Nitric acid is an important commodity chemical in agriculture and industry, yet its conventional production through the Haber-Bosch and Ostwald processes is energy and carbon-emission intensive. An electrochemical nitrogen oxidation reaction (NOR) to produce nitrates shows great potential as an environmentally friendly method of producing fertilizers under mild conditions. Progress in this field requires fundamental mechanistic understanding and establishing robust experimental methods, which is essential for the efficient design and synthesis of electrocatalysts for the NOR. We present a synergistic computational and experimental approach to exploring NOR pathways on a PtO₂ catalyst to gain mechanistic insights into the NOR. This study marks the first attempt to perform the NOR in a vapor-fed reactor designed through advanced (additive) manufacturing. The vapor-fed reactor significantly improved the N₂ mass transport to the catalyst, allowing us to report the highest rate for nitrate production to date at $3.3\mu \text{mol}\mathrm{c}{\mathrm{m}}^{-2}{\mathrm{h}}^{-1}$$3.3\mu \text{mol}\mathrm{c}{\mathrm{m}}^{-2}{\mathrm{h}}^{-1}$ at 2.01 V vs. reversible hydrogen electrode (RHE).

中文翻译：

---

通过电化学氮氧化反应使氮肥生产脱碳


硝酸是农业和工业中一种重要的商品化学品，但其通过 Haber-Bosch 和 Ostwald 工艺进行的传统生产是能源和碳排放密集型的。产生硝酸盐的电化学氮氧化反应 （NOR） 作为一种在温和条件下生产肥料的环保方法显示出巨大的潜力。该领域的进步需要基本的机理理解和建立稳健的实验方法，这对于 NOR 电催化剂的高效设计和合成至关重要。我们提出了一种协同计算和实验方法来探索 PtO ₂ 催化剂上的 NOR 途径，以获得对 NOR 的机理见解。这项研究标志着首次尝试在通过先进（增材）制造设计的蒸汽进料反应器中执行 NOR。蒸汽进料反应器显著改善了向催化剂的氮 ₂ 质量传递，使我们能够报告迄今为止在 2.01 V $3.3\mu \text{mol}\mathrm{c}{\mathrm{m}}^{-2}{\mathrm{h}}^{-1}$ 下与可逆氢电极 （RHE） 相比的最高硝酸盐生成速率。