Cerium-promoted conversion of dinitrogen into high-energy-density material CeN6 under moderate pressure

IF 4.8 1区物理与天体物理 Q1 PHYSICS, MULTIDISCIPLINARY

Matter and Radiation at Extremes Pub Date : 2023-04-20 DOI:10.1063/5.0136443

Yuan-ming Wang, Zhihui Li, Shifeng Niu, Wen-cai Yi, Shuang Liu, Zhen Yao, Bingbing Liu

{"title":"Cerium-promoted conversion of dinitrogen into high-energy-density material CeN6 under moderate pressure","authors":"Yuan-ming Wang, Zhihui Li, Shifeng Niu, Wen-cai Yi, Shuang Liu, Zhen Yao, Bingbing Liu","doi":"10.1063/5.0136443","DOIUrl":null,"url":null,"abstract":"Synthesis pressure and structural stability are two crucial factors for highly energetic materials, and recent investigations have indicated that cerium is an efficient catalyst for N2 reduction reactions. Here, we systematically explore Ce–N compounds through first-principles calculations, demonstrating that the cerium atom can weaken the strength of the N≡N bond and that a rich variety of cerium polynitrides can be formed under moderate pressure. Significantly, P1̄-CeN6 possesses the lowest synthesis pressure of 32 GPa among layered metal polynitrides owing to the strong ligand effect of cerium. The layered structure of P1̄-CeN6 proposed here consists of novel N14 ring. To clarify the formation mechanism of P1̄-CeN6, the reaction path Ce + 3N2 → trans-CeN6 → P1̄-CeN6 is proposed. In addition, P1̄-CeN6 possesses high hardness (20.73 GPa) and can be quenched to ambient conditions. Charge transfer between cerium atoms and N14 rings plays a crucial role in structural stability. Furthermore, the volumetric energy density (11.20 kJ/cm3) of P1̄-CeN6 is much larger than that of TNT (7.05 kJ/cm3), and its detonation pressure (128.95 GPa) and detonation velocity (13.60 km/s) are respectively about seven times and twice those of TNT, and it is therefore a promising high-energy-density material.","PeriodicalId":54221,"journal":{"name":"Matter and Radiation at Extremes","volume":"55 1","pages":""},"PeriodicalIF":4.8000,"publicationDate":"2023-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"2","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Matter and Radiation at Extremes","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1063/5.0136443","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"PHYSICS, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 2

Abstract

Synthesis pressure and structural stability are two crucial factors for highly energetic materials, and recent investigations have indicated that cerium is an efficient catalyst for N2 reduction reactions. Here, we systematically explore Ce–N compounds through first-principles calculations, demonstrating that the cerium atom can weaken the strength of the N≡N bond and that a rich variety of cerium polynitrides can be formed under moderate pressure. Significantly, P1̄-CeN6 possesses the lowest synthesis pressure of 32 GPa among layered metal polynitrides owing to the strong ligand effect of cerium. The layered structure of P1̄-CeN6 proposed here consists of novel N14 ring. To clarify the formation mechanism of P1̄-CeN6, the reaction path Ce + 3N2 → trans-CeN6 → P1̄-CeN6 is proposed. In addition, P1̄-CeN6 possesses high hardness (20.73 GPa) and can be quenched to ambient conditions. Charge transfer between cerium atoms and N14 rings plays a crucial role in structural stability. Furthermore, the volumetric energy density (11.20 kJ/cm3) of P1̄-CeN6 is much larger than that of TNT (7.05 kJ/cm3), and its detonation pressure (128.95 GPa) and detonation velocity (13.60 km/s) are respectively about seven times and twice those of TNT, and it is therefore a promising high-energy-density material.

查看原文本刊更多论文

铈促进二氮在中压下转化为高能量密度材料CeN6

合成压力和结构稳定性是高能材料的两个关键因素，最近的研究表明，铈是N2还原反应的有效催化剂。在这里，我们通过第一性原理计算系统地探索了Ce-N化合物，证明了铈原子可以削弱N≡N键的强度，并且在中等压力下可以形成丰富多样的铈多氮化物。值得注意的是，由于铈的强配体效应，P1 -CeN6在层状金属多氮化物中具有最低的合成压力(32 GPa)。本文提出的P1 -CeN6层状结构由新颖的N14环组成。为了阐明P1′-CeN6的形成机理，提出了Ce + 3N2→反式cen6→P1′-CeN6的反应路径。此外，P1′-CeN6具有较高的硬度(20.73 GPa)，可以淬火到环境条件。铈原子与N14环之间的电荷转移对结构的稳定性起着至关重要的作用。P1 -CeN6的体积能密度(11.20 kJ/cm3)远大于TNT (7.05 kJ/cm3)，爆轰压力(128.95 GPa)和爆轰速度(13.60 km/s)分别是TNT的7倍和2倍左右，是一种很有前途的高能量密度材料。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Matter and Radiation at Extremes Physics and Astronomy-Atomic and Molecular Physics, and Optics

CiteScore

8.60

自引率

9.80%

发文量

160

审稿时长

15 weeks

期刊介绍： Matter and Radiation at Extremes (MRE), is committed to the publication of original and impactful research and review papers that address extreme states of matter and radiation, and the associated science and technology that are employed to produce and diagnose these conditions in the laboratory. Drivers, targets and diagnostics are included along with related numerical simulation and computational methods. It aims to provide a peer-reviewed platform for the international physics community and promote worldwide dissemination of the latest and impactful research in related fields.