多价MnOx/C电催化剂用于高效氮还原反应

doi:10.11944/j.issn.1000-0518.2020.09.200085

摘要/Abstract

摘要： 氨在人类的生产生活中起着重要的作用,但目前工业上合成氨广泛采用的Haber-Bosch法耗能大,且污染严重。而N₂电还原反应(ENRR)被认为是一种有效的替代方法,由于N₂的键能较高,目前仍然缺乏高活性的催化剂。在这里,通过简单的浸渍法和氧化还原法制备了多价态的MnO_x/C催化剂,该催化剂具有较高的氮还原反应活性(氨产率达到7.8 μg_NH₃/(h·mg_cat),法拉第效率高达9.2%) 。进一步研究表明,多价态MnO_x/C催化剂具有高氮还原反应活性的主要原因是不同价态的Mn离子(Mn²⁺、Mn³⁺、Mn⁴⁺)之间存在协同效应。

关键词: 合成氨, 电催化, 过渡金属氧化物, 协同效应

Abstract: NH₃ plays an important role in human production and life, but the main way to produce NH₃ is still the high energy consumption and high pollution Haber-Bosch process. Electrocatalytic N₂ reduction reaction (ENRR) is considered to be an effective alternative method, however highly efficient catalyst is still a challenging as a result of high bond energy of NN. Here, we report an electrocatalyst of polyvalent MnO_x/C which is designed via simple redox reaction for highly efficient production of ammonia (with yield up to 7.8 μg_NH₃/(h·mg_cat) and Faradic efficiency (FE) up to 9.2%) from nitrogen reduction reaction (NRR). The high NRR performance of polyvalent MnO_x/C mainly originates from a synergistic effect among different valence states (Mn²⁺, Mn³⁺, Mn⁴⁺) of Mn for NRR.

Key words: ammonia synthesis, electrocatalysis, transition metal oxide, synergistic effect

毕一飘, 宫雪, 杨发, 阮明波, 宋平, 徐维林. 多价MnO_x/C电催化剂用于高效氮还原反应[J]. 应用化学, 2020, 37(9): 1048-1055.

BI Yipiao, GONG Xue, YANG Fa, RUAN Mingbo, SONG Ping, XU Weilin. Polyvalent MnO_x/C Electrocatalyst for Highly Efficient Nitrogen Reduction Reaction[J]. Chinese Journal of Applied Chemistry, 2020, 37(9): 1048-1055.

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