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
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.
