Refining active sites and hydrogen spillover for boosting visible-light-driven ammonia synthesis at room temperature. Issue 40 (5th October 2021)

• Record Type: Journal Article
• Authors: Fu, Rong; Pan, Ziye; Mu, Xiaowei; Li, Jiayang; Zhan, Qingyun; Zhao, Zihan; Mu, Xiaoyue; Li, Lu
• Is Part Of: Journal of materials chemistry. Volume 9:Issue 40(2021)
• Page Start: 22827
• Page End: 22832
• Publication Date: 2021-10-05
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1ta06296d
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Efficient ammonia synthesis was achieved by Mo, Pt modified TiO2− x under visible light irradiation. Pt nanoparticles trigger hydrogen spillover from Pt to Mo, enabling facile NH3 assembly and desorption, as well as increasing free Mo active sites. Abstract : It is highly desirable to develop a low-pressure, low-temperature ammonia synthesis process. Although this process is, in principle, thermodynamically feasible under ambient conditions, it remains a big challenge to find ideal catalysts with favorable kinetic pathways. Here, we demonstrate that efficient ammonia synthesis (>3700 μg h −1 gcat. −1 ) from N2 and H2 gases can proceed at room temperature using Mo, Pt modified TiO2− x under visible light irradiation up to 800 nm. The doped Mo(v ) species nearby surface oxygen vacancies (VO ) offer coordinatively unsaturated sites for N2 activation with strong adsorption energy and excellent electron back-donation ability. Distinctively, a small amount of surface-loaded Pt nanoparticles trigger hydrogen spillover from Pt to VO, enabling facile NH3 assembly and desorption, as well as increasing free Mo(v ) active sites. The incorporation of Mo and Pt also synergistically optimizes the light-harvesting ability and the band structure of TiO2, greatly facilitating the photoexcited N2 reduction and H2 oxidation.