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Tandem metabolic reaction-based sensors unlock in vivo metabolomics.
- Cheng, Xuanbing;
- Li, Zongqi;
- Zhu, Jialun;
- Wang, Jingyu;
- Huang, Ruyi;
- Yu, Lewis;
- Lin, Shuyu;
- Forman, Sarah;
- Gromilina, Evelina;
- Puri, Sameera;
- Patel, Pritesh;
- Bahramian, Mohammadreza;
- Tan, Jiawei;
- Hojaiji, Hannaneh;
- Jelinek, David;
- Voisin, Laurent;
- Yu, Kristie;
- Zhang, Ao;
- Ho, Connie;
- Lei, Lei;
- Coller, Hilary;
- Hsiao, Elaine;
- Reyes, Beck;
- Matsumoto, Joyce;
- Lu, Daniel;
- Liu, Chong;
- Milla, Carlos;
- Davis, Ronald;
- Emaminejad, Sam
- et al.
Published Web Location
https://doi.org/10.1073/pnas.2425526122Abstract
Mimicking metabolic pathways on electrodes enables in vivo metabolite monitoring for decoding metabolism. Conventional in vivo sensors cannot accommodate underlying complex reactions involving multiple enzymes and cofactors, addressing only a fraction of enzymatic reactions for few metabolites. We devised a single-wall-carbon-nanotube-electrode architecture supporting tandem metabolic pathway-like reactions linkable to oxidoreductase-based electrochemical analysis, making a vast majority of metabolites detectable in vivo. This architecture robustly integrates cofactors, self-mediates reactions at maximum enzyme capacity, and facilitates metabolite intermediation/detection and interference inactivation through multifunctional enzymatic use. Accordingly, we developed sensors targeting 12 metabolites, with 100-fold-enhanced signal-to-noise ratio and days-long stability. Leveraging these sensors, we monitored trace endogenous metabolites in sweat/saliva for noninvasive health monitoring, and a bacterial metabolite in the brain, marking a key milestone for unraveling gut microbiota-brain axis dynamics.
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