Nicotinamide adenine dinucleotide(NADH)regeneration is necessary for the sustainable application of enzymatic industry.The Rh-based complex[Cp^(*)Rh(bpy)(H)]+has been widely used as an important mediator in NADH regen...Nicotinamide adenine dinucleotide(NADH)regeneration is necessary for the sustainable application of enzymatic industry.The Rh-based complex[Cp^(*)Rh(bpy)(H)]+has been widely used as an important mediator in NADH regeneration systems,but it is limited by complexity and high cost.Here,a Z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots(CN-CNQD).The resultant catalyst achieved a high yield of NADH in a mediator-free(M-free)system of 0.283 mmol L^(−1) g^(−1) min^(−1),which is 5.29 times that of pure CN.ADH enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21%selectivity in the M-free system.Mechanism research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system,while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free system.The immobilized Rh shows more competitiveness than[Cp^(*)Rh(bpy)(H)]^(+).This study contributes to the construction of an M-free system for further application in greener,lower-cost enzymatic processes.展开更多
In this work,Z-scheme V_(2)O_(5) loaded fluorinated inverse opal carbon nitride(IO F-CN/V_(2)O_(5)) was synthesized as a product of ternary collaborative modification with heterostructure construction,element doping a...In this work,Z-scheme V_(2)O_(5) loaded fluorinated inverse opal carbon nitride(IO F-CN/V_(2)O_(5)) was synthesized as a product of ternary collaborative modification with heterostructure construction,element doping and inverse opal structure.The catalyst presented the highest photocatalytic activity and rate constant for degradation of typical organic pollutants Rhodamine B(RhB)and was also used for the efficient removal of antibiotics,represented by norfloxacin(NOR),sulfadiazine(SD)and levofloxacin(LVX).Characterizations confirmed its increased specific surface area,narrowed bandgap,and enhanced visible light utilization capacity.Further mechanism study including band structure study and electron paramagnetic resonance(EPR)proved the successful construction of Z-scheme heterojunction,which improved photogenerated charge carrier migration and provide sufficient free radicals for the degradation process.The combination of different modifications contributed to the synergetic improvement of removal efficiency towards different organic pollutants.展开更多
基金supported by the National Natural Science Foundation of China(No.21906056)Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.ESK202104)+1 种基金the Science and Technology Commission of Shanghai Municipality(No.22ZR1418600)Shanghai Municipal Science and Technology(No.20DZ2250400).
文摘Nicotinamide adenine dinucleotide(NADH)regeneration is necessary for the sustainable application of enzymatic industry.The Rh-based complex[Cp^(*)Rh(bpy)(H)]+has been widely used as an important mediator in NADH regeneration systems,but it is limited by complexity and high cost.Here,a Z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots(CN-CNQD).The resultant catalyst achieved a high yield of NADH in a mediator-free(M-free)system of 0.283 mmol L^(−1) g^(−1) min^(−1),which is 5.29 times that of pure CN.ADH enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21%selectivity in the M-free system.Mechanism research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system,while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free system.The immobilized Rh shows more competitiveness than[Cp^(*)Rh(bpy)(H)]^(+).This study contributes to the construction of an M-free system for further application in greener,lower-cost enzymatic processes.
基金the National Natural Science Foundation of China(Nos.21777044 and 22076046,22176061)the Science and Technology Commission of Shanghai Municipality(Nos.19ZR1472400,19230711300 and 20DZ2250400)。
文摘In this work,Z-scheme V_(2)O_(5) loaded fluorinated inverse opal carbon nitride(IO F-CN/V_(2)O_(5)) was synthesized as a product of ternary collaborative modification with heterostructure construction,element doping and inverse opal structure.The catalyst presented the highest photocatalytic activity and rate constant for degradation of typical organic pollutants Rhodamine B(RhB)and was also used for the efficient removal of antibiotics,represented by norfloxacin(NOR),sulfadiazine(SD)and levofloxacin(LVX).Characterizations confirmed its increased specific surface area,narrowed bandgap,and enhanced visible light utilization capacity.Further mechanism study including band structure study and electron paramagnetic resonance(EPR)proved the successful construction of Z-scheme heterojunction,which improved photogenerated charge carrier migration and provide sufficient free radicals for the degradation process.The combination of different modifications contributed to the synergetic improvement of removal efficiency towards different organic pollutants.
