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Identification of potential targets for known bioactive compounds and novel synthetic analogs is of considerable significance. In silico target fishing (TF) has become an alternative strategy because of the expensive and laborious wet-lab experiments, explosive growth of bioactivity data and rapid development of high-throughput technologies. However, these TF methods are based on different algorithms, molecular representations and training datasets, which may lead to different results when predicting the same query molecules. This can be confusing for practitioners in practical applications. Therefore, this study systematically evaluated nine popular ligand-based TF methods based on target and ligand-target pair statistical strategies, which will help practitioners make choices among multiple TF methods. The evaluation results showed that SwissTargetPrediction was the best method to produce the most reliable predictions while enriching more targets. High-recall similarity ensemble approach (SEA) was able to find real targets for more compounds compared with other TF methods. Therefore, SwissTargetPrediction and SEA can be considered as primary selection methods in future studies. In addition, the results showed that k = 5 was the optimal number of experimental candidate targets. Finally, a novel ensemble TF method based on consensus voting is proposed to improve the prediction performance. The precision of the ensemble TF method outperforms the individual TF method, indicating that the ensemble TF method can more effectively identify real targets within a given top-k threshold. The results of this study can be used as a reference to guide practitioners in selecting the most effective methods in computational drug discovery.
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Algoritmos , LigandosRESUMEN
Electrocatalytic reduction of biomass-derived furfural (FF) represents a sustainable route to produce furfuryl alcohol (FA) and 2-methylfuran (MF) as a value-added chemical and a biofuel, respectively. However, achieving high selectivity for MF as well as tuning the selectivity between FA and MF within one reaction system remain challenging. Herein, we have reported an electrode-electrolyte interface modification strategy, enabling FA and MF selectivity steering under the same reaction conditions. Specifically, by modifying copper (Cu) electrocatalysts with butyl trimethylammonium bromide (BTAB), we achieved a dramatic shift in selectivity from producing FA (selectivity: 83.8%; Faradaic efficiency, FE: 68.9%) to MF (selectivity: 80.1%; FE: 74.8%). We demonstrated that BTAB adsorption over Cu modulates the electrical double layer (EDL) structure, which repels interfacial water and weakens the hydrogen-bond (H-bond) network for proton transfer, thus impeding FF-to-FA conversion by suppression of the hydrogen atom transfer (HAT) process. On the contrary, FF-to-MF conversion was less affected. This work shows the potential of engineering of the electrode-electrolyte interface for selectivity control in electrocatalysis.
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FAT atypical cadherin 1 (FAT1) is a mutant gene frequently found in human cancers and mainly accumulates at the plasma membrane of cancer cells. Emerging evidence has implicated FAT1 in the progression of gastric cancer (GC). This study intended to identify a regulatory network related to FAT1 in GC development. Upregulated expression of FAT1 was confirmed in GC tissues, and silencing FAT1 was observed to result in suppression of GC cell oncogenic phenotypes. Mechanistic investigation results demonstrated that FAT1 upregulated AP-1 expression by phosphorylating c-JUN and c-FOS, whereas LINC00857 elevated the expression of FAT1 by recruiting a transcription factor TFAP2C. Functional experiments further suggested that LINC00857 enhanced the malignant biological characteristics of GC cells through TFAP2C-mediated promotion of FAT1. More importantly, LINC00857 silencing delayed the tumor growth and blocked epithelial-mesenchymal transition in tumor-bearing mice, which was associated with downregulated expression of TFAP2C/FAT1. To conclude, LINC00857 plays an oncogenic role in GC through regulating the TFAP2C/FAT1/AP-1 axis. Therefore, this study contributes to extended the understanding of gastric carcinogenesis and LINC00857 may serve as a therapeutic target for GC.
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Neoplasias Gástricas , Humanos , Animales , Ratones , Neoplasias Gástricas/genética , Factor de Transcripción AP-1/genética , Línea Celular Tumoral , Carcinogénesis/patología , Regulación Neoplásica de la Expresión Génica , Proliferación Celular/genética , Transición Epitelial-Mesenquimal/genética , Movimiento Celular , Cadherinas/genética , Cadherinas/metabolismo , Factor de Transcripción AP-2/genéticaRESUMEN
The development of a rechargeable battery that can produce valuable chemicals in both electricity storage and generation processes holds great promise for increasing the electron economy and economic value. However, this battery has yet to be explored. Herein, we report a biomass flow battery that generates electricity while producing furoic acid, and store electricity while yielding furfuryl alcohol. The battery is composed of a rhodium-copper (Rh1 Cu) single-atom alloy as anode, a cobalt-doped nickel hydroxide (Co0.2 Ni0.8 (OH)2 ) as cathode, and furfural-containing anolyte. In a full battery evaluation, this battery displays an open circuit voltage (OCV) of 1.29â V and a peak power density up to 107â mW cm-2 , surpassing most catalysis-battery hybrid systems. As a proof-of-concept, we demonstrate that this battery produces 1â kg furoic acid with 0.78â kWh electricity output, and yields 0.62â kg furfuryl alcohol when 1â kWh electricity is stored. This work may shed light on the design of rechargeable batteries with value-added functionality such as chemicals production.
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Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) represents an elegant route toward sustainable value-added chemicals production that circumvents the use of fossil fuel and hydrogen. However, the reaction efficiency is hampered by the high voltage and low activity of electrodes (Cu, Bi, Pb). Herein, we report a Ru1 Cu single-atom alloy (SAA) catalyst with isolated Ru atoms on Cu nanowires that exhibits an electrochemical reduction of HMF to 2,5-dihydroxymethylfuran (DHMF) with promoted productivity (0.47 vs. 0.08â mmol cm-2 h-1 ) and faradic efficiency (FE) (85.6 vs. 71.3 %) at -0.3â V (vs. RHE) compared with Cu counterpart. More importantly, the FE (87.5 %) is largely retained at high HMF concentration (100â mM). Kinetic studies by using combined electrochemical techniques suggest disparate mechanisms over Ru1 Cu and Cu, revealing that single-atom Ru promotes the dissociation of water to produce H* species that effectively react with HMF via an electrocatalytic hydrogenation (ECH) mechanism.
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Aleaciones , Furaldehído , Furaldehído/análogos & derivados , Hidrogenación , CinéticaRESUMEN
The biomass-derived alcohol oxidation reaction (BDAOR) holds great promise for sustainable production of chemicals. However, selective electrooxidation of alcohols to value-added aldehyde compounds is still challenging. Herein, we report the electrocatalytic BDAORs to selectively produce aldehydes using single-atom ruthenium on nickel oxide (Ru1 -NiO) as a catalyst in the neutral medium. For electrooxidation of 5-hydroxymethylfurfural (HMF), Ru1 -NiO exhibits a low potential of 1.283â V at 10â mA cm-2 , and an optimal 2,5-diformylfuran (DFF) selectivity of 90 %. Experimental studies reveal that the neutral electrolyte plays a critical role in achieving a high aldehyde selectivity, and the single-atom Ru boosts HMF oxidation in the neutral medium by promoting water dissociation to afford OH*. Furthermore, Ru1 -NiO can be extended to selective electrooxidation of a series of biomass-derived alcohols to corresponding aldehydes, which are conventionally difficult to obtain in the alkaline medium.
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Oxidative cleavage of C(OH)-C bonds to afford carboxylates is of significant importance for the petrochemical industry and biomass valorization. Here we report an efficient electrochemical strategy for the selective upgrading of lignin derivatives to carboxylates by a manganese-doped cobalt oxyhydroxide (MnCoOOH) catalyst. A wide range of lignin-derived substrates with C(OH)-C or C(O)-C units undergo efficient cleavage to corresponding carboxylates in excellent yields (80-99 %) and operational stability (200â h). Detailed investigations reveal a tandem oxidation mechanism that base from the electrolyte converts secondary alcohols and their derived ketones to reactive nucleophiles, which are oxidized by electrophilic oxygen species on MnCoOOH from water. As proof of concept, this approach was applied to upgrade lignin derivatives with C(OH)-C or C(O)-C motifs, achieving convergent transformation of lignin-derived mixtures to benzoate and KA oil to adipate with 91.5 % and 64.2 % yields, respectively.
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BACKGROUND: Gastric carcinoma (GC) is currently one of the most common malignant tumors of the digestive system, and gastric precancerous lesions play a vital role in studying the mechanism of GC. Multiple microRNAs (miRNAs) have been documented to be potential biomarkers to indicate progression of gastric precancerous lesions. In this study, we explained the anti-cancer effect of miR-365 in gastric precancerous lesions via regulation of the TLR4/IRF3/YAP/CDX2 axis. METHODS: miR-365, TLR4, CDX2 and IPF3 expression was determined in GC and atrophic gastritis tissues and cells. After transfection of shRNA and overexpression plasmids, in vitro experiments detected the alteration of cell viability, apoptosis and inflammatory factors. Bioinformatics analysis, Co-IP and dual luciferase reporter gene assay were conducted to evaluate the binding between miR-365 and TLR4 as well as IRF3 and YAP. Rat models were established to explore the effect of the miR-365 and TLR4 on gastric precancerous lesions. RESULTS: miR-365 was poorly expressed in GC and atrophic gastritis tissues and GC cell lines, while TLR4, CDX2 and IRF3 were overexpressed. Of note, miR-365 was indicated to target TLR4 and thereby suppressed cancer progression and increased hemoglobin content. Interestingly, silencing of TLR4 was accompanied by decreased IRF3 phosphorylation and reduced expression with less binding between CDX2 and IRF3. Downregulation of YAP resulted in declined CDX2 expression in cancer cells. Moreover, the inhibitory role of miR-365 was further confirmed in animal models. CONCLUSION: Taken together, miR-365-mediated TLR4 inhibition reduces IRF3 phosphorylation and YAP-mediated CDX2 transcription to impede progression of gastric precancerous lesions.
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As transitional zone between terrestrial and aquatic ecosystems, the soil properties of riparian zones are deeply influenced by the eco-hydrological conditions of lakes. However, with the increasing frequent drought events caused by climate change, the response of riparian soil organic matter (SOM) dynamics to the eco-hydrological process of lakes under dryness stress is unclear. In this study, we utilized the field research, indoor experiments, ecoenzymatic stoichiometry model and data analysis to identify whether riparian SOM and enzyme activity were affected by dryness stress and determine the feedback relationship between soil biochemical properties and lake eco-hydrological processes. The results showed that lake dryness stress reduced the non-vegetated riparian soil quality (the mean Carbon Pool Management Index decreased by 18 % and 6 % for water-land interface (WL) and bare land (BL), respectively), and the humification degree and molecular weight of the riparian soil dissolved organic matter (DOM) (with E2/E3 and E3/E4 value of WL 6.1 and 1.9 times higher than main lake sediment), which was not conducive to soil carbon storage. In addition, lake dryness stress reduced the C-hydrolytic enzyme activity and soil enzyme stoichiometry. The vector and Vector-TER analysis suggested the riparian soil was C and N limitation of the microbial community (vector length of 2.05 ± 0.57 and vector angle of 30.10° ± 7.70°), and dryness had reduced the limitations to some extent. Most notably, we combined structural equation model (SEM) analysis and found that lake dryness stress affects riparian soil organic carbon (SOC) dynamics by significantly affecting microbial biomass carbon (MBC) and soil pH. Finally, the response of riparian zone to eco-hydrological condition under climate change should receive further attention, which can effectively deepen our understanding of the carbon water cycle mechanism in riparian soil under changing environments.
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Lagos , Suelo , Lagos/química , Suelo/química , Hidrología , Ecosistema , CarbonoRESUMEN
Diffuse pollution, including that in the lower and middle reaches of the Yangtze River, is the primary source of pollution in several agricultural watersheds globally. As the largest river basin in China, the Yangtze River Basin has suffered from total phosphorus (TP) pollution in the past decade owing to diffuse pollution and aquatic ecology destruction, especially in the midstream tributaries and mid-lower reaches of the lakes. However, the transport dynamics of diffuse pollutants, such as phosphorus (P) from land to water bodies have not been well evaluated, which is of great significance for quantifying nutrient loss and its impact on water bodies. In this study, diffuse pollution estimation with remote sensing (DPeRS) model coupled with Soil and Water Assessment Tools (SWAT) was utilized to simulate the transport dynamics of P, investigate the spatial heterogeneity and P sources in the Poyang Lake Basin. Additionally, the P transport mechanism from land to water and the migration process in water bodies were considered to investigate the impact of each loss unit on the water body and evaluate the load generated by diverse pollution types. The estimated diffuse TP loss was 6016 t P·yr-1, and the load to inflow rivers and to Poyang Lake were 11,619 and 9812 t P·yr-1, respectively. Gan River Basin (51.09%) contributed most TP to Poyang Lake among five inflow rivers, while waterfront area demonstrated the highest TP load per unit area with 0.057 t km-2·yr-1. Our study also identified P sources in the sub-basins and emphasized agricultural diffuse sources, especially planting, as the most significant factor contributing to TP pollution. Additionally, to improve the aquatic environment and water ecological conditions, further nutrient management should be applied using a comprehensive approach that encompasses the entire process, from source transportation to the water body.
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Monitoreo del Ambiente , Contaminantes Químicos del Agua , Lagos , Fósforo/análisis , Contaminantes Químicos del Agua/análisis , China , Agua , Nitrógeno/análisisRESUMEN
ETHNOPHARMACOLOGICAL RELEVANCE: Saffron, a traditional Chinese medicine, is derived from Crocus sativus L. stigmas and has been reported to possess neuroprotective properties and potentially contribute to the inhibition of apoptosis and inflammation. Safranal, a potent monothyral aldehyde, is a main component of saffron that has been reported to have antiepileptic activity. However, the specific mechanism by which safranal suppresses epileptic seizures via its antiapoptotic and anti-inflammatory properties is unclear. AIM: To evaluate the effect of safranal on seizure severity, inflammation, and postictal neuronal apoptosis in a mouse model of pentetrazole (PTZ)-induced seizures and explore the underlying mechanism involved. MATERIALS AND METHODS: The seizure stage and latency of stage 2 and 4 were quantified to assess the efficacy of safranal in mitigating PTZ-induced epileptic seizures in mice. Electroencephalography (EEG) was employed to monitor epileptiform afterdischarges in each experimental group. The cognitive abilities and motor functions of the mice were evaluated using the novel object recognition test and the open field test, respectively. Neurons were quantified using hematoxylin and eosin staining. Additionally, bioinformatics tools were utilized to predict the interactions between safranal and specific target proteins. Glycogen synthase kinase-3ß (GSK-3ß), mitochondrial apoptosis-related proteins, and inflammatory factor levels were analyzed through western blotting. Tumor necrosis factor-α (TNF-α) and interleukin-1ß (IL-1ß) concentrations in brain tissue were assessed by ELISA. RESULTS: Safranal decreased the average seizure stage and increased the lantency of stage 2 and 4 seizures in PTZ-induced epileptic mice. Additionally, safranal exhibited neuroprotective effects on hippocampal CA1 and CA3 neurons and reduced hyperactivity caused by postictal hyperexcitability. Bioinformatics analysis revealed that safranal can bind to five specific proteins, including GSK-3ß. By promoting Ser9 phosphorylation and inhibiting GSK-3ß activity, safranal effectively suppressed the NF-κB signaling pathway. Moreover, the findings indicate that safranal treatment can decrease TNF-α and IL-1ß levels in the cerebral tissues of epileptic mice and downregulate mitochondrial apoptosis-related proteins, including Bcl-2, Bax, Bak, Caspase 9, and Caspase 3. CONCLUSION: Safranal can suppress the NF-κB signaling pathway and mitochondrial-dependent apoptosis through GSK-3ß inactivation, suggesting that it is a promising therapeutic agent for epilepsy treatment.
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Apoptosis , Ciclohexenos , Glucógeno Sintasa Quinasa 3 beta , Mitocondrias , FN-kappa B , Pentilenotetrazol , Convulsiones , Transducción de Señal , Terpenos , Animales , Ciclohexenos/farmacología , Ciclohexenos/uso terapéutico , Apoptosis/efectos de los fármacos , Terpenos/farmacología , Terpenos/uso terapéutico , Masculino , Glucógeno Sintasa Quinasa 3 beta/metabolismo , Transducción de Señal/efectos de los fármacos , FN-kappa B/metabolismo , Ratones , Convulsiones/inducido químicamente , Convulsiones/tratamiento farmacológico , Convulsiones/metabolismo , Mitocondrias/efectos de los fármacos , Mitocondrias/metabolismo , Anticonvulsivantes/farmacología , Epilepsia/tratamiento farmacológico , Epilepsia/inducido químicamente , Modelos Animales de EnfermedadRESUMEN
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a sustainable strategy to produce bio-based plastic monomer, is always conducted in a high-concentration alkaline solution (1.0 mol L-1 KOH) for high activity. However, such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation. Herein, we report a single-atom-ruthenium supported on Co3O4 (Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L-1 KOH), exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 mA cm-2 in 0.1 mol L-1 KOH, which outperforms previous catalysts. Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH-) adsorption with insufficient OH- supply, thus improving HMF oxidation. To showcase the potential of Ru1-Co3O4 catalyst, we demonstrate its high efficiency in a flow reactor under industrially relevant conditions. Eventually, techno-economic analysis shows that substitution of the conventional 1.0 mol L-1 KOH with 0.1 mol L-1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%. This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.
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Diffuse terrestrial pollution in bay area has important ecological impacts on coastal ecosystems. This study investigated spatiotemporal changes in N, P, and chlorophyll a (Chla) in the Jiaozhou Bay (JZB) and phytoplankton biomass dynamics under terrestrial nutrients loading. The results from SWAT (Soil and Water Assessment Tool) model demonstrated that the annual average total N (TN) and total P (TP) loading from main rivers were 3626.3 t and 335.6 t, respectively, and were affected by land use type, precipitation, and temperature. Chla value interpreted by remote sensing showed a decrease from nearshore to the far shore. Changes in Chla concentration were usually "dual-cycle" in February and September, but explosive growth of Enteromorpha can cause multiple peaks. TN concentration in the bay was more susceptible to the impact of terrestrial input than TP. Phytoplankton biomass had a stronger correlation with P than with N in JZB. Enteromorpha contributing 4.05% of the phytoplankton biomass played a major role in phytoplankton biomass variability and responded most to nutrients loadings reduction. Under setting 5 m filter strip scenario, the Enteromorpha biomass removal efficiency could reach 35.25%. Furthermore, the findings of this study provide insights for sea-land integration and pollution prevention and control in urbanised bays.
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Ecosistema , Fitoplancton , Clorofila A/análisis , Biomasa , Nutrientes , China , Monitoreo del AmbienteRESUMEN
Enzymes are characteristic of catalytic efficiency and specificity by maneuvering multiple components in concert at a confined nanoscale space. However, achieving such a configuration in artificial catalysts remains challenging. Herein, we report a microenvironment regulation strategy by modifying carbon paper with hexadecyltrimethylammonium cations, delivering electrochemical carbon-carbon coupling of benzaldehyde with enhanced activity and racemate stereoselectivity. The modified electrode-electrolyte interface creates an optimal microenvironment for electrocatalysis-it engenders dipolar interaction with the reaction intermediate, giving a 2.2-fold higher reaction rate (from 0.13 to 0.28 mmol h-1 cm-2); Moreover, it repels interfacial water and modulates the conformational specificity of reaction intermediate by facilitating intermolecular hydrogen bonding, affording 2.5-fold higher diastereomeric ratio of racemate to mesomer (from 0.73 to 1.82). We expect that the microenvironment regulation strategy will lead to the advanced design of electrode-electrolyte interface for enhanced activity and (stereo)selectivity that mimics enzymes.
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Chemical oxygen demand (COD) is an important index used to assess organic oxygen consumption pollution. To explore COD composition in the natural water in Baiyangdian Lake, the main composition, source, and influencing factors of oxygen-consuming organic substances in the water body were revealed through physical continuous classification, three-dimensional fluorescence, and other methods. The results showed that the COD of the two waters was affected by dissolved organic substances (protein-like and humus-like organic matters) with size of less than 220 nm (59%-93%), and inorganic substances had little effect on COD. The source of organic matter in overlying water was primarily affected by endophytic vegetation decomposition, sediment release (the release flux of TOC was in the range of 1.55-2.28 mg·(m2·d)-1), and other endogenous sources (biological index>0.8), as well as by land-based sources such as reed platform and artificial pollution (1.4
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Gastric cancer (GC) as a serious global health problem is a threat to human longevity. Plasmacytoma variant translocation 1 (PVT1) participates in the formation and progression of various cancers, including GC. The aim of this study is to investigate the mechanism underlying the functions of PVT1 and explore a novel target for the diagnosis and treatment of GC. Analysis of the TCGA dataset using the R software identified that the lncRNA PVT1 was greatly upregulated in GC tissues. Twenty pairs of GC and adjacent normal tissues were acquired from patients with GC, and the expression of PVT1 was evaluated using RT-qPCR. Furthermore, PVT1 expression was knocked down in GC cells using siRNA, and the GC cells were divided into control, negative control (NC), and siRNA groups. Cell proliferation ability was analyzed using Cell Counting Kit-8 (CCK8) and colony formation assays, whereas cell migration and invasion ability were investigated through wound healing and Transwell assays. Moreover, Western blotting was used to analyze the expression of Yes-associated protein (YAP) and epithelial-to-mesenchymal transition (EMT) proteins. We also found that PVT1 and YAP expressions were upregulated in the GC tissues compared with those in the adjacent nontumor tissues. Knockdown of PVT1 was found to inhibit the proliferation, invasion, and migration and promote apoptosis of GC cells. Furthermore, knockdown of PVT1 downregulated YAP and promoted phosphorylation of YAP, suggesting that PVT1 exerts actions on GC cells by targeting YAP and inhibits cell apoptosis in vitro. The EMT process was also inhibited by the knockdown of PVT1. In summary, lncRNA PVT1 facilitated cell proliferation, invasion, and migration and suppressed cell apoptosis by targeting YAP. This study suggests that the expressions of PVT1 and YAP could be used for the early detection of GC and the occurrence and development of GC could be inhibited by interfering the interaction of PVT1 and YAP, which will provide new insights for the diagnosis, treatment, and prognosis of GC.
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ARN Largo no Codificante , Neoplasias Gástricas , Apoptosis/genética , Línea Celular Tumoral , Proliferación Celular/genética , Humanos , ARN Largo no Codificante/genética , ARN Interferente Pequeño/metabolismo , Neoplasias Gástricas/genética , Neoplasias Gástricas/metabolismoRESUMEN
Adipic acid is an important building block of polymers, and is commercially produced by thermo-catalytic oxidation of ketone-alcohol oil (a mixture of cyclohexanol and cyclohexanone). However, this process heavily relies on the use of corrosive nitric acid while releases nitrous oxide as a potent greenhouse gas. Herein, we report an electrocatalytic strategy for the oxidation of cyclohexanone to adipic acid coupled with H2 production over a nickel hydroxide (Ni(OH)2) catalyst modified with sodium dodecyl sulfonate (SDS). The intercalated SDS facilitates the enrichment of immiscible cyclohexanone in aqueous medium, thus achieving 3.6-fold greater productivity of adipic acid and higher faradaic efficiency (FE) compared with pure Ni(OH)2 (93% versus 56%). This strategy is demonstrated effective for a variety of immiscible aldehydes and ketones in aqueous solution. Furthermore, we design a realistic two-electrode flow electrolyzer for electrooxidation of cyclohexanone coupling with H2 production, attaining adipic acid productivity of 4.7 mmol coupled with H2 productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm-2) in 24 h.
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Hydrogen production via electrochemical water splitting is one of the most green and promising ways to produce clean energy and address resource crisis, but still suffers from low efficiency and high cost mainly due to the sluggish oxygen evolution reaction (OER) process. Alternatively, electrochemical hydrogen-evolution coupled with alternative oxidation (EHCO) has been proposed as a considerable strategy to improve hydrogen production efficiency combined with the production of high value-added chemicals. Although with these merits, high-efficient electrocatalysts are always needed in practical operation. Typically, layered double hydroxides (LDHs) have been developed as a large class of advanced electrocatalysts toward both OER and EHCO with high efficiency and stability. In this review, we have summarized the latest progress of hydrogen production from the perspectives of designing efficient LDHs-based electrocatalysts for OER and EHCO. Particularly, the influence of structure design and component regulation on the efficiency of their electrocatalytic process have been discussed in detail. Finally, we look forward to the challenges in the field of hydrogen production via electrochemical water splitting coupled with organic oxidation, such as the mechanism, selected oxidation as well as system design, hoping to provide certain inspiration for the development of low-cost hydrogen production technology.
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Single-atom site catalysts (SACs) have been used in multitudinous reactions delivering ultrahigh atom utilization and enhanced performance, but it is challenging for one single atom site to catalyze an intricate tandem reaction needing different reactive sites. Herein, we report a robust SAC with dual reactive sites of isolated Pt single atoms and the Ni3Fe intermetallic support (Pt1/Ni3Fe IMC) for tandem catalyzing the hydrodeoxygenation of 5-hydroxymethylfurfural (5-HMF). It delivers a high catalytic performance with 99.0% 5-HMF conversion in 30 min and a 2, 5-dimethylfuran (DMF) yield of 98.1% in 90 min at a low reaction temperature of 160 °C, as well as good recyclability. These results place Pt1/Ni3Fe IMC among the most active catalysts for the 5-HMF hydrodeoxygenation reaction reported to date. Rational control experiments and first-principles calculations confirm that Pt1/Ni3Fe IMC can readily facilitate the hydrodeoxygenation reaction by a tandem mechanism, where the single Pt site accounts for C[double bond, length as m-dash]O group hydrogenation and the Ni3Fe interface promotes the C-OH bond cleavage. This interfacial tandem catalysis over the Pt single-atom site and Ni3Fe IMC support may develop new opportunities for the rational structural design of SACs applied in other heterogeneous tandem reactions.
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BACKGROUND: Endoscopic submucosal dissection (ESD) has been advocated by digestive endoscopists because of its comparable therapeutic effect to surgery, reduced trauma, faster recovery, and fewer complications. However, ESD for lesions of the duodenum is more challenging than those occurring at other levels of the gastrointestinal tract due to the thin intestinal wall of the duodenum, narrow intestinal space, rich peripheral blood flow, proximity to vital organs, and high risks of critical adverse events including intraoperative and delayed bleeding and perforation. Because of the low prevalence of the disease and the high risks of severe adverse events, successful ESD for lesions of the duodenum has rarely been reported in recent years. AIM: To investigate the efficacy and safety of ESD in the treatment of duodenal space-occupying lesions. METHODS: Clinical data of 24 cases of duodenal lesions treated by ESD at the Digestive Endoscopy Center of the Affiliated Hospital of Qingdao University from January 2016 to December 2019 were retrospectively analyzed. RESULTS: All of the 24 cases from 23 patients underwent ESD treatment for duodenal space-occupying lesions under general anesthesia, including 15 male and 8 female patients, with a mean age of 58.5 (32.0-74.0) years. There were 12 lesions (50%) in the duodenal bulb, 9 (37.5%) in the descending part, and 3 (12.5%) in the ball-descending junction. The mean diameter of the lesion was 12.75 (range, 11-22) mm. Thirteen lesions originated from the mucosa, of which 4 were low-grade intraepithelial neoplasia, 3 were hyperplastic polyps, 2 were chronic mucositis, 2 were adenomatous hyperplasia, 1 was high-grade intraepithelial neoplasia, and 1 was tubular adenoma. Eleven lesions were in the submucosa, including 5 neuroendocrine neoplasms, 2 cases of ectopic pancreas, 1 stromal tumor, 1 leiomyoma, 1 submucosal duodenal adenoma, and 1 case of submucosal lymph follicular hyperplasia. The intraoperative perforation rate was 20.8% (5/24), including 4 submucosal protuberant lesions and 1 depressed lesion. The mean length of hospital stay was 5.7 (range, 3-10) d, and the average follow-up time was 25.8 (range, 3.0-50.0) mo. No residual disease or recurrence was found in all patients, and no complications, such as infection and stenosis, were found during the follow-up period. CONCLUSION: ESD is safe and effective in the treatment of duodenal lesions; however, the endoscopists should pay more attention to the preoperative preparation, intraoperative skills, and postoperative treatment.