3 years ago

Non-Enzymatic RNA Backbone Proofreading through Energy-Dissipative Recycling

Non-Enzymatic RNA Backbone Proofreading through Energy-Dissipative Recycling
John D. Sutherland, Angelica Mariani
Non-enzymatic oligomerization of activated ribonucleotides leads to ribonucleic acids that contain a mixture of 2′,5′- and 3′,5′-linkages, and overcoming this backbone heterogeneity has long been considered a major limitation to the prebiotic emergence of RNA. Herein, we demonstrate non-enzymatic chemistry that progressively converts 2′,5′-linkages into 3′,5′-linkages through iterative degradation and repair. The energetic costs of this proofreading are met by the hydrolytic turnover of a phosphate activating agent and an acylating agent. With multiple rounds of this energy-dissipative recycling, we show that all-3′,5′-linked duplex RNA can emerge from a backbone heterogeneous mixture, thereby delineating a route that could have driven RNA evolution on the early earth. If at first you don't succeed, try, try again: With enzymes not available on the early Earth, energy-dissipative cycles might have contributed to the correction and recycling of ribonucleic acids, which defines a plausible scenario for the prebiotic evolution of RNA.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201703169

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