【Frontiers in HaiChuan Chemical Technology】Dalian Institute of Chemical Physics develops hydroxyl-rich surface photocatalysts to achieve highly selective control of methane conversion to ethane
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Recently, the research team led by Researcher Zhang Fuxiang from the Group on Solar Hydrogen Production and Storage Materials and Catalysis (DNL1621) in our Institute’s Solar Energy Research Department designed and synthesized a hydroxyl-rich modified photocatalyst (R-MnOx/CeO2), enabling highly active and selective control of the methane-to-ethane conversion reaction. Studies have found that the enrichment of hydroxyl groups on the surface of the catalyst can enhance the chemical adsorption of methane, reduce the energy barrier for ethane formation, and suppress carbon dioxide generation; these factors are key to improving the performance of photocatalytic methane activation and C-C coupling for ethane production. As the main component of natural gas, the efficient conversion of methane into high-value chemicals holds great promise for energy utilization and the upgrading of carbon resources. Photocatalytic technology offers a viable solution for the efficient conversion of methane under mild conditions, thanks to its ability to activate inert C-H bonds at room temperature. Despite certain progress in photocatalytic methane conversion in recent years, its overall efficiency remains limited by three key issues: the difficulty in activating C-H bonds, the tendency of the products to be highly oxidized to CO2, and the lack of clarity regarding the relevant reaction mechanisms. The introduction of a catalyst can effectively improve reaction activity and selectivity. However, traditional studies on catalyst modifiers focus mainly on factors such as their chemical composition, morphology, and interface contact with the photocatalyst; there is relatively little research on the impact of the microstructural environment on the surface of the catalyst modifier, and a deep understanding of the mechanisms underlying these structural effects is lacking. In this work, researchers conducted systematic studies on the fine structure regulation of various promoters on the surface of CeO2 photocatalysts, and their impact on the adsorption, activation, and conversion of methane through photocatalysis. Studies have found that increasing the hydroxyl group concentration on the surface of the catalyst promoter facilitates the chemical adsorption and activation of methane, reduces the energy barrier for ethane formation, and suppresses excessive oxidation to carbon dioxide; these factors are key to promoting methane activation for efficient C-C coupling. Based on this, researchers developed a hydroxyl-rich modified photocatalyst R-MnOx/CeO2, achieving a visible-light catalyzed methane-to-ethane conversion rate of 187 μmol·g-1·h-1 with a selectivity of 97%, and the catalyst was able to operate stably for over 200 hours. The related work was published in Angewandte Chemie International Edition under the title “Hydroxyl-Promoted C-C Coupling for Selective Methane Conversion into Ethane on Cerium Oxide Photocatalyst”. The co-first authors of this achievement are Luo Lei, an assistant researcher in our DNL1621 group, and Wang Rong, a postdoctoral fellow. This research was supported by projects such as the **Key Research and Development Program**, the National Natural Science Foundation, the Beijing Light Source, the China Postdoctoral Science Foundation, the Special Research Assistant Program of the Chinese Academy of Sciences, and the Outstanding Postdoctoral Awards of our institute.
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I. Basic concepts of surface hydroxylation catalysis Surface hydroxylation catalysis refers to the process of using hydroxyl functional groups on the surface of a catalyst to facilitate chemical reactions. Surface hydroxyl groups play a very important role in many catalytic reactions; they can increase the hydrophilicity of the active centers and enhance the adsorption capacity for reactants, thereby facilitating the progress of the reactions. The ability of the catalyst surface to form surface hydroxyl groups is influenced by various factors such as the catalyst’s composition, structure, and preparation method. II. Catalyst Types and Formation Mechanisms The following are some common catalyst types that can generate surface hydroxyl groups: 1. Metal oxide catalysts: such as alumina, titanium dioxide, etc. These catalyst surfaces possess high hydrophilicity, chemical activity, and catalytic properties, and can form surface hydroxyl groups by adsorbing water molecules. 2. Fertal halogen-type catalysts: such as aluminum fluoride, zinc chloride, etc. The surfaces of these catalysts possess strong Lewis acidity, allowing them to react with water molecules to form surface hydroxyl groups. 3. Metal catalysts: such as copper, silver, etc. The surfaces of these catalysts can adsorb water molecules from the air to form surface hydroxyl groups, enabling them to exhibit excellent catalytic performance when catalyzing reactions in aqueous media. 4. Carbon material catalysts: such as activated carbon, activated carbon fibers, etc. These catalysts possess abundant functional groups and pore structures on their surfaces, which enable them to adsorb and catalyze molecular reactions; they also contain a large number of surface hydroxyl groups. Whether the catalyst surface has hydroxyl groups depends on the environmental conditions and the way the catalyst is treated. Under dry conditions, hydroxyl groups tend to dehydrate to form surface oxygen vacancies. Furthermore, the surface properties of catalysts are also influenced by factors such as their crystal structure, physical state, and surface modification. III. The role of surface hydroxyl groups in catalytic reactions In catalytic reactions, surface hydroxyl groups can facilitate the progress of the reaction by forming hydrogen bonds or other interactions with reactant molecules. For example, in the dehydration reaction of alcohols, surface hydroxyl groups can act as active centers for the reaction, forming hydrogen bonds with alcohol molecules to facilitate the dehydration process within those molecules. Furthermore, surface hydroxyl groups can also facilitate the progress of reactions through mechanisms such as electron transfer with reactant molecules. IV. Application prospects of surface hydroxylation catalysis Surface hydroxylation catalysis is an important type of catalytic reaction that is widely used in fields such as chemistry, energy, and environmental protection. By conducting in-depth research on the formation mechanism of hydroxyl groups on the catalyst surface and its catalytic behavior, important theoretical foundations and practical guidance can be provided for the design and optimization of catalysts. In the future, surface hydroxylation catalysis technology will find wider applications in fields such as new energy, new materials, and biomedicine. In summary, surface hydroxylation catalysis is an important type of catalytic reaction with broad application prospects. By conducting in-depth research on the formation mechanism and catalytic role of surface hydroxyl groups, important theoretical foundations and practical guidance can be provided for the design and optimization of catalysts.