Active and Selective Conversion of CO<sub>2</sub> to CO on Ultrathin Au Nanowires

Zhu, Wenlei; Zhang, Yin-Jia; Zhang, Hongyi; Lv, Haifeng; Li, Qing; Michalsky, Ronald; Peterson, Andrew A.; Sun, Shouheng

doi:10.1021/ja5095099

Cited by 788 publications

(659 citation statements)

References 30 publications

(48 reference statements)

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“…However, as we described before, stubbornly reducing the size would risk the stability, and lose the merits of nanomaterials – easy recycle, NFs could be a solution. On the other hand, UNW may be another solution, as we have seen in section 3.2, ultrathin Au nanowires which possess high edge atom content could improve the CO production 75. Ultrathin Pt nanowire with diameter about 3 nm also shows enhanced properties of electrochemical oxidation of formic acid or methanol comparing with commercial Pt/C catalysts 119.…”

Section: Novel Structures and Atypical Edgesmentioning

confidence: 94%

“…This could be achieved by ultrathin nanowires (UNWs), ultrathin structure would maximally expose edges and long nanowire would further elongate the edges (Figure 4e). The ultrathin Au nanowire with diameter of 2.1 nm and length of 500 nm reaches 94% of FE at relative low potential (–0.35 V) (Figure 4f,g),75 putting forward the realization of CO 2 reduction. In computation results, Au(211) is the best for COOH* stabilization, but the binding energy of CO* offset the advantage (Figure 4h).…”

Section: Edges As Active Sitesmentioning

confidence: 98%

“…Binding energies of the key COOH and CO intermediates calculated on the Au NW, Au 13 cluster, and Au(211) are shown in the right. Reproduced with permission 75. Copyright 2013, American Chemical Society.…”

Section: Edges As Active Sitesmentioning

confidence: 99%

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Face the Edges: Catalytic Active Sites of Nanomaterials

Wang

2015

Advanced Science

151

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Edges are special sites in nanomaterials. The atoms residing on the edges have different environments compared to those in other parts of a nanomaterial and, therefore, they may have different properties. Here, recent progress in nanomaterial fields is summarized from the viewpoint of the edges. Typically, edge sites in MoS2 or metals, other than surface atoms, can perform as active centers for catalytic reactions, so the method to enhance performance lies in the optimization of the edge structures. The edges of multicomponent interfaces present even more possibilities to enhance the activities of nanomaterials. Nanoframes and ultrathin nanowires have similarities to conventional edges of nanoparticles, the application of which as catalysts can help to reduce the use of costly materials. Looking beyond this, the edge structures of graphene are also essential for their properties. In short, the edge structure can influence many properties of materials.

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Section: Novel Structures and Atypical Edgesmentioning

confidence: 94%

Section: Edges As Active Sitesmentioning

confidence: 98%

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Face the Edges: Catalytic Active Sites of Nanomaterials

Wang

2015

Advanced Science

151

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“…There is an enriched library of Au nanostructures with the precisely controlled geometry that provides the necessary material basis for electrochemical studies. For example, Sun and co‐workers prepared ultrathin Au nanowires by seed‐mediated growth method 67. The product was featured with dominant surface edge sites, and capable of highly efficient CO 2 reduction to CO with low onset potential of −0.2 V versus RHE, high Faradaic efficiency of 94%, and mass activity of 1.84 A g −1 Au at −0.35 V. Stable Au concave rhombic dodecahedra were prepared by Nam and co‐workers by adding 4‐aminothiophenol during seed‐mediated growth to bind and stabilize various high‐index crystal planes such as (331), (221) and (553) 68.…”

Section: Electrocatalytic Materials For Co2 Reductionmentioning

confidence: 99%

CO₂ Reduction: From the Electrochemical to Photochemical Approach

et al. 2017

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Increasing CO2 concentration in the atmosphere is believed to have a profound impact on the global climate. To reverse the impact would necessitate not only curbing the reliance on fossil fuels but also developing effective strategies capture and utilize CO2 from the atmosphere. Among several available strategies, CO2 reduction via the electrochemical or photochemical approach is particularly attractive since the required energy input can be potentially supplied from renewable sources such as solar energy. In this Review, an overview on these two different but inherently connected approaches is provided and recent progress on the development, engineering, and understanding of CO2 reduction electrocatalysts and photocatalysts is summarized. First, the basic principles that govern electrocatalytic or photocatalytic CO2 reduction and their important performance metrics are discussed. Then, a detailed discussion on different CO2 reduction electrocatalysts and photocatalysts as well as their generally designing strategies is provided. At the end of this Review, perspectives on the opportunities and possible directions for future development of this field are presented.

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“…Likewise, de--alloyed porous Ag films 8 and carbon--supported Au nanoparticle 9 --11 and nan--owire electrodes 12 have been shown to catalyze the reduction of CO 2 to CO with high selectivity. This enhanced selectivity may arise from increases in the specific (surface area normal--ized) activity for CDR and/or from a decrease in specific ac--tivity for HER.…”

Section: --7mentioning

confidence: 99%

Mesostructure-Induced Selectivity in CO₂ Reduction Catalysis

et al. 2015

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Gold inverse opal (Au--IO) thin films are active for CO 2 reduction to CO with high efficiency at modest over--potentials and high selectivity relative to hydrogen evolution. The specific activity for hydrogen evolution diminishes by ten fold with increasing porous film thickness while CO evo--lution activity is largely unchanged. We demonstrate that the origin of hydrogen suppression in Au--IO films stems from the generation of diffusional gradients within the pores of the mesostructured electrode rather than changes in surface faceting or Au grain size. For electrodes with optimal meso--porosity, 99% selectivity for CO evolution can be obtained at overpotentials as low as 0.4 V. These results establish elec--trode mesostructuring as a complementary method for tun--ing selectivity in CO 2 --to--fuels catalysis.The electroreduction of carbon dioxide is a promising meth--od for storing intermittent renewable electricity in energy dense carbonaceous fuels. 1--4 However, the high cost and low efficiency of electrochemical CO 2 reduction (CDR) has pre--vented this technology from reaching economic viability. 4 CDR is most practically achieved in aqueous electrolytes, in which the more kinetically facile reduction of protons to H 2 often outcompetes CO 2 reduction, eroding reaction selectivi--ty. Indeed, the paucity of general materials design principles for selectively inhibiting the hydrogen evolution reaction (HER) impedes the systematic development of improved CDR catalysts. 1 Recently, numerous nanostructured metals have been shown to catalyze CO 2 reduction with improved selectivity relative to planar polycrystalline foils. For example gold, copper, and lead films prepared by electrochemical reduction of copper, gold, and lead oxides, respectively, display high CDR selectiv--ity at low overpotentials. 5--7Likewise, de--alloyed porous Ag films 8 and carbon--supported Au nanoparticle 9 --11 and nan--owire electrodes 12 have been shown to catalyze the reduction of CO 2 to CO with high selectivity. This enhanced selectivity may arise from increases in the specific (surface area normal--ized) activity for CDR and/or from a decrease in specific ac--tivity for HER. For oxide--derived gold, evidence points to both effects, 13 whereas for oxide--derived Cu and Pb, specific HER activity have been shown to diminish more dramatically than CDR activity, giving rise to enhanced selectivity for the latter. 5,7 In general, selectivity differences have been attribut--ed to the intrinsic selectivity of the active sites in the materi--al. However, observations of thickness--dependent product selectivity for electrodeposited porous copper thin films 14 suggest that mass transport effects may also play a role in determining product selectivity. For example, when consid--ering CO 2 reduction catalyzed by Au, which generates CO and H 2 predominantly, both the desired reaction (eq. 1) and H 2 evolution (eq. 2) consume protons,necessitating the formation of a pH gradient at the electrode surface irrespective of the product...

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Active and Selective Conversion of CO₂ to CO on Ultrathin Au Nanowires

Cited by 788 publications

References 30 publications

Face the Edges: Catalytic Active Sites of Nanomaterials

Face the Edges: Catalytic Active Sites of Nanomaterials

CO₂ Reduction: From the Electrochemical to Photochemical Approach

Mesostructure-Induced Selectivity in CO₂ Reduction Catalysis

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Active and Selective Conversion of CO2 to CO on Ultrathin Au Nanowires

Cited by 788 publications

References 30 publications

Face the Edges: Catalytic Active Sites of Nanomaterials

Face the Edges: Catalytic Active Sites of Nanomaterials

CO2 Reduction: From the Electrochemical to Photochemical Approach

Mesostructure-Induced Selectivity in CO2 Reduction Catalysis

Contact Info

Product

Resources

About

Active and Selective Conversion of CO₂ to CO on Ultrathin Au Nanowires

CO₂ Reduction: From the Electrochemical to Photochemical Approach

Mesostructure-Induced Selectivity in CO₂ Reduction Catalysis