Highly Electrocatalytic Ethylene Production from CO<sub>2</sub> on Nanodefective Cu Nanosheets

Zhang, Bingxing; Zhang, Jianling; Hua, Manli; Wan, Qiang; Su, Zhuizhui; Tan, Xiuniang; Liu, Lifei; Zhang, Fanyu; Chen, Gang; Tan, Dongxing; Cheng, Xiuyan; Han, Buxing; Zheng, Lirong; Mo, Guang

doi:10.1021/jacs.0c06420

Cited by 303 publications

(280 citation statements)

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“…They could neutralize OH − generated on the electrode surface and help the local pH recover to the bulk level. Such buffering action would fail to work with the confinement of pores, cavities, or pits in the catalysts [12,30] . The resulting limited mass transport would hinder the neutralization process and keep the locally alkaline environment intact.…”

Section: Resultsmentioning

confidence: 99%

“…To improve the catalyst selectivity, several strategies have been put forward to suppress HER in aqueous solutions, to name a few, hydrophobic layer incorporating, [22–24] strain engineering, [25] alloying, [26] hydrogen bonding [27] and hydrogen adsorption site blocking [28] . Recently, a confinement effect induced by pores, cavities or pits has turned out to be effective in suppressing HER in various electrochemical reactions [12,29–32] . The physical isolation and unique compartment endow the catalysts with special local environments that are beneficial for improving the product selectivity.…”

Section: Introductionmentioning

confidence: 99%

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Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

et al. 2021

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It still remains challenging to simultaneously achieve high stability, selectivity, and activity in CO2 reduction. Herein, a dual chainmail‐bearing nickel‐based catalyst (Ni@NC@NCNT) was fabricated via a solvothermal‐evaporation‐calcination approach. In situ encapsulated N‐doped carbon layers (NCs) and nanotubes (NCNTs) gave a dual protection to the metallic core. The confined space well maintained the local alkaline pH value and suppressed hydrogen evolution. Large surface area and abundant pyridinic N and Niδ+ sites ensured high CO2 adsorption capacity and strength. Benefitting from these, it delivered a CO faradaic efficiency of 94.1 % and current density of 48.0 mA cm−2 at −0.75 and −1.10 V, respectively. Moreover, the performance remained unchanged after continuous electrolysis for 43 h, far exceeding Ni@NC with single chainmail, Ni@NC/NCNT with Ni@NC sitting on the walls of NCNT, bare NCNT and most state‐of‐the‐art catalysts, demonstrating structural superiority of Ni@NC@NCNT. This work sheds light on designing unique architectures to improve electrochemical performances.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

et al. 2021

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“…Interestingly, CO gas was not detected in the potential range, even for the two La 2 O 2 CO 3 samples . This indicates that La 2 O 2 CO 3 catalysts are efficient for C-C coupling rather than desorption to form CO gas, since CO is an intermediate for CO 2 transformation to ethene during CO 2 reduction [ 36 ]. The superior electrocatalytic activity of HL-12h to PL-12h would result from the better CO 2 adsorption ability which can optimize the first step involving electron and proton transfer to form a *COOH intermediate, which is then converted to other carbonaceous products [ 37 ].…”

Section: Resultsmentioning

confidence: 99%

Hexagonal and Monoclinic Phases of La2O2CO3 Nanoparticles and Their Phase-Related CO2 Behavior

Jiang

Kang

et al. 2020

Nanomaterials

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In this study, we prepared hexagonal and monoclinic phases of La2O2CO3 nanoparticles by different wet preparation methods and investigated their phase-related CO2 behavior through field-emission scanning microscopy, high-resolution transmission electron microscopy, Fourier transform infrared, thermogravimetric analysis, CO2-temperature programmed desorption, and linear sweeping voltammetry of CO2 electrochemical reduction. The monoclinic La2O2CO3 phase was synthesized by a conventional precipitation method via La(OH)CO3 when the precipitation time was longer than 12 h. In contrast, the hydrothermal method produced only the hexagonal La2O2CO3 phase, irrespective of the hydrothermal reaction time. The La(OH)3 phase was determined to be the initial phase in both preparation methods. During the precipitation, the La(OH)3 phase was transformed into La(OH)CO3 owing to the continuous supply of CO2 from air whereas the hydrothermal method of a closed system crystallized only the La(OH)3 phase. Based on the CO2-temperature programmed desorption and thermogravimetric analysis, the hexagonal La2O2CO3 nanoparticles (HL-12h) showed a higher surface CO2 adsorption and thermal stability than those of the monoclinic La2O2CO3 (PL-12h). The crystalline structures of both La2O2CO3 phases predicted by the density functional theory calculation explained the difference in the CO2 behavior on each phase. Consequently, HL-12h showed a higher current density and a more positive onset potential than PL-12h in CO2 electrochemical reduction.

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“…[ 127 ] Nanoscaled defects on Cu can enrich the reaction intermediates (*CO and *OCCO) and hydroxyl ions on the electrocatalyst, thus promoting C−C coupling for ethylene formation. [ 125,128 ] Organic molecules or metal complexes can also functionalize Cu catalysts with the other binding interactions that may tune the stability of the reaction intermediates, improving catalytic performance by increasing FE, as well as decreasing overpotential. [ 31b ] Oxygenates of Cu catalysts play important roles in ECO 2 RR for C 2+ productions.…”

Section: The “Firework” Between Co and Other Materialsmentioning

confidence: 99%

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

Chen

Zhang

et al. 2020

Small

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million (ppm), which is ≈50% higher than that of the pre-industrial level (280 ppm). [1] The consequent climate change (the average temperature increase of 0.8 °C above the pre-industrial level) causes global warming, one of the top environmental concerns. [2] To maintain the sustainable development of the society, the Intergovernmental Panel on Climate Change (IPCC) recently recommended the warming limit to 1.5 °C rather than 2.0 °C to reduce catastrophic climate change issues, requiring the commitment to take action to control global carbon emission. [3] Under the Paris Agreement, many countries endeavor to reduce greenhouse gas emissions gradually by 2030. [4] The carbon capture and storage (CCS) is a feasible strategy to lower the CO 2 emissions substantially. Long-term storage issues related to the leakage of CO 2 and the lack of economic incentives limited its development. [5] The CO 2 reduction reactions (CO 2 RR) that convert CO 2 into other value-added carbon products could provide a well alternative to the utilization of the captured CO 2 , which not only contributes to the mitigation of CO 2 emission but also offers useful products that can serve as fuels such as CO, HCOOH, CH 3 OH, and CH 4. [6] Moreover, the drive power of CO 2 RR could come from renewable energy resources, such as solar, wind, and hydraulic resources, which indicates that in a green concept, CO 2 RR could complete the carbon loop and potentially solve the issues of global warming and energy crisis simultaneously. [7] 1.1. Fundamental Reaction Pathways of CO 2 RR CO 2 RR is not thermodynamically and kinetically favorable. Every reduction pathway demands a certain amount of energy input. Equations (1-13) shows the reaction steps involved in CO 2 RR (in pH = 7 aqueous solution, vs Normal Hydrogen Electrode (NHE)). [8] As illustrated, it requires a significant amount of reorganizational energy between the linear molecule CO 2 and the bent radical anion − CO 2 • (Equation (1)). When coupling with proton in the reaction, the required reaction energy decreases (Equations (2-12)). Aqueous media with H 2 O molecules become ideal for providing proton into the CO 2 RR system. The reduction potential of hydrogen evolution reaction (HER) (Equation (13)) is close to that of CO 2 RR. It makes HER a competitive reaction against CO 2 RR during the reduction CO 2 reduction reaction (CO 2 RR) provides a promising strategy for sustainable carbon fixation by converting CO 2 into value-added fuels and chemicals. In recent years, considerable efforts are focused on the development of transition-metal (TM)-based catalysts for the selectively electrochemical CO 2 reduction reaction (ECO 2 RR). Co-based catalysts emerge as one of the most promising electrocatalysts with high Faradaic efficiency, current density, and low overpotential, exhibiting excellent catalytic performance toward ECO 2 RR for CO and HCOOH productions that are economically viable. The intrinsic contribution of Co and the synergistic effects in Co-hybrid catalysts play essential roles for ...

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Highly Electrocatalytic Ethylene Production from CO₂ on Nanodefective Cu Nanosheets

Cited by 303 publications

References 41 publications

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

Hexagonal and Monoclinic Phases of La2O2CO3 Nanoparticles and Their Phase-Related CO2 Behavior

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

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Highly Electrocatalytic Ethylene Production from CO2 on Nanodefective Cu Nanosheets

Cited by 303 publications

References 41 publications

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO2

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO2

Hexagonal and Monoclinic Phases of La2O2CO3 Nanoparticles and Their Phase-Related CO2 Behavior

Nanostructured Cobalt‐Based Electrocatalysts for CO2Reduction: Recent Progress, Challenges, and Perspectives

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Highly Electrocatalytic Ethylene Production from CO₂ on Nanodefective Cu Nanosheets

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO₂

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives