As a safe and efficient hydrogen storage material, ammonia borane (NH₃–BH₃, AB) shows great promise in the era of clean energy advocated by hydrogen. Thus, it is imperative to focus on the exploitation of high-performance heterogeneous catalytic systems for the effective utilization of hydrogen energy stored in AB. However, noble metal catalysts as high-efficiency systems suffer from high expenditure, and the traditional powder-based catalyst faces poor processability and recoverability. Herein, a bimetallic (Co/Ni) MOF-derived CoNiP/hierarchically porous carbon (HPC) monolithic aerogel was successfully prepared by the gelation–carbonization–phosphorization method and applied in the hydrolysis of AB. The ultrasmall transition bimetallic phosphide CoNiP nanoparticles were uniformly fabricated in the hierarchically porous aerogel after pyrolysis. Benefiting from the rapid mass transfer and high exposure of well-defined CoNiP-active species within the hierarchical aerogel support, the Co_0.3Ni_0.7P/HPC aerogel performed high hydrogen evolution activity and exhibited fast hydrogen generation rate with a completion time of 2 min under mild conditions. The theoretical calculations reveal the key effects of the adsorption energies between AB and water on CoNiP-active sites in the Co_0.3Ni_0.7P/HPC aerogel. Furthermore, the Co_0.3Ni_0.7P/HPC monolithic aerogel catalyst can be effortlessly separated and recycled at least 10 times without a remarkable loss of activity. The controllable design of P-doped bimetallic species in the porous aerogel herein should serve as the foundation for the preparation of practical functional monolithic applied catalysts for the hydrolysis of AB.

中文翻译：

---

双金属 （Co/Ni） MOF 衍生的 CoNiP 分层多孔碳整体气凝胶，用于氨硼烷的水解


氨硼烷 （NH₃–BH₃， AB） 作为一种安全高效的储氢材料，在氢能倡导的清洁能源时代显示出巨大的前景。因此，当务之急是专注于开发高性能多相催化系统，以有效利用 AB 中储存的氢能。然而，贵金属催化剂作为高效系统，成本高，传统的粉末基催化剂加工性和可回收性较差。在此，通过凝胶-碳化-磷酸化方法成功制备了双金属 （Co/Ni） MOF 衍生的 CoNiP/多孔碳 （HPC） 整体气凝胶，并应用于 AB 的水解。热解后，超小过渡双金属磷化物 CoNiP 纳米颗粒在分层多孔气凝胶中均匀制备。得益于分层气凝胶载体内快速传质和明确定义的 CoNiP 活性物质的高暴露，Co_0.3Ni_0.7P/HPC 气凝胶具有较高的析氢活性，并表现出快速的氢气生成速率，在温和条件下完成时间为 2 min。理论计算揭示了 AB 和水之间的吸附能对 Co_0.3Ni_0.7P/HPC 气凝胶中 CoNiP 活性位点的关键影响。此外，Co_0.3Ni_0.7P/HPC 整体气凝胶催化剂可以毫不费力地分离和回收至少 10 次，而不会造成明显的活性损失。 本文中多孔气凝胶中 P 掺杂双金属物种的可控设计应作为制备用于水解 AB 的实用功能整体应用催化剂的基础。