Favoring the unfavored: Selective electrochemical nitrogen fixation using a reticular chemistry approach.
Favoring the unfavored: Selective electrochemical nitrogen fixation using a reticular chemistry approach.
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DOI：
10.1126/sciadv.aar3208
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发表时间：
2018-03
期刊：
影响因子：
13.6
通讯作者：
Ling XY
中科院分区：
文献类型：
--
作者：
Lee HK;Koh CSL;Lee YH;Liu C;Phang IY;Han X;Tsung CK;Ling XY
最初不受欢迎的氮到氨的电转化现在优于使用网状化学的竞争反应。电化学固氮制氨是解决哈伯-博世工艺氨生产中氢和能源密集型操作的一种可持续策略。然而，目前的电化学氮还原反应（NRR）进展受到来自所有传统NRR催化剂的析氢反应（HER）的压倒性竞争和对升高的温度/压力的要求的阻碍。通过在NRR电催化剂上涂覆超疏水金属有机框架（MOF）层，我们实现了优异的NRR选择性（~90%）和法拉第效率的10个百分点的显著提高，即使在环境操作下也是如此。我们的网状化学方法利用MOF的斥水和分子浓缩效应来克服HER施加的瓶颈，揭示了NRR前所未有的电化学特征，这对未来的理论研究至关重要。通过支持最初不受欢迎的NRR，我们设想我们的电催化设计作为直接从水蒸气丰富的空气中进行高性能氮-氨电转化的起点，以解决（生物）化学和能源行业对氨日益增长的全球需求。
Originally unfavored nitrogen-to-ammonia electroconversion is now preferred over competing reaction using reticular chemistry. Electrochemical nitrogen-to-ammonia fixation is emerging as a sustainable strategy to tackle the hydrogen- and energy-intensive operations by Haber-Bosch process for ammonia production. However, current electrochemical nitrogen reduction reaction (NRR) progress is impeded by overwhelming competition from the hydrogen evolution reaction (HER) across all traditional NRR catalysts and the requirement for elevated temperature/pressure. We achieve both excellent NRR selectivity (~90%) and a significant boost to Faradic efficiency by 10 percentage points even at ambient operations by coating a superhydrophobic metal-organic framework (MOF) layer over the NRR electrocatalyst. Our reticular chemistry approach exploits MOF’s water-repelling and molecular-concentrating effects to overcome HER-imposed bottlenecks, uncovering the unprecedented electrochemical features of NRR critical for future theoretical studies. By favoring the originally unfavored NRR, we envisage our electrocatalytic design as a starting point for high-performance nitrogen-to-ammonia electroconversion directly from water vapor–abundant air to address increasing global demand of ammonia in (bio)chemical and energy industries.
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影响因子：
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作者：
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