Direct Photoconversion of Shale Gas into Liquid Oxygenates Over Interfacially Coupled Ni/ZnO Nanomesh.

Shale gas, a mixture of methane (CH4), ethane (C2H6), and propane (C3H8), provides an alternative feedstock for producing chemicals in industry. As the increasing energy crisis and environmental concern, the conversion of shale gas to value-added chemical in a sustainable manner has emerged as a new frontier yet remains great challenges. Herein, we realize the solar-driven conversion of shale gas into alcohols over ZnO nanomeshes incorporated with Ni nanoparticles (Ni/ZnO NM) with oxygen and water. Specifically, the isopropanol yield from C3H8 oxidation reaches 7.1 mmol  g-1  h-1 at a selectivity of 83.5%, with an apparent quantum efficiency (AQE) of 0.65% at 350 nm, surpassing the reported catalysts for propane-to-oxygenates. Moreover, both the selectivity of methanol and ethanol surpass 90% from solar-driven CH4 and C2H6 oxidation. Impressively, a mixture of methane, ethane, and propane, the analogue of shale gas, can be selectively converted into methanol, ethanol, and isopropanol. Mechanism studies suggest the strong interaction induces electron transfer from ZnO to Ni and creates electron-rich Ni sites and electron-deficient oxygen vacancies (Vo) in ZnO NM. Under light irradiation, electron-rich Ni sites and electron-deficient Vo can serve as hole and electron acceptors, respectively, promoting the separation of photogenerated carriers and enhancing performance toward alkane oxidation.