Valorization of C1 gases including CO, CO₂, and CH₄ to useful chemicals is one of the carbon-neutral strategies and it supports a process of global consensus on climate change. This talk will cover three subjects of oxidative carbonylation of alcohols, CO₂ hydrogenation, and CH₄ selective oxidation using heterogeneous catalysts. The main target product from CO₂ hydrogenation and CH₄ selective oxidation is methanol and dialkyl carbonate through oxidative carbonylation of alcohol. These strategic developments are underway for practical applications.

Although TS-1 with an MFI framework is a useful catalyst for phenol oxidation, [Ti]-MCM-68, a novel MSE-type titanosilicate with 12-ring and 10-ring micropores, has been developed as a phenol oxidation catalyst with high activity and selectivity toward the para -isomer, hydroquinone. The thermal treatment after Ti insertion into the MSE framework significantly enhanced the catalytic activity of [Ti]-MCM-68, mainly due to an improvement in the hydrophobicity in the micropores. The addition of EtOH to the reaction mixture resulted in the best para-selectivity (>94%) due to enhancement of hydrophobicity by covering external Ti sites through Si–OH and EtOH interactions.