Tailorable Formation of Hierarchical Structure Silica (HMS) and Its Application in Hydrogen Production

Relentless endeavors have been committed to seeking simple structure-directing agents for synthesizing hierarchical mesoporous silica (HMS) materials but remaining challenges. In this contribution, we offered an improved one-pot hydrothermal route to prepare HMS materials using a single non-ionic triblock copolymer (F127) structure-directing agent under a mild polycarboxylic (citric acid) mediated condition. Via studies of key synthetic parameters including acid concentration, crystallization temperature and aging time, it was found that citric acid medium presents an important bridging effect under the optimal concentration from 0.018 M (pH = 2.57) to 1.82 M (pH = 1.09), contributing to the self-assemblage of partially protonated non-ionic triblock copolymer and tetraethyl orthosilicate (TEOS) into a high-quality multistage structure of silica materials. The specific surface area (SSA) of HMS shows a volcanic trend and is closely associated with the concentration of citric acid while the highest SSA of 739.9 m(2)/g can be achieved at the citric concentration of 0.28 M. Moreover, the as-synthesized HMS-CTA supported Ni/CeO2 catalysts indicate an excellent production of hydrogen through dry reforming of methane (DRM) reaction over 172 h stability. The improved, facile synthesis strategy under polycarboxylic medium displays an expanded perspective for synthesizing other mesoporous materials in a wide range of applications such as catalytic material carriers and drug inhibitors.

Automated summary

In this study, an improved method was proposed to prepare HMS materials using a single non-ionic triblock copolymer (F127) structure-directing agent under a mild polycarboxylic (citric acid) mediated condition. The citric acid medium was found to have an important bridging effect, contributing to the self-assemblage of partially protonated non-ionic triblock copolymer and tetraethyl orthosilicate (TEOS) into a high-quality multistage structure of silica materials. The specific surface area (SSA) of HMS showed a volcanic trend and was closely associated with the concentration of citric acid.