Molecular-Level Insight into How Hydroxyl Groups Boost Catalytic Activity in CO2 Hydrogenation into Methanol

Abstract

Exploring how hydrophilicity regulates catalytic properties at the molecular level remains a grand challenge, although it has great potential to offer guidelines for developing highly efficient catalysts and deepen the mechanistic understanding of heterogeneous catalysis. Here, we provide molecular-level insight into the influence of surface hydroxyl groups on hydrophilic SiC quantum dots (QDs) on CO 2 hydrogenation. In CO 2 hydrogenation into methanol, SiC QDs exhibited higher catalytic activity and lower activation energy than commercial SiC. Mechanistic studies revealed that the surface hydroxyl species on SiC QDs was directly involved in CO 2 hydrogenation through the addition of H atoms in hydroxyl groups into CO 2 to form HCOO* as the intermediate. The unique reaction path decreased the energy barrier for the formation of HCOO*, facilitating the activation of CO 2 . Our understanding of surface hydrophilicity directly instructs the development of efficient catalysts toward CO 2 hydrogenation.

Fabrication of Pd/SiO2 with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H2 Pressure

“…The reason was simply ascribed to the accumulation of more hydrophobic substrates on the hydrophobic surface during reactions. However, the precise and deep mechanism for this widespread improvement in catalytic activity had very little reports . The main reasons could be that it is difficult to precisely regulate the wettability of catalysts without affecting the active center .…”

“…However, the precise and deep mechanism for this widespread improvement in catalytic activity had very little reports. [38,39] The main reasons could be that it is difficult to precisely regulate the wettability of catalysts without affecting the active center. [40] Typically, there are two strategies to adjust the wettability of catalysts.…”

Ultrathin SiC Nanosheets with High Reduction Potential for Improved CH4 Generation from Photocatalytic Reduction of CO2

“…And the C 1s spectra in Figure d shows two bands centered at 283.3, 284.6 ascribed to C−Si and Si 3 C−O surface fragments, respectively . The formation of some C 3 Si‐OH or Si 3 C‐OH groups on the surface should be originated from the the etching treatment exposing abundant edge structures …”

Double Perovskite LaFexNi1−xO3 Nanorods Enable Efficient Oxygen Evolution Electrocatalysis

“…On the other hand, electronic property of perovskites is also a very important factor . The electronic structure of catalysts can control the adsorption of reactants and thus change the catalytic activity, in which the metal‐oxygen bridge in perovskite provides a basis for tailoring their electronic structure . For double perovskite (AA′BB′O 6 ), the A or B cations are substituted by different cations and can generate enhanced properties, where substituting B site by other TMs is an effective method for tuning the d‐band center to Fermi level ( E F ).…”