Photoelectrochemical driving and simultaneous synthesis of 3-pyridinecarboxylic acid and hydrogen in WO3 photoanode-based cell
Photoelectrochemical driving and simultaneous synthesis of 3-pyridinecarboxylic acid and hydrogen in WO3 photoanode-based cell
复制标题
WO3光阳极电池中光电化学驱动并同时合成3-吡啶甲酸和氢气
DOI：
10.1149/2.0941913jes
复制
发表时间：
2019-09
影响因子：
3.9
通讯作者：
Yong Zhou
中科院分区：
文献类型：
--
作者：
Yi Tang;Bo Wu;Huichao He;Cheng Fu;Jun Wang;Kun Liu;Gaili Ke;Yong Zhou
在传统的太阳能水分解光电化学（PEC）电池中，其太阳能制氢效率受到其光阳极上缓慢的氧气析出的限制。3-吡啶甲酸（3-PA）是一种重要的有机化工原料，但其传统的合成方法存在诸多不足。为了提高PEC电池的析氢效率和产品附加值，本文报道了以3-甲基吡啶（3-MP）氧化为3-PA替代WO 3光阳极上的析氧。在以WO 3膜为光阳极的双室光电转换电池中，同时合成了3-PA和氢气。由于3-MP氧化成3-PA比水氧化在热力学和动力学上更有利，因此相对于用于水裂解的常规PEC电池，在具有3-PA合成功能的PEC电池中实现了更高的析氢效率。研究表明，WO 3光阳极上3-MP氧化为3-PA的反应是由光生空穴和来自WO 3上太阳能水氧化双空穴途径的H2 O2中间体共同引发的.此外，Cr2 O 72-/Cr 3+氧化还原对可以介导和促进WO 3光阳极氧化3-MP生成3-PA，因此，在H2SO 4-3-MP电解液中添加Cr 3+可以提高3-PA的PEC合成效率.
In conventional photoelectrochemical (PEC) cell for solar water splitting, its solar-to-hydrogen efficiency is limited by the sluggish oxygen evolution on its photoanode. 3-pyridinecarboxylic acid (3-PA) is an important organic in industry, but there are several disadvantages in its conventional synthesis approaches. Here, we reported that the oxidation of 3-methylpyridine (3-MP) into 3-PA as an alternative to the oxygen evolution on WO 3 photoanode for improving the hydrogen-evolution efficiency and the product added-value of PEC cell. In a WO 3 film photoanode-based dual-chamber PEC cell, 3-PA and hydrogen were simultaneously synthetized. Since the oxidation of 3-MP into 3-PA is more thermodynamically and kinetically favorable than water oxidation, higher efficiency of hydrogen evolution was achieved in the PEC cell with function of 3-PA synthesis relative to the conventional PEC cell for water splitting. Our investigations indicated that the oxidation of 3-MP into 3-PA on WO 3 photoanode is co-initiated by the photogenerated holes and the H 2 O 2 intermediate that originated from two-holes pathway of solar water oxidation on WO 3. Additionally, the Cr 2 O 7 2−/Cr 3+ redox pair could mediate and promote the oxidation of 3-MP into 3-PA on WO 3 photoanode, and thus the PEC efficiency of 3-PA synthesis can be improved by adding Cr 3+ into the H 2 SO 4-3-MP electrolyte.
登录
查看更多内容
影响因子：
11.9
作者：
He, Huichao;Berglund, Sean P.;Mullins, C. Buddie
通讯作者：
Mullins, C. Buddie
影响因子：
15
作者：
S. McElvain;M. Goese
通讯作者：
S. McElvain;M. Goese
影响因子：
3.6
作者：
C. DePuy;S. Kass;G. P. Bean
通讯作者：
C. DePuy;S. Kass;G. P. Bean
影响因子：
3.6
作者：
Kalanur, Shankara S.;Duy, Le Thai;Seo, Hyungtak
通讯作者：
Seo, Hyungtak
影响因子：
8.3
作者：
Hong Ju;Yan Li
通讯作者：
Hong Ju;Yan Li