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Ideal dopant to increase charge separation efficiency in hematite photoanodes: germanium
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-06-08 , DOI: 10.1039/d2ta03932j
Murillo Henrique de Matos Rodrigues 1, 2 , Ingrid Rodriguez-Gutierréz 2, 3 , Carlos Alberto Ospina Ramirez 2 , Carlos Alberto Rodrigo Costa 2 , Cleyton Alexandre Biffe 2 , João Batista de Souza Junior 2 , Flavio Leandro Souza 2, 3 , Edson Roberto Leite 1, 2
Affiliation  

Hematite, owing to its ideal physical properties, chemical stability, and abundance on Earth, has become a potential candidate as a photoanode in solar water-splitting device applications. However, the high photogenerated charge recombination due to its low efficiency of charge separation as a consequence of poor electronic transport and collection at the back contact has hindered its commercial application. Based on the limitations of hematite, this study describes germanium as a potentially ideal element that combines the beneficial improvement in charge transfer efficiency and morphology control toward high hematite-based photoanode performance. Intensity-modulated photocurrent spectroscopy results demonstrated that the addition of Ge enhanced the charge mobility, leading to a superior charge separation efficiency compared to the pristine hematite photoanode. C-AFM measurements demonstrate that Ge improves the electronic conductivity and increases the majority carrier mobility. Photoelectrochemical measurements performed at different wavelengths show the Ge interferes with the formation of small polarons, making the charges more mobile (delocalized), thus favoring the process of photoinduced charge separation. The combined role played by Ge addition resulted in a significant improvement in the photoelectrochemical performance from 0.5 to 3.2 mA cm−2 at 1.23 VRHE by comparing the pristine and Ge–hematite-based photoanodes.

中文翻译:

提高赤铁矿光电阳极电荷分离效率的理想掺杂剂:锗

赤铁矿由于其理想的物理性质、化学稳定性和在地球上的丰富性,已成为太阳能水分解装置应用中作为光电阳极的潜在候选者。然而,由于背接触处的电子传输和收集差,导致电荷分离效率低,光生电荷复合的高光生电荷复合阻碍了其商业应用。基于赤铁矿的局限性,本研究将锗描述为一种潜在的理想元素,它结合了电荷转移效率和形态控制的有益改进,从而实现了基于赤铁矿的高光阳极性能。强度调制光电流光谱结果表明,Ge的添加增强了电荷迁移率,与原始赤铁矿光阳极相比,它具有更高的电荷分离效率。C-AFM 测量表明,Ge 提高了电子电导率并增加了多数载流子迁移率。在不同波长下进行的光电化学测量表明,Ge 会干扰小极化子的形成,使电荷更具移动性(离域),从而有利于光致电荷分离的过程。Ge 添加所起的综合作用导致光电化学性能从 0.5 到 3.2 mA cm 显着提高 使电荷更具移动性(离域),从而有利于光致电荷分离的过程。Ge 添加所起的综合作用导致光电化学性能从 0.5 到 3.2 mA cm 显着提高 使电荷更具移动性(离域),从而有利于光致电荷分离的过程。Ge 添加所起的综合作用导致光电化学性能从 0.5 到 3.2 mA cm 显着提高-2在 1.23 V RHE通过比较原始和基于 Ge-赤铁矿的光电阳极。
更新日期:2022-06-08
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