多级孔Ti-MOFs负载超细Pd纳米颗粒实现高效光热CO2还原

The exploration of robust titanium-based metal-organic framework (MOF) photocatalysts for efficient CO2 reduction is of critical significance but remains challenging. Herein, a hierarchically porous titanium-MOF (hMUV-10) anchored with ultrafine Pd nanoparticles was rationally designed via a convenient one-step in-situ water-etching strategy. The hierarchical MUV-10 structure provided abundant sites for the anchoring of Pd nanoparticles on the outside and inside of MOFs. The optimized Pd/hMUV-10 demonstrated an ultrahigh CO production rate of 65.9 mmol g−1 h−1 under light irradiation at 350°C, approximately two orders of magnitude higher than the state-of-the-art MOF-based catalysts and surpassed most reported inorganic semiconductor-based catalysts. The CO production rate under a relatively mild temperature of 200°C also reached as high as 3.36 mmol g−1 h−1, and negligible activity decay was observed during continuous cycling measurement under 350°C. Theoretical calculations suggested that Pd enhanced CO2 adsorption ability and reduced the energy barrier for CO2 reduction, thereby leading to a highly improved CO yield from photothermal CO2 reduction.