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1.
J Hazard Mater ; 444(Pt B): 130436, 2023 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-36435041

RESUMO

Surface hydroxyl groups play a decisive role in the generation of hydroxyl radicals with stronger oxidizing ability, which is indispensable in photocatalytic VOCs removal, especially under the condition of low humidity. In this work, non-noble amorphous SnO2 decorated ZnSn(OH)6 (ZSH) was synthesized by an in-situ method. The charge transport, reactant activation and hydroxyl polarization are enhanced through decoration of amorphous SnO2 on ZSH. Combined with the designed experiment, in-situ EPR, DTF calculation and in-situ DRIFTS, the role and mechanism of interfacial hydroxyl polarization are revealed on SnO2 decorated ZnSn(OH)6. Compared with pristine ZSH and noble-metal modified ZSH, the toluene degradation rate of amorphous SnO2 decorated ZSH is increased by 13.0 and 3.8 times, and the toluene mineralization rate is increased by 5.2 and 2.2 times. The ZSH-24 sample maintains a high toluene degradation activity after 6 cyclic utilization without catalyst deactivation. This work emphasizes the role of non-noble metal and the origin of hydroxyl group polarization on ZnSn(OH)6 for photocatalytic VOCs mineralization.

2.
J Colloid Interface Sci ; 639: 133-144, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36804786

RESUMO

A facile in-situ preparation strategy is proposed to anchor amorphous SnO2 nanoparticles into the porous N-doped carbon (NC) matrix to fabricate amorphous composite powders (am-SnO2@p-NC), which feature the hierarchically interconnected and well interlaced porous configurations by employing polyvinylpyrrolidone as the soft template. The morphology regulation of the porous structure is precisely realized by adjusting the content of the template and the relationship between structural evolution and electrochemical performance of composite powders is accurately described to explore the optimal template dosage. The results indicate that the am-SnO2@p-NC-50 % composite electrode can deliver the improved lithium storage capacity and cycling performance when the content of the template is controlled at 0.500 g, in which the initial discharge specific capacity is about 1557.6 mAh/g and the reversible value retains at 841.5 mAh/g after 100 cycles at 100 mA/g. Meanwhile, the discharge specific capacity of 869.8 mAh/g is exhibited for the am-SnO2@p-NC-50 % composite electrode after 60 cycles when the current density is recovered from 2000 to 100 mA/g. Moreover, the Li+ ions diffusion coefficient up to about 5.5 × 10-12 cm2/s is calculated from galvanostatic intermittent titration technique tests, which can be partly ascribed to the conductive NC substrate that provides the high electronic conductivity, and partly to the highly porous structure that shortens Li+ ions transfer pathways and guarantees the fast reaction kinetics. Therefore, the hierarchically porous engineering of carbon networks to confine amorphous transition metal oxide nanoparticles is of great significance in the development of high-performance anode materials for lithium-ion batteries.

3.
ACS Sens ; 7(7): 2058-2068, 2022 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-35757893

RESUMO

Two-dimensional (2D) transition metal dichalcogenides (TMDs) and metal chalcogenides (MCs), despite their excellent gas sensing properties, are subjected to spontaneous oxidation in ambient air, negatively affecting the sensor's signal reproducibility in the long run. Taking advantage of spontaneous oxidation, we synthesized fully amorphous a-SnO2 2D flakes (≈30 nm thick) by annealing in air 2D SnSe2 for two weeks at temperatures below the crystallization temperature of SnO2 (T < 280 °C). These engineered a-SnO2 interfaces, preserving all the precursor's 2D surface-to-volume features, are stable in dry/wet air up to 250 °C, with excellent baseline and sensor's signal reproducibility to H2S (400 ppb to 1.5 ppm) and humidity (10-80% relative humidity (RH)) at 100 °C for one year. Specifically, by combined density functional theory and ab initio molecular dynamics, we demonstrated that H2S and H2O compete by dissociative chemisorption over the same a-SnO2 adsorption sites, disclosing the humidity cross-response to H2S sensing. Tests confirmed that humidity decreases the baseline resistance, hampers the H2S sensor's signal (i.e., relative response (RR) = Ra/Rg), and increases the limit of detection (LOD). At 1 ppm, the H2S sensor's signal decreases from an RR of 2.4 ± 0.1 at 0% RH to 1.9 ± 0.1 at 80% RH, while the LOD increases from 210 to 380 ppb. Utilizing a suitable thermal treatment, here, we report an amorphization procedure that can be easily extended to a large variety of TMDs and MCs, opening extraordinary applications for 2D layered amorphous metal oxide gas sensors.

4.
ACS Appl Mater Interfaces ; 7(50): 27735-42, 2015 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-26606590

RESUMO

Amorphous SnO2 (a-SnO2) thin films were conformally coated onto the surface of reduced graphene oxide (G) using atomic layer deposition (ALD). The electrochemical characteristics of the a-SnO2/G nanocomposites were then determined using cyclic voltammetry and galvanostatic charge/discharge curves. Because the SnO2 ALD films were ultrathin and amorphous, the impact of the large volume expansion of SnO2 upon cycling was greatly reduced. With as few as five formation cycles best reported in the literature, a-SnO2/G nanocomposites reached stable capacities of 800 mAh g(-1) at 100 mA g(-1) and 450 mAh g(-1) at 1000 mA g(-1). The capacity from a-SnO2 is higher than the bulk theoretical values. The extra capacity is attributed to additional interfacial charge storage resulting from the high surface area of the a-SnO2/G nanocomposites. These results demonstrate that metal oxide ALD on high surface area conducting carbon substrates can be used to fabricate high power and high capacity electrode materials for lithium-ion batteries.

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