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Hematite Nanorods Photoanodes Decorated by Cobalt Hexacyanoferrate: The Role of Mixed Oxidized States on the Enhancement of Photoelectrochemical Performance
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-09-14 , DOI: 10.1021/acsaem.0c01782 Saulo Amaral Carminati 1 , Bruno Leuzinger da Silva 1 , José Luiz Bott-Neto 1 , Mauricio Alves de Melo 2 , Miguel Tayar Galante 1 , Pablo Sebástian Fernández 1 , Claudia Longo 1 , Juliano Alves Bonacin 1 , Ana Flávia Nogueira 1
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2020-09-14 , DOI: 10.1021/acsaem.0c01782 Saulo Amaral Carminati 1 , Bruno Leuzinger da Silva 1 , José Luiz Bott-Neto 1 , Mauricio Alves de Melo 2 , Miguel Tayar Galante 1 , Pablo Sebástian Fernández 1 , Claudia Longo 1 , Juliano Alves Bonacin 1 , Ana Flávia Nogueira 1
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In this work, we report on the incorporation of cobalt hexacyanoferrate (Co-NC-Fe) with different iron oxidation states (FeII and FeIII) on hematite (α-Fe2O3) nanorod photoanodes with a systematic investigation of enhanced photoelectrochemical performance under a neutral pH. A detailed investigation using in situ techniques was carried out to understand the fundamental aspects of chemical reactions during photoelectrochemical characterization. The α-Fe2O3/Co-NC-Fe photoanodes showed a higher photoelectrochemical performance compared to the individual materials. Despite the higher achieved performance of α-Fe2O3/Co-NC-Fe, the elucidation of the main contribution upon Co-NC-Fe incorporation was found to be dependent on the different charge transfer mechanism under light illumination. Therefore, given the complexity of the redox processes that take place in Co-NC-Fe under an applied bias, we have systematically investigated the dark- and light-induced effects on α-Fe2O3/Co-NC-Fe by in situ UV–vis and Fourier transform infrared spectroscopies. These techniques allowed us to monitor the effect of the electro and photoelectrochemical potential in several redox processes. The insightful results indicate that, in addition to surface state modification effects, the improvement of the photocurrent density may also result from long-lived holes at the electrode surface as a consequence of the electron transfer from the conduction band α-Fe2O3 to Co-NC-Fe with a FeIII oxidation state. This indicates a second electron pathway during charge separation, thereby contributing to the increase in the electron–hole pair lifetime and the accumulation of photogenerated holes at the α-Fe2O3/Co-NC-Fe photoanode surface to drive water oxidation.
中文翻译：
六氰合铁酸钴修饰的赤铁矿纳米棒光阳极：混合氧化态对光电化学性能增强的作用
在这项工作中，我们对钴氰化铁（联合NC-Fe）的不同的铁氧化态（Fe的掺入报告II和铁III赤铁矿）（的α-Fe 2 Ø 3）纳米棒的光阳极具有增强光电的系统调查在中性pH下的性能。使用原位技术进行了详细的研究，以了解光电化学表征过程中化学反应的基本方面。所述的α-Fe 2 ö 3相比于单独材料/共NC-铁光阳极表现出较高的光电化学性能。尽管更高达到的性能的α-Fe 2 ö 3/ Co-NC-Fe，发现对掺入Co-NC-Fe的主要贡献取决于光照射下不同的电荷转移机制。因此，考虑到的是采取联合NC-铁地方所施加的偏压下的氧化还原过程的复杂性，我们已经系统地研究上的α-Fe的黑暗和光照诱导的效应2 ö 3 / Co的-NC-铁通过在原位紫外可见和傅里叶变换红外光谱。这些技术使我们能够在几种氧化还原过程中监测电势和光电化学势的影响。通透的结果表明，除了表面状态改性效果，光电流密度的改善也可以从在电极表面处的长寿命孔从导带中的电子转移的结果产生的α-Fe 2 ö 3至具有Fe III氧化态的Co-NC-Fe 。这表明在电荷分离的第二电子通路，从而有助于在电子-空穴对的寿命的增加和光生空穴的在积累的α-Fe 2 ö 3/ Co-NC-Fe光电阳极表面可驱动水氧化。
更新日期：2020-10-26
中文翻译：
六氰合铁酸钴修饰的赤铁矿纳米棒光阳极：混合氧化态对光电化学性能增强的作用
在这项工作中，我们对钴氰化铁（联合NC-Fe）的不同的铁氧化态（Fe的掺入报告II和铁III赤铁矿）（的α-Fe 2 Ø 3）纳米棒的光阳极具有增强光电的系统调查在中性pH下的性能。使用原位技术进行了详细的研究，以了解光电化学表征过程中化学反应的基本方面。所述的α-Fe 2 ö 3相比于单独材料/共NC-铁光阳极表现出较高的光电化学性能。尽管更高达到的性能的α-Fe 2 ö 3/ Co-NC-Fe，发现对掺入Co-NC-Fe的主要贡献取决于光照射下不同的电荷转移机制。因此，考虑到的是采取联合NC-铁地方所施加的偏压下的氧化还原过程的复杂性，我们已经系统地研究上的α-Fe的黑暗和光照诱导的效应2 ö 3 / Co的-NC-铁通过在原位紫外可见和傅里叶变换红外光谱。这些技术使我们能够在几种氧化还原过程中监测电势和光电化学势的影响。通透的结果表明，除了表面状态改性效果，光电流密度的改善也可以从在电极表面处的长寿命孔从导带中的电子转移的结果产生的α-Fe 2 ö 3至具有Fe III氧化态的Co-NC-Fe 。这表明在电荷分离的第二电子通路，从而有助于在电子-空穴对的寿命的增加和光生空穴的在积累的α-Fe 2 ö 3/ Co-NC-Fe光电阳极表面可驱动水氧化。
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