Restructuring the interfacial active sites to generalize the volcano curves for platinum-cobalt synergistic catalysis

Wenyao Chen, Yao Shi, Changwei Liu, Zhouhong Ren, Zikun Huang, Zhou Chen, Xiangxue Zhang, Shanshan Liang, Lei Xie, Cheng Lian (), Gang Qian, Jing Zhang, Xi Liu (), Chen De, Xinggui Zhou, Weikang Yuan and Xuezhi Duan ()
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Wenyao Chen: East China University of Science and Technology
Yao Shi: East China University of Science and Technology
Changwei Liu: East China University of Science and Technology
Zhouhong Ren: Shanghai Jiao Tong University
Zikun Huang: East China University of Science and Technology
Zhou Chen: East China University of Science and Technology
Xiangxue Zhang: East China University of Science and Technology
Shanshan Liang: East China University of Science and Technology
Lei Xie: Chinese Academy of Sciences
Cheng Lian: East China University of Science and Technology
Gang Qian: East China University of Science and Technology
Jing Zhang: East China University of Science and Technology
Xi Liu: Shanghai Jiao Tong University
Chen De: Norwegian University of Science and Technology
Xinggui Zhou: East China University of Science and Technology
Weikang Yuan: East China University of Science and Technology
Xuezhi Duan: East China University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Computationally derived volcano curve has become the gold standard in catalysis, whose practical application usually relies on empirical interpretations of composition or size effects by the identical active site assumption. Here, we present a proof-of-concept study on disclosing both the support- and adsorbate-induced restructuring of Pt-Co bimetallic catalysts, and the related interplays among different interfacial sites to propose the synergy-dependent volcano curves. Multiple characterizations, isotopic kinetic investigations, and multiscale simulations unravel that the progressive incorporation of Co into Pt catalysts, driven by strong Pt-C bonding (metal-support interfaces) and Co-O bonding (metal-adsorbate interfaces), initiates the formation of Pt-rich alloys accompanied by isolated Co species, then Co segregation to epitaxial CoOx overlayers and adjacent Co3O4 clusters, and ultimately structural collapse into amorphous alloys. Accordingly, three distinct synergies, involving lattice oxygen redox from Pt-Co alloy/Co3O4 clusters, dual-active sites engineering via Pt-rich alloy/CoOx overlayer, and electron coupling within exposed alloy, are identified and quantified for CO oxidation (gas-phase), ammonia borane hydrolysis (liquid-phase), and hydrogen evolution reaction (electrocatalysis), respectively. The resultant synergy-dependent volcano curves represent an advancement over traditional composition-/size-dependent ones, serving as a bridge between theoretical models and experimental observations in bimetallic catalysis.

Date: 2024
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DOI: 10.1038/s41467-024-53474-0

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