Abstract Supported bimetallic catalysts have become an important class of catalysts in heterogeneous catalysis. Although well-defined bimetallic nanoparticles (BNPs) can be synthesized by seeded-growth in liquid phase, uniform deposition of these BNPs onto porous supports is very challenging. Here, we develop a universal nanoreactor strategy to directly fabricate the PdAu BNPs in the solid support of coral-like nitrogen-doped mesoporous polymer (NMP) with uniform dispersion in a large scale. This strategy is based on coordination chemistry to introduce the high-quality seeds of Pd nanoclusters and the Au ions into the NMP, and thus to be used as a nanoreactor for seeded growth of PdAu BNPs in solid state during thermal reduction. Many other supported Pd-based BNPs (diameters ranging from 2 to 3 nm) have also been successfully synthesized by adoption of this strategy, including PdRu, PdCo, PdNi, PdZn, PdAg and PdCu BNPs. As an example, the as-synthesized Pd1Au1/4 sample shows enhanced catalytic performance in formic acid (FA) dehydrogenation compared with the monometallic analogues, indicating the synergistic effect between Pd and Au. In addition, the Pd1Au1/4 product is molded into monolith without any binders due to its coral-like structure. The Pd1Au1/4 monolith shows considerable activity in FA dehydrogenation with a turnover frequency (TOF) value of 3684 h−1 at 333 K, which is recycled five times without changes in activity. We believe that the nanoreactor strategy provides an effective route to synthesize various supported bimetallic catalysts that have potential for applications in green and sustainable catalytic processes.

中文翻译：

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用于可扩展支持的超细双金属纳米粒子合成的通用纳米反应器策略

摘要 负载型双金属催化剂已成为多相催化中一类重要的催化剂。尽管可以通过液相中的种子生长合成明确定义的双金属纳米粒子 (BNP)，但将这些 BNP 均匀沉积到多孔载体上是非常具有挑战性的。在这里，我们开发了一种通用的纳米反应器策略，以在珊瑚状氮掺杂介孔聚合物 (NMP) 的固体载体中直接制造 PdAu BNP，并大规模均匀分散。该策略基于配位化学，将高质量的 Pd 纳米团簇种子和 Au 离子引入 NMP，从而用作纳米反应器，用于热还原过程中固态 PdAu BNP 的种子生长。通过采用这种策略，还成功合成了许多其他受支持的 Pd 基 BNP（直径范围为 2 至 3 nm），包括 PdRu、PdCo、PdNi、PdZn、PdAg 和 PdCu BNP。例如，与单金属类似物相比，合成的 Pd1Au1/4 样品在甲酸 (FA) 脱氢中的催化性能增强，表明 Pd 和 Au 之间存在协同效应。此外，由于其珊瑚状结构，Pd1Au1/4 产品被模制成没有任何粘合剂的整体。Pd1Au1/4 整料在 FA 脱氢中显示出相当大的活​​性，在 333 K 时的周转频率 (TOF) 值为 3684 h-1，可循环使用 5 次而活性没有变化。