Accessing the rich carbon nitride materials chemistry by heat treatments of ammonium thiocyanate, NH_4SCN

Finn Krebs Larsen; Aref Hasen Mamakhel; Jacob Overgaard; Jens-Erik J?rgensen; Kenichi Kato; Bo Brummerstedt Iversen

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Accessing the rich carbon nitride materials chemistry by heat treatments of ammonium thiocyanate, NH_4SCN

机译：通过热处理硫氰酸铵，NH_4SCN的热处理进入富碳氮化物材料化学

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Carbon nitride materials include functional materials, and their chemical diversity and complexity are becoming increasingly appreciated. Heating of NH_4SCN leads to a range of new carbon nitride compounds, which have been structurally characterized by single-crystal X-ray diffraction. Heating at ambient pressure to 175°C leads to guanidinium thiocyanate, H_6CN_3SCN (1), and when maintaining that temperature for about 12 h a water-insoluble carbon nitride product is formed, which is a co-crystal between melamine and melamium thiocyanate, [H_6C_3N_6]·[H_(10)C_6N_(11)]~+·[SCN]~- (2). In situ powder X-ray diffraction measurements of this material reveal a gradual transformation from (2), via two intermediate products, to a final melon-like end product. The first of these forms between 350 and 400°C, and is an adduct of melam and melamium thiocyanate, [H_9C_6N_(11)]·2[H_(10)C_6N_(11)]~+·2[SCN]~- (3). The second forms between 400 and 480°C, and is identified as melem, 2,5,8-triamino-tri-s-triazine, H_6C_6N_(10) (4). On heating of (2) in a sealed ampoule to 600°C, various crystals were obtained and six crystal structures were determined from the batch: 1,3,5-triazine-2,4,6- triamino, H_6C_3N_6 (5), 1,3,5-triazine-2,4-diamino, H_5C_3N_5 (6), 1,1',3,3',5,5'- triazine-2,2',4,4'-tetraamino, H_8C_6N_(10) (7), 2[H_6C_3N_6]·[H_(10)C_6N_(11)]~+·[SCN]~- (8) and 2[H_6C_3N_6]·[H_7C_3N_6]~+·[SCN]~- (9). Finally, a recrystallized decomposition product was found to be [H_6C_3N_6]·[H_7C_3N_6]~+·[SCN]~-·[H_2O] (10).

机译：碳氮化物材料包括功能材料，其化学多样性和复杂性变得越来越欣赏。 NH_4SCN的加热导致一系列新的碳氮化物化合物，其通过单晶X射线衍射进行了结构形式。在环境压力下加热至175℃，导致硫氰酸胍，H_6CN_3SCN（1），并且在保持该温度下形成约12个水不溶性碳氮化物产物，这是三聚氰胺和蛋白氰酸酯之间的共晶，[H_6C_3N_6 ]·[H_（10）C_6N_（11）]〜+·[SCN]〜 - （2）。本材料的原位粉末X射线衍射测量揭示了通过两种中间产物的（2），通过两个中间产物转化为最终的甜瓜的最终产物。其中的第一种形式在350至400°C之间，是素质和硫代氰酸酯的加合物，[H_9C_6N_（11）]·2 [H_（10）C_6N_（11）]〜+·2 [SCN]〜 - （ 3）。在400至480°C之间的第二种形式，并被鉴定为Melem，2,5,8- Triamino-Tri-S-Tri zine，H_6C_6N_（10）（4）。在将密封安瓿中的加热（2）加热至600℃，获得各种晶体，并从批次中测定六个晶体结构：1,3,5-三嗪-2,4,6- Triaminino，H_6C_3N_6（5）， 1,3,5-三嗪-2,4-二氨基，H_5C_3N_5（6），1,1'，3,3'，5,5'-三嗪-2,2'，4,4'-Tetraamino，H_8C_6N_（ 10）（7），2 [H_6C_3N_6]·[H_（10）C_6N_（11）]〜+·[SCN]〜 - （8）和2 [H_6C_3N_6]·[H_7C_3N_6]〜+·[SCN]〜 - （ 9）。最后，发现重结晶分解产物是[H_6C_3N_6]·[H_7C_3N_6]〜+·[SCN]〜 - ·[H_2O]（10）。

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《Acta Crystallographica, Section B. Structural science, crystal engineering and materials》 |2019年第4期|共13页
作者
Finn Krebs Larsen; Aref Hasen Mamakhel; Jacob Overgaard; Jens-Erik J?rgensen; Kenichi Kato; Bo Brummerstedt Iversen;
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作者单位

Department of Chemistry University of Aarhus Langelandsgade 140 Aarhus DK-8000 Denmark;

Department of Chemistry University of Aarhus Langelandsgade 140 Aarhus DK-8000 Denmark;

Department of Chemistry University of Aarhus Langelandsgade 140 Aarhus DK-8000 Denmark;

Department of Chemistry University of Aarhus Langelandsgade 140 Aarhus DK-8000 Denmark;

Structural Materials Science Laboratory RIKEN SPring-8 Center 1-1-1 Kouto Sayo-cho Sayo-gun Hyogo 679-5148 Japan.;

Department of Chemistry University of Aarhus Langelandsgade 140 Aarhus DK-8000 Denmark;

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正文语种 eng
中图分类晶体学;
关键词
carbon nitride compounds; 2D materials; crystal structure; ammonium thiocyanate decomposition;

机译：碳氮化物化合物;2D材料;晶体结构;硫氰酸铵分解;

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专利

1. Accessing the rich carbon nitride materials chemistry by heat treatments of ammonium thiocyanate, NH_4SCN [J] . Finn Krebs Larsen, Aref Hasen Mamakhel, Jacob Overgaard, Acta Crystallographica, Section B. Structural science, crystal engineering and materials . 2019,第4期

机译：通过热处理硫氰酸铵，NH_4SCN的热处理进入富碳氮化物材料化学
2. Synthesis of bulk and nanoporous carbon nitride polymers from ammonium thiocyanate for photocatalytic hydrogen evolution [J] . Yanjuan Cui, Jinshui Zhang, Guigang Zhang Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology . 2011,第34期

机译：由硫氰酸铵合成本体和纳米孔氮化碳聚合物用于光催化制氢
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机译：通过空气中热液碳的低温热处理来简单处理富含羧基的材料
4. High-pressure chemistry of carbon nitride materials [C] . Andrew J. Stevens, Carl B. Agree, Charles M. Lieber, Symposium on high-pressure materials research . 1998

机译：碳氮化物质的高压化学
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机译：纳米碳材料的化学：单壁碳纳米管的气相纯化，陨石碳中纳米碳氮化物和纳米金刚石的合成以及相关的金刚石表面化学。
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机译：海洋废弃物中的多孔富氮碳质材料：壳聚糖衍生的氮化碳催化剂用于将5-羟甲基糠醛（HMF）空气氧化为25-呋喃二甲酸
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机译：（183）压力下氨和碳迟缓之间的反应。 II。理论治疗硫氰酸铵的形成。
8. Investigation of Nitrogen-Rich Carbon Nitride Networks as Redox-Active Metal Catalyst Support Materials. [R] . Gillan, E., Leddy, J., Miller, D., 2004

机译：富氮碳氮化物网络作为氧化还原活性金属催化剂载体材料的研究。

Accessing the rich carbon nitride materials chemistry by heat treatments of ammonium thiocyanate, NH_4SCN

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