Abstract
Atmospheric pollution demands the development of solar-driven photocatalytic technologies for the conversion of CO(2) into a fuel; state-of-the-art cocatalyst systems demonstrate conversion efficiencies currently unattainable by a single catalyst. Here, we upend the status quo demonstrating that the nanofibrillar conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) is a record-breaking single catalyst for the photoreduction of CO(2) to CO. This high catalytic efficiency stems from a highly conductive nanofibrillar structure that significantly enhances surface area, CO(2) adsorption and light absorption. Moreover, the polymer's band gap is optimized via chemical doping/dedoping treatments using hydrochloric acid, ammonia hydroxide, and hydrazine. The hydrazine-treated PEDOT catalyst exhibits 100% CO yield under a stable regime (>10 h) with a maximum rate of CO evolution (3000 μmol g(cat) (-1) h(-1)) that is 2 orders of magnitude higher than the top performing single catalyst and surpassed only by three other cocatalyst systems. Nanofibrillar PEDOT provides a new direction for designing the next generation of high-efficiency photoreduction catalysts.