通过降低速率决定步骤中的过电势，表面 Rh 促进的 α-Fe2O3 光电化学水氧化,ACS Applied Materials & Interfaces

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通过降低速率决定步骤中的过电势，表面 Rh 促进的 α-Fe2O3 光电化学水氧化
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-07-25 , DOI: 10.1021/acsami.3c04458
Young-Min Kim ₁ , Yerin Hong ₂ , Kahyun Hur ₂ , Min-Seok Kim ₂ , Yun-Mo Sung ₁

Affiliation

研究了Rh簇沉积的赤铁矿(α-Fe ₂ O ₃ )光阳极(α-Fe ₂ O ₃ @Rh)的光电化学行为。_{Rh簇和α-Fe 2} O ₃纳米棒之间的相互作用通过实验和计算得到了阐明。一种简便的紫外辅助溶液浇铸沉积方法允许在α-Fe ₂ O ₃上沉积2 nm的Rh簇。沉积的Rh团簇有效增强了α-Fe ₂ O ₃光阳极的光电化学性能，电化学阻抗谱（EIS）和莫特-肖特基分析被用来了解α-Fe ₂ O ₃ @Rh光阳极的工作机制。结果揭示了α-Fe ₂ O ₃ @Rh 独特的载流子传输机制并增加了载流子密度，而吸收光谱保持不变。此外，析氧反应（OER）机制的密度泛函理论（DFT）计算与实验结果吻合良好，表明速率决定步骤的超电势降低。_{此外，基于X射线衍射（XRD）测量和X射线光电子能谱（XPS）结果的DFT计算模型为所制备的α-Fe 2} O ₃和α-Fe ₂ O ₃ @提供了精确的水分解机制。Rh 纳米棒。由于载流子生成和空穴传输增强，与原始α-Fe ₂ O 3 相比，最佳 α-Fe 2 O ₃ @ _Rh3样品的光电流密度增加了 78%，在 1.23 V _RHE^{下达到 1.12 mA/}_cm –2纳米棒电极。

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Surface Rh-Boosted Photoelectrochemical Water Oxidation of α-Fe2O3 by Reduced Overpotential in the Rate-Determining Step

The photoelectrochemical behavior of Rh cluster-deposited hematite (α-Fe₂O₃) photoanodes (α-Fe₂O₃@Rh) was investigated. The interactions between Rh clusters and α-Fe₂O₃ nanorods were elucidated both experimentally and computationally. A facile UV-assisted solution casting deposition method allowed the deposition of 2 nm Rh clusters on α-Fe₂O₃. The deposited Rh clusters effectively enhanced the photoelectrochemical performance of the α-Fe₂O₃ photoanode, and electrochemical impedance spectroscopy (EIS) and Mott–Schottky analysis were applied to understand the working mechanism for the α-Fe₂O₃@Rh photoanodes. The results revealed a distinctive carrier transport mechanism for α-Fe₂O₃@Rh and increased carrier density, while the absorbance spectra remained unchanged. Furthermore, density functional theory (DFT) calculations of the oxygen evolution reaction (OER) mechanism corresponded well with the experimental results, indicating a reduced overpotential of the rate-determining step. In addition, DFT calculation models based on the X-ray diffraction (XRD) measurements and X-ray photoelectron spectroscopy (XPS) results provided precise water-splitting mechanisms for the fabricated α-Fe₂O₃ and α-Fe₂O₃@Rh nanorods. Owing to enhanced carrier generation and hole transfer, the optimum α-Fe₂O₃@Rh3 sample showed 78% increased photocurrent density, reaching 1.12 mA/cm^–2 at 1.23 V_RHE compared to that of the pristine α-Fe₂O₃ nanorods electrode.

更新日期：2023-07-25

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