Dataset for : A mechanistic study of CO2 gas hydrate formation in a mesoporous zeolite

Carbon Capture Utilization and Storage (CCUS) is essential for mitigating climate change and enabling a low-carbon future. Gas hydrate formation within confined space offers a promising strategy to advance gas hydrate technology, including CCUS. This study employs the first mesoporous zeolite ZMQ-1, with 2.3 nm-wide channels, as a scaffold for CO2 hydrate formation. CO2 adsorption experiments were conducted on pre-humidified ZMQ-1 at 275 K and pressures up to 3 MPa, with hydrate formation confirmed by identifying specific vibrational modes of CO2 through Fourier Transform Infrared (FTIR) spectroscopy. Hydrate formation occurred under mild conditions (1.3 MPa and 275 K) with an extremely short induction time of just 2 minutes at an optimal water-to-zeolite ratio (Rw = 2). The mesoporous zeolite-gas hydrate system demonstrated high volumetric CO2 capacity, reaching 151 wt.% (176 v/v). Comparative experiments with calcined (open-pore) and non-calcined (blocked-pore) zeolite revealed the spatial and temporal distribution of hydrate formation, providing insights into the role of pore confinement. These findings position mesoporous ZMQ-1 as a promising platform for CO2 storage via hyrate formation, with strong potential for future development in scalable and energy-efficient CCUS technologies.

碳捕获、利用与封存（Carbon Capture Utilization and Storage, CCUS）对于减缓气候变化、支撑低碳未来建设至关重要。受限空间内的气体水合物生成技术，为包括碳捕获、利用与封存在内的气体水合物技术发展提供了极具前景的优化路径。本研究首次采用具备2.3纳米级通道的介孔沸石ZMQ-1作为二氧化碳水合物生成的载体。研究人员在275 K、最高3 MPa的压力条件下，对经预润湿处理的ZMQ-1开展了二氧化碳吸附实验，并通过傅里叶变换红外（FTIR）光谱识别二氧化碳的特征振动模式，证实了水合物的生成。在最优水与沸石质量比（Rw=2）条件下，体系可在温和工况（1.3 MPa、275 K）下实现水合物生成，且诱导时间仅为2分钟，极为短暂。该介孔沸石-气体水合物体系展现出优异的体积二氧化碳存储容量，可达151 wt.%（176 v/v）。通过对煅烧（开孔）与未煅烧（闭孔）沸石开展对比实验，研究人员揭示了水合物生成的时空分布特征，阐明了孔道限域效应的作用机制。本研究结果表明，介孔ZMQ-1是极具应用潜力的二氧化碳水合物存储平台，为可规模化、节能型碳捕获、利用与封存技术的未来发展提供了强劲支撑。