Embedding of a ruthenium(ii) water oxidation catalyst into nanofibers via self-assembly

2015 ◽  
Vol 51 (2) ◽  
pp. 290-293 ◽  
Author(s):  
Valentin Kunz ◽  
Vladimir Stepanenko ◽  
Frank Würthner

Self-assembled nanofibers of a ruthenium(ii)–PBI complex exhibited an appreciable catalytic performance in the oxidative water splitting reaction.

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Yong Zhu ◽  
Degao Wang ◽  
Qing Huang ◽  
Jian Du ◽  
Licheng Sun ◽  
...  

Abstract Understanding and controlling the properties of water-splitting assemblies in dye-sensitized photoelectrosynthesis cells is a key to the exploitation of their properties. We demonstrate here that, following surface loading of a [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) chromophore on nanoparticle electrodes, addition of the molecular catalysts, Ru(bda)(L)2 (bda  =  2,2′-bipyridine-6,6′-dicarboxylate) with phosphonate or pyridyl sites for water oxidation, gives surfaces with a 5:1 chromophore to catalyst ratio. Addition of the surface-bound phosphonate derivatives with L = 4-pyridyl phosphonic acid or diethyl 3-(pyridin-4-yloxy)decyl-phosphonic acid, leads to well-defined surfaces but, following oxidation to Ru(III), they undergo facile, on-surface dimerization to give surface-bound, oxo-bridged dimers. The dimers have a diminished reactivity toward water oxidation compared to related monomers in solution. By contrast, immobilization of the Ru-bda catalyst on TiO2 with the 4,4′-dipyridyl anchoring ligand can maintain the monomeric structure of catalyst and gives relatively stable photoanodes with photocurrents that reach to 1.7 mA cm−2 with an optimized, applied bias photon-to-current efficiency of 1.5%.


2019 ◽  
Vol 14 (1) ◽  
Author(s):  
Zhou Cao ◽  
Yanling Yin ◽  
Peng Fu ◽  
Dong Li ◽  
Yulan Zhou ◽  
...  

Abstract Converting solar energy into sustainable hydrogen fuel by photoelectrochemical (PEC) water splitting is a promising technology to solve increasingly serious global energy supply and environmental issues. However, the PEC performance based on TiO2 nanomaterials is hindered by the limited sunlight-harvesting ability and its high recombination rate of photogenerated charge carriers. In this work, layered SnS2 absorbers and CoOx nanoparticles decorated two-dimensional (2D) TiO2 nanosheet array photoelectrode have been rationally designed and successfully synthesized, which remarkably enhanced the PEC performance for water splitting. As the result, photoconversion efficiency of TiO2/SnS2/CoOx and TiO2/SnS2 hybrid photoanodes increases by 3.6 and 2.0 times under simulated sunlight illumination, compared with the bare TiO2 nanosheet arrays photoanode. Furthermore, the TiO2/SnS2/CoOx photoanode also presented higher PEC stability owing to CoOx catalyst served as efficient water oxidation catalyst as well as an effective protectant for preventing absorber photocorrosion.


Nanoscale ◽  
2019 ◽  
Vol 11 (7) ◽  
pp. 3378-3385 ◽  
Author(s):  
Changhong Zhan ◽  
Zheng Liu ◽  
Yang Zhou ◽  
Mingliang Guo ◽  
Xiaolin Zhang ◽  
...  

Electrochemical water splitting requires an efficient water oxidation catalyst to accelerate the oxygen evolution reaction (OER).


2011 ◽  
Vol 4 (7) ◽  
pp. 2389 ◽  
Author(s):  
Gary F. Moore ◽  
James D. Blakemore ◽  
Rebecca L. Milot ◽  
Jonathan F. Hull ◽  
Hee-eun Song ◽  
...  

2016 ◽  
Vol 1 (1) ◽  
pp. 231-236 ◽  
Author(s):  
Matthew V. Sheridan ◽  
Benjamin D. Sherman ◽  
Rodolfo L. Coppo ◽  
Degao Wang ◽  
Seth L. Marquard ◽  
...  

2021 ◽  
Author(s):  
Fei Wang ◽  
Xiaoxian Sun ◽  
Yi Wang ◽  
Huawei Zhou ◽  
Jie Yin ◽  
...  

The surface treatment method has a great influence on the structure and properties of applied materials for interface catalysis. In this study, we prepare Ni(OH)<sub>2</sub>·NiO/FeOOH by surface treatment in acid solution using oxidation-corrosion equilibrium (OCE). For comparison, we also treat Ni foam with the same process in alkaline solution. Ni(OH)<sub>2</sub>·NiO/FeOOH can arrive steady-morphology and metallization by oxidation-corrosion equilibrium and exhibits superior catalytic activity as water oxidation catalyst. Ni(OH)<sub>2</sub>·NiO/FeOOH(OCE) needs only 232 mV to reach a current density of 10 mA cm<sup>-2</sup>, while it is 254 mV for a reference IrO<sub>2</sub>/Ni foam. The mechanism study shows that the small charge transfer resistance (2.04 Ωcm<sup>2</sup>) is favorable for the rapid interface electron exchange between Ni(OH)<sub>2</sub>·NiO/FeOOH(OCE) and reactive species in water oxidation. In addition, the results of X-ray photoelectron spectroscopy and series impedance show that the catalyst is metallic property in virtue of exposed mental Ni in Ni(OH)<sub>2</sub>·NiO/FeOOH(OCE). The volume ratio of hydrogen to oxygen (about 2:1) indicates overall water splitting by the double electrode system. When the volume ratio of hydrogen to oxygen is 2:1, the Faraday efficiency of H<sub>2</sub> or O<sub>2</sub> is close to 100%. Ni(OH)<sub>2</sub>·NiO/FeOOH(OCE) exhibits good stability for one month. The research results provide a feasible approach for finding low cost metallized catalysts to replace noble metal as water oxidation catalysts and improving the efficiency of water splitting.


2011 ◽  
Vol 83 (8) ◽  
pp. 1529-1542 ◽  
Author(s):  
Francesca Maria Toma ◽  
Andrea Sartorel ◽  
Mauro Carraro ◽  
Marcella Bonchio ◽  
Maurizio Prato

Carbon nanotubes (CNTs) are versatile nanomaterials with applications spanning from medicinal chemistry and biology, to electronics as field effect transistors or energy as fuel cells. The major drawback stems from the CNT insolubility in most of the organic and aqueous media, which severely hampers the material processability. To overcome this problem, functionalization of CNTs is generally accomplished by either covalent strategies resulting in the modification of the CNT backbone via radical reactions, fluorination, and/or cycloaddition reactions, or noncovalent protocols, exploiting multiple weak interactions (hydrophobic, van der Waals, electrostatic) with suitable reagents. Herein, we highlight that a rewarding approach includes a combination of covalent/noncovalent methods, by a tailored synthetic modification of the CNT surface with polycationic dendrimeric chains, fostering the successive decoration with a multimetallic and polyanionic water oxidation catalyst. The outcome is a hybrid nanomaterial with unperturbed CNT electrical properties, in close contact with a unique multi-electron catalyst enabling electrocatalytic water splitting with high efficiency at low overpotentials.


Polymers ◽  
2020 ◽  
Vol 12 (8) ◽  
pp. 1774
Author(s):  
Andrew Harrison ◽  
Michael P. Zeevi ◽  
Christopher L. Vasey ◽  
Matthew D. Nguyen ◽  
Christina Tang

Performing reactions in the presence of self-assembled hierarchical structures of amphiphilic macromolecules can accelerate reactions while using water as the bulk solvent due to the hydrophobic effect. We leveraged non-covalent interactions to self-assemble filled-polymer micelle nanoreactors (NR) incorporating gold nanoparticle catalysts into various amphiphilic polymer nanostructures with comparable hydrodynamic nanoreactor size and gold concentration in the nanoreactor dispersion. We systematically studied the effect of the hydrophobic co-precipitant on self-assembly and catalytic performance. We observed that co-precipitants that interact with gold are beneficial for improving incorporation efficiency of the gold nanoparticles into the nanocomposite nanoreactor during self-assembly but decrease catalytic performance. Hierarchical assemblies with co-precipitants that leverage noncovalent interactions could enhance catalytic performance. For the co-precipitants that do not interact strongly with gold, the catalytic performance was strongly affected by the hydrophobic microenvironment of the co-precipitant. Specifically, the apparent reaction rate per surface area using castor oil (CO) was over 8-fold greater than polystyrene (750 g/mol, PS 750); the turnover frequency was higher than previously reported self-assembled polymer systems. The increase in apparent catalytic performance could be attributed to differences in reactant solubility rather than differences in mass transfer or intrinsic kinetics; higher reactant solubility enhances apparent reaction rates. Full conversion of 4-nitrophenol was achieved within three minutes for at least 10 sequential reactions demonstrating that the nanoreactors could be used for multiple reactions.


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