In conclusion, catalysts and sorbents applicable for the sorption-enhanced NH3 synthesis are presented in literature. However, the potential of the in situ removal was not yet demonstrated experimentally and accordingly is aimed for in this work. Based on modeling and simulation of the in situ removal, the increase in the weight-time yield of the NH3 synthesis in the kinetic and thermodynamic regime is estimated. Therefore, kinetic models for Ru and Fe catalysts are applied to compare the sorptionenhancement effect for both materials. The sorptive in situ separation is applied experimentally using different spatial configurations of the Fe catalyst and a metal chloride based sorbent in a tubular reactor. The specific configurations allow the discrimination between sorption and synthesis during sorption-enhanced NH3 synthesis. For evaluation of experimental and simulation results, the relative increase in the weight-time-yield through the in situ removal of NH3 is expressed as a sorptionenhancement factor. Furthermore, the model-based predictions for the in situ removal are validated by comparison to experimental data.