TY - JOUR
T1 - Assessing the environmental performance of NADH regeneration methods
T2 - A cleaner process using recyclable Pt/Fe3O4 and hydrogen
AU - Saba, Tony
AU - Burnett, Joseph W. H.
AU - Li, Jianwei
AU - Wang, Xiaonan
AU - Anderson, James A.
AU - Kechagiopoulos, Panagiotis N.
AU - Wang, Xiaodong
N1 - This work was supported by The Royal Society (IES\R3\170162 and RG150001) and The Binks Trust (1225).
PY - 2020/1/1
Y1 - 2020/1/1
N2 - Cofactor (reduced) Nicotinamide Adenine Dinucleotide (NAD(P)H) is an energy carrier in enzymatic redox reactions that are employed for the synthesis of valuable chemicals and pharmaceuticals. The high cost of NAD(P)H makes it impractical to use in stoichiometric amounts in industrial processes. This has led to the development of a variety of methods for NAD(P)H regeneration. In this work, process cleanliness of the current NADH recycling systems was evaluated using E-factor (kgwaste/kgNADH) as a green chemistry metric. The E-factor obtained, depending on the process method, reaches values higher than 20000, where non-recyclable agents, including sacrificial hydride/electron donors, catalysts and electron mediators, alongside by-products (from cosubstrates), account for the overall waste. A promising alternative methodology for NADH regeneration using H2 and recyclable Pt/Fe3O4 is presented and characterisation performed by temperature-programmed reduction (TPR), nitrogen adsorption (surface area/porosity), powder X-ray diffraction (XRD) and transmission electron microscopy (TEM) is used to elucidate observed performance. The Pt/Fe3O4 system at room temperature delivers a turnover frequency of 20 h-1 and the catalyst can be recycled for reuse, producing a significantly low level of waste (E-factor = ˜1).
AB - Cofactor (reduced) Nicotinamide Adenine Dinucleotide (NAD(P)H) is an energy carrier in enzymatic redox reactions that are employed for the synthesis of valuable chemicals and pharmaceuticals. The high cost of NAD(P)H makes it impractical to use in stoichiometric amounts in industrial processes. This has led to the development of a variety of methods for NAD(P)H regeneration. In this work, process cleanliness of the current NADH recycling systems was evaluated using E-factor (kgwaste/kgNADH) as a green chemistry metric. The E-factor obtained, depending on the process method, reaches values higher than 20000, where non-recyclable agents, including sacrificial hydride/electron donors, catalysts and electron mediators, alongside by-products (from cosubstrates), account for the overall waste. A promising alternative methodology for NADH regeneration using H2 and recyclable Pt/Fe3O4 is presented and characterisation performed by temperature-programmed reduction (TPR), nitrogen adsorption (surface area/porosity), powder X-ray diffraction (XRD) and transmission electron microscopy (TEM) is used to elucidate observed performance. The Pt/Fe3O4 system at room temperature delivers a turnover frequency of 20 h-1 and the catalyst can be recycled for reuse, producing a significantly low level of waste (E-factor = ˜1).
KW - Cofactor NADH regeneration
KW - E-factor
KW - Heterogeneous catalysis
KW - Hydrogen
KW - Pt/Fe O
KW - SYSTEM
KW - CARBON ELECTRODE
KW - Pt/Fe3O4
KW - RHODIUM
KW - COFACTOR NADH
KW - ARTIFICIAL PHOTOSYNTHESIS
KW - COMPLEXES
KW - DIRECT ELECTROCHEMICAL REGENERATION
KW - REDUCTION
KW - NAD(P)H
KW - CATALYSTS
UR - http://www.scopus.com/inward/record.url?scp=85061355569&partnerID=8YFLogxK
UR - http://www.mendeley.com/research/assessing-environmental-performance-nadh-regeneration-methods-cleaner-process-using-recyclable-ptfe
UR - http://pure.abdn.ac.uk:8080/portal/en/researchoutput/assessing-the-environmental-performance-of-nadh-regeneration-methods(c4bd0ac9-9183-47c7-8705-1b8388e9b384).html
U2 - 10.1016/j.cattod.2019.01.049
DO - 10.1016/j.cattod.2019.01.049
M3 - Article
SN - 0920-5861
VL - 339
SP - 281
EP - 288
JO - Catalysis Today
JF - Catalysis Today
ER -