Proteinaceous catalysts found in extant biology are products of life that were potentially derived through prolonged periods of evolution. Given their complexity, it is reasonable to assume that they were not accessible to prebiotic chemistry as such. Nevertheless, the dependence of many enzymes on metal ions or metal–ligand cores suggests that catalysis relevant to biology could also be possible with just the metal centers. Given their availability on the Hadean/Archean Earth, it is fair to conjecture that metal ions could have constituted the first forms of catalysts. A slow increase of complexity that was facilitated through the provision of organic ligands and amino acids/peptides possibly allowed for further evolution and diversification, eventually demarcating them into specific functions. Herein, we summarize some key experimental developments and observations that support the possible roles of metal catalysts in shaping the origins of life. Further, we also discuss how they could have evolved into modern-day enzymes, with some suggestions for what could be the imminent next steps that researchers can pursue, to delineate the putative sequence of catalyst evolution during the early stages of life.
Organic materials are a sustainable alternative to replace inorganic transition metal-based cathodes in rechargeable intercalation batteries. Among the possible redox active organic materials, conjugated polymers with multiple redox sites per repeat unit are expected to afford high energy and power densities while being resistant to dissolution when in contact with battery electrolytes. However, accessing the full capacity of polymeric electrodes while ensuring electrochemical reversibility has been challenging. Using diketopyrrolopyrrole (DPP)-based donor− acceptor (D−A) polymers as model systems and complementary electrochemical experiments and first-principles calculations, we show that conjugated backbone moieties that minimize charge localization on the electron accepting repeat units lead to near theoretical discharge capacities. Further, the capacity enhancement is associated with better rate performance and improved electrochemical stability of the polymer over prolonged cycling. Our work suggests that charge density on the electron accepting moiety is a potential descriptor for rationally designing redox-active polymer electrodes that afford high discharge capacities along with a long cycle life.
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