A high-throughput, solvent free method for dispersing metal atoms directly onto supports

DOI: 10.1039/D1TA08372D

Authors: Emerson Cristofer Kohlrausch (University of Nottingham; Universidade Federal do Rio Grande do Sul) , Higor A. Centurion (University of São Paulo) , Rhys Lodge (University of Nottingham) , Xuanli Luo (University of Nottingham) , Thomas Slater (Diamond Light Source) , Marcos J. L. Santos (Universidade Federal do Rio Grande do Sul) , Sanliang Ling (University of Nottingham) , Valmor R. Mastelaro (University of São Paulo) , Matthew J. Cliffe (University of Nottingham) , Renato Vitalino Goncalves (University of São Paulo) , Jesum Alves Fernandes (University of Nottingham)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of Materials Chemistry A

State: Published (Approved)
Published: November 2021
Diamond Proposal Number(s): 25120 , 17198 , 24914

Abstract: Atomically-dispersed metal catalysts (ADMCs) on surfaces have demonstrated high activity and selectivity in many catalytic reactions. However, dispersing and stabilising individual atoms in support materials in an atom/energy-efficient scalable way still presents a significant challenge. Currently, the synthesis of ADMCs involves many steps and further filtration procedures, creating a substantial hurdle to their production at industrial scale. In this work, we develop a new pathway for producing ADMCs in which Pt atoms are stabilised in the nitrogen-interstices of a graphitic carbon nitride (g-C3N4) framework using scalable, solvent-free, one-pot magnetron sputtering deposition. Our approach has the highest reported rate of ADMC production of 4.8 mg h-1 and generates no chemical waste. Deposition of only 0.5 weight percent of Pt onto g-C3N4 led to improved hydrogen production by factor of ca. 3333 ± 450 when compared to bare g-C3N4. PL analysis showed that the deposition of Pt atoms onto g-C3N4 suppressed the charge carrier recombination from the photogenerated electron-hole pairs of Pt/g-C3N4 thereby enhance hydrogen evolution. Scanning transmission electron microscope imaging before and after the hydrogen evolution reaction revealed that the Pt atoms stabilised in g-C3N4 have a high stability, with no agglomeration observed. Herein, it is shown that this scalable and clean approach can produce effective ADMCs with no further synthetic steps required, and that they can be readily used for catalytic reactions.

Subject Areas: Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B18-Core EXAFS , E01-JEM ARM 200CF

Other Facilities: MAX IV

Added On: 24/11/2021 09:31

Documents:
d1ta08372d.pdf

Discipline Tags:

Physical Chemistry Catalysis Chemistry Chemical Engineering Engineering & Technology

Technical Tags:

Microscopy Spectroscopy Electron Microscopy (EM) X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS) Scanning Transmission Electron Microscopy (STEM)