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1.
Angew Chem Int Ed Engl ; 61(26): e202204948, 2022 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-35560974

RESUMO

Photocatalytic conversion of CO2 into transportable fuels such as formic acid (HCOOH) under sunlight is an attractive solution to the shortage of energy and carbon resources as well as to the increase in Earth's atmospheric CO2 concentration. The use of abundant elements as the components of a photocatalytic CO2 reduction system is important, and a solid catalyst that is active, recyclable, nontoxic, and inexpensive is strongly demanded. Here, we show that a widespread soil mineral, alpha-iron(III) oxyhydroxide (α-FeOOH; goethite), loaded onto an Al2 O3 support, functions as a recyclable catalyst for a photocatalytic CO2 reduction system under visible light (λ>400 nm) in the presence of a RuII photosensitizer and an electron donor. This system gave HCOOH as the main product with 80-90 % selectivity and an apparent quantum yield of 4.3 % at 460 nm, as confirmed by isotope tracer experiments with 13 CO2 . The present work shows that the use of a proper support material is another method of catalyst activation toward the selective reduction of CO2 .

2.
Commun Chem ; 3(1): 129, 2020 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-36703370

RESUMO

The development of simple catalysts with high performance in the selective oxidation of methane to syngas at low temperature has attracted much attention. Here we report a nickel-based solid catalyst for the oxidation of methane, synthesised by a facile impregnation method. Highly dispersed ultra-small NiO particles of 1.6 nm in size are successfully formed on the MOR-type zeolite. The zeolite-supported nickel catalyst gives continuously 97-98% methane conversion, 91-92% of CO yield with a H2/CO ratio of 2.0, and high durability without serious carbon deposition onto the catalyst at 973 K. DFT calculations demonstrate the effect of NiO particle size on the C-H dissociation process of CH4. A decrease in the NiO particle size enhances the production of oxygen originating from the NiO nanoparticles, which contributes to the oxidation of methane under a reductive environment, effectively producing syngas.

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