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Co-Doped Fe3S4 Nanoflowers for Boosting Electrocatalytic Nitrogen Fixation to Ammonia under Mild Conditions
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-11-28 , DOI: 10.1021/acs.inorgchem.2c03578 Xue Chen 1 , Hongfei Yin 1 , Xiaoyong Yang 2, 3 , Weining Zhang 1 , Dongdong Xiao 4 , Zhen Lu 4 , Yongzheng Zhang 1 , Ping Zhang 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-11-28 , DOI: 10.1021/acs.inorgchem.2c03578 Xue Chen 1 , Hongfei Yin 1 , Xiaoyong Yang 2, 3 , Weining Zhang 1 , Dongdong Xiao 4 , Zhen Lu 4 , Yongzheng Zhang 1 , Ping Zhang 1
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Compared with the Haber Bosch process, the electrochemical nitrogen reduction reaction (NRR) under mild conditions provides an alternative and promising route for ammonia synthesis due to its green and sustainable features. However, the great energy barrier to break the stable N≡N bond hinders the practical application of NRR. Though Fe is the only common metal element in all biological nitrogenases in nature, there is still a lack of study on developing highly efficient and low-cost Fe-based catalysts for N2 fixation. Herein, Co-doped Fe3S4 nanoflowers were fabricated as the intended catalyst for NRR. The results indicate that 4% Co-doped Fe3S4 nanoflowers achieve a high Faradaic efficiency of 17% and a NH3 yield rate of 37.5 μg·h–1·mg–1cat. at −0.55 V versus RHE potential in 0.1 M HCl, which is superior to most Fe-based catalysts. The introduction of Co atoms can not only shift the partial density states of Fe3S4 toward the Fermi level but also serve as new active centers to promote N2 absorption, lowering the energy barrier of the potential determination step to accelerate the catalytic process. This work paves a pathway of the morphology and doping engineering for Fe-based electrocatalysts to enhance ammonia synthesis.
中文翻译：
共掺杂 Fe3S4 纳米花促进温和条件下电催化固氮
与 Haber Bosch 工艺相比，温和条件下的电化学氮还原反应 (NRR) 因其绿色和可持续的特点为合成氨提供了一条替代和有前景的途径。然而，打破稳定的N≡N键的巨大能垒阻碍了NRR的实际应用。尽管Fe是自然界所有生物固氮酶中唯一常见的金属元素，但目前仍缺乏开发高效低成本的Fe基固氮催化剂的研究。在此，制备了 Co 掺杂的 Fe 3 S 4纳米花作为 NRR 的预期催化剂。结果表明，4% Co 掺杂的 Fe 3 S 4纳米花实现了 17% 的高法拉第效率和 NH3产率为37.5 μg·h –1 ·mg –1 cat。在-0.55 V与0.1 M HCl 中的 RHE 电位相比，这优于大多数铁基催化剂。Co原子的引入不仅可以使Fe 3 S 4的偏密度态向费米能级移动，还可以作为新的活性中心促进N 2的吸收，降低电位测定步骤的能垒，加速催化过程。这项工作为铁基电催化剂的形貌和掺杂工程铺平了道路，以增强氨的合成。
更新日期：2022-11-28
中文翻译：
共掺杂 Fe3S4 纳米花促进温和条件下电催化固氮
与 Haber Bosch 工艺相比，温和条件下的电化学氮还原反应 (NRR) 因其绿色和可持续的特点为合成氨提供了一条替代和有前景的途径。然而，打破稳定的N≡N键的巨大能垒阻碍了NRR的实际应用。尽管Fe是自然界所有生物固氮酶中唯一常见的金属元素，但目前仍缺乏开发高效低成本的Fe基固氮催化剂的研究。在此，制备了 Co 掺杂的 Fe 3 S 4纳米花作为 NRR 的预期催化剂。结果表明，4% Co 掺杂的 Fe 3 S 4纳米花实现了 17% 的高法拉第效率和 NH3产率为37.5 μg·h –1 ·mg –1 cat。在-0.55 V与0.1 M HCl 中的 RHE 电位相比，这优于大多数铁基催化剂。Co原子的引入不仅可以使Fe 3 S 4的偏密度态向费米能级移动，还可以作为新的活性中心促进N 2的吸收，降低电位测定步骤的能垒，加速催化过程。这项工作为铁基电催化剂的形貌和掺杂工程铺平了道路，以增强氨的合成。
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