Renewable electricity shows immense potential as a driving force for the carbon dioxide reduction reaction (CO2RR) in production of formate (HCOO‐) at industrial current density, providing a promising path for value‐added chemicals and chemical manufacturing. However, achieving high selectivity and stable production of HCOO‐ at industrial current density remains a challenge. Here, we present a robust Bi0.6Cu0.4 NSs catalyst capable of regenerating necessary catalytic core (Bi‐O) through cyclic voltammetry (CV) treatment. Notably, at 260 mA cm‐2, faradaic efficiency of HCOO‐ reaches an exceptional selectivity to 99.23%, maintaining above 90% even after 400h, which is longest reaction time reported at industrial current density. Furthermore, in stability test, the catalyst was constructed by CV reconstruction to achieve stable and efficient production of HCOO‐. In 20h reaction test, the catalyst has a rate of HCOO‐ production of 13.24mmol m‐2 s‐1, a HCOO‐ concentration of 1.91mol L‐1, and an energy consumption of 129.80kWh kmol‐1. In‐situ Raman spectroscopy reveals the formation of Bi‐O structure during the gradual transformation of catalyst from Bi0.6Cu0.4 NBs to Bi0.6Cu0.4 NSs. Theoretical studies highlight the pivotal role of Bi‐O structure in modifying the adsorption behavior of reaction intermediates, which further reduces energy barrier for *OCHO conversion in CO2RR.

中文翻译：

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一种可再生双基催化剂，可在工业电流密度下高效稳定地电化学二氧化碳还原生成甲酸盐


可再生电力作为工业电流密度下甲酸（HCOO-）生产中二氧化碳还原反应（CO2RR）的驱动力显示出巨大的潜力，为增值化学品和化学品制造提供了一条有前途的道路。然而，在工业电流密度下实现HCOO-的高选择性和稳定生产仍然是一个挑战。在这里，我们提出了一种坚固的 Bi0.6Cu0.4 NSs 催化剂，能够通过循环伏安法 (CV) 处理再生必要的催化核心 (Bi-O)。值得注意的是，在 260 mA cm-2 下，HCOO- 的法拉第效率达到了 99.23% 的优异选择性，即使在 400 小时后仍保持在 90% 以上，这是工业电流密度下报道的最长反应时间。此外，在稳定性测试中，通过CV重构构建催化剂，实现HCOO-的稳定高效生产。 20h反应测试中，催化剂HCOO-生成率为13.24mmol m-2 s-1，HCOO-浓度为1.91mol·L-1，能耗为129.80kWh kmol-1。原位拉曼光谱揭示了催化剂从 Bi0.6Cu0.4 NBs 逐渐转变为 Bi0.6Cu0.4 NSs 过程中 Bi-O 结构的形成。理论研究强调了 Bi-O 结构在改变反应中间体吸附行为中的关键作用，这进一步降低了 CO2RR 中*OCHO 转化的能垒。