Promoting the electroreduction of CO<sub>2</sub> with oxygen vacancies on a plasma-activated SnO<sub>x</sub>/carbon foam monolithic electrode

Li, Hongqiang; Xiao, Nan; Wang, Yuwei; Liu, Chang; Shengji, Zhang; Zhang, Huihui; Bai, Jinpeng; Jian, Xi Gao; Li, Chen; Guo, Zhen; Zhao, Shijia; Qiu, Jieshan

doi:10.1039/c9ta12401b

Cited by 62 publications

(45 citation statements)

References 58 publications

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“…For the V O ‐rich N‐SnO 2 NS, a prominent reductive peak observed at −0.2 V (Figure 2a) is due to the reduction of unstable oxide layers at the catalyst surface. [ 18 ] The V O ‐rich N‐SnO 2 NS exhibited a high HCOO − FE of 83% at a low potential of −0.9 V (Figure 2b). In contrast, only 68% and 70% HCOO − FEs were determined on the pristine SnO x NS and the V O ‐poor N‐SnO 2 NS, respectively, at the same potential.…”

Section: Figurementioning

confidence: 99%

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

et al. 2020

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Sn‐based materials are identified as promising catalysts for the CO2 electroreduction (CO2RR) to formate (HCOO−). However, their insufficient selectivity and activity remain grand challenges. A new type of SnO2 nanosheet with simultaneous N dopants and oxygen vacancies (VO‐rich N‐SnO2 NS) for promoting CO2 conversion to HCOO− is reported. Due to the likely synergistic effect of N dopant and VO, the VO‐rich N‐SnO2 NS exhibits high catalytic selectivity featured by an HCOO− Faradaic efficiency (FE) of 83% at −0.9 V and an FE of > 90% for all C1 products (HCOO− and CO) at a wide potential range from −0.9 to −1.2 V. Low coordination Sn–N moieties are the active sites with optimal electronic and geometric structures regulated by VO and N dopants. Theoretical calculations elucidate that the reaction free energy of HCOO* protonation is decreased on the VO‐rich N‐SnO2 NS, thus enhancing HCOO− selectivity. The weakened H* adsorption energy also inhibits the hydrogen evolution reaction, a dominant side reaction during the CO2RR. Furthermore, using the catalyst as the cathode, a spontaneous Galvanic Zn‐CO2 cell and a solar‐powered electrolysis process successfully demonstrated the efficient HCOO− generation through CO2 conversion and storage.

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Section: Figurementioning

confidence: 99%

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

et al. 2020

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“…The results show that the O V ‐TiO 2 /MXene electrode exhibited a higher CO 2 adsorption capacity than the Ti 3 C 2 T x MXene electrode, indicating that O V s allow for increased CO 2 adsorption [48] . It should be noted that O V s can decrease the bonding state and increase the anti‐bonding state to enhance CO 2 adsorption sites, thereby enhancing the adsorption of CO 2 to strengthen CO 2 RR [49,50] . Besides that, introducing mesopores to O V ‐TiO 2 /MXene plays a vital role in increasing the number of active sites for CO 2 adsorption [51] and effectively avoiding particle agglomeration during reactions [52] …”

Section: Resultsmentioning

confidence: 95%

“…Meanwhile, they exhibited highest discharge voltage and lowest discharge‐charge overpotential. These benefits in O V ‐TiO 2 /MXene electrocatalysts can be attributed to the possession of weakly bounded electrons in O V s, which play an indispensable role in capturing CO 2 to consolidate the reversibility of Li‐CO 2 batteries [50] . Intriguingly, the discharge platform slightly ascended and then descended with the rise of cycling numbers.…”

Section: Resultsmentioning

confidence: 99%

Promoting the Electrocatalytic Activity of Ti₃C₂T_x MXene by Modulating CO₂ Adsorption through Oxygen Vacancies for High‐Performance Lithium‐Carbon Dioxide Batteries

et al. 2020

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Lithium‐carbon dioxide (Li‐CO2) batteries are considered as a most auspicious energy storage systems owing to their high capacity and the ability of capturing CO2. However, there are still some critical issues needed to be addressed before their practical application, such as high charge potential and poor cyclability. Herein, oxygen vacancy‐enriched TiO2 nanoparticles grown in situ on Ti3C2Tx MXene (OV‐TiO2/MXene) are synthesized as catalysts for Li‐CO2 batteries by facile one‐step ethanol heat treatment of the MXene nanosheets. The thermodynamically metastable Ti atom on the surface of MXenes serves as nucleating sites, which play a critical role in generating the relatively stable vacancy‐rich TiO2 nanoparticles. The spontaneously generated oxygen vacancies can enhance CO2 adsorption, which is beneficial to CO2 involved electrode reactions. The Li‐CO2 batteries with OV‐TiO2/MXene electrodes deliver noteworthily reduced charge voltage of 3.37 V at 100 mA g−1, and a superb cycling performance of 158 cycles. This work highlights the significant role of oxygen vacancies in activating CO2 in Li‐CO2 batteries, instrumental to the development of high‐performance electrocatalysts for Li‐CO2 batteries and beyond.

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“…Plentiful defect sites and carrier density can not only enhance the conductivity of the electrocatalyst but also enhance the density of exposed active sites. For example, Qiu et al [ 77 ] focused on introducing defect engineering strategies, designing and synthesizing carbon foam–supported SnO x nanosheets with oxygen‐enriched vacancies. The catalyst exhibited high product selectivity, demonstrating the highest FE of 86% with the highest current density of 30 mA cm −2 for formic acid production.…”

Section: Strategies For Improving Efficiency and Selectivitymentioning

confidence: 99%

Recent Progress of Sn‐Based Derivative Catalysts for Electrochemical Reduction of CO₂

Cheng

Zhang

et al. 2020

Energy Tech

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With the development of industry and improvement in living standards, carbon dioxide emissions have increased significantly year by year, causing serious environmental problems, such as global warming and climate change, which have been receiving much attention. [1] Effective capture and utilization of carbon dioxide is an important means to alleviate the increase in carbon dioxide content in the atmosphere. [2] The electrochemical reduction reaction of carbon dioxide (CO 2 RR) can not only effectively solve the problem of the environmental impact of excessive carbon dioxide emissions, but also convert unstable renewable resources to stable chemical energy for storage. [3] Therefore, the target of recent research is how to transfer carbon dioxide into valuable chemicals and fuels. [4] Among these high-value-added chemical substances, formic acid has one of the most wide ranges of application as a reactant material in the dye and leather industry. [5] Moreover, formic acid can also be treated as one of the centers of energy transportation and preservation, that is, for simple and effective conversion into H 2 or CO. [6] Compared with other possible chemical product conversion pathways, the reduction process of CO 2 to C1 products (CO and formic acid) is a classic double electron transfer reaction that occurs easily, and the electron utilization efficiency is very high. Therefore, it is considered to be an economically feasible, simple, and effective method. [7] Due to the thermodynamic stability of carbon dioxide molecules, the reduction process is difficult to complete spontaneously. The participation of the catalyst can shorten the time

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Promoting the electroreduction of CO₂ with oxygen vacancies on a plasma-activated SnO_x/carbon foam monolithic electrode

Abstract: A defect engineering strategy is proposed to synthesize carbon foam supported oxygen vacancy-enriched SnOx nanosheets as a promising monolithic electrode for electrocatalytic reduction of CO2 to formate with high activity and selectivity.

Cited by 62 publications

References 58 publications

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

Promoting the Electrocatalytic Activity of Ti₃C₂T_x MXene by Modulating CO₂ Adsorption through Oxygen Vacancies for High‐Performance Lithium‐Carbon Dioxide Batteries

Recent Progress of Sn‐Based Derivative Catalysts for Electrochemical Reduction of CO₂

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Promoting the electroreduction of CO2 with oxygen vacancies on a plasma-activated SnOx/carbon foam monolithic electrode

Abstract: A defect engineering strategy is proposed to synthesize carbon foam supported oxygen vacancy-enriched SnOx nanosheets as a promising monolithic electrode for electrocatalytic reduction of CO2 to formate with high activity and selectivity.

Cited by 62 publications

References 58 publications

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO2 Electroreduction to Formate

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO2 Electroreduction to Formate

Promoting the Electrocatalytic Activity of Ti3C2Tx MXene by Modulating CO2 Adsorption through Oxygen Vacancies for High‐Performance Lithium‐Carbon Dioxide Batteries

Recent Progress of Sn‐Based Derivative Catalysts for Electrochemical Reduction of CO2

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Promoting the electroreduction of CO₂ with oxygen vacancies on a plasma-activated SnO_x/carbon foam monolithic electrode

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

Elucidation of the Synergistic Effect of Dopants and Vacancies on Promoted Selectivity for CO₂ Electroreduction to Formate

Promoting the Electrocatalytic Activity of Ti₃C₂T_x MXene by Modulating CO₂ Adsorption through Oxygen Vacancies for High‐Performance Lithium‐Carbon Dioxide Batteries

Recent Progress of Sn‐Based Derivative Catalysts for Electrochemical Reduction of CO₂