Developing high-performance electrocatalysts for CO₂ reduction reaction (CO₂RR) is vital in achieving a carbon-neutral society by converting CO₂ into valuable chemicals. CO₂RR electrocatalyst with lower overpotential, higher selectivity and wider working potential range is urgently desired, but it is still challenging to realize these factors simultaneously. Here, high-performance bismuthene-based electrocatalysts were synthesized by reducing bismuth precursors like BiCl₃, BiBr₃, and BiI₃ in liquid phases. Especially, bismuthene-I derived from BiI₃ showed a nanosheet morphology (around four-layer) with significantly enhanced (110) surfaces. It enabled an ultrawide potential window (0.7 V) for high formate selectivity (>90%) in a H-type cell and achieved an ultralow potential (−0.46 V vs. reversible hydrogen electrode) to attain a current density of 200 mA cm⁻² in a gas-diffusion flow cell. The prominent long-term operational capability of bismuthene-I was demonstrated in both H-type and gas-diffusion cells. Density functional theory calculations revealed that bismuthene-I possessed abundant topological Bi(110) surfaces states that can reduce the CO₂RR overpotential, suppress the competitive hydrogen evolution reaction, and facilitate electron donation during CO₂ electrocatalysis. The bismuthene-I realized low overpotential, high selectivity and wide working potential range simultaneously for electrochemical CO₂RR. This work unfolds the broader plausibility of facilely reducing precursors for the scalable fabrication of high-performing CO₂RR electrocatalysts.

中文翻译：

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卤化物前驱体还原策略以高选择性和宽电位窗口调节铋，用于电化学 CO2 还原

_{开发用于CO 2}还原反应（CO ₂ RR）的高性能电催化剂对于通过将CO ₂转化为有价值的化学品来实现碳中和社会至关重要。人们迫切需要具有更低过电位、更高选择性和更宽工作电位范围的CO ₂ RR电催化剂，但同时实现这些因素仍然具有挑战性。在此，通过在液相中还原BiCl ₃、BiBr ₃和BiI ₃等铋前体来合成高性能铋基电催化剂。特别是，源自 BiI ₃的 Bismuthene-I显示出具有显着增强的 (110) 表面的纳米片形态（大约四层）。它在H型电池中实现了超宽电位窗口（0.7 V）以实现高甲酸盐选择性（> 90％），并实现了超低电位（-0.46 V vs.可逆氢电极）以获得200 mA cm的电流密度^{- 2}在气体扩散流通池中。 Bismuthene-I 突出的长期运行能力在 H 型和气体扩散池中得到了证明。密度泛函理论计算表明，Bismuthene-I具有丰富的拓扑Bi(110)表面态，可以降低CO ₂ RR过电势，抑制竞争性析氢反应，并促进CO ₂电催化过程中的电子供给。 Bismuthene-I同时实现了电化学CO ₂ RR的低过电位、高选择性和宽工作电位范围。这项工作揭示了轻松还原前体以大规模制造高性能 CO ₂ RR 电催化剂的更广泛的可能性。