AtomCat4Fuel: Atomically construction of AuPd catalyst for efficient CO2 hydrogenation to ethanol

点击翻译按钮获取中文摘要

Climate change is arguably one of the most top challenges our planet facing during the 21st century, mainly due to huge amounts of greenhouse gas emissions in CO2 form to the atmosphere. In this regard, the catalytic upgradation of CO2 into fuels and high-value chemicals, e.g., ethanol, appears to be one of the most valuable solutions to address the overloaded CO2 in air. Catalytic CO2 hydrogenation to ethanol (CTE) not only contributes to slow down the global warming but also contributes to alleviate the global food shortage. Among various developed catalysts, Au- and Pd-based nano-materials emerge as one of the most effective catalysts for CO2 hydrogenation to ethanol, which deserves more research efforts. While the limited ethanol activity (TOF < 400 h-1) and relatively harsh reaction conditions (T greater than or equal to 200 oC, P > 3 MPa) preclude these works from industrialization. Herein, this proposal focuses on developing the strategies to maximize the atom utilization efficiency and the sites number of metal/adjacent oxygen vacancy, through atom-by-atom constructing atomically precise Au/Pd sites on oxygen-vacancy-rich My/TiO2-x (i.e., M=In3+, Fe3+), to further improve ethanol productivity under mild conditions. Furthermore, various operando spectroscopy techniques (e.g., operando X-ray absorption spectroscopy and steady-state isotopic transient kinetic analysis) will be integrated to identify the intermediates and mechanism of C-C coupling, thus establishing a clear structure-performance relationship and providing a rational guidance for the design of future CO2 catalysts, all of which will contribute to the ambitious goal of European Commission for reducing CO2 emissions from all sources by 80%-95% by 2050.