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Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles

机译:在缺电子的铜纳米颗粒上促进选择性氮还原成氨

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摘要

Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N2 fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date. In this work, we boost the N2 reduction reaction catalytic activity of Cu nanoparticles, which originally exhibited negligible N2 reduction reaction activity, via a local electron depletion effect. The electron-deficient Cu nanoparticles are brought in a Schottky rectifying contact with a polyimide support which retards the hydrogen evolution reaction process in basic electrolytes and facilitates the electrochemical N2 reduction reaction process under ambient aqueous conditions. This strategy of inducing electron deficiency provides new insight into the rational design of inexpensive N2 reduction reaction catalysts with high selectivity and activity.
机译:目前,氨的生产是通过Haber-Bosch工艺实现的,而环境条件下的电化学N2固定被认为是在不久的将来有希望的绿色替代品。缺乏有效的电催化剂仍然是引发潜在的氨电催化合成的主要障碍。迄今为止,对于较便宜的金属,例如铜,进展有限。在这项工作中,我们通过局部电子耗竭效应提高了最初显示可忽略的N2还原反应活性的Cu纳米颗粒的N2还原反应催化活性。缺电子的Cu纳米颗粒与聚酰亚胺载体进行肖特基整流接触,这会延迟碱性电解质中的氢释放反应过程,并有助于在环境水性条件下进行电化学N2还原反应过程。这种诱导电子缺乏的策略为合理设计具有高选择性和活性的廉价N2还原反应催化剂提供了新的见识。

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