Mn-doped Pt/ZnO adsorbent with enhanced synergetic Pt-sulfur acceptor interaction for effective atmospheric ultra-deep desulfurization

• Published in: Chemical engineering science 2024-08, Vol.295, p.120149, Article 120149
• Main Authors: Niu, Hongyu, Li, Chuang, Luo, Jingjie, Cong, Haiyue, Liang, Changhai
• Format: Article
• Language: English
• Subjects: Dibenzothiophene; Mn-doped Pt/ZnO; Reactive adsorption; Sulfur transfer; Ultra-deep desulfurization
• ISSN: 0009-2509; 1873-4405
• DOI: 10.1016/j.ces.2024.120149

This work presents an innovative insight into the relationship between the rate-determining steps of reactive adsorption desulfurization (RADS) and the synergetic metal-sulfur acceptor interaction, which paves an avenue for the rational design of high-performance and high-sulfur capacity adsorbent for RADS reactions. [Display omitted] •Pt/ZnO-1MnO-400 has shown to be excellent adsorbent for atmospheric RADS.•Mn amount and calcination temperatures for Mn-doped Pt/ZnO are investigated.•Sulfur transfer is confirmed by direct transfer of sulfur from PtSx to sulfur acceptor.•The activity and sulfur capacity have relied on Pt and sulfur acceptor states.•Relationship between rate-determining steps and Pt-sulfur acceptor is established. Developing high-activity and high-sulfur capacity adsorbent for reactive adsorption desulfurization (RADS) can be challenging when the relationship between rate-determining steps and synergetic metal-sulfur acceptor interaction is poorly understood. Herein, we report the desulfurization performance of Mn-doped Pt/ZnO with different Mn amounts and calcination temperatures under atmospheric RADS of dibenzothiophene (DBT) to understand rate-determining steps. Results suggested that the C-S cleavage of DBT and direct transfer of sulfur from PtSx to the sulfur acceptor were two rate-determining steps and relied on Pt and sulfur acceptor states. The Pt/ZnO-1MnO-400 was verified as the most outstanding adsorbent with 100 % desulfurization efficiency, 0.316 g-S/g-Ads sulfur capacity, and 55.3 h−1 TOF, attributing to form small Pt (∼2.5 nm) and agglomerate-free sulfur acceptor (∼35 nm) particles. This work provides innovative insight into the relationship between rate-determining steps and synergetic Pt-sulfur acceptor interaction, which paves the way for the design and synthesis of efficient adsorbent for RADS.