Novel approaches to harness earth abundant silicates as building blocks for carbon dioxide removal, capture, utilization, and storage are gaining increasing attention in the context of sustainable and low carbon energy and resource recovery. Advancing a calibrated understanding of these fluid-silicate interactions is essential for developing scalable processes. One of the challenges in developing predictive controls over these interactions is the compositional and morphological heterogeneity of naturally occurring, heterogeneous magnesium silicate minerals. To address this challenge, the synthesis of architected mesoporous crystalline magnesium silicate (Mg₂SiO₄) is proposed. While synthesis routes for producing amorphous mesoporous magnesium silicates have been developed via sol-gel methods, approaches to synthesize crystalline magnesium silicates with well-controlled pore size distributions have not been explored. The conventional approaches of converting matter that is amorphous to crystalline states at elevated temperatures results in a heterogeneous pore size distribution. To develop controls on pore size distribution, amorphous mesoporous magnesium silicates are coated with carbon. This approach retains the pore structure during the amorphous to crystalline transformations of Mg-silicates at elevated temperatures. The carbon coating is removed on heating. Magnesium silicate particles produced using this approach have highly ordered pores around 2.58 nm and a specific surface area of 124.25 m²/g. In this study, we report the chemical compositions, morphologies, phase transitions, and pore structures of the intermediate materials produced during the synthesis of crystalline mesoporous magnesium silicates. The synthesis routes discussed in this study can be applied translationally to produce metal silicates with ordered mesoporous structures.

在可持续和低碳能源和资源回收的背景下，利用地球上丰富的硅酸盐作为二氧化碳去除、捕获、利用和储存的基石的新方法越来越受到关注。推进对这些流体-硅酸盐相互作用的校准理解对于开发可扩展的过程至关重要。开发对这些相互作用的预测控制的挑战之一是天然存在的异质硅酸镁矿物的成分和形态异质性。为了应对这一挑战，结构化介孔结晶硅酸镁（Mg ₂ SiO ₄) 提出。虽然通过溶胶-凝胶方法开发了生产无定形介孔硅酸镁的合成路线，但尚未探索合成具有良好控制的孔径分布的结晶硅酸镁的方法。在升高的温度下将非晶态物质转化为结晶态的常规方法导致不均匀的孔径分布。为了控制孔径分布，无定形中孔硅酸镁涂有碳。这种方法在高温下镁硅酸盐从无定形到结晶转变过程中保留了孔结构。加热时去除碳涂层。使用这种方法生产的硅酸镁颗粒具有约 2.58 nm 的高度有序的孔隙和 124.25 m 的比表面积² /克。在这项研究中，我们报告了在结晶介孔硅酸镁合成过程中产生的中间材料的化学成分、形态、相变和孔隙结构。本研究中讨论的合成路线可用于生产具有有序介孔结构的金属硅酸盐。