研究目的
To investigate the relation between photocatalytic activity and surface doping structure in RuO2-loaded Sm3+-doped CeO2 for overall water splitting.
研究成果
The research demonstrates that heterogeneous doping structure in Sm3+-doped CeO2, achieved via solid-state reaction, significantly enhances photocatalytic water splitting activity compared to homogeneous structures. The interface between pure and doped phases facilitates charge separation, preventing recombination and enabling stable hydrogen and oxygen production. This highlights the importance of doping structure and ionic size in designing efficient photocatalysts, with implications for renewable energy technologies.
研究不足
The study is limited to Sm3+ doping in CeO2 and may not generalize to other dopants or materials. The mechanisms at the interface are not fully elucidated, requiring further investigation into charge separation sites. The use of UV light restricts applicability to visible light conditions, and scalability for practical energy applications is not addressed.
1：Experimental Design and Method Selection:
The study compared Sm3+-doped CeO2 samples synthesized via solid-state reaction and co-precipitation methods to examine the effect of doping structure (heterogeneous vs. homogeneous) on photocatalytic activity for water splitting. Theoretical models from DFT calculations were referenced to understand electronic structure changes.
2：Sample Selection and Data Sources:
Samples were prepared with Sm3+ doping at 10 mol% using CeO2 and Sm2O3 or Ce(NO3)3·6H2O and Sm(NO3)3·6H2O as starting materials. Calcination temperatures ranged from 1273 to 1773 K. Data on elemental composition and structure were obtained from XRD, XPS, ICP-OES, and STEM/EDS analyses.
3：List of Experimental Equipment and Materials:
Equipment included XRD (Rigaku RINT-2200HF), XPS (JEOL JPS-9010TR), STEM (Hitachi High-Tech HT7700), EDS (Bruker Quantax), ICP-OES (Shimadzu ICPS-7510), BET surface area analyzer, UV-Vis spectrometer, gas chromatograph (Shimadzu GC-390B), and high-pressure Hg lamp (USHIO UM-452). Materials included CeO2 (Nacalai Tesque, 99%), Sm2O3 (High Purity Materials, 99.9%), Ce(NO3)3·6H2O (Nacalai Tesque, 99.9%), Sm(NO3)3·6H2O (Nacalai Tesque, 99.9%), ammonia aqueous solution (Nacalai Tesque, 28%), Ru3(CO)12 (Aldrich Chemical Co., 99%), THF, nitric acid, and distilled water.
4：2). Materials included CeO2 (Nacalai Tesque, 99%), Sm2O3 (High Purity Materials, 9%), Ce(NO3)3·6H2O (Nacalai Tesque, 9%), Sm(NO3)3·6H2O (Nacalai Tesque, 9%), ammonia aqueous solution (Nacalai Tesque, 28%), Ru3(CO)12 (Aldrich Chemical Co., 99%), THF, nitric acid, and distilled water.
Experimental Procedures and Operational Workflow:
4. Experimental Procedures and Operational Workflow: For solid-state synthesis, mixtures were calcined at various temperatures, treated with nitric acid to remove unreacted Sm2O3, and analyzed. For co-precipitation, precursors were precipitated with ammonia, dried, and calcined. RuO2 loading was done via impregnation with Ru3(CO)12 in THF, followed by heating. Photocatalytic reactions were conducted in a closed gas circulation system with UV irradiation, and gas evolution was monitored by GC.
5：Data Analysis Methods:
Data from XRD, XPS, ICP-OES, and BET were used to determine doping levels, phase composition, and surface areas. Photocatalytic activity was quantified by hydrogen and oxygen evolution rates per surface area, with statistical analysis implied from repeated measurements.
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