CO <sub>2</sub> reduction driven by a pH gradient
Reuben Hudson, Ruvan de Graaf, Mari Strandoo Rodin, Aya Ohno, Nick Lane, Shawn E. McGlynn, Yoichi M. A. Yamada, Ryuhei Nakamura, Laura M. Barge, Dieter Braun, Víctor Sojo
Abstract
Significance Biology is built of organic molecules, which originate primarily from the reduction of CO 2 through several carbon-fixation pathways. Only one of these—the Wood–Ljungdahl acetyl-CoA pathway—is energetically profitable overall and present in both Archaea and Bacteria, making it relevant to studies of the origin of life. We used geologically pertinent, life-like microfluidic pH gradients across freshly deposited Fe(Ni)S precipitates to demonstrate the first step of this pathway: the otherwise unfavorable production of formate (HCOO – ) from CO 2 and H 2 . By separating CO 2 and H 2 into acidic and alkaline conditions—as they would have been in early-Earth alkaline hydrothermal vents—we demonstrate a mild indirect electrochemical mechanism of pH-driven carbon fixation relevant to life’s emergence, industry, and environmental chemistry.