School of Materials and Energy , University of Electronic Science and Technology of China , Chengdu 611731 , Sichuan , China.
Henan Joint International Research Laboratory of Environmental Pollution Control Materials, College of Chemistry and Chemical Engineering , Henan University , Kaifeng 475004 , Henan , China.
ACS Appl Mater Interfaces. 2019 Oct 2;11(39):35764-35769. doi: 10.1021/acsami.9b12675. Epub 2019 Sep 20.
Industrial production of NH heavily depends on the conventional Haber-Bosch process under rigorous conditions with a large amount of energy consumption and carbon emissions. Electrocatalysis exhibits an intriguing prospect for the N reduction reaction (NRR) at ambient conditions. In this case, a high-efficiency and low-cost catalyst is paramount. In this letter, CrC nanoparticles and carbon nanofiber composite (CrC@CNF) are proposed as a noble-metal-free NRR electrocatalyst for converting N to NH with an excellent selectivity. The optimal Faradic efficiency and NH yield rate achieved are as high as 8.6% and 23.9 μg h mg at -0.3 V vs reversible hydrogen electrode in 0.1 M HCl, respectively. Theoretical calculations show a low reaction barrier of merely 0.53 eV in the enzymatic route for this catalyst.
工业生产 NH 严重依赖于常规 Haber-Bosch 工艺，该工艺在严格的条件下进行，需要大量的能源消耗和碳排放。电催化在环境条件下的氮还原反应 (NRR) 表现出了引人入胜的前景。在这种情况下，高效、低成本的催化剂至关重要。在这封信中，我们提出了 CrC 纳米颗粒和碳纤维复合材料 (CrC@CNF) 作为一种无贵金属的 NRR 电催化剂，可将 N 高效且选择性地转化为 NH。在 0.1 M HCl 中，在 -0.3 V 相对于可逆氢电极的最优法拉第效率和 NH 产率分别高达 8.6%和 23.9 μg h mg。理论计算表明，对于这种催化剂，酶途径的反应势垒仅为 0.53 eV。
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