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XAS/DRIFTS/MS spectroscopy for time-resolved operando study of integrated carbon capture and utilisation process

DOI: 10.1016/j.seppur.2022.121622 DOI Help

Authors: Hongman Sun (China University of Petroleum; Queen's University of Belfast) , Chunfen Wang (China University of Petroleum) , Shuzhuang Sun (Queen’s University Belfast) , Antonio T. Lopez (University of Manchester) , Youhe Wang (China University of Petroleum) , Jingbin Zeng (China University of Petroleum) , Zhen Liu (China University of Petroleum) , Zifeng Yan (China University of Petroleum) , Christopher M. A. Parlett (University of Manchester; Diamond Light Source; The University of Manchester at Harwell; UK Catalysis Hub, Research Complex at Harwell) , Chunfei Wu (Queen’s University Belfast)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Separation And Purification Technology , VOL 298

State: Published (Approved)
Published: October 2022
Diamond Proposal Number(s): 23645

Abstract: An integrated carbon capture and utilization (ICCU) process present an ideal solution to address anthropogenic carbon dioxide (CO2) emissions from fossil fuel-driven electricity production, allowing for capturing and subsequent utilization of CO2 instead of current release into the atmosphere. Effective dual-functional materials (DFMs), through the combination of CO2 sorbents and catalysts, can not only capture CO2 but also convert it into higher-value chemicals, such as CH4 or CO, under isothermal conditions within a single reactor are highly desirable for ICCU processes. In this study, we investigate the mechanism of ICCU over 10 %NiCaO by the time-resolved operando XAS/DRIFTS/MS and the influence of a reduction pretreatment on the process and the products formed. During the 1st stage of the ICCU process (carbon capture), CaO adsorbs CO2 resulting in bicarbonate, carbonate, and formate species formation. At the same time, the Ni catalytic active species are oxidized by CO2, leading to the formation of NiO and CO. However, pre-treating the same DFM under hydrogen, during heating to operating temperature, resulted in a switch to CH4 production, suggesting the presence of high levels of surface adsorbed H2. During the 2nd stage of ICCU (CO2 conversion), the NiO generated during capture is reduced by H2 to metallic Ni, which facilitates the reduction of bicarbonates, carbonates, and formats, via H2 dissociation, to produce and liberate gaseous CO. Thus, both adsorption and catalytic sites are regenerated for the subsequent ICCU cycle.

Journal Keywords: Integrated carbon capture and utilisation; CaO; Dual-functional materials; Operando XAS/DRIFTS/MS; Mechanism

Diamond Keywords: Carbon Capture and Storage (CCS)

Subject Areas: Chemistry, Environment

Instruments: I20-EDE-Energy Dispersive EXAFS (EDE)

Added On: 06/07/2022 08:53

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Energy Dispersive EXAFS (EDE)