Atomic Structure Evolution of Pt–Co Binary Catalysts: Single Metal Sites versus Intermetallic Nanocrystals

Li, Xing; He, Yanghua; Cheng, Shaobo; Li, Boyang; Zeng, Yachao; Xie, Zhenhua; Meng, Qingping; Ma, Lu; Kisslinger, Kim; Tong, Xiao; Hwang, Sooyeon; Yao, Siyu; Li, Chenzhao; Qiao, Zhi; Shan, Chongxin; Zhu, Yimei; Xie, Jian; Wang, Guofeng; Wu, Gang; Su, Dong

doi:10.1002/adma.202106371

Title: Atomic Structure Evolution of Pt–Co Binary Catalysts: Single Metal Sites versus Intermetallic Nanocrystals

Journal Article · Mon Oct 04 00:00:00 EDT 2021 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202106371· OSTI ID:1827164

^[1]; He, Yanghua ^[2]; Cheng, Shaobo ^[3]; Li, Boyang ^[4]; Zeng, Yachao ^[2]; Xie, Zhenhua ^[3]; Meng, Qingping ^[3]; Ma, Lu ^[3]; Kisslinger, Kim ^[3]; Tong, Xiao ^[3]; Hwang, Sooyeon ^[3]; Yao, Siyu ^[3]; Li, Chenzhao ^[5]; Qiao, Zhi ^[2]; Shan, Chongxin ^[6]; Zhu, Yimei ^[3]; Xie, Jian ^[5]; Wang, Guofeng ^[4]; Wu, Gang ^[2]; Su, Dong ^[7]

Zhengzhou University (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
University at Buffalo, The State University of New York, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
University of Pittsburgh, PA (United States)
Indiana University-Purdue University, Indianapolis, IN (United States)
Zhengzhou University (China)
Brookhaven National Lab. (BNL), Upton, NY (United States); Chinese Academy of Sciences (CAS), Beijing (China)

Due to their exceptional catalytic properties for the oxygen reduction reaction (ORR) and other crucial electrochemical reactions, PtCo intermetallic nanoparticle (NP) and single atomic (SA) Pt metal site catalysts have received considerable attention. However, their formation mechanisms at the atomic level during high-temperature annealing processes remain elusive. Furthermore, the thermally driven structure evolution of Pt–Co binary catalyst systems is investigated using advanced in situ electron microscopy, including PtCo intermetallic alloys and single Pt/Co metal sites. The pre-doping of CoN₄ sites in carbon supports and the initial Pt NP sizes play essential roles in forming either Pt₃Co intermetallics or single Pt/Co metal sites. Importantly, the initial Pt NP loadings against the carbon support are critical to whether alloying to L1₂-ordered Pt₃Co NPs or atomizing to SA Pt sites at high temperatures. High Pt NP loadings (e.g., 20%) tend to lead to the formation of highly ordered Pt₃Co intermetallic NPs with excellent activity and enhanced stability toward the ORR. In contrast, at a relatively low Pt loading (<6 wt%), the formation of single Pt sites in the form of PtC₃N is thermodynamically favorable, in which a synergy between the PtC₃N and the CoN₄ sites could enhance the catalytic activity for the ORR, but showing insufficient stability.

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

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1827164

Report Number(s):: BNL-222283-2021-JAAM

Journal Information:: Advanced Materials, Vol. 33, Issue 48; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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