Efficient Nitrogen Fixation to Ammonia through Integration of Plasma Oxidation with Electrocatalytic Reduction
Efficient Nitrogen Fixation to Ammonia through Integration of Plasma Oxidation with Electrocatalytic Reduction
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DOI：
10.1002/anie.202104394
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发表时间：
2021-05-11
影响因子：
16.6
通讯作者：
Qiao, Shi-Zhang
中科院分区：
文献类型：
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作者：
Li, Laiquan;Tang, Cheng;Qiao, Shi-Zhang
目前的一步式 N-2 固定受到相当于 N 键的 N 的强活化和对 NH3 的低选择性的阻碍。在这里，我们报告N-2-到-NH3的固定可以分解为两步过程，每一步都有效解决一个问题，包括：1）通过非热等离子体技术轻松地将N-2活化为NOx-，以及2）通过电催化还原将NOx-高度选择性地转化为NH3。重要的是，该工艺使用空气和水作为低成本原材料，在环境条件下可大规模生产氨。为了将 NOx 还原为 NH3，我们提出了一种表面富硼核壳硼化镍电催化剂。表面富硼特征是通过增强NOx吸附、抑制析氢和表面镍氧化来提高活性、选择性和稳定性的关键。氨产量达到198.3 mu mol cm(-2) h(-1)，法拉第效率接近100%。
Present one-step N-2 fixation is impeded by tough activation of the N equivalent to N bond and low selectivity to NH3. Here we report fixation of N-2-to-NH3 can be decoupled to a two-step process with one problem effectively solved in each step, including: 1) facile activation of N-2 to NOx- by a non-thermal plasma technique, and 2) highly selective conversion of NOx- to NH3 by electrocatalytic reduction. Importantly, this process uses air and water as low-cost raw materials for scalable ammonia production under ambient conditions. For NOx- reduction to NH3, we present a surface boron-rich core-shell nickel boride electrocatalyst. The surface boron-rich feature is the key to boosting activity, selectivity, and stability via enhanced NOx- adsorption, and suppression of hydrogen evolution and surface Ni oxidation. A significant ammonia production of 198.3 mu mol cm(-2) h(-1) was achieved, together with nearly 100 % Faradaic efficiency.