Electrocatalytic reduction reaction of CO2 (CO2RR) is an effective way to mitigate energy and environmental issues. However, very limited catalysts are capable of converting CO2 resources into high-value products such as hydrocarbons or alcohols. Herein, we firstly propose a facile strategy to the large-scale synthesis of isolated Cu decorated through-hole carbon nanofibers (CuSAs/TCNFs). This CuSAs/TCNFs membrane has excellent mechanical properties and can be directly used as cathode for CO2RR, which could generate nearly pure methanol with 44% Faradaic efficiency in liquid phase. The self-supporting and through-hole structure of CuSAs/TCNFs greatly reduces the embed metal atoms and produce abundant efficient Cu single at-oms, which could actually participate in CO2RR, eventually causing -93 mA cm-2 partial current density for C1 products and more than 50 h stability in aqueous solution. According to DFT calculations, Cu single atoms possess a relatively higher bind-ing energy for *CO intermediate. Therefore, *CO could be further reduced to products like methanol, instead of being easily released from the catalyst surface as CO product. This report may benefit the design of efficient and high-yield single-atom cat-alysts for other electrocatalytic reaction.

中文翻译：

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用于 CO2 电还原为甲醇的高效单原子铜装饰碳膜的可扩展生产

CO2 的电催化还原反应 (CO2RR) 是缓解能源和环境问题的有效方法。然而，能够将 CO2 资源转化为高价值产品（如碳氢化合物或醇类）的催化剂非常有限。在此，我们首先提出了一种大规模合成孤立的铜装饰通孔碳纳米纤维（CuSAs/TCNFs）的简便策略。这种 CuSAs/TCNFs 膜具有优异的机械性能，可直接用作 CO2RR 的阴极，可在液相中以 44% 的法拉第效率生成近乎纯的甲醇。CuSAs/TCNFs 的自支撑和通孔结构大大减少了嵌入的金属原子并产生了大量有效的 Cu 单原子，这些原子实际上可以参与 CO2RR，最终导致 C1 产物的局部电流密度为 -93 mA cm-2，并且在水溶液中具有超过 50 小时的稳定性。根据 DFT 计算，Cu 单原子对 *CO 中间体具有相对较高的结合能。因此，*CO 可以进一步还原为甲醇等产物，而不是作为 CO 产物轻易从催化剂表面释放。该报告可能有助于设计用于其他电催化反应的高效和高产单原子催化剂。