A single-atom library for guided monometallic and concentration-complex multimetallic designs
A single-atom library for guided monometallic and concentration-complex multimetallic designs
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用于引导单金属和浓度复杂多金属设计的单原子库
DOI：
10.1038/s41563-022-01252-y
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发表时间：
2022-05-23
期刊：
影响因子：
41.2
通讯作者：
Xin, Huolin L.
中科院分区：
文献类型：
--
作者：
Han, Lili;Cheng, Hao;Xin, Huolin L.
单原子催化剂表现出增强的催化性能，但大多数系统只探索几种不同金属的组合。在这里，研究了37种不同元素的文库，结果表明，在一个体系中加载12个金属原子可以提高电化学活性。原子分散的单原子催化剂具有跨越多相催化和均相催化的潜力。几十种单原子催化剂已经被开发出来，它们表现出显著的催化活性和选择性，这在金属表面是无法实现的。尽管前景广阔，但人们对单金属单原子相空间边界的认识有限，更不用说多金属相空间了。本文采用溶解-碳化的方法合成了37种单金属元素的单原子催化剂，并对其进行了表征和分析，建立了目前报道的最大的单原子催化剂文库。结合原位研究，我们揭示了单原子的氧化态、配位数、键长、配位元素和金属负载的统一原理，以指导原子分散原子锚定在n掺杂碳上的单原子催化剂的设计。我们利用该文库为单原子催化剂开辟了复杂的多金属相空间，并证明了使用单原子锚点作为结构单元来组装含有多达12种不同元素的浓度复杂单原子催化剂材料没有基本限制。我们的工作为合理设计单原子催化剂提供了从单金属到浓度复杂的多金属材料的单原子库。
Single-atom catalysts demonstrate enhanced catalytic properties, but most systems only explore combinations of a few different metals. Here, a library of 37 different elements is investigated, and it is shown that loading 12 metallic atoms in one system presents improved electrochemical activity.Atomically dispersed single-atom catalysts have the potential to bridge heterogeneous and homogeneous catalysis. Dozens of single-atom catalysts have been developed, and they exhibit notable catalytic activity and selectivity that are not achievable on metal surfaces. Although promising, there is limited knowledge about the boundaries for the monometallic single-atom phase space, not to mention multimetallic phase spaces. Here, single-atom catalysts based on 37 monometallic elements are synthesized using a dissolution-and-carbonization method, characterized and analysed to build the largest reported library of single-atom catalysts. In conjunction with in situ studies, we uncover unified principles on the oxidation state, coordination number, bond length, coordination element and metal loading of single atoms to guide the design of single-atom catalysts with atomically dispersed atoms anchored on N-doped carbon. We utilize the library to open up complex multimetallic phase spaces for single-atom catalysts and demonstrate that there is no fundamental limit on using single-atom anchor sites as structural units to assemble concentration-complex single-atom catalyst materials with up to 12 different elements. Our work offers a single-atom library spanning from monometallic to concentration-complex multimetallic materials for the rational design of single-atom catalysts.