Abstract
Two-dimensional(2D)ordered carbon-nitrogen binary compounds(CxNy)show great potential in many fields owing to their diverse structures and outstanding properties.However,the scalable and selective synthesis of 2D CxNy compounds remain a challenge due to the variable C/N stoichiometry induced coex-istence of graphitic,pyridinic,and pyrrolic N species and the competitive growth of graphene.Here,this work systematically explored the mechanism of selective growth of a series of 2D ordered CxNy com-pounds,namely,the g-C3N4,C2N,C3N,and C5N,on various epitaxial substrates via first-principles calcu-lations.By establishing the thermodynamic phase diagram,it is revealed that the individualized surface interaction and symmetry match between 2D CxNy compounds and substrates together enable the selec-tive epitaxial growth of single crystal 2D CxNy compounds within distinct chemical potential windows of feedstock.The kinetics behaviors of the diffusion and attachment of the decomposed feedstock C/N atoms to the growing CxNy clusters further confirmed the feasibility of the substrate mediated selective growth of 2D CxNy compounds.Moreover,the optimal experimental conditions,including the temperature and partial pressure of feedstock,are suggested for the selective growth of targeted 2D CxNy compound on individual epitaxial substrates by carefully considering the chemical potential of carbon/nitrogen as the functional of experimental parameters based on the standard thermochemical tables.This work pro-vides an insightful understanding on the mechanism of selective epitaxial growth of 2D ordered CxNy compounds for guiding the future experimental design.
基金项目
National Key R&D Program of China(2021YFA1500703)
National Key R&D Program of China(2023ZD0120704)
National Natural Science Foundation of China(22222302)
National Natural Science Foundation of China(22033002)
National Natural Science Foundation of China(T2321002)
the"Shuang Chuang"Talent Program(JSSCRC2021489)
Major Project of Natural Science Foundation(BK20222007of Jiangsu Province)
Fundamental Research Funds for the Central Universities(2242023k30028)
NETL
NSTL
万方数据