Cupric porphyrin frameworks on multi-junction silicon photocathodes to expedite the kinetics of CO2 turnover,Nanoscale

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Cupric porphyrin frameworks on multi-junction silicon photocathodes to expedite the kinetics of CO2 turnover
Nanoscale ( IF 5.8 ) Pub Date : 2022-06-01 , DOI: 10.1039/d2nr01921c
Zhihe Wei _{1,

2} , Qiaoqiao Mu ₁ , Ronglei Fan ₂ , Yanhui Su ₁ , Yongtao Lu ₁ , Zhao Deng ₁ , Mingrong Shen ₂ , Yang Peng ₁

Affiliation

Photoelectrochemical CO₂ reduction utilizing silicon-based photocathodes offers a promising route to directly store solar energy in chemical bonds, provoking the development of heterogeneous molecular catalysts with high turnover rates. Herein, an in situ surface transformation strategy is adopted to grow metal–organic frameworks (MOFs) on Si-based photocathodes, serving as catalytic scaffolds for boosting both the kinetics and selectivity of CO₂ reduction. Benefitting from the multi-junctional configuration for enhanced charge separation and the porous MOF scaffold enriching redox-active metalloporphyrin sites, the Si photocathode demonstrates a high CO faradaic efficiency of 87% at a photocurrent density of 10.2 mA cm⁻², which is among the best seen for heterogeneous molecular catalysts. This study highlights the exploitation of reticular chemistry and macrocycle complexes as Earth-abundant alternatives for catalyzing artificial photosynthesis.

中文翻译：

多结硅光电阴极上的铜卟啉骨架加速 CO2 周转动力学

利用硅基光阴极进行光电化学 CO ₂还原提供了一条有前途的途径，可以直接将太阳能存储在化学键中，从而促进了具有高周转率的非均相分子催化剂的开发。在此，采用原位表面转化策略在硅基光电阴极上生长金属有机骨架（MOF），作为催化支架，提高CO ₂还原的动力学和选择性。得益于用于增强电荷分离的多结结构和富含氧化还原活性金属卟啉位点的多孔 MOF 支架，Si 光电阴极在 10.2 mA cm ^{-2的光电流密度下表现出 87% 的高 CO 法拉第效率}，这是多相分子催化剂中最好的。这项研究强调了利用网状化学和大环复合物作为地球上丰富的催化人工光合作用的替代品。

更新日期：2022-06-01

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