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一种用于双功能电化学固氮的Janus铁-氧化锡催化剂。

A Janus Fe-SnO Catalyst that Enables Bifunctional Electrochemical Nitrogen Fixation.

作者信息

Zhang Linlin, Cong Meiyu, Ding Xin, Jin Yu, Xu Fanfan, Wang Yong, Chen Lin, Zhang Lixue

机构信息

College of Chemistry and Chemical Engineering, Institution Qingdao University, Qingdao, 266071, Shandong, P. R. China.

State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian, 116024, Liaoning, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2020 Jun 26;59(27):10888-10893. doi: 10.1002/anie.202003518. Epub 2020 May 8.

Abstract

Electrochemical N reduction reactions (NRR) and the N oxidation reaction (NOR), using H O and N , are a sustainable approach to N fixation. To date, owing to the chemical inertness of nitrogen, emerging electrocatalysts for the electrochemical NRR and NOR at room temperature and atmospheric pressure remain largely underexplored. Herein, a new-type Fe-SnO was designed as a Janus electrocatalyst for achieving highly efficient NRR and NOR catalysis. A high NH yield of 82.7 μg h  mg and a Faraday efficiency (FE) of 20.4 % were obtained for NRR. This catalyst can also serve as an excellent NOR electrocatalyst with a NO yields of 42.9 μg h  mg and a FE of 0.84 %. By means of experiments and DFT calculations, it is revealed that the oxygen vacancy-anchored single-atom Fe can effectively adsorb and activate chemical inert N molecules, lowering the energy barrier for the vital breakage of N≡N and resulting in the enhanced N fixation performance.

摘要

利用H₂O和N₂进行的电化学氮还原反应(NRR)和氮氧化反应(NOR)是一种可持续的固氮方法。迄今为止,由于氮气的化学惰性,用于室温常压下电化学NRR和NOR的新型电催化剂在很大程度上仍未得到充分探索。在此,设计了一种新型的Fe-SnO₂作为双功能电催化剂,以实现高效的NRR和NOR催化。NRR获得了82.7 μg h⁻¹ mg⁻¹的高NH₃产率和20.4%的法拉第效率(FE)。该催化剂还可以作为一种优异的NOR电催化剂,NO₃⁻产率为42.9 μg h⁻¹ mg⁻¹,FE为0.84%。通过实验和密度泛函理论(DFT)计算表明,氧空位锚定的单原子Fe可以有效吸附和活化化学惰性的N₂分子,降低N≡N键断裂的能垒,从而提高固氮性能。

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