Biomass valorization by photoreforming approach provides a promising and alternative strategy to generate value-added chemicals and fuels.In this work,we demonstrate the selective production of lactic acid from glu-co...Biomass valorization by photoreforming approach provides a promising and alternative strategy to generate value-added chemicals and fuels.In this work,we demonstrate the selective production of lactic acid from glu-cose photoreforming over pristine graphitic carbon nitride(g-C_(3) N_(4))photocatalyst.Control experiments screen the best condition for the highest yield of lactic acid,including modulating pH,catalyst loading,and reaction time.100%glucose conversion is achieved along with almost 100%lactic acid yield under the optimized con-dition.Density functional theory(DFT)calculations reveal that the rate-determining step(RDS)of the overall reaction on g-C_(3) N_(4) is the conversion of pyruvaldehyde,where an electron transfer takes place.This present work provides experimental insights and theoretical understanding for selective lactic acid production from biomass photoreforming.展开更多
Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are ...Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are still the main bottlenecks for photocatalytic biomass conversion.Herein,we report the highly selective photocatalytic conversion of glucose solution on holosymmetrically spherical three-dimensionally ordered macroporous TiO_(2)-CdSe heterojunction photonic crystal structure(s-TCS).The obtained s-TCS photocatalysts show excellent stability and strong light harvesting,uniform mass diffusion and exchange,and efficient photogenerated electrons/holes separation and utilization.The optimized s-TCS-4 photocatalyst displays the highest photocatalytic performance for glucose oxidation and hydrogen production.The glucose conversion,lactic acid selectivity,and yield on s-TCS-4 are about 95.9%,94.3%,and 96.4%,respectively.The photocatalytic production of lactic acid for s-TCS-4(18.5 g/L)is 2.3 times higher than the pure spherical TiO_(2) photonic crystal without CdSe(s-TiO_(2),8.1 g/L),and the hydrogen production rate of s-TCS-4 is 9.4 times that of s-TiO_(2).For the first time,we reveal that the photocatalytic conversion of glucose to lactic acid is a third-order and four-electron-involved reaction.This work could shed some new light on the efficient photocatalysis conversion of biomass to highly value-added products with high selectivity and yield,and simultaneously sustainable hydrogen evolution.展开更多
基金Supported by the Canada First Research Excellence Fund(CFREF),Fonds de recherche du Québec-Nature et technologies(FRQNT)New Researchers Fund(2021-NC-283234)NSERC Discovery Grant(RGPIN-2020-04960)Canada Research Chair(950-23288).
文摘Biomass valorization by photoreforming approach provides a promising and alternative strategy to generate value-added chemicals and fuels.In this work,we demonstrate the selective production of lactic acid from glu-cose photoreforming over pristine graphitic carbon nitride(g-C_(3) N_(4))photocatalyst.Control experiments screen the best condition for the highest yield of lactic acid,including modulating pH,catalyst loading,and reaction time.100%glucose conversion is achieved along with almost 100%lactic acid yield under the optimized con-dition.Density functional theory(DFT)calculations reveal that the rate-determining step(RDS)of the overall reaction on g-C_(3) N_(4) is the conversion of pyruvaldehyde,where an electron transfer takes place.This present work provides experimental insights and theoretical understanding for selective lactic acid production from biomass photoreforming.
基金supported by the National Key R&D Program of China(grant nos.2016YFA0202602 and 2021YFE0115800)National Natural Science Foundation of China(grant nos.21805220,U20A20122,and 52103285)+3 种基金Program of Introducing Talents of Discipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China(grant no.B20002)Natural Science Foundation of Hubei Province(grant nos.2020CFB416,2018CFB242,and 2018CFA054)the Fundamental Research Funds for the Central Universities(WUT:grant no.2021III016GX)Youth Innovation Research Fund project and the Open Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing。
文摘Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and hydrogen.However,the limited conversion efficiency and poor selectivity are still the main bottlenecks for photocatalytic biomass conversion.Herein,we report the highly selective photocatalytic conversion of glucose solution on holosymmetrically spherical three-dimensionally ordered macroporous TiO_(2)-CdSe heterojunction photonic crystal structure(s-TCS).The obtained s-TCS photocatalysts show excellent stability and strong light harvesting,uniform mass diffusion and exchange,and efficient photogenerated electrons/holes separation and utilization.The optimized s-TCS-4 photocatalyst displays the highest photocatalytic performance for glucose oxidation and hydrogen production.The glucose conversion,lactic acid selectivity,and yield on s-TCS-4 are about 95.9%,94.3%,and 96.4%,respectively.The photocatalytic production of lactic acid for s-TCS-4(18.5 g/L)is 2.3 times higher than the pure spherical TiO_(2) photonic crystal without CdSe(s-TiO_(2),8.1 g/L),and the hydrogen production rate of s-TCS-4 is 9.4 times that of s-TiO_(2).For the first time,we reveal that the photocatalytic conversion of glucose to lactic acid is a third-order and four-electron-involved reaction.This work could shed some new light on the efficient photocatalysis conversion of biomass to highly value-added products with high selectivity and yield,and simultaneously sustainable hydrogen evolution.
