研究目的
To develop Ni-promoted ceria-titanium oxide redox catalysts for efficient solar thermochemical CO2 and H2O splitting and CH4 partial oxidation at lower temperatures, addressing challenges in high redox kinetics and yields.
研究成果
The Ni-promoted CeO2-TiO2 catalyst demonstrated exceptional performance in solar thermochemical processes, with high CH4 conversion, syngas selectivity, and unprecedented CO/H2 production rates. The synergy between catalytic Ni sites and the stoichiometric redox cycle of CeO2-TiO2/Ce2Ti2O7 enhances lattice oxygen transport and reaction kinetics, providing a foundation for designing efficient materials for sustainable solar fuel production.
研究不足
The study is limited to laboratory-scale experiments at 900°C; scalability to industrial applications and long-term stability under real solar conditions were not fully addressed. Potential carbon deposition issues and the use of non-noble metals may require further optimization for cost-effectiveness and durability.
1：Experimental Design and Method Selection:
The study used a two-step redox cycle involving methane-driven reduction (MDR) followed by CO2 or H2O splitting. Experimental methods included catalyst synthesis via co-precipitation and wet impregnation, reactivity tests in a differential quartz tube microreactor, and characterization using XRD, XPS, H2-TPR, SEM, TEM, STEM-EDX, XANES, and ICP-AES, complemented by DFT calculations for mechanistic insights.
2：Sample Selection and Data Sources:
Catalysts with varying Ni loadings (0.5-5 wt%) on CeO2-TiO2 were synthesized. Data were collected from laboratory experiments and computational simulations.
3：5-5 wt%) on CeO2-TiO2 were synthesized. Data were collected from laboratory experiments and computational simulations. List of Experimental Equipment and Materials:
3. List of Experimental Equipment and Materials: Equipment included a quartz tube microreactor, infrared image furnace (VTH-E44, ULVAC-RIKO), mass flow controllers, quadrupole mass spectrometer (GAM200, InProcess Instruments), XRD diffractometer (PANalytical), XPS spectrometer (ESCALAB 250, Thermo Fisher Scientific), H2-TPR apparatus (Micromeritics Auto Chem II 2920), SEM (JSM-7800F, JEOL), TEM (JEM-2200F, JEOL), XANES at BL14W1 beamline (Shanghai Synchrotron Radiation Facility), and ICP-AES (IRIS Intrepid II XSP, Thermo Electron Corporation). Materials included Ce(NO3)3·6H2O, (C4H9O)4Ti, Ni(NO3)2·6H2O, NH3·H2O, deionized water, ethanol, CH4, CO2, H2O, Ar, and calibration gases.
4：Experimental Procedures and Operational Workflow:
Catalysts were synthesized, calcined, and tested in cyclic redox reactions at 900°C. Reduction with CH4 for 6 min, followed by oxidation with CO2 or H2O for 10 min, with Ar purging between cycles. Gas concentrations were monitored by mass spectrometry, and data were analyzed for conversion, selectivity, and production rates.
5：Data Analysis Methods:
Data analysis involved calculating CH4 conversion, CO selectivity, H2/CO ratio, and production rates using integral methods. DFT calculations used VASP with PBE functional and DFT+U method for energy barriers and reaction pathways.
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X-ray Diffractometer
PANalytical
PANalytical
Investigating crystallographic phase evolution of catalysts.
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XPS Spectrometer
ESCALAB 250
Thermo Fisher Scientific
Probing near-surface element states and oxidation states.
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SEM
JSM-7800F
JEOL
Observing microstructure and morphology of catalyst samples.
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TEM
JEM-2200F
JEOL
Identifying morphology, crystallinity, and elemental distribution.
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ICP-AES Instrument
IRIS Intrepid II XSP
Thermo Electron Corporation
Quantifying actual Ni loadings in catalysts.
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Infrared Image Furnace
VTH-E44
ULVAC-RIKO
Heating the reactor for catalytic activity tests at high temperatures.
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Quadrupole Mass Spectrometer
GAM200
InProcess Instruments
Analyzing and recording outlet gas concentrations during experiments.
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H2-TPR Apparatus
Auto Chem II 2920
Micromeritics
Assessing redox behavior of catalysts using temperature-programmed reduction.
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