Bi(OH)<sub>3</sub>/PdBi Composite Nanochains as Highly Active and Durable Electrocatalysts for Ethanol Oxidation

Yuan, Xiaolei; Zhang, Yong; Cao, Muhan; Zhou, Tong; Jiang, Xiaojing; Chen, Jinxing; Lyu, Fenglei; Xu, Yong; Luo, Jun; Zhang, Qiao; Yin, Yadong

doi:10.1021/acs.nanolett.9b01843

Cited by 110 publications

(113 citation statements)

References 49 publications

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“…These results confirm the extremely promising longevity of PtBi@PtRh 1 nanoplates in the EOR. [52,53] Typically, the outstanding durability would originate from superior anti-poisoning ability and structural stability. As shown in Figure 3g,h; Figure S37 in the Supporting Information, the PtBi@PtRh 1 catalyst exhibits superior antipoisoning ability, possessing a steady platform to high current density with a negative shift in potential, and easily recovering/ retaining the higher current densities by introducing CO/ CH 3 CHO compared with PtBi@Pt and Pt/C catalysts.…”

Section: Resultsmentioning

confidence: 99%

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

et al. 2021

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which is also considered a biorenew able energy carrier. However, the anodic ethanol oxidation reaction (EOR) is a complicated and kinetically sluggish process, involving the transfer of multiple electrons and various reaction intermediates and products. Typically, the C2-pathway dominates the EOR in both acidic and alkaline electrolytes, resulting in the formation of acetic acid or acetate by delivering four electrons, and acetaldehyde by delivering two electrons, respectively. The C1-pathway, which involves complete oxidation and the transfer of 12 electrons generating CO 2 or carbonate, is preferred to the C2-pathway, aiming for maximum DEFCs efficiency. [1][2][3][4][5] Specially, highly efficient catalysts have been developed by engineering Pt-based nanocrystals, and the C1-pathway selectivity has been promoted by Rh-based catalysts. [6][7][8][9] In designing electrochemical surfaces toward maximum performance, modifying the electronic structure and strain of catalytic surfaces are considered state-of-the-art strategies, which can for instance be achieved by introducing metals with different intrinsic reactivities and constructing core-shell nanostructures, respectively. [10][11][12][13][14][15] Combining these approaches in a rational manner would be a promising way to substantially improve the EOR, yet the underlying knowledge about their contributions is largely lacking. [10][11][12][13][14][15][16][17][18] Therefore, it is highly desirable to employ tailored nanostructures to resolve these important issues and contribute to the practical deployment of DEFCs by identifying versatile EOR electrocatalysts possessing high atom utilization of noble metals, high mass-normalized activity at low overpotentials, high C1-pathway selectivity, long-term durability, and superior anti-poisoning ability. [1] To maximize atom utilization, single-atom catalysts (SACs) have emerged as one of the most promising frontiers in materials chemistry. [19][20][21] Using specific support materials such as reducible metal oxides, activated carbons, and anisotropic materials such as MoS 2 , single atoms of catalytically metals can be stabilized, which exhibit intriguing physicochemical properties compared with their counterpart clusters and nanoparticles. [22][23][24] Typically, high-performance EOR catalysts should facilitate multiple dehydrogenation and oxidation steps as well as CC bond cleavage reactions. All these reactions typically require ensembles of surface metal atoms, implying that thisThe rational design and control of electrocatalysts at single-atomic sites could enable unprecedented atomic utilization and catalytic properties, yet it remains challenging in multimetallic alloys. Herein, the first example of isolated Rh atoms on ordered PtBi nanoplates (PtBi-Rh 1 ) by atomic galvanic replacement, and their subsequent transformation into a tensile-strained Pt-Rh single-atom alloy (PtBi@PtRh 1 ) via electrochemical dealloying are presented. Benefiting from the Rh 1 -tailored Pt (110) surface with tensile strain, the PtBi@...

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Section: Resultsmentioning

confidence: 99%

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

et al. 2021

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“…Furthermore, a harsher environment wherein the catalysts were directly exposed to CO gas was created to test their stabilities in EOR. [ 36 ] The catalysts were exposed to CO for 400 s during CA tests. As shown in Figure 2h, once Pt/C and Pt NWs/C were exposed to CO, their current densities immediately dropped dramatically.…”

Section: Resultsmentioning

confidence: 99%

Single‐Atom In‐Doped Subnanometer Pt Nanowires for Simultaneous Hydrogen Generation and Biomass Upgrading

Zhu

et al. 2020

Adv Funct Materials

105

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Replacing the anodic oxygen evolution reaction (OER) with a thermodynamically favorable ethanol oxidation reaction (EOR) is regarded as a promising approach to simultaneously realize energy-saving H 2 evolution and highvalue chemical production. Herein, the single-atom In-doped subnanometer Pt nanowires (SA In-Pt NWs) as high-performance electrocatalysts for both the hydrogen evolution reaction (HER) and EOR under universal pH conditions is designed. The SA In-Pt NWs/C can be employed to integrate HER with EOR to avoid the large overpotential caused by sluggish OER, which requires a smaller voltage of 0.62 V to reach 10 mA cm-2 compared with that of water splitting (2.07 V). The reaction also exhibits a high faradaic efficiency of over 93% in upgrading ethanol to valuable acetate in the anodic cell. Mechanistic investigations indicate that the combination of the ultrathin 1D morphology and single-atom In decoration provides the maximum number of active sites and effectively activates Pt atoms for catalysis. Density functional theory calculations further demonstrate that doped In can effectively promote the HER, while also promoting the conversion of ethanol to acetate. Moreover, through the use of SA In-Pt NWs/C as electrocatalysts, many other alcohols can also be employed as anodic feedstock to achieve coupled electrolysis.

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“…4a, b). All catalysts exhibit two peaks in the forward and backward scan, indicating the oxidation of ethanol and the further oxidation of intermediates generated during the forward scan, respectively 15,16,46 . The two most important parameters, i.e., the forward current density (I f ) and the ratio of forward/backward current density (I f / I b ), were evaluated.…”

Section: Supplementarymentioning

confidence: 99%

“…4c). The performance decay may result from the morphology change, the depletion of the reactants, or the reversible blocking of active sites by intermediates 46 . Because the performance fade of Au-Pd-1 almost fully recovered after CV cleaning (see inset diagram of Fig.…”

Section: Supplementarymentioning

confidence: 99%

Unveiling reductant chemistry in fabricating noble metal aerogels for superior oxygen evolution and ethanol oxidation

et al. 2020

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Amongst various porous materials, noble metal aerogels attract wide attention due to their concurrently featured catalytic properties and large surface areas. However, insufficient understanding and investigation of key factors (e.g. reductants and ligands) in the fabrication process limits on-target design, impeding material diversity and available applications. Herein, unveiling multiple roles of reductants, we develop an efficient method, i.e. the excessive-reductant-directed gelation strategy. It enables to integrate ligand chemistry for creating gold aerogels with a record-high specific surface area (59.8 m 2 g −1), and to expand the composition to all common noble metals. Moreover, we demonstrate impressive electrocatalytic performance of these aerogels for the ethanol oxidation and oxygen evolution reaction, and discover an unconventional organic-ligand-enhancing effect. The present work not only enriches the composition and structural diversity of noble metal aerogels, but also opens up new dimensions for devising efficient electrocatalysts for broad material systems.

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Bi(OH)₃/PdBi Composite Nanochains as Highly Active and Durable Electrocatalysts for Ethanol Oxidation

Cited by 110 publications

References 49 publications

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Single‐Atom In‐Doped Subnanometer Pt Nanowires for Simultaneous Hydrogen Generation and Biomass Upgrading

Unveiling reductant chemistry in fabricating noble metal aerogels for superior oxygen evolution and ethanol oxidation

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Bi(OH)3/PdBi Composite Nanochains as Highly Active and Durable Electrocatalysts for Ethanol Oxidation

Cited by 110 publications

References 49 publications

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

A Tensile‐Strained Pt–Rh Single‐Atom Alloy Remarkably Boosts Ethanol Oxidation

Single‐Atom In‐Doped Subnanometer Pt Nanowires for Simultaneous Hydrogen Generation and Biomass Upgrading

Unveiling reductant chemistry in fabricating noble metal aerogels for superior oxygen evolution and ethanol oxidation

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Product

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Bi(OH)₃/PdBi Composite Nanochains as Highly Active and Durable Electrocatalysts for Ethanol Oxidation