The rational design of cost-effective and stable heterogeneous nanocatalysts with high activities is vital yet challenged for utilization of sustainable hydrogen fuel. Herein, we report a novel surficial alkaline functional strategy for immobilization of non-noble CuCo nanoparticles (NPs) on diamine-alkalized-functionalized Ti₃C₂ surfaces (CuCo/PDA-Ti₃C₂). By virtue of coordination effect, ultrafine CuCo NPs with the size of 1.8 nm were well dispersed on Ti₃C₂ surface. Strikingly, the optimized CuCo/PDA-Ti₃C₂ nanocatalyst presents an impressive catalytic performance toward ammonia borane hydrolysis (ABH) without any additive, with a completed conversion and a high turnover frequency (TOF) value of 71.8 mol_H2mol_cat^-1min^-1 at mild condition. The alkaline amine groups induced a strong support-metal synergistic interaction (SMSI) to not only regulate the localized charge distribution and electron energy levels near active sites, but also optimize the surface d center and adsorption/desorption behavior, resulting in an accelerating O-H bond cleavage in water molecular. This work presents a novel and universal strategy for developing alkaline titanium carbide (MXene)-based heterogeneous nanocatalysts for hydrogen energy society.

中文翻译：

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碱性碳化钛 （MXene） 工程超细非贵金属纳米催化剂，显著促进氨硼烷水解析氢


合理设计经济高效且稳定的高活性非均相纳米催化剂对于可持续氢燃料的利用至关重要，但也面临挑战。在此，我们报道了一种新的表面碱性功能策略，用于将非贵金属 CuCo 纳米颗粒 （NPs） 固定在二胺碱化功能化的 Ti₃C₂ 表面 （CuCo/PDA-Ti₃C₂） 上。凭借配位效应，尺寸为 1.8 nm 的超细 CuCo NPs 在 Ti₃C₂ 表面上具有良好的分散性。引人注目的是，优化的 CuCo/PDA-Ti₃C₂ 纳米催化剂在没有任何添加剂的情况下对氨硼烷水解 （ABH） 表现出令人印象深刻的催化性能，在温和条件下具有 71.8 mol_H2mol ^{cat-1 min-1} 的高周转频率 （TOF） 值。碱性胺基团诱导了强载体-金属协同作用 （SMSI），不仅调节了活性位点附近的局部电荷分布和电子能级，还优化了表面 d 中心和吸附/解吸行为，导致水分子中 O-H 键裂解加速。这项工作为氢能社会开发了一种基于碱性碳化钛 （MXene） 的非均相纳米催化剂的新型通用策略。