Mechanistic Insights into the Light-Driven Catalysis of an Immobilized Lipase on Plasmonic Nanomaterials

Autor(es)

Ribeiro de Barros, Heloise ^{[1, 2]} ; Garcia, Isabel ^{[2, 3]} ; Kuttner, Christian ^[2] ; Zeballos, Nicoll ^[2] ; Camargo, Pedro H. C. ^{[1, 4]} ; Cordoba de Torresi, Susana Ines ^[1] ; Lopez-Gallego, Fernando ^{[5, 2]} ; Liz-Marzan, Luis M. ^{[5, 2, 3]}

Afiliação do(s) autor(es)

^[1] Univ Sao Paulo, Dept Fundamental Chem, Inst Chem, BR-05508000 Sao Paulo - Brazil

^[2] Basque Res & Technol Alliance BRTA, CIC BiomaGUNE, Donostia San Sebastian 20014 - Spain

^[3] Ctr Invest Biomed Red Bioingn Biomat & Nanomed CI, Donostia San Sebastian 20014 - Spain

^[4] Univ Helsinki, Dept Chem, Helsinki 00100 - Finland

^[5] Basque Fdn Sci, Ikerbasque, Bilbao 48013 - Spain

• Tipo de documento: Artigo Científico
• Fonte: ACS CATALYSIS; v. 11, n. 1, p. 414-423, JAN 1 2021.
• Citações Web of Science: 0

Resumo

The use of light as an external stimulus to control the enzyme activity is an emerging strategy that enables accurate, remote, and noninvasive biotransformations. In this context, immobilization of enzymes on plasmonic nanoparticles offers an opportunity to create light-responsive biocatalytic materials. Nevertheless, a fundamental and mechanistic understanding of the effects of localized surface plasmon resonance (LSPR) excitation on enzyme regulation remains elusive. We herein investigate the plasmonic effects on biocatalysis using Au nanospheres (AuNSp) and nanostars (AuNSt) as model plasmonic nanoparticles, lipase from Candida antarctica fraction B (CALB) as a proof-of-concept enzyme, and 808 nm as near-infrared light excitation. Our data show that LSPR excitation enables an enhancement of 58% in the enzyme activity for CALB adsorbed on AuNSt, compared with the dark conditions. This work shows how photothermal heating over the LSPR excitation enhances the CALB activity through favoring product release in the last step of the enzyme mechanism. We propose that the results reported herein shed important mechanistic and kinetic insights into the field of plasmonic biocatalysis and may inspire the rational development of plasmonic nanomaterial-enzyme hybrids with tailored activities under external light irradiation. (AU)

• Processo FAPESP: 18/13492-2 - Arcabouços sintéticos e naturais aplicados à medicina regenerativa
• Beneficiário: Luiz Henrique Catalani
• Modalidade de apoio: Auxílio à Pesquisa - Temático
• Processo FAPESP: 19/09668-0 - Estudo das interações biofisicoquímicas entre nanopartículas plasmônicas e enzimas para obtenção de bio-nanomateriais com propriedades controladas
• Beneficiário: Heloise Ribeiro de Barros
• Modalidade de apoio: Bolsas no Exterior - Estágio de Pesquisa - Pós-Doutorado
• Processo FAPESP: 15/26308-7 - Otimização das propriedades físico-químicas de materiais nano-estruturados e suas aplicações em reconhecimento molecular, catálise e conversão/armazenamento de energia
• Beneficiário: Roberto Manuel Torresi
• Modalidade de apoio: Auxílio à Pesquisa - Temático
• Processo FAPESP: 17/20892-4 - Catalisadores nanobioplasmônicos: uma nova abordagem para o controle da seletividade direcionada pela luz em reações one-pot
• Beneficiário: Heloise Ribeiro de Barros
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado