Cascade NH3 oxidation and N2O decomposition via bifunctional Co and Cu catalysts

DOI: 10.1021/acscatal.3c02392

Authors: Xuze Guan (University College London) , Hiroyuki Asakura (Kindai University; Kyoto University) , Rong Han (Wuhan University) , Siyuan Xu (Wuhan University) , Hao-Xin Liu (Shandong University) , Lu Chen (University of Cambridge) , Zhangyi Yao (University College London) , Jay Hon Cheung Yan (University College London) , Tsunehiro Tanaka (Kyoto University) , Yuzheng Guo (Wuhan University) , Chun-Jiang Jia (Shandong University) , Feng Ryan Wang (University College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis

State: Published (Approved)
Published: October 2023
Diamond Proposal Number(s): 23759 , 24450 , 14239

Abstract: The selective catalytic oxidation of NH3 (NH3–SCO) to N2 is an important reaction for the treatment of diesel engine exhaust. Co3O4 has the highest activity among non-noble metals but suffers from N2O release. Such N2O emissions have recently been regulated due to having a 300× higher greenhouse gas effect than CO2. Here, we design CuO-supported Co3O4 as a cascade catalyst for the selective oxidation of NH3 to N2. The NH3–SCO reaction on CuO–Co3O4 follows a de-N2O pathway. Co3O4 activates gaseous oxygen to form N2O. The high redox property of the CuO–Co3O4 interface promotes the breaking of the N–O bond in N2O to form N2. The addition of CuO–Co3O4 to the Pt–Al2O3 catalyst reduces the full NH3 conversion temperature by 50 K and improves the N2 selectivity by 20%. These findings provide a promising strategy for reducing N2O emissions and will contribute to the rational design and development of non-noble metal catalysts.

Journal Keywords: ammonia-selective oxidation; CuO/Co3O4 catalyst; N2O decomposition; metal−support interaction; O2 activation

Subject Areas: Chemistry, Materials, Environment


Instruments: B18-Core EXAFS

Other Facilities: BL01B1 at SPring-8; ISISS at BESSY II

Added On: 16/10/2023 08:29

Documents:
guan-et-al-2023-cascade-nh3-oxidation-and-n2o-decomposition-via-bifunctional-co-and-cu-catalysts.pdf

Discipline Tags:

Desertification & Pollution Earth Sciences & Environment Physical Chemistry Catalysis Chemistry Materials Science

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS) X-ray Absorption Near Edge Structure (XANES)