Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Li, Jun; Xu, Aoni; Li, Fengwang; Wang, Ziyun; Zou, Chengqin; Gabardo, Christine M.; Wang, Yuhang; Ozden, Adnan; Xu, Yi; Nam, Dae‐Hyun; Lum, Yanwei; Wicks, Joshua; Chen, Bin; Wang, Zhiqiang; Chen, Jiatang; Wen, Yunzhou; Zhuang, Tao‐Tao; Luo, Mingchuan; Du, Xi‐Wen; Sham, Tsun‐Kong; Zhang, Bo; Sargent, Edward H.; Sinton, David

doi:10.1038/s41467-020-17499-5

Cited by 101 publications

(71 citation statements)

References 46 publications

(70 reference statements)

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“…Electrolysis in systems where CO 2 is fed in the gas phase overcomes mass transport limitations and as a result is operational at impressive current densities (>100 mA cm −2 ); however, this produces high local pH conditions, promoting the formation of C 2+ products instead of CH 4 (refs. 22 – 24 ).…”

Section: Introductionmentioning

confidence: 99%

Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

Lum

et al. 2020

Nat Commun

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107

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Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.

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Section: Introductionmentioning

confidence: 99%

Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

Lum

et al. 2020

Nat Commun

Self Cite

107

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“…37 On the other hand, PdCu SAA enhances the selectivity toward alcohols for electrochemical CO2 reduction, compared to common Cu-based catalysts. 38 Hydrogen oxidation reaction (HOR) activity can be regulated by isolating single Ni atom into Ru nanosheet. 39 Inspired by these works, we proposed a singleatom alloying strategy to improve the performance of Au-based materials for NNR.…”

Section: Abstract: Single-atom Alloy Nitrogen Reduction Reaction Electrocatalysismentioning

confidence: 99%

High-Throughput Screening Single-Atom Alloy for Electroreduction of Dinitrogen to Ammonia

Zheng

Tian²,

Zhang³

et al. 2021

Preprint

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Exploring electrocatalyst with high activity, selectivity and stability is essential for development of applicable electrocatalytic ammonia synthesis technology. By performing density functional theory calculations, we systematically investigated a series of transition-metal doped Au-based single atom alloys (SAAs) as promising electrocatalysts for nitrogen reduction reaction (NRR). For Au-based electrocatalyst, the first hydrogenation step (*N2→*NNH) normally determines the limiting potential of the overall reaction process. Compared with pristine Au(111) surface, introducing single atom can significantly enhance the binding strength of N2, leading to decreased energy barrier of the key step, i.e., ΔG(*N2→*NNH). According to simulation results, three descriptors were proposed to describe ΔG(*N2→*NNH), including ΔG(*NNH), d-band center, and . Eight doped elements (Ti, V, Nb, Ru, Ta, Os, W, and Mo) were initially screened out with limiting potential ranging from -0.75V to -0.30 V. Particularly, Mo- and W-doped systems possess the best activity with limiting potentials of -0.30 V, respectively. Then the intrinsic relationship between structure and the potential performance was further analyzed by using machine-learning. The selectivity, feasibility, stability of these candidates were also evaluated, confirming that SAA containing Mo, Ru ,Ta, and W could be outstanding NRR electrocatalysts. This work not only broadens the understating of SAA application in electrocatalysis, but also devotes to the discovery of novel NRR electrocatalysts.

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“…Li et al. reported a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production using CO as original substrate [74] . Using density functional theory calculations, a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C2 intermediates.…”

Section: Strategies To Achieve High Performance For Co2rr With Producmentioning

confidence: 99%

Electrochemical Reduction of Carbon Dioxide to Ethanol: An Approach to Transforming Greenhouse Gas to Fuel Source

Zhang

Liu

2021

Chemistry An Asian Journal

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Converting carbon dioxide (CO2) into high‐value fuels or chemicals is considered as a promising way to utilize CO2 and alleviate the excessive greenhouse gas emission. Among multiple catalysis approaches, electrochemical reduction of CO2 to ethanol has an important prospect due to the high energy density and widely applications of ethanol. In recent years, many electrocatalysts for CO2 reduce reaction (CO2RR) have shown promising catalytic activity for ethanol production. In this review, we will introduce the recent progress in this field. The basic principles and electrochemical performances of CO2RR are reviewed at first. Then, several categories of active electrocatalysts for CO2RR to ethanol are summarized, including the discussion of reaction mechanism and catalytic sites. Finally, several possible strategies are proposed, providing guidance for future design and preparation of high‐performance catalysts.

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Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Cited by 101 publications

References 46 publications

Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

High-Throughput Screening Single-Atom Alloy for Electroreduction of Dinitrogen to Ammonia

Electrochemical Reduction of Carbon Dioxide to Ethanol: An Approach to Transforming Greenhouse Gas to Fuel Source

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