Unlocking bimetallic active sites via a desalination strategy for photocatalytic reduction of atmospheric carbon dioxide

Abstract

Ultrathin two-dimensional (2D) metal oxyhalides exhibit outstanding photocatalytic properties with unique electronic and interfacial structures. Compared with monometallic oxyhalides, bimetallic oxyhalides are less explored. In this work, we have developed a novel top-down wet-chemistry desalination approach to remove the alkali-halide salt layer within the complicated precursor bulk structural matrix Pb0.6Bi1.4Cs0.6O2Cl2, and successfully fabricate a new 2D ultrathin bimetallic oxyhalide Pb0.6Bi1.4O2Cl1.4. The unlocked larger surface area, rich bimetallic active sites, and faster carrier dynamics within Pb0.6Bi1.4O2Cl1.4 layers significantly enhance the photocatalytic efficiency for atmospheric CO2 reduction. It outperforms the corresponding parental matrix phase and other state-of-the-art bismuth-based monometallic oxyhalides photocatalysts. This work reports a top-down desalination strategy to engineering ultrathin bimetallic 2D material for photocatalytic atmospheric CO2 reduction, which sheds light on further constructing other ultrathin 2D catalysts for environmental and energy applications from similar complicate structure matrixes.

State-of-the-art advancements of atomically thin two-dimensional photocatalysts for energy conversion

“…The unlocked larger surface area, rich bimetallic active sites, and faster carrier dynamics within Pb 0.6 Bi 1.4 O 2 Cl 1.4 layers significantly enhance the photocatalytic efficiency for atmospheric CO 2 reduction. 142 Ultrathin 2D photocatalysts also display effective regulation of product selectivity for CO 2 reduction. Atomically thin, singlecrystalline InVO 4 sheets exposing (110) facets with a uniform thickness of B1.5 nm possess high selectivity for transformation of CO 2 to CO in the presence of water vapor, relative to the referred nanocubes with an exposed (100) facet.…”

“…The unlocked larger surface area, rich bimetallic active sites, and faster carrier dynamics within Pb 0.6 Bi 1.4 O 2 Cl 1.4 layers significantly enhance the photocatalytic efficiency for atmospheric CO 2 reduction. 142…”

Identification of the Active Sites on Metallic MoO2−xNano‐Sea‐Urchin for Atmospheric CO2Photoreduction Under UV, Visible, and Near‐Infrared Light Illumination

“…[19] From reported works and this study, it can be found that the adsorption and activation of CO 2 on the surface of photocatalysts would be influenced by the competitive O 2 adsorption in atmospheric CO 2 reduction process. [18,19] Therefore, we further added different amounts of O 2 in pure CO 2 to study the effect of O 2 on the selectivity of products in PCR (Figure S23). When the volume of added oxygen increased from 0 to 10 mL, the yield of CH 4 decreased and the yield of CO increased, which confirmed that the presence of O 2 changed the selectivity of products in PCR, which is consistent with previous reports.…”

Constructing a built-in electric field by anchoring highly dispersed Zn single atoms on UiO-66-NH2 for efficient CO2 photoreduction

“…Excessive emissions of CO 2 can lead to many intractable environmental issues. [1][2][3][4][5] In this context, in September 2020, our country put forward "peaking carbon emissions by 2030 and achieving carbon neutrality by 2060". 6 Moreover, the "double carbon" target was incorporated into the general layout of ecological civilization construction, aiming to solve a series of problems caused by the greenhouse effect.…”