In-situ synthesis of interfacial In-O-Mn lewis acid-base pairs for low-temperature photothermal CO2 hydrogenation to methanol
Jie Ding, Xiaofang Shang, Yimeng Zhou, Aizhe Han, Fan Zhang, Yanghe Fu, Yulong Zhang, Runping Ye, Maohong Fan, Shule Zhang, Qin Zhong
Abstract
CO2 hydrogenation into methanol suffers from a huge obstacle of low methanol yield due to the leverage effect of CO2 conversion and methanol selectivity. Here, we report an In2O3-MnCO3 catalyst consisting of In2O3 covalently linked to MnCO3 for efficiently photothermal CO2 hydrogenation into methanol. Covalent linkage, the O atoms of In2O3 occupy the oxygen vacancies of MnCO3, enables the formation of In-O-Mn Lewis acid-base pairs at the In2O3-MnCO3 interface. Both light irradiations and heatings improve the electron excitations and transfers from In to O, promoting CO2 activation and methanol production. The In2O3-MnCO3 containing 30 mol.% In achieves 67.5% methanol selectivity and 13.5% CO2 conversion at 150 °C, 4.0 MPa, and 14400 mL·h−1·g−1 with a high stability for at least 500 h on stream. This study provides a serial In-Mn catalyst design and understanding of the molecular-level structure-mediated photothermal catalytic hydrogenation. A In2O3-MnCO3 catalyst is constructed to form interfacial In-O-Mn Lewis acid-base pairs. Both light irradiation and heating strengthen the In-O-Mn Lewis acid-base pairs and drives photothermal CO2 hydrogenation to methanol at low temperature.