4.6 Article

Highly efficient and selective photocatalytic CO2 reduction based on water-soluble CdS QDs modified by the mixed ligands in one pot

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 10, Issue 9, Pages 2821-2829

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cy00308e

Keywords

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Funding

  1. National Natural Science Foundation of China [21402113]
  2. National Natural Science Foundation of Shaanxi Province [2019JQ-175]
  3. Fundamental Research Funds for the Central Universities [GK201802033, GK201903041]

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To date, the facile preparation of photocatalysts with high efficiency, selectivity and photostability to promote CO2 conversion remains a big challenge. Here, we fabricated a novel photocatalyst, namely, MPA&MUA QDs prepared from CdS quantum dots (QDs) anchored by mixed MPA (3-mercaptopronic acid) and MUA (11-mercaptoalkanoic acid) ligands in one pot. Assisted by the sacrificial agent, the MPA&MUA QDs exhibited excellent performance and selectivity for photocatalytic CO2 reduction to carbonaceous products HCOOH, CO and CH4 with the corresponding rates of 2.8, 5.4 x 10(-2) and 6.3 x 10(-3) mu mol mg(cat)(-1) h(-1), respectively, under irradiation for 32 h. The apparent quantum efficiency (AQE) for the production of HCOOH achieved a high value up to 23.2%, while for CO and CH4, it was 0.4% and 0.2%, respectively. The attractive duration for photocatalysis under irradiation implied that the MPA&MUA QDs possessed enhanced photostability. Compared with the QDs solely decorated by MPA or MUA, the MPA&MUA QDs could enhance the energy gap E-g and tune the conduction band to smoothly generate CH4, CO and HCOOH. From the combination of steady-state photoluminescence and time-resolved lifetime, we inferred that the MPA&MUA coatings had a decreased number of available hole trapping sites and improved passivation on the surface, which allowed for efficient hole and electron migration. With this work, we introduce a facial and feasible strategy to create an inexpensive and efficient visible-light photocatalyst for the multi-electron reduction of CO2.

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