A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4+3]annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time,and used to produce a range of hitherto unreport...A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4+3]annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time,and used to produce a range of hitherto unreported precedentedβ-monofluorinated benzo[b]azepin-5-ones with good yields and complete regioselectivity.This approach features a broad substrate scope,good functional group tolerance,and high regioselectivity,which may include Rh(Ⅲ)-catalyzed aldehydic C-H activation,tandem site-/regioselective insertion,defluorinated ring-scission,and 1,2-elimination.展开更多
Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF_(3)-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethy...Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF_(3)-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethylbenzaldehyde(2-CF_(3)-BzH),are crucial raw materials for the synthesis of various pesticides and pharmaceuticals[1].展开更多
The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively red...The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively reduce C=C or C=O bonds while preserving other functional groups within the molecule.This approach serves as a critical strategy for the directional synthesis of high-value molecules.However,achieving such selectivity remains challenging due to the thermodynamic equilibrium and kinetic competition between C=O and C=C bonds inα,β-unsaturated systems.Consequently,constructing precisely targeted catalytic systems is essential to overcome these limitations,offering both fundamental scientific significance and industrial application potential.Metal-organic frameworks(MOFs)and their derivatives have emerged as innovative platforms for designing such systems,owing to their programmable topology,tunable pore microenvironments,spatially controllable active sites,and modifiable electronic structures.This review systematically summarizes the research progress of MOF-based catalysts for selec-tive hydrogenation ofα,β-unsaturated aldehydes/ketones in the last decade,with emphasis on the design strategy,conformational relationship,and catalytic mechanism,aiming to provide new ideas for the design of targeted catalyt-ic systems for the selective hydrogenation ofα,β-unsaturated aldehydes/ketones.展开更多
Aldehydes have attracted increasing attention owing to their odor and potential carcinogenicity.Because aldehydes are formed during oxidation processes(e.g.,ozonation and chlorination)and easily penetrate reverse osmo...Aldehydes have attracted increasing attention owing to their odor and potential carcinogenicity.Because aldehydes are formed during oxidation processes(e.g.,ozonation and chlorination)and easily penetrate reverse osmosis(RO)membranes,they are the main organic substances in RO permeates designated for potable reuse.In this study,peroxydisulfate(PDS)was combined with VUV/UV(185/254 nm)irradiation(VUV/UV/PDS)to generate multiple reactive species,including·OH and SO_(4)^(·−),for the elimination of acetaldehyde(CH_(3)CHO)and mineralization of organic matters.With VUV/UV/PDS at 0.05 and 0.5 mmol/L PDS,99%of CH_(3)CHOwas eliminated within 6 and 1.5min,respectively,whichwere approximately 2-fold and 7-foldmore efficient with VUV/UV.Additionally,with VUV/UV/PDS at 0.05 and 0.5 mmol/L PDS,the proportions of total organic carbon mineralized were 90.7%and 93.7%,respectively.In contrast to VUV/UV,VUV/UV/PDS rapidlymineralized CH_(3)CHO without the obvious accumulation of acetate or oxalate.The computational toxicity assessment indicated that the organic substances generated during VUV/UV/PDS posed lower potential risks to various organisms than those generated during VUV/UV.Moreover,the energy efficiency of VUV/UV/PDS was greater than that of VUV/UV.This study demonstrated that VUV/UV/PDS is a promising alternative treatment for the elimination of aldehydes in RO permeates designated for potable reuse.展开更多
The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived alde...The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining,and has become a frontier of mainstream research.This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes(5-hydroxymethylfurfural,furfural,glucose,xylose,vanillin and benzaldehyde,etc.).The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde.It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies,catalyst stability,and reaction scalability remain,but the rapid progress offers hope for future advancements.Finally,we elucidate the challenges in this domain and provide the perspectives on future developments.This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.展开更多
Utilizing small molecules as markers for specific cells or organs within biosystems is a crucial approach for studying and regulating physiological processes. However, current tagging strategies, due to the presence o...Utilizing small molecules as markers for specific cells or organs within biosystems is a crucial approach for studying and regulating physiological processes. However, current tagging strategies, due to the presence of exposed highly reactive groups, suffer from drawbacks such as low tagging efficiency or insufficient spatial specificity, thereby diminishing their expected effectiveness. Consequently, there is a pressing need to develop a strategy capable of in situ labeling of active groups in response to cellular or in vivo stimuli, ensuring both high tagging efficiency and spatial specificity. In this work, we devised a strategy for releasing aldehyde groups activated by hypochlorous acid(HOCl). Compounds synthesized through this strategy can release the fiuorophore methylene blue(MB) and aldehyde-based compounds upon HOCl activation. Given high reactivity of the released aldehyde group, it can effectively interact with macromolecules in biological systems, facilitating tagging and enabling prolonged imaging. To validate this concept, we further incorporated a naphthalimide structure with stable light emission to create SW-110. SW-110 can specifically respond to in vitro and endogenous HOCl, when release MB, it also releases naphthalimide fiuorophore with highly reactive aldehyde group for tagging within cells. This strategy provides a simple but efficient strategy for proximity tagging in situ.展开更多
Prostaglandin E2(PGE2) serves as the ultimate mediator of fever induced by infiammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-est...Prostaglandin E2(PGE2) serves as the ultimate mediator of fever induced by infiammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-established clinical history in effectively managing fever. However, the specific mechanisms underlying their efficacy remain unclear. Following the screening for lead compounds that inhibit PGE2from antipyretic herbs, alkynylated active molecule probes were designed and synthesized to track and identify potential targets. The target investigation revealed that three antipyretic compounds, namely cinnamaldehyde, 2,4-decadienal, and perillaldehyde, containing α,β-unsaturated aldehyde groups irreversibly targeted the microsomal PGES1-TM4 helix(m PGES1-TM4) at Ser139. This specific interaction effectually inhibited PGE2 production in the cerebral vasculature, leading to exert potent antipyretic effects.α,β-Unsaturated aldehydes targeting m PGES1-TM4 offer a new approach for antipyretic effects with significant potential for various applications.展开更多
Flaxseed oil,a key source of plant-based ω-3α-linolenic acid,is susceptible to oxidation and hazardous substance formation during refining and storage.This study evaluated the effects of refining stages(crude,degumm...Flaxseed oil,a key source of plant-based ω-3α-linolenic acid,is susceptible to oxidation and hazardous substance formation during refining and storage.This study evaluated the effects of refining stages(crude,degumming,complete refining)on aldehydes,trans fatty acids,and oxidative stability in flaxseed oil.The results indicate that heat-pressed oil has dark color with high a*and b*values,but exhibits the relatively highest oxidative stability during the oxidation process.However,compared to cold-pressing,heat-pressing promotes the generation of three additional aldehydes,butenal,nonanal,and trans,trans-2,4-decadienal.Degumming optimizes the color of crude oil while maintaining α-linolenic acid.In contrast,complete refining(degumming,deacidification,bleaching,and deodorization)caused the loss of substantial carotenoids and polyphenols,and α-linolenic acid decreased by 3.48%–4.47%,as well as a large amount of production of trans fatty acids.In addition,complete refining not only leads to the formation of newborn acrolein and trans-2-nominal but also results in a significant increase in most aldehydes concentration.This study provides a reference for the processing of flaxseed oil when considering the formation of hazardous substances induced by the oxidation and isomerization of polyunsaturated fatty acids.展开更多
Hydroformylation of olefins is one of the highest-volume industrial reactions to meet the vast demands for aldehydes as well as their derivatives.Homogeneous Co complexes were the original catalysts industrialized sin...Hydroformylation of olefins is one of the highest-volume industrial reactions to meet the vast demands for aldehydes as well as their derivatives.Homogeneous Co complexes were the original catalysts industrialized since 1960s.Heterogeneous catalysis is considered superior owing to the facile separation of catalysts from products,shorter technical process,and reduced manufacturing costs.Unexpectedly,there has not been a single case of plant using heterogenized Co-based catalyst successfully.To address the separation issue and understand the catalytic mechanism of the reactions,this review summarizes the progress in heterogeneous systems and provides a detailed discussion of their catalytic performance.Strategies for stabilizing Co species through support modification and additive incorporation are carefully considered to elucidate why heterogeneous systems have not yet succeeded on an industrial scale.Furthermore,we provide our insights for the development of heterogeneous catalytic hydroformylation,including the challenges,opportunities,and outlooks.The aim is to deepen the fundamental understanding of heterogeneous alkene hydroformylation,guiding the community's research efforts towards realizing its successful application in the future.展开更多
Metal-organic frameworks(MOFs)usually exist in the state of powder or crystal.When they are exposed to hydrophilic solvents,their structure will change and become unstable.Therefore,it is a challenge to construct MOF ...Metal-organic frameworks(MOFs)usually exist in the state of powder or crystal.When they are exposed to hydrophilic solvents,their structure will change and become unstable.Therefore,it is a challenge to construct MOF materials with tunable mechanical properties.Herein,we report in-situ growth lanthanide metal-organic framework(LnMOF)in sodium alginate(SA)and polyvinyl alcohol(PVA)hydrogel matrix.The prepared composite hydrogel not only displays characteristic lanthanide narrow-band emission under ultraviolet light,but also demonstrates excellent mechanical properties.The addition of LnMOF significantly enhances the compressive strength of the hydrogel(from 0.75 to 7.32 MPa).Furthermore,the composite hydrogel shows highly selective recognition of glutaraldehyde and gaseous formaldehyde at room temperature.The detection limits(LOD)of SP-EuMOF for glutaraldehyde and formaldehyde are 0.27 and 0.22 ppm,respectively.Based on these results,the LnMOF composite hydrogel is deemed to have significant potential as a fluorescent sensor for both glutaraldehyde and formaldehyde detection.展开更多
Multiple phytohormones,including gibberellin(GA),abscisic acid(ABA),and indole-3-acetic acid(IAA),regulate seed germination.In this study,a barley aldehyde oxidase 1(HvAO1)gene was identified,which is located near the...Multiple phytohormones,including gibberellin(GA),abscisic acid(ABA),and indole-3-acetic acid(IAA),regulate seed germination.In this study,a barley aldehyde oxidase 1(HvAO1)gene was identified,which is located near the SD2(seed dormancy 2)region at the telomeric end of chromosome 5H.A doubledhaploid population(AC Metcalfe/Baudin)was used to characterize HvAO1 and validated its association with seed germination and malting quality.Aldehyde oxidase is predicted to catalyse the oxidation of various aldehydes,such as indoleacetaldehyde and abscisic aldehyde,into IAA and ABA,which is the final step of IAA/ABA biogenesis.This process influences the final IAA/ABA concentration in the seed,affecting the seed dormancy.Sequence analysis revealed substantial variations in the HvAO1 promoter regions between AC Metcalfe and Baudin.The combining seed germination tests,genetic variation analysis,gene expression,and phytohormone measurements showed that Baudin,which displays strong seed dormancy,has a specific sequence variation in the promoter region of the HvAO1 gene.This variation is associated with a higher expression level of the HvAO1 gene and an increased level of ABA than those in AC Metcalfe,which shows weak dormancy and lacks this sequence variation.In addition to its strong effect on the SD2 gene,HvAO1 shows excellent potential to fine-tune malting quality and seed dormancy,as evidenced by genotyping with HvAO1-specific markers,dormancy phenotypes,and malting quality.Our findings provide a new strategy for introducing favourable HvAO1 alleles to achieve the desired level of seed dormancy and high malting quality in barley.展开更多
Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation a...Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.展开更多
Background:Despite the insights into the role of aldehyde dehydrogenase 1 family member A1(ALDH1A1)in various liver diseases,the expression and its prognostic significance in patients with hepatitis E virus-related ac...Background:Despite the insights into the role of aldehyde dehydrogenase 1 family member A1(ALDH1A1)in various liver diseases,the expression and its prognostic significance in patients with hepatitis E virus-related acute liver failure(HEV-ALF)remain unclear.This study delved into the assessment of serum exosome-derived ALDH1A1 expression and its prognostic implications for HEV-ALF patients.Methods:Between January 2018 and December 2023,a total of 226 individuals with acute hepatitis E(AHE)and 210 patients with HEV-ALF were recruited from member units of Chinese Consortium for the Study of Hepatitis E.According to the number of organ failure,we categorized 210 HEV-ALF patients into three groups:two organs failure(n=131),three organs failure(n=46),and more than three organs failure(n=33).In addition,200 health controls from Suzhou Municipal Hospital were included.Results:The levels of serum exosome-derived ALDH1A1 in HEV-ALF patients were significantly higher than those in AHE patients and health controls(both P<0.05).Furthermore,the levels of serum exosome-derived ALDH1A1 were the highest in more than three organs failure group,followed by three organs failure group and two organs failure group(all P<0.001).Moreover,serum exosome-derived ALDH1A1 was positively correlated with total bilirubin in HEV-ALF patients(r=0.315,P<0.001).The comparisons of serum exosome-derived ALDH1A1 levels in treatment response showed that serum exosome-derived ALDH1A1 levels were decreased in the improvement group,while increased in the fluctuation and deterioration groups(all P<0.001).Moreover,serum exosome-derived ALDH1A1 was an independent risk factor for predicting the 30-day mortality(P<0.001).Furthermore,the area under the receiver operating characteristic curve was 0.943,with the sensitivity of 94.87%and specificity of 87.72%,indicating the robust decision-making ability.However,no significant differences were found in serum exosome-derived ALDH1A1 levels between patients aged<60 and≥60 years old(P=0.131).Conclusions:Serum exosome-derived ALDH1A1 can greatly predict the prognosis of HEV-ALF patients.展开更多
In this editorial,we highlight the study by Wang et al published in a recent issue of the World Journal of Diabetes.Type 2 diabetes is increasingly recognized as a β-cell dysfunction disorder,with apoptosis and dedif...In this editorial,we highlight the study by Wang et al published in a recent issue of the World Journal of Diabetes.Type 2 diabetes is increasingly recognized as a β-cell dysfunction disorder,with apoptosis and dedifferentiation being key factors in insulin secretion loss.β-cell dedifferentiation is a regression from a mature insulin-secretory phenotype to a progenitor-like state,characterized by the loss of key transcription factors such as pancreatic and duodenal homeobox 1 and MAF bZIP transcription factor A,and the ectopic expression of developmental markers such as neurogenin 3 and aldehyde dehydrogenase 1 family member A3.This editorial discusses the key role of metabolic stress-saturated fatty acids and high glucose-in triggering dedifferentiation through endoplasmic reticulum(ER)stress and repression of the forkhead box protein O1(FoxO1)transcription factor.The study by Wang et al demonstrated how ER dysfunction and FoxO1 suppression collaborate to destabilizeβ-cell identity.Notably,evidence suggests that this process can be reversed under certain circumstances,with potential for therapies aiming to redifferentiateβ-cells or prevent identity loss.We also outline the therapeutic potential of modulating ER stress pathways,controlling FoxO1 activity,and developing biomarkers to trackβ-cell plasticity in patients.Overall,β-cell dedifferentiation knowledge and manipulation offer new avenues for the treatment of diabetes by restoring functionalβ-cell mass.展开更多
The technique for preparing phenol formaldehyde resin from phenolated wood (PWF) and its characters were studied and analyzed. Poplar (Populus spp.) wood meal was liquefied by phenol in the presence of sulfuric acid a...The technique for preparing phenol formaldehyde resin from phenolated wood (PWF) and its characters were studied and analyzed. Poplar (Populus spp.) wood meal was liquefied by phenol in the presence of sulfuric acid as a catalyst. After the liquefied products were cooled, alkaline catalyst and formaldehyde were added. The mixture was kept at (60?) C for 1h and then was heated to (85?) C for 1h. The influence of molar ratio of formaldehyde to phenol (F/P) was investigated. The results showed when the molar ratio of formaldehyde to phenol was over 1.8, the PWF adhesives had high bond quality, bond durability and extremely low aldehydes emissions.展开更多
A method for preparing D-valine from L-valine by racemization and chemical resolution is presented. The resolving reagent, D-2,3-dibenzoyl tartaric acid was obtained by hydrolyzation of D-2,3-dibenzoyl tartaric anhydr...A method for preparing D-valine from L-valine by racemization and chemical resolution is presented. The resolving reagent, D-2,3-dibenzoyl tartaric acid was obtained by hydrolyzation of D-2,3-dibenzoyl tartaric anhydride prepared by reaction of benzoyl chloride with D-tartaric acid. DL-valine was prepared by racemization of L-valine in the presence of aldehyde in a medium of acetic acid at 100 to 110°C for 3 h. In the presence of mineral acid, reaction of D-2,3-dibenzoyl tartaric acid with DL-valine formed diastreroisomeric salts at 84 to 95°C. Salt composed of D-2,3-dibenzoyl tartaric acid and D-valine precipitated when the diastreroisomeric salts mixtures were cooled to 15°C. The salt was reacted with base giving D-valine with yield of 70% to 80% and optical purity of over 98%.展开更多
基金financial support from the schoollevel research projects of Yancheng Institute of Technology(No.xjr2020044)the National Natural Science Foundation of China(Nos.22101151 and 21971090)。
文摘A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4+3]annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time,and used to produce a range of hitherto unreported precedentedβ-monofluorinated benzo[b]azepin-5-ones with good yields and complete regioselectivity.This approach features a broad substrate scope,good functional group tolerance,and high regioselectivity,which may include Rh(Ⅲ)-catalyzed aldehydic C-H activation,tandem site-/regioselective insertion,defluorinated ring-scission,and 1,2-elimination.
基金supported by National Natural Science Foundation of China(22361031,22308260).
文摘Volatile aromatic aldehydes,including benzaldehyde(BzH),4-fluorobenzaldehyde(4-F-BzH),4-isobutylbenzaldehyde(4-iBu-BzH),3-trifluoromethylbenzaldehyde(3-CF_(3)-BzH),p-methoxybenzaldehyde(4-MeO-BzH),and o-trifluoromethylbenzaldehyde(2-CF_(3)-BzH),are crucial raw materials for the synthesis of various pesticides and pharmaceuticals[1].
文摘The selective hydrogenation ofα,β-unsaturated aldehydes/ketones enables precise control over product structures and properties by regulating hydrogen transport pathways and bond cleavage sequences to selectively reduce C=C or C=O bonds while preserving other functional groups within the molecule.This approach serves as a critical strategy for the directional synthesis of high-value molecules.However,achieving such selectivity remains challenging due to the thermodynamic equilibrium and kinetic competition between C=O and C=C bonds inα,β-unsaturated systems.Consequently,constructing precisely targeted catalytic systems is essential to overcome these limitations,offering both fundamental scientific significance and industrial application potential.Metal-organic frameworks(MOFs)and their derivatives have emerged as innovative platforms for designing such systems,owing to their programmable topology,tunable pore microenvironments,spatially controllable active sites,and modifiable electronic structures.This review systematically summarizes the research progress of MOF-based catalysts for selec-tive hydrogenation ofα,β-unsaturated aldehydes/ketones in the last decade,with emphasis on the design strategy,conformational relationship,and catalytic mechanism,aiming to provide new ideas for the design of targeted catalyt-ic systems for the selective hydrogenation ofα,β-unsaturated aldehydes/ketones.
基金supported by the National Natural Science Foundation of China(No.52270045)the Science,Technology and Innovation Commol/Lission of Shenzhen(Nos.JCYJ20220818101010022 and JCYJ20220530143003007)+1 种基金Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(No.SZPR2023004)Guangdong Higher Education Institutions Innovative Research Team of UrbanWater Cycle and Ecological Safety(No.2023KCXTD053).
文摘Aldehydes have attracted increasing attention owing to their odor and potential carcinogenicity.Because aldehydes are formed during oxidation processes(e.g.,ozonation and chlorination)and easily penetrate reverse osmosis(RO)membranes,they are the main organic substances in RO permeates designated for potable reuse.In this study,peroxydisulfate(PDS)was combined with VUV/UV(185/254 nm)irradiation(VUV/UV/PDS)to generate multiple reactive species,including·OH and SO_(4)^(·−),for the elimination of acetaldehyde(CH_(3)CHO)and mineralization of organic matters.With VUV/UV/PDS at 0.05 and 0.5 mmol/L PDS,99%of CH_(3)CHOwas eliminated within 6 and 1.5min,respectively,whichwere approximately 2-fold and 7-foldmore efficient with VUV/UV.Additionally,with VUV/UV/PDS at 0.05 and 0.5 mmol/L PDS,the proportions of total organic carbon mineralized were 90.7%and 93.7%,respectively.In contrast to VUV/UV,VUV/UV/PDS rapidlymineralized CH_(3)CHO without the obvious accumulation of acetate or oxalate.The computational toxicity assessment indicated that the organic substances generated during VUV/UV/PDS posed lower potential risks to various organisms than those generated during VUV/UV.Moreover,the energy efficiency of VUV/UV/PDS was greater than that of VUV/UV.This study demonstrated that VUV/UV/PDS is a promising alternative treatment for the elimination of aldehydes in RO permeates designated for potable reuse.
基金supported by the National Key R&D Program of China(2023YFC3905804)the National Natural Science Foundation of China(22078374,22378434,41920104003)the Scientific and Technological Planning Project of Guangzhou(202206010145)。
文摘The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources.Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining,and has become a frontier of mainstream research.This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes(5-hydroxymethylfurfural,furfural,glucose,xylose,vanillin and benzaldehyde,etc.).The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde.It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies,catalyst stability,and reaction scalability remain,but the rapid progress offers hope for future advancements.Finally,we elucidate the challenges in this domain and provide the perspectives on future developments.This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.
基金financially supported by the National Natural Science Foundation of China (Nos. 22177019, 22377010, 22371038)State Key Laboratory for Modification of Chemical Fibers and Polymer Materials (No. KF2206)。
文摘Utilizing small molecules as markers for specific cells or organs within biosystems is a crucial approach for studying and regulating physiological processes. However, current tagging strategies, due to the presence of exposed highly reactive groups, suffer from drawbacks such as low tagging efficiency or insufficient spatial specificity, thereby diminishing their expected effectiveness. Consequently, there is a pressing need to develop a strategy capable of in situ labeling of active groups in response to cellular or in vivo stimuli, ensuring both high tagging efficiency and spatial specificity. In this work, we devised a strategy for releasing aldehyde groups activated by hypochlorous acid(HOCl). Compounds synthesized through this strategy can release the fiuorophore methylene blue(MB) and aldehyde-based compounds upon HOCl activation. Given high reactivity of the released aldehyde group, it can effectively interact with macromolecules in biological systems, facilitating tagging and enabling prolonged imaging. To validate this concept, we further incorporated a naphthalimide structure with stable light emission to create SW-110. SW-110 can specifically respond to in vitro and endogenous HOCl, when release MB, it also releases naphthalimide fiuorophore with highly reactive aldehyde group for tagging within cells. This strategy provides a simple but efficient strategy for proximity tagging in situ.
基金supported by the National Key R&D Program of China (Nos. 2022YFC3500800 and 2022YFC3500805)。
文摘Prostaglandin E2(PGE2) serves as the ultimate mediator of fever induced by infiammatory factors. In contrast to cyclooxygenase inhibitors that suppress arachidonic acid metabolism, antipyretic herbs possess a well-established clinical history in effectively managing fever. However, the specific mechanisms underlying their efficacy remain unclear. Following the screening for lead compounds that inhibit PGE2from antipyretic herbs, alkynylated active molecule probes were designed and synthesized to track and identify potential targets. The target investigation revealed that three antipyretic compounds, namely cinnamaldehyde, 2,4-decadienal, and perillaldehyde, containing α,β-unsaturated aldehyde groups irreversibly targeted the microsomal PGES1-TM4 helix(m PGES1-TM4) at Ser139. This specific interaction effectually inhibited PGE2 production in the cerebral vasculature, leading to exert potent antipyretic effects.α,β-Unsaturated aldehydes targeting m PGES1-TM4 offer a new approach for antipyretic effects with significant potential for various applications.
文摘Flaxseed oil,a key source of plant-based ω-3α-linolenic acid,is susceptible to oxidation and hazardous substance formation during refining and storage.This study evaluated the effects of refining stages(crude,degumming,complete refining)on aldehydes,trans fatty acids,and oxidative stability in flaxseed oil.The results indicate that heat-pressed oil has dark color with high a*and b*values,but exhibits the relatively highest oxidative stability during the oxidation process.However,compared to cold-pressing,heat-pressing promotes the generation of three additional aldehydes,butenal,nonanal,and trans,trans-2,4-decadienal.Degumming optimizes the color of crude oil while maintaining α-linolenic acid.In contrast,complete refining(degumming,deacidification,bleaching,and deodorization)caused the loss of substantial carotenoids and polyphenols,and α-linolenic acid decreased by 3.48%–4.47%,as well as a large amount of production of trans fatty acids.In addition,complete refining not only leads to the formation of newborn acrolein and trans-2-nominal but also results in a significant increase in most aldehydes concentration.This study provides a reference for the processing of flaxseed oil when considering the formation of hazardous substances induced by the oxidation and isomerization of polyunsaturated fatty acids.
文摘Hydroformylation of olefins is one of the highest-volume industrial reactions to meet the vast demands for aldehydes as well as their derivatives.Homogeneous Co complexes were the original catalysts industrialized since 1960s.Heterogeneous catalysis is considered superior owing to the facile separation of catalysts from products,shorter technical process,and reduced manufacturing costs.Unexpectedly,there has not been a single case of plant using heterogenized Co-based catalyst successfully.To address the separation issue and understand the catalytic mechanism of the reactions,this review summarizes the progress in heterogeneous systems and provides a detailed discussion of their catalytic performance.Strategies for stabilizing Co species through support modification and additive incorporation are carefully considered to elucidate why heterogeneous systems have not yet succeeded on an industrial scale.Furthermore,we provide our insights for the development of heterogeneous catalytic hydroformylation,including the challenges,opportunities,and outlooks.The aim is to deepen the fundamental understanding of heterogeneous alkene hydroformylation,guiding the community's research efforts towards realizing its successful application in the future.
基金Project supported by the National Natural Science Foundation of China(21661034)Reserve Talents Project for Youth and Middle-Aged Academic and Technical Leaders of Yunnan Province(202205AC160032)。
文摘Metal-organic frameworks(MOFs)usually exist in the state of powder or crystal.When they are exposed to hydrophilic solvents,their structure will change and become unstable.Therefore,it is a challenge to construct MOF materials with tunable mechanical properties.Herein,we report in-situ growth lanthanide metal-organic framework(LnMOF)in sodium alginate(SA)and polyvinyl alcohol(PVA)hydrogel matrix.The prepared composite hydrogel not only displays characteristic lanthanide narrow-band emission under ultraviolet light,but also demonstrates excellent mechanical properties.The addition of LnMOF significantly enhances the compressive strength of the hydrogel(from 0.75 to 7.32 MPa).Furthermore,the composite hydrogel shows highly selective recognition of glutaraldehyde and gaseous formaldehyde at room temperature.The detection limits(LOD)of SP-EuMOF for glutaraldehyde and formaldehyde are 0.27 and 0.22 ppm,respectively.Based on these results,the LnMOF composite hydrogel is deemed to have significant potential as a fluorescent sensor for both glutaraldehyde and formaldehyde detection.
基金supported by the Engineering Research Center of Ecology and Agricultural Use of Wetland,Ministry of Education(KFT202302)the National Natural Science Foundation of China(32372052).
文摘Multiple phytohormones,including gibberellin(GA),abscisic acid(ABA),and indole-3-acetic acid(IAA),regulate seed germination.In this study,a barley aldehyde oxidase 1(HvAO1)gene was identified,which is located near the SD2(seed dormancy 2)region at the telomeric end of chromosome 5H.A doubledhaploid population(AC Metcalfe/Baudin)was used to characterize HvAO1 and validated its association with seed germination and malting quality.Aldehyde oxidase is predicted to catalyse the oxidation of various aldehydes,such as indoleacetaldehyde and abscisic aldehyde,into IAA and ABA,which is the final step of IAA/ABA biogenesis.This process influences the final IAA/ABA concentration in the seed,affecting the seed dormancy.Sequence analysis revealed substantial variations in the HvAO1 promoter regions between AC Metcalfe and Baudin.The combining seed germination tests,genetic variation analysis,gene expression,and phytohormone measurements showed that Baudin,which displays strong seed dormancy,has a specific sequence variation in the promoter region of the HvAO1 gene.This variation is associated with a higher expression level of the HvAO1 gene and an increased level of ABA than those in AC Metcalfe,which shows weak dormancy and lacks this sequence variation.In addition to its strong effect on the SD2 gene,HvAO1 shows excellent potential to fine-tune malting quality and seed dormancy,as evidenced by genotyping with HvAO1-specific markers,dormancy phenotypes,and malting quality.Our findings provide a new strategy for introducing favourable HvAO1 alleles to achieve the desired level of seed dormancy and high malting quality in barley.
基金supported by the National Key Research and Development Program of China(No.2020YFA0607800)the National Natural Science Foundation of China(Nos.42022039 and 42130606)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011),the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.Y2021013).
文摘Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.
基金supported by grants from the National Nat-ural Science Foundation of China(82272396)Suzhou Med-ical and Health Science and Technology Innovation Project(SKY2022057)。
文摘Background:Despite the insights into the role of aldehyde dehydrogenase 1 family member A1(ALDH1A1)in various liver diseases,the expression and its prognostic significance in patients with hepatitis E virus-related acute liver failure(HEV-ALF)remain unclear.This study delved into the assessment of serum exosome-derived ALDH1A1 expression and its prognostic implications for HEV-ALF patients.Methods:Between January 2018 and December 2023,a total of 226 individuals with acute hepatitis E(AHE)and 210 patients with HEV-ALF were recruited from member units of Chinese Consortium for the Study of Hepatitis E.According to the number of organ failure,we categorized 210 HEV-ALF patients into three groups:two organs failure(n=131),three organs failure(n=46),and more than three organs failure(n=33).In addition,200 health controls from Suzhou Municipal Hospital were included.Results:The levels of serum exosome-derived ALDH1A1 in HEV-ALF patients were significantly higher than those in AHE patients and health controls(both P<0.05).Furthermore,the levels of serum exosome-derived ALDH1A1 were the highest in more than three organs failure group,followed by three organs failure group and two organs failure group(all P<0.001).Moreover,serum exosome-derived ALDH1A1 was positively correlated with total bilirubin in HEV-ALF patients(r=0.315,P<0.001).The comparisons of serum exosome-derived ALDH1A1 levels in treatment response showed that serum exosome-derived ALDH1A1 levels were decreased in the improvement group,while increased in the fluctuation and deterioration groups(all P<0.001).Moreover,serum exosome-derived ALDH1A1 was an independent risk factor for predicting the 30-day mortality(P<0.001).Furthermore,the area under the receiver operating characteristic curve was 0.943,with the sensitivity of 94.87%and specificity of 87.72%,indicating the robust decision-making ability.However,no significant differences were found in serum exosome-derived ALDH1A1 levels between patients aged<60 and≥60 years old(P=0.131).Conclusions:Serum exosome-derived ALDH1A1 can greatly predict the prognosis of HEV-ALF patients.
基金Supported by Kuwait Foundation for the Advancement of Sciences,No.RACB-2021-007.
文摘In this editorial,we highlight the study by Wang et al published in a recent issue of the World Journal of Diabetes.Type 2 diabetes is increasingly recognized as a β-cell dysfunction disorder,with apoptosis and dedifferentiation being key factors in insulin secretion loss.β-cell dedifferentiation is a regression from a mature insulin-secretory phenotype to a progenitor-like state,characterized by the loss of key transcription factors such as pancreatic and duodenal homeobox 1 and MAF bZIP transcription factor A,and the ectopic expression of developmental markers such as neurogenin 3 and aldehyde dehydrogenase 1 family member A3.This editorial discusses the key role of metabolic stress-saturated fatty acids and high glucose-in triggering dedifferentiation through endoplasmic reticulum(ER)stress and repression of the forkhead box protein O1(FoxO1)transcription factor.The study by Wang et al demonstrated how ER dysfunction and FoxO1 suppression collaborate to destabilizeβ-cell identity.Notably,evidence suggests that this process can be reversed under certain circumstances,with potential for therapies aiming to redifferentiateβ-cells or prevent identity loss.We also outline the therapeutic potential of modulating ER stress pathways,controlling FoxO1 activity,and developing biomarkers to trackβ-cell plasticity in patients.Overall,β-cell dedifferentiation knowledge and manipulation offer new avenues for the treatment of diabetes by restoring functionalβ-cell mass.
文摘The technique for preparing phenol formaldehyde resin from phenolated wood (PWF) and its characters were studied and analyzed. Poplar (Populus spp.) wood meal was liquefied by phenol in the presence of sulfuric acid as a catalyst. After the liquefied products were cooled, alkaline catalyst and formaldehyde were added. The mixture was kept at (60?) C for 1h and then was heated to (85?) C for 1h. The influence of molar ratio of formaldehyde to phenol (F/P) was investigated. The results showed when the molar ratio of formaldehyde to phenol was over 1.8, the PWF adhesives had high bond quality, bond durability and extremely low aldehydes emissions.
文摘A method for preparing D-valine from L-valine by racemization and chemical resolution is presented. The resolving reagent, D-2,3-dibenzoyl tartaric acid was obtained by hydrolyzation of D-2,3-dibenzoyl tartaric anhydride prepared by reaction of benzoyl chloride with D-tartaric acid. DL-valine was prepared by racemization of L-valine in the presence of aldehyde in a medium of acetic acid at 100 to 110°C for 3 h. In the presence of mineral acid, reaction of D-2,3-dibenzoyl tartaric acid with DL-valine formed diastreroisomeric salts at 84 to 95°C. Salt composed of D-2,3-dibenzoyl tartaric acid and D-valine precipitated when the diastreroisomeric salts mixtures were cooled to 15°C. The salt was reacted with base giving D-valine with yield of 70% to 80% and optical purity of over 98%.
