Developing Atomically Thin Li_1.81H_0.19Ti₂O₅·2H₂O Nanosheets for Selective Photocatalytic CO₂ Reduction to CO

Abstract

Solar-driven CO2 conversion to carbon-based fuels is an attractive approach to alleviate the worsening global climate change and increasing energy issues. However, exploring and designing efficient photocatalysts with excellent activity and stability still remain challenging. Herein, layered Li1.81H0.19Ti2O5·2H2O (LHTO) nanosheets were explored as the photocatalyst for photocatalytic CO2 reduction, and atomically thin LHTO nanosheets with one-unit-cell thickness were successfully constructed for photocatalytic CO2 reduction. The atomically thin LHTO nanosheets exhibited excellent performance for CO2 photoreduction to CO, with a yield rate of 4.0 μmol g–1 h–1, a selectivity of 93%, and over 25 h photostability, dramatically outperforming the bulk LHTO. The better performance of the atomically thin LHTO nanosheets was experimentally verified to benefit from more sites for CO2 adsorption, faster electron transfer rate, and a more negative conduction band edge compared with bulk LHTO. This work provided a methodological basis for designing more efficient photocatalytic CO2 reduction catalysts.

Visible-Light-Driven Reduction of CO2 to CO with Highly Active and Selective Earth-Abundant Metal Porphyrin-Conjugated Organic Polymers

“…2−6 The most important part of this work is the construction of photocatalysts. Although some inorganic oxides 7,8 or some organic semiconductor materials (MOFs, COFs, COPs, etc. ), have been reported for photocatalytic reduction of CO 2 , 9,10 complexes of noble metals such as Ru, Ir, Rh, and Re are usually added as visible-light photosensitizers to achieve higher catalytic yields.…”

“…Photosynthesis by plants can mitigate this phenomenon by converting CO 2 and water into oxygen and carbohydrates under sunlight irradiation, inspiring researchers to explore simulated plant photosynthesis and develop artificial photocatalytic systems that convert CO 2 into economically valuable chemical products, such as CH 4 , CO, and CH 3 OH. − The most important part of this work is the construction of photocatalysts. Although some inorganic oxides , or some organic semiconductor materials (MOFs, COFs, COPs, etc. ), have been reported for photocatalytic reduction of CO 2 , , complexes of noble metals such as Ru, Ir, Rh, and Re are usually added as visible-light photosensitizers to achieve higher catalytic yields. − But in fact, these materials containing noble metals are difficult to promote their large-scale commercial application due to the high cost and scarcity.…”