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Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-01-18 , DOI: 10.1002/anie.201811728 Lili Han 1, 2 , Xijun Liu 1 , Jinping Chen 1 , Ruoqian Lin 2 , Haoxuan Liu 1 , Fang Lü 1 , Seongmin Bak 3 , Zhixiu Liang 3 , Shunzheng Zhao 4 , Eli Stavitski 5 , Jun Luo 1 , Radoslav R. Adzic 3 , Huolin L. Xin 6
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-01-18 , DOI: 10.1002/anie.201811728 Lili Han 1, 2 , Xijun Liu 1 , Jinping Chen 1 , Ruoqian Lin 2 , Haoxuan Liu 1 , Fang Lü 1 , Seongmin Bak 3 , Zhixiu Liang 3 , Shunzheng Zhao 4 , Eli Stavitski 5 , Jun Luo 1 , Radoslav R. Adzic 3 , Huolin L. Xin 6
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NH3 synthesis by the electrocatalytic N2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen‐doped porous carbon as a cost‐effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH3 yield rate (34.0±3.6 μg
h−1 mgcat.−1) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non‐precious‐metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single‐atom non‐precious‐metal catalysts for the electrocatalytic NRR.
中文翻译：
原子分散钼催化剂用于高效固氮
在环境条件下通过电催化N 2还原反应（NRR）合成NH 3是目前需要高温和高压的工业方法Haber-Bosch工艺的一种有吸引力的替代方法。我们报道了固定在氮掺杂多孔碳上的单个Mo原子，是一种具有成本效益的NRR催化剂。从活性位点和分级多孔碳框架的最佳高密度受益，该催化剂实现了高的NH 3收率（34.0±3.6微克ħ -1 毫克猫。-1），并在高法拉第效率（14.6±1.6％） 0.1 米室温下KOH。与先前报道的非贵金属电催化剂相比，这些值要高得多。此外，该催化剂在50 000 s的NRR期间没有显示出明显的电流下降，并且在0.1 m HCl中实现了高活性和耐久性 。这些发现为设计用于电催化NRR的高效，耐用的单原子非贵金属催化剂提供了有希望的线索。
更新日期：2019-01-18
h−1 mgcat.−1) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non‐precious‐metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single‐atom non‐precious‐metal catalysts for the electrocatalytic NRR.
中文翻译：
原子分散钼催化剂用于高效固氮
在环境条件下通过电催化N 2还原反应（NRR）合成NH 3是目前需要高温和高压的工业方法Haber-Bosch工艺的一种有吸引力的替代方法。我们报道了固定在氮掺杂多孔碳上的单个Mo原子，是一种具有成本效益的NRR催化剂。从活性位点和分级多孔碳框架的最佳高密度受益，该催化剂实现了高的NH 3收率（34.0±3.6微克ħ -1 毫克猫。-1），并在高法拉第效率（14.6±1.6％） 0.1 米
室温下KOH。与先前报道的非贵金属电催化剂相比，这些值要高得多。此外，该催化剂在50 000 s的NRR期间没有显示出明显的电流下降，并且在0.1 m HCl中实现了高活性和耐久性 。这些发现为设计用于电催化NRR的高效，耐用的单原子非贵金属催化剂提供了有希望的线索。
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