2022年2月,国仪量子推出了“国仪量子EPR用户奖励政策”
最高奖励8000元!
截至目前,国仪量子的EPR产品已助力27项高水平研究成果发表
2023年,奖励政策将继续施行
欢迎各位老师同学积极参与!
Vanadium-Catalyzed Dinitrogen Reduction to Ammonia via a [V]═NNH2 Intermediate.Journal of the American Chemical Society(2023)
摘要
地球大气中含有丰富的N2(78%),但由于其化学惰性,氮气的活化和转化一直是一项具有挑战性的任务。合成氨工业中使用高温高压条件将N2和H2在固体催化剂表面转化为NH3。在环境条件下,某些微生物可以通过基于Fe(Mo/V)的固氮酶与N2结合并转化为NH3,尽管在固氮酶的结构和中间体方面取得了巨大进展,但N2与活性位点结合的性质和N2还原的详细机制仍不确定。
为了更好地理解反应机理并开发温和条件下氨合成催化剂,已经开展关于用过渡金属配合物活化N2的各种研究。但是目前为止,过渡金属配合物对N2到NH3的催化转化仍是一个挑战。尽管钒在生物固氮中起着至关重要的作用,但能够催化N2转化为NH3的明确钒络合物却很少。特别是,从配位N2的质子/电子转移反应中得到的V(NxHy)中间物仍然是未知的。在此,本文报道了钒金属配合物催化氮气还原为氨气,并首次从氮气活化体系分离和表征了中性酰肼配合物中间体([V]=NNH2),通过还原质子化钒的氨基配合物([V]-NH2)得到双氮化合物并释放氨气模拟了循环转化过程,结合理论计算阐明了在该催化体系中氮气可能经过端位反应途径(distal pathway)转化为氨气,这些发现为与FeV固氮酶有关的N2还原机制提供了前所未有的见解。
北京师范大学胡少伟课题组致力于发展过渡金属配合物活化惰性小分子的研究,近日与崔刚龙教授课题组合作,通过理论计算和实验研究相结合的方式报道了钒金属配合物催化氮气还原为氨气。相关研究结果发表在Journal of the American Chemical Society,黄文双(硕士研究生)和彭灵雅(博士研究生)为本文的共同第一作者,分别从事实验和理论计算的相关工作,该研究也得到了北京师范大学方维海院士、北京林业大学宋国勇教授和中国科学技术大学苏吉虎教授的大力支持。
钒金属配合物催化剂合成
EPR
配合物5b固氮反应机理图
结论
研究结果表明,带有POCOP和芳氧基辅助配体的过渡金属钒配合物可稳定活性含氮物种(NHy)并促进N2到NH3的催化转化,从而为生物固氮机理,特别是为FeV固氮酶有关的N2还原机制提供了更多的视角,为设计出更为高效的合成氨催化剂提供了新的思路。
1.Vanadium-Catalyzed Dinitrogen Reduction to Ammonia via a [V]═NNH2 Intermediate.Journal of the American Chemical Society(2023)
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22.Interfacial chemical behaviors and petroleum hydrocarbon removal performances of the biochar-mineral composites prepared by one-step pyrolysis. Colloids and Surfaces A: Physicochemical and Engineering Aspects (2022)
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1.IF < 3.0(影响因子取最近的影响因子)的SCI、EI期刊,每篇奖励200元现金;
2.3.0≤IF<6的SCI期刊,每篇奖励500元现金;
3.6.0≤IF<10的SCI期刊,每篇奖励1000元现金;
4.IF≥10的SCI期刊,每篇奖励2000元现金;
5.如论文发表于Nature、Science或Cell期刊,每篇奖励 8000元现金。
提及国仪量子仪器型号的方法:
要求在实验方法中提及仪器品牌型号:国仪量子EPR200-Plus,国仪量子EPR200M等,英文参考如下:
Electron paramagnetic resonance spectroscopy spectra were measured on CIQTEK EPR200-Plus with continues-wave X band frequency.
奖励申请说明:
1.奖励后我司内部备注,每篇文章原则上只奖励一次;
2.作品获得奖励后,即默认为作者授权主办方可以使用作者名及成果名称进行宣传推广活动,包括但不限于媒体宣传、现场展示、网络推广等;
3.本政策有效期截至2023年12月31日(如有变化会另行通知);
4.本奖励政策最终解释权归国仪量子(合肥)技术有限公司所有。
近年来,国家大力支持国产高端科学仪器发展,推进高水平科技成果自立自强,国产高端科学仪器迎来了长足进步。
国仪量子电子顺磁共振波谱仪为直接检测顺磁性物质提供了一种非破坏性的分析方法。可研究磁性分子、过渡金属离子、稀土离子、离子团簇、掺杂材料、缺陷材料、自由基、金属蛋白等含有未成对电子物质的组成、结构以及动力学等信息,能够提供原位和无损的电子自旋、轨道和原子核等微观尺度的信息。在物理、化学、生物、材料、工业等领域具有广泛的应用。
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