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基于碳纳米管的电催化剂在常温常压下从水和氮气中电化学合成氨。

Electrocatalytic Synthesis of Ammonia at Room Temperature and Atmospheric Pressure from Water and Nitrogen on a Carbon-Nanotube-Based Electrocatalyst.

机构信息

Depts. MIFT and ChimBioFarAM (Industrial Chemistry), University of Messina, ERIC aisbl and INSTM/CASPE, V.le F. Stagno D'Alcontres 31, 98166, Messina, Italy.

Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, 116023, Dalian, China.

出版信息

Angew Chem Int Ed Engl. 2017 Mar 1;56(10):2699-2703. doi: 10.1002/anie.201609533. Epub 2017 Jan 27.

DOI:10.1002/anie.201609533
PMID:28128489
Abstract

Ammonia is synthesized directly from water and N at room temperature and atmospheric pressure in a flow electrochemical cell operating in gas phase (half-cell for the NH synthesis). Iron supported on carbon nanotubes (CNTs) was used as the electrocatalyst in this half-cell. A rate of ammonia formation of 2.2×10  gNH3  m  h was obtained at room temperature and atmospheric pressure in a flow of N , with stable behavior for at least 60 h of reaction, under an applied potential of -2.0 V. This value is higher than the rate of ammonia formation obtained using noble metals (Ru/C) under comparable reaction conditions. Furthermore, hydrogen gas with a total Faraday efficiency as high as 95.1 % was obtained. Data also indicate that the active sites in NH electrocatalytic synthesis may be associated to specific carbon sites formed at the interface between iron particles and CNT and able to activate N , making it more reactive towards hydrogenation.

摘要

氨可以在室温、常压下,于气相中在流动电化学池中直接由水和氮气合成(用于氨合成的半电池)。在该半电池中,负载在碳纳米管(CNT)上的铁被用作电催化剂。在施加-2.0 V 电压、氮气流速为的条件下,氨的形成速率可达 2.2×10  gNH3  m  h,在至少 60 h 的反应时间内表现出稳定的行为。该值高于在可比反应条件下使用贵金属(Ru/C)获得的氨形成速率。此外,还获得了总法拉第效率高达 95.1%的氢气。数据还表明,NH 电催化合成的活性位点可能与铁颗粒和 CNT 之间界面处形成的特定碳位点有关,这些碳位点能够活化 N,使其更易与氢气发生氢化反应。

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