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Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots
Communications Chemistry ( IF 5.9 ) Pub Date : 2021-01-29 , DOI: 10.1038/s42004-021-00449-7
Wenyi Li 1, 2 , Ke Li 1 , Yixing Ye 1 , Shengbo Zhang 1 , Yanyan Liu 1, 2 , Guozhong Wang 1 , Changhao Liang 1 , Haimin Zhang 1 , Huijun Zhao 3
Affiliation  

The electrocatalytic nitrogen (N2) reduction reaction (NRR) relies on the development of highly efficient electrocatalysts and electrocatalysis systems. Herein, we report a non-loading electrocatalysis system, where the electrocatalysts are dispersed in aqueous solution rather than loading them on electrode substrates. The system consists of aqueous Ag nanodots (AgNDs) as the catalyst and metallic titanium (Ti) mesh as the current collector for electrocatalytic NRR. The as-synthesized AgNDs, homogeneously dispersed in 0.1 M Na2SO4 solution (pH = 10.5), can achieve an NH3 yield rate of 600.4 ± 23.0 μg h−1 mgAg−1 with a faradaic efficiency (FE) of 10.1 ± 0.7% at −0.25 V (vs. RHE). The FE can be further improved to be 20.1 ± 0.9% at the same potential by using Ti mesh modified with oxygen vacancy-rich TiO2 nanosheets as the current collector. Utilizing the aqueous AgNDs catalyst, a Ti plate based two-electrode configured flow-type electrochemical reactor was developed to achieve an NH3 yield rate of 804.5 ± 30.6 μg h−1 mgAg−1 with a FE of 8.2 ± 0.5% at a voltage of −1.8 V. The designed non-loading electrocatalysis system takes full advantage of the AgNDs’ active sites for N2 adsorption and activation, following an alternative hydrogenation mechanism revealed by theoretical calculations.



中文翻译:

使用含水银纳米点将氮高效电催化还原为氨

电催化氮(N 2)还原反应(NRR)依赖于高效电催化剂和电催化系统的发展。在此,我们报告了一种非负载电催化系统,其中电催化剂分散在水溶液中,而不是将它们负载在电极基板上。该系统由作为催化剂的水银纳米点 (AgNDs) 和作为电催化 NRR 集电器的金属钛 (Ti) 网组成。合成后的 AgNDs 均匀分散在 0.1 M Na 2 SO 4溶液(pH = 10.5)中,可实现 600.4 ± 23.0 μg h −1 mg Ag −1的 NH 3产率在 −0.25 V(相对于 RHE)时法拉第效率 (FE) 为 10.1 ± 0.7%。使用富含氧空位的TiO 2纳米片修饰的Ti网作为集流体,在相同电位下FE可以进一步提高到20.1±0.9% 。利用水性 AgNDs 催化剂,开发了基于 Ti 板的双电极配置流动型电化学反应器,在 a 下实现了804.5 ± 30.6 μg h -1 mg Ag −1的 NH 3产率和 8.2 ± 0.5% 的 FE。电压为-1.8 V。设计的非负载电催化系统充分利用AgNDs 的活性位点进行N 2吸附和活化,遵循理论计算揭示的替代加氢机制。

更新日期:2021-01-29
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