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A Cooperative DNA Catalyst.

ABSTRACT: DNA catalysts are fundamental building blocks for diverse molecular information-processing circuits. Allosteric control of DNA catalysts has been developed to activate desired catalytic pathways at desired times. Here we introduce a new type of DNA catalyst that we call a cooperative catalyst: a pair of reversible reactions are employed to drive a catalytic cycle in which two signal species, which can be interpreted as an activator and an input, both exhibit catalytic behavior for output production. We demonstrate the role of a dissociation toehold in controlling the kinetics of the reaction pathway and the significance of a wobble base pair in promoting the robustness of the activator. We show near-complete output production with input and activator concentrations that are 0.1 times the gate concentration. The system involves just a double-stranded gate species and a single-stranded fuel species, as simple as the seesaw DNA catalyst, which has no allosteric control. The simplicity and modularity of the design make the cooperative DNA catalyst an exciting addition to strand-displacement motifs for general-purpose computation and dynamics.

SUBMITTER: Taylor DN

PROVIDER: S-EPMC8609974 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:ConspectusTo say the least, releasing CO2 into the atmosphere is reaping undue environmental consequences given the ever-present increase in severe global weather events over the past five years. However, it can be argued that-at least in the confines of current technological capabilities-the atmospheric release of CO2 is somewhat unavoidable given that even shifting toward clean energy sources-such as solar, nuclear, wind, battery, or H2 power-incurs an initial carbon requirement by way of manufacturing the very production abilities through which "clean" energy is generated. Even years from now, experts agree that energy production will be diversified and-as the global population continues to drive the growth of global energy consumption-thermal power derived from carbon combustion is likely to remain one intrinsic energetic source, of which CO2 will always be a byproduct. In this context, it is the responsibility of the scientific community to devise improved pathways of carbon management such that (i) the consequences of combustion on the global environment are reduced and (ii) carbon fuels can be leveraged in a sustainable fashion.In this Account, we discuss a pivotal perspective shift on CO2 emissions derived from a considerable breakthrough in material science from our work on shape engineering of nanoporous adsorbents and catalysts. This account details the development of materials which no longer vilify CO2 emissions as a valueless combustion byproduct, instead providing a path for them to become a potential feedstock. In more specific terms, this work details the development of structured, cooperative "bifunctional" materials (BFMs) comprised of (i) a high-temperature adsorbent and (ii) a heterogeneous catalyst that enable single-bed CO2 capture and utilization in oxidative ethane dehydrogenation (ODHE), oxidative propane dehydrogenation (ODHP), and dry methane reforming (DMR) processes. This Account begins with the conceptual development of the BFMs in the powdered state, followed by detailing the first-ever reports of structuring the materials into facile honeycomb contactors by 3D printing. The Account then summarizes the impressive performance of the 3D-printed BFMs, specifically focusing on how their catalysts (metal oxides and perovskites) influence their reactive CO2 capture performances in ODHE, ODHP, and DMR processes. Such promise of CO2-as-fuel offers a glimpse into the future of a diversified energy economy, in which CO2/fuel looping can play an important role. A major factor in achieving this future is, of course, developing an appropriately active catalyst; an account of whose first breakthroughs in material science are detailed herein.

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A Cooperative DNA Catalyst.

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