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Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO.

ABSTRACT: Formic acid is considered a promising energy carrier and hydrogen storage material for a carbon-neutral economy. We present an inexpensive system for the selective room-temperature photocatalytic conversion of formic acid into either hydrogen or carbon monoxide. Under visible-light irradiation (λ>420 nm, 1 sun), suspensions of ligand-capped cadmium sulfide nanocrystals in formic acid/sodium formate release up to 116±14 mmol H2 g(cat)(-1) h(-1) with >99% selectivity when combined with a cobalt co-catalyst; the quantum yield at λ=460 nm was 21.2±2.7%. In the absence of capping ligands, suspensions of the same photocatalyst in aqueous sodium formate generate up to 102±13 mmol CO g(cat)(-1) h(-1) with >95% selectivity and 19.7±2.7% quantum yield. H2 and CO production was sustained for more than one week with turnover numbers greater than 6×10(5) and 3×10(6), respectively.

SUBMITTER: Kuehnel MF

PROVIDER: S-EPMC4552973 | biostudies-literature | 2015 Aug

REPOSITORIES: biostudies-literature

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Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO.

Kuehnel Moritz F MF Wakerley David W DW Orchard Katherine L KL Reisner Erwin E

Angewandte Chemie (International ed. in English) 20150716 33

Formic acid is considered a promising energy carrier and hydrogen storage material for a carbon-neutral economy. We present an inexpensive system for the selective room-temperature photocatalytic conversion of formic acid into either hydrogen or carbon monoxide. Under visible-light irradiation (λ>420 nm, 1 sun), suspensions of ligand-capped cadmium sulfide nanocrystals in formic acid/sodium formate release up to 116±14 mmol H2 g(cat)(-1) h(-1) with >99% selectivity when combined with a cobalt co ...[more]

PMID: 26201752

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Project description:A combined approach for CO2 capture and photoreduction provides a comprehensive solution to address exhaust emissions. This study aims to develop a hybrid system integrating membrane contactor and photocatalytic technology for CO2 conversion to formic acid by optimizing the synthesis of ZnO-ZnS heterojunction photocatalysts through controlled variations in precursor concentrations and calcination temperatures. The catalysts are characterized to assess their structural and optical properties, photocatalytic activity, stability and reaction kinetics. Additionally, the photocatalytic performance is also tested using a model gas composition that simulates power plant emission with UV or visible light serving as the energy source. The synthesized ZnO-ZnS catalysts exhibit diffraction patterns consistent with standard references, with a measured band gap interval of 3.06-3.13 eV. Among the three most effective catalysts, labeled as Z1 (ZnO:ZnS ratio of 1:2 at 400 °C), Z2 (ZnO:ZnS ratio of 1:1 at 400 °C), and Z4 (ZnO:ZnS ratio of 1:2 at 500 °C), the formic acid yields were 0.643, 0.554, and 0.626 mmol/(L gcat h), respectively. The highest yield, 0.936 mmol/(L gcat), was achieved under a low CO2 feed gas concentration (15 vol%). Furthermore, under LED irradiation, the Z1 catalyst produced a formic acid yield of 0.394 mmol/(L gcat) after 4 h, demonstrating higher selectivity for formic acid production. Electrochemical impedance spectroscopy (EIS) analysis shows that Z1 exhibits lower resistance, enhancing charge transfer efficiency. Scanning electron microscopy (SEM) analysis reveals nanorod-like ZnO and globular ZnS structures ranging from 50 to 100 nm, while high-resolution transmission electron microscopy (HRTEM) confirms the presence of ZnO-ZnS diffraction patterns. After 4 h of photocatalytic test, the XRD analysis confirmed that most of the ZnO-ZnS catalyst peaks remained intact, indicating structural stability. Ultimately, the optimized ZnO-ZnS catalysts demonstrate promising efficiency for selective CO2 conversion to formic acid under visible light, offering a viable approach for emission reduction through advanced hybrid membrane-photocatalytic technology.

Dataset Information

Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO.

Publications

Photocatalytic Formic Acid Conversion on CdS Nanocrystals with Controllable Selectivity for H2 or CO.

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