Final published version
Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Heterogeneous catalysis mediated cofactor NADH regeneration for enzymatic reduction
AU - Wang, Xiaodong
AU - Yiu, Humphrey H. P.
PY - 2016/2/18
Y1 - 2016/2/18
N2 - Enzymatic reduction using oxidoreductases is important in commercial chemical production. This enzymatic action requires a cofactor (e.g., NADH) as a hydrogen source that is consumed during reaction and must be regenerated. We present, for the first time, an in situ NADH regeneration (NAD+ → NADH) using a heterogeneous catalyst (Pt/Al2O3) and H2 coupled with an enzymatic reduction. This regeneration system can be operated at ambient pressure where NADH yield and turnover frequency (TOF) increased with temperature (20–37 °C) and pH (4.0–9.9) delivering full selectivity to enzymatically active NADH. Cofactor regeneration by heterogeneous catalysis represents a cleaner (H+ as sole byproduct) alternative to current enzymatic and homogeneous (electro- and photo-) catalytic methods with the added benefit of facile catalyst separation. The viability of coupling cofactor regeneration with enzymatic (alcohol dehydrogenase, ADH) reaction is established in aldehyde reduction (propanal to propanol) where 100% alcohol yield was achieved. The potential of this hybrid inorganic–enzymatic system is further demonstrated in the continuous (fed-batch) conversion of propanal with catalyst (activity/selectivity) stability for up to 100 h.
AB - Enzymatic reduction using oxidoreductases is important in commercial chemical production. This enzymatic action requires a cofactor (e.g., NADH) as a hydrogen source that is consumed during reaction and must be regenerated. We present, for the first time, an in situ NADH regeneration (NAD+ → NADH) using a heterogeneous catalyst (Pt/Al2O3) and H2 coupled with an enzymatic reduction. This regeneration system can be operated at ambient pressure where NADH yield and turnover frequency (TOF) increased with temperature (20–37 °C) and pH (4.0–9.9) delivering full selectivity to enzymatically active NADH. Cofactor regeneration by heterogeneous catalysis represents a cleaner (H+ as sole byproduct) alternative to current enzymatic and homogeneous (electro- and photo-) catalytic methods with the added benefit of facile catalyst separation. The viability of coupling cofactor regeneration with enzymatic (alcohol dehydrogenase, ADH) reaction is established in aldehyde reduction (propanal to propanol) where 100% alcohol yield was achieved. The potential of this hybrid inorganic–enzymatic system is further demonstrated in the continuous (fed-batch) conversion of propanal with catalyst (activity/selectivity) stability for up to 100 h.
U2 - 10.1021/acscatal.5b02820
DO - 10.1021/acscatal.5b02820
M3 - Journal article
VL - 6
SP - 1880
EP - 1886
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 3
ER -