A single-atom library for guided monometallic and concentration-complex multimetallic designs

Han, Lili; Cheng, Hao; Liu, Wei; Li, Haoqiang; Ou, Pengfei; Lin, Ruoqian; Wang, Hsiao-Tsu; Pao, Chih-Wen; Head, Ashley R.; Wang, Chia-Hsin; Tong, Xiao; Sun, Cheng-Jun; Pong, Way-Faung; Luo, Jun; Zheng, Jin-Cheng; Xin, Huolin L.

doi:10.1038/s41563-022-01252-y

A single-atom library for guided monometallic and concentration-complex multimetallic designs

Journal Article · Mon May 23 00:00:00 EDT 2022 · Nature Materials

DOI:https://doi.org/10.1038/s41563-022-01252-y· OSTI ID:1876830

Han, Lili ^[1]; ^[1]; Liu, Wei ^[2]; Li, Haoqiang ^[2]; Ou, Pengfei ^[3]; Lin, Ruoqian ^[4]; ^[5]; Pao, Chih-Wen ^[6]; ^[4]; Wang, Chia-Hsin ^[6]; Tong, Xiao ^[4]; Sun, Cheng-Jun ^[7]; Pong, Way-Faung ^[5]; ^[8]; ^[9]; ^[1]

Univ. of California, Irvine, CA (United States)
Tianjin Univ. of Technology (China)
McGill Univ., Montreal, QC (Canada)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Tamkang Univ., New Taipei City (Taiwan)
National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
Argonne National Lab. (ANL), Lemont, IL (United States)
Tianjin Univ. of Technology (China); Univ. of Electronic Science and Technology of China, Shenzhen (China)
Xiamen Univ. (China); Xiamen Univ., Selangor (Malaysia)

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 analyzed 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. Furthermore, our work offers a single-atom library spanning from monometallic to concentration-complex multimetallic materials for the rational design of single-atom catalysts.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 1876830

Report Number(s):: BNL-223153-2022-JAAM

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 6 Vol. 21; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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A single-atom library for guided monometallic and concentration-complex multimetallic designs

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