ABSTRACT
Electrocatalytic generation of H2O2 via the 2-electron pathway of oxygen reduction reaction (2e-ORR) is an attractive technology compared to the anthraquinone process due to convenience and environmental friendliness. However, catalysts with excellent selectivity and high activity for 2e-ORR are necessary for practical applications. Reported here is a catalyst comprising boron-doped porous carbon hollow spheres (B-PCHSs) prepared using the hard template method coupled with borate transesterification. In an alkali electrolyte, the selectivity of B-PCHS for 2e-ORR above 90% in range of 0.4-0.7 VRHE and an onset potential of 0.833 V was obtained. Meanwhile, the generation rate of H2O2 reached 902.48 mmol h-1 gcat-1 at 0.4 VRHE under 59.13 mA cm-2 in batch electrolysis. The excellent catalytic selectivity of B-PCHS for 2e-ORR originates from the boron element, and the catalytic activity of B-PCHS for H2O2 generation is contributed to the morphology of porous hollow spheres, which facilitates mass transfer processes.
ABSTRACT
Exploring an active and cost-effective electrocatalyst alternative to carbon-supported platinum nanoparticles for alkaline hydrogen evolution reaction (HER) have remained elusive to date. Here, we report a catalyst based on platinum single atoms (SAs) doped into the hetero-interfaced Ru/RuO2 support (referred to as Pt-Ru/RuO2), which features a low HER overpotential, an excellent stability and a distinctly enhanced cost-based activity compared to commercial Pt/C and Ru/C in 1 M KOH. Advanced physico-chemical characterizations disclose that the sluggish water dissociation is accelerated by RuO2 while Pt SAs and the metallic Ru facilitate the subsequent H* combination. Theoretical calculations correlate with the experimental findings. Furthermore, Pt-Ru/RuO2 only requires 1.90 V to reach 1 A cm-2 and delivers a high price activity in the anion exchange membrane water electrolyzer, outperforming the benchmark Pt/C. This research offers a feasible guidance for developing the noble metal-based catalysts with high performance and low cost toward practical H2 production.
ABSTRACT
Integrating single atoms and clusters into one system represents a novel strategy for achieving the desired catalytic performance. In comparison to single-atom catalysts, catalysts combining single atoms and clusters harness the advantages of both, thus displaying greater potential. Nevertheless, constructing single-atom-cluster systems remains challenging, and the fundamental mechanism for enhancing catalytic activity remains elusive. In this study, a directly confined preparation of a 3D hollow sea urchin-like carbon structure (MnSA /MnAC -SSCNR) is developed. Mn single atoms synergistically interact with Mn clusters, optimizing and reducing energy barriers in the reaction pathway, thus enhancing reaction kinetics. Consequently, in contrast to Mn single-atom catalysts (MnSA -SSCNR), MnSA /MnAC -SSCNR exhibits significantly improved oxygen reduction activity, with a half-wave potential (E1/2 ) of 0.90 V in 0.1 m KOH, surpassing that of MnSA -SSCNR and Pt/C. This work demonstrates a strategy of remote synergy between heterogeneous single atoms and clusters, which not only contributes to electrocatalytic reactions but also holds potential for reactions involving more complex products.
