Gibberellins(GAs)are a class of plant hormones that can affect plant growth and development.GA-oxidases are rate-limiting enzymes,which play a direct role in GA accumulation in plants.However,the roles of GA-oxidase o...Gibberellins(GAs)are a class of plant hormones that can affect plant growth and development.GA-oxidases are rate-limiting enzymes,which play a direct role in GA accumulation in plants.However,the roles of GA-oxidase on carrot(Daucus carota L.)taproot development are still unclear.In this study,two GA-oxidase genes,DcGA20ox2 and DcGA2ox1,were identified in carrot.Transgenic carrot plants were obtained by using Agrobacterium-mediated genetic transformation method.The results showed that overexpression of DcGA20ox2 significantly promoted the accumulation of active GAs in carrot,increased plant height,generated more branches,and enhanced xylem development.Overexpression of DcGA2ox1 significantly reduced the total contents of active GAs compared with the control group,resulting in a dwarf phenotype and markedly increased lignin content of the transgenic carrot.The expression profiling showed that the genes of GA metabolic pathway responded to the negative feedback regulation mechanism.At the same time,the expression of most genes in lignin biosynthesis and polymerization process was up-regulated,corresponding to the massive accumulation of lignin.These findings indicated that DcGA20ox2 and DcGA2ox1affected carrot growth and development by regulating the levels of endogenous GAs.The results from current work might shed light on further studies aimed to regulate lignification in carrot and other crops.展开更多
Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owin...Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO_(2) hydrogenation,reverse water-gas shift reaction,and propane-CO_(2) coupling aromatization.Herein,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO_(2) during the propane and CO_(2) coupling reaction.After optimizing the reaction conditions,a notable propane conversion rate of 97.9%and an impressive aromatics selectivity of 80.6%in hydrocarbons can be achieved at the conditions of 550℃and CO_(2)/C_(3)H_(8) of 4.^(13)CO_(2)isotope experiments illustrate that C-atoms of CO_(2) can enter into CO(86.5%)and aromatics(10.8%)during the propane-CO_(2) coupling reaction process.In situ XANES and FTIR spectroscopies at 550℃and H_(2)/C_(3)H_(8) atmosphere reveal that GaO_(x) species can be gradually dispersed into[GaH_(2)]^(+)/[GaH]^(2+)on the Bronsted acid sites of ZSM-5 zeolite during H_(2) and/or C_(3)H_(8) treatment,which are the real active sites for propane-CO_(2) coupling conversion.In situ CO_(2)-FTIR experiments demonstrate that the[GaH_(2)]^(+)/[GaH]^(2+)species can react with CO_(2) and accelerate the propane and CO_(2) coupling process.This work not only presents a cost-effective avenue for CO_(2) utilization,but also contributes to the active site design for improved alkane and CO_(2) activation in coupling reaction system.展开更多
Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified ...Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work.Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+) species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+) species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio.This disparity in Ga_(2)O_(2)^(2+) species stems from their differing capacity in completing the catalytic cycle.Spectroscopic results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+) species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+) species corresponding to GaHHW.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.3210236932372681)+1 种基金Natural Science Foundation of Jiangsu Province(BK20211366)the Priority Academic Program Development of Jiangsu Higher Education Institutions Project(PAPD)。
文摘Gibberellins(GAs)are a class of plant hormones that can affect plant growth and development.GA-oxidases are rate-limiting enzymes,which play a direct role in GA accumulation in plants.However,the roles of GA-oxidase on carrot(Daucus carota L.)taproot development are still unclear.In this study,two GA-oxidase genes,DcGA20ox2 and DcGA2ox1,were identified in carrot.Transgenic carrot plants were obtained by using Agrobacterium-mediated genetic transformation method.The results showed that overexpression of DcGA20ox2 significantly promoted the accumulation of active GAs in carrot,increased plant height,generated more branches,and enhanced xylem development.Overexpression of DcGA2ox1 significantly reduced the total contents of active GAs compared with the control group,resulting in a dwarf phenotype and markedly increased lignin content of the transgenic carrot.The expression profiling showed that the genes of GA metabolic pathway responded to the negative feedback regulation mechanism.At the same time,the expression of most genes in lignin biosynthesis and polymerization process was up-regulated,corresponding to the massive accumulation of lignin.These findings indicated that DcGA20ox2 and DcGA2ox1affected carrot growth and development by regulating the levels of endogenous GAs.The results from current work might shed light on further studies aimed to regulate lignification in carrot and other crops.
基金supported by the National Key Research and Development Program of China (No.2022YFE0116000)the National Natural Science Foundation of China (No.22288101,21991092,21991090,22202193,and 22172166)+1 种基金the Youth Innovation Promotion Association CAS (2021182)the Innovation Research Foundation of Dalian Institute of Chemical Physics,Chinese Academy of Sciences (DICP I202429 and I202217)。
文摘Alkane coupling with CO_(2) by metal-containing zeolites catalysis is found to be a promising way to produce aromatics and syngas in recent years,but the real active sites and the role of CO_(2) are still unclear owing to the quick evolution of the metallic active sites and the complex reaction processes including direct propane aromatization,CO_(2) hydrogenation,reverse water-gas shift reaction,and propane-CO_(2) coupling aromatization.Herein,Ga/ZSM-5 catalysts were constructed to study the dynamic evolution of the metallic active sites and the role of CO_(2) during the propane and CO_(2) coupling reaction.After optimizing the reaction conditions,a notable propane conversion rate of 97.9%and an impressive aromatics selectivity of 80.6%in hydrocarbons can be achieved at the conditions of 550℃and CO_(2)/C_(3)H_(8) of 4.^(13)CO_(2)isotope experiments illustrate that C-atoms of CO_(2) can enter into CO(86.5%)and aromatics(10.8%)during the propane-CO_(2) coupling reaction process.In situ XANES and FTIR spectroscopies at 550℃and H_(2)/C_(3)H_(8) atmosphere reveal that GaO_(x) species can be gradually dispersed into[GaH_(2)]^(+)/[GaH]^(2+)on the Bronsted acid sites of ZSM-5 zeolite during H_(2) and/or C_(3)H_(8) treatment,which are the real active sites for propane-CO_(2) coupling conversion.In situ CO_(2)-FTIR experiments demonstrate that the[GaH_(2)]^(+)/[GaH]^(2+)species can react with CO_(2) and accelerate the propane and CO_(2) coupling process.This work not only presents a cost-effective avenue for CO_(2) utilization,but also contributes to the active site design for improved alkane and CO_(2) activation in coupling reaction system.
文摘Propane dehydrogenation(PDH)on Ga/H-ZSM-5 catalysts is a promising reaction for propylene production,while the detail mechanism remains debatable.Ga_(2)O_(2)^(2+) stabilized by framework Al pairs have been identified as the most active species in Ga/H-ZSM-5 for PDH in our recent work.Here we demonstrate a strong correlation between the PDH activity and a fraction of Ga_(2)O_(2)^(2+) species corresponding to the infrared GaH band of higher wavenumber(GaHHW)in reduced Ga/H-ZSM-5,instead of the overall Ga_(2)O_(2)^(2+) species,by employing five H-ZSM-5 supports sourced differently with comparable Si/Al ratio.This disparity in Ga_(2)O_(2)^(2+) species stems from their differing capacity in completing the catalytic cycle.Spectroscopic results suggest that PDH proceeds via a two-step mechanism:(1)C-H bond activation of propane on H-Ga_(2)O_(2)^(2+) species(rate determining step);(2)β-hydride elimination of adsorbed propyl group,which only occurs on active Ga_(2)O_(2)^(2+) species corresponding to GaHHW.
