Unveiling the Local Structure and Electronic Properties of PdBi Surface Alloy for Selective Hydrogenation of Propyne

Wang, Xuchun; Chu, Mingyu; Wang, Mengwen; Zhong, Qixuan; Chen, Jiatang; Wang, Zhiqiang; Cao, Muhan; Yang, Hao; Cheng, Tao; Chen, Jinxing; Sham, Tsun‐Kong; Zhang, Qiao

doi:10.1021/acsnano.2c06834

Cited by 24 publications

(20 citation statements)

References 52 publications

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“…Finally, all the information points to the formation of PtBi surface alloy on the Pt-rich core (Figure 2i). 28 The catalytic performance was evaluated in a typical threeelectrode system in an alkaline solution containing 1 M KOH and 1 M CH 3 OH. Figure 3a shows the cyclic voltammograms (CVs) of Pt NPs and Pt 92 Bi 8 .…”

Section: T H Imentioning

confidence: 99%

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The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

Wang

Liu

et al. 2023

Nano Lett.

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While tuning the electronic structure of Pt can thermodynamically alleviate CO poisoning in direct methanol fuel cells, the impact of interactions between intermediates on the reaction pathway is seldom studied. Herein, we contrive a PtBi model catalyst and realize a complete inhibition of the CO pathway and concurrent enhancement of the formate pathway in the alkaline methanol electrooxidation. The key role of Bi is enriching OH adsorbates (OH ad ) on the catalyst surface. The competitive adsorption of CO adsorbates (CO ad ) and OH ad at Pt sites, complementing the thermodynamic contribution from alloying Bi with Pt, switches the intermediate from CO ad to formate that circumvents CO poisoning. Hence, 8% Bi brings an approximately 6-fold increase in activity compared to pure Pt nanoparticles. This notion can be generalized to modify commercially available Pt/C catalysts by a microwaveassisted method, offering opportunities for the design and practical production of CO-tolerance electrocatalysts in an industrial setting.

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Section: T H Imentioning

confidence: 99%

“…It indicates that Bi mainly exists in the metallic state and that charge transfers from less electronegative Bi to Pt atoms, in good agreement with core-level observations in XPS and electronegativity argument. Finally, all the information points to the formation of PtBi surface alloy on the Pt-rich core (Figure i) …”

mentioning

confidence: 99%

The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

Wang

Liu

et al. 2023

Nano Lett.

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“…To this end, the realization of alloying structure between Bi and Pd is mostly limited to organic phase or electrodeposition reaction. [33][34][35][36][37][38] Here, the UPD of Bi was demonstrated in the colloidal synthesis of Pd-based NCs for the first time. PdBi alloys with excellent uniformity, controllable morphology and composition were obtained by the combination of UPD and seed-mediated growth method at low-temperature aqueous phase.…”

Section: Introductionmentioning

confidence: 99%

“…To this end, the realization of alloying structure between Bi and Pd is mostly limited to organic phase or electrodeposition reaction. [ 33–38 ]…”

Section: Introductionmentioning

confidence: 99%

Maneuvering the Peroxidase‐Like Activity of Palladium‐Based Nanozymes by Alloying with Oxophilic Bismuth for Biosensing

Xia

Cheng

et al. 2022

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Among different types of nanozymes, noble metal-based nanocrystals (NCs) play an indispensable role because of their excellent catalytic activity, electronic conductivity, thermal stability, and biocompatibility. [6][7][8][9][10][11][12] Furthermore, their catalytic efficiency could be judiciously tailored by modulating their composition, sizes, and morphologies. [13,14] The formation of bimetallic NCs through the introduction of non-noble metals proves to be a powerful means for the enhancement of catalytic performance of noble metal NCs, which not only reduces cost, but also endows the NCs with new advantages of electronic effect, ensemble effect and tunable components. [15][16][17][18] To fully implement the advantageous properties of bimetallic NCs, the exploration of versatile synthetic methods is highly desired. [19,20] Underpotential deposition (UPD) has been introduced into colloidal synthesis of NCs and allows for the regulation of the surface structures and shapes of NCs. Recently, UPD has also been demonstrated in the synthesis of bimetallic noble metal-based NCs by controlling the interaction between noble metals and foreign metals. [21,22] This capability of UPD opens up many possibilities for designing bimetallic noble metal-based NCs. Nonetheless, current reports about this capability are still limited, especially for foreign metals with weak metallicity.As a kind of metal with weak metallicity, the oxophilicity of p (M p ) region metal bismuth (Bi) has been well elucidated, which is beneficial to improve the catalytic oxidation ability of NCs through forming oxygen-containing species on the catalyst surface. [23][24][25] Moreover, the merits of low cost, easy availability, low toxicity, noncarcinogenicity, and high abundance make Bi an attractive material in various applications, especially in biology-related ones. [26,27] However, M p metals are difficult to form alloys with Pd, which usually leads to nanostructures with irregular morphology or poor monodispersity, bringing difficulties to the elucidation of their structure-function relationships in catalysis. [18,[28][29][30][31][32] The challenges in the synthesis of Bi-based alloy NCs are mainly attributed to two reasons: first, Bi precursors are easily hydrolyzed to form oxygen-containing species, second, the low melting point of Bi (271.3 °C) could lead to the Engineering the catalytic performance of nanozymes is of vital importance for their broad applications in biological analysis, cancer treatment, and environmental management. Herein, a strategy to boost the peroxidase-like activity of Pd-based nanozymes with oxophilic metallic bismuth (Bi) is demonstrated, which is based on the incorporation of oxophilic Bi in the Pd-based alloy nanocrystals (NCs). To synthesize PdBi alloy NCs, a seed-mediated method is employed with the assistance of underpotential deposition (UPD) of Bi on Pd. The strong interaction of Bi atoms with Pd surfaces favors the formation of alloy structures with controllable shapes and excellent monodispersity. More import...

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“…Such structural modulations are key for the development of more effective catalysts. [12][13][14] Dopamine undergoes a two-step oxidation process: 11 the rst redox step (a multi-step process) involves a two-electron oxidation process that transforms dopamine to dopamine-o-quinone (redox step I, RS1). The second step then transforms the quinone to aminochrome in a two-electron (multi-step) oxidation process (redox step II, RS2), Scheme 1a.…”

Section: Introductionmentioning

confidence: 99%

Au–Pt–Ni nanochains as dopamine catalysts: role of elements and their spatial distribution

2023

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Unveiling the Local Structure and Electronic Properties of PdBi Surface Alloy for Selective Hydrogenation of Propyne

Cited by 24 publications

References 52 publications

The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

The Role of Bismuth in Suppressing the CO Poisoning in Alkaline Methanol Electrooxidation: Switching the Reaction from the CO to Formate Pathway

Maneuvering the Peroxidase‐Like Activity of Palladium‐Based Nanozymes by Alloying with Oxophilic Bismuth for Biosensing

Au–Pt–Ni nanochains as dopamine catalysts: role of elements and their spatial distribution

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