Efficient hydrogen peroxide synthesis by metal-free polyterthiophene via photoelectrocatalytic dioxygen reduction,Energy & Environmental Science

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Efficient hydrogen peroxide synthesis by metal-free polyterthiophene via photoelectrocatalytic dioxygen reduction
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2019-11-26 , DOI: 10.1039/c9ee02247c
Wenjun Fan _{1,

2,

3,

4,

5} , Bingqing Zhang _{1,

2,

3,

4,

5} , Xiaoyu Wang _{6,

7,

8,

9} , Weiguang Ma _{1,

2,

3,

4,

5} , Deng Li _{1,

2,

3,

4,

5} , Zhiliang Wang _{1,

2,

3,

4,

5} , Michel Dupuis _{6,

7,

8,

9} , Jingying Shi _{1,

2,

3,

4,

5} , Shijun Liao _{10,

11,

12,

13,

14} , Can Li _{1,

2,

3,

4,

5}

Affiliation

Solar hydrogen peroxide (H₂O₂) produced through the selective two-electron (2e⁻) oxygen reduction pathway is an ideal alternative to liquid fuel in addition to being a versatile chemical. Up to now, low photocatalytic activity, low selectivity and serious competing reactions have been big hurdles in the production of solar H₂O₂ in an efficient way. Herein, we report that polyterthiophene (pTTh), a metal-free narrow-bandgap polymeric semiconductor, is an efficient photocathode for H₂O₂ production in alkaline solution. We found that 2e⁻ selectivity for the ORR is dependent on the pH of electrolytes and approaches 100% at pH ∼ 13. A record-high H₂O₂ concentration of 110 mmol L⁻¹ is achieved, which is two orders of magnitude higher than the previous photosynthesized H₂O₂. Furthermore, NiFeO_x/BiVO₄–pTTh dual-photoelectrodes in photoelectrochemical devices enabled bias-free synthesis of solar H₂O₂ of concentration ∼90 mmol L⁻¹ for several cycles without any noticeable decay. This extremely high 2e⁻ selectivity is attributed to the intrinsic electrochemical properties of pTTh. Theoretical calculations suggested that the selectivity-determining step in the 2e⁻ process is over ∼200 times faster than that in the 4e⁻ pathway. Our work paves an alternative way of generating liquid solar fuel that is very promising for practical applications.

中文翻译：

光电催化双氧还原无金属聚噻吩高效合成过氧化氢

太阳能过氧化氢（H ₂ ö ₂）通过选择性二-电子（2E产生^-）氧还原途径是液体燃料的理想替代除了是一种多用途的化学品。迄今为止，低光催化活性，低选择性和严重的竞争反应一直是有效生产太阳能H ₂ O _2的主要障碍。在这里，我们报道聚对噻吩（pTTh），一种无金属的窄带隙聚合物半导体，是在碱性溶液中生产H ₂ O ₂的有效光电阴极。我们发现，2E ^-对ORR的选择性取决于电解质的pH值，并且在pH约为13时接近100％。达到了创纪录的110 mmol L ^-1的H ₂ O ₂浓度，这比先前的光合作用H高了两个数量级。₂ O ₂。此外，光电化学装置中的NiFeO _x / BiVO ₄ -pTTh双光电极可在几个循环中无偏合成约90 mmol L ^-1的浓度约为90 mmol L ^-1的太阳H ₂ O ₂，而不会出现任何明显的衰减。这种极其高2E ^-选择性归因于pTTh的固有电化学性质。理论计算表明，在图2e的选择性确定步骤^-工艺比快于4E以上〜200倍^-通路。我们的工作为产生液态太阳能的替代方法铺平了道路，这在实际应用中非常有前途。

更新日期：2019-11-26

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