Ammonia borane (AB) represents a promising hydrogen storage material, while high-performing catalysts allowing efficient release of hydrogen from the hydrolysis of AB are desired. Here, Pd nanoclusters (NCs) are successfully immobilized within pores of a bipyridyl covalent triazine framework (CTF-BPDA-TPDH) via a metal-nitrogen coordination reduction strategy. The porous structure and tailored N sites of CTF facilitate the anchoring of Pd ions and the in situ formation of monodisperse Pd NCs confined in the pores of CTF. The resulting Pd-NCs@CTF composites exhibit high activity toward the hydrolysis of AB with turnover frequencies (TOFs) of 273 and 434 mol_H2·mol⁻¹_Pd·min⁻¹ in neutral and alkaline solutions, respectively. The Pd-NCs@CTF catalyst is also demonstrated for the tandem dehydrogenation of AB and hydrogenation of nitroarenes featuring short reaction time and high yields. These findings emphasize the promise of the porous CTFs encapsulated metal NCs for active catalysts.

氨硼烷 (AB) 是一种很有前途的储氢材料，而高性能催化剂则需要能够从 AB 的水解中有效释放氢气。在这里，Pd 纳米团簇 (NCs) 通过金属-氮配位还原策略成功地固定在联吡啶共价三嗪骨架 (CTF-BPDA-TPDH) 的孔中。CTF 的多孔结构和定制的 N 位点有助于 Pd 离子的锚定和限制在 CTF 孔隙中的单分散 Pd NCs 的原位形成。所得 Pd-NCs@CTF 复合材料对 AB 的水解表现出高活性，转换频率 (TOF) 为 273 和 434 mol _H2 ·mol ^-1 _Pd ·min ^-1分别在中性和碱性溶液中。Pd-NCs@CTF催化剂还被证明可用于AB的串联脱氢和硝基芳烃的加氢，具有反应时间短、收率高的特点。这些发现强调了多孔 CTF 封装金属 NC 用于活性催化剂的前景。