Ammonia Synthesis via an Associative Mechanism on Alkali Earth Metal Sites of Ca3CrN3H
Ammonia Synthesis via an Associative Mechanism on Alkali Earth Metal Sites of Ca3CrN3H
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Ca3CrN3H 碱土金属位点上缔合机制合成氨
DOI：
10.1002/cssc.202300234
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发表时间：
2023
期刊：
影响因子：
8.4
通讯作者：
Kobayashi Yoji
中科院分区：
文献类型：
--
作者：
Cao Yu;Toshcheva Ekaterina;Almaksoud Walid;Ahmad Rafia;Tsumori Tatsuya;Rai Rohit;Tang Ya;Cavallo Luigi;Kageyama Hiroshi;Kobayashi Yoji
通常，过渡金属被认为是二氮活化的中心。在这里，我们证明了氮氢化物Ca3CrN3H具有强大的氨合成活性，可以通过钙提供初级配位环境的活性位点激活二氮。DFT计算还表明，与传统的Ru或Fe催化剂的解离机制不同，缔合机制是有利的。这项工作显示了碱土金属氢化物催化剂和其他相关的一维氢化物/电极在氨合成中的潜力。
Typically, transition metals are considered as the centers for the activation of dinitrogen. Here we demonstrate that the nitride hydride compound Ca3CrN3H, with robust ammonia synthesis activity, can activate dinitrogen through active sites where calcium provides the primary coordination environment. DFT calculations also reveal that an associative mechanism is favorable, distinct from the dissociative mechanism found in traditional Ru or Fe catalysts. This work shows the potential of alkaline earth metal hydride catalysts and other related 1 D hydride/electrides for ammonia synthesis.