Tuning the Chemical Hardness of Boron Nitride Nanosheets by Doping Carbon for Enhanced Adsorption Capacity

[Image: see text] The chemical hardness of adsorbents is an important physicochemical property in the process of adsorption based on the hard and soft acids and bases (HSAB) theory. Tuning chemical hardness of adsorbents modulated by their concomitants is a promising approach to enhance the adsorptive capacity in principle. In the present work, we report an efficient strategy that the adsorption capacity for aromatic sulfocompounds can be enhanced by tuning the chemical hardness. This strategy is first theoretically explored by introducing C element into the network of hexagonal boron nitride (h-BN) based on a series of model materials (model_xC, x = 1–5). Computational results show that the chemical hardness is reduced after gradually C-doping, which may lead to an enhancement of adsorption capacity according to the HSAB theory. Then, a series of C-doped h-BN materials (BCN-x, x = 10–50) were controlled synthesized. All of the as-prepared materials show better adsorption capacities (e.g., 27.43 mg g(–1) for BCN-50) than pure h-BN. Experiment results show that the adsorption capacity correlates well with the C content in the BCN-x, which is consistent with the results predicted by theoretical calculation. This strategy may be helpful to rationally design highly efficient adsorbents in separation engineering and may be expanded to similar two-dimensional materials, where the π–π interaction is the dominant driven force.