The resource recovery of heavy metals from effluent has significant environmental implications and potential commercial value.Chromium phosphide nanoparticles embedded in a nitrogen-/phosphorus-doped porous carbon mat...The resource recovery of heavy metals from effluent has significant environmental implications and potential commercial value.Chromium phosphide nanoparticles embedded in a nitrogen-/phosphorus-doped porous carbon matrix(CrP/NPC)are synthesized via a consecutive Cr^(6+)leachate treatment and resource recovery process.Electrochemical testing shows that CrP/NPC shows excellent nitrogen reduction reaction(NRR)performance,which yields the highest NH_(3) production rate of 22.56μg h^(−1) mg^(−1)_(cat).and Faradaic efficiency(16.37%)at−0.5 V versus the reversible hydrogen electrode in a 0.05M Na_(2)SO_(4) aqueous solution,as well as robust catalytic stability.The isotopic experiments using ^(15)N^(2) as a nitrogen source confirm that the detected NH_(3) is derived from the NRR process.Finally,density functional theory(DFT)calculations show that the electron deficiency environment of the Cr site can significantly reduce the barrier of the NRR process and promote the formation of intermediate species.展开更多
Mushroom-derived cyathane-type diterpenes possess unusual chemical skeleton and diverse bioactivities.To efficiently supply bioactive cyathanes for deep studies and explore their structural diversity,de novo synthesis...Mushroom-derived cyathane-type diterpenes possess unusual chemical skeleton and diverse bioactivities.To efficiently supply bioactive cyathanes for deep studies and explore their structural diversity,de novo synthesis of cyathane diterpenes in a geranylgeranyl pyrophosphate engineered Saccharomyces cerevisiae is investigated.Aided by homologous analyses,one new unclustered FAD-dependent oxidase EriM accounting for the formation of allyl aldehyde and three new NADP(H)-dependent reductases in the biosynthesis of cyathanes are identified and elucidated.By combinatorial biosynthetic strategy,S.cerevisiae strains generating twenty-two cyathane-type diterpenes,including seven"unnatural"cyathane xylosides(12,13,14a,14b,19,20,and 22)are established.Compounds 12-14,19,and 20 show significant neurotrophic effects on PC 12 cells in the dose of 6.3-25.0μmol/L.These studies provide new insights into the divergent biosynthesis of mushroom-originated cyathanes and a straightforward approach to produce bioactive cyathane-type diterpenes.展开更多
Terpenoid indole(TIAs)andβ-carboline alkaloids(BCAs),such as suppressant reserpine,vasodilatory yohimbine,and antimalarial quinine,are natural compounds derived from strictosidine.These compounds can exert powerful p...Terpenoid indole(TIAs)andβ-carboline alkaloids(BCAs),such as suppressant reserpine,vasodilatory yohimbine,and antimalarial quinine,are natural compounds derived from strictosidine.These compounds can exert powerful pharmacological effects but be obtained from limited source in nature.the whole biosynthetic pathway of TIAs and BCAs,The Pictet–Spengler reaction catalyzed by strictosidine synthase(STR;EC:4.3.3.2)is the rate-limiting step.Therefore,it is necessary to investigate their biosynthesis pathways,especially the role of STR,and related findings will support the biosynthetic generation of natural and unnatural compounds.This review summarizes the latest studies concerning the function of STR in TIA and BCA biosynthesis,and illustrates the compounds derived from strictosidine.The substrate specificity of STR based on its structure is also summarized.Proteins that contain sixbladed four-strandedβ-propeller folds in many organisms,other than plants,are listed.The presence of these folds may lead to similar functions among organisms.The expression of STR gene can greatly influence the production of many compounds.STR is mainly applied to product various valuable drugs in plant cell suspension culture and biosynthesis in other carriers.展开更多
Isonitrile group has been identified in many natural products.Due to the broad reactivity of N≡C triple bond,these natural products have valuable pharmaceutical potentials.This review summarizes the current biosynthe...Isonitrile group has been identified in many natural products.Due to the broad reactivity of N≡C triple bond,these natural products have valuable pharmaceutical potentials.This review summarizes the current biosynthetic pathways and the corresponding enzymes that are responsible for isonitrile-containing natural product generation.Based on the strategies utilized,two fundamentally distinctive approaches are discussed.In addition,recent progress in elucidating isonitrile group formation mechanisms is also presented.展开更多
基金This study was supported by Taishan Scholars Project Special Funds(tsqn201812083)the Natural Science Foundation of Shandong Province(ZR2019YQ20 and 2019JMRH0410)the National Natural Science Foundation of China(51972147,52022037 and 52002145).
文摘The resource recovery of heavy metals from effluent has significant environmental implications and potential commercial value.Chromium phosphide nanoparticles embedded in a nitrogen-/phosphorus-doped porous carbon matrix(CrP/NPC)are synthesized via a consecutive Cr^(6+)leachate treatment and resource recovery process.Electrochemical testing shows that CrP/NPC shows excellent nitrogen reduction reaction(NRR)performance,which yields the highest NH_(3) production rate of 22.56μg h^(−1) mg^(−1)_(cat).and Faradaic efficiency(16.37%)at−0.5 V versus the reversible hydrogen electrode in a 0.05M Na_(2)SO_(4) aqueous solution,as well as robust catalytic stability.The isotopic experiments using ^(15)N^(2) as a nitrogen source confirm that the detected NH_(3) is derived from the NRR process.Finally,density functional theory(DFT)calculations show that the electron deficiency environment of the Cr site can significantly reduce the barrier of the NRR process and promote the formation of intermediate species.
基金supported by the grants from the National Key R&D program of China(Grant 2018YFD0400203 and 2017YEE0108200)the National Natural Science Foundation of China(Grant 21472233)the“Innovative Cross Team”project,CAS(Grant E0222L01R1,China)
文摘Mushroom-derived cyathane-type diterpenes possess unusual chemical skeleton and diverse bioactivities.To efficiently supply bioactive cyathanes for deep studies and explore their structural diversity,de novo synthesis of cyathane diterpenes in a geranylgeranyl pyrophosphate engineered Saccharomyces cerevisiae is investigated.Aided by homologous analyses,one new unclustered FAD-dependent oxidase EriM accounting for the formation of allyl aldehyde and three new NADP(H)-dependent reductases in the biosynthesis of cyathanes are identified and elucidated.By combinatorial biosynthetic strategy,S.cerevisiae strains generating twenty-two cyathane-type diterpenes,including seven"unnatural"cyathane xylosides(12,13,14a,14b,19,20,and 22)are established.Compounds 12-14,19,and 20 show significant neurotrophic effects on PC 12 cells in the dose of 6.3-25.0μmol/L.These studies provide new insights into the divergent biosynthesis of mushroom-originated cyathanes and a straightforward approach to produce bioactive cyathane-type diterpenes.
基金supported by the National Natural Science Foundation of China(Nos.81872933 and 81173119)the National Natural Science Foundation of China and Xinjiang Uygur Autonomous Region of China(No.U1130303)+1 种基金the Technology Cooperation Projects of Science in Shanghai,China(No.20015800100)the Key Project of Ministry of Science and Technology of China(No.2018ZX09731016-004)。
文摘Terpenoid indole(TIAs)andβ-carboline alkaloids(BCAs),such as suppressant reserpine,vasodilatory yohimbine,and antimalarial quinine,are natural compounds derived from strictosidine.These compounds can exert powerful pharmacological effects but be obtained from limited source in nature.the whole biosynthetic pathway of TIAs and BCAs,The Pictet–Spengler reaction catalyzed by strictosidine synthase(STR;EC:4.3.3.2)is the rate-limiting step.Therefore,it is necessary to investigate their biosynthesis pathways,especially the role of STR,and related findings will support the biosynthetic generation of natural and unnatural compounds.This review summarizes the latest studies concerning the function of STR in TIA and BCA biosynthesis,and illustrates the compounds derived from strictosidine.The substrate specificity of STR based on its structure is also summarized.Proteins that contain sixbladed four-strandedβ-propeller folds in many organisms,other than plants,are listed.The presence of these folds may lead to similar functions among organisms.The expression of STR gene can greatly influence the production of many compounds.STR is mainly applied to product various valuable drugs in plant cell suspension culture and biosynthesis in other carriers.
基金This work is supported by the Harry C.Kelly Memorial Fund for U.S.-Japan Scientific Cooperation,through the Office of Global Engagementthe NC Japan Center,at NC State University,Natinnal Institute of Health(GM177588 to W.-c.Cr and Y.G.)MOST(2019YFA09005000 and 2018YFA0901900 to J.Z).
文摘Isonitrile group has been identified in many natural products.Due to the broad reactivity of N≡C triple bond,these natural products have valuable pharmaceutical potentials.This review summarizes the current biosynthetic pathways and the corresponding enzymes that are responsible for isonitrile-containing natural product generation.Based on the strategies utilized,two fundamentally distinctive approaches are discussed.In addition,recent progress in elucidating isonitrile group formation mechanisms is also presented.
