The four-decade quest for synthesizing ambient-stable polymeric nitrogen,a promising high-energy-density material,remains an unsolved challenge in materials science.We develop a multi-stage computational strategy empl...The four-decade quest for synthesizing ambient-stable polymeric nitrogen,a promising high-energy-density material,remains an unsolved challenge in materials science.We develop a multi-stage computational strategy employing density functional tight-binding-based rapid screening combined with density functional theory refinement and global structure searching,effectively bridging computational efficiency with quantum accuracy.This integrated approach identifies four novel polymeric nitrogen phases(Fddd,P3221,I4m2,and𝑃P6522)that are thermodynamically stable at ambient pressure.Remarkably,the helical𝑃6522 configuration demonstrates exceptional thermal resilience up to 1500 K,representing a predicted polymeric nitrogen structure that maintains stability under both atmospheric pressure and high-temperature extremes.Our methodology establishes a paradigm-shifting framework for the accelerated discovery of metastable energetic materials,resolving critical bottlenecks in theoretical predictions while providing experimentally actionable targets for polymeric nitrogen synthesis.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.11974154,and 12304278)the Taishan Scholars Special Funding for Construction Projects(Grant No.tstp20230622)+1 种基金the Natural Science Foundation of Shandong Province(Grant Nos.ZR2022MA004,ZR2023QA127,and ZR2024QA121)the Special Foundation of Yantai for Leading Talents above Provincial Level。
文摘The four-decade quest for synthesizing ambient-stable polymeric nitrogen,a promising high-energy-density material,remains an unsolved challenge in materials science.We develop a multi-stage computational strategy employing density functional tight-binding-based rapid screening combined with density functional theory refinement and global structure searching,effectively bridging computational efficiency with quantum accuracy.This integrated approach identifies four novel polymeric nitrogen phases(Fddd,P3221,I4m2,and𝑃P6522)that are thermodynamically stable at ambient pressure.Remarkably,the helical𝑃6522 configuration demonstrates exceptional thermal resilience up to 1500 K,representing a predicted polymeric nitrogen structure that maintains stability under both atmospheric pressure and high-temperature extremes.Our methodology establishes a paradigm-shifting framework for the accelerated discovery of metastable energetic materials,resolving critical bottlenecks in theoretical predictions while providing experimentally actionable targets for polymeric nitrogen synthesis.
