To develop efficient and durable acidic oxygen–reduction–reaction (ORR) catalysts based on all platinum group metals (PGMs) is crucial for large-scale application of proton-exchange membrane fuel cells (PEMFCs) but challenging. Here, we report a nitrogen coordination-induced strong metal–support interaction that can tune the surface atoms of ORR-inactive PGM clusters into efficient and durable active sites. Taking Rh as an example, the carbonization of Rh-overdoped zeolitic imidazolate framework-8 results in a large number of Rh clusters (with a little atomic Rh) in porous nitrogen-doped carbon. The cluster surface atoms coordinate with the nitrogen of the carbon support, forming much stronger metal–support interactions than that of common N-doped carbon-supported metal nanoparticles. The activity of surface-activated Rh clusters is close to that of Pt/C. The regulation rules for the surface active sites inherit most of the characteristics of the corresponding single-atom catalysts, but without their severe instability problem. This surface activation strategy has also shown applicable to other PGMs, thereby it is a promising way to alleviate the reliance of PEMFCs on platinum.

中文翻译：

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铂族金属簇的表面活化用于质子交换膜燃料电池中高效持久的氧还原

开发基于全铂族金属 (PGM) 的高效且耐用的酸性氧还原反应 (ORR) 催化剂对于质子交换膜燃料电池 (PEMFC) 的大规模应用至关重要，但具有挑战性。在这里，我们报告了氮配位诱导的强金属-载体相互作用，可以将 ORR 非活性 PGM 团簇的表面原子调整为高效且持久的活性位点。以Rh为例，Rh-overdoped沸石咪唑盐骨架-8的碳化导致多孔氮掺杂碳中存在大量Rh簇（带有少量原子Rh）。团簇表面原子与碳载体的氮配位，形成比普通氮掺杂碳负载金属纳米粒子更强的金属-载体相互作用。表面活化的 Rh 团簇的活性接近于 Pt/C。表面活性位点的调节规则继承了相应单原子催化剂的大部分特性，但没有严重的不稳定问题。这种表面活化策略也适用于其他 PGM，因此它是减轻 PEMFC 对铂的依赖的有前途的方法。