Developing on-demand biomass valorization represents an ideal path to alleviate the double burden of a sustainable energy-environment future,yet exploring tunable lignin-first chemistry to accomplish multifunctional w...Developing on-demand biomass valorization represents an ideal path to alleviate the double burden of a sustainable energy-environment future,yet exploring tunable lignin-first chemistry to accomplish multifunctional water purification remains elusive.Herein,we report a versatile solvent-fractionation to construct heteroatom-doped multicolor lignin carbon quantum dots(CQDs)with the functions of bimodal pollutant sensing,metal-ionic visualization,and photocatalytic antibiotic dissociation.With the aid of oxidation cleavage and biphasic extraction,the underlying lignin features of molecular weight and functional linkages influence the quantum size and core-surface state of CQDs conferring the unique optical-structure-performance.The N,S co-doped blue-emitting CQDs via light-quenching offer the selective identification of Fe^(3+)-ions in a broad response range with an acceptable limit of detection.The addition of L-cysteine can efficiently restore the fluorescence of CQDs by forming a stable Fe^(3+)-L-cys complex.The green-emissive CQDs are facilely embedded into cellulose hydrogel to directly visualize the presence of metal-ions.A red-CQDs modified ternary ZnIn2S4(ZIS)composite is fabricated to achieve photocatalytic antibiotic removal with an efficiency of~85%.The excellent photo-generated electron and storage capabilities of CQDs improve the light-capturing,electron conduction,and charge carrier separation of ZIS.The reactive species are of importance to photocatalytic tetracycline oxidation,wherein the electron holes(h+)function as the main contributor followed by∙O_(2)^(-),1O2 and∙OH.The directly interfacial electron escaping-shuttling with the help of optimized electronic and energy-band structures is confirmed via electrochemical test and theoretical computation.We anticipate that the present work not only sheds substantial light to manipulate polychromatic lignin-based CQDs via a tailored solvent-engineering,but also presents an emerging green route of emphasizing biomass-water nexus.展开更多
基金the National Natural Science Foundation of China(32171728 and 22008159)Wuhan Knowledge Innovation Project(2022020801020312).
文摘Developing on-demand biomass valorization represents an ideal path to alleviate the double burden of a sustainable energy-environment future,yet exploring tunable lignin-first chemistry to accomplish multifunctional water purification remains elusive.Herein,we report a versatile solvent-fractionation to construct heteroatom-doped multicolor lignin carbon quantum dots(CQDs)with the functions of bimodal pollutant sensing,metal-ionic visualization,and photocatalytic antibiotic dissociation.With the aid of oxidation cleavage and biphasic extraction,the underlying lignin features of molecular weight and functional linkages influence the quantum size and core-surface state of CQDs conferring the unique optical-structure-performance.The N,S co-doped blue-emitting CQDs via light-quenching offer the selective identification of Fe^(3+)-ions in a broad response range with an acceptable limit of detection.The addition of L-cysteine can efficiently restore the fluorescence of CQDs by forming a stable Fe^(3+)-L-cys complex.The green-emissive CQDs are facilely embedded into cellulose hydrogel to directly visualize the presence of metal-ions.A red-CQDs modified ternary ZnIn2S4(ZIS)composite is fabricated to achieve photocatalytic antibiotic removal with an efficiency of~85%.The excellent photo-generated electron and storage capabilities of CQDs improve the light-capturing,electron conduction,and charge carrier separation of ZIS.The reactive species are of importance to photocatalytic tetracycline oxidation,wherein the electron holes(h+)function as the main contributor followed by∙O_(2)^(-),1O2 and∙OH.The directly interfacial electron escaping-shuttling with the help of optimized electronic and energy-band structures is confirmed via electrochemical test and theoretical computation.We anticipate that the present work not only sheds substantial light to manipulate polychromatic lignin-based CQDs via a tailored solvent-engineering,but also presents an emerging green route of emphasizing biomass-water nexus.
