A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affordi...A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affording aldehydes in isolated yields of up to 88%with broad functional group tolerance,including cyano,halogen,alkenyl,ketone,and ester groups.Moreover,the method enables gram-scale aldehyde synthesis and shows high efficiency in reducing in situ generated acyl chlorides,thereby enhancing its synthetic practicality.展开更多
Non-naturalα-amino acids(α-AAs)are pivotal in drug and catalysis,yet their synthesis remains challenges.A photocatalytic strategy for the direct construction of N-heteroaryl-containingα-AAs from heteroaryl aldehyde...Non-naturalα-amino acids(α-AAs)are pivotal in drug and catalysis,yet their synthesis remains challenges.A photocatalytic strategy for the direct construction of N-heteroaryl-containingα-AAs from heteroaryl aldehydes via acyl radical intermediates is reported.This method exhibits exceptional functional group tolerance and enables late-stage diversification of peptides and carbonyl-group derivatization.Mechanistic studies confirm a radical-based pathway,while applications in peptide modification highlight its utility in bioorganic chemistry.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
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
Aldehyde dehydrogenase 2(ALDH2),a mitochondrial enzyme,is the main acetaldehyde dehydrogenase involved in the scavenging of alcohol-derived acetaldehyde and endogenous aldehydes.The ALDH2^(rs671)mutation affects 560 m...Aldehyde dehydrogenase 2(ALDH2),a mitochondrial enzyme,is the main acetaldehyde dehydrogenase involved in the scavenging of alcohol-derived acetaldehyde and endogenous aldehydes.The ALDH2^(rs671)mutation affects 560 million East Asians and is closely related to an increased risk of various human diseases.In addition to its well-known function in detoxifying alcohol-derived acetaldehyde and endogenous aldehydes,ALDH2 is implicated in human health through its regulation of autophagic machinery and multiple cell death pathways(e.g.,apoptosis,necroptosis,pyroptosis,ferroptosis,and NETosis).This review summarizes the current knowledge of ALDH2 and the regulatory mechanism through which ALDH2 regulates autophagy and cell death.In addition,we outline the potential role of ALDH2 in the regulation of autophagy and cell death during the occurrence and progression of human diseases,aiming to provide a novel theoretical framework for human disease treatment.展开更多
提出一种创新性方法,通过衍生化处理结合超高效液相色谱-高分辨质谱联用技术,实现食品样本中23种醛酮类化合物(aldehydes and ketones,AKs)的同步定量分析。通过系统考察提取方法、酸溶液类型与组成、衍生化试剂质量浓度等关键因素,对...提出一种创新性方法,通过衍生化处理结合超高效液相色谱-高分辨质谱联用技术,实现食品样本中23种醛酮类化合物(aldehydes and ketones,AKs)的同步定量分析。通过系统考察提取方法、酸溶液类型与组成、衍生化试剂质量浓度等关键因素,对提取与衍生化效率进行优化。最优条件下,选用超声辅助提取法(功率50 W、时间10 min、温度30℃)作为固体样品中AKs的最佳提取方式;以磷酸(1%,V/V)为优选酸溶液;2,4-二硝基苯肼衍生化试剂质量浓度为50μg/mL。该方法展现出宽动态线性范围(R^(2)≥0.995)、高灵敏度(定量限:0.002 0~0.132 4µg/mL)及良好准确度。应用本方法成功测定了茶叶与咖啡样本中的23种AKs。相较于现有方法,本研究实现了更高通量,同时显著缩短了分析时长。展开更多
A rapid and eco-friendly one-pot protocol for the synthesis of nitriles has been developed by treating various araldehydes bearing electron withdrawing as well as electron donating groups with hydroxylamine hydrochlor...A rapid and eco-friendly one-pot protocol for the synthesis of nitriles has been developed by treating various araldehydes bearing electron withdrawing as well as electron donating groups with hydroxylamine hydrochloride in the presence of non-toxic,non-corrosive and reusable zinc oxide（ZnO） as the catalyst under solvent-free microwave irradiation.The present approach offers the advantages of a clean reaction,simple methodology,employing readily available catalyst,short reaction duration（〈1 min）,high selectivity;and high yield（90-98%）.展开更多
文摘A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affording aldehydes in isolated yields of up to 88%with broad functional group tolerance,including cyano,halogen,alkenyl,ketone,and ester groups.Moreover,the method enables gram-scale aldehyde synthesis and shows high efficiency in reducing in situ generated acyl chlorides,thereby enhancing its synthetic practicality.
文摘Non-naturalα-amino acids(α-AAs)are pivotal in drug and catalysis,yet their synthesis remains challenges.A photocatalytic strategy for the direct construction of N-heteroaryl-containingα-AAs from heteroaryl aldehydes via acyl radical intermediates is reported.This method exhibits exceptional functional group tolerance and enables late-stage diversification of peptides and carbonyl-group derivatization.Mechanistic studies confirm a radical-based pathway,while applications in peptide modification highlight its utility in bioorganic chemistry.
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 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supported by the State Key Program of the National Natural Science Foundation of China(82030059)the National Science and Technology Major Project(2023ZD0505501)+2 种基金the National Natural Science Foundation of China(81701952 and 82172127)the National Key Research and Development Program of China(2020YFC1512700)the Key Research and Development Program of Shandong Province(2021SFGC0503 and 2022ZLGX03).
文摘Aldehyde dehydrogenase 2(ALDH2),a mitochondrial enzyme,is the main acetaldehyde dehydrogenase involved in the scavenging of alcohol-derived acetaldehyde and endogenous aldehydes.The ALDH2^(rs671)mutation affects 560 million East Asians and is closely related to an increased risk of various human diseases.In addition to its well-known function in detoxifying alcohol-derived acetaldehyde and endogenous aldehydes,ALDH2 is implicated in human health through its regulation of autophagic machinery and multiple cell death pathways(e.g.,apoptosis,necroptosis,pyroptosis,ferroptosis,and NETosis).This review summarizes the current knowledge of ALDH2 and the regulatory mechanism through which ALDH2 regulates autophagy and cell death.In addition,we outline the potential role of ALDH2 in the regulation of autophagy and cell death during the occurrence and progression of human diseases,aiming to provide a novel theoretical framework for human disease treatment.
文摘A rapid and eco-friendly one-pot protocol for the synthesis of nitriles has been developed by treating various araldehydes bearing electron withdrawing as well as electron donating groups with hydroxylamine hydrochloride in the presence of non-toxic,non-corrosive and reusable zinc oxide（ZnO） as the catalyst under solvent-free microwave irradiation.The present approach offers the advantages of a clean reaction,simple methodology,employing readily available catalyst,short reaction duration（〈1 min）,high selectivity;and high yield（90-98%）.
