Nanoscale defect engineering plays a crucial role in incorporating extraordinary catalytic properties in two-dimensional materials by varying the surface groups or site interactions. Herein, we synthesized high-loaded nitrogen-doped Boridene (N-Boridene (Mo_4/3(B_nN_1–n)_2–mT_z), N-doped concentration up to 26.78 at %) nanosheets by chemical exfoliation followed by cyanamide intercalation. Three different nitrogen sites are observed in N-Boridene, wherein the site of boron vacancy substitution mainly accounts for its high chemical activity. Attractively, as a cathode for Mg–CO₂ batteries, it delivers a long-term lifetime (305 cycles), high-energy efficiency (93.6%), and ultralow overpotential (∼0.09 V) at a high current of 200 mA g^–1, which overwhelms all Mg–CO₂ batteries reported so far. Experimental and computational studies suggest that N-Boridene can remarkably change the adsorption energy of the reaction products and lower the energy barrier of the rate-determining step (*MgCO₂ → *MgCO₃·xH₂O), resulting in the rapid reversible formation/decomposition of new MgCO₃·5H₂O products. The surging Boridene materials with defects provide substantial opportunities to develop other heterogeneous catalysts for efficient capture and converting of CO₂.

中文翻译：

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氮锚定硼化物使镁-二氧化碳电池具有高可逆性

纳米级缺陷工程通过改变表面基团或位点相互作用，在二维材料中融入非凡的催化性能方面发挥着至关重要的作用。在此，我们通过化学剥离合成了高负载氮掺杂硼化物（N-硼化物（Mo _4/3 (B _n N _{1– n} ) _{2– m} T _z），N掺杂浓度高达26.78 at%）纳米片，然后通过氰胺插层。 N-硼化烯中观察到三个不同的氮位点，其中硼空位取代位点主要是其高化学活性的原因。有吸引力的是，作为 Mg-CO ₂电池的阴极，它在 200 mA g-1 的高电流下具有长寿命（305 个循环）、高能效（93.6%）和超低过电势（∼0.09 V）^{– 1} ，压倒了迄今为止报道的所有Mg-CO ₂电池。实验和计算研究表明，N-硼化物可以显着改变反应产物的吸附能，降低限速步骤(*MgCO ₂ → *MgCO ₃ · x H ₂ O)的能垒，从而导致快速可逆反应。新MgCO ₃ ·5H ₂ O产物的形成/分解。具有缺陷的激增硼化物材料为开发其他多相催化剂以有效捕获和转化CO ₂提供了巨大的机会。