Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will ben...Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.展开更多
Jasminum sambac(jasmine flower),a world-renowned plant appreciated for its exceptional flower fragrance,is of cultural and economic importance.However,the genetic basis of its fragrance is largely unknown.Here,we pres...Jasminum sambac(jasmine flower),a world-renowned plant appreciated for its exceptional flower fragrance,is of cultural and economic importance.However,the genetic basis of its fragrance is largely unknown.Here,we present the first de novo genome assembly of J.sambac with 550.12 Mb(scaffold N50=40.10 Mb)assembled into 13 pseudochromosomes.Terpene synthase(TPS)genes associated with flower fragrance are considerably amplified in the form of gene clusters through tandem duplications in the genome.Gene clusters within the salicylic acid/benzoic acid/theobromine(SABATH)and benzylalcohol O-acetyltransferase/anthocyanin O-hydroxycinnamoyltransferases/anthranilate N-hydroxycinnamoyl/benzoyltransferase/deacetylvindoline 4-O-acetyltransferase(BAHD)superfamilies were identified to be related to the biosynthesis of phenylpropanoid/benzenoid compounds.Several key genes involved in jasmonate biosynthesis were duplicated,causing an increase in copy numbers.In addition,multi-omics analyses identified various aromatic compounds and many genes involved in fragrance biosynthesis pathways.Furthermore,the roles of JsTPS3 in b-ocimene biosynthesis,as well as JsAOC1 and JsAOS in jasmonic acid biosynthesis,were functionally validated.The genome assembled in this study for J.sambac offers a basic genetic resource for studying floral scent and jasmonate biosynthesis,and provides a foundation for functional genomic research and variety improvements in Jasminum.展开更多
Electrochemical conversion of carbon dioxide into fuel and chemicals with added value represents an appealing approach to reduce the greenhouse effect and realize a carbon-neutral cycle,which has great potential in mi...Electrochemical conversion of carbon dioxide into fuel and chemicals with added value represents an appealing approach to reduce the greenhouse effect and realize a carbon-neutral cycle,which has great potential in mitigating global warming and effectively storing renewable energy.The electrochemical CO_(2) reduction reaction(CO_(2)RR)usually involves multiproton coupling and multielectron transfer in aqueous electrolytes to form multicarbon products(C_(2+) products),but it competes with the hydrogen evolution reaction(HER),which results in intrinsically sluggish kinetics and a complex reaction mechanism and places higher requirements on the design of catalysts.In this review,the advantages of electrochemical CO_(2) reduction are briefly introduced,and then,different categories of Cu-based catalysts,including monometallic Cu catalysts,bimetallic catalysts,metal-organic frameworks(MOFs)along with MOF-derived catalysts and other catalysts,are summarized in terms of their synthesis method and conversion of CO_(2) to C2+products in aqueous solution.The catalytic mechanisms of these catalysts are subsequently discussed for rational design of more efficient catalysts.In response to the mechanisms,several material strategies to enhance the catalytic behaviors are proposed,including surface facet engineering,interface engineering,utilization of strong metal-support interactions and surface modification.Based on the above strategies,challenges and prospects are proposed for the future development of CO_(2)RR catalysts for industrial applications.展开更多
基金The National Natural Science Foundation of China(Grant Nos.52072114 and 51922008)the 111 Project(Grant No.D17007),the Henan Center for Outstanding Overseas Scientists(Grant No.GZS2018003)+2 种基金Xinxiang Major Science and Technology Projects(Grant No.21ZD001)Guangdong Innovative and Entrepreneurial Research Team Program(2016ZT06N500)Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)all provided financial support for this work.
文摘Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.
基金We thank Novogene for genome sequencing and assembly.We thank Dr.Feng Cheng for his comments on our manuscript.This work was supported by the Elite Young Scientists Program of Chinese Academy of Agricultural Sciences(CAAS),the Agricultural Science and Technology Innovation Program in China and self-raised funds.
文摘Jasminum sambac(jasmine flower),a world-renowned plant appreciated for its exceptional flower fragrance,is of cultural and economic importance.However,the genetic basis of its fragrance is largely unknown.Here,we present the first de novo genome assembly of J.sambac with 550.12 Mb(scaffold N50=40.10 Mb)assembled into 13 pseudochromosomes.Terpene synthase(TPS)genes associated with flower fragrance are considerably amplified in the form of gene clusters through tandem duplications in the genome.Gene clusters within the salicylic acid/benzoic acid/theobromine(SABATH)and benzylalcohol O-acetyltransferase/anthocyanin O-hydroxycinnamoyltransferases/anthranilate N-hydroxycinnamoyl/benzoyltransferase/deacetylvindoline 4-O-acetyltransferase(BAHD)superfamilies were identified to be related to the biosynthesis of phenylpropanoid/benzenoid compounds.Several key genes involved in jasmonate biosynthesis were duplicated,causing an increase in copy numbers.In addition,multi-omics analyses identified various aromatic compounds and many genes involved in fragrance biosynthesis pathways.Furthermore,the roles of JsTPS3 in b-ocimene biosynthesis,as well as JsAOC1 and JsAOS in jasmonic acid biosynthesis,were functionally validated.The genome assembled in this study for J.sambac offers a basic genetic resource for studying floral scent and jasmonate biosynthesis,and provides a foundation for functional genomic research and variety improvements in Jasminum.
基金supported by the Higher Education Discipline Innovation Project(Grant No.D17007)Henan Center for Outstanding Overseas Scientists(Grant No.GZS2022017)+2 种基金National Science Foundation of China(Grant Nos.21908045,51922008,52072114 and 51872075)China Postdoctoral Science Foundation(Grant No.2018M642754)Talent Postdoctoral Program for Henan Province(Grant No.ZYQR201810170).
文摘Electrochemical conversion of carbon dioxide into fuel and chemicals with added value represents an appealing approach to reduce the greenhouse effect and realize a carbon-neutral cycle,which has great potential in mitigating global warming and effectively storing renewable energy.The electrochemical CO_(2) reduction reaction(CO_(2)RR)usually involves multiproton coupling and multielectron transfer in aqueous electrolytes to form multicarbon products(C_(2+) products),but it competes with the hydrogen evolution reaction(HER),which results in intrinsically sluggish kinetics and a complex reaction mechanism and places higher requirements on the design of catalysts.In this review,the advantages of electrochemical CO_(2) reduction are briefly introduced,and then,different categories of Cu-based catalysts,including monometallic Cu catalysts,bimetallic catalysts,metal-organic frameworks(MOFs)along with MOF-derived catalysts and other catalysts,are summarized in terms of their synthesis method and conversion of CO_(2) to C2+products in aqueous solution.The catalytic mechanisms of these catalysts are subsequently discussed for rational design of more efficient catalysts.In response to the mechanisms,several material strategies to enhance the catalytic behaviors are proposed,including surface facet engineering,interface engineering,utilization of strong metal-support interactions and surface modification.Based on the above strategies,challenges and prospects are proposed for the future development of CO_(2)RR catalysts for industrial applications.