scholarly journals Zn- and Ti-Doped SnO2 for Enhanced Electroreduction of Carbon Dioxide

Materials ◽  
2021 ◽  
Vol 14 (9) ◽  
pp. 2354
Author(s):  
Katarzyna Bejtka ◽  
Nicolò B. D. Monti ◽  
Adriano Sacco ◽  
Micaela Castellino ◽  
Samuele Porro ◽  
...  

The electrocatalytic reduction of CO2 into useful fuels, exploiting rationally designed, inexpensive, active, and selective catalysts, produced through easy, quick, and scalable routes, represents a promising approach to face today’s climate challenges and energy crisis. This work presents a facile strategy for the preparation of doped SnO2 as an efficient electrocatalyst for the CO2 reduction reaction to formic acid and carbon monoxide. Zn or Ti doping was introduced into a mesoporous SnO2 matrix via wet impregnation and atomic layer deposition. It was found that doping of SnO2 generates an increased amount of oxygen vacancies, which are believed to contribute to the CO2 conversion efficiency, and among others, Zn wet impregnation resulted the most efficient process, as confirmed by X-ray photoelectron spectroscopy analysis. Electrochemical characterization and active surface area evaluation show an increase of availability of surface active sites. In particular, the introduction of Zn elemental doping results in enhanced performance for formic acid formation, in comparison to un-doped SnO2 and other doped SnO2 catalysts. At −0.99 V versus reversible hydrogen electrode, the total faradaic efficiency for CO2 conversion reaches 80%, while the partial current density is 10.3 mA cm−2. These represent a 10% and a threefold increases for faradaic efficiency and current density, respectively, with respect to the reference un-doped sample. The enhancement of these characteristics relates to the improved charge transfer and conductivity with respect to bare SnO2.

2021 ◽  
Author(s):  
Shenglin Yan ◽  
Samah Awadh Mahyoub ◽  
Jing Lin ◽  
Chunxiao Zhang ◽  
Qing Hu ◽  
...  

Abstract Noble metal aerogels (NMAs) have been used in a variety of (photo-)electrocatalytic reactions, but pure Au aerogels (AG) have not been used in CO2 electroreduction to date. To explore the potential application in this direction, AG was prepared to be used as the cathode in CO2 electroreduction to CO. However, the gelation time of NMAs is usually very long, up to several weeks. Here, an excess NaBH4 and turbulence mixing-promoted gelation approach was developed by introducing magnetic stirring as an external force field, which therefore greatly shortened the formation time of Au gels to several seconds. The AG-3 (AG with Au loading of 0.003 g) exhibited a high CO Faradaic efficiency (FE) of 95.6% at an extremely low overpotential of 0.39 V, and over 91% of CO FE was reached in a wide window of -0.4 ~ -0.7 V vs. the reversible hydrogen electrode (RHE). Partial current density in CO was measured to be -19.35 mA cm-2 at -0.8 V vs. RHE under 1 atm of CO2. The excellent performance should be ascribed to its porous structure, abundant active sites, and large electrochemical active surface area. It provides a new method for preparation of AG with ultrafast gelation time and large production at room temperature, and the resulting pure AG was for the first time used in the field of CO2 electroreduction.


Author(s):  
Sabarinathan Ravichandran ◽  
Narayanamoorthy Bhuvanendran ◽  
Kai Peng ◽  
Weiqi Zhang ◽  
Qian Xu ◽  
...  

Abstract The Pt–Fe2O3 nanoparticles embedded over N, P-doped carbon (Pt–Fe2O3/NPC) was successfully synthesized by chemical reduction method demonstrating an enhanced electrocatalytic efficacy in alkaline media toward oxygen reduction reaction (ORR). The surface morphology of Pt–Fe2O3/NPC has been characterized by electron microscopy scanning, X-ray diffraction, electron microscopy transmission, Raman spectra, and X-ray photoelectron spectroscopy. The ORR electrocatalytic activity of Pt–Fe2O3/NPC was found to be the superior mass activity of 0.120 mA µg−1, which are almost twice higher than those for Pt–Fe2O3/VC (0.068 mA µg−1) and Pt/C (0.061 mA µg−1) catalysts. The durability tests revealed that the Pt–Fe2O3/NPC exhibited enhanced stability observed from the order of electrochemical active surface area (ECA) loss determined as Pt–Fe2O3/NPC (45.67%) <Pt–Fe2O3/VC (62.5%) <(Pt/C (72.13%) after 5000 cycles. This present investigation unveiled a facile approach to develop the number of active sites with the combination between P–Fe2O3 and N, P-doped carbon for improved electrocatalytic performance toward ORR.


Nanomaterials ◽  
2020 ◽  
Vol 10 (8) ◽  
pp. 1547
Author(s):  
Kai Xia ◽  
Meiyu Cong ◽  
Fanfan Xu ◽  
Xin Ding ◽  
Xiaodong Zhang

The development of non-noble metal catalysts for hydrogen revolution in alkaline media is highly desirable, but remains a great challenge. Herein, synergetic ultrathin NiO/MoS2 catalysts were prepared to improve the sluggish water dissociation step for HER in alkaline conditions. With traditional electrode assembly methods, MoS2:NiO-3:1 exhibited the best catalytic performance; an overpotential of 158 mV was required to achieve a current density of 10 mA/cm2. Further, a synergetic ultrathin NiO/MoS2/nickel foam (NF) electrode was assembled by electrophoretic deposition (EPD) and post-processing reactions. The electrode displayed higher electrocatalytic ability and stability, and an overpotential of only 121 mV was needed to achieve a current density of 10 mA/cm2. The improvement was ascribed to the better catalytic environment, rather than a larger active surface area, a higher density of exposed active sites or other factors. DFT calculations indicated that the hybrid NiO/MoS2 heterostuctured interface is advantageous for the enhanced water dissociation step and the corresponding lower kinetic energy barrier—from 1.53 to 0.81 eV.


2020 ◽  
Vol 4 (4) ◽  
pp. 1747-1753 ◽  
Author(s):  
Yuanyuan Ma ◽  
Wenjie Zang ◽  
Afriyanti Sumboja ◽  
Lu Mao ◽  
Ximeng Liu ◽  
...  

Hollow structuring of active components is an effective strategy to improve the kinetics of oxygen electrode catalysts, arising from the increased the active surface area, the defects on the exposed surface, and the accessible active sites.


Sensors ◽  
2019 ◽  
Vol 19 (7) ◽  
pp. 1604 ◽  
Author(s):  
Venkatesh Manikandan ◽  
Boopathi Sidhureddy ◽  
Antony Thiruppathi ◽  
Aicheng Chen

We report here a novel electrochemical sensor developed using fluorine-doped graphene oxide (F-GO) for the detection of caffeic acid (CA). The synthesized graphene oxide (GO) and F-GO nanomaterials were systematically characterized with a scanning electron microscope (SEM), and the presence of semi-ionic bonds was confirmed in the F-GO using X-ray photoelectron spectroscopy. The electrochemical behaviours of bare glassy carbon electrode (GCE), F-GO/GCE, and GO/GCE toward the oxidation of CA were studied using cyclic voltammetry (CV), and the results obtained from the CV investigation revealed that F-GO/GCE exhibited the highest electrochemically active surface area and electrocatalytic activity in contrast to the other electrodes. Differential pulse voltammetry (DPV) was employed for the analytical quantitation of CA, and the F-GO/GCE produced a stable oxidation signal over the selected CA concentration range (0.5 to 100.0 μM) with a low limit of detection of 0.018 μM. Furthermore, the acquired results from the selectivity studies revealed a strong anti-interference capability of the F-GO/GCE in the presence of other hydroxycinnamic acids and ascorbic acid. Moreover, the F-GO/GCE offered a good sensitivity, long-term stability, and an excellent reproducibility. The practical application of the electrochemical F-GO sensor was verified using various brands of commercially available wine. The developed electrochemical sensor successfully displayed its ability to directly detect CA in wine samples without pretreatment, making it a promising candidate for food and beverage quality control.


2020 ◽  
Author(s):  
Wu Tong ◽  
Bolong Huang ◽  
Pengtang Wang ◽  
Qi Shao ◽  
Xiaoqing Huang

Abstract Understanding the correlation between exposed surfaces and performances of controlled nanocatalysts can aid effective strategies to enhance electrocatalysis, but this is as yet unexplored for the nitrogen reduction reaction (NRR). Here, we first report controlled synthesis of well-defined Pt3Fe nanocrystals with tunable morphologies (nanocube, nanorod and nanowire) as ideal model electrocatalysts for investigating the NRR on different exposed facets. The detailed electrocatalytic studies reveal that the Pt3Fe nanocrystals exhibit shape-dependent NRR electrocatalysis. The optimized Pt3Fe nanowires bounded with high-index facets exhibit excellent selectivity (no N2H4 is detected), high activity with NH3 yield of 18.3 μg h−1 mg−1cat (0.52 μg h−1 cm−2ECSA; ECSA: electrochemical active surface area) and Faraday efficiency of 7.3% at −0.05 V versus reversible hydrogen electrode, outperforming the {200} facet-enclosed Pt3Fe nanocubes and {111} facet-enclosed Pt3Fe nanorods. They also show good stability with negligible activity change after five cycles. Density functional theory calculations reveal that, with high-indexed facet engineering, the Fe-3d band is an efficient d-d coupling correlation center for boosting the Pt 5d-electronic exchange and transfer activities towards the NRR.


Clean Energy ◽  
2019 ◽  
Vol 4 (1) ◽  
pp. 58-66
Author(s):  
Qiuping Gan ◽  
Benzhi Wang ◽  
Judan Chen ◽  
Jianniao Tian ◽  
Tayirjan Taylor Isimjan ◽  
...  

Abstract The developing high-efficiency urea fuel cells have an irreplaceable role in solving the increasingly severe environmental crisis and energy shortages. The sluggish six-electron dynamic anodic oxidation reaction is the bottleneck of the rapid progress of urea fuel-cell technology. To tackle this challenge, we select the NiCr bimetallic system due to the unique synergic effect between the Ni and the Cr. Moreover, better conductivity is assured using carbon nanotubes (CNTs) as the support. Most importantly, we use a simple hydrothermal method in catalyst preparation for easy scale-up at a low cost. The results show that the hybrid catalysts of NiCrx-oxide-CNTs with different Ni/Cr ratios show much better catalytic performance in terms of active surface area and current density as compared to that of Ni-hydro-CNTs. The optimized NiCr2-oxide-CNTs catalyst exhibits not only the largest electrochemically active surface area (ESA, 50.7 m2 g−1) and the highest urea electrocatalytic current density (115.6 mA cm−2), but also outstanding long-term stability. The prominent performance of the NiCr2-oxide-CNTs catalyst is due to the combined effect of the improved charge transfer between Ni and Cr species, the large ESA, along with an elegant balance between the oxygen-defect sites and hydrophilicity. Moreover, we have proposed a synergistically enhanced urea catalytic mechanism.


2010 ◽  
Vol 25 (9) ◽  
pp. 1755-1760 ◽  
Author(s):  
Changsheng Shan ◽  
Dongxue Han ◽  
Jiangfeng Song ◽  
Ari Ivaska ◽  
Li Niu

Flowerlike submicrometer gold particles were synthesized through a simple one-step method using p-diaminobenzene as a reductant in the presence of poly(sodium 4-styrenesulfonate) in aqueous solution. The particle size with diameters ranging from 267 to 725 nm could be tuned by varying the molar ratio of poly(sodium 4-styrenesulfonate) to HAuCl4, which also resulted in tunable roughness. The gold particles were confirmed by scanning electron microscopy, energy dispersive x-ray spectroscopy, x-ray diffraction, and x-ray photoelectron spectroscopy. Cyclic voltammetry showed that the specific surface area of the flowerlike particles was larger than that of sphere particles. The obtained flowerlike particles with higher surface area also exhibited higher electrocatalytic activity toward H2O2 and O2. The increase of electrocatalytic activity could be attributed to the increase of the active surface area.


Processes ◽  
2021 ◽  
Vol 9 (9) ◽  
pp. 1592
Author(s):  
Chunxiao Zhang ◽  
Shenglin Yan ◽  
Jing Lin ◽  
Qing Hu ◽  
Juhua Zhong ◽  
...  

Due to CO2 mass transfer limitation as well as the competition of hydrogen evolution reaction in electroreduction of CO2 in the aqueous electrolyte, Zn-based electrodes normally exhibit unsatisfying selectivity for CO production, especially at high potentials. In this work, we introduced a zinc myristate (Zn [CH3(CH2)12COO]2) hydrophobic layer on the surface of zinc foam electrode by an electrodeposition method. The obtained hydrophobic zinc foam electrode showed a high Faradaic efficiency (FE) of 91.8% for CO at −1.9 V (vs. saturated calomel electrode, SCE), which was a remarkable improvement over zinc foam (FECO = 81.87%) at the same potentials. The high roughness of the hydrophobic layer has greatly increased the active surface area and CO2 mass transfer performance by providing abundant gas-liquid-solid contacting area. This work shows adding a hydrophobic layer on the surface of the catalyst is an effective way to improve the electrochemical CO2 reduction performance.


2019 ◽  
Author(s):  
Emmanuel Abdul ◽  
Jason Pitts ◽  
Deepak Rajput ◽  
Shankar Rananavare

Gas sensors fabricated with antimony doped tin oxide (ATO) nanomaterials exhibit remarkable sensitivity for detecting oxidizing and reducing gases. This study highlights the enhanced selectivity and stability of the porous ATO nanomaterial electrode made for electrochemical reduction of CO2 in aqueous media. During electrochemical reduction, these electrodes prepared from compressed powders tend to crumble within a few hours in aqueous media. To overcome this electrode disintegration effect, we modified the surface of the doped tin-Oxide nanoparticles with Nafion and a dipodal silane (1,2-Bis(triethoxysilyl)ethane). The electrode characterization studies include Cyclic Voltammetry (CV), and Electrochemical Impedance Spectroscopy (EIS). Scanning electron microscopic investigation of electrode surface morphology and roughness before and after electrochemical CO2 reduction for derivatized and underivatized electrode revealed lower surface roughness for former than the latter.The derivatized electrodes allowed CO2 electrochemical reduction at low overpotentials and high current density without any electrode crumbling over more than 24 hours of continuous operation. Formate/formic acid and methanol were the major products of reduction at electrode potentials ranging from -0.4 to -1.0V vs. RHE in the CO2 saturated 0.1M KHCO3 electrolyte. Higher current density and Faradaic Efficiency of formic acid was observed when compared to planar tin electrode materials and tin oxide nanoparticles deposited on FTO glass.


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