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1.
ChemSusChem ; 16(5): e202201901, 2023 Mar 08.
Artículo en Inglés | MEDLINE | ID: mdl-36524753

RESUMEN

Stable and efficient SnO2 electrodes are very promising for effectively degrading refractory organic pollutants in wastewater treatment. In this regard, we firstly prepared Ti3+ self-doped urchin-like rutile TiO2 nanoclusters (TiO2-x NCs) on a Ti mesh substrate by hydrothermal and electroreduction to serve as an interlayer for the deposition of Sb-SnO2 . The TiO2-x NCs/Sb-SnO2 anode exhibited a high oxygen evolution potential (2.63 V vs. SCE) and strong ⋅OH generation ability for the enhanced amount of absorbed oxygen species. Thus, the degradation results demonstrated its good rhodamine B (RhB), methylene blue (MB), alizarin yellow R (AYR), and methyl orange (MO) removal performance, with the rate constant increased 5.0, 1.9, 1.9, and 4.7 times, respectively, compared to the control Sb-SnO2 electrode. RhB and AYR degradation mechanisms are also proposed based on the results of high-performance liquid chromatography coupled with mass spectrometry and quenching experiments. More importantly, this unique rutile interlayer prolonged the anode lifetime sixfold, given its good lattice match with SnO2 and the three-dimensional concave-convex structure. Consequently, this work paves a new way for designing the crystal form and structure of the interlayers to obtain efficient and stable SnO2 electrodes for addressing dye wastewater problems.

2.
J Hazard Mater ; 430: 128440, 2022 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-35158250

RESUMEN

Stable electrode materials with high catalytic activity are urgently required for electrochemical degradation of refractory organic pollutants in wastewater treatment. Herein, high conductive MXene (Ti3C2Tx) was firstly fabricated by electrophoretic deposition (EPD) as an interlayer for preparing a novel PbO2 electrode. The well-conducted Ti3C2Tx interlayer significantly improved the electrochemical performance of the EPD-2.0/PbO2 (EPD time was 2.0 min) electrode with the charge transfer resistance decreased by 9.51 times, the inner active sites increased by 5.21 times and the ∙OH radicals generation ability enhanced by 4.07 times than the control EPD-0/PbO2 anode. Consequently, the EPD-2.0/PbO2 electrode achieved nearly 100% basic fuchsin (BF) and 86.78% COD removal efficiency after 3.0 h electrolysis. Therefore, this new PbO2 electrode presented a promising potential for electrochemical degradation of BF and the new Ti3C2Tx middle layer could also be used to fabricate other efficient and stable anodes, such as SnO2, MnO2, TiO2, etc.

3.
J Colloid Interface Sci ; 610: 653-662, 2022 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-34848059

RESUMEN

Electrocatalysts play important role in various energy conversion and storage devices. The catalytic performance of electrocatalysts can be enhanced through the increasement of intrinsic catalytic activity by optimizing electronic structure and the improvement of exposed active sites by designing proper nanostructures. In this work, CoS2@MoS2@NiS2 nano polyhedron with double-shelled structure was prepared using metal organic framework as a precursor. Due to the rational integration of multifunctional active center, the strong electronic interaction of the various component, the high electrochemical surface area and shortened mass transport induced by the special structure, CoS2@MoS2@NiS2 exhibits high catalytic activity for hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Specifically, low overpotentials of 156 and 200 mV was achieved to deliver a current density of 10 mA cm-2 for HER and OER, and a high half-wave potential of 0.80 V was observed for ORR. More importantly, the Zn-air battery assembled by CoS2@MoS2@NiS2 exhibits a high-power density of 80.28 mW cm-2 and could effectively drive overall water splitting. This work provides a new platform for designing multifunctional catalysts with high activity for energy conversion and storage.

4.
ChemSusChem ; 14(1): 73-93, 2021 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-33089643

RESUMEN

Single-atom catalysts (SACs) have attracted increasing research interests owing to their unique electronic structures, quantum size effects and maximum utilization rate of atoms. Metal organic frameworks (MOFs) are good candidates to prepare SACs owing to the atomically dispersed metal nodes in MOFs and abundant N and C species to stabilize the single atoms. In addition, the distance of adjacent metal atoms can be turned by adjusting the size of ligands and adding volatile metal centers to promote the formation of isolated metal atoms. Moreover, the diverse metal centers in MOFs can promote the preparation of dual-atom catalysts (DACs) to improve the metal loading and optimize the electronic structures of the catalysts. The applications of MOFs derived SACs and DACs for electrocatalysis, including oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction reaction and nitrogen reduction reaction are systematically summarized in this Review. The corresponding synthesis strategies, atomic structures and electrocatalytic performances of the catalysts are discussed to provide a deep understanding of MOFs-based atomic electrocatalysts. The catalytic mechanisms of the catalysts are presented, and the crucial challenges and perspectives are proposed to promote further design and applications of atomic electrocatalysts.

5.
Chem Sci ; 11(43): 11646-11671, 2020 Oct 06.
Artículo en Inglés | MEDLINE | ID: mdl-34094409

RESUMEN

Zinc-air batteries (ZABs) are regarded as ideal candidates for next-generation energy storage equipment due to their high energy density, non-toxicity, high safety, and environmental friendliness. However, the slow oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics on the air cathode limit their efficiency and the development of highly efficient, low cost and stable bifunctional electrocatalysts is still challenging. Metal-Organic Framework (MOF) based bifunctional oxygen electrocatalysts have been demonstrated as promising alternative catalysts due to the regular structure, tunable chemistry, high specific surface area, and simple and easy preparation of MOFs, and great progress has been made in this area. Herein, we summarize the latest research progress of MOF-based bifunctional oxygen electrocatalysts for ZABs, including pristine MOFs, derivatives of MOFs and MOF composites. The effects of the catalysts' composites, morphologies, specific surface areas and active sites on catalytic performances are specifically addressed to reveal the underlying mechanisms for different catalytic activity of MOF based catalysts. Finally, the main challenges and prospects for developing advanced MOF-based bifunctional electrocatalysts are proposed.

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