detoxification and carbon sequestration of phenolic pollutants and the application of their polymeric precipitates in global crop production.


Assuntos
Poluentes Ambientais , Lacase , Substâncias Húmicas/análise , Polyporaceae , Trametes
19.
Org Biomol Chem ; 19(24): 5348-5352, 2021 06 28.
Artigo em Inglês | MEDLINE | ID: mdl-34042936

RESUMO

An efficient and mild synthetic approach for 2-alkyl-substituted chroman-4-ones via zinc-mediated cascade decarboxylative ß-alkylation and dechlorination of 3-chlorochromones was developed. This transformation employed commercially available starting materials and was performed under mild conditions without heat, visible light, peroxide or heavy metals. Moreover, various alkyl NHPI esters with functional groups and differently substituted 3-chlorochromones were tolerated, affording the targeted products with moderate to excellent yields. This protocol could be utilized to construct a diverse library of 2-substituted chroman-4-one derivatives, which could be useful in the discovery of lead compounds for drug discovery in the future.


Assuntos
Cromanos/síntese química , Cromonas/química , Alquilação , Cromanos/química , Halogenação , Estrutura Molecular
20.
Crit Rev Biotechnol ; 41(7): 969-993, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-33818232

RESUMO

This is the first comprehensive overview of laccase-triggered anabolism from fundamental theory to biotechnology applications. Laccase is a typical biological oxidordeuctase that induces the one-electronic transfer of diverse substrates for engendering four phenoxy radicals with concomitant reduction of O2 into 2H2O. In vivo, laccase can participate in anabolic processes to create multifarious functional biopolymers such as fungal pigments, plant lignins, and insect cuticles, using mono/polyphenols and their derivatives as enzymatic substrates, and is thus conducive to biological tissue morphogenesis and global carbon storage. Exhilaratingly, fungal laccase has high redox potential (E° = 500-800 mV) and thermodynamic efficiency, making it a remarkable candidate for utilization as a versatile catalyst in the green and circular economy. This review elaborates the anabolic mechanisms of laccase in initiating the polymerization of natural phenolic compounds and their derivatives in vivo via radical-based self/cross-coupling. Information is also presented on laccase immobilization engineering that expands the practical application ranges of laccase in biotechnology by improving the enzymatic catalytic activity, stability, and reuse rate. Particularly, advances in biotechnology applications in vitro through fungal laccase-triggered macromolecular biosynthesis may provide a key research direction beneficial to the rational design of green chemistry.


Assuntos
Biotecnologia , Lacase , Catálise , Fungos/metabolismo , Lacase/metabolismo , Lignina/metabolismo , Oxirredução
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