Catalyst-Free Carbon Dioxide Conversion in Water Facilitated by Pulse Discharges

Zhang, Tianqi; Knezevic, Josip; Zhu, Mengying; Hong, Jungmi; Zhou, Rusen; Song, Qiang; Ding, Luyao; Sun, Jing; Liu, Dingxin; Ostrikov, Kostya Ken; Zhou, Renwu; Cullen, Patrick J.

doi:10.1021/jacs.3c11102

Cited by 12 publications

(8 citation statements)

References 27 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The formation rate of H 2 O 2 increases significantly with the increase of flow rate, reaching 0.82 mmol h −1 at 100 sccm flow rate. This finding diverges from the prevalent understanding in the literature, which suggests that a lower flow rate within a specific range is favorable for microbubble generation and that microbubble rupture further leads to the formation of •OH and H 2 O 2 [21]. However, comparison of ICCD images at flow rates of 10 and 50 sccm revealed that lower flow rates may not support the desired stability and uniformity of the discharge in our experimental setup.…”

Section: Effect Of Gas Flow Ratecontrasting

confidence: 95%

“…CO 2 conversion at gas phase plasma primarily through high-energy electrons dissociating CO 2 into CO and O [34][35][36]. At the gas-liquid interface, the plasma produces solvated electrons and some CO 2 enters the solution to form CO 2 − aq and HCO 2 − aq [20,21,37]. H 2 generation, possibly originating from either plasma region H 2 O decomposition or ground electrode hydrogen evolution.…”

Section: Discussionmentioning

confidence: 99%

“…Rumbach et al used solvated electrons produced by plasma to convert dissolved CO 2 into oxalate and formate [20]. More recently, Zhang et al demonstrated the utilization of gasliquid discharge plasma for the reduction of CO 2 and subsequent synthesis of oxalic acid in aqueous solutions [21]. These findings collectively advance our understanding of gasliquid plasma technologies for CO 2 conversion.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Gao,

Zhou,

Hong

et al. 2024

J. Phys. D: Appl. Phys.

Self Cite

View full text Add to dashboard Cite

In the context of escalating global efforts to mitigate carbon emissions and explore sustainable energy resources, the transformation of CO2 into valuable chemicals and fuels via plasma technology has garnered significant attention. This study demonstrated a new pathway of CO2 conversion into CO and H2O2 via the bubble-enabled gas-liquid discharge driven by a nanosecond pulse. Results showed that the increased discharge frequency and larger pulse widths could enhance CO2 conversion rates and H2O2 yields, albeit potentially at the cost of reduced energy efficiency. Conversely, the rising time of pulse showed negligible impact on the process, whereas varying gas flow rates significantly altered CO and H2O2 yields, underscoring the nuanced influence of these parameters on the efficiency and selectivity of conversion processes. Through illuminating the dynamics of bubble discharge-assisted CO2 transformation, this study contributes to the broader understanding of gas-liquid discharge driven by nanosecond pulse, underlining its potential for addressing environmental and energy challenges.energy challenges.

show abstract

Section: Effect Of Gas Flow Ratecontrasting

confidence: 95%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Gao,

Zhou,

Hong

et al. 2024

J. Phys. D: Appl. Phys.

Self Cite

View full text Add to dashboard Cite

show abstract

“…The analysis of the outlet gases revealed the presence of H 2 , CO, and C 2 –C 3 hydrocarbons (C 2 H 2 , C 2 H 4 , C 2 H 6 , C 3 H 4 , C 3 H 4 (isomer), C 3 H 6 , and C 3 H 8 ), along with unreacted CO 2 and CH 4 . O 2 was sporadically observed under 100% CO 2 condition, albeit at low concentrations (<2.5%), due to the formation of H 2 O 2 and O 2 dissolution Figure A illustrates the relative composition breakdown based on the feed ratio, where the axes represent the percentage of CO 2 used in the feed gas (with pure CO 2 and pure CH 4 being denoted as 100 and 0%).…”

Section: Resultsmentioning

confidence: 99%

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Knezevic,

Zhang,

Zhou

et al. 2024

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

The burgeoning necessity to discover new methodologies for the synthesis of long-chain hydrocarbons and oxygenates, independent of traditional reliance on high-temperature, high-pressure, and fossil fuel-based carbon, is increasingly urgent. In this context, we introduce a nonthermal plasma-based strategy for the initiation and propagation of long-chain carbon growth from biogas constituents (CO 2 and CH 4 ). Utilizing a plasma reactor operating at atmospheric room temperature, our approach facilitates hydrocarbon chain growth up to C40 in the solid state (including oxygenated products), predominantly when CH 4 exceeds CO 2 in the feedstock. This synthesis is driven by the hydrogenation of CO 2 and/or amalgamation of CH x radicals. Global plasma chemistry modeling underscores the pivotal role of electron temperature and CH x radical genesis, contingent upon varying CO 2 /CH 4 ratios in the plasma system. Concomitant with long-chain hydrocarbon production, the system also yields gaseous products, primarily syngas (H 2 and CO), as well as liquid-phase alcohols and acids. Our finding demonstrates the feasibility of atmospheric room-temperature synthesis of long-chain hydrocarbons, with the potential for tuning the chain length based on the feed gas composition.

show abstract

“…The consumption of traditional fossil fuels and the increasing concentration of CO 2 have caused serious environmental problems. − Electrochemical CO 2 reduction reaction (eCO 2 RR) is considered an ideal approach for converting it into renewable fuels and chemicals, achieving energy and environmental sustainability while effectively addressing the greenhouse effect. − Among the various CO 2 conversion products, CO is a vital industrial raw material that has been widely used in synthesizing multiple organic chemicals. eCO 2 RR-to-CO is widely recognized as one of the most economically viable reactions because of it lower electron and energy consumption compared with traditional methods. − Despite numerous studies on the eCO 2 RR-to-CO catalytic system, the stability and activity of the reaction still fall short of meeting the needs for the large-scale production of CO.…”

Section: Introductionmentioning

confidence: 99%

Indium Metal Oxide Tandem Ag Catalyst toward Highly Selective CO₂ Electroreduction to CO over a Wide Potential Window

Duan,

Guo,

Fang

et al. 2024

ACS Sustainable Chem. Eng.

View full text Add to dashboard Cite

We report In 2 O 3 tandem Ag-based catalysts for an electrochemical CO 2 reduction reaction (eCO 2 RR), which achieve remarkable selectivity toward CO and desirable Faradaic efficiencies (FEs) exceeding 90%, with a maximum value of 97.8%, achieved over 12.25%In 2 O 3 − Ag using the H-type cell within a wide potential window ranging from −0.48 to −0.88 V vs RHE. Moreover, a high current density of −102.6 mA cm −2 can be attained in the flow cell while maintaining an FE of CO above 90%. The theoretical calculations show a more negative Gibbs free energy for the formation of the key intermediate *CO 2 − on the In site, which demonstrates that In 2 O 3 of the tandem catalyst exhibits a stronger adsorption and activation capacity for CO 2 . Additionally, DFT simulation reveals the thermodynamic feasibility of the surface transport of *CO 2 − , wherein the *CO 2 − intermediate migrates from the In site to the Ag site. The rapid electron transfer at the In 2 O 3 −Ag heterointerface influences the electronic environment of the Ag site, accelerating migration and reducing the energy barrier for *CO 2 − conversion to *COOH, ultimately facilitating the generation of CO.

show abstract

Catalyst-Free Carbon Dioxide Conversion in Water Facilitated by Pulse Discharges

Cited by 12 publications

References 27 publications

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Indium Metal Oxide Tandem Ag Catalyst toward Highly Selective CO₂ Electroreduction to CO over a Wide Potential Window

Contact Info

Product

Resources

About

Catalyst-Free Carbon Dioxide Conversion in Water Facilitated by Pulse Discharges

Cited by 12 publications

References 27 publications

Efficient synthesis of CO and H2O2 via nanosecond pulsed CO2 bubble discharge

Efficient synthesis of CO and H2O2 via nanosecond pulsed CO2 bubble discharge

Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling

Indium Metal Oxide Tandem Ag Catalyst toward Highly Selective CO2 Electroreduction to CO over a Wide Potential Window

Contact Info

Product

Resources

About

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Efficient synthesis of CO and H₂O₂ via nanosecond pulsed CO₂ bubble discharge

Indium Metal Oxide Tandem Ag Catalyst toward Highly Selective CO₂ Electroreduction to CO over a Wide Potential Window