Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

Wang, Xue; Wang, Ziyun; Arquer, F. Pelayo Garcı́a de; Dinh, Cao-Thang; Ozden, Adnan; Li, Yuguang C.; Nam, Dae‐Hyun; Li, Jun; Liu, Yi Sheng; Wicks, Joshua; Chen, Zitao; Chi, Miaofang; Chen, Bin; Wang, Ying; Tam, Jason; Howe, Jane Y.; Proppe, Andrew H.; Todorovič, P.; Li, Fengwang; Zhuang, Tao; Gabardo, Christine M.; Kirmani, Ahmad R.; McCallum, Christopher; Hung, Sung‐Fu; Lum, Yanwei; Luo, Mingchuan; Min, Yimeng; Xu, Aoni; O’Brien, Colin P.; Stephen, Bello; Sun, Bin; Ip, Alexander H.; Richter, Lee J.; Kelley, Shana O.; Sinton, David; Sargent, Edward H.

doi:10.1038/s41560-020-0607-8

Cited by 442 publications

(335 citation statements)

References 64 publications

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“…The atomic structures resulting from the deposition simulations are also provided online in extended XYZ format [95], in the hope that they may enable further work in the future. Indeed, libraries of (small-scale) GAP-generated carbon structures have begun to be successfully used as starting points for simulation studies by others [96,97].…”

Section: In This Context)mentioning

confidence: 99%

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

et al. 2020

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Amorphous carbon (a-C) materials have diverse interesting and useful properties, but the understanding of their atomic-scale structures is still incomplete. Here, we report on extensive atomistic simulations of the deposition and growth of a-C films, describing interatomic interactions using a machine learning (ML) based Gaussian Approximation Potential (GAP) model. We expand widely on our initial work [Phys. Rev. Lett. 120, 166101 (2018)] by now considering a broad range of incident ion energies, thus modeling samples that span the entire range from low-density (sp 2-rich) to high-density (sp 3-rich, "diamond-like") amorphous forms of carbon. Two different mechanisms are observed in these simulations, depending on the impact energy: low-energy impacts induce sp-and sp 2-dominated growth directly around the impact site, whereas high-energy impacts induce peening. Furthermore, we propose and apply a scheme for computing the anisotropic elastic properties of the a-C films. Our work provides fundamental insight into this intriguing class of disordered solids, as well as a conceptual and methodological blueprint for simulating the atomic-scale deposition of other materials with ML-driven molecular dynamics.

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Section: In This Context)mentioning

confidence: 99%

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

et al. 2020

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“…Therefore, the BN-GFLP catalyst showed high alcohol selectivity in the C2+ product distribution ( Supplementary Fig. 15) over hydrocarbon products in the CO2R process 45 ( Supplementary Fig. 27).…”

Section: Dft Calculations For Mechanistic Insights Of Bn-gflpmentioning

confidence: 95%

CO2 Reduction for C2+ in Seawater Using a Graphitic Frustrated Lewis Pair Catalyst

Kwon¹,

Kim²,

Park³

et al. 2020

Preprint

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Ocean acidification due to the absorption of 40% of the world’s anthropogenic CO2 emissions severely affects the faltering marine ecosystem and the economy. However, there are few reports on reducing CO2 dissolved in seawater. Herein, we introduce an electrochemical CO2 reduction battery system for use in seawater with a graphitic frustrated Lewis pair catalytic cathode doped with boron and nitrogen (BN-GFLP). BN-GFLP converts CO2 dissolved in seawater to multi-carbon (C2+) products during the discharge process, thus increasing the pH of intentionally acidified seawater from 6.4 to 8.0 with more than 87% Faradaic efficiency. In computational chemistry and spectroscopy, BN-GFLP binds CO2 in a unique manner that enables exothermic C–C coupling pathway to deliver 95% selectivity for valuable C2+ products. Based on our results, we suggest a molecular design strategy for next-generation CO2 reduction catalysts for both green oceans and the atmosphere.

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“…DFT calculations suggest that coating a nitrogen‐doped carbon (N‐C) layer with the strong electron‐donating ability on a Cu surface promotes C–C coupling and suppresses the breaking of the CO bond in HOCCH*, thereby promoting ethanol selectivity in ECO 2 RR. [ 130 ] As aforementioned, HCOOH is the most commercially viable product among all the products from CO 2 RR. In this case, maximizing the product selectivity of HCOOH for Cu‐based catalysts would be very practical.…”

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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Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

Cited by 442 publications

References 64 publications

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

CO2 Reduction for C2+ in Seawater Using a Graphitic Frustrated Lewis Pair Catalyst

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

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Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

Cited by 442 publications

References 64 publications

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

Machine learning driven simulated deposition of carbon films: From low-density to diamondlike amorphous carbon

CO2 Reduction for C2+ in Seawater Using a Graphitic Frustrated Lewis Pair Catalyst

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

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Product

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