Theoretical Investigations of Transition Metal Surface Energies under Lattice Strain and CO Environment

Tang, Mingshu; Ulissi, Zachary W.; Chan, Karen

doi:10.1021/acs.jpcc.8b02094

Cited by 20 publications

(28 citation statements)

References 41 publications

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“…To comprehensively model CO (2) reduction, we estimated the reaction energetics for various reaction pathways using explicit- solvent simulations. According to recent experimental spectroscopic 25 and computational work 43 , the presence of CO increases the density of highly active, low-coordinated step sites on polycrystalline copper. Given the generally lower activation barriers associated on steps vs. terraces 16,44 , the activity of steps would, from a simple consideration of the Arrhenius equation, dominate the overall activity.…”

Section: Resultsmentioning

confidence: 99%

pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

et al. 2019

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We present a microkinetic model for CO(2) reduction (CO(2)R) on Cu(211) towards C2 products, based on energetics estimated from an explicit solvent model. We show that the differences in both Tafel slopes and pH dependence for C1 vs C2 activity arise from differences in their multi-step mechanisms. We find the depletion in C2 products observed at high overpotential and high pH to arise from the 2nd order dependence of C-C coupling on CO coverage, which decreases due to competition from the C1 pathway. We further demonstrate that CO(2) reduction at a fixed pH yield similar activities, due to the facile kinetics for CO2 reduction to CO on Cu, which suggests C2 products to be favored for CO2R under alkaline conditions. The mechanistic insights of this work elucidate how reaction conditions can lead to significant enhancements in selectivity and activity towards higher value C2 products.

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Section: Resultsmentioning

confidence: 99%

pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

et al. 2019

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“…The Wulff shapes of the Cu nanoparticles are based on a previous manuscript that followed similar computational steps in creating Wulff shapes. 45 Figure 4D presents the clean Cu particle with various facets. Figure 4E presents the shape after being exposed under a minimal CO partial pressure of around 4.4 3 10 À9 bars.…”

Section: Morphology For Both Samples Was Investigated By Scanning Electron Microscopy (Sem) (Figuresmentioning

confidence: 99%

Self-Selective Catalyst Synthesis for CO2 Reduction

Wang

Liang

Tang

et al. 2019

Joule

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We developed a novel one-step simple method that introduces reactant during the synthesis process of metal nanoparticle. Taking the CO 2 electrochemical reduction reaction as an example, crystal morphology is modulated by intermediates generated from CO 2 reduction reaction, and the as-prepared material exhibits superior electrochemical catalytic performances toward CO 2 RR. Computational results confirm that the reaction intermediates of CO 2 RR could favorably stabilize the chosen facets, thus shaping the catalyst particles and facilitating the entire reduction reaction.

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“…Chan and co-workers performed theoretical investigations of transition metal Cu, Pt, and Ni surface energies under lattice strain and CO environment, in which they have found that the strain effects favor the formation of stepped terraces rather than low index facets such as (111), and the CO environment clearly favors such stepped facets. [93] The two effects above consider the situation where the adsorbate only is bond to one single elemental metal. Ensemble effect, on the other hand, takes into account the interaction with an ensemble of surface atoms.…”

Section: H O H O Oxidation Products H E Anode Reactionmentioning

confidence: 99%

Progress and Perspectives in Photo‐ and Electrochemical‐Oxidation of Biomass for Sustainable Chemicals and Hydrogen Production

Luo

Barrio

Sunny

et al. 2021

Advanced Energy Materials

280

197

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Elevated concentrations of atmospheric greenhouse gases (GHGs), particularly carbon dioxide (CO 2 ), have affected the global environment, causing climate deviations and threatening the biodiversity. [1,2] Deep-cutting solutions and new technologies are thus imperative to repay the carbon debt. [3] Hydrogen (H 2 ) is an ideal fuel to enable a successful transition to a global zero emission economy: With a gravimetric energy density more than double that of conventional fuels like diesel, gasoline, and natural gas it is a lightweight energy carrier which can be converted to electricity and water via fuel cells and thus holds great promise to cut emissions of the transport and energy sectors to zero. Furthermore, it is an energy dense chemical which is already used in the chemical industry (i.e., ammonia via the Haber-Bosch process) and steel manufacturing. However, these industries currently use brown (made from coal via gasification and subsequent water gas shift reaction) and gray (made by steam methane reforming) hydrogen which both have significant CO 2 footprints. Thus, synthesizing green (meaning renewable) hydrogen cost-effectively is a solution which could green such industries and the transport sector and simultaneously meet our growing demands for viable energy storage solutions. However, switching from fossilfuels to a hydrogen economy requires efficient technologies that permit clean, sustainable and cost-effective production, storage, and utilization of H 2 . [4][5][6] Water electrolysis is a clean technology for green H 2 production, where water is split into H 2 at the cathode while O 2 is generated at the anode. Thermodynamically, the energy input required for this reaction equals an applied voltage of 1.23 V but in practice >1.8 V is commonly applied due to the sluggish kinetics of the oxygen evolution reaction (OER). The kinetics of the OER are complex. In addition to the thermodynamic potential of 1.23 V, even the best OER catalysts to date show significant overpotentials (0.35-0.4 V) which is due to suboptimal scaling relation between OOH and OH adsorption energies. [7,8] As a consequence, a significant amount of energy is spent on Biomass is recognized as an ideal CO 2 neutral, abundant, and renewable resource substitute to fossil fuels. The rich proton content in most biomass derived materials, such as ethanol, 5-hydroxymethylfurfural (HMF) and glycerol allows it to be an effective hydrogen carrier. The oxidation derivatives, such as 2,5-difurandicarboxylic acid from HMF, glyceric acid from glycerol are valuable products to be used in biodegradable polymers and pharmaceuticals. Therefore, combining biomass-derived compound oxidation at the anode and hydrogen evolution reaction at the cathode in a biomass electrolysis or photo-reforming reactor would present a promising strategy for coproducing high value chemicals and hydrogen with low energy consumption and CO 2 emissions. This review aims to combine fundamental knowledge on photo and electro-assisted catalysis to provide a comprehensive und...

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Theoretical Investigations of Transition Metal Surface Energies under Lattice Strain and CO Environment

Cited by 20 publications

References 41 publications

pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper

Self-Selective Catalyst Synthesis for CO2 Reduction

Progress and Perspectives in Photo‐ and Electrochemical‐Oxidation of Biomass for Sustainable Chemicals and Hydrogen Production

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