Molecular tuning of CO2-to-ethylene conversion

Li, Fengwang; Thevenon, Arnaud; Rosas‐Hernández, Alonso; Wang, Ziyun; Li, Yilin; Gabardo, Christine M.; Ozden, Adnan; Dinh, Cao-Thang; Li, Jun; Wang, Yuhang; Edwards, Jonathan P.; Xu, Yi; McCallum, Christopher; Tao, Lizhi; Liang, Zhiqin; Luo, Mingchuan; Wang, Xue; Li, Huihui; O’Brien, Colin P.; Tan, Chih Shan; Nam, Dae‐Hyun; Quintero-Bermúdez, Rafael; Zhuang, Tao‐Tao; Li, Yuguang C.; Han, Zhiji; Britt, R. David; Sinton, David; Agapie, Theodor; Peters, Jonas C.; Sargent, Edward H.

doi:10.1038/s41586-019-1782-2

Cited by 877 publications

(781 citation statements)

References 51 publications

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“…Excessive CO 2 emission form combustion of fossil fuels has caused a series of environmental problems. Electrocatalytic CO 2 reduction to value added chemicals by renewable electricity is of great significance for tackling the carbon emissions and recycle use of CO 2 …”

Section: Introductionmentioning

confidence: 99%

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

et al. 2020

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The carbon dioxide reduction reaction (CO 2 RR) driven by renewable electricity is a promising way to tackle the CO 2 emission woes and recycle use of CO 2 . The synthesis of electrocatalysts with high activity and selectivity for CO 2 RR to ethylene remains a great challenge. Herein, leaf-like CuO nanosheets are fabricated in situ on nitrogen-doped graphene (NG) by using a novel reduction-oxidation-reconstruction process. When used as a catalyst for the CO 2 RR in 0.1 M KHCO 3 , a high faradaic efficiency of approximately 30 % for ethylene with an ultra-high ethylene/methane ratio of 190 was achieved at À 1.3 V vs. the reversible hydrogen electrode. The SEM and TEM images confirm the leaf-like CuO nanosheets display highcurvature structures, while multiple distinguished grain boundaries constructed by CuO(110) and CuO(111) planes are verified by HRTEM. For the first time, we present a facile method to combine the high-curvature structure and the grain boundary to enhance the selectivity of the CO 2 RR to ethylene over a CuO catalyst.

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Section: Introductionmentioning

confidence: 99%

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

et al. 2020

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“…It can not only reduce the CO 2 concentration in the environment, but also can facilitate the storage of renewable energy on a large scale. [1][2][3][4][5] In recent years, various valuable products have been obtained, and the C2 + products are more attractive owing to their high energy densities and high economic value per unit mass. [6][7][8][9][10] Among the various C2 + products, alcohols (such as ethanol and npropanol) are highly desirable, which can be either used directly as a fuel or blended with gasoline to give an overall cleaner-burning fuel.…”

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confidence: 99%

Highly Efficient Electroreduction of CO₂ to C2+ Alcohols on Heterogeneous Dual Active Sites

et al. 2020

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Electroreduction of CO2 to liquid fuels such as ethanol and n‐propanol, powered by renewable electricity, offers a promising strategy for controlling the global carbon balance and addressing the need for the storage of intermittent renewable energy. In this work, we discovered that the composite composed of nitrogen‐doped graphene quantum dots (NGQ) on CuO‐derived Cu nanorods (NGQ/Cu‐nr) was an outstanding electrocatalyst for the reduction of CO2 to ethanol and n‐propanol. The Faradaic efficiency (FE) of C2+ alcohols could reach 52.4 % with a total current density of 282.1 mA cm−2. This is the highest FE for C2+ alcohols with a commercial current density to date. Control experiments and DFT studies show that the NGQ/Cu‐nr could provide dual catalytic active sites and could stabilize the CH2CHO intermediate to enhance the FE of alcohols significantly through further carbon protonation. The NGQ and Cu‐nr had excellent synergistic effects for accelerating the reduction of CO2 to alcohols.

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“…2,3 So far elemental copper (Cu) and Cu-based compounds are the only materials that can produce C2 (+) hydrocarbons and oxygenates of any significance albeit at high overpotential and with poor selectivity. 4 To optimize Cu-based catalysts or find alternative materials for selective C2(+) production from CO (2), in-depth mechanistic insight is needed in order to untangle the complexities of CO(2)R. 5 Recent experimental efforts have focused on improving the selectivity towards C2(+) products on Cu by tailoring catalyst composition, [6][7][8][9] the surface morphology, [10][11][12][13] the reaction conditions at the catalyst/electrode interface, 14,15 and by engineering the electrochemical reactors. [16][17][18] To identify key intermediates and tie into theoretical efforts, in situ or operando characterization tools have been employed, 15,19 but the precise mechanism of the first C-C bond formation is still inconclusive.…”

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The Role of Atomic Carbon in Directing Electrochemical CO(2) Reduction to Multicarbon Products

Peng¹,

Tang²,

Li³

et al. 2019

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Electrochemical reduction of carbon-dioxide/carbon-monoxide (CO(2)R) to fuels and chemicals presents an attractive approach for sustainable chemical synthesis, but also poses a serious challenge in catalysis. Understanding the key aspects that guide CO(2)R towards value-added multicarbon (C2+) products is imperative in designing an efficient catalyst. Herein, we identify the critical steps toward C2 products on copper through a combination of energetics from density functional theory and micro-kinetic modeling. We elucidate the importance of atomic carbon in directing C2+ selectivity and how it introduces surface structural sensitivity on copper catalysts. This insight enables us to propose two simple thermodynamic descriptors that effectively describe C2+ selectivity on metal catalysts beyond copper and hence it identifies an intelligible protocol to screen for materials that selectively catalyze CO(2) to C2+ products.

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Molecular tuning of CO2-to-ethylene conversion

Cited by 877 publications

References 51 publications

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

Highly Efficient Electroreduction of CO₂ to C2+ Alcohols on Heterogeneous Dual Active Sites

The Role of Atomic Carbon in Directing Electrochemical CO(2) Reduction to Multicarbon Products

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Molecular tuning of CO2-to-ethylene conversion

Cited by 877 publications

References 51 publications

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO2 Electroreduction to Ethylene

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO2 Electroreduction to Ethylene

Highly Efficient Electroreduction of CO2 to C2+ Alcohols on Heterogeneous Dual Active Sites

The Role of Atomic Carbon in Directing Electrochemical CO(2) Reduction to Multicarbon Products

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Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

Controllable Synthesis of Leaf‐Like CuO Nanosheets for Selective CO₂ Electroreduction to Ethylene

Highly Efficient Electroreduction of CO₂ to C2+ Alcohols on Heterogeneous Dual Active Sites