Exceeding the volcano relationship in oxygen reduction/evolution reactions using single-atom-based catalysts with dual-active-sites. Issue 20 (18th May 2020)

• Record Type: Journal Article
• Authors: Li, Xiyu; Duan, Sai; Sharman, Edward; Zhao, Yuan; Yang, Li; Zhuo, Zhiwen; Cui, Peng; Jiang, Jun; Luo, Yi
• Is Part Of: Journal of materials chemistry. Volume 8:Issue 20(2020)
• Page Start: 10193
• Page End: 10198
• Publication Date: 2020-05-18
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d0ta01399d
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Both a linear OER activity trend that reaches an ideal 0 V overpotential and a new volcano ORR activity trend with the volcano apex around ideal 1.23 V limiting potential are associated with our dual-active-site designs. Abstract : Finding cost-effective catalysts to drive oxygen reduction/evolution reactions (ORR/OER) is a highly attractive goal. Most catalysts follow a volcano relationship of performance, making it difficult to search thoroughly enough among the huge number of possible structures to reach the volcano apex. Using first-principles simulations, we demonstrated that the design of single-atom-based catalysts (SACs) incorporating dual-active-sites breaks the universal scaling relationship between *OOH and *OH adsorption, leading to performances superior to those constrained to follow the volcano plot. Both a linear OER activity trend that reaches an ideal 0 V overpotential and a new linear scaling relation (free energy difference Δ G OOH = Δ G OH + 2.41 eV) that crosses the region of optimal limiting potentials in the volcano plot of the ORR are associated with our dual-active-site designs. This novel strategy of breaking the volcano dependence with dual-active-sites in SACs may promote the development of efficient electrocatalysts for the ORR/OER and other chemical reactions.