Electrocatalytic reduction of NO₂^– to NH₃ (NO₂RR) offers an effective method for alleviating NO₂^– pollution and generating valuable NH₃. Herein, a p-block single-atom alloy, namely, isolated Sb alloyed in a Cu substrate (Sb₁Cu), is explored as a durable and high-current-density NO₂RR catalyst. As revealed by the theoretical calculations and operando spectroscopic measurements, we demonstrate that Sb₁ incorporation can not only hamper the competing hydrogen evolution reaction but also optimize the d-band center of Sb₁Cu and intermediate adsorption energies to boost the protonation energetics of NO₂^–-to-NH₃ conversion. Consequently, Sb₁Cu integrated in a flow cell achieves an outstanding NH₃ yield rate of 2529.4 μmol h^–1 cm^–2 and FE_NH3 of 95.9% at a high current density of 424.2 mA cm^–2, as well as a high durability for 100 h of electrolysis.

中文翻译：

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用于选择性亚硝酸盐电还原制氨的 P 区锑-铜单原子合金

电催化还原NO ₂ ^-为NH ₃ (NO _{2 RR)为减轻NO 2} ^-污染和产生有价值的NH ₃提供了有效的方法。在此，p区单原子合金，即在Cu基底中合金化的孤立Sb (Sb ₁ Cu)，被探索作为耐用且高电流密度的NO ₂ RR催化剂。正如理论计算和操作光谱测量所揭示的那样，我们证明Sb _{1 的}掺入不仅可以阻碍竞争性析氢反应，还可以优化Sb _{1 Cu的d带中心和中间吸附能，以提高NO 2}的质子化能量。 ^–至-NH ₃转化。因此，集成在流通池中的Sb _{1 Cu 在 424.2 mA cm} ^–2的高电流密度下实现了 2529.4 μmol h ^–1 cm ^{–2的出色 NH} ₃产率和 95.9% 的 FE _NH3以及高耐用性电解100小时。