Porous carbonaceous materials have many important industrial applications including energy storage, water purification, and adsorption of volatile organic compounds. Most of their applications rely upon the adsorption of molecules or ions within the interior pore volume of the carbon particles. Understanding the behaviour and properties of adsorbate species on the molecular level is therefore key for optimising porous carbon materials, but this is very challenging owing to the complexity of the disordered carbon structure and the presence of multiple phases in the system. In recent years, NMR spectroscopy has emerged as one of the few experimental techniques that can resolve adsorbed species from those outside the pore network. Adsorbed, or “in-pore” species are shielded with respect to their free (or “ex-pore”) counterparts. This shielding effect arises primarily due to ring currents in the carbon structure in the presence of a magnetic field, such that the observed chemical shift differences upon adsorption are independent of the observed nucleus to a first approximation. Theoretical modelling has played an important role in rationalising and explaining these experimental observations. Together, experiments and simulations have enabled a large amount of information to be gained on the adsorption and diffusion of adsorbed species, as well as on the structural and magnetic properties of the porous carbon adsorbent. Here, we review the methodological developments and applications of NMR spectroscopy and related modelling in this field, and provide perspectives on possible future applications and research directions.

多孔碳质材料具有许多重要的工业应用，包括能量存储、水净化和挥发性有机化合物的吸附。它们的大多数应用依赖于分子或离子在碳颗粒内部孔体积内的吸附。因此，在分子水平上了解吸附物质的行为和性质是优化多孔碳材料的关键，但由于无序碳结构的复杂性和系统中多相的存在，这非常具有挑战性。近年来，核磁共振光谱已成为少数可以从孔隙网络之外的物质中分辨吸附物质的实验技术之一。吸附的或“孔内”物质相对于它们的游离（或“孔外”）对应物是屏蔽的。这种屏蔽效应主要是由于存在磁场时碳结构中的环电流引起的，因此在吸附时观察到的化学位移差异与观察到的原子核无关。理论建模在合理化和解释这些实验观察方面发挥了重要作用。通过实验和模拟，我们可以获得大量关于吸附物质的吸附和扩散以及多孔碳吸附剂的结构和磁性的信息。在这里，我们回顾了 NMR 光谱和相关建模在该领域的方法学发展和应用，并提供了未来可能的应用和研究方向的观点。