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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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Mohamed, Tarek |
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Ertürk, Emre |
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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Ajayan, Pulickel
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (9/9 displayed)
- 2024Deciphering Sodium‐Ion Storage: 2D‐Sulfide versus Oxide Through Experimental and Computational Analysescitations
- 2024Tunable 2D Conjugated Porous Organic Polymer Films for Precise Molecular Nanofiltration and Optoelectronicscitations
- 2023Cooperative Copper Single Atom Catalyst in Two‐dimensional Carbon Nitride for Enhanced CO<sub>2</sub> Electrolysis to Methanecitations
- 2022Explosive percolation yields highly-conductive polymer nanocompositescitations
- 2022Sustainable valorization of asphaltenes via flash joule heatingcitations
- 2021Highly efficient photoelectric effect in halide perovskites for regenerative electron sourcescitations
- 2019Optical Control of Non-Equilibrium Phonon Dynamics.citations
- 2019Structural determination of Enzyme-Graphene Nanocomposite Sensor Material
- 2017Ultrafast non-radiative dynamics of atomically thin MoSe2citations
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article
Cooperative Copper Single Atom Catalyst in Two‐dimensional Carbon Nitride for Enhanced CO<sub>2</sub> Electrolysis to Methane
Abstract
<jats:title>Abstract</jats:title><jats:p>Renewable electricity powered carbon dioxide (CO<jats:sub>2</jats:sub>) reduction (eCO<jats:sub>2</jats:sub>R) to high‐value fuels like methane (CH<jats:sub>4</jats:sub>) holds the potential to close the carbon cycle at meaningful scales. However, this kinetically staggered 8‐electron multistep reduction still suffers from inadequate catalytic efficiency and current density. Atomic Cu‐structures can boost eCO<jats:sub>2</jats:sub>R‐to‐CH<jats:sub>4</jats:sub> selectivity due to enhanced intermediate binding energies (BEs) resulting from favorably shifted d‐band centers. Herein, we exploit two‐dimensional carbon nitride (CN) matrices, viz. Na‐polyheptazine (PHI) and Li‐polytriazine imides (PTI), to host Cu‐N<jats:sub>2</jats:sub> type single atom sites with high density (∼1.5 at%), via a facile metal ion exchange process. Optimized Cu loading in nanocrystalline Cu‐PTI maximizes eCO<jats:sub>2</jats:sub>R‐to‐CH<jats:sub>4</jats:sub> performance with Faradaic efficiency (FE<jats:sub>CH4</jats:sub>) of ≈68% and a high partial current density of 348 mA cm<jats:sup>−2</jats:sup> at a low potential of ‐0.84 V versus RHE, surpassing the state‐of‐the‐art catalysts. Multi‐Cu substituted N‐appended nanopores in the CN frameworks yield thermodynamically stable quasi‐dual/triple sites with large interatomic distances dictated by the pore dimensions. First‐principles calculations elucidate the relative Cu‐CN cooperative effects between the two matrices and how the Cu‐Cu distance and local environment dictate the adsorbate BEs, density of states, and CO<jats:sub>2</jats:sub>‐to‐CH<jats:sub>4</jats:sub> energy profile landscape. The 9N pores in Cu‐PTI yield cooperative Cu‐Cu sites that synergistically enhance the kinetics of the rate‐limiting steps in the eCO<jats:sub>2</jats:sub>R‐to‐CH<jats:sub>4</jats:sub> pathway.</jats:p><jats:p>This article is protected by copyright. All rights reserved</jats:p>