The combination of chemo-and biocatalysts offers a powerful platform to address synthetic challenges in chemistry, particularly in synthetic cascades. However, transferring both of them into organic solvents remains technically difficult due to the enzyme inactivation and catalyst precipitation. Herein, we designed a facile approach using functionalized mesoporous silica nanoparticles (MSN) to transfer chemo-and biocatalysts into a variety of organic solvents. As a proof-of-concept, two distinct catalysts, palladium nanoparticles (Pd NPs) and Candida antarctica lipase B (CalB), were stepwise loaded into separate locations of the mesoporous structure, which not only provided catalysts with heterogeneous supports for the recycling but also avoided their mutual inactivation. Moreover, mesoporous particles were hydrophobized by surface alkylation, resulting in a tailor-made particle hydrophobicity, which allowed bifunctional catalysts to be dispersed in eight organic solvents. Eventually, these attractive material properties provided the MSN-based bifunctional catalysts with remarkable catalytic performance for cascade reaction synthesizing benzyl hexanoate in toluene. On a broader perspective, the success of this study opens new avenues in the field of multifunctional catalysts where a plethora of other chemo-and biocatalysts can be incorporated into surface-functionalized materials ranging from soft matters to porous networks for synthetic purpose in organic solvents.

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Oxygen reduction reaction (ORR) not only needs the excellent electrode materials, but also requires quick mass transfer of dissolved oxygen. To strengthen the ORR and O 2 − oxidation desulfurization, pressurized water electrolysis was carried out in this work. The results showed that the desulfurization ratio increased with increasing pressure, indicating that the pressure has strengthened the O 2 − generation. As expected, the ORR initial potential shifted from −0.034 V to −0.030 V with increasing pressure from 0.1Mpa to 2Mpa. The peak current, the limit current density and the peak integral area all increased with increasing pressure. On the other hand, the reduction in solution resistance (R s ) and reaction resistance (R ct ) further verified that the pressure can strengthen the transfer of dissolved oxygen and the ORR dynamics. More importantly, the pressure has improved O 2 − generated potential in a large parameter window (the width of the metastable zone, the difference between the initial potential and the peak potential of the ORR). The pressure could enhance the O 2 − formation, and improve the desulfurization process.

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