000136183 001__ 136183
000136183 005__ 20240719195438.0
000136183 0247_ $$2doi$$a10.1021/acssuschemeng.4c02396
000136183 0248_ $$2sideral$$a139145
000136183 037__ $$aART-2024-139145
000136183 041__ $$aeng
000136183 100__ $$aSantiago-Arcos, Javier
000136183 245__ $$aOptimized Spatial Configuration of Heterogeneous BiocatalystsMaximizes Cell-Free Biosynthesis of ¿-Hydroxy and ¿-Amino Acids
000136183 260__ $$c2024
000136183 5060_ $$aAccess copy available to the general public$$fUnrestricted
000136183 5203_ $$aCell-free biocatalysis is gaining momentum in producing value-added chemicals, particularly in stepwise reaction cascades. However, the stability of enzyme cascades in industrial settings is often compromised when free enzymes are involved. In this study, we have developed a stable multifunctional heterogeneous biocatalyst coimmobilizing five enzymes on microparticles to transform 1,ω-diols into 1,ω-hydroxy acids. We improved the operational efficiency and stability of the heterogeneous biocatalyst by fine-tuning the enzyme loading and spatial organization. Stability issues are overcome through postimmobilization polymer coating. The general applicability of this heterogeneous biocatalyst is demonstrated by its scale-up in both batch and packed bed reactors, allowing a product yield of >80%. The continuous process is fed with H2O2 as the oxygen source, reaching a space-time yield (STY) of 0.76 g·L–1·h–1, maintained for the first 12 h. Finally, this flow system is telescoped with a second plug-flow reactor packed with a different heterogeneous biocatalyst integrating an additional transaminase. As a result, this 6-enzyme 2-reactor system sequentially transforms 1,ω-diols into 1,ω-amino acids while in situ recycling NAD+, depleting H2O2, and generating O2.
000136183 536__ $$9info:eu-repo/grantAgreement/ES/AEI/PRE2019-090835
000136183 540__ $$9info:eu-repo/semantics/openAccess$$aAll rights reserved$$uhttp://www.europeana.eu/rights/rr-f/
000136183 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/acceptedVersion
000136183 700__ $$0(orcid)0000-0001-9478-6750$$aVelasco-Lozano, Susana
000136183 700__ $$aDiamanti, Eleftheria
000136183 700__ $$aBenítez-Mateos, Ana I.
000136183 700__ $$aGrajales-Hernández, Daniel
000136183 700__ $$aParadisi, Francesca
000136183 700__ $$0(orcid)0000-0003-0031-1880$$aLópez-Gallego, Fernando
000136183 773__ $$g12, 25 (2024), 9474-9489$$pACS sustain. chem. & eng.$$tACS Sustainable Chemistry and Engineering$$x2168-0485
000136183 8564_ $$s1552087$$uhttps://zaguan.unizar.es/record/136183/files/texto_completo.pdf$$yPostprint
000136183 8564_ $$s1184717$$uhttps://zaguan.unizar.es/record/136183/files/texto_completo.jpg?subformat=icon$$xicon$$yPostprint
000136183 909CO $$ooai:zaguan.unizar.es:136183$$particulos$$pdriver
000136183 951__ $$a2024-07-19-18:28:50
000136183 980__ $$aARTICLE