The electrochemical CO₂ reduction reaction (CO₂RR) to value-added and readily collectable liquid products is promising but remains a great challenge due to the lack of efficient and robust electrocatalysts. Herein, a self-supported large-size three-dimensional porous conductive network of bismuthene (Bi-ene-NW) as an efficient superstructured electrocatalytic membrane (ECM) has been pioneeringly assembled, in which the atomically thin Bi-ene with rich edge-site-involved defects is interconnected, highly exposing the active sites. Such ECM can be utilized as an ascendant catalytic cathode, displaying an unprecedented CO₂RR performance with near-unity selectivity in a wide potential window and large current density for formate production. Remarkably, when integrated into a gas diffusion electrode (GDE) in a flow cell, Bi-ene-NW was capable of delivering industry-compatible current densities up to 560 mA cm⁻² for formate production. Moreover, it was ultrastable to continuously operate for over 500 h at a high current density without significant activity decay. Such outstanding performance should be inseparable from its abundant accessible sites with high intrinsic activity, multiple interconnected channels and superior conductivity for mass/charge transport. The operando ATR-IR and theoretical calculations further deciphered that the rich defects in the roughened plane edges and in-plane pore edges of Bi-ene are conducive to the *OCHO intermediate stabilization.

中文翻译：

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设计具有丰富缺陷的原子级薄铋的导电网络，使 CO2 还原以具有工业兼容的电流密度和稳定性

电化学 CO ₂还原反应 (CO ₂ RR) 转化为具有附加值且易于收集的液体产品是有前景的，但由于缺乏高效且稳定的电催化剂，这仍然是一个巨大的挑战。在此，首次组装了一种自支撑大尺寸铋烯（Bi-ene-NW）作为高效超结构电催化膜（ECM）的三维多孔导电网络，其中原子级薄的 Bi-ene 具有丰富的边缘-位点相关缺陷是相互关联的，高度暴露了活性位点。这种 ECM 可以用作上升的催化阴极，显示出前所未有的 CO ₂RR 性能在广泛的电位窗口中具有接近统一的选择性和用于甲酸盐生产的大电流密度。值得注意的是，当集成到流通池中的气体扩散电极 (GDE) 中时，Bi-ene-NW 能够提供高达 560 mA cm ^{-2 的}行业兼容电流密度用于甲酸盐生产。此外，它在高电流密度下连续运行 500 小时以上是超稳定的，而没有显着的活性衰减。如此出色的性能与其丰富的可访问位点、高内在活性、多个互连通道和优异的质量/电荷传输导电性密不可分。操作数ATR-IR和理论计算进一步破译了Bi-ene粗糙面边缘和面内孔边缘中的丰富缺陷有利于*OCHO中间稳定。