Motivated by compelling fundamental benefits of the variable-volume batch reaction approach with hydrogen membrane separation(CHAMP reactor)in combination with in situ carbon dioxide(CO2)removal via sorption(SORB),we invented and investigated a new class of dynamically-adaptive,multifunctional reactors(CHAMP-SORB)for hydrogen generation via natural gas steam reforming for challenging distributed power generation applications.CHAMP-SORB concept exploits synergies of CO2 removal from the product stream,as it is being produced to shift the reforming reaction equilibrium towards full fuel conversion at low temperature,with enhancement of heat/mass transfer and reaction kinetics realized by a variable volume batch reactor integrated with hydrogen-selective membrane separation.This results in two-fold reduction in the reaction temperature(and equivalent improvement in process energy efficiency)as well as nearly stoichiometric 2-to-1 steam-to-carbon ratio(i.e.,minimization of parasitic use of excess in steam)in the feedstock.Through complimentary theoretical and experimental research,we discovered the fundamental laws governing the CHAMP-SORB reactor operation and developed a comprehensive analytical framework based on first principles of multiscale reaction-transport modeling and bench-scale experimentation for optimal design and operation of CHAMP-SORB reactors.