Photo-electrochemical hydrogen production from neutral phosphate buffer and seawater using micro-structured p-Si photo-electrodes functionalized by solution-based methods†,Sustainable Energy & Fuels

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Photo-electrochemical hydrogen production from neutral phosphate buffer and seawater using micro-structured p-Si photo-electrodes functionalized by solution-based methods†
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2018-08-16 00:00:00 , DOI: 10.1039/c8se00291f
Anurag Kawde _{1,

2,

3,

4,

5} , Alagappan Annamalai _{3,

6,

7} , Lucia Amidani _{4,

5,

8} , Manuel Boniolo _{3,

9,

10,

11} , Wai Ling Kwong _{3,

9,

10,

11} , Anita Sellstedt _{1,

3,

12,

13,

14} , Pieter Glatzel _{4,

5,

8} , Thomas Wågberg _{3,

6,

7} , Johannes Messinger _{1,

2,

3,

9,

10}

Affiliation

Solar fuels such as H₂ generated from sunlight and seawater using earth-abundant materials are expected to be a crucial component of a next generation renewable energy mix. We herein report a systematic analysis of the photo-electrochemical performance of TiO₂ coated, microstructured p-Si photo-electrodes (p-Si/TiO₂) that were functionalized with CoO_x and NiO_x for H₂ generation. These photocathodes were synthesized from commercial p-Si wafers employing wet chemical methods. In neutral phosphate buffer and standard 1 sun illumination, the p-Si/TiO₂/NiO_x photoelectrode showed a photocurrent density of −1.48 mA cm⁻² at zero bias (0 V_RHE), which was three times and 15 times better than the photocurrent densities of p-Si/TiO₂/CoO_x and p-Si/TiO₂, respectively. No decline in activity was observed over a five hour test period, yielding a Faradaic efficiency of 96% for H₂ production. Based on the electrochemical characterizations and the high energy resolution fluorescence detected X-ray absorption near edge structure (HERFD-XANES) and emission spectroscopy measurements performed at the Ti Kα₁ fluorescence line, the superior performance of the p-Si/TiO₂/NiO_x photoelectrode was attributed to improved charge transfer properties induced by the NiO_x coating on the protective TiO₂ layer, in combination with a higher catalytic activity of NiO_x for H₂-evolution. Moreover, we report here an excellent photo-electrochemical performance of p-Si/TiO₂/NiO_x photoelectrode in corrosive artificial seawater (pH 8.4) with an unprecedented photocurrent density of 10 mA cm⁻² at an applied potential of −0.7 V_RHE, and of 20 mA cm⁻² at −0.9 V_RHE. The applied bias photon-to-current conversion efficiency (ABPE) at −0.7 V_RHE and 10 mA cm⁻² was found to be 5.1%.

中文翻译：

使用基于溶液的方法功能化的微结构p-Si光电极从中性磷酸盐缓冲液和海水中产生光电化学制氢†

预计使用大量地球物质从太阳光和海水中产生的H ₂等太阳能燃料将成为下一代可再生能源组合的重要组成部分。我们在本文中报告了用CoO _x和NiO _x进行H ₂生成功能化的TiO ₂涂层，微结构化p-Si光电极（p-Si / TiO ₂）的光电化学性能的系统分析。这些光阴极是使用湿化学方法从商业化的p-Si晶片合成的。在中性磷酸盐缓冲液和标准1阳光照射下，p-Si / TiO ₂ / NiO _x光电极显示的光电流密度为-1.48 mA cm ^-2在零偏压（0 V _RHE）下，分别比p-Si / TiO ₂ / CoO _x和p-Si / TiO ₂的光电流密度高三倍和15倍。在五个小时的测试期间未观察到活性降低，产生H ₂的法拉第效率为96％。基于电化学表征和高能量分辨率荧光来检测邻近处的TiKα执行边缘结构（HERFD-XANES）和发射光谱的测量X射线吸收_1条荧光线，对p-Si / TiO 2的性能优越₂ /氧化镍_x光电极归因于NiO诱导的电荷转移性能提高在保护性TiO₂层上涂覆_x涂层，以及NiO_x对H₂析出具有更高的催化活性。此外，我们在此报告p-Si / TiO₂ / NiO_x光电极在腐蚀性人工海水（pH 8.4）中具有优异的光电化学性能，在-0.7 V_RHE的施加电势下具有前所未有的10 mA cm^-2的光电流密度，在-0.9 V_RHE时为20 mA cm^-2。发现在-0.7 V_RHE和10 mA cm^-2时施加的偏置光子-电流转换效率（ABPE）为5.1％。

更新日期：2018-08-16

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