Abstract

Atmospheric pollution demands the development of solar-driven photocatalytic technologies for the conversion of CO2 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 CO2 to CO. This high catalytic efficiency stems from a highly conductive nanofibrillar structure that significantly enhances surface area, CO2 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 gcat–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.

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