Carbon Encapsulation of Organic–Inorganic Hybrid Perovskite toward Efficient and Stable Photo‐Electrochemical Carbon Dioxide Reduction,Advanced Energy Materials

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Carbon Encapsulation of Organic–Inorganic Hybrid Perovskite toward Efficient and Stable Photo‐Electrochemical Carbon Dioxide Reduction
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-10-08 , DOI: 10.1002/aenm.202002105
Hefeng Zhang _{1,

2} , Yu Chen ₃ , Hong Wang _{1,

2} , Hui Wang ₁ , Weiguang Ma ₁ , Xu Zong ₁ , Can Li ₁

Affiliation

Photo‐electrochemical (PEC) carbon dioxide reduction to chemicals or fuels has been regarded as an attractive strategy that can close the anthropogenic carbon cycle. However, identifying a PEC system capable of driving efficient and durable CO₂ conversion remains a critical challenge. Herein, the fabrication of a sandwich‐like organic–inorganic hybrid perovskite‐based photocathode with carbon encapsulation for PEC CO₂ reduction is reported. The carbon encapsulation not only affords protection to the perovskite, but also allows for efficient conductance of photogenerated electrons. When decorated with a cobalt phthalocyanine molecular catalyst, the photocathode shows an onset potential at 0.58 V versus reversible hydrogen electrode (RHE) and a high photocurrent density of −15.5 mA cm⁻² at −0.11 V versus RHE in CO₂‐saturated 0.5 m KHCO₃ under AM 1.5G illumination (100 mW cm⁻²), which represents state‐of‐the‐art performance in this field. Moreover, the photocathode remains stable during a continuous reaction that lasted for 25 h. Unbiased PEC CO₂ reduction is further realized by integrating the photocathode with an amorphous Si photoanode in tandem, delivering a solar‐to‐CO energy conversion efficiency of 3.34% and a total solar‐to‐fuel energy conversion efficiency of 3.85%.

中文翻译：

有机-无机杂化钙钛矿的碳包封以实现高效稳定的光电电化学二氧化碳还原

将光电化学（PEC）二氧化碳还原为化学物质或燃料被认为是可以关闭人为碳循环的有吸引力的策略。然而，确定一种能够驱动高效且持久的CO ₂转化的PEC系统仍然是一项严峻的挑战。在此，据报道制造了一种三明治式的有机-无机杂化钙钛矿基光电阴极，该碳阴极具有用于PEC CO ₂还原的碳封装。碳封装不仅可以保护钙钛矿，还可以有效传导光生电子。当用钴酞菁分子催化剂修饰时，与可逆氢电极（RHE）相比，光电阴极在0.58 V时显示出开始电势，并且光电流密度为-15.5 mA cm在−0.11 V时为⁻²，而在AM 1.5G照度（100 mW cm ⁻²）下在CO _2中饱和的0.5 m KHCO _3中的RHE为^-2，代表了该领域的最新性能。此外，在持续25小时的连续反应过程中，光电阴极保持稳定。通过将光电阴极与非晶硅光电阳极串联在一起进一步实现无偏PEC CO _2的减少，实现的太阳能到CO的能量转换效率为3.34％，总的太阳能到燃料的能量转换效率为3.85％。

更新日期：2020-11-25

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