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Epitaxial heterostructures, in particular those 2D vertical heterostructures with close face-to-face contact, are appealing candidates for photocatalytic CO2reduction. Usually, precise control of the growth rate and a seed nanosheet having a small lattice mismatch with the overlayer is essential for the realization of epitaxial growth. Here we present a CO2-initiated solution-phase epitaxial growth strategy to directly fabricate 2D facet-coupled vertical heterostructures without a seed-layer assistant, in which supercritical CO2liquid can not only manipulate the nucleation and growth of BiOIO3to match with the epitaxial growth of the Bi2O2CO3layer, but also provide better wetting conditions to minimize the interfacial energy, thus facilitating the 2D layer-by-layer growth. The obtained heterostructures exhibit the highest CO2-to-CO conversion rate of 224.71 µmol g-1h-1in pure water. These findings open up a new platform for highly controlled epitaxial growth of heterostructures.

CO2capture, storage and utilization (CCSU) is the most promising strategy for ameliorating the ever-increasing atmospheric CO2concentrations problem. The development of advanced porous solid adsorbents for efficient CCSU is a burgeoning interest in materials science. Currently, porous carbon-based adsorbents face the major challenge of balancing the structural features of porosity and surface chemistry for CCSU in a durable and scalable material. To this end, we designed hierarchically porous carbons with tailorable porosity and adjustable surface chemistry, and clarify the influence of porosity and surface chemistry on CO2capture. Meanwhile, the systematic study revealed the synergetic effect of microporosity of less than 10 Å and surface chemistry on CO2capture, and the synergistic effect mechanism of various surface groups on CO2capture property was also ascertained in detail. Porosity was found to be the determinant role on CO2capture, in particular the microporosity of < 10 Å and ultramicroporosity of < 7.0 Å. While, surface chemistry played a significant role on the improvement of CO2capture, especially the CO2/N2selectivity at higher temperature. Importantly, this work provided an instructive guideline for rational design of high-efficient porous carbon CO2adsorbents with a balanced porosity and surface chemistry property.