14390-96-6Relevant articles and documents
Stability of H, D, 14N, and 15N atoms in solid ammonia above 100 K
DeMarco,Brill,Crabb
, p. 1423 - 1428 (1998)
The measurements reported below quantify the stability and decay of hydrogen, deuterium, and nitrogen atoms in frozen ammonia above 100 K. The decay of H atoms is observed on a time scale of minutes in the range of 100-110 K and follows first-order kinetics. Analogous decays of D and N atoms are observed in the ranges 105-120 and 140-160 K, respectively. Activation energies for the decay processes range from 0.1 to 0.4 eV.
Amorphization engineered VSe2-: Xnanosheets with abundant Se-vacancies for enhanced N2electroreduction
Chu, Ke,Li, Qingqing,Liu, Yaping,Luo, Yaojing,Tian, Ye
supporting information, p. 1742 - 1749 (2022/02/02)
Electrochemical N2 fixation through the nitrogen reduction reaction (NRR) is a promising route for sustainable NH3 synthesis, while exploring high-performance NRR catalysts lies at the heart of achieving high-efficiency NRR electrocatalysis. Herein, we reported the structural regulation of VSe2 by amorphization engineering, which simultaneously triggered the enriched Se-vacancies. The developed amorphous VSe2-x nanosheets with abundant Se-vacancies (a-VSe2-x) delivered a much enhanced NRR activity with an NH3 yield of 65.7 μg h-1 mg-1 and a faradaic efficiency of 16.3% at -0.4 V, being 8.8- and 3.5-fold higher than those of their crystalline counterparts, respectively. Density functional theory computations combined with molecular dynamics simulations revealed that the amorphization-triggered Se-vacancies could induce the upraised d-band center of unsaturated V atoms, capable of promoting the binding of key ?N2/?NNH species to result in an energetically favorable NRR process. This journal is
Regulation of the electronic structure of perovskites to improve the electrocatalytic performance for the nitrogen-reduction reaction
Bao, Di,Jiao, Meng-Gai,Li, Kai,Shi, Miao-Miao,Wang, Jia-Zhi,Wen, Zi,Zhang, Yan
supporting information, p. 2819 - 2825 (2022/02/21)
Ammonia has received widespread attention as an indispensable chemical for humans and a potential energy source for a future low-carbon society. To meet the urgent requirements for a high output of synthetic ammonia by the electrocatalytic nitrogen reduction reaction (ENRR), the design of robust catalysts has become particularly important. Adjusting the charge and spin configuration of catalysts is a novel and effective way to optimize the ENRR barrier. We found that, through doping Co atoms, there was a correlation between the effective spin magnetic moment of the Co-LNO (Co-doped LaNiO3) catalyst and its catalytic performance for the ENRR. Uniquely, LaNi0.995Co0.005O3-δ with a high spin configuration was endowed with an excellent ENRR performance, including a high ammonia yield rate of 14.57 μg h-1 mg-1, an outstanding faradaic efficiency of 26.44%, and a remarkable energy efficiency of 21.35% (-0.1 V vs. the reversible hydrogen electrode). According to density functional theory calculations, we infer that Co-LNO provides Co with catalytically active sites and the accompanying oxygen vacancies to adjust the electronic structure and promote N2 adsorption and the first protonation to form ?NNH.
A thiolate-bridged FeIVFeIV μ-nitrido complex and its hydrogenation reactivity toward ammonia formation
Chen, Hui,Mei, Tao,Qu, Jingping,Wang, Baomin,Wang, Junhu,Yang, Dawei,Ye, Shengfa,Zhang, Yixin,Zhao, Jinfeng,Zhou, Yuhan
, p. 46 - 52 (2021/12/27)
Iron nitrides are key intermediates in biological nitrogen fixation and the industrial Haber–Bosch process, used to form ammonia from dinitrogen. However, the proposed successive conversion of nitride to ammonia remains elusive. In this regard, the search for well-described multi-iron nitrido model complexes and investigations on controlling their reactivity towards ammonia formation have long been of great challenge and importance. Here we report a well-defined thiolate-bridged FeIVFeIV μ-nitrido complex featuring an uncommon bent Fe–N–Fe moiety. Remarkably, this complex shows excellent reactivity toward hydrogenation with H2 at ambient conditions, forming ammonia in high yield. Combined experimental and computational studies demonstrate that a thiolate-bridged FeIIIFeIII μ-amido complex is a key intermediate, which is generated through an unusual two-electron oxidation of H2. Moreover, ammonia production was also realized by treating this diiron μ-nitride with electrons and water as a proton source. [Figure not available: see fulltext.].
