Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites

DOI: 10.1038/s41467-024-54820-y

Authors: Lu Chen (University College London) , Xuze Guan (University College London) , Zhaofu Fei (École Polytechnique Fedérale de Lausanne (EPFL)) , Hiroyuki Asakura (Kindai University) , Lun Zhang (University College London) , Zhipeng Wang (University College London) , Xinlian Su (University College London) , Zhangyi Yao (University College London) , Luke L. Keenan (Diamond Light Source) , Shusaku Hayama (Diamond Light Source) , Matthijs A. Van Spronsen (Diamond Light Source) , Burcu Karagoz (Diamond Light Source) , Georg Held (Diamond Light Source) , Christopher S. Allen (Diamond Light Source; University of Oxford) , David G. Hopkinson (Diamond Light Source) , Donato Decarolis (Diamond Light Source; UK Catalysis Hub, Research Complex at Harwell (RCaH)) , June Callison (UK Catalysis Hub, Research Complex at Harwell (RCaH)) , Paul J. Dyson (École Polytechnique Fedérale de Lausanne (EPFL)) , Feng Ryan Wang (University College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 16

State: Published (Approved)
Published: January 2025
Diamond Proposal Number(s): 30622 , 33257 , 31922

Abstract: Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods used to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx remains a significant challenge. Here, we report a bi-metallic surficial catalyst (PtSCuO/Al2O3) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH3 conversion at 250 °C with a weight hourly space velocity of 600 ml NH3·h−1·g−1, which is 50 °C lower than commercial Pt/Al2O3, and maintains high N2 selectivity through a wide temperature window. Operando XAFS studies reveal that the surface Pt atoms in PtSCuO/Al2O3 enhance the redox properties of the Cu species, thus accelerating the Cu2+ reduction rate and improving the rate of the NH3-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in PtSCuO/Al2O3 contributes to the high selectivity by facilitating internal selective catalytic reduction.

Subject Areas: Chemistry, Materials, Environment

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: B07-C-Versatile Soft X-ray beamline: Ambient Pressure XPS and NEXAFS , E01-JEM ARM 200CF , E02-JEM ARM 300CF , I20-EDE-Energy Dispersive EXAFS (EDE)

Other Facilities: BL14B2 at SPring-8; ID-24 at ESRF; Balder at MAX IV

Added On: 08/01/2025 08:47

Documents:
s41467-024-54820-y.pdf

Discipline Tags:

Earth Sciences & Environment Physical Chemistry Catalysis Chemistry Materials Science Chemical Engineering Engineering & Technology

Technical Tags:

Microscopy Spectroscopy Electron Microscopy (EM) Transmission Electron Microscopy (TEM) X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS) Near Edge X-ray Absorption Fine Structures (NEXAFS)